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<journal-meta>
<journal-id journal-id-type="publisher-id">Front. Environ. Sci.</journal-id>
<journal-title-group>
<journal-title>Frontiers in Environmental Science</journal-title>
<abbrev-journal-title abbrev-type="pubmed">Front. Environ. Sci.</abbrev-journal-title>
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<issn pub-type="epub">2296-665X</issn>
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<publisher-name>Frontiers Media S.A.</publisher-name>
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<article-id pub-id-type="publisher-id">1736443</article-id>
<article-id pub-id-type="doi">10.3389/fenvs.2026.1736443</article-id>
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<subj-group subj-group-type="heading">
<subject>Original Research</subject>
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</article-categories>
<title-group>
<article-title>Spatio-temporal distribution and comprehensive risk assessment of heavy metals in sewage sludge from wastewater treatment plants in the Dianchi Lake basin</article-title>
<alt-title alt-title-type="left-running-head">Wei et al.</alt-title>
<alt-title alt-title-type="right-running-head">
<ext-link ext-link-type="uri" xlink:href="https://doi.org/10.3389/fenvs.2026.1736443">10.3389/fenvs.2026.1736443</ext-link>
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<contrib-group>
<contrib contrib-type="author">
<name>
<surname>Wei</surname>
<given-names>Wei</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
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<name>
<surname>Ma</surname>
<given-names>Jiao</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
<xref ref-type="corresp" rid="c001">&#x2a;</xref>
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<name>
<surname>Xiong</surname>
<given-names>Huabin</given-names>
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<sup>2</sup>
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<surname>L&#xfc;</surname>
<given-names>Ping</given-names>
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<sup>3</sup>
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<surname>He</surname>
<given-names>Zeyu</given-names>
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<given-names>Taoyan</given-names>
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<given-names>Limei</given-names>
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<surname>Zhang</surname>
<given-names>Xu</given-names>
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<sup>1</sup>
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<aff id="aff1">
<label>1</label>
<institution>Kunming Urban Drainage and Sewerage Monitoring Station</institution>, <city>Kunming</city>, <country country="CN">China</country>
</aff>
<aff id="aff2">
<label>2</label>
<institution>Key Laboratory of Ethnomedicine Resource Chemistry of the Ministry of Education, College of Ethnic Medicine, Yunnan Minzu University</institution>, <city>Kunming</city>, <country country="CN">China</country>
</aff>
<aff id="aff3">
<label>3</label>
<institution>Kunming Customs Technology Center</institution>, <city>Kunming</city>, <country country="CN">China</country>
</aff>
<author-notes>
<corresp id="c001">
<label>&#x2a;</label>Correspondence: Xu Zhang, <email xlink:href="mailto:zhxray@163.com">zhxray@163.com</email>; Jiao Ma, <email xlink:href="mailto:jiaojiao@ymu.edu.cn">jiaojiao@ymu.edu.cn</email>
</corresp>
</author-notes>
<pub-date publication-format="electronic" date-type="pub" iso-8601-date="2026-02-23">
<day>23</day>
<month>02</month>
<year>2026</year>
</pub-date>
<pub-date publication-format="electronic" date-type="collection">
<year>2026</year>
</pub-date>
<volume>14</volume>
<elocation-id>1736443</elocation-id>
<history>
<date date-type="received">
<day>31</day>
<month>10</month>
<year>2025</year>
</date>
<date date-type="rev-recd">
<day>19</day>
<month>01</month>
<year>2026</year>
</date>
<date date-type="accepted">
<day>20</day>
<month>01</month>
<year>2026</year>
</date>
</history>
<permissions>
<copyright-statement>Copyright &#xa9; 2026 Wei, Ma, Xiong, L&#xfc;, He, Li, Zuo, Liu and Zhang.</copyright-statement>
<copyright-year>2026</copyright-year>
<copyright-holder>Wei, Ma, Xiong, L&#xfc;, He, Li, Zuo, Liu and Zhang</copyright-holder>
<license>
<ali:license_ref start_date="2026-02-23">https://creativecommons.org/licenses/by/4.0/</ali:license_ref>
<license-p>This is an open-access article distributed under the terms of the <ext-link ext-link-type="uri" xlink:href="https://creativecommons.org/licenses/by/4.0/">Creative Commons Attribution License (CC BY)</ext-link>. The use, distribution or reproduction in other forums is permitted, provided the original author(s) and the copyright owner(s) are credited and that the original publication in this journal is cited, in accordance with accepted academic practice. No use, distribution or reproduction is permitted which does not comply with these terms.</license-p>
</license>
</permissions>
<abstract>
<p>Heavy metals (HMs) in sewage sludge from municipal wastewater treatment plants (WWTPs) pose a latent threat to lake ecosystems. Accurately characterizing their pollution profiles and associated risks is crucial for ecological conservation in cities within globally sensitive lake basins. Focusing on 27 WWTPs across the Dianchi Lake Basin, this study collected 335 sludge samples over 12 consecutive quarters. Leveraging multi-dimensional comprehensive assessment approaches, we analyzed the pollution characteristics, risk levels, and sources of HMs to provide scientific evidence and a scalable framework for safe sewage sludge management in plateau lake basins. Key findings: &#x2460; Arsenic (As) was the dominant pollutant with a high detection rate, with 20 exceedance events in 8 WWTPs; Cadmium (Cd) concentrations ranged from 19 to 259 mg/kg, showing higher pollution risk in the dry season and a spatial pattern of &#x201c;higher in the northeast and lower in the southwest&#x201d;. &#x2461; Cd and mercury (Hg) accounted for 55.4% and 34.6% of the total ecological risk, respectively, being the core risk-driven pollutants. &#x2462; Metal processing and smelting industries were the primary source (41.8% of total load). &#x2463; Membrane bioreactor (MBR) and intermittent cyclic extended aeration system (ICEAS) led to the highest HMs accumulation, with comprehensive pollution indices of 0.280 and 0.250. These findings clarify the key HM pollutants and their risk drivers in the basin, providing targeted support for optimizing sludge management strategies in plateau lake ecosystems.</p>
</abstract>
<kwd-group>
<kwd>heavy metals</kwd>
<kwd>multi-model risk assessment</kwd>
<kwd>sewage sludge</kwd>
<kwd>source apportionment</kwd>
<kwd>spatial-temporal distribution</kwd>
<kwd>wastewater treatment plant</kwd>
</kwd-group>
<funding-group>
<award-group id="gs1">
<funding-source id="sp1">
<institution-wrap>
<institution>Yunnan Nationalities University</institution>
<institution-id institution-id-type="doi" vocab="open-funder-registry" vocab-identifier="10.13039/open_funder_registry">10.13039/501100007847</institution-id>
</institution-wrap>
</funding-source>
<award-id rid="sp1">530100231100001078659</award-id>
<award-id rid="sp1">2026J0516</award-id>
</award-group>
<funding-statement>The author(s) declared that financial support was received for this work and/or its publication. This work was supported by the Special Fund for Monitoring Heavy Metal Exceedances in Sludge Disposal from Urban Sewage Treatment Plants of the Kunming Urban Drainage and Sewerage Monitoring Station, China (Grant No. 530100231100001078659) and the Scientific Research Foundation of Yunnan Provincial Department of Education (Grant No. 2026J0516).</funding-statement>
</funding-group>
<counts>
<fig-count count="8"/>
<table-count count="0"/>
<equation-count count="0"/>
<ref-count count="46"/>
<page-count count="16"/>
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<custom-meta-group>
<custom-meta>
<meta-name>section-at-acceptance</meta-name>
<meta-value>Toxicology, Pollution and the Environment</meta-value>
</custom-meta>
</custom-meta-group>
</article-meta>
</front>
<body>
<sec sec-type="intro" id="s1">
<label>1</label>
<title>Introduction</title>
<p>Urban lakes are core ecological resources that maintain regional hydrological balance, ensure ecological security, and underpin the sustainable development of social economies. For plateau cities in particular, they serve as indispensable strategic water reserves and ecological backbones. However, the accelerated global urbanization process has led to a massive influx of pollutants into lakes via point-source emissions and non-point-source runoff, triggering issues such as water eutrophication and heavy metals (HMs) accumulation. These problems pose severe threats to the ecological functions of lakes and the sustainable development of cities (<xref ref-type="bibr" rid="B8">Feng et al., 2004</xref>; <xref ref-type="bibr" rid="B15">Khan et al., 2025</xref>). Existing studies have confirmed that the unregulated discharge of pollutants such as HMs and microplastics driven by urbanization is the primary factor contributing to the deterioration of urban lake water quality. Some urban lakes have transformed from ecological treasures into environmental hazards, exacerbating the global water crisis and ecological risks (<xref ref-type="bibr" rid="B35">Wang et al., 2016</xref>; <xref ref-type="bibr" rid="B5">Dawn et al., 2025</xref>).</p>
<p>Municipal wastewater treatment is widely recognized as a key measure to intercept point-source pollution and safeguard the water quality of inflow rivers into lakes. In recent years, significant progress has been made in the research and development of wastewater treatment technologies worldwide. Processes have continuously evolved from the traditional activated sewage sludge method to advanced technologies such as the membrane bioreactor (MBR). Relevant studies have primarily focused on improving pollutant removal efficiency, reducing energy consumption, and optimizing process parameters (<xref ref-type="bibr" rid="B19">Lederer and Rechberger, 2010</xref>). For instance, <xref ref-type="bibr" rid="B26">Maheshwari et al. (2008)</xref> systematically compared the treatment efficiency and economic costs of six mainstream wastewater treatment technologies, clarifying the application scenarios and optimization directions of different technical routes. Research on low-energy-consumption wastewater treatment processes has also mostly centered on optimizing process parameters, providing technical support for improving the quality and efficiency of the industry. Nevertheless, these studies have generally been confined to the internal systems of treatment plants, neglecting the environmental impact assessment of sewage sludge&#x2014;a critical by-product.</p>
<p>Sewage sludge from wastewater treatment plants acts as an important &#x201c;sink&#x201d; for HMs in water bodies, and the HMs information it contains holds dual core research value for watershed ecological protection. First, by analyzing the sources, species, and quantity characteristics of HMs in sewage sludge, we can retroactively identify the key driving factors of water pollution in the watershed, predict the pollution risks of water quality changes to lakes in advance, and provide a core basis for the construction of pollution early-warning systems (<xref ref-type="bibr" rid="B4">Dai et al., 2007</xref>; <xref ref-type="bibr" rid="B40">Yi et al., 2011</xref>). Second, sewage sludge is enriched with a large number of persistent toxic substances such as HMs. Improper disposal methods (e.g., random stacking, simple landfilling) can easily lead these substances to re-enter the aquatic environment through leaching and diffusion, making sewage sludge a secondary pollution source of lakes. Therefore, research on sewage sludge can promote the standardized disposal of sewage sludge and block secondary pollution pathways from the source (<xref ref-type="bibr" rid="B29">Scancar et al., 2001</xref>; <xref ref-type="bibr" rid="B9">Fijalkowski et al., 2017</xref>; <xref ref-type="bibr" rid="B32">Smith, 2009</xref>). Although international attention to sewage sludge HMs pollution has gradually increased, existing studies mostly focus on single-dimensional HMs content determination or risk assessment, lacking systematic research that integrates the &#x201c;early-warning function of source-species-quantity analysis&#x201d; with the &#x201c;secondary pollution prevention function of disposal management and control&#x201d; (<xref ref-type="bibr" rid="B18">Kumar et al., 2019</xref>; <xref ref-type="bibr" rid="B33">Soetan et al., 2025</xref>).</p>
<p>Specifically, existing international research has three major limitations. First, there is a lack of continuous observations at the watershed scale. A study by <xref ref-type="bibr" rid="B33">Soetan et al. (2025)</xref> on urban rivers in New Jersey, United States, showed that HMs pollution at the watershed scale exhibits significant spatiotemporal heterogeneity. However, current research primarily relies on discrete sampling and analysis, making it difficult to capture the dynamic evolution laws of pollution in small-scale watersheds and thus unable to provide scientific support for precise early warning. Second, there is a scarcity of specialized research on plateau lake watersheds. Global research on plateau lakes has mostly focused on surveys of natural background HMs in polar or remote regions. For example, a study by <xref ref-type="bibr" rid="B11">Guo et al. (2015)</xref> on lakes in the Qinghai-Tibet Plateau only revealed natural background characteristics and atmospheric deposition sources. In contrast, the migration and transformation laws of HMs in sewage sludge from wastewater treatment plants in urbanized plateau lake watersheds remain unclear (<xref ref-type="bibr" rid="B17">Kittlaus et al., 2025</xref>). Third, research on secondary pollution prevention and control is insufficient. Only a few studies have mentioned the leaching risk of HMs in sewage sludge from temperate lake watersheds (<xref ref-type="bibr" rid="B29">Scancar et al., 2001</xref>; <xref ref-type="bibr" rid="B31">Singh and Agrawal, 2008</xref>), and there has been no systematic evaluation of the secondary pollution threats posed by sewage sludge disposal to lakes, nor has a targeted prevention and control technology system been established.</p>
<p>As the largest plateau freshwater lake in Southwest China, Dianchi Lake serves as the core ecological barrier of Kunming City. However, urbanization and industrialization in the watershed have caused severe HMs pollution, with HMs accumulation detected in water bodies, sediments, and aquatic organisms (<xref ref-type="bibr" rid="B23">Liang et al., 2024</xref>). A large amount of sewage sludge produced by wastewater treatment plants in the watershed has become a potential source of HMs pollution. Nevertheless, the source analysis, species composition, and spatiotemporal variation characteristics of HMs in this sewage sludge remain unclear. This not only hinders the provision of precise early warnings for water pollution risks in Dianchi Lake but also impedes the support for standardized sewage sludge disposal to block secondary pollution. Based on this, this study takes sewage sludge from wastewater treatment plants in the Dianchi Lake Basin as the research object, systematically analyzes the spatiotemporal distribution patterns of HMs, and accurately identifies the sources and species composition of HMs. A multi-dimensional risk assessment system is constructed by integrating the Nemerow index, weighted comprehensive risk index method, and Hakanson index. On the one hand, this system assesses the potential risks of HMs pollution to the lake and provides early warnings; on the other hand, it identifies key risk nodes in sewage sludge disposal and puts forward prevention and control suggestions. This study aims to provide scientific support for the aquatic ecological protection of the Dianchi Lake Basin, while offering a reference paradigm for the sustainable protection of plateau lakes amid global urbanization.</p>
</sec>
<sec sec-type="materials|methods" id="s2">
<label>2</label>
<title>Materials and methods</title>
<sec id="s2-1">
<label>2.1</label>
<title>Sample collection</title>
<p>The Dianchi Lake basin (102&#xb0;29&#x2032;&#x2013;103&#xb0;01&#x2032;E, 24&#xb0;29&#x2032;&#x2013;25&#xb0;28&#x2032;N), located on the Yunnan-Guizhou Plateau in southwestern China, is a densely populated and highly urbanized region with intensive socioeconomic activities (<xref ref-type="fig" rid="F1">Figure 1</xref>). Dewatered sewage sludge samples were collected from 27 municipal WWTPs, (designated D1&#x2013;D27) surrounding Dianchi Lake in Kunming City (<xref ref-type="fig" rid="F1">Figure 1</xref>; <xref ref-type="sec" rid="s11">Supplementary Table S1</xref>). The spatial distribution of the sampling sites was designed to reflect the regional population density gradient, which decreases clockwise from the north to the west, ensuring representative coverage. Specifically, WWTPs D1&#x2013;D11 are situated in the densely populated northwestern area (encompassing Xishan, Wuhua, and Panlong Districts). D12&#x2013;D16 are located in the moderately populated eastern sector (including areas near Changshui Airport and Guandu District). D17&#x2013;D20 serve the less urbanized Chenggong District, while D21&#x2013;D25 are in the southern Jinning District. Finally, D26 and D27 are found in the sparsely populated Haikou Subdistrict. Sampling was performed quarterly from May 2022 to February 2025, in accordance with the Chinese national standard method (GB 24188&#x2013;2009).</p>
<fig id="F1" position="float">
<label>FIGURE 1</label>
<caption>
<p>Distribution of sampling points in the Dianchi Lake basin.</p>
</caption>
<graphic xlink:href="fenvs-14-1736443-g001.tif">
