Molybdenum Carbide‐Oxide Heterostructures: In Situ Surface Reconfiguration toward Efficient Electrocatalytic Hydrogen Evolution

He Liuqing; Zhang Wenbiao; Mo Qijie; Huang Wenjie; Yang Lichun; Gao Qingsheng

摘要

Abstract > Heterostructured Mo <sub>2</sub> C‐MoO <sub> x </sub> on carbon cloth (Mo <sub>2</sub> C‐MoO <sub> x </sub> /CC), as a model of easily oxidized electrocatalysts under ambient conditions, is investigated to uncover surface reconfiguration during the hydrogen evolution reaction (HER). Raman spectroscopy combined with electrochemical tests demonstrates that the Mo VI oxides on the surface are in situ reduced to Mo IV , accomplishing promoted HER in acidic condition. As indicated by density functional theoretical calculations, the in situ reduced surface with terminal Mo=O moieties can effectively bring the negative Δ G <sub>H*</sub> on bare Mo <sub>2</sub> C close to a thermodynamic neutral value, addressing difficult H* desorption toward fast HER kinetics. The optimized Mo <sub>2</sub> C‐MoO <sub> x </sub> /CC only requires a low overpotential ( η <sub>10</sub> ) of 60?mV at ?10?mA?cm ?2 in 1.0? <sc>m</sc> HClO <sub>4</sub> , outperforming Mo <sub>2</sub> C/CC and most non‐precious electrocatalysts. In situ surface reconfiguration are shown on W <sub>2</sub> C‐WO <sub> x </sub> , highlighting the significance to boost various metal‐carbides and to identify active sites. </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> > 异性结构 <sub> 2 </ sub> c-moo <sub> x </ i> </ sub> 在碳布上（MO <sub> 2 </ sub> c-moo <sub> x </ i> </ sub> / CC），作为在环境条件下容易氧化电催化剂的型号，研究以在氢进化反应（她）期间露出表面重新配置。拉曼光谱与电化学测试相结合，证明了Mo vi </ sup> 表面上的氧化物原位还原为Mo iv </ sup> ，完成促进她的酸性条件。如密度官能化理论计算所示，原位减少表面与端子Mo = O部分可以有效地带来负δ g </ i> <sub> h * </ sub> 在裸露的mo. <sub> 2 </ sub> C接近热力学中性值，解决困难的H *对快速的动力学解散。优化的mo. <sub> 2 </ sub> c-moo <sub> x </ i> </ sub> / cc只需要低过势（ η</ i> <sub> 10 </ sub> ）60？mv在？10？ma？cm ？2 </ sup> 在1.0？ <sc> m </ sc> HCLO. <sub> 4 </ sub> ，优于mo. <sub> 2 </ sub> C / CC和大多数非珍贵电催化剂。原位表面重新配置显示在w上 <sub> 2 </ sub> C-WO. <sub> x </ i> </ sub> ，突出促进各种金属碳化物和识别活性位点的重要性。 </ 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9期</span><b style="margin: 0 2px;">|</b><span>共5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=He Liuqing&option=202" target="_blank" rel="nofollow">He Liuqing;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Zhang Wenbiao&option=202" target="_blank" rel="nofollow">Zhang Wenbiao;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Mo Qijie&option=202" target="_blank" rel="nofollow">Mo Qijie;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Huang Wenjie&option=202" target="_blank" rel="nofollow">Huang Wenjie;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Yang Lichun&option=202" target="_blank" rel="nofollow">Yang Lichun;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Gao Qingsheng&option=202" target="_blank" rel="nofollow">Gao Qingsheng;</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>College of Chemistry and Materials ScienceJinan UniversityGuangzhou 510632 China;</p> <p>College of Chemistry and Materials ScienceJinan UniversityGuangzhou 510632 China;</p> <p>College of Chemistry and Materials ScienceJinan UniversityGuangzhou 510632 China;</p> <p>School of Materials Science and Engineering and Guangdong Provincial Key Laboratory of Advanced Energy Storage MaterialsSouth China University of TechnologyGuangzhou 510640 China;</p> <p>School of Materials Science and Engineering and Guangdong Provincial Key Laboratory of Advanced Energy Storage MaterialsSouth China University of TechnologyGuangzhou 510640 China;</p> <p>College of Chemistry and Materials ScienceJinan UniversityGuangzhou 510632 China;</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=heterointerfaces&option=203" rel="nofollow">heterointerfaces;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=hydrogen evolution reaction&option=203" rel="nofollow">hydrogen evolution reaction;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=in situ reconfiguration&option=203" rel="nofollow">in situ reconfiguration;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=molybdenum carbides&option=203" rel="nofollow">molybdenum carbides;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=surface oxides&option=203" rel="nofollow">surface oxides;</a> </p> <div class="translation"> 机译：异丙酸蔗渣;氢气进化反应;原位重新配置;钼碳化物;表面氧化物; </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/0704028160948.html">Molybdenum Carbide‐Oxide Heterostructures: In Situ Surface Reconfiguration toward Efficient Electrocatalytic Hydrogen Evolution</a> <b>[J]</b> . <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=He Liuqing&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">He Liuqing,</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Zhang Wenbiao&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Zhang Wenbiao,</a> <a 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