B‐MWW Zeolite: The Case Against Single‐Site Catalysis

Altvater Natalie R.; Dorn Rick W.; Cendejas Melissa C.; McDermott William P.; Thomas Brijith; Rossini Aaron J.; Hermans Ive

摘要

Abstract > Boron‐containing materials have recently been identified as highly selective catalysts for the oxidative dehydrogenation (ODH) of alkanes to olefins. It has previously been demonstrated by several spectroscopic characterization techniques that the surface of these boron‐containing ODH catalysts oxidize and hydrolyze under reaction conditions, forming an amorphous B <sub>2</sub> (OH) <sub> x </sub> O <sub> (3? x /2) </sub> ( x= 0–6) layer. Yet, the precise nature of the active site(s) remains elusive. In this Communication, we provide a detailed characterization of zeolite MCM‐22 isomorphously substituted with boron (B‐MWW). Using 11 B solid‐state NMR spectroscopy, we show that the majority of boron species in B‐MWW exist as isolated BO <sub>3</sub> units, fully incorporated into the zeolite framework. However, this material shows no catalytic activity for ODH of propane to propene. The catalytic inactivity of B‐MWW for ODH of propane falsifies the hypothesis that site‐isolated BO <sub>3</sub> units are the active site in boron‐based catalysts. This observation is at odds with other traditionally studied catalysts like vanadium‐based catalysts and provides an important piece of the mechanistic puzzle. </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> > 最近已鉴定为含硼的氧化脱氢（ODH）对烯烃的高选择性催化剂的材料。先前已经证明了几种光谱表征技术，即含有这些含硼的ODH催化剂的表面在反应条件下氧化和水解，形成无定形B. <sub> 2 </ sub> （哦） <sub> x </ i> </ sub> O. <sub> （3？ x </ i> / 2） </ sub> （ x = </ i> 0-6）层。然而，活跃场地的确切性质仍然难以捉摸。在这种通信中，我们提供了用硼（B-MWW）成像异构被替代的沸石MCM-22的详细表征。使用 11 </ sup> B固态NMR光谱，我们表明B-MWW中的大多数硼种类存在于孤立的博中 <sub> 3 </ sub> 单位，完全纳入沸石框架中。然而，该材料表明丙烷与丙烯的ODH的催化活性没有催化活性。 B-MWW对丙烷ODH的催化不活值伪造了位点分离的博的假设 <sub> 3 </ sub> 单位是硼基催化剂的活性位点。该观察结果与其他传统上研究的催化剂如钒基催化剂相对，并且提供了一种重要的机械拼图。 </ 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16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=Altvater Natalie R.&option=202" target="_blank" rel="nofollow">Altvater Natalie R.;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Dorn Rick W.&option=202" target="_blank" rel="nofollow">Dorn Rick W.;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Cendejas Melissa C.&option=202" target="_blank" rel="nofollow">Cendejas Melissa C.;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=McDermott William P.&option=202" target="_blank" rel="nofollow">McDermott William P.;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Thomas Brijith&option=202" target="_blank" rel="nofollow">Thomas Brijith;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Rossini Aaron J.&option=202" target="_blank" rel="nofollow">Rossini Aaron J.;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Hermans Ive&option=202" target="_blank" rel="nofollow">Hermans Ive;</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>Department of Chemical and Biological EngineeringUniversity of Madison – Wisconsin1415 Engineering Drive Madison WI 53706 USA;</p> <p>Department of ChemistryIowa State University2438 Pammel Dr. Ames IA 50011 USA;</p> <p>Department of ChemistryUniversity of Wisconsin – Madison1101 University Avenue Madison WI 53706 USA;</p> <p>Department of ChemistryUniversity of Wisconsin – Madison1101 University Avenue Madison WI 53706 USA;</p> <p>Department of ChemistryIowa State University2438 Pammel Dr. Ames IA 50011 USA;</p> <p>Department of ChemistryIowa State University2438 Pammel Dr. Ames IA 50011 USA;</p> <p>Department of Chemical and Biological EngineeringUniversity of Madison – Wisconsin1415 Engineering Drive Madison WI 53706 USA;</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=boron&option=203" rel="nofollow">boron;</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=oxidative dehydrogenation&option=203" rel="nofollow">oxidative dehydrogenation;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=solid-state NMR&option=203" rel="nofollow">solid-state NMR;</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：硼;异质催化;氧化脱氢;固态NMR;沸石; 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target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 马晓玲</a> <span> . 2009</span> </span> </div> </li> </ul> <ul style="display: none;"> <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/patent-detail/061201477565.html">在单活性中心催化剂存在的情况下的聚丙烯制备</a> <b>[P]</b> . <span> 中国专利： CN102666603B </span> <span> . 2014.10.15</span> </div> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/patent-detail/06120106847295.html">在单活性中心催化剂存在的情况下的聚丙烯制备</a> <b>[P]</b> . <span> 中国专利： CN102666603A </span> <span> . 2012-09-12</span> </div> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/patent-detail/06130417425424.html">METHOD FOR PREPARING THE TITANOSILICATE FORM OF MWW ZEOLITE USING A PURE SILICA MWW MATERIAL AS A PRECURSOR, AND THE USE THEREOF</a> <b>[P]</b> . <span> 外国专利：  WO2013171350A8 </span> <span> . 2014-02-06</span> </div> <p class="zwjiyix translation" style="max-width: initial;height: auto;word-break: break-all;white-space: initial;text-overflow: 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