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<front>
<journal-meta>
<journal-id journal-id-type="publisher-id">Front. Therm. Eng.</journal-id>
<journal-title>Frontiers in Thermal Engineering</journal-title>
<abbrev-journal-title abbrev-type="pubmed">Front. Therm. Eng.</abbrev-journal-title>
<issn pub-type="epub">2813-0456</issn>
<publisher>
<publisher-name>Frontiers Media S.A.</publisher-name>
</publisher>
</journal-meta>
<article-meta>
<article-id pub-id-type="publisher-id">1079789</article-id>
<article-id pub-id-type="doi">10.3389/fther.2022.1079789</article-id>
<article-categories>
<subj-group subj-group-type="heading">
<subject>Thermal Engineering</subject>
<subj-group>
<subject>Original Research</subject>
</subj-group>
</subj-group>
</article-categories>
<title-group>
<article-title>Electric field assisted reduction of NO<sub>x</sub> emission: A numerical study</article-title>
<alt-title alt-title-type="left-running-head">Ahmed 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/fther.2022.1079789">10.3389/fther.2022.1079789</ext-link>
</alt-title>
</title-group>
<contrib-group>
<contrib contrib-type="author">
<name>
<surname>Ahmed</surname>
<given-names>Sheikh F.</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
<uri xlink:href="https://loop.frontiersin.org/people/1263262/overview"/>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Aghdam</surname>
<given-names>Ali Charchi</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
<uri xlink:href="https://loop.frontiersin.org/people/2122516/overview"/>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Pleis</surname>
<given-names>Jackson</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Geiger</surname>
<given-names>Robert</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
</contrib>
<contrib contrib-type="author" corresp="yes">
<name>
<surname>Farouk</surname>
<given-names>Tanvir I.</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/296631/overview"/>
</contrib>
</contrib-group>
<aff id="aff1">
<sup>1</sup>
<institution>Department of Mechanical Engineering</institution>, <institution>University of South Carolina</institution>, <addr-line>Columbia</addr-line>, <addr-line>SC</addr-line>, <country>United States</country>
</aff>
<aff id="aff2">
<sup>2</sup>
<institution>ClearSign Combustion Corporation</institution>, <addr-line>Seattle</addr-line>, <addr-line>WA</addr-line>, <country>United States</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/1394622/overview">Boxiang Wang</ext-link>, Shanghai Jiao Tong 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/1448061/overview">Fan Zhang</ext-link>, Tianjin University, China</p>
<p>
<ext-link ext-link-type="uri" xlink:href="https://loop.frontiersin.org/people/224170/overview">Milan S. Dimitrijevic</ext-link>, Astronomical Observatory, Serbia</p>
</fn>
<corresp id="c001">&#x2a;Correspondence: Tanvir I. Farouk, <email>tfarouk@sc.edu</email>
</corresp>
<fn fn-type="other">
<p>This article was submitted to Heat Transfer Mechanisms and Applications, a section of the journal Frontiers in Thermal Engineering</p>
</fn>
</author-notes>
<pub-date pub-type="epub">
<day>16</day>
<month>01</month>
<year>2023</year>
</pub-date>
<pub-date pub-type="collection">
<year>2022</year>
</pub-date>
<volume>2</volume>
<elocation-id>1079789</elocation-id>
<history>
<date date-type="received">
<day>25</day>
<month>10</month>
<year>2022</year>
</date>
<date date-type="accepted">
<day>06</day>
<month>12</month>
<year>2022</year>
</date>
</history>
<permissions>
<copyright-statement>Copyright &#xa9; 2023 Ahmed, Aghdam, Pleis, Geiger and Farouk.</copyright-statement>
<copyright-year>2023</copyright-year>
<copyright-holder>Ahmed, Aghdam, Pleis, Geiger and Farouk</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 paper reports simulation results on the influence of a direct-current driven radial electric field on the emission characteristics; especially NO<sub>x</sub> and CO of a premixed methane/air laminar jet flame. A multi-physics computational model is developed in the OpenFOAM framework to simulate electric-field-coupled premixed combustion process. The computational framework consists of coupled species, momentum and energy conservation together with a Poisson&#x2019;s equation solver to resolve the electric field distribution. Electron and ion conservation equations are resolved to consider the ionic wind body force in the momentum conservation equation and the associated possible electric field distortion due to the space charge distribution. The simulations are conducted for a stochiometric and fuel rich condition and over a range of jet flow rates for a configuration representative of a test-scale experimental setup. The model predictions show that for an applied voltage of 50&#xa0;kV, the flame structure changes significantly for both the stoichiometric and fuel rich conditions. The flame is stretched significantly by the electric field due to ionic wind. For the fuel rich condition, the ionic wind allows additional mixing of the fuel rich stream with the surrounding air and drastically altering the flame structure. The electric field was found to reduce the NO<sub>x</sub> emission significantly for both stoichiometric and rich conditions. Over the entire range of flowrate conditions, the stochiometric fuel-oxidizer mixture showed a decrease in maximum NO<sub>x</sub> by a factor of 1.6 in presence of electric field. For the fuel rich case, however as the flow rate is increased, the NO<sub>x</sub> reduction factor decreased from 12.0 to 1.6. For CO emissions, the presence of electric field reduces the concentration under fuel rich conditions and <italic>vice versa</italic> for the stoichiometric flame. The role of kinetics is analyzed and discussed.</p>
