Determination of Molybdenum Species Evolution during Non‐Oxidative Dehydroaromatization of Methane and its Implications for Catalytic Performance

摘要

Abstract > Mo/H‐ZSM‐5 has been studied using a combination of operando X‐ray absorption spectroscopy and High Resolution Powder Diffraction in order to study the evolution of Mo species and their location within the zeolite pores. The results indicate that after calcination the majority of the species present are isolated Mo‐oxo species, attached to the zeolite framework at the straight channels. During reaction, Mo is first partially carburized to intermediate MoC <sub>x</sub> O <sub>y</sub> species. At longer reaction times Mo fully carburizes detaching from the zeolite and aggregates forming initial Mo <sub>1.6</sub> C <sub>3</sub> clusters; this is coincident with maximum benzene production. The Mo <sub>1.6</sub> C <sub>3</sub> clusters are then observed to grow, predominantly on the outer zeolite surface and this appears to be the primary cause of catalyst deactivation. The deactivation is not only due to a decrease in the amount of active Mo surface but also due to a loss in shape‐selectivity which leads to an increased carbon deposition at the outer shell of the zeolite crystals and eventually to pore blockage. </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> > MO / H-ZSM-5已经使用组合研究手术室</ i> X射线吸收光谱和高分辨率粉末衍射，以研究Mo物种及其位置在沸石孔内的进化。结果表明，在煅烧后，存在的大部分物种是分离的Mo-氧杂物物种，其在直线通道上附着在沸石框架上。在反应过程中，首先将Mo部分渗碳为中间MOC <sub> x </ sub> O. <sub> y </ sub> 物种。在较长的反应时间Mo完全渗碳从沸石和聚集体形成初始Mo的蜕皮 <sub> 1.6 </ sub> C <sub> 3 </ sub> 簇;这与最大苯生产一致。莫 <sub> 1.6 </ sub> C <sub> 3 </ sub> 然后观察到簇生长，主要是在外沸石表面上，这似乎是催化剂失活的主要原因。失活不仅是由于活性Mo表面的量减少，而且由于形状选择性的损失，导致沸石晶体的外壳处的碳沉积增加，最终孔隙堵塞。 </ 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-16041/'>《ChemCatChem》</a> <b style="margin: 0 2px;">|</b><span>2019年第1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"> </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/1186.html" title="物理化学（理论化学）、化学物理学">物理化学（理论化学）、化学物理学;</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=MDA&option=203" rel="nofollow">MDA;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Mo-ZSM-5&option=203" rel="nofollow">Mo-ZSM-5;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=operando&option=203" rel="nofollow">operando;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=XAFS&option=203" rel="nofollow">XAFS;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=HRPD&option=203" rel="nofollow">HRPD;</a> </p> <div class="translation"> 机译：MDA;Mo-ZSM-5;Operando;XAFS;HRPD; 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href="/patent-detail/06130403933835.html">A method of preparing a molybdenum-nickel catalyst for the catalytic hydrogenation of carbon dioxide to methane using hydrogen</a> <b>[P]</b> . <span> 外国专利：  CZ307583B6 </span> <span> . 2018-12-27</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：一种制备钼镍催化剂的方法，该催化剂用于使用氢气将二氧化碳催化加氢为甲烷 </span> </p> </li> <li> <div> <b>4. </b><a class="enjiyixqcontent" href="/patent-detail/06130406722744.html">A method of preparing a molybdenum-nickel catalyst for catalytic hydrogenation of carbon dioxide with hydrogen to methane</a> <b>[P]</b> . <span> 外国专利：  CZ2016-387A3 </span> <span> . 2018-01-10</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：一种制备钼镍催化剂的方法，该催化剂用于将氢气中的二氧化碳催化加氢成甲烷 </span> </p> </li> <li> <div> <b>5. </b><a class="enjiyixqcontent" href="/patent-detail/06130403319715.html">HZSM-11 BTX Preparation of Metal Oxide Catalyst Supported on Mesoporous HZSM-11 for Direct Dehydroaromatization of Methane and Propane and Production Method of BTX Using Said Catalyst</a> <b>[P]</b> . <span> 外国专利：  KR20190020394A </span> <span> . 2019-03-04</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：HZSM-11 BTX负载在介孔HZSM-11上的甲烷和丙烷直接脱氢芳构化的金属氧化物催化剂及其制备方法 </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: 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