Mesoporous Single-Crystalline Particles as Robust and Efficient Acidic Oxygen Evolution Catalysts

IF 14.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of the American Chemical Society Pub Date : 2025-04-08 DOI:10.1021/jacs.4c18390

Yong Wang, Yunpu Qin, Sijia Liu, Yongzhi Zhao, Luan Liu, Di Zhang, Shangqing Zhao, Jianfang Liu, Jie Wang, Yadong Liu, Haoyang Wu, Baorui Jia, Xuanhui Qu, Hao Li, Mingli Qin

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Abstract

The scarcity of iridium (Ir) limits its widespread use in acidic oxygen evolution reaction (OER). Herein, mesoporous single-crystalline spinel Co₃O₄ with atomically dispersed low-valence-state Ir has been developed to enable Ir’s efficient and stable utilization. The surface Pourbaix diagram suggests that under acidic OER conditions, O* fully covers both Co₃O₄(111) and (110) surfaces, passivating Co sites but enhancing Co₃O₄’s structural stability, a benefit further improved by Ir doping. Mesopores offer numerous loading sites for Ir single atoms (13.8 wt %), which activate the originally O*-passivated Co₃O₄(111) surface by creating high-intrinsic-activity Co–Ir bridge sites; meanwhile, Ir and Co leaching rates are reduced to about 1/4 and 1/5, respectively, compared to conventional Ir/Co₃O₄ catalysts. Our catalyst exhibits a low η₁₀ of 248 mV for over 100 h, showcasing its potential in water electrolysis.

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介孔单晶颗粒作为强效酸性析氧催化剂

铱（Ir）的稀缺性限制了其在酸性析氧反应（OER）中的广泛应用。本文开发了具有原子分散低价态Ir的介孔单晶尖晶石Co3O4，以实现Ir的高效稳定利用。表面Pourbaix图表明，在酸性OER条件下，O*完全覆盖了Co3O4（111）和（110）表面，钝化了Co位点，增强了Co3O4的结构稳定性，通过Ir掺杂进一步提高了这一优势。介孔为Ir单原子提供了大量的加载位点（13.8 wt %），通过创建高本然活性的Co-Ir桥位，激活了原来O*钝化的Co3O4（111）表面；同时，与常规Ir/Co3O4催化剂相比，Ir和Co的浸出率分别降低到1/4和1/5左右。该催化剂的低η值为248mv，持续时间超过100 h，显示了其在水电解中的潜力。

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来源期刊

Journal of the American Chemical Society 化学-化学综合

CiteScore

24.40

自引率

6.00%

发文量

2398

审稿时长

1.6 months

期刊介绍： The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.