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<article article-type="brief-report" dtd-version="2.3" xml:lang="EN" xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">
<front>
<journal-meta>
<journal-id journal-id-type="publisher-id">Front. Environ. Sci.</journal-id>
<journal-title>Frontiers in Environmental Science</journal-title>
<abbrev-journal-title abbrev-type="pubmed">Front. Environ. Sci.</abbrev-journal-title>
<issn pub-type="epub">2296-665X</issn>
<publisher>
<publisher-name>Frontiers Media S.A.</publisher-name>
</publisher>
</journal-meta>
<article-meta>
<article-id pub-id-type="publisher-id">1085386</article-id>
<article-id pub-id-type="doi">10.3389/fenvs.2022.1085386</article-id>
<article-categories>
<subj-group subj-group-type="heading">
<subject>Environmental Science</subject>
<subj-group>
<subject>Brief Research Report</subject>
</subj-group>
</subj-group>
</article-categories>
<title-group>
<article-title>Application of iron&#x2013;carbon microbial galvanic activated sludge combined with MBR process in the treatment of wastewater from comprehensive railway station</article-title>
<alt-title alt-title-type="left-running-head">Zhang 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.2022.1085386">10.3389/fenvs.2022.1085386</ext-link>
</alt-title>
</title-group>
<contrib-group>
<contrib contrib-type="author" corresp="yes">
<name>
<surname>Zhang</surname>
<given-names>Qi</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
<xref ref-type="corresp" rid="c001">&#x2a;</xref>
<uri xlink:href="https://loop.frontiersin.org/people/2077061/overview"/>
</contrib>
<contrib contrib-type="author" corresp="yes">
<name>
<surname>Liang</surname>
<given-names>Zheng</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
<xref ref-type="corresp" rid="c001">&#x2a;</xref>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Guan</surname>
<given-names>Xiaotao</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Liang</surname>
<given-names>Jingwen</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Gao</surname>
<given-names>Pan</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
</contrib>
</contrib-group>
<aff id="aff1">
<sup>1</sup>
<institution>School of Civil Engineering and Architecture</institution>, <institution>East China Jiaotong University</institution>, <addr-line>Nanchang</addr-line>, <country>China</country>
</aff>
<aff id="aff2">
<sup>2</sup>
<institution>Planning and Standard Research Institute</institution>, <institution>The National Railway Administration of the Republic of China</institution>, <addr-line>Beijing</addr-line>, <country>China</country>
</aff>
<author-notes>
<fn fn-type="edited-by">
<p>
<bold>Edited by:</bold> <ext-link ext-link-type="uri" xlink:href="https://loop.frontiersin.org/people/1074777/overview">Shihai Deng</ext-link>, Xi&#x2019;an Jiaotong University, China</p>
</fn>
<fn fn-type="edited-by">
<p>
<bold>Reviewed by:</bold> <ext-link ext-link-type="uri" xlink:href="https://loop.frontiersin.org/people/2071436/overview">Zhifeng Hu</ext-link>, Beijing Academy of Science and Technology, China</p>
<p>
<ext-link ext-link-type="uri" xlink:href="https://loop.frontiersin.org/people/1983797/overview">Xiaowei Wang</ext-link>, Beijing Technology and Business University, China</p>
<p>
<ext-link ext-link-type="uri" xlink:href="https://loop.frontiersin.org/people/1995472/overview">Qiang Kong</ext-link>, Shandong Normal University, China</p>
</fn>
<corresp id="c001">&#x2a;Correspondence: Qi Zhang, <email>qzhang@ecjtu.edu.cn</email>; Zheng Liang, <email>twyliang@126.com</email>
</corresp>
<fn fn-type="other">
<p>This article was submitted to Water and Wastewater Management, a section of the journal Frontiers in Environmental Science</p>
</fn>
</author-notes>
<pub-date pub-type="epub">
<day>22</day>
<month>12</month>
<year>2022</year>
</pub-date>
<pub-date pub-type="collection">
<year>2022</year>
</pub-date>
<volume>10</volume>
<elocation-id>1085386</elocation-id>
<history>
<date date-type="received">
<day>31</day>
<month>10</month>
<year>2022</year>
</date>
<date date-type="accepted">
<day>12</day>
<month>12</month>
<year>2022</year>
</date>
</history>
<permissions>
<copyright-statement>Copyright &#xa9; 2022 Zhang, Liang, Guan, Liang and Gao.</copyright-statement>
<copyright-year>2022</copyright-year>
<copyright-holder>Zhang, Liang, Guan, Liang and Gao</copyright-holder>
<license xlink:href="http://creativecommons.org/licenses/by/4.0/">
<p>This is an open-access article distributed under the terms of the Creative Commons Attribution License (CC BY). 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.</p>
</license>
</permissions>
<abstract>
<p>The application of iron&#x2013;carbon microbial cell activated sludge (ICMC-AS) was carried out in a membrane bioreactor (MBR) processor to treat wastewater from an integrated railway station. Results showed that the chemical oxygen demand (COD), total nitrogen (TN), and total phosphorus (TP) removal efficiencies of the original MBR processor increased from 80%, 30%, and 10% to 92%, 93.5%, and 92%, respectively. Further research showed that the combined sewage treatment system also had a strong impact resistance ability. The combined sewage treatment system ran stably when the COD, TN, and TP concentrations changed greatly. The in-depth analysis of the reaction process and reaction rate of the combined sewage treatment system revealed that the combined system is dominated by COD removal with high nitrogen removal efficiency. The removal rate constants of various pollutants were in the order: <italic>K</italic>
<sub>COD</sub> (0.647 &#xb1; 0.017) &#x3e; <inline-formula id="inf1">
<mml:math id="m1">
<mml:mrow>
<mml:msub>
<mml:mi mathvariant="bold-italic">K</mml:mi>
<mml:mrow>
<mml:mi mathvariant="bold">N</mml:mi>
<mml:msubsup>
<mml:mi mathvariant="bold">O</mml:mi>
<mml:mn mathvariant="bold">3</mml:mn>
<mml:mo>&#x2212;</mml:mo>
</mml:msubsup>
<mml:mo>&#x2212;</mml:mo>
<mml:mi mathvariant="bold">N</mml:mi>
</mml:mrow>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula> (0.416 &#xb1; 0.044) &#x3e; <inline-formula id="inf2">
<mml:math id="m2">
<mml:mrow>
<mml:msub>
<mml:mi mathvariant="bold-italic">K</mml:mi>
<mml:mrow>
<mml:mi mathvariant="bold">N</mml:mi>
<mml:msubsup>
<mml:mi mathvariant="bold">H</mml:mi>
<mml:mn mathvariant="bold">4</mml:mn>
<mml:mo>&#x2b;</mml:mo>
</mml:msubsup>
<mml:mo>&#x2212;</mml:mo>
<mml:mi mathvariant="bold">N</mml:mi>
</mml:mrow>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula> (0.275 &#xb1; 0.014) &#x3e; <italic>K</italic>
<sub>TN</sub> (0.258 &#xb1; 0.083). Calculations of the energy saving and carbon emission reduction of the combined system showed that the system&#x2019;s annual carbon emission reduction could reach more than 388,203.55&#xa0;kg CO<sub>2</sub>e, which remarkably improves the carbon emission reduction effect and obtains a good green effect. The results indicate that adding ICMC-AS to the MBR processor for combined wastewater treatment can substantially improve the efficiency of wastewater treatment and obtain better energy-saving and emission-reducing effects. This combined application provides an effective way for the transformation and upgrading of small- and medium-scale water treatment systems.</p>
</abstract>
<kwd-group>
<kwd>railway wastewater</kwd>
<kwd>micro-electrolytic</kwd>
<kwd>iron-carbon microbial galvanic cell</kwd>
<kwd>combined wastewater treatment</kwd>
<kwd>MBR</kwd>
<kwd>carbon emissions</kwd>
</kwd-group>
</article-meta>
</front>
<body>
<sec id="s1">
<title>1 Introduction</title>
<p>The basic principle of wastewater treatment by activated sludge is based on a series of electrochemical and microbial reactions, such as microelectrolysis and electronic exchange (between different microorganisms, between microorganisms and various organic or inorganic substances, and between various substances) in the water formed by iron&#x2013;carbon galvanic cells. A large number of studies have shown that microelectrolysis has a remarkable degradation effect on refractory substances in sewage treatment (<xref ref-type="bibr" rid="B4">Deng et al., 2020a</xref>). However, the application mechanism and removal efficiency of biochemical water treatment under the action of microelectrolysis are not clear because of the complexity of the microelectrolysis process. Current research on microelectrolysis wastewater treatment focuses on iron and carbon microelectric decontamination technologies. For example, Deng et al. developed a microelectrolytic process coupled with microbial nitrogen removal, which is a contact oxidation process based on the loading of microelectrolytic biological carrier formed by mixing Fe<sup>0</sup> and activated carbon. The process removes nitrogen under micro-oxygen condition. The NH<sub>4</sub>
<sup>&#x2b;</sup>-N and TN removal efficiencies of this process were 92.6% and 95.3%, respectively (<xref ref-type="bibr" rid="B2">Deng et al., 2016a</xref>). Hu et al. developed an iron-rich substrate (IRS) based on iron&#x2013;carbon microelectrolysis that can be used for sediment and overlying water remediation. NH<sub>4</sub>
<sup>&#x2b;</sup>-N, PO<sub>4</sub>
<sup>3&#x2212;</sup>-P, organo-N, organo-P, TN, and total phosphorus (TP) in the overlying water were reduced by 48.6%, 97.9%, 34.2%, 67.1%, 53.2%, and 90.4%, respectively, by IRS during the 90&#xa0;day long-term restoration. Moreover, NO<sub>3</sub>
<sup>&#x2212;</sup>-N, NH<sub>4</sub>
<sup>&#x2b;</sup>-N, and organic N in sediments were reduced by 98.5%, 26.5%, and 6.3%, respectively (<xref ref-type="bibr" rid="B6">Hu et al., 2020</xref>).</p>
