C?C Bond Formation in Syngas Conversion over Zinc Sites Grafted on ZSM‐5 Zeolite

Chen Yuxiang; Gong Ke; Jiao Feng; Pan Xiulian; Hou Guangjin; Si Rui; Bao Xinhe

摘要

Abstract > Despite significant progress achieved in Fischer–Tropsch synthesis (FTS) technology, control of product selectivity remains a challenge in syngas conversion. Herein, we demonstrate that Zn 2+ ‐ion exchanged ZSM‐5 zeolite steers syngas conversion selectively to ethane with its selectivity reaching as high as 86?% among hydrocarbons (excluding CO <sub>2</sub> ) at 20?% CO conversion. NMR spectroscopy, X‐ray absorption spectroscopy, and X‐ray fluorescence indicate that this is likely attributed to the highly dispersed Zn sites grafted on ZSM‐5. Quasi‐in‐situ solid‐state NMR, obtained by quenching the reaction in liquid N <sub>2</sub> , detects C <sub>2</sub> species such as acetyl (‐COCH <sub>3</sub> ) bonding with an oxygen, ethyl (‐CH <sub>2</sub> CH <sub>3</sub> ) bonding with a Zn site, and epoxyethane molecules adsorbing on a Zn site and a Br?nsted acid site of the catalyst, respectively. These species could provide insight into C?C bond formation during ethane formation. Interestingly, this selective reaction pathway toward ethane appears to be general because a series of other Zn 2+ ‐ion exchanged aluminosilicate zeolites with different topologies (for example, SSZ‐13, MCM‐22, and ZSM‐12) all give ethane predominantly. By contrast, a physical mixture of ZnO‐ZSM‐5 favors formation of hydrocarbons beyond C <sub>3+</sub> . These results provide an important guide for tuning the product selectivity in syngas conversion. </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> > 尽管在Fischer-Tropsch合成（FTS）技术中取得了显着进展，但对产品选择性的控制仍然是合成气转化的挑战。在此，我们证明了Zn 2 + </ sup> - 加入ZSM-5沸石带合成气转化为乙烷的选择性转化，其选择性达到碳氢化合物中高达86？％（不包括CO） <sub> 2 </ sub> ）在20？％CO转换时。 NMR光谱，X射线吸收光谱和X射线荧光表明，这可能归因于接枝在ZSM-5上的高度分散的Zn位点。通过淬火液体N中的反应获得准原位固态NMR <sub> 2 </ sub> ，检测C. <sub> 2 </ sub> 乙酰基（-COCH）等物种 <sub> 3 </ sub> ）用氧，乙基键合（-CH <sub> 2 </ sub> CH. <sub> 3 </ sub> ）用Zn位点键合，并分别吸附在Zn位点上的环氧乙烷分子和催化剂的Brαnsted酸部位。这些物种可以在乙烷形成期间提供对C？C键形成的洞察力。有趣的是，这种选择性反应途径向乙烷似乎是一般的，因为一系列其他Zn 2 + </ sup> - 加入用不同的拓扑（例如，SSZ-13，MCM-22和ZSM-12）交换了硅铝酸盐沸石（SSZ-13，MCM-22和ZSM-12）。相比之下，Zno-ZSM-5的物理混合物融合了超出C之外的碳氢化合物 <sub> 3 + </ sub> 。这些结果提供了调整合成气转化中产品选择性的重要指南。 </ 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6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=Chen Yuxiang&option=202" target="_blank" rel="nofollow">Chen Yuxiang;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Gong Ke&option=202" target="_blank" rel="nofollow">Gong Ke;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Jiao Feng&option=202" target="_blank" rel="nofollow">Jiao Feng;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Pan Xiulian&option=202" target="_blank" rel="nofollow">Pan Xiulian;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Hou Guangjin&option=202" target="_blank" rel="nofollow">Hou Guangjin;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Si Rui&option=202" target="_blank" rel="nofollow">Si Rui;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Bao Xinhe&option=202" target="_blank" rel="nofollow">Bao Xinhe;</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>State Key Laboratory of CatalysisChinese Academy of Sciences457 Zhongshan Road Dalian 116023 China;</p> <p>State Key Laboratory of CatalysisChinese Academy of Sciences457 Zhongshan Road Dalian 116023 China;</p> <p>State Key Laboratory of CatalysisChinese Academy of Sciences457 Zhongshan Road Dalian 116023 China;</p> <p>State Key Laboratory of CatalysisChinese Academy of Sciences457 Zhongshan Road Dalian 116023 China;</p> <p>State Key Laboratory of CatalysisChinese Academy of Sciences457 Zhongshan Road Dalian 116023 China;</p> <p>Shanghai Synchrotron Radiation FacilityChinese Academy of SciencesShanghai 201204 China;</p> <p>State Key Laboratory of CatalysisChinese Academy of Sciences457 Zhongshan Road Dalian 116023 