Computational Approaches to Photoelectrode Design through Molecular Functionalization for Enhanced Photoelectrochemical Water Splitting

Iyer Ashwathi; Kearney Kara; Ertekin Elif

摘要

Abstract >Photoelectrochemical water splitting is a promising carbon‐free approach to produce hydrogen from water. A photoelectrochemical cell consists of a semiconductor photoelectrode in contact with an aqueous electrolyte. Its performance is sensitive to properties of the photoelectrode/electrolyte interface, which may be tuned through functionalization of the photoelectrode surface with organic molecules. This can lead to improvements in the photoelectrode's properties. This Minireview summarizes key computational investigations on using molecular functionalization to modify photoelectrode stability, barrier height, and catalytic activity. It is discussed how first‐principles density functional theory, first‐principles molecular dynamics, and device modeling simulations can provide predictive insights and complement experimental investigations of functionalized photoelectrodes. Challenges and future directions in the computational modeling of functionalized photoelectrode/electrolyte interfaces within the context of experimental studies are also highlighted. </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> 光电化学水分裂是一种有望的无碳含碳方法来生产水中的氢气。光电化学电池由与含水电解质接触的半导体光电极组成。其性能对光电极/电解质界面的性能敏感，这可以通过与有机分子的光电极表面的功能化调谐。这可能导致光电极的性质改进。该MiniView总结了使用分子官能化以改变光电极稳定性，阻挡高度和催化活性的关键计算研究。讨论了第一原理密度泛函理论，第一原理分子动力学和器件建模模拟如何提供功能化光电极的预测洞察力和补充实验研究。还强调了实验研究中功能化光电极/电解质接口的计算建模中的挑战和未来方向。</ 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-16185/'>《ChemSusChem》</a> <b style="margin: 0 2px;">|</b><span>2019年第9期</span><b style="margin: 0 2px;">|</b><span>共14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=Iyer Ashwathi&option=202" target="_blank" rel="nofollow">Iyer Ashwathi;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Kearney Kara&option=202" target="_blank" rel="nofollow">Kearney Kara;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Ertekin Elif&option=202" target="_blank" rel="nofollow">Ertekin Elif;</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 PhysicsUniversity of Illinois at Urbana-Champaign1110 W Green Street Urbana Illinois 61801 USA;</p> <p>Department of Mechanical Science and EngineeringUniversity of Illinois at Urbana-Champaign1206 W Green Street Urbana Illinois 61801 USA;</p> <p>Department of Mechanical Science and EngineeringUniversity of Illinois at Urbana-Champaign1206 W Green Street Urbana Illinois 61801 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/159.html" title="化学">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=ab initio calculations&option=203" rel="nofollow">ab initio calculations;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=monolayers&option=203" rel="nofollow">monolayers;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=hybrid composites&option=203" rel="nofollow">hybrid composites;</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=semiconductors&option=203" rel="nofollow">semiconductors;</a> </p> <div class="translation"> 机译：AB Initio计算;单层;混合复合材料;光催化;半导体; 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