<p>Engineering applications are mostly carried out by iron and carbon microelectrolysis combined with biochemical decontamination technology. For example, Qi et al. applied microelectrolysis combined with sequencing batch reactor process to treat oxytetracycline production wastewater. When the influent chemical oxygen demand (COD) was 500&#xa0;mg/L, the average COD removal rate increased from 76.1% to 94.4% (<xref ref-type="bibr" rid="B10">Qi et al., 2016</xref>). Microelectrolysis combined with expanded granular sludge bed and anaerobic/oxic system was used to treat oxytetracycline production wastewater. The oxytetracycline removal rate in the microelectrolysis reaction cell reached more than 95% (<xref ref-type="bibr" rid="B15">Wu et al., 2016</xref>).</p>
<p>In this study, iron&#x2013;carbon microbial cell activated sludge (ICMC-AS) was formed by implanting iron&#x2013;carbon-based materials into activated sludge microbial mass. ICMC-AS &#x2b; membrane bioreactor (MBR) process was used for wastewater treatment in an integrated railway station. In order to solve the pollution problem of low nitrogen, phosphorus and other refractory elements in the original MBR reactor. The reaction principle of ICMC-AS is shown in Equations <xref ref-type="disp-formula" rid="e1">1</xref>&#x2013;<xref ref-type="disp-formula" rid="e4">4</xref>. The operation law of the combined processing system was obtained by studying its operation efficiency and parameters. The application mechanism of biochemical water treatment under the action of microelectrolysis was clarified through in-depth analysis of the reaction process and mechanism of the iron&#x2013;carbon-based microelectrolysis wastewater treatment system. This study provides an effective way for the transformation and upgrading of small- and medium-scale water treatment systems. It also provides technical support and research data basis for the application of microelectrolysis in sewage treatment technology.<disp-formula id="e1">
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</sec>
<sec sec-type="materials|methods" id="s2">
<title>2 Materials and methods</title>
<sec id="s2-1">
<title>2.1 Sewage treatment equipment and raw sewage main quality</title>
<p>The main body of the sewage treatment equipment is an integrated MBR reactor. Raw sewage was used to discharge wastewater from a comprehensive railway station, which consists of a railway passenger station, a large warehouse area, and related supporting facilities. The water quality indexes were COD levels of 100&#x2013;400&#xa0;mg/L, NH<sub>4</sub>
<sup>&#x2b;</sup>-N concentrations of 15&#xa0;&#x2013;45&#xa0;mg/L, TN concentrations of 20&#x2013;60&#xa0;mg/L, and TP concentrations of 2&#x2013;6&#xa0;mg/L.</p>
</sec>
<sec id="s2-2">
<title>2.2 Sewage treatment process</title>
<p>As shown in <xref ref-type="fig" rid="F1">Figure 1</xref> 1) sewage from the integrated railway station was collected through the pipeline to the grid pool of the sewage treatment plant. Inorganic suspended matter in the sewage was removed through a thick and fine grid to reduce the wear on the subsequent pipelines and equipment. The effluent enters the catchment pool. As shown in <xref ref-type="fig" rid="F1">Figure 1</xref> 2) A large number of facultative aerobic bacteria are contained in the facultative MBR system and can degrade organic matter in sewage by the dual action of microelectrolysis and facultative bacteria metabolism to degrade macromolecular organic pollutants into small molecular organic matter, which are eventually oxidized and decomposed into stable inorganic substances. Such as carbon dioxide and water. Moreover, power consumption is reduced, because the generation of facultative bacteria does not need the guarantee of dissolved oxygen (DO). The main function of aeration in a sewage treatment system is to scour and shock membrane filaments, and the DO produced can be used to oxidize a part of the small molecular organic matter and maintain the DO value of the effluent to ensure the normal microbial metabolism in the combined MBR system with concurrent oxygen microelectrolysis.</p>
<fig id="F1" position="float">
<label>FIGURE 1</label>
<caption>
<p>ICMC-AS combined MBR device schematic diagram and process flow chart. 1) Flow chart of Fe&#x2013;C microelectrolysis combined with MBR process. 2) Schematic diagram of ICMC-AS combined MBR device.</p>
</caption>
<graphic xlink:href="fenvs-10-1085386-g001.tif"/>
</fig>
<p>The design scale of the combined treatment system is 400&#xa0;m<sup>3</sup>/day, the design total sludge age is infinite, the organic residual sludge discharge is nearly &#x201c;zero&#x201d; discharge, the mixed liquid concentration (MLSS) is 8000&#x2013;20000&#xa0;mg/L, and the sludge load is 0.02&#xa0;&#x2013;0.10&#xa0;kg COD/(kg MLSS&#x00B7;day).</p>
</sec>
<sec id="s2-3">
<title>2.3 Preparation of iron&#x2013;carbon-based materials</title>