China;</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=hydrocarbons&option=203" rel="nofollow">hydrocarbons;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=NMR spectroscopy&option=203" rel="nofollow">NMR spectroscopy;</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> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=zinc&option=203" rel="nofollow">zinc;</a> </p> <div class="translation"> 机译：碳氢化合物;NMR光谱;沸石;锌; 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Pierella,</a> <span>2021</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：使用在ZSM-11沸石上支持的贵金属的半连续批量反应器中将甘油转化为增值产物</span> </p> </li> <li> <div> <b>7. </b><a class="enjiyixqcontent" href="/open-access_resources_thesis/01000127187585.html">Active sites and mechanism of the direct conversion of methane and carbon dioxide to acetic acid over the zinc-modified H-ZSM-5 zeolite</a> <b>[O] </b> . <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Peng Zhang&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Peng Zhang,</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Xuejing Yang&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Xuejing Yang,</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Xiuli Hou&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Xiuli Hou,</a> <span>2019</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：在锌改性的H-ZSM-5沸石上甲烷和二氧化碳直接转化为乙酸的活性位点和机制</span> </p> </li> <li> <div> <b>8. </b><a class="enjiyixqcontent" href="/ntis-science-report_de_thesis/020711539341.html">Correlation of Zeolites Nul and ZSM-5 Acid Site Strength with Catalytic Activity and Selectivity. Final Report</a> <b>[R] </b> . <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Hayhurst, D. T.&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Hayhurst, D. T. </a> <span>1984</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：沸石Nul和Zsm-5酸位强度与催化活性和选择性的关系。总结报告</span> </p> </li> </ul> <ul style="display: none;"> <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/academic-journal-cn_chinese-journal-catalysis_thesis/0201296795431.html">合成气在铁锰/沸石催化剂上合成低碳烯烃的研究 Ⅲ.碱改性ZSM-5沸石担载Fe-MnO催化剂的强碱作用及MnO助剂的作用</a> <b>[J]</b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=徐龙伢&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 徐龙伢</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=陈国权&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,陈国权</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=蔡光宇&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,蔡光宇</a> <span> <a href="/journal-cn-28399/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 催化学报 </a> </span> <span> . 1990</span><span>,第6期</span> </span> </div> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/academic-journal-cn_chinese-journal-catalysis_thesis/0201295861616.html">合成气在铁锰/沸石催化剂上合成低碳烯烃的研究——Ⅱ.碱改性ZSM-5担载Fe-MnO催化剂反应性能的考察</a> <b>[J]</b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=徐龙伢&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 徐龙伢</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=陈国权&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,陈国权</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=蔡光宇&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,蔡光宇</a> <span> <a href="/journal-cn-28399/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 催化学报 </a> </span> <span> . 1990</span><span>,第5期</span> </span> </div> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/academic-journal-cn_chemical-journal-chinese-universities_thesis/0201231620547.html">沸石表面有机金属化学ZSM-5外表面上——Ge(n-C4H9)x基团的接枝及其性质研究</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> <span> <a href="/journal-cn-10958/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 高等学校化学学报 </a> </span> <span> . 2001</span><span>,第002期</span> </span> </div> </li> <li> <div> <b>4. </b><a class="enjiyixqcontent" href="/academic-journal-cn_chinese-journal-catalysis_thesis/0201298176551.html">合成气在铁锰/沸石催化剂上合成低碳烯烃的研究 Ⅳ.