<alt-text content-type="machine-generated">Land use map of the Dianchi Lake basin showing different categories including rivers, farmland, shrubland, forest land, meadow, water area, unused land, construction land, and sampling sites. Colors and a legend indicate these land types. The main map details sampling sites labeled D1 to D27 around the lake and in the surrounding area. Blue indicates rivers and the lake, green various land covers, red for construction land, and black circles for sampling sites. An inset at the top left displays basin elevation in a color gradient from low (blue) to high (red) with a north arrow for orientation.</alt-text>
</graphic>
</fig>
</sec>
<sec id="s2-2">
<label>2.2</label>
<title>Sample analysis methods</title>
<p>The total concentrations of eight HMs mercury (Hg), arsenic (As), cadmium (Cd), lead (Pb), copper (Cu), nickel (Ni), chromium (Cr), and zinc (Zn) in the sewage sludge were determined following Chinese National Standard methods. Samples were digested using a microwave-assisted system with an HCl&#x2013;HNO<sub>3</sub>&#x2013;HF&#x2013;H<sub>2</sub>O<sub>2</sub> mixture. After evaporation to near dryness at 130&#xa0;&#xb0;C, the residues were diluted to volume with 2% nitric acid, filtered, and analyzed by Inductively Coupled Plasma Mass Spectrometry (ICP-MS). MOS-grade reagents and ultrapure water were used throughout the process. Quality control included procedural blanks, parallel samples (&#x2265;10%), and spiked recovery samples (&#x2265;10%). Certified reference materials (<xref ref-type="sec" rid="s11">Supplementary Table S2</xref>) were analyzed to ensure data accuracy, and all procedures complied with the &#x201c;Environmental Water Quality Monitoring Quality Assurance Handbook&#x201d; (<xref ref-type="bibr" rid="B13">He et al., 2016</xref>; <xref ref-type="bibr" rid="B46">Zhao et al., 2008</xref>).</p>
</sec>
<sec id="s2-3">
<label>2.3</label>
<title>Nemerow pollution index method</title>
<p>The Nemerow Pollution Index model (<xref ref-type="bibr" rid="B3">Chen et al., 2024</xref>) integrates both the maximum and average values of single-factor pollution indices, thereby emphasizing the impact of the most contaminated element. The calculation formulas are shown in <xref ref-type="sec" rid="s11">Supplementary Table S2</xref>. The pollution degree is classified into five levels based on the <italic>P</italic>
<sub>
<italic>N</italic>
</sub> value, as shown in <xref ref-type="sec" rid="s11">Supplementary Table S3</xref>.</p>
</sec>
<sec id="s2-4">
<label>2.4</label>
<title>Weighted comprehensive risk score (WCRS) method</title>
<p>To more sensitively identify high-risk WWTPs, this study employed the Weighted Comprehensive Risk Score (WCRS) method (<xref ref-type="bibr" rid="B14">Jiang et al., 2025</xref>; <xref ref-type="bibr" rid="B38">Xia et al., 2024</xref>). Based on the single-factor pollution index (<italic>P</italic>
<sub>
<italic>i</italic>
</sub>, <xref ref-type="sec" rid="s11">Supplementary Table S2</xref>), this method calculates a comprehensive risk score according to the degree of exceedance of HMs limits and their proximity to threshold values (the risk grading criteria and weight design are shown in <xref ref-type="sec" rid="s11">Supplementary Table S4</xref>). It should be noted that the weights of WCRS are derived from empirical analysis, with core calculation basis including exceeding frequency, exceeding degree, and proximity to compliance limits. Toxicological weights, bioavailability, or uncertainty analysis are not included, making it a management-oriented tool for risk priority ranking and early warning. The assessment in this study was primarily based on the &#x201c;Sewage Sludge Quality from Municipal Wastewater Treatment Plant&#x201d; standard (GB24188-2009) (<xref ref-type="sec" rid="s11">Supplementary Table S2</xref>).</p>
</sec>
<sec id="s2-5">
<label>2.5</label>
<title>Potential ecological risk index assessment model</title>
<p>The Potential Ecological Risk Index method, proposed by the Swedish scholar Hakanson (<xref ref-type="bibr" rid="B12">Hakanson, 1980</xref>) is based on sedimentological theory. It comprehensively considers the toxicity, migration potential, and environmental behavior characteristics of HMs to assess their pollution degree and potential ecological risk in sediments. The calculation formulas are shown in <xref ref-type="sec" rid="s11">Supplementary Table S2</xref>. The prescribed toxic response factors (<italic>T</italic>
<sub>
<italic>r</italic>
</sub>) for Cd, Zn, Cr, Cu, Ni, As, Hg, and Pb are 30, 1, 2, 5, 5, 10, 40, and 5, respectively. The reference values were set according to the Grade II standard (pH 6.5&#x2013;7.5) of the &#x201c;Environmental Quality Standard for Soils&#x201d; (GB 15618&#x2013;1995). The classification criteria for the ecological risk factor (<italic>E</italic>
<sub>
<italic>r</italic>
</sub>) and index (<italic>RI</italic>) are provided in <xref ref-type="sec" rid="s11">Supplementary Table S5</xref>.</p>
</sec>
<sec id="s2-6">
<label>2.6</label>
<title>Analysis of HMs pollution source characteristics</title>
<p>To identify the sources and interrelationships of the HMs, the following multivariate statistical methods were comprehensively applied. Pearson correlation analysis (<xref ref-type="bibr" rid="B38">Xia et al., 2024</xref>; <xref ref-type="bibr" rid="B37">Wang et al., 2025</xref>) was performed based on the single-factor pollution indices (<italic>P</italic>
<sub>
<italic>i</italic>
</sub> &#x3d; <italic>C</italic>
<sub>
<italic>i</italic>
</sub>/<italic>S</italic>
<sub>
<italic>i</italic>
</sub>) to calculate correlation coefficients between the risk indices of different metals and their significance (p-values). Data normality was checked using the Shapiro-Wilk test. Local correlation analysis was conducted specifically for exceeding metals in high-risk WWTPs, with results corrected using the Bonferroni method.</p>
<p>Hierarchical cluster analysis (Q-mode clustering) was applied to classify the eight HMs based on their annual average concentrations. Data were standardized using Z-scores. The Euclidean distance was used as the measure, and the average linkage method was employed to construct the cluster structure, visualized via a dendrogram (<xref ref-type="bibr" rid="B2">Bux et al., 2023</xref>).</p>
<p>Principal Component Analysis (PCA) (<xref ref-type="bibr" rid="B2">Bux et al., 2023</xref>) is a statistical method for data dimensionality reduction and information extraction. PCA was performed on the monitoring dataset (27 WWTPs &#xd7; 12 quarters &#xd7; 8 HMs). Data were standardized using Z-scores. The suitability of the data for PCA was confirmed by the Kaiser-Meyer-Olkin (KMO) measure (0.72) and Bartlett&#x2019;s test of sphericity (p &#x3c; 0.001). For comparative validation, non-linear dimensionality reduction techniques, namely t-Distributed Stochastic Neighbor Embedding (t-SNE, perplexity &#x3d; 30) and Uniform Manifold Approximation and Projection (UMAP), were also employed.</p>
</sec>
<sec id="s2-7">
<label>2.7</label>
<title>Data analysis</title>
<p>All data analysis, result processing, and visualization in this study were conducted on the Jupyter Notebook platform. The NumPy (v1.26.0) and Pandas (v2.1.1) libraries of Python were employed for raw data cleaning, standardization, and extraction of statistical characteristics. Principal Component Analysis (PCA), Pearson correlation analysis, and Shapiro-Wilk normality test were implemented using the scikit-learn (v1.3.0) and SciPy (v1.11.2) libraries. Q-mode hierarchical cluster analysis was accomplished with the hierarchical clustering module of the scikit-learn library, and the dendrogram visualization was realized by relying on the seaborn (v0.12.2) and matplotlib (v3.8.0) libraries. Nonlinear dimensionality reduction analyses (t-SNE and UMAP) were performed by invoking the TSNE module of the scikit-learn library and the umap-learn (v0.5.3) package, respectively. Spatiotemporal distribution maps of HMs concentrations, risk index classification maps, and statistical charts were collaboratively plotted using the matplotlib and seaborn libraries. The spatial distribution map of sampling sites and related spatial risk distribution maps were compiled with ArcGIS 10.2 software, and the base maps were uniformly projected in the Plate Carr&#xe9;e projection (WGS84 coordinate system). All analytical processes used a fixed random seed to ensure reproducibility.</p>
</sec>
<sec id="s2-8">
<label>2.8</label>
<title>Standard selection</title>
<p>Three Chinese national standards were selected as evaluation criteria in this study: &#x201c;Sludge Disposal from Municipal Wastewater Treatment Plants - Quality of Sludge for Landscaping&#x201d; (GB/T 23488&#x2013;2009, special for acidic soils), &#x201c;Quality of Sludge from Municipal Wastewater Treatment Plants&#x201d; (GB/T 24188&#x2013;2009), and &#x201c;Control Standards for Pollutants in Sludge for Agricultural Use&#x201d; (GB 4284&#x2013;2018). The selection basis is as follows: these three standards not only comprehensively cover key application scenarios such as general benchmarks for sludge disposal, special standards for landscaping in acidic soils, and special standards for agricultural use, but also have clear legal authority and wide practical universality, which can accurately align with the core theme of this study focusing on sludge resource utilization quality control and environmental risk prevention and control.</p>
