分级孔结构的Fe-N-C催化剂用于高效电催化氧还原

doi:10.19894/j.issn.1000-0518.230067

摘要/Abstract

摘要：

氧还原反应（ORR）是金属空气电池以及质子交换膜燃料电池（PEMFCs）系统重要的阴极反应，研究具有高活性与高稳定性的非贵金属催化剂具有重要意义。本研究使用了一种具有分级孔结构的MIL-101-（Al-Fe）作为金属前驱体模板，成功制备出具有分级多孔结构的Fe-N-C催化剂。电化学测试结果表明，在0.1 mol/L KOH电解液中，Fe-N-C-MIL-900催化剂表现出最优的氧还原性能（半波电位0.905 V以及5000圈CV测试后半波电位仅下降5 mV），远高于纯碳基N-C-MIL-900催化剂（0.845 V）。通过旋转环盘电极测试发现，Fe-N-C-MIL-900催化剂ORR电子转移数为3.98，H₂O₂产率低于3%，表现出明显的4电子ORR路径。这一工作为制备具有高ORR活性的Fe-N-C催化剂提供了一种新的途径。

关键词: 氧还原, 分级孔结构, 铁基催化剂, 4电子路径

Abstract: <graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="1000-0518-2023-40-8-1187/6205B116-E601-4f2f-8CF2-C14036AD8C64-F501.jpg"/><p>The as-prepared Fe-N-C-MIL-900 catalyst exhibits higher ORR activity （half-wave potential of 0.905 V） than the pure N-C-MIL-900 sample in 0.1 mol/L KOH conditions.</p></sec></p> <p><strong>Key words: </strong> <a href="#" onClick="searchEnKeyword('http://yyhx.ciac.jl.cn','1','Oxygen reduction reaction')">Oxygen reduction reaction, </a> <a href="#" onClick="searchEnKeyword('http://yyhx.ciac.jl.cn','1','Hierarchically porous structure')">Hierarchically porous structure, </a> <a href="#" onClick="searchEnKeyword('http://yyhx.ciac.jl.cn','1','Fe-based catalysts')">Fe-based catalysts, </a> <a href="#" onClick="searchEnKeyword('http://yyhx.ciac.jl.cn','1','4-Electron pathway')">4-Electron pathway</a> </p> </form>  <form name="subjectSchemeForm" action="" method=post target=_blank> <input type="hidden" name="searchSQL" /> <input type="hidden" name="language" /> </form>  <p> <strong> 中图分类号: </strong> </p> <ul class="list-unstyled pacs"> <li> <p> <a href="#" onclick="subjectScheme('http://yyhx.ciac.jl.cn','O646','1');return false;" target="_blank"> O646 </a> </p> </li> </ul>  <div class="row hidden-xs hidden-sm"> <div class="col-xs-12 col-sm-2 col-md-2 col-lg-2 margin-bottom-10 text-center"> <div class="text-primary btn-menu"> <h4>引用本文</h4> </div> </div> <div class="col-xs-12 col-sm-10 col-md-10 col-lg-10 margin-bottom-10"> <div class="primary-border"> <p>郑锐雪, 孟庆磊, 张丽, 刘长鹏, 邢巍, 肖梅玲. 分级孔结构的Fe-N-C催化剂用于高效电催化氧还原[J]. 应用化学, 2023, 40(8): 1187-1194. </p> <p>Rui-Xue ZHENG, Qing-Lei MENG, Li ZHANG, Chang-Peng LIU, Wei XING, Mei-Ling XIAO. Hierarchically Porous Fe<strong>-</strong>N<strong>-</strong>C Catalysts for Efficient Electrocatalytic Oxygen Reduction Reaction[J]. Chinese Journal of Applied Chemistry, 2023, 40(8): 1187-1194.</p> </div> </div> </div> <div class="row hidden-xs hidden-sm"> <div class="col-xs-12 col-sm-2 col-md-2 col-lg-2 margin-bottom-10 text-center"> <div class="btn-menu bs-callout-warning"> <h4>使用本文</h4> </div> </div> <div class="col-xs-12 col-sm-10 col-md-10 col-lg-10 margin-bottom-10"> <div class="primary-border"> <p> <b> <form name=mail action="http://yyhx.ciac.jl.cn/CN/article/sendMail.jsp" method=post target=_blank> <div class="bshare-custom pull-left"> <div class="bsPromo bsPromo2"></div> <a title="分享到微信" class="bshare-weixin" href="javascript:void(0);"></a> <a