Interrogating the Surface Intermediates and Water Oxidation Products of Boron‐Doped Diamond Electrodes with Scanning Electrochemical Microscopy

Counihan Michael J.; Setwipatanachai Worapol; Rodríguez‐López Joaquín

摘要

Abstract > Boron‐doped diamond (BDD) electrodes are widely used in electrochemical sensing and water purification owing to their chemical and structural stability under harsh reaction conditions. Water oxidation at BDD electrodes is known to produce reactive oxygen species, but the discharged and surface chemistries involved in these processes have not been studied in depth. Here, we present scanning electrochemical microscopy (SECM) studies of electrogenerated intermediates and products formed on sp 2 carbon‐containing BDD electrodes that display stark differences in their reactivity as a function of electrolyte type and pH during water oxidation. The most reactive and abundant species discharged from the electrode were observed at pH?11 in sulfate electrolyte. With the surface interrogation mode of SECM, two kinetically distinct surface intermediates were clearly distinguished, with one forming two orders of magnitude faster than the other but displaying a slower desorption rate. The surface coverage of these species was estimated in the range of 4–7×10 ?5 ?mol/cm 2 for the first, and 3–4.4×10 ?5 ?mol/cm 2 for the second one. SECM imaging suggested that regions of increased product evolution have decreased electron transfer kinetics and limited surface sites for intermediate binding. This work establishes methods for studying highly reactive intermediates found in BDD and paves the way for the inspection of other interfaces where solvolysis impacts their reactivity and evolution. </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> > 由于在恶劣的反应条件下，硼掺杂的金刚石（BDD）电极广泛用于电化学传感和水净化。已知BDD电极的水氧化产生活性氧物质，但涉及这些方法的排出和表面化学尚未深入研究。在此，我们呈现扫描电化学显微镜（SECM）研究的电流中间体和在SP上形成的产品 2 </ sup> 含碳的BDD电极，其在水氧化过程中显示其反应性的缺点差异和水氧化过程中的pH。在硫酸盐电解质中在pHα11中观察到从电极排出的最具反应性和丰富的物质。利用SECM的表面询问模式，清楚地区分两个动力学，不同的表面中间体，一个比另一个形成两个数量级，但显示较慢的解吸速率。这些物种的表面覆盖率估计为4-7×10 ？5 </ sup> ？mol / cm 2 </ sup> 第一个，3-4.4×10 ？5 </ sup> ？mol / cm 2 </ sup> 对于第二个。 SECM成像表明，增加产品进化的区域具有降低的电子转移动力学和中间结合的有限表面位点。这项工作建立了研究BDD中发现的高反应性中间体的方法，并为其他界面进行检查，铺设溶剂影响其反应性和进化。 </ 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-16042/'>《ChemElectroChem》</a> <b style="margin: 0 2px;">|</b><span>2019年第13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"> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Counihan Michael J.&option=202" target="_blank" rel="nofollow">Counihan Michael J.;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Setwipatanachai Worapol&option=202" target="_blank" rel="nofollow">Setwipatanachai Worapol;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Rodríguez‐López Joaquín&option=202" target="_blank" rel="nofollow">Rodríguez‐López Joaquín;</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 ChemistryUniversity of Illinois at Urbana-Champaign600 South Mathews Avenue Urbana Illinois 61801 Untied States;</p> <p>Department of ChemistryUniversity of Illinois at Urbana-Champaign600 South Mathews Avenue Urbana Illinois 61801 Untied States;</p> <p>Department of ChemistryUniversity of Illinois at Urbana-Champaign600 South Mathews Avenue Urbana Illinois 61801 Untied States;</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/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=boron-doped diamond&option=203" rel="nofollow">boron-doped diamond;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=scanning electrochemical microscopy&option=203" rel="nofollow">scanning electrochemical microscopy;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=water splitting&option=203" rel="nofollow">water splitting;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=surface chemistry&option=203" rel="nofollow">surface chemistry;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=reactive intermediates&option=203" rel="nofollow">reactive intermediates;</a> </p> <div class="translation"> 机译：硼掺杂的金刚石;扫描电化学显微镜;水分裂;表面化学;反应性中间体; 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