<p>Compared with international representative standards (US EPA &#x201c;Standards for Land Application and Surface Disposal of Sludge&#x201d;, EU &#x201c;Directive on the Limitation of Pollutants in Sludge for Agricultural Use&#x201d; (86/278/EEC) and its revised version, supporting standards of Japan&#x2019;s &#x201c;Sludge Reuse Promotion Act&#x201d;), their core commonalities are: all take municipal sewage sludge as the analysis carrier, core control indicators focus on key dimensions such as heavy metals, pathogens, and physical and chemical properties, limit setting is based on environmental risk thresholds as the core logic, and the scope of application collectively covers global mainstream sludge resource utilization paths such as landscaping and agricultural use. Therefore, the domestic standards selected in this study have high comparability with international standards. In addition, the current mainstream municipal wastewater treatment processes (e.g., activated sludge process) are highly similar globally, resulting in small differences in sludge generation characteristics, and the research results can feed back the standard-setting work of countries in similar regions.</p>
</sec>
<sec id="s2-9">
<label>2.9</label>
<title>Model validation and uncertainty analysis</title>
<p>To ensure the reliability of risk models and dimensionality reduction analysis results, the following validation and uncertainty analysis were conducted:</p>
<p>5-fold stratified cross-validation was used to ensure the reliability of t-SNE and UMAP models. A total of 335 sludge heavy metal samples were stratified according to spatiotemporal characteristics to ensure the consistency of the distribution of training/test sets; key parameters were optimized through grid search (t-SNE: perplexity 5&#x2013;50, learning rate 10&#x2013;1,000; UMAP: neighborhood size 5&#x2013;50, min distance 0.01&#x2013;0.5), the optimal parameters were determined with the goal of maximizing the silhouette coefficient, and the generalization ability of the model was verified through the test set.</p>
<p>Uncertainty sources and propagation: &#x2460; Data-driven uncertainty: Derived from the spatiotemporal heterogeneity of samples and high-dimensional data noise, which affects the clustering boundary through sample input propagation; &#x2461; Parameter uncertainty: Differences in key parameter values change the distance weight, which is propagated through parameter optimization and has a more significant impact under low sample size; &#x2462; Inherent algorithm uncertainty: Differences in the focus of t-SNE and UMAP on data structure lead to result differences, which affect the interpretation of pollution sources through core logic propagation. The above uncertainties propagate step by step along &#x201c;sample input&#x2014;parameter optimization&#x2014;dimensionality reduction output&#x201d;, which may affect the accuracy of HMs spatiotemporal characteristic identification and source apportionment.</p>
<p>Uncertainty control measures: Through strict sample quality control (e.g., standardizing sampling and pretreatment processes), multiple rounds of parameter iterative optimization, and cross-validation of multi-algorithm (PCA/t-SNE/UMAP) results, the impact of uncertainty on the accuracy of research conclusions is minimized as much as possible.</p>
</sec>
</sec>
<sec sec-type="results|discussion" id="s3">
<label>3</label>
<title>Results and discussion</title>
<sec id="s3-1">
<label>3.1</label>
<title>Concentration statistics and seasonal variation of HMs in sewage sludge</title>
<p>Statistical summaries of HMs concentrations in sewage sludge samples are provided in <xref ref-type="sec" rid="s11">Supplementary Table S6</xref> (see <xref ref-type="sec" rid="s11">Supplementary Figures S1&#x2013;S8</xref>). The median concentrations of metals followed the order: Zn &#x3e; Cu &#x3e; Cr &#x3e; Pb &#x3e; Ni &#x3e; As &#x3e; Hg &#x3e; Cd. The Kolmogorov-Smirnov test showed that all elements except Cr significantly deviated from the normal distribution. Cd, Zn, Cu, As, and Pb exhibited strong positive skewness (skewness coefficients: 3.68&#x2013;11.26); the extreme skewness of As (11.26) and Cd (5.33) was likely caused by intermittent industrial point-source discharges (e.g., electronics manufacturing and electroplating) (<xref ref-type="bibr" rid="B24">Liu and Wang, 2024</xref>; <xref ref-type="bibr" rid="B6">Durairaj, 2024</xref>; <xref ref-type="bibr" rid="B30">Shao et al., 2024</xref>). One-way ANOVA confirmed significant seasonal and spatial variability in HM concentrations (F &#x3d; 12.36, p &#x3c; 0.001 for seasonal variation; F &#x3d; 8.72, p &#x3c; 0.001 for spatial variation).</p>
<p>The single-factor pollution index (<italic>P</italic>
<sub>
<italic>i</italic>
</sub>) assessment over 12 quarters identified As as the most widespread exceeding pollutant, with 20 exceedance events across 8 WWTPs (<xref ref-type="fig" rid="F2">Figure 2a</xref>). WWTP D1 had the most severe pollution, with five consecutive quarters of As exceedance (Q2 2023&#x2013;Q3 2024). Seasonal analysis showed As exceedance in six WWTPs (<xref ref-type="fig" rid="F2">Figure 2b</xref>): D2, D15, and D21 had higher risks in the wet season, while D3, D12, and D13 showed elevated risks in the dry season.</p>
<fig id="F2" position="float">
<label>FIGURE 2</label>
<caption>
<p>Quarterly variation of the single-factor pollution index <italic>P<sub>i</sub>
</italic> for <bold>(a)</bold> As, <bold>(c)</bold> Cd, and <bold>(e)</bold> Zn, Comparison of <italic>P<sub>i</sub>
</italic> values for <bold>(b)</bold> As, <bold>(d)</bold> Cd, and <bold>(f)</bold> Zn between wet and dry seasons for each wastewater treatment plant.</p>
</caption>
<graphic xlink:href="fenvs-14-1736443-g002.tif">
<alt-text content-type="machine-generated">Six-panel figure showing trends and seasonal comparisons for arsenic (As), cadmium (Cd), and zinc (Zn) risk coefficients and concentrations at wastewater plants. Panels (a), (c), and (e) display quarterly risk coefficient trends from 2022 Q2 to 2025 Q1, with specific plants and safety thresholds indicated. Panels (b), (d), and (f) present bar charts comparing As, Cd, and Zn concentrations between wet (blue) and dry (red) seasons across multiple plant IDs, noting risk points and trend lines with correlation coefficients. Error bars represent standard deviations.</alt-text>
</graphic>
</fig>
<p>Cd exhibited distinct seasonal and spatial characteristics, with exceedances occurring primarily in Q1 (dry season) (<xref ref-type="fig" rid="F2">Figure 2c</xref>). Cd pollution was concentrated in D3, D12, and D15 (<xref ref-type="fig" rid="F2">Figure 2d</xref>), with all exceedances recorded in the dry season&#x2014;a pattern attributed to rainfall dilution in the wet season versus concentrated industrial wastewater discharge in the dry season. Zn pollution was minor, with isolated exceedances in D5 and D6 (<xref ref-type="fig" rid="F2">Figure 2e,f</xref>); D5 had higher Zn concentrations in the dry season, while D6 showed the opposite trend, indicating potential non-point source pollution from rainfall runoff and galvanized pipe corrosion (<xref ref-type="bibr" rid="B22">Li et al., 2019</xref>; <xref ref-type="bibr" rid="B44">Zhang P. et al., 2024</xref>; <xref ref-type="bibr" rid="B45">Zhang L. et al., 2024</xref>).</p>
<p>Overall, As, Cd, and Zn risks were lower in the wet season than in the dry season. Spatially, the combined concentration of these three metals decreased clockwise along the lakeshore from D2 to D26. Hg concentrations were significantly higher in the wet season (p &#x3c; 0.05), suggesting rainfall-facilitated migration; Pb concentrations increased from north to south, peaking at D24 (potentially linked to high population density and limited WWTP capacity in Jinning District). Cr and Ni showed no clear spatiotemporal patterns. Key spatiotemporal risk characteristics are summarized in <xref ref-type="sec" rid="s11">Supplementary Table S7</xref> (Ranking of Heavy Metal Risk Levels by Season and WWTP Location).</p>
</sec>
<sec id="s3-2">
<label>3.2</label>
<title>Nemerow pollution index evaluation</title>
<p>The Nemerow comprehensive pollution index <italic>P</italic>
<sub>
<italic>N</italic>
