Defect‐Mediated Ordering of Condensed Water Structures in Microporous Zeolites

摘要

Abstract >Ab‐initio molecular dynamics simulations and transmission infrared spectroscopy are employed to characterize the structure of water networks in defect‐functionalized microporous zeolites. Thermodynamically stable phases of clustered water molecules are localized at some of the defects in zeolite Beta, which include catalytic sites such as framework Lewis acidic Sn atoms in closed and hydrolyzed‐open forms, as well as silanol nests. These water clusters compete with ideal gas‐like structures at low water densities and pore‐filling phases at higher water densities, with the equilibrium phase determined by the water chemical potential. The physical characteristics of these phases are determined by the defect identity, with the local binding and orientation of hydroxyl moieties around the defects playing a central role. The results suggest general principles for how the structure of polar solvents in microporous solid acids is influenced by local defect functionalization, and the thermodynamic stability of the condensed phases surrounding such sites, in turn, implies that the catalysis of Lewis acids will be influenced by local water ordering. </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> > AB-Initio分子动力学模拟和传输红外光谱法用于表征缺陷官能化的微孔沸石中的水网络结构。聚集水分子的热力学稳定阶段在沸石β的一些缺陷处定位，其包括催化位点，例如封闭和水解 - 开放形式的框架Lewis酸性Sn原子，以及硅烷醇巢。这些水簇以低水密度和孔隙率在更高的水密度下竞争的理想气体状结构，具有通过水化学势确定的平衡相。这些相的物理特性由缺陷同一性确定，局部结合和取向周围的羟基部分呈现核心作用。结果表明，微孔固体酸中的极性溶剂结构的一般原理受到局部缺陷官能化的影响，以及依次围绕此类部位的凝聚相的热力学稳定性意味着路易斯酸的催化将受到当地的影响津津。</ 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=catalysis&option=203" rel="nofollow">catalysis;</a> <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=molecular dynamics&option=203" rel="nofollow">molecular dynamics;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=solvents&option=203" rel="nofollow">solvents;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=zeolites&option=203" rel="nofollow">zeolites;</a> </p> <div class="translation"> 机译：催化;DFT计算;分子动力学;溶剂;沸石; </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/0704028165226.html">Defect‐Mediated Ordering of Condensed Water Structures in Microporous Zeolites</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 class="zwjiyix translation" style="max-width: initial;height: auto;word-break: break-all;white-space: initial;text-overflow: initial;overflow: initial;"> <span>机译：微孔沸石中凝聚水结构的缺陷介导的排序</span> </p> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/journal-foreign-detail/0704013198250.html">Crystal structure analyses of two TMA silicates with ordered defects: RUB-20, a layered zeolite precursor, and RUB-22, a microporous framework silicate</a> <b>[J]</b> . <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Bernd Marler&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Bernd Marler,</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Hermann Gies&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Hermann Gies </a> <a href="/journal-foreign-33007/" target="_blank" rel="nofollow" class="tuijian_authcolor">Zeitschrift fur Kristallographie. 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<a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=田瓅&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 田瓅</a> <span> . 2017</span> </span> </div> </li> </ul> <ul style="display: none;"> <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/patent-detail/061201953534.html">微孔沸石包覆中孔沸石催化剂的制备及其在甲醇制丙烯反应中的应用</a> <b>[P]</b> . <span> 中国专利： CN103551188B </span> <span> . 2016.03.09</span> </div> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/patent-detail/06120102179582.html">微孔沸石包覆中孔沸石催化剂的制备及其在甲醇制丙烯反应中的应用</a> <b>[P]</b> . <span> 中国专利： CN103551188A </span> <span> . 2014-02-05</span> </div> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/patent-detail/06130422077706.html">PREPARATION METHOD OF RANDOMLY ASSEMBLED MESOSTRUCTURE CONSTRUCTED WITH HIERARCHICALLY MESOPOROUS AND MICROPOROUS MFI ZEOLITE NANOSHEETS OF SINGLE-UNIT-CELL THICKNESS, USING WATER GLASS AS THE SILICA SOURCE</a> <b>[P]</b> . <span> 外国专利：  KR20120022089A </span> <span> . 2012-03-12</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：以玻璃为硅源的单单元厚度MME沸石分子筛的层级介孔结构的组装方法 </span> </p> </li> <li> <div> <b>4. </b><a class="enjiyixqcontent" href="/patent-detail/06130421890458.html">Preparation method of randomly assembled mesostructure constructed with hierarchically mesoporous and microporous MFI zeolite nanosheets of single-unit-cell thickness, using water glass as the silica source</a> <b>[P]</b> . <span> 外国专利：  KR101189757B1 </span> <span> . 2012-10-10</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：以水玻璃为二氧化硅源，由单孔厚度的分层介孔和微孔MFI沸石纳米片构成的随机组装介观结构的制备方法 </span> </p> </li> <li> <div> <b>5. </b><a class="enjiyixqcontent" href="/patent-detail/06130446842739.html">Process for obtaining Microporous Zeolite zsm-5 Family pentasil where stirring a mixture of water, NaOH and silicate Source, reacts to pressure Weld, is filtered and dried.The process comprises that the Zeolite is obtained from using Diatomite as Guiding Agent Grid Shells of the Diatomite.</a> <b>[P]</b> . <span> 外国专利：  CL2000003595A1 </span> <span> . 2002-06-14</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：制备微孔沸石zsm-5族戊二醇的方法，其中搅拌水，NaOH和硅酸盐源的混合物，使其在压力下反应焊接，过滤并干燥。该方法包括将硅藻土用作硅藻土的导向剂网格壳而获得。硅藻土。 </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" 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