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氟化钌触发的加速去质子化使酸性电解高效稳定
作者:小柯机器人 发布时间:2025/12/19 17:01:00


近日,中国科学技术大学吴长征团队报道了氟化钌触发的加速去质子化使酸性电解高效稳定。这一研究成果发表在2025年12月18日出版的《美国化学会志》上。

钌基催化剂被认为是实现低成本质子交换膜水电解槽(PEMWEs)的极具前景的候选材料。然而,在酸性析氧反应(OER)的苛刻条件下,钌活性位点易发生不利的过度氧化,导致催化活性显著下降。

研究组在RuO2 (RuO1.86F0.14) 中展示了一种由氟离子(F-)触发的氢键介导机制,该机制同时实现了催化剂的高活性与高稳定性。通过氢键实现的质子向桥氧位点的自发转移,加速了氧中间体的去质子化过程,从而改善了酸性条件下的OER动力学。此外,高电负性的F-削弱了Ru-O键的共价性,进而提升了RuO2的稳定性。

优化后的RuO1.86F0.14催化剂在10 mA cm-2电流密度下表现出153 mV的超低过电位,并能够稳定运行超过980小时,其性能衰减速率低至27 μV h-1。值得注意的是,将该催化剂应用于PEMWEs时,仅需1.63 V电压即可在1 A cm-2电流密度下稳定运行超过100小时。该工作为设计高性能酸性OER催化剂展示了一种具有前景的阴离子调制策略。

附:英文原文

Title: Accelerated Deprotonation Triggered by Fluorinated RuO2 Enables Efficient and Stable Acidic Water Electrolysis

Author: Jian Zheng, Zheng-jie Chen, Wei Lu, Jiajing Wu, Tao Zhang, Lili Zhang, Shida Bao, Siyi Ming, Baihua Feng, Fei Meng, Huanyu Jin, Yuanmiao Sun, Jing Peng, Changzheng Wu

Issue&Volume: December 18, 2025

Abstract: Ru-based catalysts are considered highly promising candidates for enabling cost-effective proton exchange membrane water electrolyzers (PEMWEs). However, under the harsh conditions of acidic oxygen evolution reaction (OER), Ru sites are prone to undesired overoxidation, leading to substantial deterioration in catalytic activity. Herein, we demonstrate a hydrogen-bond-mediated mechanism triggered by fluoride ion (F–) in RuO2 (RuO1.86F0.14) to achieve both high activity and stability. The spontaneous transfer of protons to bridging oxygen through hydrogen bonds accelerates the deprotonation of an oxo-intermediate, which improves the kinetics of the OER in acidic conditions. Moreover, the highly electronegative F– diminishes the covalency of Ru–O bonds and thus boosts the stability of RuO2. The optimized RuO1.86F0.14 catalyst presents an ultralow overpotential of 153 mV at 10 mA cm–2 and can sustain for more than 980 h with a low degradation rate of 27 μV h–1. Notably, the RuO1.86F0.14 applied in PEMWEs requires only 1.63 V and maintains stable operation for over 100 h at 1 A cm–2. This work demonstrates a promising anion-modulated approach to the design of high-performance acidic OER catalysts.

DOI: 10.1021/jacs.5c08859

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.5c08859

期刊信息

JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:16.383
官方网址:https://pubs.acs.org/journal/jacsat
投稿链接:https://acsparagonplus.acs.org/psweb/loginForm?code=1000