<p>The iron&#x2013;carbon-based material consisted of 40%&#x2013;50% elemental iron powder (300 mesh), 35%&#x2013;42% activated carbon powder (200 mesh), 6%&#x2013;8% metal catalyst (made of various metals), 5%&#x2013;8% adhesive, and foaming agent, etc. The materials were mixed evenly to prepare 1&#xa0;&#x2013;2&#xa0;cm balls, which were dried at 105&#xa0;C for about 2&#xa0;h in a drying oven, preheated at 600&#xa0;C for half an hour in a muffle furnace, and heated at 1000&#xa0;C for 3&#xa0;h. After annealing and cooling, the balls were crushed and sifted to retain particles below 150&#xa0;mesh. The time between production and use should not be too long and should be suitable for real-time production before use to ensure the activity of iron powder and avoid excessive oxidation.</p>
</sec>
<sec id="s2-4">
<title>2.4 Analysis of operation parameters</title>
<sec id="s2-4-1">
<title>2.4.1 Water quality index detection and analysis methods</title>
<p>The wastewater treatment efficiency of the new technology was determined by detecting the water quality indexes (COD<sub>Cr</sub>, NH<sub>4</sub>
<sup>&#x2b;</sup>, NO<sub>3</sub>
<sup>&#x2212;</sup>, NO<sub>2</sub>
<sup>2-</sup>, TP, and TN) in and out of the MBR reactor and comparing with the corresponding indexes of the original MBR reactor without ICMC-AS. COD<sub>Cr</sub> was determined by potassium dichromate method, NH<sub>4</sub>
<sup>&#x2b;</sup> was determined by sodium chlorite spectrophotometry, NO<sub>3</sub>
<sup>&#x2212;</sup> was determined by phenol disulfonic acid spectrophotometry, NO<sub>2</sub>
<sup>2&#x2212;</sup> was determined by N-(1-naphthol)-ethylenediamine spectrophotometry, and TP was determined by potassium persulfate oxidation and ultraviolet spectrophotometry. TN is the sum of the values of NH<sub>4</sub>
<sup>&#x2b;</sup>, NO<sub>3</sub>
<sup>&#x2212;</sup>, and NO<sub>2</sub>
<sup>2&#x2212;</sup>.</p>
</sec>
<sec id="s2-4-2">
<title>2.4.2 Reaction process data detection and reaction rate analysis</title>
<p>Carbon&#x2013;nitrogen reaction rate was determined and the reaction characteristics of the combined process were defined by detecting the concentration changes of COD, NH<sub>4</sub>
<sup>&#x2b;</sup>-N, NO<sub>3</sub>
<sup>&#x2212;</sup>-N, and NO<sub>2</sub>
<sup>&#x2212;</sup>-N during the operation of the MBR reactor (sampling every 30&#xa0;min). The carbon&#x2013;nitrogen reaction rate was calculated by the Origin software.</p>
</sec>
<sec id="s2-4-3">
<title>2.4.3 Estimation methods for energy saving and carbon emissions</title>
<p>Energy saving and carbon emission were estimated from three aspects: power consumption, water consumption, and drug consumption. Power consumption was converted according to the removal rate of the major pollutant (TN) and the increase rate. Water consumption only included the backwashing water. Other supporting water was relatively small, and water condition changed greatly; therefore, it was not measured. Carbon emissions were calculated on the basis of CO<sub>2</sub>.</p>
</sec>
</sec>
</sec>
<sec id="s3">
<title>3 Result and discussion</title>
<sec id="s3-1">
<title>3.1 Variation characteristics of carbon, nitrogen, and phosphorus in the combined sewage treatment system</title>
<p>The data shown in <xref ref-type="fig" rid="F2">Figure 2</xref> 1) show that the COD of the influent municipal sewage varies at 112&#x2013;328&#xa0;mg/L without regularity, and a large change in COD value will have a load impact on the water treatment system (<xref ref-type="bibr" rid="B13">Vleeschauwer et al., 2020</xref>). Studies have shown that such a load impact will often have a great impact on the water treatment system (<xref ref-type="bibr" rid="B17">Yadu et al., 2019</xref>). Experimental data show that the sewage treatment system formed a larger organic shock load, the stable effluent COD value was between 19 and 43&#xa0;mg/L, and the water COD and effluent COD values had a significant positive correlation. However, the ratio changed, which allowed the sewage treatment system to have a good performance and strong load impact resistance. Compared with the original MBR system without ICMC-AS, the COD removal rate of the combined system increased from 80% to 92%.</p>
<fig id="F2" position="float">
<label>FIGURE 2</label>
<caption>
<p>Changes in water quality indicators in the combined sewage treatment system. 1) Changes in COD concentration. 2) Changes in TN and NH<sub>4</sub>
<sup>&#x2b;</sup>-N concentrations. 3) Changes in TP concentration.</p>
</caption>
<graphic xlink:href="fenvs-10-1085386-g002.tif"/>
</fig>
<p>As shown in <xref ref-type="fig" rid="F2">Figure 2</xref> 2), the NH<sub>4</sub>
<sup>&#x2b;</sup>-N value measured at the inlet in the small test fluctuated greatly between 16 and 42&#xa0;mg/L, and the TN value was between 2 and 55&#xa0;mg/L, resulting in the large load impacts of NH<sub>4</sub>
<sup>&#x2b;</sup>-N and TN on the sewage treatment system. The load impacts of NH<sub>4</sub>