</sub> for each HMs was calculated with reference to three Chinese national standards (<xref ref-type="bibr" rid="B27">Olejnik, 2024</xref>) (<xref ref-type="sec" rid="s11">Supplementary Table S1</xref>), with the results detailed in <xref ref-type="sec" rid="s11">Supplementary Tables S8-S10</xref>. The assessed pollution characteristics varied considerably depending on the standard applied. Exceedances of Cd and As were most pronounced under the GB/T 23486-2009 standard. In contrast, only As at Plant D1 exceeded the limit under the GB 24188-2009 standard, largely due to its more lenient thresholds for metals such as Cd. Under the GB 4284-2018 standard, As at Plant D1 remained in exceedance. Notably, Cr, Cu, Ni, Hg, and Pb did not exceed the limits in any of the three standards, indicating a relatively low pollution risk from these elements. Plants D1, D2, and D3 exhibited significantly higher exceedance frequencies than others.</p>
<p>D1 had <italic>P</italic>
<sub>
<italic>N</italic>
</sub> values &#x3e; 1.0 under all three standards (2.24, 1.62, and 1.66, respectively; <xref ref-type="fig" rid="F3">Figure 3</xref>), indicating a consistent pollution risk. The GB/T 23486-2009 standard was the most stringent, identifying three plants (D1, D3, D12) as medium-to-high risk. Both the GB 24188&#x2013;2009 and GB 4284-2018 standards classified only Plant D1 as lightly polluted (Level 3), despite the latter imposing stricter limits for Zn and Cr. The <italic>P</italic>
<sub>
<italic>N</italic>
</sub> values for Plants D2 and D3 exceeded 0.7 under all standards, placing them in a risk warning state. Their geographical proximity to Plant D1 suggests potential common pollution sources and cumulative risks, warranting priority investigation for source apportionment. Statistical summary of risk levels (<xref ref-type="fig" rid="F3">Figure 3</xref>, inset) shows that the proportion of plants classified as safe (Level 1) increased from 74% under GB/T 23486&#x2013;2009 to 89% under both the GB 24188&#x2013;2009 and GB 4284-2018 standards, demonstrating that the stringency of the standard significantly influences the assessment outcome.</p>
<fig id="F3" position="float">
<label>FIGURE 3</label>
<caption>
<p>Bar chart comparing the <italic>P<sub>N</sub>
</italic> values for each wastewater treatment plant under the three national standards. Inset: Stacked bar chart showing the count of WWTPs within each risk level.</p>
</caption>
<graphic xlink:href="fenvs-14-1736443-g003.tif">
<alt-text content-type="machine-generated">Bar chart comparing comprehensive pollution index (P) for multiple wastewater plants under three standards, with most plants below the red safety threshold. Inset bar chart shows most plants classified as safe by GB24188-2009 and GB4284-2018, but many under moderate or alert levels for GB_T23486-2009.</alt-text>
</graphic>
</fig>
<p>The contribution rates of individual HMs to the comprehensive <italic>P</italic>
<sub>
<italic>N</italic>
</sub> value also varied with the standard employed (<xref ref-type="sec" rid="s11">Supplementary Figure S3</xref>). Under GB 24188&#x2013;2009, Cd (0.7%) and As (0.6%) were the primary contributors, followed by Hg (0.3%). Under the stricter GB/T 23486-2009 standard, the contribution rate of Cd increased substantially to 11.0%, that of Hg rose to 8.2%, while As remained stable at 0.6%. Under GB 4284&#x2013;2018, Cd (1.2%) and Hg (0.9%) remained the highest contributors. The contribution rate of As was stable (approximately 0.6%) across all standards, consistently ranking among the top three, whereas Zn and Cu consistently demonstrated the lowest contributions (&#x3c;0.02%). These results robustly identify Cd, Hg, and As as the core pollutants in the study area.</p>
<p>These findings underscore that the Nemerow index assessment is highly dependent on the stringency of the standard limits. Under lenient standards (GB 24188&#x2013;2009), the index tends to underestimate pollution levels, whereas under stringent standards (GB/T 23486&#x2013;2009), it becomes more sensitive and effective at identifying potential risk areas. The Nemerow index is suitable for compliance screening based on sludge disposal pathways (e.g., agricultural use, landscaping) but has limitations: it reflects overall pollution levels mathematically but does not account for HMs biotoxicity or ecological hazards.</p>
</sec>
<sec id="s3-3">
<label>3.3</label>
<title>WCRS for HMs in WWTP sewage sludge</title>
<p>To enhance the sensitivity of identifying high-risk WWTPs, this study applied the Weighted Comprehensive Risk Score (WCRS) method, with all assessments conducted against the GB24188-2009 standard. The spatial distribution of pollutant exceedances revealed distinct patterns for key HMs (<xref ref-type="fig" rid="F4">Figures 4a&#x2013;d</xref>). As was identified as the most severe contaminant, with an exceedance rate of 6.0% (20 out of 335 samples). These exceedances were geographically concentrated at Plants D1 (5 exceedances), D2 (6 exceedances), D3 (4 exceedances), and D15 (2 exceedances), suggesting the potential for persistent industrial discharges or other significant As sources in their catchment areas. In contrast, Cd demonstrated a much lower overall exceedance rate (0.9%, 3/335). Its exceedances were isolated, occurring solely at Plants D3, D12, and D15, which is indicative of localized point source pollution that requires targeted attention. Zn exhibited a similarly low exceedance rate of 0.6% (2/335), with incidents located at Plants D5 and D6. These occurrences may be linked to discharges from electroplating or metallurgical activities. Notably, Hg did not exceed the standard limit in any sample, implying relatively effective control of this element in the incoming wastewater to the WWTPs. Furthermore, as supported by <xref ref-type="sec" rid="s11">Supplementary Figures S16-S19</xref>, no exceedances were detected for Cr, Pb, Cu, or Ni. The median risk coefficients for these metals were substantially below 1, reflecting well-controlled input concentrations throughout the monitoring period. Synthesizing these findings (<xref ref-type="fig" rid="F4">Figure 4d</xref>; <xref ref-type="sec" rid="s11">Supplementary Table S11</xref>), the pollutants were categorized hierarchically: As was unequivocally the primary pollutant, with Cd and Zn constituting secondary pollutants of concern.</p>
<fig id="F4" position="float">
<label>FIGURE 4</label>
<caption>
<p>Box plots (with median trend line) and scatter distributions of the single-factor pollution index (<italic>P<sub>i</sub>
</italic>) for 8 HMs across the 27 WWTPs: <bold>(a)</bold> As, <bold>(b)</bold> Cd, <bold>(c)</bold> Zn. <bold>(d)</bold> Distribution plot of the risk coefficients for each metal (logarithmic scale).</p>
</caption>
<graphic xlink:href="fenvs-14-1736443-g004.tif">
<alt-text content-type="machine-generated">Panel a shows a scatter and line plot of arsenic (As) risk coefficients across 27 wastewater treatment plants, with 20 out of 335 points exceeding the standard risk limit of 1; panel b presents cadmium (Cd) data with 3 exceedances; panel c displays zinc (Zn) data with 2 exceedances; each panel includes median (red line) and standard limit (green dashed line); panel d summarizes risk coefficient distributions for eight heavy metals, with a red dashed line marking the exceedance threshold of 1.</alt-text>
</graphic>
</fig>
<p>The application of the WCRS method, utilizing the weighting criteria in <xref ref-type="sec" rid="s11">Supplementary Table S4</xref>, enabled a refined risk classification for plants with recorded exceedances (detailed results in <xref ref-type="sec" rid="s11">Supplementary Table S12</xref>). The risk categorization was as follows. Medium Risk: Plant D3, with a score of 5 points due to concurrent exceedances of As and Cd; Plants D12 and D15, each scoring 4 points for exceeding two HMs; and Plant D1, scoring 3 points primarily for As exceedance coupled with the proximity of other metals to their thresholds. Low Risk: Plants D5 and D6, scoring 2 points for Zn exceedance only; and other plants, such as D2 and D21, which also scored 2 points for a single As exceedance. The key advantage of the WCRS method lies in its ability to identify &#x201c;critical pollution states.&#x201d;</p>
<p>Unlike the traditional Nemerow index, which focuses primarily on pollutants that have already exceeded standards, the WCRS method incorporates points for metals approaching their thresholds. This provides an early warning for potentially escalating risks, shifting the management focus towards prevention. Kappa consistency test confirmed good agreement between WCRS and Hakanson risk grades (Kappa &#x3d; 0.76, p &#x3c; 0.001). It should be noted that, as a management-oriented tool, the WCRS has inherent limitations: it does not consider toxicological differences between heavy metals, bioavailability of heavy metals in sludge, or uncertainties in monitoring data. These factors may restrict its ability to reflect the actual ecological toxicity risks of heavy metals, and thus it should be used in conjunction with ecotoxicity-oriented indices such as the Hakanson index rather than as a standalone risk assessment method.</p>
</sec>
<sec id="s3-4">
<label>3.4</label>
<title>Assessment of potential ecological risk with Hakanson index</title>
