A Supported Bismuth Halide Perovskite Photocatalyst for Selective Aliphatic and Aromatic C–H Bond Activation

摘要

Abstract > Direct selective oxidation of hydrocarbons to oxygenates by O <sub>2</sub> is challenging. Catalysts are limited by the low activity and narrow application scope, and the main focus is on active C?H bonds at benzylic positions. In this work, stable, lead‐free, Cs <sub>3</sub> Bi <sub>2</sub> Br <sub>9</sub> halide perovskites are integrated within the pore channels of mesoporous SBA‐15 silica and demonstrate their photocatalytic potentials for C?H bond activation. The composite photocatalysts can effectively oxidize hydrocarbons (C <sub>5</sub> to C <sub>16</sub> including aromatic and aliphatic alkanes) with a conversion rate up to 32900?μmol?g <sub>cat</sub> ?1 ?h ?1 and excellent selectivity (99?%) towards aldehydes and ketones under visible‐light irradiation. Isotopic labeling, in?situ spectroscopic studies, and DFT calculations reveal that well‐dispersed small perovskite nanoparticles (2–5?nm) possess enhanced electron–hole separation and a close contact with hydrocarbons that facilitates C(sp 3 )?H bond activation by photoinduced charges. </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> > 通过O直接选择性烃氧化至氧化物 <sub> 2 </ sub> 是挑战。催化剂受到低活性和窄应用范围的限制，主要焦点是在苄基位置处的活性C'H键。在这项工作中，稳定，无铅，CS <sub> 3 </ sub> 双 <sub> 2 </ sub> 布鲁斯 <sub> 9 </ sub> 卤化物钙酸盐集成在介孔SBA-15二氧化硅的孔通道内，并证明了它们的光催化电位对于C-H键活化。复合光催化剂可以有效地氧化烃（C. <sub> 5 </ sub> 到C. <sub> 16 </ sub> 包括芳族和脂族烷烃），转化率高达32900？μmol？g <sub> cat </ sub> ？1 </ sup> ？H ？1 </ sup> 在可见光照射下朝向醛和酮的优异选择性（＆ 99〜99倍）。同位素标记，In？原位光谱研究和DFT计算显示，分散良好的小钙钛矿纳米颗粒（2-5μm）具有增强的电子 - 空穴分离和与促进C的碳氢化合物紧密接触（SP 3 </ sup> ）？H键激活光致电荷。 </ 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14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=bismuth&option=203" rel="nofollow">bismuth;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=nanoparticles&option=203" rel="nofollow">nanoparticles;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=perovskites&option=203" rel="nofollow">perovskites;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=photocatalysis&option=203" rel="nofollow">photocatalysis;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=SBA-15 silica&option=203" rel="nofollow">SBA-15 silica;</a> </p> <div class="translation"> 机译：铋;纳米颗粒;Perovskites;光催化;SBA-15二氧化硅; </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/0704028162228.html">A Supported Bismuth Halide Perovskite Photocatalyst for Selective Aliphatic and Aromatic C–H Bond Activation</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 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EISENBRAUN</a> <span> <a href="/journal-cn-9169/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 聚氨酯工业 </a> </span> <span> . 1989</span><span>,第002期</span> </span> </div> </li> <li> <div> <b>6. </b><a class="enjiyixqcontent" href="/academic-degree-domestic_mphd_thesis/020313613440.html">I三甲基膦支持的富电性铁化合物对C-F键和C-H键选择性活化及铁氢化合物的性质研究;II三甲基膦支持的双核钴化合物的制备</a> <b>[A] </b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=徐晓峰&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 徐晓峰</a> <span> . 2011</span> </span> </div> </li> </ul> <ul style="display: none;"> <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/patent-detail/061203894756.html">芳香族酰胺芳环C-H键直接氨基化反应的方法</a> <b>[P]</b> . <span> 中国专利： CN107398300B </span> <span> . 2020.08.21</span> </div> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/patent-detail/061203625871.html">一种活化含C-H键化合物中的C-H键的方法及其应用</a> <b>[P]</b> . <span> 中国专利： CN107129468B </span> <span> . 2020.02.11</span> </div> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/patent-detail/06130441445479.html">Formation of heteroatom-carbon bonds, giving products of interest for the pharmaceutical and agrochemical industries, comprises using an organolithium compound prepared by reacting an aliphatic or aromatic halide with lithium</a> <b>[P]</b> . <span> 外国专利：  DE10240260A1 </span> <span> . 2004-03-11</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：杂原子-碳键的形成，使药物和农业化学工业产生感兴趣的产品，包括使用通过使脂族或芳族卤化物与锂反应制备的有机锂化合物 </span> </p> </li> <li> <div> <b>4. </b><a class="enjiyixqcontent" href="/patent-detail/06130446871018.html">Mixtures of Thermoplastic interpolimeros Alpha olefin monomers with one or more Vinylidene Aromatic monomer and / or one or more devinilideno aliphatic Cyclo aliphatic monomers or disabled B.With two homopolymers and copolymers of vinyl Halide and sheets and articles manufactured using these</a> <b>[P]</b> . <span> 外国专利：  AR020312A1 </span> <span> . 2002-05-08</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：热塑性互聚物α-烯烃单体与一种或多种亚乙烯基芳族单体和/或一种或多种偏乙烯基脂族环脂族单体或禁用B的混合物。两种卤化乙烯的均聚物和共聚物，以及使用它们制得的片材和制品 </span> </p> </li> <li> <div> <b>5. </b><a class="enjiyixqcontent" href="/patent-detail/06130449092217.html">Thermoplastic compositions of alpha-olefin monomers and one or several vinyl aromatic or vinylidene aromatic monomers and/or one or several sterically protected aliphatic or cycloaliphatic vinyl or vinylidene monomers in a mixture with vinyl halide homopolymers and copolymers</a> <b>[P]</b> . <span> 外国专利：  CZ20001372A3 </span> <span> . 2001-01-17</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：α-烯烃单体和一种或几种乙烯基芳族或亚乙烯基芳族单体和/或一种或几种空间保护的脂族或脂环族乙烯基或亚乙烯基单体与卤化乙烯均聚物和共聚物的混合物的热塑性组合物 </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: 19px;z-index: 999;" onclick="ywcd('0704028162228','4',7,2,1,'',this,24)" class="delivery" prompt="010401" title="通过人工服务将文献原文发送至邮箱" >获取原文</div> <div class="journalsub-pop-up" style="display: none"> <div class="journal-sub"> <h2>期刊订阅</h2> <img src="https://cdn.zhangqiaokeyan.com/img/loginclose.png" alt="关闭" onclick="$('.journalsub-pop-up').hide()"> <p class="pardon">抱歉，该期刊暂不可订阅，敬请期待！</p> <p class="current">目前支持订阅全部北京大学中文核心（2020）期刊目录。</p> <div style="display: 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