</abstract>
<kwd-group>
<kwd>chemi-ionization</kwd>
<kwd>electric field</kwd>
<kwd>ionic wind</kwd>
<kwd>NO<sub>x</sub> kinetics</kwd>
<kwd>OpenFOAM</kwd>
</kwd-group>
</article-meta>
</front>
<body>
<sec id="s1">
<title>1 Introduction</title>
<p>For several decades, researchers have been interested in the electrical properties of flames and how they can be controlled by the application of electric fields. It has been shown that electric fields affect flames and combustion processes in three distinctive, and major ways&#x2013;thermal effect (<xref ref-type="bibr" rid="B15">Uddi et al., 2009</xref>), ionic wind effect (<xref ref-type="bibr" rid="B9">Marcum and Ganguly, 2005</xref>), and electro-chemical effect (<xref ref-type="bibr" rid="B10">Ombrello et al., 2010a</xref>,<xref ref-type="bibr" rid="B11">b</xref>). The thermal effect contributes to the neutral gas heating through Joule heating when there is large current across the electric field. The ionic wind effect causes fluid dynamic changes in the flow field via electrical body force resulting from space charge and electric field. The electro-chemical effect produces energetic electrons, ions, radicals and excited molecules in the gas stream which directly contributes to the reaction kinetics.</p>
<p>Studies involving experimental and modeling approaches have been conducted, in an effort to elucidate the influence of both direct-current (DC) and alternating-current (AC) electric fields on the combustion characteristics. Experimental studies have demonstrated that DC electric fields have a strong influence on the flame shape (<xref ref-type="bibr" rid="B17">Vega et al., 2007</xref>), flame propagation speed (<xref ref-type="bibr" rid="B9">Marcum and Ganguly, 2005</xref>), and emission and soot characteristics (<xref ref-type="bibr" rid="B12">Saito et al., 1999</xref>; <xref ref-type="bibr" rid="B13">Sakhrieh et al., 2005</xref>). Simulations employing multi-physics models have shown the role of ionic wind under DC external fields (<xref ref-type="bibr" rid="B18">Yamashita et al., 2009</xref>; <xref ref-type="bibr" rid="B5">Belhi et al., 2010</xref>; <xref ref-type="bibr" rid="B6">Belhi et al., 2019</xref>). In recent years, there has been growing interest in utilizing AC electric field to modify the combustion characteristics of flames (<xref ref-type="bibr" rid="B20">Zhang et al., 2013</xref>; <xref ref-type="bibr" rid="B8">Kim et al., 2017</xref>). Despite the large volume of work on electric field&#x2013;flame interactions, studies related to the impact of electric field on NO<sub>x</sub> emission is limited. <xref ref-type="bibr" rid="B16">Vatazhin et al. (1995)</xref> in their laminar propane diffusion flame experiments observed up to 30% reduction in NO<sub>x</sub> emission with respect to the emission index with the implementation of electric field on a negatively polarized burner. <xref ref-type="bibr" rid="B19">Zake et al. (2000)</xref> applied a DC electric field in a flame channel flow and observed a reduction in the NO<sub>x</sub> emission by &#x223c; 80%. The decrease in the emission characteristics was attributed to the reduction in the flame temperature in presence of the electric field. <xref ref-type="bibr" rid="B13">Sakhrieh et al. (2005)</xref> experimentally investigated the influence of electric field on premixed methane/air flames at elevated pressures. They observed as much as 95% reduction of CO emission, accompanied by 25% increase of NO<sub>x</sub> irrespective of pressure. They attributed the decrease in CO to ionic winds that changed the flame geometry and reduced the amount of incompletely burned fuel. However, explanation related to the increase in NO<sub>x</sub> was not provided. In their experimental work, <xref ref-type="bibr" rid="B17">Vega et al. (2007)</xref> showed that for a premixed CH<sub>4</sub>/O<sub>2</sub>/N<sub>2</sub> flame, the NO<sub>x</sub> emission is unaffected under applied electric field conditions for which the flame remains undeformed. In a recent paper, <xref ref-type="bibr" rid="B20">Zhang et al. (2013)</xref> examined the behavior of NO emission of laminar non-premixed CH<sub>4</sub>/air flame when subjected to high frequency (10&#xa0;kHz) AC electric fields. For a voltage range of 0&#x2013;4.0 kV, a non-linear response of NO emission was observed. In between 0&#x2013;1&#xa0;kV peak voltage, the NO in flue gas showed a sharp decrease which then steadily increased to high values for 1.0&#x2013;3.0 kV, followed by a steady decrease by further increase of the applied peak potential to 4&#xa0;kV.</p>
<p>In this paper, we numerically investigate the effects of an externally driven radial DC electric field on the flame and combustion characteristics, more specifically on the NO<sub>x</sub> and CO emission in a laminar premixed CH<sub>4</sub>/air jet flame under atmospheric condition. The simulation was conducted for a multi-dimensional configuration representative of a laboratory scale mockup of an industrial system at ClearSign Combustion Corporation. A stochiometric and fuel-rich condition is investigated. The flame structure is analyzed, and the role of underlying thermo-kinetic/transport properties on emission characteristics is elucidated. The kinetic analysis shows that the NO<sub>x</sub> recycling pathways undergo distinct changes in presence of the external fields.</p>
