电化学二氧化碳转化的微环境前沿

IF 14 Q1 CHEMISTRY, MULTIDISCIPLINARY Accounts of materials research Pub Date : 2024-10-30 DOI:10.1021/accountsmr.4c00294
Andrew B. Wong
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(c) Description of the activity and activity coefficient for CO<sub>2</sub>, CO, and H<sub>2</sub>O (or other proton donors). Activity is the lens through which to understand numerous phenomena within the CO<sub>2</sub>RR microenvironment Figure 2. Schematic overview for macroscale, microscale, and nanoscale effects on planar (a–c) and porous (d–f) electrodes. First, the activity coefficient and concentration terms offer a helpful parameter space to compare the effects of various interventions and adjustments to the microenvironment that had previously been difficult to compare based on objective measures (Figure 1b). Second, this approach highlights the importance of improving our understanding of the relative contributions of three-phase (gas–liquid–solid) and larger area two-phase (liquid–solid) interfaces on CO<sub>2</sub>RR, which has attracted recent attention. (12,13) Third, this understanding highlights the importance of developing new <i>in situ</i> and <i>in operando</i> analytical techniques to probe the local distributions of CO<sub>2</sub>, CO, and H<sub>2</sub>O under reaction conditions. Attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) has already shown promise for quantifying bound versus free water during CO<sub>2</sub>RR. (13) What are strategies to extend recent fundamental developments on controlling water activity to improve CO<sub>2</sub>RR performance at high current densities? How can we use the microenvironment to explore electrochemical strategies to simultaneously accomplish CO<sub>2</sub> capture and conversion? Based on the historical development of CO<sub>2</sub>RR approaches, can we or should we adopt new materials for CO<sub>2</sub>RR GDLs and ionomers (typically materials developed for other chemical transformations with different requirements) to specialize in CO<sub>2</sub>RR’s requirements? In CO<sub>2</sub>RR, what is the structure of the three-phase gas–liquid–solid and other interfaces under reaction conditions? Leveraging the microenvironment, how can CO<sub>2</sub> be used to make higher-value products or products that can integrate into the economy to achieve net negative CO<sub>2</sub> emissions? What can new CO<sub>2</sub>RR systems look like? Moreover, can we reimagine our strategies to valorize CO<sub>2</sub>? Are there advantages to performing CO<sub>2</sub>RR electrochemistry at high temperatures or high pressures? To what extent can we leverage the enzymatic microenvironment of living systems to achieve electrochemical CO<sub>2</sub> conversion to high-value products beyond C<sub>3+</sub>? <b>Andrew B. Wong</b> is an Assistant Professor in the Department of Materials Science and Engineering at the National University of Singapore. Prior to his independent career, he was a postdoctoral researcher at Stanford University, where he was coadvised by Thomas Jaramillo and James Harris. He received his Ph.D. in Chemistry from UC Berkeley in 2016 under Peidong Yang and received his joint B.S.–M.S. degree in Chemistry at the University of Chicago in 2011. The A.B. Wong Group focuses on understanding and developing control of the microenvironment for electrochemical CO<sub>2</sub> conversion and exploring emerging strategies to valorize CO<sub>2</sub>. 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引用次数: 0

摘要

二氧化碳在水溶液条件下的低溶解度 CO2RR 所需的质子供体与通过竞争性氢进化反应 (HER) 将供体质子转化为 H2 的强烈倾向之间的微妙平衡 CO2RR 多种产物的反应途径之间的微妙平衡 局部 pH 值、离子浓度、疏水性和活性位点随碳酸盐形成和电催化剂重组等现象而发生的动态变化 图 1。CO2RR 微环境效应示意图概览。(a) 微环境对 CO2RR 性能的影响。(b) 微环境考虑因素:实验条件、电催化剂特性和电解质特性。(c) 描述 CO2、CO 和 H2O(或其他质子供体)的活性和活性系数。活性是了解 CO2RR 微环境中众多现象的透视镜。平面(a-c)和多孔(d-f)电极的宏观、微观和纳米效应示意图概览。首先,活性系数和浓度项提供了一个有用的参数空间,可用于比较各种干预和微环境调整的效果,而这些效果以前很难根据客观测量进行比较(图 1b)。其次,这种方法强调了提高我们对三相(气-液-固)和较大面积的两相(液-固)界面对 CO2RR 的相对贡献的理解的重要性,这一点最近引起了人们的关注。(12,13)第三,这种认识凸显了开发新的原位和操作分析技术以探测反应条件下 CO2、CO 和 H2O 局部分布的重要性。衰减全反射表面增强红外吸收光谱(ATR-SEIRAS)已经显示出在 CO2RR 过程中量化结合水和自由水的前景。(13) 有什么策略可以扩展最近在控制水活性方面的基本发展,以提高高电流密度下的 CO2RR 性能?我们如何利用微环境来探索同时完成二氧化碳捕获和转化的电化学策略?基于 CO2RR 方法的历史发展,我们是否可以或应该采用新材料作为 CO2RR 的 GDLs 和离子体(通常是为具有不同要求的其他化学转化开发的材料),以专门满足 CO2RR 的要求?在 CO2RR 中,反应条件下气-液-固三相界面和其他界面的结构是怎样的?利用微环境,如何利用二氧化碳制造更高价值的产品或可融入经济的产品,以实现二氧化碳净负排?新的 CO2RR 系统是什么样的?此外,我们能否重新构想二氧化碳的价值化战略?在高温或高压下进行 CO2RR 电化学反应是否有优势?我们能在多大程度上利用生物系统的酶微环境实现电化学 CO2 转化为 C3+ 以外的高价值产品?Andrew B. Wong 是新加坡国立大学材料科学与工程系助理教授。在独立工作之前,他曾在斯坦福大学从事博士后研究,师从 Thomas Jaramillo 和 James Harris。他于2016年获得加州大学伯克利分校化学博士学位,师从杨培东,并于2011年在芝加哥大学获得化学学士-硕士联合学位。A.B. Wong 小组的研究重点是了解和开发电化学二氧化碳转化的微环境控制,并探索二氧化碳价值化的新兴战略。A.B.W. 感谢新加坡国立大学通过总统青年教授早期职业奖(WBS:A-0009245-05-00)提供的启动资金。目前正在进行的生物电化学二氧化碳转化工作得到了新加坡国家研究基金会竞争性研究计划(NRF-CRP27-2021-0004)的资助。本文引用了 14 篇其他出版物。本文尚未被其他出版物引用。
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The Microenvironment Frontier for Electrochemical CO2 Conversion
low CO2 solubility in aqueous conditions the delicate balance between the delivery of essential proton donors for CO2RR versus the strong tendency to convert donated protons to H2 via the competing hydrogen evolution reaction (HER) the delicate balance between reaction pathways toward multiple CO2RR products dynamic changes in local pH, ion concentrations, hydrophobicity, and active sites in response to phenomena such as carbonate formation and restructuring of electrocatalysts Figure 1. Schematic overview of CO2RR microenvironment effects. (a) Microenvironment impact on CO2RR performance. (b) Microenvironment considerations: experimental conditions, electrocatalyst characteristics, and electrolyte characteristics. (c) Description of the activity and activity coefficient for CO2, CO, and H2O (or other proton donors). Activity is the lens through which to understand numerous phenomena within the CO2RR microenvironment Figure 2. Schematic overview for macroscale, microscale, and nanoscale effects on planar (a–c) and porous (d–f) electrodes. First, the activity coefficient and concentration terms offer a helpful parameter space to compare the effects of various interventions and adjustments to the microenvironment that had previously been difficult to compare based on objective measures (Figure 1b). Second, this approach highlights the importance of improving our understanding of the relative contributions of three-phase (gas–liquid–solid) and larger area two-phase (liquid–solid) interfaces on CO2RR, which has attracted recent attention. (12,13) Third, this understanding highlights the importance of developing new in situ and in operando analytical techniques to probe the local distributions of CO2, CO, and H2O under reaction conditions. Attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) has already shown promise for quantifying bound versus free water during CO2RR. (13) What are strategies to extend recent fundamental developments on controlling water activity to improve CO2RR performance at high current densities? How can we use the microenvironment to explore electrochemical strategies to simultaneously accomplish CO2 capture and conversion? Based on the historical development of CO2RR approaches, can we or should we adopt new materials for CO2RR GDLs and ionomers (typically materials developed for other chemical transformations with different requirements) to specialize in CO2RR’s requirements? In CO2RR, what is the structure of the three-phase gas–liquid–solid and other interfaces under reaction conditions? Leveraging the microenvironment, how can CO2 be used to make higher-value products or products that can integrate into the economy to achieve net negative CO2 emissions? What can new CO2RR systems look like? Moreover, can we reimagine our strategies to valorize CO2? Are there advantages to performing CO2RR electrochemistry at high temperatures or high pressures? To what extent can we leverage the enzymatic microenvironment of living systems to achieve electrochemical CO2 conversion to high-value products beyond C3+? Andrew B. Wong is an Assistant Professor in the Department of Materials Science and Engineering at the National University of Singapore. Prior to his independent career, he was a postdoctoral researcher at Stanford University, where he was coadvised by Thomas Jaramillo and James Harris. He received his Ph.D. in Chemistry from UC Berkeley in 2016 under Peidong Yang and received his joint B.S.–M.S. degree in Chemistry at the University of Chicago in 2011. The A.B. Wong Group focuses on understanding and developing control of the microenvironment for electrochemical CO2 conversion and exploring emerging strategies to valorize CO2. A.B.W. would like to acknowledge startup funds from the National University of Singapore through the Presidential Young Professorship early career award (WBS: A-0009245-05-00). Ongoing efforts on bioelectrochemical CO2 conversion are financially supported by the Competitive Research Programme of the National Research Foundation Singapore (NRF-CRP27-2021-0004). This article references 14 other publications. This article has not yet been cited by other publications.
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