<sup>&#x2b;</sup>-N and TN loads have great influence on water treatment system (<xref ref-type="bibr" rid="B8">Meng et al., 2018</xref>). The NH<sub>4</sub>
<sup>&#x2b;</sup>-N and TN values measured at the outlet were maintained at about 2&#x2013;3&#xa0;mg/L, indicating that the sewage treatment system has a strong ability to resist the load impacts of NH<sub>4</sub>
<sup>&#x2b;</sup>-N and TN. In addition, the NH<sub>4</sub>
<sup>&#x2b;</sup>-N and TN removal rates were about 93.5% and 94%, respectively, which are not much different from the removal rates in the laboratory. This finding indicates that the removal capacities for NH<sub>4</sub>
<sup>&#x2b;</sup> and TN in the sewage treatment system were strong, and the current concentrations of NH<sub>4</sub>
<sup>&#x2b;</sup> and TN did not reach the treatment limits. Additionally, the results show that the sewage treatment system has strong adaptability and adjustment ability and can maintain efficient nitrogen pollutant removal ability under a large load shock. Compared with the original MBR system without ICMC-AS, the NH<sub>4</sub>
<sup>&#x2b;</sup>-N and TN removal rates increased from 40% and 30% to 93% and 93.5%, respectively, in the combined system.</p>
<p>As shown in <xref ref-type="fig" rid="F2">Figure 2</xref> 3), the sewage treatment system has a good removal effect. TP values oscillated between 2 and 6&#xa0;mg/L and were maintained at 0.3&#xa0;mg/L after being treated by the sewage treatment system. This result indicates that the system had a stable treatment capacity for the TP of municipal sewage between 2 and 6&#xa0;mg/L (most municipal sewage is within this range), and its removal rate was 92.58% on average. Compared with the original MBR system without ICMC-AS, the TP removal rate of the combined system increased from 10% to 92%.</p>
</sec>
<sec id="s3-2">
<title>3.2 Variation characteristics of carbon and nitrogen in the combined sewage treatment system during operation</title>
<p>As shown in <xref ref-type="fig" rid="F3">Figure 3</xref> 1), COD was removed by rapid consumption within the first 120&#xa0;min, and the value decreased from 400&#xa0;mg/L to 100&#xa0;mg/L. NH<sub>4</sub>
<sup>&#x2b;</sup>-N decreased from 20&#xa0;mg/L to 2.32&#xa0;mg/L within 270&#xa0;min, and NH<sub>4</sub>
<sup>&#x2b;</sup>-N decreased more slowly at 40&#xa0;&#x2013;60 and 90&#xa0;&#x2013;120&#xa0;min. The DO values in these two periods oscillated between 0.2 and 0.3&#xa0;mg/L, indicating that the biochemical reaction of the system was very violent between 0 and 120&#xa0;min, which made the DO values hover between 0.2 and 0.3&#xa0;mg/L and inhibited NH<sub>4</sub>
<sup>&#x2b;</sup>-N decomposition. However, NO<sub>3</sub>
<sup>&#x2212;</sup>-N concentration decreased from 5&#xa0;mg/L to 2.81&#xa0;mg/L between 0 and 40&#xa0;min, increased from 2.58&#xa0;mg/L to 2.89&#xa0;mg/L between 40 and 180&#xa0;min, and gradually decreased to 0.65&#xa0;mg/L between 180 and 360&#xa0;min. This finding is because the concentration change of NO<sub>3</sub>
<sup>&#x2212;</sup>-N is affected by nitrification and denitrification reactions, as well as the biochemical reactions of other elements (such as the biochemical absorption of iron and carbon) (<xref ref-type="bibr" rid="B16">Xing et al., 2016</xref>). Therefore, during the first 0&#x2013;40&#xa0;min, NO<sub>3</sub>
<sup>&#x2212;</sup>-N gradually entered the adsorption plane of various reactions and participated in various reactions. Therefore, its value was rapidly reduced to 2.81&#xa0;mg/L. When these participating reactions reached saturation or equilibrium state, it reflects the comparison between the rates of nitrification reaction (NO<sub>3</sub>
<sup>&#x2212;</sup>-N generation) and denitrification reaction (NO<sub>3</sub>
<sup>&#x2212;</sup>-N transformation and removal) (<xref ref-type="bibr" rid="B3">Deng et al., 2016b</xref>). When the rates of nitrification and denitrification reactions reach equilibrium, the value of NO<sub>3</sub>
<sup>&#x2212;</sup>-N will keep oscillating within a certain numerical range. However, when the denitrification reaction is larger than the nitrification reaction, the value of NO<sub>3</sub>
<sup>&#x2212;</sup>-N will gradually decrease. In this case, NO<sub>2</sub>
<sup>&#x2212;</sup>-N is usually seen as an intermediate product in the conversion of NH<sub>4</sub>
<sup>&#x2b;</sup>-N to NO<sub>3</sub>
<sup>&#x2212;</sup>-N (<xref ref-type="bibr" rid="B5">Deng et al., 2020b</xref>). NO<sub>2</sub>
<sup>&#x2212;</sup>-N accumulated gradually from 0&#xa0;mg/L to 2.21&#xa0;mg/L at 0&#x2013;60&#xa0;min, decreased to 0.61&#xa0;mg/L at 40&#x2013;90&#xa0;min, accumulated gradually accumulated from 0.61&#xa0;m/L to 1.57&#xa0;mg/L at 90&#x2013;240&#xa0;min, and then decreased to 0.35&#xa0;mg/L at 240&#x2013;360&#xa0;min. In the whole process, the value of NO<sub>2</sub>