</sec>
<sec sec-type="methods" id="s2">
<title>2 Methods</title>
<p>A custom test furnace was designed and built to study the effects of electric fields on the combustion process. The furnace was designed to operate up to 5.86&#xa0;kW at temperatures up to 1366&#xa0;K. As shown in <xref ref-type="fig" rid="F1">Figure 1</xref>, the furnace consists of a main vessel, a transition, a stack, and a burner assembly (not shown in figure). The main vessel is 1.37&#xa0;m tall and has an outer diameter of 0.61&#xa0;m. It contains a 0.152&#xa0;m thick refractory resulting in an inner opening diameter of 0.3048&#xa0;m. The transition piece is 0.360&#xa0;m tall and takes the 0.61&#xa0;m outer diameter of the main vessel down to a 0.305&#xa0;m to match the outer diameter of the stack. The main vessel sits on four standoff electrical insulators capable of withstanding up to 50&#xa0;kV. The support stand is kept at ground potential, while the rest of the vessel is electrically floating. To monitor the floating voltage of the cooling jackets and the main vessel, and to protect from large over voltages, the voltage of each is monitored through a voltage divider circuit connected to a spark gap. The spark gap can be adjusted to the desired allowable maximum voltage. The output of the voltage divider is monitored through the data acquisition system. The main vessel has two gated 0.15&#xa0;m quartz windows and four 0.051&#xa0;m viewing ports all on the same plane. There is a total of 26&#xa0;K-type thermocouples located throughout the furnace to measure the temperatures of vessel wall and axis, cooling jackets and the top and bottom of the stack. Fuel and air are monitored using FMA 2300 series omega mass flow meters. NO<sub>x</sub>, CO and CO<sub>2</sub> emission analyzers allow assessment of emission in the stacks.</p>
<fig id="F1" position="float">
<label>FIGURE 1</label>
<caption>
<p>Customized test furnace for testing electric field effects on combustion process (burner assembly not shown).</p>
</caption>
<graphic xlink:href="fther-02-1079789-g001.tif"/>
</fig>
<sec id="s2-1">
<title>2.1 Computational domain and boundary conditions</title>
<p>A schematic of the experimental test scale setup at ClearSign Combustion Corporation is presented in <xref ref-type="fig" rid="F2">Figure 2A</xref>. The computational domain illustrated in <xref ref-type="fig" rid="F2">Figure 2B</xref> takes into account only the burner and part of the post-combustion zone of the experimental setup. The domain contains part of the burner height (i.e., 0.15&#xa0;m) and covers a 1.0&#xa0;m long post-combustion zone having a constant diameter of 0.6&#xa0;m. To reduce computational overhead, the simulations are performed on a 2-D axisymmeteric configuration with structured non-uniform mesh. The mesh was finer near the central region (i.e., jet location) as well as near the wall boundaries. All the simulations reported here are for a domain composed of 10,850 mesh elements for which grid independent results were confirmed.</p>
<fig id="F2" position="float">
<label>FIGURE 2</label>
<caption>
<p>Schematic illustrations of <bold>(A)</bold> the experimental setup and, <bold>(B)</bold> the computational domain denoting the different boundaries.</p>
</caption>
<graphic xlink:href="fther-02-1079789-g002.tif"/>
</fig>
<p>The burner acts as the powered electrode (50&#xa0;kV for base case simulations) with the side walls grounded (0&#xa0;kV). Both are prescribed with an isothermal (i.e., 300&#xa0;K) boundary conditions. The side walls and the burner surfaces are considered to be reactively non-participating for the neutral species, but the ionic species reaching the surfaces are prescribed to undergo quenching/neutralization reactions (<xref ref-type="bibr" rid="B7">Farouk et al., 2006</xref>). A Dirichlet boundary condition for velocity is employed at the inlet, representing the different flow rate conditions considered. Outflow boundary conditions are provided at the outlet of the tubular section. Premixed methane/air mixtures at equivalence ratios <italic>&#x3d5;</italic> &#x3d; 1.0 and 3.0, and flowrates &#x223c; 6.70 and 9.93 slpm, respectively are simulated. An initial high temperature region of 2100&#xa0;K is prescribed to ensure ignition of the fuel/air mixture. All simulations are conducted for an operating pressure of 1&#xa0;atm.</p>
</sec>
<sec id="s2-2">
<title>2.2 Mathematical model</title>
<p>The numerical study is performed using a multi-dimensional, reacting flow computational code that has been developed in the OpenFOAM framework, the details of which (both the physics and the numerical schemes) have been thoroughly presented in <xref ref-type="bibr" rid="B4">Asgari et al., 2017</xref> and <xref ref-type="bibr" rid="B1">Ahmed et al., 2021</xref>. As a new implementation, the CVODE solver from SUNDIAL is employed to solve the reaction terms. In brief, the mathematical model comprises of time dependent conservation equations of total mass, species mass fraction, mixture momentum, and mixture energy, together with a Poisson&#x2019;s equation to resolve the electric field distribution, reported respectively in the following:<disp-formula id="e1">
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<mml:mo>&#x2202;</mml:mo>
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<mml:mo>&#x3d;</mml:mo>
