Proton‐Reduction Reaction Catalyzed by Homoleptic Nickel–bis‐1,2‐dithiolate Complexes: Experimental and Theoretical Mechanistic Investigations

摘要

Abstract > A series of homoleptic monoanionic nickel dithiolene complexes [Ni(bdt) <sub>2</sub> ](NBu <sub>4</sub> ), [Ni(tdt) <sub>2</sub> ](NBu <sub>4</sub> ), and [Ni(mnt) <sub>2</sub> ](NBu <sub>4</sub> ) containing the ligands benzene‐1,2‐dithiolate (bdt 2? ), toluene‐3,4‐dithiolate (tdt 2? ), and maleonitriledithiolate (mnt 2? ), respectively, were employed as electrocatalysts in the hydrogen‐evolution reaction with trifluoroacetic acid as the proton source in acetonitrile. All complexes are active catalysts with TONs reaching 113, 158, and 6 for [Ni(bdt) <sub>2</sub> ](NBu <sub>4</sub> ), [Ni(tdt) <sub>2</sub> ](NBu <sub>4</sub> ), and [Ni(mnt) <sub>2</sub> ](NBu <sub>4</sub> ), respectively. The Faradaic yield for the hydrogen evolution reaction reaches 88?% for 2 ? , which also displays the minimal overpotential requirement value (467?mV) within the series. Two pathways for H <sub>2</sub> evolution can be hypothesized that differ in the sequence of protonation and reduction steps. DFT calculations are in agreement with experimental data and indicate that protonation at sulfur follows the reduction to the dianion. Hydrogen evolves from the direduced–diprotonated form via a highly distorted nickel hydride intermediate. The effects of acid strength and concentration in the hydrogen‐evolving mechanism are also discussed. </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> > 一系列经络单壬二镍二硫胺配合物[Ni（BDT） <sub> 2 </ sub> ]（NBU. <sub> 4 </ sub> ），[ni（tdt） <sub> 2 </ sub> ]（NBU. <sub> 4 </ sub> ），[ni（mnt） <sub> 2 </ sub> ]（NBU. <sub> 4 </ sub> ）含有配体苯-1,2-二硫酸盐（BDT 2？</ sup> ），甲苯-3,4-二酸盐（TDT 2？</ sup> ）和马来腈酸（MnT） 2？</ sup> ）分别用作与三氟乙酸作为乙腈中的质子源的氢进化反应中的电催化剂。所有复合物都是活性催化剂，吨为113,158和6，用于[Ni（BDT） <sub> 2 </ sub> ]（NBU. <sub> 4 </ sub> ），[ni（tdt） <sub> 2 </ sub> ]（NBU. <sub> 4 </ sub> ），[ni（mnt） <sub> 2 </ sub> ]（NBU. <sub> 4 </ sub> ），分别。氢进化反应的游览产量达到88？％ 2 ？</ sup> </ b> ，这也显示了该系列内最小的过电需求值（467？MV）。 h的两个途径 <sub> 2 </ sub> 进化可以假设质子化和减少步骤的序列不同。 DFT计算与实验数据一致，并表明硫磺的质子遵循对Dianion的减少。氢通过高度扭曲的氢化镍中间体从DiRoud诱导的掺量形式中发育。还讨论了酸强度和浓度在氢不变机理中的影响。 </ 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-16041/'>《ChemCatChem 》</a> <b style="margin: 0 2px;">|</b><span>2017年第12期</span><b style="margin: 0 2px;">|</b> <span>共10页</span> </div> </li> <li> <div class="author"> <span class="lefttit">作者</span> <p id="fAuthorthree" class="threelineshidden zhankaihshouqi"> </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"> </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/1186.html" title="物理化学（理论化学）、化学物理学">物理化学（理论化学）、化学物理学 ;</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=density functional calculations&option=203" rel="nofollow">density functional calculations;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=electrochemistry&option=203" rel="nofollow">electrochemistry;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=hydrogen&option=203" rel="nofollow">hydrogen;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=ligand effects&option=203" rel="nofollow">ligand effects;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=nickel&option=203" rel="nofollow">nickel;</a> </p> <div class="translation"> 机译：密度函数计算;电化学;氢;配体效果;镍; </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/0704022057364.html">Proton‐Reduction Reaction Catalyzed by Homoleptic Nickel–bis‐1,2‐dithiolate Complexes: Experimental and Theoretical Mechanistic Investigations</a> <b>[J]</b> . <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> </a> <a href="/journal-foreign-16041/" target="_blank" rel="nofollow" class="tuijian_authcolor">ChemCatChem .</a> <span>2017</span> <span>,第12期</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：经络镍 - 双1,2-二硫酸盐复合物催化的质子还原反应：实验和理论机制研究</span> </p> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/journal-foreign-detail/070408724730.html">Binuclear iron(I), ruthenium(I), and osmium(I) hexacarbonyl complexes containing a bridging benzene-1,2-dithiolate ligand. 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href="/patent-detail/06120103431322.html">一种氧化镍-钴酸镍-黑二氧化钛复合物光催化还原处理含六价铬废水的方法</a> <b>[P]</b> . <span> 中国专利： CN110918099A </span> <span> . 2020-03-27</span> </div> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/patent-detail/061204188861.html">一种光氧化还原/铁(II)催化体系下烯烃类化合物分子间1,2-二烷基化反应方法</a> <b>[P]</b> . <span> 中国专利： CN108640839B </span> <span> . 2021.01.05</span> </div> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/patent-detail/06130453305512.html">Ferrocene bis(phosphonite) ligands and complexes for transition- metal- catalyzed reactions</a> <b>[P]</b> . <span> 外国专利：  US5817850A </span> <span> . 1998-10-06</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：二茂铁双（亚膦酸酯）配体和配合物用于过渡金属催化的反应 </span> </p> </li> <li> <div> <b>4. </b><a class="enjiyixqcontent" href="/patent-detail/06130465964496.html">Reactions of bis-oxazolines with 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