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journal article·2025-02Open access

Dynamic Redox Induced Localized Charge Accumulation Accelerating Proton Exchange Membrane Electrolysis

Bin Chang, Yuanfu Ren, Nan Mu, Shouwei Zuo, Chen Zou, Wei Zhou, Linrui Wen, Huabing Tao, Weijia Zhou, Zhiping Lai, Yoji Kobayashi, Huabin Zhang

Advanced Materials· Volume 37· Issue 7
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Abstract

Abstract The sluggish anodic oxygen evolution reaction (OER) in proton exchange membrane (PEM) electrolysis necessitates applied bias to facilitate electron transfer as well as bond cleavage and formation. Traditional electrocatalysis focuses on analyzing the effects of electron transfer, while the role of charge accumulation induced by the applied overpotential has not been thoroughly investigated. To explore the influence mechanism of bias‐driven charge accumulation, capacitive Mn is incorporated into IrO2 to regulate the local electronic structure and the adsorption behavior. The applied bias triggers dynamic redox reactions at the active sites, which introduce local charge accumulation on the surface of electrocatalyst. Under bias, Mn oxidation induced a noticeable pseudocapacitance in the pre‐OER region, promoting the OER kinetics of iridium sites. Meanwhile, the increased oxygen vacancy formation energy further prevents the lattice oxygen activation. The PEM electrolyzer, equipped with optimal materials as an anode, operates at a low driving voltage of 1.637 V under 2.0 A cm−2, maintaining stable performance for over 800 h with a low degradation rate (19.4 µV h−1). This work provides insights into the performance of metal oxide catalysts in acidic environments and offers forward‐looking strategies for enhancing the catalytic performance through dynamic redox induced capacitive behavior.
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Research context

Energy storageCatalysis & surfaces

OpenAlex topics: Electrocatalysts for Energy Conversion · Fuel Cells and Related Materials · Advanced battery technologies research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Center for Renewable Energy and Storage Technologies (CREST) Physical Science and Engineering Division King Abdullah University of Science and Technology (KAUST) Thuwal 23955‐6900 Kingdom of Saudi Arabia

KAUST Catalysis Center (KCC) Division of Physical Science and Engineering King Abdullah University of Science and Technology (KAUST) Thuwal 23955‐6900 Kingdom of Saudi Arabia

Institute for Advanced Interdisciplinary Research (iAIR) School of Chemistry and Chemical Engineering University of Jinan Jinan 250022 P. R. China

Department of Applied Physics Tianjin Key Laboratory of Low Dimensional Materials Physics and Preparing Technology Faculty of Science Tianjin University Tianjin 300072 P. R. China

State Key Laboratory for Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials and College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 P. R. China

Division of Physical Sciences and Engineering and Advanced Membranes and Porous Materials Center King Abdullah University of Science and Technology (KAUST) Thuwal 23955‐6900 Kingdom of Saudi Arabia

Funding

King Abdullah University of Science and Technology

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