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<mml:mrow>
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<mml:msub>
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</mml:mrow>
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<mml:mstyle displaystyle="true">
<mml:munderover>
<mml:mo>&#x2211;</mml:mo>
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<mml:mi mathvariant="bold-italic">k</mml:mi>
<mml:mo>&#x3d;</mml:mo>
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</mml:mrow>
<mml:mi mathvariant="bold-italic">N</mml:mi>
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</mml:mrow>
<mml:mi mathvariant="bold-italic">k</mml:mi>
</mml:msub>
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</mml:mrow>
<mml:mn>0</mml:mn>
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</mml:mrow>
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<mml:mo>,</mml:mo>
</mml:mtd>
</mml:mtr>
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<label>(4)</label>
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<disp-formula id="e5">
<mml:math id="m5">
<mml:mtable columnalign="left">
<mml:mtr>
<mml:mtd>
<mml:mo>&#x2207;</mml:mo>
<mml:mo>.</mml:mo>
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<mml:mo>&#x2207;</mml:mo>
<mml:mi mathvariant="bold-italic">&#x3a6;</mml:mi>
</mml:mrow>
<mml:mo>)</mml:mo>
</mml:mrow>
<mml:mo>&#x3d;</mml:mo>
<mml:msub>
<mml:mi mathvariant="bold-italic">q</mml:mi>
<mml:mn>0</mml:mn>
</mml:msub>
<mml:mstyle displaystyle="true">
<mml:mo>&#x2211;</mml:mo>
<mml:mrow>
<mml:msub>
<mml:mi mathvariant="bold-italic">Z</mml:mi>
<mml:mi mathvariant="bold-italic">k</mml:mi>
</mml:msub>
<mml:msub>
<mml:mi mathvariant="bold-italic">N</mml:mi>
<mml:mi mathvariant="bold-italic">k</mml:mi>
</mml:msub>
</mml:mrow>
</mml:mstyle>
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</mml:mtd>
</mml:mtr>
<mml:mtr>
<mml:mtd>
<mml:mi mathvariant="bold-italic">E</mml:mi>
<mml:mo>&#x3d;</mml:mo>
<mml:mo>&#x2212;</mml:mo>
<mml:mo>&#x2207;</mml:mo>
<mml:mi mathvariant="bold-italic">&#x3a6;</mml:mi>
<mml:mo>,</mml:mo>
</mml:mtd>
</mml:mtr>
</mml:mtable>
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<label>(5)</label>
</disp-formula>where, <inline-formula id="inf1">
<mml:math id="m6">
<mml:mi>&#x3c1;</mml:mi>
</mml:math>
</inline-formula> is the mixture density of gas phase, <inline-formula id="inf2">
<mml:math id="m7">
<mml:mi>u</mml:mi>
</mml:math>
</inline-formula> is the velocity, <inline-formula id="inf3">
<mml:math id="m8">
<mml:mrow>
<mml:msub>
<mml:mrow>
<mml:mover accent="true">
<mml:mi>&#x3c9;</mml:mi>
<mml:mo>&#x2d9;</mml:mo>
</mml:mover>
</mml:mrow>
<mml:mi>k</mml:mi>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula> is the rate of productions (ROP) of species <italic>k</italic> by chemical reaction, <inline-formula id="inf4">
<mml:math id="m9">
<mml:mrow>
<mml:msub>
<mml:mi>W</mml:mi>
<mml:mrow>
<mml:mi>k</mml:mi>
<mml:mo>,</mml:mo>
<mml:mi>i</mml:mi>
</mml:mrow>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula> is the thermophoretic diffusion velocity which is neglected in the present investigation, <inline-formula id="inf5">
<mml:math id="m10">
<mml:mrow>
<mml:msubsup>
<mml:mi>V</mml:mi>
<mml:mi>i</mml:mi>
<mml:mi>C</mml:mi>
</mml:msubsup>
</mml:mrow>
</mml:math>
</inline-formula> is the correction velocity to ensure that the diffusion velocities of all the species add up to zero, <inline-formula id="inf6">
<mml:math id="m11">
<mml:mrow>
<mml:msub>
<mml:mi>D</mml:mi>
<mml:mrow>
<mml:mi>k</mml:mi>
<mml:mi>m</mml:mi>
</mml:mrow>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula> is the mass diffusion coefficient of species <inline-formula id="inf7">
<mml:math id="m12">
<mml:mi>k</mml:mi>
</mml:math>
</inline-formula> into the rest of the mixture, <italic>P</italic> is the pressure, <inline-formula id="inf8">
<mml:math id="m13">
<mml:mrow>
<mml:msub>
<mml:mi>h</mml:mi>
<mml:mi>s</mml:mi>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula> is the specific enthalpy of species <italic>k</italic>, <inline-formula id="inf9">
<mml:math id="m14">
<mml:mi>&#x3b1;</mml:mi>
</mml:math>
</inline-formula> is the mixture thermal diffusivity, <inline-formula id="inf10">
<mml:math id="m15">
<mml:mrow>
<mml:mi mathvariant="normal">&#x394;</mml:mi>
<mml:msubsup>
<mml:mi>h</mml:mi>
<mml:mrow>
<mml:mi>f</mml:mi>
<mml:mo>,</mml:mo>
<mml:mi>k</mml:mi>
</mml:mrow>
<mml:mi>o</mml:mi>
</mml:msubsup>
</mml:mrow>
</mml:math>
</inline-formula> is the formation enthalpy for species <italic>k</italic>, <inline-formula id="inf11">
<mml:math id="m16">
<mml:mrow>
<mml:mover accent="true">
<mml:mi>Q</mml:mi>
<mml:mo>&#x2d9;</mml:mo>
</mml:mover>
</mml:mrow>
</mml:math>
</inline-formula> is the energy source term due to radiation, <inline-formula id="inf12">
<mml:math id="m17">
<mml:mi>&#x3a6;</mml:mi>
</mml:math>
</inline-formula> is the electric potential, <inline-formula id="inf13">
<mml:math id="m18">
<mml:mi>&#x3b5;</mml:mi>
</mml:math>
</inline-formula> is the electric permittivity, <inline-formula id="inf14">
<mml:math id="m19">
<mml:mrow>
<mml:msub>
<mml:mi>q</mml:mi>
<mml:mn>0</mml:mn>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula> is the elementary charge, <inline-formula id="inf15">
<mml:math id="m20">
<mml:mrow>
<mml:msub>
<mml:mi>Z</mml:mi>
<mml:mi>k</mml:mi>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula> is the electric charge of species <inline-formula id="inf16">
<mml:math id="m21">
<mml:mi>k</mml:mi>