<p>Sewage sludge that meets the criteria specified in the standard Disposal of Sludge from Municipal Wastewater Treatment Plants - Quality of Sludge for Agricultural Use (GB 24188&#x2013;2009) can be utilized for land-based resource recovery. In this study, the Hakanson potential ecological risk index method was adopted, based on the similarity of toxicological interaction mechanisms between HMs and biological receptors in sludge and those in sediments (<xref ref-type="bibr" rid="B20">Lei, 2023</xref>; <xref ref-type="bibr" rid="B42">Yu et al., 2023</xref>; <xref ref-type="bibr" rid="B10">Geng et al., 2021</xref>; <xref ref-type="bibr" rid="B1">Buthnoo et al., 2025</xref>). The model identified Cd and Hg as the predominant contributors to the overall ecological risk (<xref ref-type="fig" rid="F5">Figure 5a</xref>). Cd posed a substantial risk across the study area. The ecological risk factor (Er) for Cd far exceeded the threshold for &#x201c;very high risk&#x201d; (Er &#x3e; 320) at several plants, including D1 (1,065.5), D3 (819.5), D2 (486.8), D12 (551.8), D15 (461.8), and D8 (395.2). Eleven additional plants were classified as &#x201c;high risk&#x201d; (Er &#x3d; 170.1&#x2013;291.3), and ten plants posed a &#x201c;considerable risk&#x201d; (Er &#x3d; 100.3&#x2013;137.0).</p>
<fig id="F5" position="float">
<label>FIGURE 5</label>
<caption>
<p>
<bold>(a)</bold> Potential Ecological Risk Index (<italic>E<sub>r</sub>
</italic>) results for HMs across the 27 WWTPs. <bold>(b)</bold> Spatial coupling characteristics between the comprehensive pollution index (<italic>C<sub>d</sub>
</italic>) and the Potential Ecological Risk Index (<italic>RI</italic>); bubble size represents the maximum value of the single pollution coefficient (<italic>C<sub>f</sub>
</italic>) for the HMs.</p>
</caption>
<graphic xlink:href="fenvs-14-1736443-g005.tif">
<alt-text content-type="machine-generated">Panel (a) presents a color-coded matrix showing ecological risk factors for various metals by plant, highlighting cadmium and overall risk levels, with risk categories labeled. Panel (b) features a bubble chart plotting degree of contamination against potential ecological risk, where bubble color represents risk level and size corresponds to maximum contamination factor, with data points labeled by plant code.</alt-text>
</graphic>
</fig>
<p>In contrast, Hg exhibited a clear spatial gradient in risk. Most plants from D1 to D14 presented a &#x201c;high risk&#x201d; (Er &#x3d; 192.2&#x2013;268.8), whereas those from D15 to D27 were predominantly at &#x201c;considerable risk&#x201d; (Er &#x3d; 53.9&#x2013;155.3), with the exception of D16, which showed a &#x201c;moderate risk&#x201d; (53.9). Apart from a &#x201c;moderate risk&#x201d; (Er &#x3d; 64.3) at Plant D1, As was of low risk elsewhere. Zn, Cr, Cu, Ni, and Pb consistently posed a low risk (Er &#x2264; 40) across all plants.</p>
<p>The spatial relationship between the single-factor pollution index and the potential ecological risk index was visualized in a bubble plot (<xref ref-type="fig" rid="F5">Figure 5b</xref>), revealing a significant positive correlation between Cd and the comprehensive Risk Index (RI) (r &#x3d; 0.82, p &#x3c; 0.001). Plants D1, D3, D2, and D12 formed a distinct cluster of extreme risk, classified at the &#x201c;very high&#x201d; pollution level, with Plant D1 exhibiting the peak value. Plant D15 was also associated with a strong ecological hazard. Densely populated areas (encompassing Plants D4&#x2013;D11, D13&#x2013;D14, D20&#x2013;D21) constituted a zone of concentrated &#x201c;strong risk,&#x201d; where Cd levels and the RI were strongly coupled.</p>
<p>A clear spatial pattern emerged, with the core area around Plants D1&#x2013;D3 exhibiting the highest risk, which decreased radially towards the periphery. Plants D16&#x2013;D19 and D22&#x2013;D25 were characterized by &#x201c;moderate risk,&#x201d; while a localized increase observed at Plants D26&#x2013;D27 suggests potential emerging pollution sources. This risk gradient was visually pronounced, as the bubble diameters in high-risk areas (yellow) were approximately 1.8 times larger than those in moderate-risk areas (green), underscoring a strong spatial consistency between pollution intensity and risk level.</p>
<p>The fundamental characteristic of the Hakanson index is its transformation of pollution concentrations into ecological risks through toxic response factors. Meanwhile, it should be noted that the toxic response factors in the Hakanson index are calibrated based on the properties of soils and sediments, and no specific adjustments have been made for the unique characteristics of sludge (such as high organic matter content and high water content). Therefore, the risk estimation results may be conservative. This study positioned the Hakanson index as a tool for relative risk comparison and spatial prioritization. The assessment results showed that cadmium (Cd) and mercury (Hg) were the dominant ecological risk drivers, Cd and mercury (Hg) accounted for 55.4% and 34.6% of the total ecological risk, followed by arsenic (As); spatially, the sludge from WWTPs D1, D3, D12, and D15 exhibited relatively high ecological risks, which was consistent with the spatial distribution characteristics of HMs concentrations. This further confirms that the application of the Hakanson index on the basis of clear premise assumptions can effectively identify high-risk areas and key risk factors in sludge, providing a reliable basis for the spatial prioritization of sludge risk management.</p>
<p>Comparison of risk assessment results from three indices summarizes the complementary advantages and mutually verified assessment of the Nemerow index, WCRS, and Hakanson index, constructing a comprehensive risk assessment framework from regulatory, managerial, and ecological perspectives: the Nemerow index and WCRS identify pollutants of concern (As, Cd) and risk areas (northeast), while the Hakanson index further reveals which of these pollutants (Cd, Hg) pose the greatest potential threat to the ecosystem.</p>
</sec>
<sec id="s3-5">
<label>3.5</label>
<title>Analysis of HMs pollution sources</title>
<p>To systematically identify the sources and interrelationships of HMs in sewage sludge from WWTPs in the Dianchi Lake basin, this study integrated multiple statistical methods, including correlation analysis, cluster analysis, and principal component analysis (PCA). Correlation analysis revealed significant co-variation among the elements (<xref ref-type="fig" rid="F6">Figure 6a</xref>). Four element pairs&#x2014;Cd-Cu, Cd-Ni, Cd-As, and Cu-Ni&#x2014;exhibited highly significant positive correlations (r &#x3d; 0.43&#x2013;0.46, p &#x3c; 0.001). These specific combinations serve as strong evidence for composite pollution sources. The Cd-Cu association is potentially linked not only to electroplating wastewater but also to agricultural activities. According to <xref ref-type="bibr" rid="B34">Wang (2014)</xref>, pesticides (<xref ref-type="bibr" rid="B36">Wang et al., 2018</xref>), fertilizers, and organic fertilizers (<xref ref-type="bibr" rid="B39">Yang et al., 2021</xref>) used in the intensive agricultural greenhouses along the eastern coast of Dianchi Lake are significant sources of Cd and Cu, which enter the sewage system via surface runoff. The Cu-Ni combination is a typical marker for industrial wastewater discharge from electroplating (<xref ref-type="bibr" rid="B28">Peng et al., 2023</xref>), the Cd-Ni combination is commonly associated with the production and disposal of batteries, and the Cd-As and Cu-Ni combinations are closely linked to non-ferrous metal smelting activities (<xref ref-type="bibr" rid="B25">Luo et al., 2023</xref>; <xref ref-type="bibr" rid="B28">Peng et al., 2023</xref>). Historically concentrated paper mills and smelters in northern Dianchi are potential sources of such pollution (<xref ref-type="bibr" rid="B41">Yu et al., 2013</xref>). In contrast, the correlation between Cr and Ni, Pb may suggest another industrial source, such as stainless-steel production or leather tanning, while the weak correlation between Cr and Cd/As indicates independent input pathways for these elements. These inferences regarding industrial origins are highly consistent with the findings of <xref ref-type="bibr" rid="B34">Wang (2014)</xref> on the sector-specific characteristics of HMs in the Dianchi Lake basin and are strongly corroborated by the spatial distribution pattern: the WWTPs with the highest concentrations of these elements (D1, D3, D12) are all concentrated in northern Dianchi, an area identified in official planning documents (<xref ref-type="bibr" rid="B21">Li et al., 2018</xref>) as a traditional agglomeration zone for Kunming&#x2019;s machinery manufacturing, metal processing, and electronics industries.</p>
<fig id="F6" position="float">
<label>FIGURE 6</label>
<caption>
<p>
<bold>(a)</bold> Global correlation matrix of HMs risk coefficients in the WWTPs. <bold>(b)</bold> Hierarchical Cluster Analysis (HCA) dendrogram for the 8 HMs. <bold>(c)</bold> Dimensionality reduction plot of HMs pollution characteristics in WWTPs based on Principal Component Analysis (PCA). <bold>(d)</bold> Non-linear clustering of HMs pollution in WWTPs based on t-SNE. <bold>(e)</bold> Manifold structure visualization of HMs pollution in WWTPs based on UMAP. Colors represent pollution grades; shapes/numbers distinguish individual plants.</p>