title="分享到Facebook" class="bshare-facebook"></a> <a title="分享到Twitter" class="bshare-twitter"></a> <span class="BSHARE_COUNT bshare-share-count" style="float: none;">0</span> </div> <script type="text/javascript" charset="utf-8" src="https://static.bshare.cn/b/buttonLite.js#style=-1&uuid=&pophcol=2&lang=zh"></script><script type="text/javascript" charset="utf-8" src="https://static.bshare.cn/b/bshareC0.js"></script> / <a href="#" id="collectArticle" class="shouc"></a> <span id="collectCount"></span> / <a onclick="mail.submit()" href="javascript:void(null)" class="tuij">推荐</a> <input type="hidden" name="articleId" value='18179'> <form> </b> </p> <p><b>导出引用管理器</b> <span class="daochu"><a href="http://yyhx.ciac.jl.cn/CN/article/getTxtFile.do?fileType=EndNote&id=18179" id="ris_export">EndNote</a>|<a href="http://yyhx.ciac.jl.cn/CN/article/getTxtFile.do?fileType=Ris&id=18179">Ris</a>|<a id="bibtex_export" href="http://yyhx.ciac.jl.cn/CN/article/getTxtFile.do?fileType=BibTeX&id=18179">BibTeX</a></span> </p> <p><strong>链接本文:</strong> <a href="http://yyhx.ciac.jl.cn/CN/10.19894/j.issn.1000-0518.230067" class="txt_zhaiyao1">http://yyhx.ciac.jl.cn/CN/10.19894/j.issn.1000-0518.230067</a> </p> <p> <strong> </strong> <a href="http://yyhx.ciac.jl.cn/CN/Y2023/V40/I8/1187" class="txt_zhaiyao1"> http://yyhx.ciac.jl.cn/CN/Y2023/V40/I8/1187</a> </p> </div> </div> </div> </div> </div> </div> <div class="panel panel-default" > <div class="panel-heading" role="tab" id="tubiao" onClick="xianshi(this)"> <h4 class="panel-title"> <a id="figure" class="collapsed" href="javascript:;"> 图/表 <span class="badge badge-info">4</span> </a> </h4> </div> <div id="collapseTwo" class="panel-collapse collapse" role="tabpanel" aria-labelledby="headingTwo" style="display: none;"> <div class="panel-body">  <div class="row figureCon"> <div class="col-lg-3 col-md-4 col-sm-6" style ="width:100%;"> <div class="thumbnail" style="background:#f8f8f8; border: 1px #eee solid; margin-top:20px;border-radius:15px; padding: 10px;"> <div class="img_div"> <a class="figureClass" href="#figureClass3464" data-toggle="tooltip" data-placement="bottom" data-original-title="图1 Fe-N-C-MIL-900的SEM图片（A、B）；　Fe-N-C-MIL-900的TEM图片（C、D、E）； HRTEM图片（F）以及元素分布图片（G-J）"> <img src="http://yyhx.ciac.jl.cn/fileup/1000-0518/FIGURE/2023-40-8/Images/1000-0518-2023-40-8-1187/6205B116-E601-4f2f-8CF2-C14036AD8C64-F001.jpg" style="height:auto;max-width:90%;margin:15px auto;" class="zhaiyao_img"> </a> </div> <div style="color:#666;font-size: 14px;padding: 0px;text-align: center;"> <b>图1</b> Fe-N-C-MIL-900的SEM图片（A、B）；　Fe-N-C-MIL-900的TEM图片（C、D、E）； HRTEM图片（F）以及元素分布图片（G-J） </div> <div style="color:#666;font-size: 14px;padding: 0px;text-align: center;margin-bottom:15px;"> <b>Fig.1</b> SEM images of Fe-N-C-MIL-900 （A，B）； TEM images of Fe-N-C-MIL-900 （C，D，E）； HRTEM image of Fe-N-C-MIL-900 （F） and the corresponding energy dispersive spectroscopy （EDS） elemental maps （G-J） </div> <div style='display:none'> <div