</mml:math>
</inline-formula>, and <inline-formula id="inf17">
<mml:math id="m22">
<mml:mrow>
<mml:msub>
<mml:mi>N</mml:mi>
<mml:mi>k</mml:mi>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula> is the number density of species <inline-formula id="inf18">
<mml:math id="m23">
<mml:mi>k</mml:mi>
</mml:math>
</inline-formula>. The momentum conservation includes the effect of electrical body force i.e., <inline-formula id="inf19">
<mml:math id="m24">
<mml:mrow>
<mml:mi>q</mml:mi>
<mml:mo>.</mml:mo>
<mml:mrow>
<mml:mover accent="true">
<mml:mi>E</mml:mi>
<mml:mo>&#x2192;</mml:mo>
</mml:mover>
</mml:mrow>
</mml:mrow>
</mml:math>
</inline-formula>. Conservation equation for both electrons and ions are solved including the effect of drift velocity (<inline-formula id="inf20">
<mml:math id="m25">
<mml:mrow>
<mml:msub>
<mml:mi>v</mml:mi>
<mml:mrow>
<mml:mtext>drift</mml:mtext>
</mml:mrow>
</mml:msub>
<mml:mo>&#x3d;</mml:mo>
<mml:msub>
<mml:mi>&#x3bc;</mml:mi>
<mml:mrow>
<mml:mtext>mobility</mml:mtext>
</mml:mrow>
</mml:msub>
<mml:mrow>
<mml:mover accent="true">
<mml:mi>E</mml:mi>
<mml:mo>&#x2192;</mml:mo>
</mml:mover>
</mml:mrow>
</mml:mrow>
</mml:math>
</inline-formula> ) of the ionic species. Even though electrons are included in the computation, their effect on the system is not significant due to their very low number density and extremely high mobility.</p>
</sec>
<sec id="s2-3">
<title>2.3 Chemical kinetics</title>
<p>The hydrocarbon/NO<sub>x</sub> model of <xref ref-type="bibr" rid="B2">Ahmed et al. (2016)</xref> consisting of 301 species and 1945 reactions is used as the chemical kinetic model for neutral species, culminated from the previous works of the authors (<xref ref-type="bibr" rid="B14">Santner et al., 2016</xref>). An eleven-step ionic reaction mechanism (<xref ref-type="table" rid="T1">Table 1</xref>) and associated thermodynamics and transport property from <xref ref-type="bibr" rid="B18">Yamashita et al. (2009)</xref> and <xref ref-type="bibr" rid="B3">Alquaity et al. (2017)</xref> is appended to the hydrocarbon/NO<sub>x</sub> model. The ionic mechanism consists of six species (electrons, HCO<sup>&#x2b;</sup>, H<sub>3</sub>O<sup>&#x2b;</sup>, C<sub>2</sub>H<sub>3</sub>O<sup>&#x2b;</sup>, CH<sub>3</sub>
<sup>&#x2b;</sup> and C<sub>3</sub>H<sub>3</sub>
<sup>&#x2b;</sup>). C<sub>3</sub>H<sub>3</sub>
<sup>&#x2b;</sup> ions are specifically considered to simulate the fuel rich flames. It should be noted that the ionic reactions are associated with chemi-ionization process and do not represent plasma breakdown by any means. The ionic mechanism has been validated by <xref ref-type="bibr" rid="B18">Yamashita et al. (2009)</xref> independently for a canonical configuration. The electron mobility values are obtained from <xref ref-type="bibr" rid="B13">Sakhrieh et al. (2005)</xref> and the Einstein relationship (<inline-formula id="inf21">
<mml:math id="m26">
<mml:mrow>
<mml:msub>
<mml:mi>D</mml:mi>
<mml:mi>e</mml:mi>
</mml:msub>
<mml:mo>&#x3d;</mml:mo>
<mml:mrow>
<mml:mrow>
<mml:msub>
<mml:mi>&#x3bc;</mml:mi>
<mml:mi>e</mml:mi>
</mml:msub>
<mml:msub>
<mml:mi>k</mml:mi>
<mml:mi>B</mml:mi>
</mml:msub>
<mml:mi>T</mml:mi>
</mml:mrow>
<mml:mo>/</mml:mo>
<mml:mrow>
<mml:msub>
<mml:mi>q</mml:mi>
<mml:mi>e</mml:mi>
</mml:msub>
</mml:mrow>
</mml:mrow>
</mml:mrow>
</mml:math>
</inline-formula>) is used to determine the diffusivity from the mobility values.</p>
<table-wrap id="T1" position="float">
<label>TABLE 1</label>
<caption>
<p>Adopted ionic reactions from <xref ref-type="bibr" rid="B18">Yamashita et al. (2009)</xref>.</p>
</caption>
<table>
<thead valign="top">
<tr>
<th align="center">Index</th>
<th align="center">Reactions</th>
</tr>
</thead>
<tbody valign="top">
<tr>
<td align="center">1</td>
<td align="center">CH &#x2b; O &#x2192; HCO<sup>&#x2b;</sup> &#x2b; e</td>
</tr>
<tr>
<td align="center">2</td>
<td align="center">HCO<sup>&#x2b;</sup> &#x2b; H<sub>2</sub>O &#x2192; CO &#x2b; H<sub>3</sub>O<sup>&#x2b;</sup>
</td>
</tr>
<tr>
<td align="center">3</td>
<td align="center">H<sub>3</sub>O<sup>&#x2b;</sup> &#x2b; e &#x2192; H<sub>2</sub>O &#x2b; H</td>
</tr>
<tr>
<td align="center">4</td>
<td align="center">CH&#x2a; &#x2b; O &#x2192; HCO<sup>&#x2b;</sup> &#x2b; e</td>
</tr>
<tr>
<td align="center">5</td>
<td align="center">H<sub>3</sub>O<sup>&#x2b;</sup> &#x2b; C<sub>2</sub>H<sub>2</sub> &#x2192; C<sub>2</sub>H<sub>3</sub>O<sup>&#x2b;</sup> &#x2b; H<sub>2</sub>
</td>
</tr>
<tr>
<td align="center">6</td>
<td align="center">HCO<sup>&#x2b;</sup> &#x2b; CH<sub>2</sub> &#x2192; CH<sub>3</sub>
<sup>&#x2b;</sup> &#x2b; CO</td>
</tr>
<tr>
<td align="center">7</td>
<td align="center">H<sub>3</sub>O<sup>&#x2b;</sup> &#x2b; CH<sub>2</sub> &#x2192; CH<sub>3</sub>
<sup>&#x2b;</sup>&#x2b; H<sub>2</sub>O</td>
</tr>
<tr>
<td align="center">8</td>
<td align="center">CH<sub>3</sub>
<sup>&#x2b;</sup> &#x2b; C<sub>2</sub>H<sub>2</sub> &#x2192; C<sub>3</sub>H<sub>3</sub>
<sup>&#x2b;</sup> &#x2b; H<sub>2</sub>
</td>
</tr>
<tr>
<td align="center">9</td>
<td align="center">C<sub>3</sub>H<sub>3</sub>
<sup>&#x2b;</sup> &#x2b; H<sub>2</sub>O &#x2192; C<sub>2</sub>H<sub>3</sub>O<sup>&#x2b;</sup> &#x2b; CH<sub>2</sub>
</td>
</tr>
<tr>
<td align="center">10</td>
<td align="center">CH<sub>3</sub>
<sup>&#x2b;</sup> &#x2b; CO<sub>2</sub> &#x2192; C<sub>2</sub>H<sub>3</sub>O<sup>&#x2b;</sup> &#x2b; O</td>
</tr>
<tr>
<td align="center">11</td>
<td align="center">CH<sub>3</sub>
<sup>&#x2b;</sup> &#x2b; e &#x2192; CH<sub>2</sub> &#x2b; H</td>