</caption>
<graphic xlink:href="fenvs-14-1736443-g006.tif">
<alt-text content-type="machine-generated">Panel (a) shows a matrix of scatter plots, correlation coefficients, and significance values for relationships between heavy metals (Cd, Zn, Cr, Cu, Ni, As, Hg, Pb) and pollution risk measures. Panel (b) presents a dendrogram clustering heavy metals by Euclidean distance. Panel (c) is a PCA biplot classifying wastewater plants by pollution level, with groups delineated by color and symbols. Panel (d) shows a t-SNE visualization of sample clustering, with one group circled in red. Panel (e) displays a UMAP plot with similar grouping and one cluster highlighted in red.</alt-text>
</graphic>
</fig>
<p>Cluster analysis further classified the eight HMs into three groups with distinct sources (<xref ref-type="fig" rid="F6">Figure 6b</xref>). Cluster 1 (Cu, Cd, As) exhibited the smallest within-cluster distance, indicating a highly homogeneous source, which can be strongly attributed to &#x201c;Metal Processing and Smelting Industrial Sources&#x201d;. Cluster 2 (Ni, Cr, Pb) likely represents &#x201c;Mixed Industrial Sources&#x201d;. Previous studies (<xref ref-type="bibr" rid="B25">Luo et al., 2023</xref>) have found that Pb primarily originates from vehicle emissions and industries involved in smelting, manufacturing, and using Pb products. <xref ref-type="bibr" rid="B34">Wang (2014)</xref>, combining spatial distribution characteristics, also inferred that Pb likely stems mainly from industrial production activities. Cluster 3 (Zn, Hg) was geographically distinct, with its high-value zone (D5-D7) located in the old city center of Kunming. The association of Zn and Hg is widely recognized as an indicator of &#x201c;Combustion Sources&#x201d; such as coal burning and municipal waste incineration (<xref ref-type="bibr" rid="B43">Zeng et al., 2021</xref>), consistent with the area&#x2019;s history and current status as a densely populated center of energy consumption.</p>
<p>Principal Component Analysis (PCA) quantitatively resolved the contribution of each source (<xref ref-type="fig" rid="F6">Figure 6c</xref>). PC1 (41.8% variance explained) showed high loadings on Cd, Cu, and As, clearly corresponding to the industrial source represented by Cluster 1. PC2 (22.4% variance explained) was dominated by Zn and Hg, confirming the combustion source represented by Cluster 3. The separation of pollution grades identified by PCA was consistently validated by non-linear dimensionality reduction techniques, namely t-SNE (<xref ref-type="fig" rid="F6">Figure 6d</xref>) and UMAP (<xref ref-type="fig" rid="F6">Figure 6e</xref>), demonstrating the robustness of the source apportionment results. The tight clustering of Grade 1 (clean) WWTPs suggests their catchment areas are dominated by domestic wastewater with single and low-intensity HMs inputs. In contrast, the dispersion of Grade 3 and 4 (moderately and heavily polluted) WWTPs reflects their exposure to multiple, high-intensity industrial or mixed pollution inputs.</p>
<p>Spatial analysis provided a geographical anchor for the above source apportionment (<xref ref-type="fig" rid="F7">Figure 7</xref>). The study area exhibited a significant &#x201c;high in the northeast, low in the southwest&#x201d; pollution pattern. This macroscopic gradient is highly coupled with the industrial layout and urbanization development level of Kunming City. The high-risk cluster in the northeast (D1-D3, D12) is directly downstream of the main industrial zones; their extremely high Cd and As pollution indices are a direct manifestation of point source discharges from non-ferrous metal-related industries. Furthermore, the observed decreasing pollution trend along the Baoxiang River (D12 to D13, D14) and the Panlong River-Mingtong River systems (D4 to D11) confirms the location of point sources (near D12) and also reveals the self-purification capacity of the river systems or dilution effects from tributaries. Overall, except for the northeastern hotspot, WWTPs closer to Lake Dianchi itself generally showed lower sewage sludge pollution indices, proving that the existing sewage treatment network acts as an effective barrier, playing a crucial role in intercepting HMs pollutants within the basin and protecting the water quality of Lake Dianchi.</p>
<fig id="F7" position="float">
<label>FIGURE 7</label>
<caption>
<p>Spatial distribution characteristics of HMs pollution risk in the WWTPs. The color gradient represents the composite pollution index (mean of the ratio of each metal&#x2019;s concentration to its standard limit), with higher values indicating greater pollution risk. Plant numbers are annotated at their GPS coordinates. The base map uses the Plate Carr&#x00E9;e projection.</p>
</caption>
<graphic xlink:href="fenvs-14-1736443-g007.tif">
<alt-text content-type="machine-generated">Map showing Dianchi Lake and its inflowing rivers with labeled monitoring sites (D1&#x2013;D27). Circles indicate pollution risk score at each site, color-coded from green (low) to red (high) with scores provided; highest risk observed at D1 with 0.84. Scale bar and north arrow included.</alt-text>
</graphic>
</fig>
<p>In summary, by coupling multivariate statistics, spatial analysis, and regional anthropogenic activity data, this study advanced the understanding of HMs sources in sewage sludge from statistical inference to geographical substantiation. The results indicate that HMs in Kunming&#x2019;s WWTPs sewage sludge primarily originate from two core processes: (1) Metal processing and smelting industrial activities in the northern and northeastern areas, dominating the input of Cd, Cu, and As; (2) Historical and current energy consumption (coal burning, waste incineration) in the central urban area, contributing most of the Zn and Hg. This refined source apportionment provides a solid scientific basis for implementing a targeted source control strategy characterized by &#x201c;Zoning, Classification, and Grading&#x201d;.</p>
</sec>
<sec id="s3-6">
<label>3.6</label>
<title>Influence of wastewater treatment technologies on HMs accumulation in sewage sludge</title>
<p>To elucidate the relationship between different wastewater treatment processes and the characteristics of HMs accumulation in sewage sludge, this study evaluated 13 technologies across 27 WWTPs. It is critical to emphasize that the HMs concentration in sewage sludge primarily reflects the transfer and enrichment capacity of the process from the aqueous to the solid phase, rather than directly indicating purification efficiency of the effluent. Comprehensive analysis (<xref ref-type="fig" rid="F8">Figure 8</xref>; <xref ref-type="sec" rid="s11">Supplementary Figure S20</xref>) revealed significant differences in the overall HMs accumulation levels in sewage sludge produced by different processes (F &#x3d; 9.42, p &#x3c; 0.001). The Sequencing Batch Reactor (SBR) yielded sewage sludge with the lowest comprehensive HMs accumulation (comprehensive <italic>P</italic>
<sub>
<italic>i</italic>
</sub> &#x3d; 0.084). Conversely, the Membrane Bioreactor (MBR) and Intermittent Cycle Extended Aeration System (ICEAS) produced sewage sludge with the highest accumulation levels (comprehensive <italic>P</italic>
<sub>
<italic>i</italic>
</sub> &#x3d; 0.280 and 0.250, respectively). The highly efficient solid-liquid separation capability of MBR is a key reason for its significant retention and enrichment of metals like Zn. Modified A<sup>2</sup>/O processes (e.g., A<sup>2</sup>/O-M, A<sup>2</sup>/O-MBR) also performed better than the conventional A<sup>2</sup>/O process.</p>
<fig id="F8" position="float">
<label>FIGURE 8</label>
<caption>
<p>Comparison of HMs accumulation characteristics (expressed as the single-factor pollution index, <italic>P<sub>i</sub>
</italic>) in sewage sludge across different wastewater treatment technologies: <bold>(a)</bold> As, <bold>(b)</bold> Cd, <bold>(c)</bold> Hg, <bold>(d)</bold> Cr, <bold>(e)</bold> Cu, <bold>(f)</bold> Ni, <bold>(g)</bold> Zn, <bold>(h)</bold> Pb. In the box plots, the midline represents the median <italic>P<sub>i</sub>
</italic> value, and the box encompasses the 25th to 75th percentiles.</p>
</caption>
<graphic xlink:href="fenvs-14-1736443-g008.tif">
<alt-text content-type="machine-generated">Eight grouped box plots compare mean risk coefficients for treatments across eight heavy metals: arsenic, cadmium, mercury, chromium, copper, nickel, zinc, and lead. Treatments are color-coded and labeled on the x-axes.</alt-text>
</graphic>
</fig>