id='figureClass3464' style='padding:10px; background:#fff;text-align:center;' class="img_div"> <img src="http://yyhx.ciac.jl.cn/fileup/1000-0518/FIGURE/2023-40-8/Images/1000-0518-2023-40-8-1187/6205B116-E601-4f2f-8CF2-C14036AD8C64-F001.jpg" style="height:auto;max-width:90%;margin:15px auto;" class="zhaiyao_img"/> <p style="color:#666;font-size: 14px;padding: 0px;text-align: center;"><b>图1</b> Fe-N-C-MIL-900的SEM图片（A、B）；　Fe-N-C-MIL-900的TEM图片（C、D、E）； HRTEM图片（F）以及元素分布图片（G-J）</p> <p style="color:#666;font-size: 14px;padding: 0px;text-align: center;margin-bottom:15px;"><b>Fig.1</b> SEM images of Fe-N-C-MIL-900 （A，B）； TEM images of Fe-N-C-MIL-900 （C，D，E）； HRTEM image of Fe-N-C-MIL-900 （F） and the corresponding energy dispersive spectroscopy （EDS） elemental maps （G-J）</p> </div> </div> </div> </div> <div class="col-lg-3 col-md-4 col-sm-6" style ="width:100%;"> <div class="thumbnail" style="background:#f8f8f8; border: 1px #eee solid; margin-top:20px;border-radius:15px; padding: 10px;"> <div class="img_div"> <a class="figureClass" href="#figureClass3465" data-toggle="tooltip" data-placement="bottom" data-original-title="图2 Fe-N-C-MIL-900与N-C-MIL-900的氮气吸脱附等温线图（A）、XRD谱图（B）以及拉曼图（C）； Fe-N-C-MIL-900的XPS总谱图（D）、N1s（E）和C1s（F）的高分辨XPS谱图"> <img src="http://yyhx.ciac.jl.cn/fileup/1000-0518/FIGURE/2023-40-8/Images/1000-0518-2023-40-8-1187/6205B116-E601-4f2f-8CF2-C14036AD8C64-F002.jpg" style="height:auto;max-width:90%;margin:15px auto;" class="zhaiyao_img"> </a> </div> <div style="color:#666;font-size: 14px;padding: 0px;text-align: center;"> <b>图2</b> Fe-N-C-MIL-900与N-C-MIL-900的氮气吸脱附等温线图（A）、XRD谱图（B）以及拉曼图（C）； Fe-N-C-MIL-900的XPS总谱图（D）、N1s（E）和C1s（F）的高分辨XPS谱图 </div> <div style="color:#666;font-size: 14px;padding: 0px;text-align: center;margin-bottom:15px;"> <b>Fig.2</b> N2 absorption/desorption isotherms （A）， XRD patterns （B） and Raman spectra （C） of Fe-N-C-MIL-900 and N-C-MIL-900； XPS survey spectra （D）， high-resolution N1s XPS spectrum （E） and high-resolution C1s XPS spectra （F） for Fe-N-C-MIL-900 </div> <div style='display:none'> <div id='figureClass3465' style='padding:10px; background:#fff;text-align:center;' class="img_div"> <img src="http://yyhx.ciac.jl.cn/fileup/1000-0518/FIGURE/2023-40-8/Images/1000-0518-2023-40-8-1187/6205B116-E601-4f2f-8CF2-C14036AD8C64-F002.jpg" style="height:auto;max-width:90%;margin:15px auto;" class="zhaiyao_img"/> <p style="color:#666;font-size: 14px;padding: 0px;text-align: center;"><b>图2</b> Fe-N-C-MIL-900与N-C-MIL-900的氮气吸脱附等温线图（A）、XRD谱图（B）以及拉曼图（C）； Fe-N-C-MIL-900的XPS总谱图（D）、N1s（E）和C1s（F）的高分辨XPS谱图</p> <p style="color:#666;font-size: 14px;padding: 0px;text-align: center;margin-bottom:15px;"><b>Fig.2</b> N2 absorption/desorption isotherms （A）， XRD patterns （B） and Raman spectra （C） of Fe-N-C-MIL-900 and N-C-MIL-900； XPS survey spectra （D）， high-resolution N1s XPS spectrum （E） and high-resolution C1s XPS spectra （F） for Fe-N-C-MIL-900</p> </div> </div> </div> </div> <div class="col-lg-3 col-md-4 col-sm-6" style ="width:100%;"> <div