</tr>
</tbody>
</table>
</table-wrap>
</sec>
</sec>
<sec sec-type="results|discussion" id="s3">
<title>3 Results and discussions</title>
<p>
<xref ref-type="fig" rid="F3">Figure 3</xref> presents the center line axial velocity, temperature and NO distribution for a flow rate condition of &#x223c; 3.45 slpm (Re &#x3d; 376) for the two different equivalence ratios of &#x3d5; &#x3d; 1.0 and 3.0. These two cases are referred to as the two base case conditions. The variations due to the presence of electric field is also summarized. The presence of electric field and ionic species increases the jet velocity significantly. For &#x3d5; &#x3d; 1.0 and 3.0, the peak axial velocity is increased by a factor of &#x223c; 6 and 17 respectively. The increase in the velocity results in stretching of the flame at &#x3d5; &#x3d; 1.0 and a complete change of the flame structure at &#x3d5; &#x3d; 3.0 (<xref ref-type="fig" rid="F4">Figure 4</xref>). Among the different ions, H<sub>3</sub>O<sup>&#x2b;</sup> is predicted to have the maximum density, followed by HCO<sup>&#x2b;</sup> for both cases. The predicted maximum number density of H<sub>3</sub>O<sub>max</sub>
<sup>&#x2b;</sup> is 8.0 &#xd7; 10<sup>15</sup>&#xa0;m<sup>&#x2212;3</sup> and 2.8 &#xd7; 10<sup>15</sup> m<sup>&#x2212;3</sup> and for HCO<sub>max</sub>
<sup>&#x2b;</sup> it is 3.2 &#xd7; 10<sup>13</sup>&#xa0;m<sup>&#x2212;3</sup> and 3.0 &#xd7; 10<sup>12</sup>&#xa0;m<sup>&#x2212;3</sup> for &#x3d5; &#x3d; 1.0 and 3.0 respectively. The resulting peak electrical body force is found to be 3875&#xa0;N/m<sup>3</sup> and 1055&#xa0;N/m<sup>3</sup> respectively. It is interesting to note that even though C<sub>3</sub>H<sub>3</sub>
<sup>&#x2b;</sup> ions are considered, under the very rich conditions studied, H<sub>3</sub>O<sup>&#x2b;</sup> are predicted to be the predominant ions. This is due to the fact that at fuel rich condition, the ionic wind promotes additional mixing of the fuel jet with the surrounding air through entrainment. The mixing allows reduction in the equivalence ratio contributing to a distinctive change in the flame structure (<xref ref-type="fig" rid="F4">Figure 4B</xref>).</p>
<fig id="F3" position="float">
<label>FIGURE 3</label>
<caption>
<p>Centerline distribution of <bold>(A)</bold> axial velocity, <bold>(B)</bold> temperature, and <bold>(C)</bold> NO concentration with and without electric field for a premixed CH<sub>4</sub>/air mixture with a flow rate of 3.45 slpm, 50&#xa0;kV applied voltage.</p>
</caption>
<graphic xlink:href="fther-02-1079789-g003.tif"/>
</fig>
<fig id="F4" position="float">
<label>FIGURE 4</label>
<caption>
<p>Spatial distribution of OH contours with and without electric field for <bold>(A)</bold> &#x3d5; &#x3d; 1.0, and <bold>(B)</bold> &#x3d5; &#x3d; 3.0 premixed CH<sub>4</sub>/air with a flow rate of 3.45 slpm and applied voltage of 50&#xa0;kV.</p>
</caption>
<graphic xlink:href="fther-02-1079789-g004.tif"/>
</fig>
<p>The temperature distribution at the centerline (<xref ref-type="fig" rid="F3">Figure 3B</xref>) clearly shows a decrease in the temperature due to the ionic wind effect. The decrease in the peak temperature for &#x3d5; &#x3d; 1.0 is minimal, &#x223c; 40&#xa0;K. For the fuel rich condition, the peak temperature is lowered by &#x223c; 230&#xa0;K. Additionally, in presence of the electric field, the peak temperature shifts closer to the burner inlet with a sharper gradient downstream. The centerline NO evolution resembles the temperature distribution. The electric field is found to significantly decrease the peak NO concentration, specially under fuel rich condition.</p>
<p>The spatial distribution of the OH concentration contours are compared to assess the change in the flame structure due to the electric field and the associated ionic wind effect. For both fuel loading, the flame structure is radially constricted. An axial stretching is only observed for the stoichiometric fuel loading. The OH distribution under fuel rich conditions in absence of electric field show a distinctive flame structure. Even though premixed CH<sub>4</sub>/air are injected, the extremely rich fuel loading results in a partially premixed fuel-oxidizer flame dynamics. Due to the entrainment of the chamber air to the fuel stream, the fuel-oxidizer diffuses and mixes in radial direction and establishes a flame in the periphery. The core remains fuel rich until sufficient oxidizer reaches the core region. Downstream of the burner inlet as fuel is depleted along the periphery, additional air from the surrounding gets transported into the core thereby extending the reaction zone into the core of the jet. A second peripheral reaction zone is established, as seen in the OH profile which is strictly dictated by the amount of unburnt fuel available in the jet stream. The double peak in the temperature (<xref ref-type="fig" rid="F3">Figure 3B</xref>) coincides with the OH peaks in the center line. High concentration of CO overlaps with the regions of low OH in the jet core. The distribution of CH<sub>4</sub> concentration confirms that fuel in the jet stream is either partially oxidized to CO or completely oxidized to CO<sub>2</sub>. In presence of electric field, the OH distribution for &#x3d5; &#x3d; 3.0 confirms that a flame structure/reaction zone close to the burner inlet is established. In addition, the OH profile looks similar to the stoichiometric fuel loading but has a smaller axial extent.</p>
<p>