<sup>&#x2212;</sup>-N experienced two accumulation processes. More complex changes occurred. This change law does not accord with the characteristics of synchronous nitrification and denitrification or short-cut nitrification (<xref ref-type="bibr" rid="B7">Jiaohui et al., 2021</xref>; <xref ref-type="bibr" rid="B14">Wang et al., 2021</xref>; <xref ref-type="bibr" rid="B11">Tong et al., 2022a</xref>; <xref ref-type="bibr" rid="B12">Tong et al., 2022b</xref>). Therefore, based on the analysis of the change values of TN and DO, COD, NH<sub>4</sub>
<sup>&#x2b;</sup>-N, NO<sub>3</sub>
<sup>&#x2212;</sup>-N, NO<sub>2</sub>
<sup>&#x2212;</sup>-N, and DO are co-changing according to a certain correlation. DO showed periodic oscillations and repeated changes during the operation of the system. The changes in DO can be divided into three stages. In the first stage, the operation time of the treatment system was between 0 and 120&#xa0;min, and the DO value in this period changed between 0.1 and 0.4&#xa0;mg/L. In the second stage, the operation time of the treatment system was between 120 and 270&#xa0;min, and the DO value in this period varied between 1.0 and 1.4&#xa0;mg/L. In the third stage, the operation time of the treatment system was between 270 and 360&#xa0;min, and the DO value in this period varied between 1.8 and 2.3&#xa0;mg/L.</p>
<fig id="F3" position="float">
<label>FIGURE 3</label>
<caption>
<p>Process changes of COD, NH<sub>4</sub>
<sup>&#x2b;</sup>-N, NO<sub>3</sub>
<sup>&#x2212;</sup>-N, NO<sub>2</sub>
<sup>&#x2212;</sup>-N, and TN in the operating cycle. 1) Process changes of COD, NH<sub>4</sub>
<sup>&#x2b;</sup>-N, NO<sub>3</sub>
<sup>&#x2212;</sup>-N, NO<sub>2</sub>
<sup>&#x2212;</sup>-N, and TN in the operating cycle. 2) Process changes of COD, NH<sub>4</sub>
<sup>&#x2b;</sup>-N, NO<sub>3</sub>
<sup>&#x2212;</sup>-N, and TN removal rates in the operating cycle.</p>
</caption>
<graphic xlink:href="fenvs-10-1085386-g003.tif"/>
</fig>
</sec>
<sec id="s3-3">
<title>3.3 Carbon and nitrogen removal efficiency of the combined sewage treatment system</title>
<p>As shown in <xref ref-type="fig" rid="F3">Figure 3</xref> 2), the change rate of the NO<sub>3</sub>
<sup>&#x2212;</sup>-N process value was close to that of COD at 0&#x2013;40&#xa0;min, indicating that the process of NO<sub>3</sub>
<sup>&#x2212;</sup>-N reaction during this period was equally dramatic. On the one hand, the reason is that many biochemical reactions of microorganisms in the system require the participation of NO<sub>3</sub>
<sup>&#x2212;</sup>-N. On the other hand, heterotrophic denitrification bacteria at this stage have sufficient organic carbon sources and a large amount of oxygen to efficiently carry out heterotrophic denitrification and consume NO<sub>3</sub>
<sup>&#x2212;</sup>-N. At 40&#x2013;180&#xa0;min, the NO<sub>3</sub>
<sup>&#x2212;</sup>-N process value hardly changed and was in a relative equilibrium state because of the lack of relative oxygen and the indominance of the number of relative denitrifiers in the whole system. However, from the analysis of TN removal rate, the overall TN removal rate was maintained at a relatively high growth level. Moreover, the change rates of the decomposition and process values of NH<sub>4</sub>
<sup>&#x2b;</sup>-N were also maintained at relatively high levels, which indicates that the nitrification and denitrification reactions were maintained at a relatively high dynamic balance. At 180&#x2013;360&#xa0;min, the change rate of the NO<sub>3</sub>
<sup>&#x2212;</sup>-N process value was relatively large, and the COD value dropped to 57&#xa0;mg/L, which made the organic carbon source become relatively short, and the NO<sub>3</sub>
<sup>&#x2212;</sup>-N reaction process was transferred into the ICMC-AS. At this time, the organic carbon source materials (such as extracellular polymers, etc.) stored in ICMC-AS can be combined with the sufficient aerobic environment outside ICMC-AS to carry out heterotrophic denitrification, and the electron supply of ICMC-AS can be combined with the anoxic, facultative, and aerobic regions of MBR to carry out different degrees of autotrophic denitrification (<xref ref-type="bibr" rid="B1">Adav and Lee 2011</xref>; <xref ref-type="bibr" rid="B9">Pellicer-Nacher et al., 2013</xref>). Thus, an efficient denitrification reaction with a change rate similar to the process value of NH<sub>4</sub>
<sup>&#x2b;</sup>-N can be achieved.</p>
</sec>
<sec id="s3-4">
<title>3.4 Carbon and nitrogen removal rate of combined sewage treatment system</title>
<p>As shown in <xref ref-type="fig" rid="F4">Figure 4</xref>, the reaction rate constants of each substance were obtained by fitting the COD, NH<sub>4</sub>
<sup>&#x2b;</sup>-N, NO<sub>3</sub>
<sup>&#x2212;</sup>-N, and TN removal efficiencies. Among them, the <italic>K</italic>
