Semiconductor/Covalent‐Organic‐Framework Z‐Scheme Heterojunctions for Artificial Photosynthesis

Zhang Mi; Lu Meng; Lang Zhong‐Ling; Liu Jiang; Liu Ming; Chang Jia‐Nan; Li Le‐Yan; Shang Lin‐Jie; Wang Min; Li Shun‐Li; Lan Ya‐Qian

摘要

Abstract > A strategy to covalently connect crystalline covalent organic frameworks (COFs) with semiconductors to create stable organic–inorganic Z‐scheme heterojunctions for artificial photosynthesis is presented. A series of COF–semiconductor Z‐scheme photocatalysts combining water‐oxidation semiconductors (TiO <sub>2</sub> , Bi <sub>2</sub> WO <sub>6</sub> , and α‐Fe <sub>2</sub> O <sub>3</sub> ) with CO <sub>2</sub> reduction COFs (COF‐316/318) was synthesized and exhibited high photocatalytic CO <sub>2</sub> ‐to‐CO conversion efficiencies (up to 69.67?μmol?g ?1 ?h ?1 ), with H <sub>2</sub> O as the electron donor in the gas–solid CO <sub>2</sub> reduction, without additional photosensitizers and sacrificial agents. This is the first report of covalently bonded COF/inorganic‐semiconductor systems utilizing the Z‐scheme applied for artificial photosynthesis. Experiments and calculations confirmed efficient semiconductor‐to‐COF electron transfer by covalent coupling, resulting in electron accumulation in the cyano/pyridine moieties of the COF for CO <sub>2</sub> reduction and holes in the semiconductor for H <sub>2</sub> O oxidation, thus mimicking natural photosynthesis. </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> > 呈递与半导体共价连接结晶共价有机骨架（COF）以产生稳定的有机无机Z-方案用于人造光合作用的策略。一系列COF-半导体Z方案光催化剂，组合水氧化半导体（TIO <sub> 2 </ sub> ，BI <sub> 2 </ sub> 禾 <sub> 6 </ sub> 和α-fe <sub> 2 </ sub> O. <sub> 3 </ sub> ）与CO. <sub> 2 </ sub> 还原COF（COF-316/318）被合成并表现出高光催化有限公司 <sub> 2 </ sub> -co-co转换效率（最高69.67？μmol？g ？1 </ sup> ？H ？1 </ sup> ），h <sub> 2 </ sub> o作为气固有限公司的电子供体 <sub> 2 </ sub> 减少，没有额外的光敏剂和牺牲剂。这是利用施用人工光合作用的Z方案的共价键合COF /无机半导体系统的第一报告。实验和计算通过共价偶联证实了高效的半导体到COF电子传递，导致COF的Cyano /吡啶部分中的电子积累 <sub> 2 </ sub> 用于H的半导体中的减少和孔 <sub> 2 </ sub> o氧化，从而模仿自然光合作用。 </ 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7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=Zhang Mi&option=202" target="_blank" rel="nofollow">Zhang Mi;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Lu Meng&option=202" target="_blank" rel="nofollow">Lu Meng;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Lang Zhong‐Ling&option=202" target="_blank" rel="nofollow">Lang Zhong‐Ling;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Liu Jiang&option=202" target="_blank" rel="nofollow">Liu Jiang;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Liu Ming&option=202" target="_blank" rel="nofollow">Liu Ming;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Chang Jia‐Nan&option=202" target="_blank" rel="nofollow">Chang Jia‐Nan;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Li Le‐Yan&option=202" target="_blank" rel="nofollow">Li Le‐Yan;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Shang Lin‐Jie&option=202" target="_blank" rel="nofollow">Shang Lin‐Jie;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Wang Min&option=202" target="_blank" rel="nofollow">Wang Min;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Li Shun‐Li&option=202" target="_blank" rel="nofollow">Li Shun‐Li;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Lan Ya‐Qian&option=202" target="_blank" rel="nofollow">Lan Ya‐Qian;</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>Jiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNo. 1 Wenyuan Road Nanjing 210023 China;</p> <p>Jiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNo. 1 Wenyuan Road Nanjing 210023 China;</p> <p>Key Laboratory of Polyoxometalate Science of the Ministry of EducationNortheast Normal UniversityChangchun 130000 P. R. China;</p> <p>Jiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNo. 1 Wenyuan Road Nanjing 210023 China;</p> <p>Jiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNo. 1 Wenyuan Road Nanjing 210023 China;</p> <p>Jiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNo. 1 Wenyuan Road Nanjing 210023 China;</p> <p>Jiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNo. 1 Wenyuan Road Nanjing 210023 China;</p> <p>Jiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNo. 1 Wenyuan Road Nanjing 210023 China;</p> <p>Jiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNo. 1 Wenyuan Road Nanjing 210023 China;</p> <p>Jiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNo. 1 Wenyuan Road Nanjing 210023 China;</p> <p>Jiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNo. 1 Wenyuan Road Nanjing 210023 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=artificial photosynthesis&option=203" rel="nofollow">artificial photosynthesis;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=CO2 photoreduction&option=203" rel="nofollow">CO2 photoreduction;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=covalent organic frameworks&option=203" rel="nofollow">covalent organic frameworks;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=semiconductors&option=203" rel="nofollow">semiconductors;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Z-scheme&option=203" rel="nofollow">Z-scheme;</a> </p> <div class="translation"> 机译：人造光合作用;CO2光电;共价有机框架;半导体;Z-Scheme; 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