Nanoporous Palladium Hydride for Electrocatalytic N2 Reduction under Ambient Conditions

Xu Wence; Fan Guilan; Chen Jialiang; Li Jinhan; Zhang Le; Zhu Shengli; Su Xuncheng; Cheng Fangyi; Chen Jun

摘要

Abstract > The electrocatalytic nitrogen reduction reaction (NRR) is an alternative eco‐friendly strategy for sustainable N <sub>2</sub> fixation with renewable energy. However, NRR suffers from sluggish kinetics owing to difficult N <sub>2</sub> adsorption and N≡N cleavage. Now, nanoporous palladium hydride is reported as electrocatalyst for electrochemical N <sub>2</sub> reduction under ambient conditions, achieving a high ammonia yield rate of 20.4?μg?h ?1 ?mg ?1 with a Faradaic efficiency of 43.6?% at low overpotential of 150?mV. Isotopic hydrogen labeling studies suggest the involvement of lattice hydrogen atoms in the hydride as active hydrogen source. In?situ Raman analysis and density functional theory (DFT) calculations further reveal the reduction of energy barrier for the rate‐limiting *N <sub>2</sub> H formation step. The unique protonation mode of palladium hydride would provide a new insight on designing efficient and robust electrocatalysts for nitrogen fixation. </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> > 电催化氮缩减反应（NRR）是可持续的替代环保策略 <sub> 2 </ sub> 固定可再生能源。然而，由于困难的n，nrr遭受了缓慢的动力学 <sub> 2 </ sub> 吸附和N≡N裂解。现在，纳米多孔钯氢化物被报告为电化学N的电催化剂 <sub> 2 </ sub> 在环境条件下降低，达到高氨屈服率为20.4ΩΩh ？1 </ sup> ？米格？1 </ sup> 在低过电位为150Ωmv的低43.6Ω％的竞争效率。同位素氢标记研究表明，晶格氢原子在氢化物中的参与作为活性氢源。在原位拉曼分析和密度泛函理论（DFT）计算进一步揭示了速率限制的能量屏障的减少 <sub> 2 </ sub> H形成步骤。纯钯的独特质子化模式将为设计用于氮固定的高效且鲁棒电催化剂提供新的洞察。 </ 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6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=Xu Wence&option=202" target="_blank" rel="nofollow">Xu Wence;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Fan Guilan&option=202" target="_blank" rel="nofollow">Fan Guilan;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Chen Jialiang&option=202" target="_blank" rel="nofollow">Chen Jialiang;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Li Jinhan&option=202" target="_blank" rel="nofollow">Li Jinhan;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Zhang Le&option=202" target="_blank" rel="nofollow">Zhang Le;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Zhu Shengli&option=202" target="_blank" rel="nofollow">Zhu Shengli;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Su Xuncheng&option=202" target="_blank" rel="nofollow">Su Xuncheng;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Cheng Fangyi&option=202" target="_blank" rel="nofollow">Cheng Fangyi;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Chen Jun&option=202" target="_blank" rel="nofollow">Chen Jun;</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>Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education)Nankai UniversityTianjin 300071 China;</p> <p>Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education)Nankai UniversityTianjin 300071 China;</p> <p>State Key Laboratory of Elemento-Organic ChemistryNankai UniversityTianjin 300071 China;</p> <p>Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education)Nankai UniversityTianjin 300071 China;</p> <p>Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education)Nankai UniversityTianjin 300071 China;</p> <p>School of Materials Science and EngineeringTianjin UniversityTianjin 300072 China;</p> <p>State Key Laboratory of Elemento-Organic ChemistryNankai UniversityTianjin 300071 China;</p> <p>Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education)Nankai UniversityTianjin 300071 China;</p> <p>Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education)Nankai UniversityTianjin 300071 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=DFT calculations&option=203" rel="nofollow">DFT calculations;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=hydrides&option=203" rel="nofollow">hydrides;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=nanoporous catalysts&option=203" rel="nofollow">nanoporous catalysts;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=nitrogen reduction reaction&option=203" rel="nofollow">nitrogen reduction reaction;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=palladium&option=203" rel="nofollow">palladium;</a> </p> <div class="translation"> 机译：DFT计算;氢化物;纳米多孔催化剂;氮还原反应;钯; </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="/academic-journal-cn_transactions-nonferrous-metals-society-china_thesis/0201270899735.html">快淬Al70Pd17Fe13准晶脱合金化制备纳米多孔钯及其电催化活性</a> <b>[J]</b> . <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=刘歆翌&option=202" target="_blank" rel="nofollow" class="tuijian_auth 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