<sub>COD</sub> (0&#x2013;120&#xa0;min) was 0.647 &#xb1; 0.017, which is the maximum reaction rate constant of each substance, and the minimum value of <italic>K</italic>
<sub>TN</sub> was 0.258 &#xb1; 0.083. If only the conversion of NH<sub>4</sub>
<sup>&#x2b;</sup>-N into NO<sub>3</sub>
<sup>&#x2212;</sup>-N under aerobic condition was considered, the converted <inline-formula id="inf3">
<mml:math id="m7">
<mml:mrow>
<mml:msub>
<mml:mi>K</mml:mi>
<mml:mrow>
<mml:msubsup>
<mml:mrow>
<mml:mi mathvariant="normal">N</mml:mi>
<mml:mi mathvariant="normal">O</mml:mi>
</mml:mrow>
<mml:mn>3</mml:mn>
<mml:mo>&#x2212;</mml:mo>
</mml:msubsup>
<mml:mo>&#x2212;</mml:mo>
<mml:mi mathvariant="normal">N</mml:mi>
</mml:mrow>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula> will be about 0.416 &#xb1; 0.044, but the actual conversion to NO<sub>3</sub>
<sup>&#x2212;</sup>-N is not only the ammonification reaction of NH<sub>4</sub>
<sup>&#x2b;</sup>-N. The actual value of <inline-formula id="inf4">
<mml:math id="m8">
<mml:mrow>
<mml:msub>
<mml:mi>K</mml:mi>
<mml:mrow>
<mml:msubsup>
<mml:mrow>
<mml:mi mathvariant="normal">N</mml:mi>
<mml:mi mathvariant="normal">O</mml:mi>
</mml:mrow>
<mml:mn>3</mml:mn>
<mml:mo>&#x2212;</mml:mo>
</mml:msubsup>
<mml:mo>&#x2212;</mml:mo>
<mml:mi mathvariant="normal">N</mml:mi>
</mml:mrow>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula> will be higher than 0.416. Ammonification reaction is the main way to convert NH<sub>4</sub>
<sup>&#x2b;</sup>-N to NO<sub>3</sub>
<sup>&#x2212;</sup>-N; thus, other transformation ways are greatly affected by the reaction conditions. Here, we only calculated the NH<sub>4</sub>
<sup>&#x2b;</sup>-N ammonification reaction after weighted estimation. According to the size of the reaction rate constant, the reaction rates were in the order: <italic>K</italic>
<sub>COD</sub> (0.647 &#xb1; 0.017) &#x3e; <inline-formula id="inf5">
<mml:math id="m9">
<mml:mrow>
<mml:msub>
<mml:mi>K</mml:mi>
<mml:mrow>
<mml:msubsup>
<mml:mrow>
<mml:mi mathvariant="normal">N</mml:mi>
<mml:mi mathvariant="normal">O</mml:mi>
</mml:mrow>
<mml:mn>3</mml:mn>
<mml:mo>&#x2212;</mml:mo>
</mml:msubsup>
<mml:mo>&#x2212;</mml:mo>
<mml:mi mathvariant="normal">N</mml:mi>
</mml:mrow>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula> (0.416 &#xb1; 0.044) &#x3e; <inline-formula id="inf6">
<mml:math id="m10">
<mml:mrow>
<mml:msub>
<mml:mi>K</mml:mi>
<mml:mrow>
<mml:msubsup>
<mml:mrow>
<mml:mi mathvariant="normal">N</mml:mi>
<mml:mi mathvariant="normal">H</mml:mi>
</mml:mrow>
<mml:mn>4</mml:mn>
<mml:mo>&#x2b;</mml:mo>
</mml:msubsup>
<mml:mo>&#x2212;</mml:mo>
<mml:mi mathvariant="normal">N</mml:mi>
</mml:mrow>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula> (0.275 &#xb1; 0.014) &#x3e; <italic>K</italic>
<sub>TN</sub> (0.258 &#xb1; 0.083). Therefore, the combined application system is a wastewater treatment system with high nitrogen removal efficiency dominated by COD removal. The removal rates of various pollutants were in the order of: COD &#x3e; NO<sub>3</sub>
<sup>&#x2212;</sup>-N &#x3e; NH<sub>4</sub>
<sup>&#x2b;</sup>-N &#x3e; TN.</p>
<fig id="F4" position="float">
<label>FIGURE 4</label>
<caption>
<p>Carbon and nitrogen removal rates of the combined sewage treatment system. 1) TN rate fitting; 2) COD rate fitting; 3) NH<sub>4</sub>
<sup>&#x2b;</sup>-N rate fitting; 4) NO<sub>3</sub>
<sup>&#x2212;</sup>-N rate fitting.</p>
</caption>
<graphic xlink:href="fenvs-10-1085386-g004.tif"/>
</fig>
</sec>
<sec id="s3-5">
<title>3.5 Variation of membrane contamination in the combined sewage treatment system</title>
<p>Membrane contamination is inevitable during the operation of the combined system. The system stops the sewage treatment operation and starts the membrane cleaning operation when the membrane pressure difference reaches 50&#xa0;kPa. The membrane cleaning system adopts full automatic control. The membrane pressure difference of the original MBR system reached 50&#xa0;kPa between 5 and 7&#xa0;days, whereas that of the combined system reached 50&#xa0;kPa between 7 and 10&#xa0;days. This finding indicates that the combined system effectively mitigated the membrane contamination. Compared with the original MBR system, the sludge settling performance of the combined system was remarkably improved, and the settling performance of the combined system can reach the settling effect of the original system (30&#xa0;min) in 5&#xa0;min.</p>
</sec>
<sec id="s3-6">
<title>3.6 Energy saving and carbon emission reduction measurement of the combined sewage treatment system</title>