<xref ref-type="fig" rid="F5">Figure 5</xref> compares the impact of electric field on the NO<sub>2</sub> distribution for the base cases. Under stoichiometric fuel loading and low flow rate, electric field has minimal effect on the NO<sub>2</sub> emission characteristics. The spatial distribution remains fairly unaltered with a slight increase in the maximum value; less than 4&#xa0;ppm. A stark contrast is observed for the fuel rich condition both in spatial distribution and peak value of NO<sub>2</sub>. In absence of the electric field, the NO<sub>2</sub> is formed in the outer periphery of the flame due to radial gradient in the temperature and through NO-NO<sub>2</sub> recycling reactions. The peak NO<sub>2</sub> is decreased by a factor &#x223c; 20 by the electric field. At the same time, the NO<sub>2</sub> are formed in the post combustion region downstream of the flame location.</p>
<fig id="F5" position="float">
<label>FIGURE 5</label>
<caption>
<p>Spatial distribution of NO<sub>2</sub> concentration contours with and without electric field for <bold>(A)</bold> &#x3d5; &#x3d; 1.0, and <bold>(B)</bold> &#x3d5; &#x3d; 3.0 premixed CH<sub>4</sub>/air with a flow rate of 3.45 slpm and applied voltage of 50&#xa0;kV.</p>
</caption>
<graphic xlink:href="fther-02-1079789-g005.tif"/>
</fig>
<p>The impact of flow rate on the NO emission for the two different fuel loadings is summarized in <xref ref-type="fig" rid="F6">Figure 6</xref>. With an increase in the flow rate under stoichiometric fuel loading, the flame temperature decreases from 2,256&#x2013;2,200&#xa0;K under applied electric field conditions. In comparison, the ionic wind decreases the flame temperature by 40&#x2013;100&#xa0;K in the range of flow rate studied. For &#x3d5; &#x3d; 1.0, a change in the flow rate between 3.45&#x2013;6.69 slpm minimal variations are observed. The peak NO decreases by &#x223c; 60&#xa0;ppm maintaining an almost identical spatial distribution. As the flow rate is increased to &#x223c; 10 slpm (<xref ref-type="fig" rid="F6">Figure 6A</xref>), the NO distribution is radially constricted to a very narrow central region and the peak NO is reduced by a factor of &#x223c; 1.8. At the highest flow rate condition, a lifted flame is established and maintained which is also observable in the NO contours. At higher fuel loading, the electric field allows significant decrease in the flame temperature. Over the range of flow rate simulated, the &#x394;T varied by &#x223c; 160&#xa0;K and 225&#xa0;K for the highest and lowest flow rate respectively. Consequentially, the peak NO was found to decrease by a factor of &#x223c; 1.8 in between 6.85 and 10.28 slpm and by &#x223c; 12.0&#xa0;at 3.43 slpm. As the electric field changes the flame structure drastically under fuel rich conditions (<xref ref-type="fig" rid="F4">Figure 4B</xref>), the NO is formed in the reaction zone established very close to the burner inlet. Unlike the stochiometric condition, the NO distribution under higher fuel loading undergoes both radial and axial constriction over the entire flow rate range.</p>
<fig id="F6" position="float">
<label>FIGURE 6</label>
<caption>
<p>Comparisons of the NO distribution in the domain with and without electric field for premixed CH<sub>4</sub>/air mixture under different flow rate conditions and <bold>(A)</bold> &#x3d5; &#x3d; 1.0, and <bold>(B)</bold> &#x3d5; &#x3d; 3.0.</p>
</caption>
<graphic xlink:href="fther-02-1079789-g006.tif"/>
</fig>
<p>The impact of electric field on the overall emission characteristics was assessed by comparing the peak CO and total NO<sub>x</sub> (NO&#x2b;NO<sub>2</sub>) prediction for the different flow rate fuel loading conditions (<xref ref-type="fig" rid="F7">Figure 7</xref>). As shown in <xref ref-type="fig" rid="F7">Figure 7A</xref> the peak CO concentration for &#x3d5; &#x3d; 1.0 increases by &#x223c; 50&#xa0;ppm as the flow rate is increased. However, in presence of electric field, a non-linear trend is apparent. The sharp transition in the maximum CO concentration occurs at the highest flow rate where a lifted flame is established. The lifted flame structure increases the region of incomplete combustion and results in the increase in CO formation in the domain. In the lower flow rate range, the CO concentration increases slightly due to the fact that the radial constriction of the flame increases the gap between the burner rim (i.e., nozzle diameter) allowing some of the fuel-air mixture to bypass the reaction zone in the core. A similar behavior was reported in <xref ref-type="bibr" rid="B13">Sakhrieh et al. (2005)</xref>. In contrast, the rich case shows an opposite trend where CO is reduced the maximum at the lowest flow rate. However, over the entire flow rate range, the electric field is found to be effective in reducing the CO emission; allowing complete combustion to occur by mixing of the fuel rich jet stream with ambient air. The total NO<sub>x</sub> under stoichiometric fuel loading decreases in a linear fashion and the electric field consistently decreases the maximum total NO<sub>x</sub> by a factor of &#x223c; 1.6 (<xref ref-type="fig" rid="F7">Figure 7B</xref>). For higher fuel loading, the total NO<sub>x</sub> is reduced by the electric field, but the emission increases with flow rate. At &#x3d5; &#x3d; 3.0, an increase in the flow rate results in a higher flame temperature, contributing to increase NO<sub>x</sub> production.</p>
<fig id="F7" position="float">
