Gold‐Palladium Nanocluster Catalysts for Homocoupling: Electronic Structure and Interface Dynamics

Ehara Masahiro; Priyakumar U. Deva

摘要

Abstract >The gold‐palladium (Au?Pd) bimetallic nanocluster (NC) catalyst in colloidal phase performs the homocoupling reaction of various aryl chlorides (Ar?Cl) under ambient conditions. We have systematically investigated various aspects of the Au?Pd NC catalysts with respect to this homocoupling reaction by using density functional theory (DFT) calculations, genetic algorithm (GA) approaches, and molecular dynamics (MD) simulations. Our findings include the geometric and electronic structures of the Au?Pd NC, the reactive Pd sites on the NC surface, the electron‐donating effects of surrounding polymer matrix, the reaction mechanism of homocoupling reaction and rate‐determining step, the inverse halogen dependence of the reaction, and the solvation dynamics at interface region between NC and polymer matrix in aqueous solution. </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”>摘录</标题> >胶体相中的金钯（AuΔpd）双金属纳米锰（Nc）催化剂表现在环境条件下各种芳基氯化物（Ar 2 Cl）的同性环耦合反应。通过使用密度泛函理论（DFT）计算，遗传算法（GA）方法和分子动力学（MD）模拟，我们系统地研究了AuαPd NC催化剂的各个方面。我们的发现包括AuαPd NC的几何和电子结构，NC表面上的反应性Pd位点，周围聚合物基质的电子赋予效应，同性环耦合反应的反应机理和速率确定步骤，反向卤素依赖性反应，与水溶液中Nc和聚合物基质界面区域的溶剂化动力学。</ 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-16132/'>《Chemical record》</a> <b style="margin: 0 2px;">|</b><span>2019年第5期</span><b style="margin: 0 2px;">|</b><span>共13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=Ehara Masahiro&option=202" target="_blank" rel="nofollow">Ehara Masahiro;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Priyakumar U. Deva&option=202" target="_blank" rel="nofollow">Priyakumar U. Deva;</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>Institute for Molecular Science and Research Center for Computational Science38 Nishigo-Naka Myodaiji Okazaki 444-8585 Japan;</p> <p>Center for Computational Natural Sciences and BioinformaticsInternational Institute of Information TechnologyHyderabad 500 032 India;</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/159.html" title="化学">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=Au?Pd nanocluster catalysts&option=203" rel="nofollow">Au?Pd nanocluster catalysts;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Ullmann coupling&option=203" rel="nofollow">Ullmann coupling;</a> <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=MD simulations&option=203" rel="nofollow">MD simulations;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Genetic algorithm&option=203" rel="nofollow">Genetic algorithm;</a> </p> <div class="translation"> 机译：au？pd纳米簇催化剂;ullmann耦合;DFT计算;MD仿真;遗传算法; </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/0704022080002.html">Gold‐Palladium Nanocluster Catalysts for Homocoupling: Electronic Structure and Interface Dynamics</a> <b>[J]</b> . <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Ehara Masahiro&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Ehara Masahiro,</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Priyakumar U. 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<b>[P]</b> . <span> 中国专利： CN108355652B </span> <span> . 2021.10.29</span> </div> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/patent-detail/06120110823035.html">一种用于CO氧化反应中的金钯纳米催化剂的制备方法</a> <b>[P]</b> . <span> 中国专利： CN108355652A </span> <span> . 2018-08-03</span> </div> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/patent-detail/06130414969098.html">Method for modifying palladium-gold catalyst, in particularfor hydrodechlorination of tetrachloromethane, and palladium-gold catalyst with suitable structure of the active metal phase produced thereby</a> <b>[P]</b> . <span> 外国专利：  SE1450912A1 </span> <span> . 2015-01-26</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：改性钯金催化剂的方法，特别是用于四氯甲烷的加氢脱氯的方法，以及由此产生的具有合适的活性金属相结构的钯金催化剂 </span> </p> </li> <li> <div> <b>4. </b><a class="enjiyixqcontent" href="/patent-detail/06130446840864.html">Process for preparing a supported Catalyst, Palladium, Gold and copper, Where The Catalyst is prepared by impregnating a porous Carrier with an aqueous solution of a water-soluble Salt of palladium and Copper.Setting the palladium and copper, and then The Catalyst impregnated with a water-soluble Salt of Gold (Divisional Application 1210 - 98).</a> <b>[P]</b> . <span> 外国专利：  CL2001002468A1 </span> <span> . 2002-10-02</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：制备负载型催化剂，钯，金和铜的方法，其中催化剂是通过将多孔载体用钯和铜的水溶性盐的水溶液浸渍而制备的，将钯和铜定型，然后将催化剂浸渍水溶性金盐（分案申请号1210-98）。 </span> </p> </li> <li> <div> <b>5. </b><a class="enjiyixqcontent" href="/patent-detail/06130412230803.html">method for preparing a palladium and gold based catalyst, palladium and gold supported catalyst, methods for preparing vinyl acetate and allyl acetate</a> <b>[P]</b> . <span> 外国专利：  BRPI0706798B1 </span> <span> . 2016-10-04</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：钯金基催化剂的制备方法，钯金负载催化剂，乙酸乙烯酯和乙酸烯丙酯的制备方法 </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('0704022080002','4',7,2,1,'',this,24)" class="delivery" prompt="010401" title="通过人工服务将文献原文发送至邮箱" >获取原文</div> <div class="journalsub-pop-up" style="display: none"> <div class="journal-sub"> <h2>期刊订阅</h2> <img 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