Fast and Selective Semihydrogenation of Alkynes by Palladium Nanoparticles Sandwiched in Metal–Organic Frameworks

Choe Kwanghak; Zheng Fengbin; Wang Hui; Yuan Yi; Zhao Wenshi; Xue Guangxin; Qiu Xueying; Ri Myonghak; Shi Xinghua; Wang Yinglong; Li Guodong; Tang Zhiyong

摘要

Abstract > The semihydrogenation of alkynes into alkenes rather than alkanes is of great importance in the chemical industry. Unfortunately, state‐of‐the‐art heterogeneous catalysts hardly achieve high turnover frequencies (TOFs) simultaneously with almost full conversion, excellent selectivity, and good stability. Here, we used metal–organic frameworks (MOFs) containing Zr metal nodes (“UiO”) with tunable wettability and electron‐withdrawing ability as activity accelerators for the semihydrogenation of alkynes catalyzed by sandwiched palladium nanoparticles (Pd NPs). Impressively, the porous hydrophobic UiO support not only leads to an enrichment of phenylacetylene around the Pd NPs but also renders the Pd surfaces more electron‐deficient, which leads to a remarkable catalysis performance, including an exceptionally high TOF of 13835?h ?1 , 100?% phenylacetylene conversion 93.1?% selectivity towards styrene, and no activity decay after successive catalytic cycles. The strategy of using molecularly tailored supports is universal for boosting the selective semihydrogenation of various terminal and internal alkynes. </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> > 炔烃的半水氢化成烯烃而不是烷烃在化学工业中具有重要意义。遗憾的是，最先进的异质催化剂几乎没有同时实现高营业额频率（TOFS），几乎完全转化，优异的选择性和良好的稳定性。在此，我们使用含有Zr金属节点（“UIO”）的金属有机框架（MOF），可调节润湿性和电子提取能力作为夹层钯纳米粒子（Pd NPS）催化的炔烃半氢化的活性促进剂。令人印象深刻地，多孔疏水性UIO支持不仅导致富含PD NPS的苯乙烯，而且还使PD表面更加电子缺陷，这导致了显着的催化性能，包括13835的极高TOF ？1 </ sup> ，100μl％苯乙烯转化93.1〜Δ％对苯乙烯的选择性，并且在连续催化循环之后没有活性衰减。使用分子定制的支撑件的策略是促进各种终端和内部炔烃的选择性半氢化的通用。 </ 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8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=Choe Kwanghak&option=202" target="_blank" rel="nofollow">Choe Kwanghak;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Zheng Fengbin&option=202" target="_blank" rel="nofollow">Zheng Fengbin;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Wang Hui&option=202" target="_blank" rel="nofollow">Wang Hui;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Yuan Yi&option=202" target="_blank" rel="nofollow">Yuan Yi;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Zhao Wenshi&option=202" target="_blank" rel="nofollow">Zhao Wenshi;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Xue Guangxin&option=202" target="_blank" rel="nofollow">Xue Guangxin;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Qiu Xueying&option=202" target="_blank" rel="nofollow">Qiu Xueying;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Ri Myonghak&option=202" target="_blank" rel="nofollow">Ri Myonghak;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Shi Xinghua&option=202" target="_blank" rel="nofollow">Shi Xinghua;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Wang Yinglong&option=202" target="_blank" rel="nofollow">Wang Yinglong;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Li Guodong&option=202" target="_blank" rel="nofollow">Li Guodong;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Tang Zhiyong&option=202" target="_blank" rel="nofollow">Tang Zhiyong;</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>CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190 P. R. China;</p> <p>CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190 P. R. China;</p> <p>CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190 P. R. China;</p> <p>CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190 P. R. China;</p> <p>CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190 P. R. China;</p> <p>CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190 P. R. China;</p> <p>CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190 P. R. China;</p> <p>CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190 P. R. China;</p> <p>CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190 P. R. China;</p> <p>Qingdao University of Science and TechnologyQingdao 266042 P. R. China;</p> <p>CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190 P. R. China;</p> <p>CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190 P. R. 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=alkynes&option=203" rel="nofollow">alkynes;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=hydrogenation&option=203" rel="nofollow">hydrogenation;</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=palladium nanoparticle&option=203" rel="nofollow">palladium nanoparticle;</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：alkynes;氢化;金属有机框架;钯纳米粒子;苯乙烯; 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style="max-width: initial;height: auto;word-break: break-all;white-space: initial;text-overflow: initial;overflow: initial;"> <span>机译：将二氧化碳吸附到多孔金属有机骨架材料上的方法，冷却多孔金属有机骨架材料的方法，使用多孔金属有机骨架材料获得醛的方法以及加热多孔金属有机骨架材料的方法 </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('0704028161445','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 src="https://cdn.zhangqiaokeyan.com/img/loginclose.png" alt="关闭" onclick="$('.journalsub-pop-up').hide()"> <p 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