Electrochemical Conversion of CO2 to Syngas with Controllable CO/H2 Ratios over Co and Ni Single‐Atom Catalysts

He Qun; Liu Daobin; Lee Ji Hoon; Liu Yumeng; Xie Zhenhua; Hwang Sooyeon; Kattel Shyam; Song Li; Chen Jingguang G.

摘要

Abstract > The electrochemical CO <sub>2</sub> reduction reaction (CO <sub>2</sub> RR) to yield synthesis gas (syngas, CO and H <sub>2</sub> ) has been considered as a promising method to realize the net reduction in CO <sub>2</sub> emission. However, it is challenging to balance the CO <sub>2</sub> RR activity and the CO/H <sub>2</sub> ratio. To address this issue, nitrogen‐doped carbon supported single‐atom catalysts are designed as electrocatalysts to produce syngas from CO <sub>2</sub> RR. While Co and Ni single‐atom catalysts are selective in producing H <sub>2</sub> and CO, respectively, electrocatalysts containing both Co and Ni show a high syngas evolution (total current 74?mA?cm ?2 ) with CO/H <sub>2</sub> ratios (0.23–2.26) that are suitable for typical downstream thermochemical reactions. Density functional theory calculations provide insights into the key intermediates on Co and Ni single‐atom configurations for the H <sub>2</sub> and CO evolution. The results present a useful case on how non‐precious transition metal species can maintain high CO <sub>2</sub> RR activity with tunable CO/H <sub>2</sub> ratios. </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> > 电化学CO. <sub> 2 </ sub> 还原反应（CO <sub> 2 </ sub> RR）产生合成气体（合成气，CO和H. <sub> 2 </ sub> ）已被认为是实现有限公司净减少的有希望的方法 <sub> 2 </ sub> 排放。但是，平衡CO的挑战 <sub> 2 </ sub> rr活动和co / h <sub> 2 </ sub> 比率。为了解决这个问题，氮掺杂的碳负载的单原子催化剂设计为电催化剂，以产生来自CO的合成气 <sub> 2 </ sub> rr。虽然CO和Ni单原子催化剂在生产H中是有选择的 <sub> 2 </ sub> 和CO，含有CO和NI的电催化剂分别显示出高合成气进化（总电流＆ 74. ma？mc ？2 </ sup> ）与CO / H <sub> 2 </ sub> 比率（0.23-2.26）适用于典型的下游热化学反应。密度泛函理论计算为H的CO和NI单原子配置的关键中间体提供见解 <sub> 2 </ sub> 和CO进化。结果为非珍贵过渡金属物种如何维持高CO的有用案例 <sub> 2 </ sub> 可调谐CO / H的RR活动 <sub> 2 </ sub> 比率。 </ 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 Qun&option=202" target="_blank" rel="nofollow">He Qun;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Liu Daobin&option=202" target="_blank" rel="nofollow">Liu Daobin;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Lee Ji Hoon&option=202" target="_blank" rel="nofollow">Lee Ji Hoon;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Liu Yumeng&option=202" target="_blank" rel="nofollow">Liu Yumeng;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Xie Zhenhua&option=202" target="_blank" rel="nofollow">Xie Zhenhua;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Hwang Sooyeon&option=202" target="_blank" rel="nofollow">Hwang Sooyeon;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Kattel Shyam&option=202" target="_blank" rel="nofollow">Kattel Shyam;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Song Li&option=202" target="_blank" rel="nofollow">Song Li;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Chen Jingguang G.&option=202" target="_blank" rel="nofollow">Chen Jingguang G.;</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>National Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei Anhui 230029 China;</p> <p>School of Materials Science and EngineeringNanyang Technological UniversitySingapore 639798 Singapore;</p> <p>Department of Chemical EngineeringColumbia UniversityNew York NY 10027 USA;</p> <p>Department of Chemical EngineeringColumbia UniversityNew York NY 10027 USA;</p> <p>Department of Chemical EngineeringColumbia UniversityNew York NY 10027 USA;</p> <p>Center for Functional NanomaterialsBrookhaven National LaboratoryUpton NY 11973 USA;</p> <p>Department of PhysicsFlorida A&</p> <p>M UniversityTallahassee FL 32307 USA;</p> <p>National Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei Anhui 230029 China;</p> <p>Department of Chemical EngineeringColumbia UniversityNew York NY 10027 USA;</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=CO2 electroreduction&option=203" rel="nofollow">CO2 electroreduction;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=density functional theory&option=203" rel="nofollow">density functional theory;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=high activity&option=203" rel="nofollow">high activity;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=selectivity control&option=203" rel="nofollow">selectivity control;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=syngas production&option=203" rel="nofollow">syngas production;</a> </p> <div class="translation"> 机译：CO2电荷;密度函数理论;高活动;选择性控制;合成气生产; </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/0704028162285.html">Inside Cover: Electrochemical Conversion of CO2 to Syngas with Controllable CO/H2 Ratios over Co and Ni 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