2024,
9(10):
1497-1517.
doi: 10.1016/j.gee.2023.11.003
Abstract:
Electricity-driven water splitting to produce hydrogen is one of the most efficient ways to alleviate energy crisis and environmental pollution problems, in which the anodic oxygen evolution reaction (OER) is the key half-reaction of performance-limiting in water splitting. Given the complicated reaction process and surface reconstruction of the involved catalysts under actual working conditions, unraveling the real active sites, probing multiple reaction intermediates and clarifying catalytic pathways through in-situ characterization techniques and theoretical calculations are essential. In this review, we summarize the recent advancements in understanding the catalytic process, unlocking the water oxidation active phase and elucidating catalytic mechanism of water oxidation by various in-situ characterization techniques. Firstly, we introduce conventionally proposed traditional catalytic mechanisms and novel evolutionary mechanisms of OER, and highlight the significance of optimal catalytic pathways and intrinsic stability. Next, we provide a comprehensive overview of the fundamental working principles, different detection modes, applicable scenarios, and limitations associated with the in-situ characterization techniques. Further, we exemplified the in-situ studies and discussed phase transition detection, visualization of speciation evolution, electronic structure tracking, observation of reaction active intermediates, and monitoring of catalytic products, as well as establishing catalytic structure-activity relationships and catalytic mechanism. Finally, the key challenges and future perspectives for demystifying the water oxidation process are briefly proposed.
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