Selective Catalytic Chemistry at Rhodium(II) Nodes in Bimetallic Metal–Organic Frameworks

摘要

Abstract > We report the first study of a gas‐phase reaction catalyzed by highly dispersed sites at the metal nodes of a crystalline metal–organic framework (MOF). Specifically, CuRhBTC (BTC 3? =benzenetricarboxylate) exhibited hydrogenation activity, while other isostructural monometallic and bimetallic MOFs did not. Our multi‐technique characterization identifies the oxidation state of Rh in CuRhBTC as +2, which is a Rh oxidation state that has not previously been observed for crystalline MOF metal nodes. These Rh 2+ sites are active for the catalytic hydrogenation of propylene to propane at room temperature, and the MOF structure stabilizes the Rh 2+ oxidation state under reaction conditions. Density functional theory calculations suggest a mechanism in which hydrogen dissociation and propylene adsorption occur at the Rh 2+ sites. The ability to tailor the geometry and ensemble size of the metal nodes in MOFs allows for unprecedented control of the active sites and could lead to significant advances in rational catalyst design. </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> > 我们报告了通过在结晶金属 - 有机骨架（MOF）的金属节点处的高度分散位点催化的气相反应的第一次研究。具体而言，粗康（BTC 3？</ sup> =苯甲酸甲酯）表现出氢化活性，而其他肌醇组织和双金属MOF没有。我们的多技术表征将RH的RH作为+2中的RH的氧化状态识别，这是对于结晶MOF金属节点之前未观察到的RH氧化状态。这些RH. 2 + </ sup> 位点在室温下为丙烯催化氢化丙烷催化加氢，并且MOF结构稳定RH 2 + </ sup> 反应条件下的氧化态。密度函数理论计算表明，在RH中发生氢解离和丙烯吸附的机制 2 + </ sup> 网站。定制MOF中的金属节点的几何和集合尺寸的能力允许前所未有的活性位点控制，并且可能导致合理催化剂设计的显着进展。 </ 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>2019年第46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"> </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/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=gas-phase reactions&option=203" rel="nofollow">gas-phase reactions;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=heterogeneous catalysis&option=203" rel="nofollow">heterogeneous catalysis;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=metal–organic frameworks&option=203" rel="nofollow">metal–organic frameworks;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=rhodium&option=203" rel="nofollow">rhodium;</a> </p> <div class="translation"> 机译：DFT计算;气相反应;异质催化;金属有机框架;铑; </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/0704028164565.html">Selective Catalytic Chemistry at Rhodium(II) Nodes in Bimetallic Metal–Organic Frameworks</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-19011/" target="_blank" rel="nofollow" class="tuijian_authcolor">Angewandte Chemie .</a> <span>2019</span><span>,第46期</span> </span> </div> <p 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<span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=杜东杰&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 杜东杰</a> <span> . 2016</span> </span> </div> </li> </ul> <ul style="display: none;"> <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/patent-detail/06120113075972.html">一种负载型镍钴双金属纳米催化剂及其在催化香兰素选择性加氢反应中的应用</a> <b>[P]</b> . <span> 中国专利： CN113101933A </span> <span> . 2021-07-13</span> </div> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/patent-detail/06120113312481.html">基于双金属纳米粒子的催化剂、其在选择性氢化中的用途及制造该催化剂的方法</a> <b>[P]</b> . <span> 中国专利： CN113365729A </span> <span> . 2021-09-07</span> </div> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/patent-detail/06130408477321.html">METHOD OF DETERMINING THE RHODIUM (III) IN AQUEOUS SOLUTIONS BY INVERSION VOLTMETERMETRY METHOD BY SELECTIVE ELECTROOXIDATION LEAD (II) FROM INTERMETAL COMPOUNDS WITH THE RHODIUM Rh<Sub>3</Sub>Pb<Sub>2</Sub> AND Rh<Sub>5</Sub>Pb<Sub>7</Sub></a> <b>[P]</b> . <span> 外国专利：  RU2624789C1 </span> <span> . 2017-07-06</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：铑（Rh <Sub> 3 </ Sub> Pb <Sub> 2 </ Sub>）与铑（Sub）之间的化合物间选择性电化学氧化铅（II）选择性溶出伏安法测定水溶液中的铑（III） > 5 </ Sub> Pb <Sub> 7 </ Sub> </span> </p> </li> <li> <div> <b>4. </b><a class="enjiyixqcontent" href="/patent-detail/06130436858062.html">Preparing method of cobalt/rhodium bimetallic nanoparticle and immobilized cobalt/rhodium hetero bimetallic nanoparticle and preparing method of chemical compounds using said catalysts</a> <b>[P]</b> . <span> 外国专利：  KR100569066B1 </span> <span> . 2006-04-10</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：钴/铑双金属纳米粒子和固定化钴/铑杂双金属纳米粒子的制备方法及使用所述催化剂的化合物的制备方法 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