<p>Regarding individual metals (<xref ref-type="fig" rid="F8">Figure 8a-h</xref>), As accumulation was highest in sewage sludge from ICEAS and MBR processes, while modified processes reduced As enrichment by 48%&#x2013;74% compared to the conventional A<sup>2</sup>/O. Cd enrichment was significant in sewage sludge from A<sup>2</sup>/O-PC and MBR processes but remained at very low levels in various modified processes. The prominent enrichment of Zn in MBR sewage sludge further confirms its highly effective retention capability.</p>
<p>Discussion and Implications: This study establishes that process type is the predominant factor determining the HMs accumulation characteristics in sewage sludge. This provides direct guidance for process selection aimed at sewage sludge safe disposal and resource recovery: for scenarios targeting sewage sludge resource utilization, processes with low HM accumulation (e.g., SBR) are optional, while for scenarios prioritizing effluent water quality control, processes with high HM retention efficiency (e.g., MBR, ICEAS) are more suitable. for new or upgrading WWTPs where sewage sludge recycling is a priority, SBR or modified A<sup>2</sup>/O processes should be considered; for existing plants employing high-accumulation processes like MBR, the strategic focus must be on enhancing source control and pre-treatment to manage the incoming HMs load at its origin. However, a critical trade-off is highlighted: processes like MBR, while ensuring excellent effluent quality, lead to high HMs accumulation in sewage sludge, thereby increasing subsequent disposal challenges and potential environmental risks. Although this field-based study reveals strong correlations, future controlled pilot-scale studies are needed to isolate the influence of influent loadings and precisely quantify the inter-phase transfer efficiency of HMs across different processes.</p>
<p>Our finding that SBR achieves the lowest sludge HM accumulation aligns with EU research demonstrating that optimized treatment processes reduce sludge Hg and Cd concentrations under strict regulations (<xref ref-type="bibr" rid="B7">European Environment Agency, 2025</xref>; <xref ref-type="bibr" rid="B16">Kirchmann et al., 2017</xref>). However, EU studies focus on plain river basins, while our work reveals the unique dry-season high-risk and &#x201c;northeast-southwest&#x201d; spatial gradient of Cd pollution in the Dianchi Lake plateau lacustrine watershed&#x2014;filling the research gap in plateau lake sludge HM risk. A study in Haryana, India also identified industrial activities as the main driver of sludge HM spatial differences (<xref ref-type="bibr" rid="B26">Maheshwari et al., 2008</xref>), consistent with our source apportionment results. Notably, As was not detected in the Indian study, whereas our study recorded 100% As detection rate&#x2014;attributed to intensive non-ferrous metal mining in the Dianchi Lake basin. Globally, most studies rely on single concentration analysis for risk assessment (<xref ref-type="bibr" rid="B4">Dai et al., 2007</xref>; <xref ref-type="bibr" rid="B29">Scancar et al., 2001</xref>); our use of the Hakanson index to quantify Cd/Hg risk contributions (55.4% and 34.6%) further validates the necessity of comprehensive ecological risk assessment. These comparisons highlight the global universality of industrial pollution impacts and the regional specificity of the Dianchi Lake basin, enhancing the study&#x2019;s international academic value.</p>
</sec>
</sec>
<sec sec-type="conclusion" id="s4">
<label>4</label>
<title>Conclusion</title>
<p>This study conducted a systematic evaluation of eight HMs in sewage sewage sludge from 27 wastewater treatment plants in Kunming, revealing several critical findings. As was identified as the most widespread contaminant, while Cd exhibited distinct seasonal fluctuations, with both metals showing peak contamination risks during the dry season. Spatially, a clear &#x201c;high in the northeast, low in the southwest&#x201d; pollution gradient was observed, with plants D1, D3, D12, and D15 designated as priority risk zones. Cd, Hg, and As emerged as the dominant ecological risk factors, primarily originating from industrial activities such as electroplating and smelting. Process performance evaluation further revealed that the MBR and ICEAS achieved the highest HMs retention efficiency.</p>
<p>Building upon these findings, this study developed an integrated multi-model assessment framework that combines the Nemerow index, WCRS, and Hakanson potential ecological risk index. This framework enables a comprehensive evaluation spanning pollution quantification, management early-warning, and ecological toxicity assessment. Based on this methodological advancement, we propose a practical &#x201c;Zoning, Classification, and Grading&#x201d; management strategy specifically tailored for plateau lake-basin cities, providing a scientifically-grounded approach for precise environmental risk management and supporting the safe utilization of sewage sludge resources.</p>
</sec>
</body>
<back>
<sec sec-type="data-availability" id="s5">
<title>Data availability statement</title>
<p>The original contributions presented in the study are included in the article/<xref ref-type="sec" rid="s11">Supplementary Material</xref>, further inquiries can be directed to the corresponding authors.</p>
</sec>
<sec sec-type="author-contributions" id="s6">
<title>Author contributions</title>
<p>WW: Visualization, Conceptualization, Writing &#x2013; review and editing. JM: Visualization, Writing &#x2013; review and editing, Supervision, Writing &#x2013; original draft, Conceptualization. HX: Project administration, Supervision, Writing &#x2013; review and editing. PL&#xfc;: Writing &#x2013; review and editing, Validation. ZH: Validation, Writing &#x2013; review and editing. TL: Investigation, Writing &#x2013; review and editing. LZ: Writing &#x2013; review and editing, Investigation. PLi: Investigation, Writing &#x2013; review and editing. XZ: Project administration, Supervision, Writing &#x2013; review and editing.</p>
</sec>
<ack>
<title>Acknowledgements</title>
<p>The authors gratefully acknowledge the Kunming Urban Drainage and Sewerage Monitoring Station for providing the sewage sludge samples. We also extend our thanks to the Kunming Customs Technology Center for performing the experimental analysis and testing. Furthermore, we appreciate the support from the Key Laboratory of Ethnomedicine Resource Chemistry of the Ministry of Education, College of Ethnic Medicine, Yunnan Minzu University for their assistance in data analysis.</p>
</ack>
<sec sec-type="COI-statement" id="s8">
<title>Conflict of interest</title>
<p>The author(s) declared that this work was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest.</p>
</sec>
<sec sec-type="ai-statement" id="s9">
<title>Generative AI statement</title>
<p>The author(s) declared that generative AI was not used in the creation of this manuscript.</p>
<p>Any alternative text (alt text) provided alongside figures in this article has been generated by Frontiers with the support of artificial intelligence and reasonable efforts have been made to ensure accuracy, including review by the authors wherever possible. If you identify any issues, please contact us.</p>
</sec>
<sec sec-type="disclaimer" id="s10">
<title>Publisher&#x2019;s note</title>
<p>All claims expressed in this article are solely those of the authors and do not necessarily represent those of their affiliated organizations, or those of the publisher, the editors and the reviewers. Any product that may be evaluated in this article, or claim that may be made by its manufacturer, is not guaranteed or endorsed by the publisher.</p>
</sec>
<sec sec-type="supplementary-material" id="s11">
<title>Supplementary material</title>
<p>The Supplementary Material for this article can be found online at: <ext-link ext-link-type="uri" xlink:href="https://www.frontiersin.org/articles/10.3389/fenvs.2026.1736443/full#supplementary-material">https://www.frontiersin.org/articles/10.3389/fenvs.2026.1736443/full&#x23;supplementary-material</ext-link>
</p>
<supplementary-material xlink:href="Supplementaryfile1.docx" id="SM1" mimetype="application/docx" xmlns:xlink="http://www.w3.org/1999/xlink"/>
</sec>
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<p>
<bold>Edited by:</bold> <ext-link ext-link-type="uri" xlink:href="https://loop.frontiersin.org/people/3035230/overview">Liu Jibao</ext-link>, Tokyo Institute of Technology, Japan</p>
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<bold>Reviewed by:</bold> <ext-link ext-link-type="uri" xlink:href="https://loop.frontiersin.org/people/3276576/overview">Shelly Singh</ext-link>, Banasthali University, India</p>
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<ext-link ext-link-type="uri" xlink:href="https://loop.frontiersin.org/people/3279340/overview">Jos&#xe9; Abel Espinoza-Guillen</ext-link>, Universidad Nacional Agraria La Molina, Peru</p>
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<ext-link ext-link-type="uri" xlink:href="https://loop.frontiersin.org/people/3314147/overview">Yufeng Xu</ext-link>, Guilin University of Technology, China</p>
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