Highly Mesoporous Metal‐Organic Frameworks as Synergistic Multimodal Catalytic Platforms for Divergent Cascade Reactions

Dutta Soumen; Kumari Nitee; Dubbu Sateesh; Jang Sun Woo; Kumar Amit; Ohtsu Hiroyoshi; Kim Junghoon; Cho Seung Hwan; Kawano Masaki; Lee In Su

摘要

Abstract >Rational engineering and assimilation of diverse chemo‐ and biocatalytic functionalities in a single nanostructure is highly desired for efficient multistep chemical reactions but has so far remained elusive. Here, we design and synthesize multimodal catalytic nanoreactors (MCNRs) based on a mesoporous metal‐organic framework (MOF). The MCNRs consist of customizable metal nanocrystals and stably anchored enzymes in the mesopores, as well as coordinatively unsaturated cationic metal MOF nodes, all within a single nanoreactor space. The highly intimate and diverse catalytic mesoporous microenvironments and facile accessibility to the active site in the MCNR enables the cooperative and synergistic participation from different chemo‐ and biocatalytic components. This was shown by one‐pot multistep cascade reactions involving a heterogeneous catalytic nitroaldol reaction followed by a [Pd/lipase]‐catalyzed chemoenzymatic dynamic kinetic resolution to yield optically pure (99?%?ee) nitroalcohol derivatives in quantitative yields. </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> <P>对单一纳米结构中不同化学和生物催化功能的合理工程和同化，高效用于高效的多步化学反应，但到目前为止难以难以捉摸。这里，我们基于介孔金属 - 有机框架（MOF）设计和合成多式型催化纳米反应器（MCNR）。 MCNR由可定制的金属纳米晶体和中孔中的稳定锚定酶组成，以及坐标不饱和阳离子金属MOF节点，全部在单个纳米反应器空间内。高度紧密且多样化的催化介孔微环境和对MCNR活性部位的容纳可接近能力使得来自不同的化疗和生物催化组分的协同和协同参与。这是由涉及非均相催化硝基甲醇反应的单盆多步级联反应显示，其次是[Pd /脂肪酶] - 催化的化学酶动态动态动力学分辨率，得到光学纯（＆ 99〜EE）的硝基醇衍生物，以定量产率。< / 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7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=Dutta Soumen&option=202" target="_blank" rel="nofollow">Dutta Soumen;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Kumari Nitee&option=202" target="_blank" rel="nofollow">Kumari Nitee;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Dubbu Sateesh&option=202" target="_blank" rel="nofollow">Dubbu Sateesh;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Jang Sun Woo&option=202" target="_blank" rel="nofollow">Jang Sun Woo;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Kumar Amit&option=202" target="_blank" rel="nofollow">Kumar Amit;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Ohtsu Hiroyoshi&option=202" target="_blank" rel="nofollow">Ohtsu Hiroyoshi;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Kim Junghoon&option=202" target="_blank" rel="nofollow">Kim Junghoon;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Cho Seung Hwan&option=202" target="_blank" rel="nofollow">Cho Seung Hwan;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Kawano Masaki&option=202" target="_blank" rel="nofollow">Kawano Masaki;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Lee In Su&option=202" target="_blank" rel="nofollow">Lee In Su;</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>Center for Nanospace-confined Chemical Reactions (NCCR)Pohang University of Science and Technology (POSTECH)Pohang 37673 South Korea;</p> <p>Center for Nanospace-confined Chemical Reactions (NCCR)Pohang University of Science and Technology (POSTECH)Pohang 37673 South Korea;</p> <p>Center for Nanospace-confined Chemical Reactions (NCCR)Pohang University of Science and Technology (POSTECH)Pohang 37673 South Korea;</p> <p>Center for Nanospace-confined Chemical Reactions (NCCR)Pohang University of Science and Technology (POSTECH)Pohang 37673 South Korea;</p> <p>Center for Nanospace-confined Chemical Reactions (NCCR)Pohang University of Science and Technology (POSTECH)Pohang 37673 South Korea;</p> <p>Department of ChemistryTokyo Institute of TechnologyTokyo 152-8550 Japan;</p> <p>Department of ChemistryPohang University of Science and Technology (POSTECH)Pohang 37673 South Korea;</p> <p>Department of ChemistryPohang University of Science and Technology (POSTECH)Pohang 37673 South Korea;</p> <p>Department of ChemistryTokyo Institute of TechnologyTokyo 152-8550 Japan;</p> <p>Center for Nanospace-confined Chemical Reactions (NCCR)Pohang University of Science and Technology (POSTECH)Pohang 37673 South Korea;</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=cascade reactions&option=203" rel="nofollow">cascade 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=mesoporous MOFs&option=203" rel="nofollow">mesoporous MOFs;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=multimodal catalysts&option=203" rel="nofollow">multimodal catalysts;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=nanocatalysts&option=203" rel="nofollow">nanocatalysts;</a> </p> <div class="translation"> 机译：级联反应;异构催化;中孔MOF;多式催化剂;纳米催化剂; </div> </li> </ul> </div> </div> <div class="literature cardcommon"> <div class="similarity "> <h3 class="all_title" id="enpatent66">相似文献</h3> <div 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