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采用汞欠电位沉积法对电化学可及的氧化铱表面积进行定量分析。

Quantification of electrochemically accessible iridium oxide surface area with mercury underpotential deposition.

作者信息

Edgington Jane, Vispute Sejal, Li Ruihan, Deberghes Adrien, Seitz Linsey C

机构信息

Department of Chemical and Biological Engineering, Northwestern University, Evanston, IL 60208-3113, USA.

出版信息

Sci Adv. 2024 Nov 8;10(45):eadp8911. doi: 10.1126/sciadv.adp8911. Epub 2024 Nov 6.

Abstract

Research drives development of sustainable electrocatalytic technologies, but efforts are hindered by inconsistent reporting of advances in catalytic performance. Iridium-based oxide catalysts are widely studied for electrocatalytic technologies, particularly for the oxygen evolution reaction (OER) for proton exchange membrane water electrolysis, but insufficient techniques for quantifying electrochemically accessible iridium active sites impede accurate assessment of intrinsic activity improvements. We develop mercury underpotential deposition and stripping as a reversible electrochemical adsorption process to robustly quantify iridium sites and consistently normalize OER performance of benchmark IrO electrodes to a single intrinsic activity curve, where other commonly used normalization methods cannot. Through rigorous deconvolution of mercury redox and reproportionation reactions, we extract net monolayer deposition and stripping of mercury on iridium sites throughout testing using a rotating ring disk electrode. This technique is a transformative method to standardize OER performance across a wide range of iridium-based materials and quantify electrochemical iridium active sites.

摘要

研究推动了可持续电催化技术的发展,但催化性能进展报告的不一致阻碍了相关工作。铱基氧化物催化剂在电催化技术中得到了广泛研究,特别是用于质子交换膜水电解的析氧反应(OER),但用于量化电化学可及铱活性位点的技术不足,妨碍了对本征活性改善的准确评估。我们开发了汞欠电位沉积和溶出作为一种可逆的电化学吸附过程,以可靠地量化铱位点,并将基准IrO电极的OER性能一致地归一化为单一的本征活性曲线,而其他常用的归一化方法则无法做到这一点。通过对汞氧化还原和再分配反应的严格反卷积,我们使用旋转环盘电极在整个测试过程中提取了汞在铱位点上的净单层沉积和溶出。该技术是一种变革性方法,可在广泛的铱基材料中标准化OER性能并量化电化学铱活性位点。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/417e/11540024/2290c8f8b42c/sciadv.adp8911-f1.jpg

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