<label>FIGURE 7</label>
<caption>
<p>Comparisons of maximum <bold>(A)</bold> CO and <bold>(B)</bold> NO<sub>x</sub> in the domain for different flow rate condition with and without electric field for a premixed CH<sub>4</sub>/air mixture for two different equivalence ratio. Applied voltage 50&#xa0;kV.</p>
</caption>
<graphic xlink:href="fther-02-1079789-g007.tif"/>
</fig>
<p>The influence of applied electric on the kinetics involved in NO<sub>x</sub> formation, and NO-NO<sub>2</sub> interconversion was assessed by comparing the variation in the rate of formation of NO and NO<sub>2</sub> through the different reactions. For this purpose, two different regions in the computational domain (Zone 1: 0.17&#x2013;0.27&#xa0;m and Zone 2: 0.55&#x2013;0.65&#xa0;m above the burner surface), are selected, which represents the location of highest temperature gradients. The rates of production of NO and NO<sub>2</sub> by the individual reactions are volume integrated in these regions and normalized against the case without the electric field.</p>
<p>The comparisons for stoichiometric condition are shown in <xref ref-type="fig" rid="F8">Figure 8</xref>. The decrease in flame temperature due to the application of electric field in zone 1 makes the extended Zeldovich channel (N<sub>2</sub> &#x2b; O &#x3d; NO &#x2b; N, N &#x2b; O<sub>2</sub> &#x3d; NO &#x2b; O, N &#x2b; OH &#x3d; NO &#x2b; H) insignificant in that region. Instead, the direct NO formation channel from the recycling reaction NO<sub>2</sub> &#x2b; H &#x3d; NO &#x2b; OH becomes important. Besides, most of the NO in this low temperature condition in presence of electric field reacts with fuel fragments to form stable intermediates HCN and HCO. However, with the absence of electric field, most of the NO participates in direct NO-NO<sub>2</sub> or NO-HNO interconversion reactions.</p>
<fig id="F8" position="float">
<label>FIGURE 8</label>
<caption>
<p>The significant NO<sub>x</sub> formation and recycling reactions with and without the application of electric field at zone 1 (2&#xa0;cm above the burner) and zone 2 (40&#xa0;cm above the burner) for stoichiometric (&#x3a6; &#x3d; 1.0) case at a flow rate of 3.45 slpm.</p>
</caption>
<graphic xlink:href="fther-02-1079789-g008.tif"/>
</fig>
<p>For zone 2 downstream of the domain, where the temperature gradients are different from those at zone 1, a significantly different set of NO<sub>x</sub> formation and recycling reactions are observed. The applied electric field changes the major NO formation path from direct oxidation (NO<sub>2</sub> &#x2b; OH &#x3d; NO &#x2b; HO<sub>2</sub>) to reactions with atomic hydrogen (NO<sub>2</sub> &#x2b; H &#x3d; NO &#x2b; OH). Besides, it prompts the N<sub>2</sub>O formation channel that is absent without ion kinetics.</p>
</sec>
<sec sec-type="conclusion" id="s4">
<title>4 Conclusion</title>
<p>A multi-dimensional multiphysics model has been developed to simulate electric-field assisted combustion process in a self-consistent fashion. The model was employed to simulate a test scale burner setup having premixed CH<sub>4</sub>/air mixture with detailed fuel-NO<sub>x</sub> kinetics with an ionic reaction scheme appended to it. Simulations were conducted over a range of flow rate and fuel loading condition with an applied electric potential of 50&#xa0;kV to generate radial electric-fields. The emission characteristics of two major pollutant classes&#x2013;CO and NO<sub>x</sub> are investigated. The predictions show that ionic wind effects resulting from the electric field significantly increases the jet velocity and constricts the flame/reaction region both in the radial and axial direction. Lifted flames are also observed at limited cases. The flame constriction has a strong dependence on the fuel loading and flow rate conditions. Under fuel rich condition, the electric field drastically changes the flame structure by allowing mixing of the fuel stream with the surrounding oxidizing environment. A significant decrease in total NO<sub>x</sub> is found to occur over the parametric space considered; attributed to a decrease in the flame temperature. Under fuel rich condition, the electric field is found to decrease the CO emission but <italic>vice versa</italic> for stoichiometric condition. The radial constriction of the flame under stochiometric fuel loading allows unburnt fuel to bypass the core reaction regime. Kinetic analysis indicates that in presence of electric field, the NO formation route shifts from Zeldovich to direct NO formation through NO<sub>x</sub> recycling reaction and forms stable intermediates.</p>
</sec>
</body>
<back>
<sec sec-type="data-availability" id="s5">
<title>Data availability statement</title>
<p>The raw data supporting the conclusions of this article will be made available by the authors, without undue reservation.</p>
</sec>
<sec sec-type="author-contributions" id="s6">
<title>Author contributions</title>
<p>JP and RG designed and built the custom test furnace. The numerical model was developed, and the simulations were run by SA, AA and TF. All the authors participated in discussing the results in the final manuscript.</p>
</sec>
<sec sec-type="COI-statement" id="s7">
<title>Conflict of interest</title>
<p>JP, RG, were employed by ClearSign Combustion Corporation.</p>
<p>The remaining 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="s8">
<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>
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