添加碱性助剂的DM-Ⅱ高硅沸石担载型催化剂的性能</a> <b>[J]</b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=徐龙伢&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 徐龙伢</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=陈国权&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,陈国权</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=蔡光宇&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,蔡光宇</a> <span> <a href="/journal-cn-28399/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 催化学报 </a> </span> <span> . 1992</span><span>,第1期</span> </span> </div> </li> <li> <div> <b>5. </b><a class="enjiyixqcontent" href="/academic-journal-cn_chinese-journal-catalysis_thesis/0201295757006.html">合成气在铁锰/沸石催化剂上合成低碳烯烃的研究——Ⅰ.不同沸石分子筛担载Fe-MnO催化剂反应性能的考察</a> <b>[J]</b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=徐龙伢&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 徐龙伢</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=陈国权&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,陈国权</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=蔡光宇&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,蔡光宇</a> <span> <a href="/journal-cn-28399/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 催化学报 </a> </span> <span> . 1990</span><span>,第5期</span> </span> </div> </li> <li> <div> <b>6. </b><a class="enjiyixqcontent" href="/academic-conference-cn_meeting-6668_thesis/020221731334.html">锌改性ZSM-5分子筛上锌羰基物种的固体核磁共振研究</a> <b>[C]</b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Guodong Qi&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . Guodong Qi</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=齐国栋&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,齐国栋</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Qiang Wang&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,Qiang Wang</a> <span> <a href="/conference-cn-6668/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 第十七届全国波谱学学术会议 </a> <span> <span> . 2012</span> </span> </div> </li> <li> <div> <b>7. </b><a class="enjiyixqcontent" href="/academic-degree-domestic_mphd_thesis/020313309594.html">改性ZSM-5及ZSM-11沸石上甲醇制汽油反应性能研究</a> <b>[A] </b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=朱桐萱&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 朱桐萱</a> <span> . 2016</span> </span> </div> </li> </ul> <ul style="display: none;"> <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/patent-detail/06120100440328.html">锌改性多级孔ZSM-5纳米沸石及其制备方法</a> <b>[P]</b> . <span> 中国专利： CN109607563A </span> <span> . 2019-04-12</span> </div> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/patent-detail/06120793989.html">用于在锌或锌合金上形成黑色的3价铬化学转化膜的处理溶液和在锌或锌合金上形成黑色的3价铬化学转化膜的方法</a> <b>[P]</b> . <span> 中国专利： CN101421434B </span> <span> . 2011.08.31</span> </div> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/patent-detail/06130472404538.html">Process for syngas conversions to liquid hydrocarbon products utilizing ZSM-45 zeolite</a> <b>[P]</b> . <span> 外国专利：  US4523047A </span> <span> . 1985-06-11</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：使用ZSM-45沸石将合成气转化为液态烃产品的方法 </span> </p> </li> <li> <div> <b>4. </b><a class="enjiyixqcontent" href="/patent-detail/06130411412595.html">ZSM-5 Preparing method of amin-grafting ZSM-5 zeolite for adsorption of carbon dioxide</a> <b>[P]</b> . <span> 外国专利：  KR101595741B1 </span> <span> . 2016-02-19</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：ZSM-5吸附性接枝ZSM-5沸石的制备方法 </span> </p> </li> <li> <div> <b>5. </b><a class="enjiyixqcontent" href="/patent-detail/06130473110333.html">Process for preparation of a zeolite ZSM - 23, zeolite crystalline material of synthetic ZSM - 23, catalyst, process for conversion of organic load.Organic compound containing nitrogen and process for preparation of said compound</a> <b>[P]</b> . <span> 外国专利：  BR8401987A </span> <span> . 1984-12-04</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：沸石ZSM-23的制备方法，合成ZSM-23的沸石晶体材料，催化剂，有机负荷的转化方法含氮的有机化合物及其制备方法 </span> </p> </li> </ul> </div> </div> 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