<p>The sewage treatment scale of the railway station is 3,000&#xa0;t/day, including six lifting pumps with a total operating power of 9&#xa0;kW and six MBR wastewater processors with a total operating power of 99&#xa0;kW. This scale translates into a daily power consumption of 1,903.2&#xa0;kWh. According to the TN removal rate, which increased by three times conversion, a total of 1268.8&#xa0;kW&#xa0;h/day energy saving was achieved, and the annual electricity saving was 463,112&#xa0;kWh. The amount of membrane-cleaning water was 159.6&#xa0;t/time, and the drug dosage was 1.92&#xa0;t/day. The average membrane-cleaning volume was reduced from 61&#xa0;times per year to 43&#xa0;times, with a reduction of 18&#xa0;times, saving 2,872.8&#xa0;t of water and 34.54&#xa0;t of drug consumption. According to CO<sub>2</sub> conversion, the annual reduction in electricity was 463,112&#xa0;kWh, which corresponds to the carbon emission reduction of 363,542.92&#xa0;kg CO<sub>2</sub>e; the water saved was 2,872.8&#xa0;t, which corresponds to the carbon emission reduction of 482.63&#xa0;kg CO<sub>2</sub>e; and the reduction in pharmaceutical dosage was 34.54&#xa0;t, which corresponds to the comprehensive carbon emission reduction of 24,178&#xa0;kg CO<sub>2</sub>e. Therefore, the annual carbon reduction of the combined system is at least 388,203.55&#xa0;kg CO<sub>2</sub>e.</p>
</sec>
</sec>
<sec sec-type="conclusion" id="s4">
<title>4 Conclusion</title>
<p>The results showed that ICMS-AS &#x2b; MBR has a strong ability to resist the impacts of COD, NH<sub>4</sub>
<sup>&#x2b;</sup>-N, and TP hydraulic loads. The COD, NH<sub>4</sub>
<sup>&#x2b;</sup>-N, and TP values of raw water vary irregularly at 112.0&#x2013;328.0&#xa0;, 16.0&#x2013;42.0&#xa0;, and 2.0&#x2013;6.0&#xa0;mg/L, respectively, whereas the COD, TN, and TP values of the combined system were all stable in the ranges of 19.2&#x2013;43.3&#xa0;, 2.1&#x2013;3.4&#xa0;, and 0.3&#x2013;0.4&#xa0;mg/L, respectively. This finding indicates that the combined system has good resistance to hydraulic load impact and has stable effluent quality. Compared with the original MBR system without ICMC-AS, the COD, TN, and TP removal efficiencies of the combined system increased from 80%, 30%, and 10% to 92%, 93.5%, and 92%, respectively.</p>
<p>The study of the operation efficiency and parameters of the combined system and the in-depth analysis of the reaction process and reaction rate of the iron&#x2013;carbon microelectrolysis wastewater treatment system revealed that the combined system is a wastewater treatment system dominated by COD removal with high nitrogen removal efficiency. The removal rate constants of various pollutants were in the order: <italic>K</italic>
<sub>COD</sub> (0.647 &#xb1; 0.017) &#x3e; <inline-formula id="inf7">
<mml:math id="m11">
<mml:mrow>
<mml:msub>
<mml:mi>K</mml:mi>
<mml:mrow>
<mml:msubsup>
<mml:mrow>
<mml:mi mathvariant="normal">N</mml:mi>
<mml:mi mathvariant="normal">O</mml:mi>
</mml:mrow>
<mml:mn>3</mml:mn>
<mml:mo>&#x2212;</mml:mo>
</mml:msubsup>
<mml:mo>&#x2212;</mml:mo>
<mml:mi mathvariant="normal">N</mml:mi>
</mml:mrow>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula> (0.416 &#xb1; 0.044) &#x3e; <inline-formula id="inf8">
<mml:math id="m12">
<mml:mrow>
<mml:msub>
<mml:mi>K</mml:mi>
<mml:mrow>
<mml:msubsup>
<mml:mrow>
<mml:mi mathvariant="normal">N</mml:mi>
<mml:mi mathvariant="normal">H</mml:mi>
</mml:mrow>
<mml:mn>4</mml:mn>
<mml:mo>&#x2b;</mml:mo>
</mml:msubsup>
<mml:mo>&#x2212;</mml:mo>
<mml:mi mathvariant="normal">N</mml:mi>
</mml:mrow>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula> (0.275 &#xb1; 0.014) &#x3e; K<sub>
<italic>T</italic>N</sub> (0.258 &#xb1; 0.083).</p>
<p>Compared with the original MBR system, the combined system had a considerably improved sludge settling performance and can reach the settling effect of the original system (30&#xa0;min) in 5&#xa0;min. This performance effectively mitigated membrane contamination in the combined system.</p>
<p>The above results indicate that adding iron&#x2013;carbon microelectrolysis activated sludge to the MBR processor for combined wastewater treatment can enhance the efficiency of wastewater treatment and obtain better energy-saving and emission-reducing effects. This combined application provides an effective way for the transformation and upgrading of small- and medium-scale water treatment systems.</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/supplementary material, further inquiries can be directed to the corresponding authors.</p>
</sec>
<sec id="s6">
<title>Author contributions</title>
<p>All authors listed have made a substantial, direct, and intellectual contribution to the work and approved it for publication.</p>
</sec>
<sec id="s7">
<title>Funding</title>
<p>This work was funded by the Science and Technology Research Project of the Education Department of Jiangxi Province, China (No. GJJ200632).</p>
</sec>
<sec sec-type="COI-statement" id="s8">
<title>Conflict of interest</title>
<p>The authors declare that the research 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="disclaimer" id="s9">
<title>Publisher&#x2019;s note</title>
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