Inducing oxygen deficiencies through amorphization in IrMoOx: A pathway to highly efficient acidicwater oxidation and water splitting

IF 8.1 2区工程技术 Q1 CHEMISTRY, PHYSICAL

International Journal of Hydrogen Energy Pub Date : 2025-05-12 DOI:10.1016/j.ijhydene.2025.04.494

Xiang Li , Zhiqiang Wang , Hui Li , Fengchi Wu , Dongzhi Li , Zixiang Su , Longtao Zhang , Shanyan Jiao , Hehe Wei , Xue-Qing Gong

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引用次数: 0

Abstract

Despite the considerable potential of acidic proton exchange membrane water electrolyzers (PEMWEs) for cost-efficient hydrogen production, their acidic oxygen evolution reaction (OER) kinetics are dramatically more sluggish than that in alkaline, causing inferior activity and stability. Herein, we successfully synthesize the amorphous IrMoO_x catalyst, featuring disordered structure, oxygen deficiencies and an increased oxidation state of Ir species compared with commercial IrO₂. The amorphous IrMoO_x catalyst demonstrates exceptional bifunctional catalytic activities and durability in both hydrogen evolution reaction (HER) and OER in acid, accompanied with the ultralow overpotentials (29 and 235 mV) for the 10 mA cm⁻², respectively. Theoretical calculations reveal the existence of special IrO₄ planar structure within the amorphous IrMoO_x and illustrate that the introduced Mo and rich oxygen vacancies optimize d-band of metal species, thereby tuning rate-determining step and enhancing OER performances compared with commercial IrO₂. