Electrode Surface Heating with Organic Films Improves CO2 Reduction Kinetics on Copper,ACS Energy Letters

当前位置： X-MOL 学术 › ACS Energy Lett. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Electrode Surface Heating with Organic Films Improves CO2 Reduction Kinetics on Copper
ACS Energy Letters ( IF 19.3 ) Pub Date : 2024-03-11 , DOI: 10.1021/acsenergylett.4c00204
Nicholas B Watkins _{1,

2} , Yungchieh Lai _{1,

3} , Zachary J Schiffer _{1,

3} , Virginia M Canestraight _{1,

2} , Harry A Atwater _{1,

3} , Theodor Agapie _{1,

2} , Jonas C Peters _{1,

2} , John M Gregoire _{1,

3}

Affiliation

Management of the electrode surface temperature is an understudied aspect of (photo)electrode reactor design for complex reactions, such as CO₂ reduction. In this work, we study the impact of local electrode heating on electrochemical reduction of CO₂ reduction. Using the ferri/ferrocyanide open circuit voltage as a reporter of the effective reaction temperature, we reveal how the interplay of surface heating and convective cooling presents an opportunity for cooptimizing mass transport and thermal assistance of electrochemical reactions, where we focus on reduction of CO₂ to carbon-coupled (C₂₊) products. The introduction of an organic coating on the electrode surface facilitates well-behaved electrode kinetics with near-ambient bulk electrolyte temperature. This approach helps to probe the fundamentals of thermal effects in electrochemical reactions, as demonstrated through Bayesian inference of Tafel kinetic parameters from a suite of high throughput experiments, which reveal a decrease in overpotential for C₂₊ products by 0.1 V on polycrystalline copper via 60 °C surface heating.

中文翻译：

使用有机薄膜进行电极表面加热可改善铜上的二氧化碳还原动力学

电极表面温度的管理是复杂反应（例如CO ₂还原）的（光）电极反应器设计的一个待研究的方面。在这项工作中，我们研究了局部电极加热对CO ₂电化学还原的影响。使用铁/亚铁氰化物开路电压作为有效反应温度的报告器，我们揭示了表面加热和对流冷却的相互作用如何为协同优化电化学反应的传质和热辅助提供了机会，其中我们重点关注 CO ₂的还原碳偶联（C ₂₊ ）产物。在电极表面引入有机涂层有助于在接近环境的本体电解质温度下表现良好的电极动力学。这种方法有助于探究电化学反应中热效应的基本原理，正如通过一系列高通量实验对 Tafel 动力学参数进行贝叶斯推断所证明的那样，这些实验揭示了多晶铜上的 C ₂₊产物的过电势通过 60 降低了 0.1 V °C 表面加热。

更新日期：2024-03-11

点击分享查看原文

点击收藏

公开下载

阅读更多本刊最新论文本刊介绍/投稿指南11