On the Influence of Oxygen on the Degradation of Fe‐N‐C Catalysts

Kumar Kavita; Dubau Laetitia; Mermoux Michel; Li Jingkun; Zitolo Andrea; Nelayah Jaysen; Jaouen Frédéric; Maillard Frédéric

摘要

Abstract > Fe‐N‐C catalysts containing atomic FeN <sub> x </sub> sites are promising candidates as precious‐metal‐free catalysts for oxygen reduction reaction (ORR) in proton exchange membrane fuel cells. The durability of Fe‐N‐C catalysts in fuel cells has been extensively studied using accelerated stress tests (AST). Herein we reveal stronger degradation of the Fe‐N‐C structure and four‐times higher ORR activity loss when performing load cycling AST in O <sub>2</sub> ‐ vs. Ar‐saturated pH?1 electrolyte. Raman spectroscopy results show carbon corrosion after AST in O <sub>2</sub> , even when cycling at low potentials, while no corrosion occurred after any load cycling AST in Ar. The load‐cycling AST in O <sub>2</sub> leads to loss of a significant fraction of FeN <sub> x </sub> sites, as shown by energy dispersive X‐ray spectroscopy analyses, and to the formation of Fe oxides. The results support that the unexpected carbon corrosion occurring at such low potential in the presence of O <sub>2</sub> is due to reactive oxygen species produced between H <sub>2</sub> O <sub>2</sub> and Fe sites via Fenton reactions. </abstract> </span> <span class="z_kbtn z_kbtnclass hoverxs" style="display: none;">展开▼</span> </div> <div class="translation abstracttxt"> <span class="zhankaihshouqi fivelineshidden" id="abstract"> <span>机译：</span><Abstract Type =“Main”XML：Lang =“en”> <标题类型=“main”>抽象</ title> > 含有原子扇的Fe-N-C催化剂 <sub> x </ i> </ sub> 位点是具有用于质子交换膜燃料电池的氧还原反应（ORR）的无金属催化剂的候选物。使用加速应力测试（AST）广泛地研究了燃料电池中Fe-N-C催化剂的耐久性。在此，我们揭示了Fe-N-C结构的较强降解和在o在O中进行负载循环AST时为四倍的orr活性损失 <sub> 2 </ sub> - 与Ar饱和pH？1电解质。拉曼光谱结果显示AST在o之后的碳腐蚀 <sub> 2 </ sub> ，即使在低电位下循环时，在AR中的任何负载循环后也没有发生腐蚀。 o的负载循环is <sub> 2 </ sub> 导致失去大量的芬 <sub> x </ i> </ sub> 由能量分散X射线光谱分析和Fe氧化物的形成而显示的位点。结果支持在o存在下发生这种低潜力的意外碳腐蚀 <sub> 2 </ sub> 是由于H之间产生的反应性氧物种 <sub> 2 </ sub> O. <sub> 2 </ sub> 通过芬顿反应和FE站点。 </ p> </摘要> </span> <span class="z_kbtn z_kbtnclass hoverxs" style="display: none;">展开▼</span> </div> </div> <div class="record"> <h2 class="all_title" id="enpatent33" >著录项</h2> <ul> <li> <span class="lefttit">来源</span> <div style="width: 86%;vertical-align: text-top;display: inline-block;"> <a href='/journal-foreign-19011/'>《Angewandte Chemie》</a> <b style="margin: 0 2px;">|</b><span>2020年第8期</span><b style="margin: 0 2px;">|</b><span>共9页</span> </div> </li> <li> <div class="author"> <span class="lefttit">作者</span> <p id="fAuthorthree" class="threelineshidden zhankaihshouqi"> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Kumar Kavita&option=202" target="_blank" rel="nofollow">Kumar Kavita;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Dubau Laetitia&option=202" target="_blank" rel="nofollow">Dubau Laetitia;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Mermoux Michel&option=202" target="_blank" rel="nofollow">Mermoux Michel;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Li Jingkun&option=202" target="_blank" rel="nofollow">Li Jingkun;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Zitolo Andrea&option=202" target="_blank" rel="nofollow">Zitolo Andrea;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Nelayah Jaysen&option=202" target="_blank" rel="nofollow">Nelayah Jaysen;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Jaouen Frédéric&option=202" target="_blank" rel="nofollow">Jaouen Frédéric;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Maillard Frédéric&option=202" target="_blank" rel="nofollow">Maillard Frédéric;</a> </p> <span class="z_kbtnclass z_kbtnclassall hoverxs" id="zkzz" style="display: none;">展开▼</span> </div> </li> <li> <div style="display: flex;"> <span class="lefttit">作者单位</span> <div style="position: relative;margin-left: 3px;max-width: 639px;"> <div class="threelineshidden zhankaihshouqi" id="fOrgthree"> <p>CNRSUniv. Grenoble Alpes38000 Grenoble France;</p> <p>CNRSUniv. Grenoble Alpes38000 Grenoble France;</p> <p>CNRSUniv. Grenoble Alpes38000 Grenoble France;</p> <p>CNRSUniversité de Montpellier2 Place Eugène Bataillon 34095 Montpellier France;</p> <p>Synchrotron SOLEILL'orme des Merisiers BP 48 Saint Aubin 91192 Gif-sur-Yvette France;</p> <p>Laboratoire Matériaux et Phénomènes QuantiquesUniversité de Paris75013 Paris France;</p> <p>CNRSUniversité de Montpellier2 Place Eugène Bataillon 34095 Montpellier France;</p> <p>CNRSUniv. Grenoble Alpes38000 Grenoble France;</p> </div> <span class="z_kbtnclass z_kbtnclassall hoverxs" id="zhdw" style="display: none;">展开▼</span> </div> </div> </li> <li > <span class="lefttit">收录信息</span> <span style="width: 86%;vertical-align: text-top;display: inline-block;"></span> </li> <li> <span class="lefttit">原文格式</span> <span>PDF</span> </li> <li> <span class="lefttit">正文语种</span> <span>eng</span> </li> <li> <span class="lefttit">中图分类</span> <span><a href="https://www.zhangqiaokeyan.com/clc/1188.html" title="应用化学">应用化学;</a></span> </li> <li class="antistop"> <span class="lefttit">关键词</span> <p style="width: 86%;vertical-align: text-top;"> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=carbon corrosion&option=203" rel="nofollow">carbon corrosion;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Fe-N-C Catalysts&option=203" rel="nofollow">Fe-N-C Catalysts;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=oxygen reduction reaction&option=203" rel="nofollow">oxygen reduction reaction;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=polymer electrolyte membrane fuel cells&option=203" rel="nofollow">polymer electrolyte membrane fuel cells;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=reactive oxygen species (ROS)&option=203" rel="nofollow">reactive oxygen species (ROS);</a> </p> <div class="translation"> 机译：碳腐蚀;Fe-N-C催化剂;氧还原反应;聚合物电解质膜燃料电池;活性氧（ROS）; </div> </li> </ul> </div> </div> <div class="literature cardcommon"> <div class="similarity "> <h3 class="all_title" id="enpatent66">相似文献</h3> <div class="similaritytab clearfix"> <ul> <li class="active" >外文文献</li> <li >中文文献</li> <li >专利</li> </ul> </div> <div class="similarity_details"> <ul > <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/journal-foreign-detail/0704028161880.html">On the 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L. </a> <span>1988</span> </span> </div> <p class="zwjiyix translation" style="max-width: initial;height: auto;word-break: break-all;white-space: initial;text-overflow: initial;overflow: initial;"> <span>机译：金刚烷的催化均相官能化。金属卟啉催化剂的电子和结构特征对原子转移选择性氧化与叠氮化/卤化的影响</span> </p> </li> </ul> <ul style="display: none;"> <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/academic-journal-cn_acta-physico-chimica-sinica_thesis/0201272785050.html">基于金属有机框架衍生的Fe-N-C纳米复合材料作为高效的氧还原催化剂</a> <b>[J]</b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=王倩倩&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 王倩倩</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=刘大军&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,刘大军</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=何兴权&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,何兴权</a> <span> <a href="/journal-cn-15102/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 物理化学学报 </a> </span> <span> . 2019</span><span>,第007期</span> </span> </div> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/academic-journal-cn_chinese-journal-catalysis_thesis/0201231560846.html">Fe-N-C单原子催化剂的C‒H键选择性氧化反应</a> <b>[J]</b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=李兴伟&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 李兴伟</a> <span> <a href="/journal-cn-28399/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 催化学报 </a> </span> <span> . 2018</span><span>,第001期</span> </span> </div> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/academic-journal-cn_chemical-research_thesis/0201235491594.html">球状多孔Fe-N-C复合催化剂的制备及其氧还原催化性能</a> <b>[J]</b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=李珅珅&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 李珅珅</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=苏苗军&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,苏苗军</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=刘威华&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,刘威华</a> <span> <a href="/journal-cn-12031/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 化学研究 </a> </span> <span> . 2018</span><span>,第004期</span> </span> </div> </li> <li> <div> <b>4. </b><a class="enjiyixqcontent" href="/academic-journal-cn_chinese-journal-analytical-chemistry_thesis/0201230482658.html">银耳状Fe-N-C复合催化剂的制备及催化氧还原性能研究</a> <b>[J]</b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=黄燕平&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 黄燕平</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=苑红艳&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,苑红艳</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=张健&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,张健</a> <span> <a href="/journal-cn-10804/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 分析化学 </a> </span> <span> . 