Molecular Pivot‐Hinge Installation to Evolve Topology in Rare‐Earth Metal–Organic Frameworks

摘要

Abstract > Linker desymmetrization has been witnessed as a powerful design strategy for the discovery of highly connected metal–organic frameworks (MOFs) with unprecedented topologies. Herein, we introduce molecular pivot‐hinge installation as a linker desymmetrization strategy to evolve the topology of highly connected rare‐earth (RE) MOFs, where a pivot group is placed in the center of a linker similar to a hinge. By tuning the composition of pivot groups and steric hindrances of the substituents on various linker rotamers, MOFs with various topologies can be obtained. The combination of L‐SO <sub>2</sub> with C <sub> 2 v </sub> symmetry and 12‐connected RE <sub>9</sub> clusters leads to the formation of a fascinating (4,12)‐c dfs new topology. Interestingly, when replacing L‐SO <sub>2</sub> with a tetrahedra linker L‐O, the stacking behaviors of RE‐organic layers switch from an eclipsed mode to a staggered stacking mode, leading to the discovery of an intriguing hjz topology. Additionally, the combination of the RE cluster and a linker [(L‐(CH <sub>3</sub> ) <sub>6</sub> )] with more bulky groups gives rise to a flu topology with a new 8‐c inorganic cluster. The diversity of these RE‐MOFs was further enhanced through post‐synthetic installation of linkers with various functional groups. Functionalization of each linker with acidic and basic units in the mesoporous RE‐based PCN‐905‐SO <sub>2</sub> allows for efficient cascade catalytic transformation within the functionalized channels. </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> > 接头去对称化已被目睹了具有前所未有的拓扑的高度连接的金属 - 有机框架（MOF）的强大设计策略。在此，我们将分子枢轴铰链安装引入连接聚乙烯偏移策略，以发展高度连接的稀土（RE）MOF的拓扑，其中枢轴组置于类似于铰链的接头的中心。通过调节各种接头旋转辊上的取代基的枢轴组的组成和旋转取代基的空间障碍，可以获得具有各种拓扑的MOF。 l-so的组合 <sub> 2 </ sub> 和 c </ i> <sub> 2 v </ i> </ sub> 对称性和12连接的重新 <sub> 9 </ sub> 群集导致形成迷人（4,12）-c dfs </ b> 新拓扑。有趣的是，在更换l-so时 <sub> 2 </ sub> 通过四面体连接器L-O，重新有机层的堆叠行为从墨西多的模式切换到交错的堆叠模式，导致发现有趣的堆叠模式 hjz </ b> 拓扑。另外，RE群集和链接器的组合[（L-（CH） <sub> 3 </ sub> 的） <sub> 6 </ sub> ）]有更庞大的团体引起了一个流感</ b> 具有新的8-C无机集群的拓扑。通过具有各种官能团的接头的合成综合安装，进一步增强了这些RE-MOF的多样性。每个接头的官能化与酸性和基于中孔的PCN-905 - 所以的酸性和基本单元 - 所以 <sub> 2 </ sub> 允许在功能化通道内有效的级联催化转化。 </ 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9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=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=linker desymmetrization&option=203" rel="nofollow">linker desymmetrization;</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=structural evolution&option=203" rel="nofollow">structural evolution;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=topology&option=203" rel="nofollow">topology;</a> </p> <div class="translation"> 机译：异质催化;接头去对比;金属 - 有机框架;结构演变;拓扑; </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/0704028164249.html">Molecular Pivot‐Hinge Installation to Evolve Topology in Rare‐Earth Metal–Organic 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