class="thumbnail" style="background:#f8f8f8; border: 1px #eee solid; margin-top:20px;border-radius:15px; padding: 10px;"> <div class="img_div"> <a class="figureClass" href="#figureClass3466" data-toggle="tooltip" data-placement="bottom" data-original-title="图3 Fe-N-C-MIL-700、Fe-N-C-MIL-800、Fe-N-C-MIL-900和N-C-MIL-900在0.1 mol/L KOH溶液中的LSV曲线（A）； Fe-N-C-MIL-900和N-C-MIL-900在O2中的CV曲线（B）；半波电位（E1/2）和0.9 V处的动电流密度（jk）的比较（C）； Fe-N-C-MIL-900和N-C-MIL-900的Tafel图（D）"> <img src="http://yyhx.ciac.jl.cn/fileup/1000-0518/FIGURE/2023-40-8/Images/1000-0518-2023-40-8-1187/6205B116-E601-4f2f-8CF2-C14036AD8C64-F004.jpg" style="height:auto;max-width:90%;margin:15px auto;" class="zhaiyao_img"> </a> </div> <div style="color:#666;font-size: 14px;padding: 0px;text-align: center;"> <b>图3</b> Fe-N-C-MIL-700、Fe-N-C-MIL-800、Fe-N-C-MIL-900和N-C-MIL-900在0.1 mol/L KOH溶液中的LSV曲线（A）； Fe-N-C-MIL-900和N-C-MIL-900在O2中的CV曲线（B）；半波电位（E1/2）和0.9 V处的动电流密度（jk）的比较（C）； Fe-N-C-MIL-900和N-C-MIL-900的Tafel图（D） </div> <div style="color:#666;font-size: 14px;padding: 0px;text-align: center;margin-bottom:15px;"> <b>Fig.3</b> LSV curves of Fe-N-C-MIL-700， Fe-N-C-MIL-800， Fe-N-C-MIL-900 and N-C-MIL-900 （A）； CV curves of Fe-N-C-MIL-900 and N-C-MIL-900 （B）； Comparisons of half wave potential （E1/2） and kinetic current density （jk） at 0.9 V （C）； Tafel plots for Fe-N-C-MIL-900 and N-C-MIL-900 （D） </div> <div style='display:none'> <div id='figureClass3466' style='padding:10px; background:#fff;text-align:center;' class="img_div"> <img src="http://yyhx.ciac.jl.cn/fileup/1000-0518/FIGURE/2023-40-8/Images/1000-0518-2023-40-8-1187/6205B116-E601-4f2f-8CF2-C14036AD8C64-F004.jpg" style="height:auto;max-width:90%;margin:15px auto;" class="zhaiyao_img"/> <p style="color:#666;font-size: 14px;padding: 0px;text-align: center;"><b>图3</b> Fe-N-C-MIL-700、Fe-N-C-MIL-800、Fe-N-C-MIL-900和N-C-MIL-900在0.1 mol/L KOH溶液中的LSV曲线（A）； Fe-N-C-MIL-900和N-C-MIL-900在O2中的CV曲线（B）；半波电位（E1/2）和0.9 V处的动电流密度（jk）的比较（C）； Fe-N-C-MIL-900和N-C-MIL-900的Tafel图（D）</p> <p style="color:#666;font-size: 14px;padding: 0px;text-align: center;margin-bottom:15px;"><b>Fig.3</b> LSV curves of Fe-N-C-MIL-700， Fe-N-C-MIL-800， Fe-N-C-MIL-900 and N-C-MIL-900 （A）； CV curves of Fe-N-C-MIL-900 and N-C-MIL-900 （B）； Comparisons of half wave potential （E1/2） and kinetic current density （jk） at 0.9 V （C）； Tafel plots for Fe-N-C-MIL-900 and N-C-MIL-900 （D）</p> </div> </div> </div> </div> <div class="col-lg-3 col-md-4 col-sm-6" style ="width:100%;"> <div class="thumbnail" style="background:#f8f8f8; border: 1px #eee solid; margin-top:20px;border-radius:15px; padding: 10px;"> <div class="img_div"> <a class="figureClass" href="#figureClass3467" data-toggle="tooltip" data-placement="bottom" data-original-title="图4 Fe-N-C-MIL-900在不同转速下的LSV曲线（A）； Fe-N-C-MIL-900的K-L曲线（B）； Fe-N-C-MIL-900的H2O2产率以及ORR电子转移数（C）； Fe-N-C-MIL-900在不同扫速下的CV曲线（D）； 1.12 V电位下的电流密度与扫速的线性关系（E）； Fe-N-C-MIL-900在5000圈CV前后的LSV曲线（F）"> <img