2017</span><span>,第009期</span> </span> </div> </li> <li> <div> <b>5. </b><a class="enjiyixqcontent" href="/academic-journal-cn_chinese-journal-catalysis_thesis/0201231564880.html">高分散Fe-N-C氧还原反应电催化剂及其在直接甲醇燃料电池中的应用</a> <b>[J]</b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=谷领峥&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 谷领峥</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=姜鲁华&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,姜鲁华</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=李旭宁&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,李旭宁</a> <span> <a href="/journal-cn-28399/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 催化学报 </a> </span> <span> . 2016</span><span>,第004期</span> </span> </div> </li> <li> <div> <b>6. </b><a class="enjiyixqcontent" href="/academic-conference-cn_meeting-41598_thesis/020222485920.html">氮化铁在高性能Fe-N-C氧还原催化剂中的作用</a> <b>[C]</b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Min Wang&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . Min Wang</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=王敏&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,王敏</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Shichun Mu&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,Shichun Mu</a> <span> <a href="/conference-cn-41598/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 2016新能源新材料研究生论坛 </a> <span> <span> . -1</span> </span> </div> </li> <li> <div> <b>7. </b><a class="enjiyixqcontent" href="/academic-degree-domestic_mphd_thesis/020316328600.html">Fe-N-C催化剂的制备及其电催化氧还原性能的研究</a> <b>[A] </b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=杨丹琪&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 杨丹琪</a> <span> . 2021</span> </span> </div> </li> </ul> <ul style="display: none;"> <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/patent-detail/061204219207.html">铋铜硫氧和/或其复合材料及其制备方法和用途、温度影响的光催化降解甲醛的设备和方法</a> <b>[P]</b> . <span> 中国专利： CN108465473B </span> <span> . 2021.01.26</span> </div> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/patent-detail/06120110951172.html">铋铜硫氧和/或其复合材料及其制备方法和用途、温度影响的光催化降解甲醛的设备和方法</a> <b>[P]</b> . <span> 中国专利： CN108465473A </span> <span> . 2018-08-31</span> </div> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/patent-detail/06130443764447.html">Increasing the resistance to degradation of polymeric materials under the influence of atmospheric influences or improving the resistance to degradation of polymeric materials under the influence of atmospheric influences</a> <b>[P]</b> . <span> 外国专利：  RU2001132867A </span> <span> . 2003-09-20</span> </div> <p class="zwjiyix translation" style="max-width: initial;height: auto;word-break: break-all;white-space: initial;text-overflow: initial;overflow: initial;"> <span>机译：在大气影响下提高聚合材料的抗降解性，或在大气影响下提高聚合材料的抗降解性 </span> </p> </li> <li> <div> <b>4. </b><a class="enjiyixqcontent" href="/patent-detail/06130420364887.html">Extended Life Packaging comprising a material to the ingestion of a Mammal that is degraded by oxidation of Oxygen sensor comprising a sensor comprising a transition metalOxygen impermeable to Oxygen, a container, the container contains a Filter suspended which holding the material to the ingestion of a mamiefero and has an oxygen Scavenger.</a> <b>[P]</b> . <span> 外国专利：  CL2012002723A1 </span> <span> . 2013-09-06</span> </div> <p class="zwjiyix translation" style="max-width: initial;height: auto;word-break: break-all;white-space: initial;text-overflow: initial;overflow: initial;"> <span>机译：延长寿命的包装，其中包含一种可被哺乳动物吸收的材料，该材料可通过氧气的氧化而降解，包括一个包含过渡金属的传感器，该传感器包含氧气不可渗透的氧气，一个容器，该容器内装有一个悬浮的过滤器，该过滤器将材料保持在可吸收哺乳动物体内。并有氧气清除剂。 </span> </p> </li> <li> <div> <b>5. </b><a class="enjiyixqcontent" href="/patent-detail/06130441413776.html">Catalyst degradation detector for internal combustion engine of vehicle, detects degradation of catalyst when temperature of catalyst exceeds activity temperature and nitrogen oxide purification effectiveness reduces</a> <b>[P]</b> . <span> 外国专利：  DE10345405A1 </span> <span> . 2004-05-13</span> </div> <p class="zwjiyix translation" style="max-width: initial;height: auto;word-break: break-all;white-space: initial;text-overflow: initial;overflow: initial;"> <span>机译：用于车辆的内燃机的催化剂降解检测器，当催化剂的温度超过活性温度并且氮氧化物的净化效率降低时，检测催化剂的降解 </span> </p> </li> </ul> </div> </div> </div> <div class="theme cardcommon" style="overflow: auto;display:none"> <h3 class="all_title" id="enpatent55">相关主题</h3> <ul id="subject"> </ul> </div> </div> </div> </div> <div class="right rightcon"> <div class="details_img cardcommon clearfix" style="margin-bottom: 10px;display:none;" > </div> </div> </div> <div id="thesis_get_original1" class="downloadBth" style="bottom: 19px;z-index: 999;" onclick="ywcd('0704028161880','4',7,2,1,'',this,24)" class="delivery" prompt="010401" 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