Styrene Hydroformylation with In Situ Hydrogen: Regioselectivity Control by Coupling with the Low‐Temperature Water–Gas Shift Reaction

Li Tianbo; Chen Fang; Lang Rui; Wang Hua; Su Yang; Qiao Botao; Wang Aiqin; Zhang Tao

摘要

Abstract >The hydroformylation of olefins is one of the most important homogeneously catalyzed industrial reactions for aldehyde synthesis. Various ligands can be used to obtain the desired linear aldehydes in the hydroformylation of aliphatic olefins. However, in the hydroformylation of aromatic substrates, branched aldehydes are formed preferentially with common ligands. In this study, a novel approach to selectively obtain linear aldehydes in the hydroformylation of styrene and its derivatives was developed by coupling with a water–gas shift reaction on a Rh single‐atom catalyst without the use of ligands. Detailed studies revealed that the hydrogen generated in situ from the water–gas shift is critical for the highly regioselective formation of linear products. The coupling of a traditional homogeneous catalytic process with a heterogeneous catalytic reaction to tune product selectivity may provide a new avenue for the heterogenization of homogenous catalytic processes. </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> >烯烃的加氢甲酰化是醛合成的最重要的均匀催化工业反应之一。各种配体可用于在脂族烯烃的加氢甲酰化中获得所需的线性醛。然而，在芳族基材的加氢甲酰化中，优先用普通配体优先形成支链醛。在该研究中，通过在RH单原子催化剂上的水气移反应与RH单原子催化剂上的水气移反应偶联，产生一种在苯乙烯的加氢甲酰化中选择性地获得线性醛的新方法。详细研究表明，原位产生的氢气气体变化对于线性产物的高度区域形成至关重要。传统均匀催化过程与异质催化反应的偶联以调整产品选择性可以为均匀催化过程的异质化提供新的途径。</ 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19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=Li Tianbo&option=202" target="_blank" rel="nofollow">Li Tianbo;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Chen Fang&option=202" target="_blank" rel="nofollow">Chen Fang;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Lang Rui&option=202" target="_blank" rel="nofollow">Lang Rui;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Wang Hua&option=202" target="_blank" rel="nofollow">Wang Hua;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Su Yang&option=202" target="_blank" rel="nofollow">Su Yang;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Qiao Botao&option=202" target="_blank" rel="nofollow">Qiao Botao;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Wang Aiqin&option=202" target="_blank" rel="nofollow">Wang Aiqin;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Zhang Tao&option=202" target="_blank" rel="nofollow">Zhang Tao;</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>Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023 China;</p> <p>Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023 China;</p> <p>Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023 China;</p> <p>Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023 China;</p> <p>Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023 China;</p> <p>Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023 China;</p> <p>Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023 China;</p> <p>Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023 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=hydroformylation&option=203" rel="nofollow">hydroformylation;</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=regioselectivity&option=203" rel="nofollow">regioselectivity;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=single-atom catalysts&option=203" rel="nofollow">single-atom catalysts;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=styrene&option=203" rel="nofollow">styrene;</a> </p> <div class="translation"> 机译：加氢甲酰化;氢;区域胶凝;单原子催化剂;苯乙烯; </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/0704028161513.html">Styrene Hydroformylation with In Situ Hydrogen: Regioselectivity Control by Coupling with the Low‐Temperature Water–Gas Shift Reaction</a> <b>[J]</b> . <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Li Tianbo&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Li Tianbo,</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Chen Fang&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Chen Fang,</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Lang Rui&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Lang Rui,</a> <a href="/journal-foreign-19011/" target="_blank" rel="nofollow" class="tuijian_authcolor">Angewandte Chemie .</a> <span>2020</span><span>,第19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：具有原位氢的苯乙烯加氢甲酰化：通过与低温水气移反应偶联的区域选择性控制</span> </p> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/academic-journal-foreign_international-journal-hydrogen-energy_thesis/020416474267.html">Modeling And Simulation Of Hydrogen Generation From High-temperature And Low-temperature Water Gas Shift Reactions</a> <b>[J]</b> . <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Wei-Hsin Chen&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Wei-Hsin Chen,</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Mu-Rong lin&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Mu-Rong lin,</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Tsung Leo Jiang&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Tsung Leo Jiang,</a> <a href="/journal-foreign-1283/" target="_blank" rel="nofollow" class="tuijian_authcolor">International journal of hydrogen energy .</a> <span>2008</span><span>,第22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：高温和低温水煤气变换反应产氢的建模与模拟</span> </p> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/journal-foreign-detail/070403020308.html">Low temperature water-gas shift:in situ DRIFTS-reaction study of ceria surface area on te evolution of formates on Pt/CeO_2 fuel processing catalysts for fuel cell applications</a> <b>[J]</b> . <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Gary Jacobs&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Gary Jacobs,</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Leann Williams&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Leann Williams,</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Uschi Graham&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Uschi Graham,</a> <a href="/journal-foreign-19278/" target="_blank" rel="nofollow" class="tuijian_authcolor">Applied Catalysis, A. 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href="/academic-degree-domestic_mphd_thesis/020314946607.html">机械力促进的N-去甲酰化，交叉脱氢偶联反应用于制备喹啉/四氢异喹啉类衍生物</a> <b>[A] </b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=俞静波&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 俞静波</a> <span> . 2013</span> </span> </div> </li> </ul> <ul style="display: none;"> <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/patent-detail/06120210559713.html">氢甲酰化合成反应釜和氢甲酰化合成反应的反应系统</a> <b>[P]</b> . <span> 中国专利： CN210560168U </span> <span> . 2020.05.19</span> </div> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/patent-detail/06120101055282.html">一种氢甲酰化和加氢反应的多相催化剂、其制法及应用</a> <b>[P]</b> . <span> 中国专利： CN110280310A </span> <span> . 2019-09-27</span> </div> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/patent-detail/06130437564325.html">Preparation of hydrogen from natural gas, by reaction with air and water vapor in a single reactor then high- and low-temperature shift reactions of carbon monoxide with water</a> <b>[P]</b> . <span> 外国专利：  ES2243146A1 </span> <span> . 2005-11-16</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：由天然气制备氢气，方法是在单个反应器中与空气和水蒸气反应，然后一氧化碳与水进行高温和低温转化反应 </span> </p> </li> <li> <div> <b>4. </b><a class="enjiyixqcontent" href="/patent-detail/06130445895658.html">Reforming device used for producing a hydrogen-rich gas from a mixture containing hydrocarbons comprises a high temperature shift reaction unit, a low temperature shift reaction unit and a heat exchanger contained in a converter</a> <b>[P]</b> . <span> 外国专利：  DE10041712A1 </span> <span> . 2002-03-07</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：用于从包含烃的混合物中产生富氢气体的重整装置包括高温转化反应单元，低温转化反应单元和转换器中包含的热交换器 </span> </p> </li> <li> <div> <b>5. </b><a class="enjiyixqcontent" href="/patent-detail/06130432138175.html">Method for creating hydrogen by water gas shift reaction at very low temperatures</a> <b>[P]</b> . <span> 外国专利：  EP1878782A1 </span> <span> . 2008-01-16</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：在非常低的温度下通过水煤气变换反应产生氢气的方法 </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('0704028161513','4',7,2,1,'',this,24)" class="delivery" prompt="010401" 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