src="http://yyhx.ciac.jl.cn/fileup/1000-0518/FIGURE/2023-40-8/Images/1000-0518-2023-40-8-1187/6205B116-E601-4f2f-8CF2-C14036AD8C64-F003.jpg" style="height:auto;max-width:90%;margin:15px auto;" class="zhaiyao_img"> </a> </div> <div style="color:#666;font-size: 14px;padding: 0px;text-align: center;"> <b>图4</b> Fe-N-C-MIL-900在不同转速下的LSV曲线（A）； Fe-N-C-MIL-900的K-L曲线（B）； Fe-N-C-MIL-900的H2O2产率以及ORR电子转移数（C）； Fe-N-C-MIL-900在不同扫速下的CV曲线（D）； 1.12 V电位下的电流密度与扫速的线性关系（E）； Fe-N-C-MIL-900在5000圈CV前后的LSV曲线（F） </div> <div style="color:#666;font-size: 14px;padding: 0px;text-align: center;margin-bottom:15px;"> <b>Fig.4</b> LSV curves of Fe-N-C-MIL-900 at different rotating rates （A）； K-L plots for Fe-N-C-MIL-900 （B）； H2O2 yield and electron transfer number （n） of Fe-N-C-MIL-900 （C）； CV curves of Fe-N-C-MIL-900 at various scan rates （D）； Current density at 1.12 V against scan rate of for Fe-N-C-MIL-900 （E）； LSV curves of Fe-N-C-MIL-900 before and after 5000 cycles （F） </div> <div style='display:none'> <div id='figureClass3467' style='padding:10px; background:#fff;text-align:center;' class="img_div"> <img src="http://yyhx.ciac.jl.cn/fileup/1000-0518/FIGURE/2023-40-8/Images/1000-0518-2023-40-8-1187/6205B116-E601-4f2f-8CF2-C14036AD8C64-F003.jpg" style="height:auto;max-width:90%;margin:15px auto;" class="zhaiyao_img"/> <p style="color:#666;font-size: 14px;padding: 0px;text-align: center;"><b>图4</b> Fe-N-C-MIL-900在不同转速下的LSV曲线（A）； Fe-N-C-MIL-900的K-L曲线（B）； Fe-N-C-MIL-900的H2O2产率以及ORR电子转移数（C）； Fe-N-C-MIL-900在不同扫速下的CV曲线（D）； 1.12 V电位下的电流密度与扫速的线性关系（E）； Fe-N-C-MIL-900在5000圈CV前后的LSV曲线（F）</p> <p style="color:#666;font-size: 14px;padding: 0px;text-align: center;margin-bottom:15px;"><b>Fig.4</b> LSV curves of Fe-N-C-MIL-900 at different rotating rates （A）； K-L plots for Fe-N-C-MIL-900 （B）； H2O2 yield and electron transfer number （n） of Fe-N-C-MIL-900 （C）； CV curves of Fe-N-C-MIL-900 at various scan rates （D）； Current density at 1.12 V against scan rate of for Fe-N-C-MIL-900 （E）； LSV curves of Fe-N-C-MIL-900 before and after 5000 cycles （F）</p> </div> </div> </div> </div> </div>  </div> </div> </div> <div class="panel panel-default" > <div class="panel-heading" role="tab" id="cankaowenxian" onClick="xianshi(this)"> <a name="reference"></a> <h4 class="panel-title"> <a id="reference" class="collapsed" href="javascript:;"> 参考文献 <span class="badge badge-info">30</span> </a> </h4> </div> <div id="collapseThree" class="panel-collapse collapse" role="tabpanel" aria-labelledby="headingThree" style="display: none;"> <div class="panel-body">  <table width="98%" border="0" align="center" cellpadding="0" cellspacing="8"> <tr> <td valign='top' align='right' style="padding-right:13px;">1</td> <td style="padding-bottom: 13px;"> <span class='magtech_ref_source'>SHAN J Q， YE C， CHEN S M， et al. 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分级孔结构的Fe-N-C催化剂用于高效电催化氧还原

Hierarchically Porous Fe-N-C Catalysts for Efficient Electrocatalytic Oxygen Reduction Reaction

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