Bubble Trouble: Quantifying the Effects of Bubbles on the Electrochemical Interface

IF 13.1 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-04-04 DOI:10.1021/acscatal.5c0014410.1021/acscatal.5c00144

Anja Logar, Dževad K. Kozlica, Ožbej Vodeb, Miran Gaberšček, Nejc Hodnik and Dušan Strmčnik*,

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引用次数: 0

Abstract

The accumulation of electrochemically produced bubbles is inevitable in gas-evolving reactions and can induce potential losses by theoretically increasing activation, concentration, and ohmic overpotentials. These effects are often either overstated or completely neglected in the literature, which complicates the accurate analysis of experimental results for gas evolution reactions. This study systematically identifies and quantifies the overpotential losses induced by bubbles by combining experimental results for hydrogen (HER) and oxygen evolution reactions (OER), obtained using the rotating disk electrode (RDE) technique, with simulations based on a two-dimensional transmission line model. Our results show that ohmic overpotential is the primary cause of apparent activity loss due to bubbles in RDE. This effect leads to catalyst activity misestimates exceeding 2 orders of magnitude, and Tafel slope errors of 100% at higher currents if left uncorrected. By identifying these effects, this work provides a robust framework for mitigating inaccuracies and improving the characterization of electrocatalysts for gas evolution reactions.

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气泡问题：量化气泡对电化学界面的影响

在气体演化反应中，电化学产生的气泡的积累是不可避免的，并且可以通过理论上增加活化、浓度和欧姆过电位来诱导潜在的损失。这些效应在文献中往往被夸大或完全忽略，这使得气体演化反应实验结果的准确分析变得复杂。本研究将旋转圆盘电极（RDE）技术得到的析氢反应（HER）和析氧反应（OER）的实验结果与基于二维传输线模型的模拟相结合，系统地识别和量化了气泡引起的过电位损失。我们的研究结果表明，欧姆过电位是RDE中气泡造成明显活性损失的主要原因。这种影响导致催化剂活性的错误估计超过2个数量级，如果不加以纠正，在高电流下的塔菲尔斜率误差为100%。通过识别这些影响，这项工作为减轻不准确性和改进气体演化反应电催化剂的表征提供了一个强大的框架。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.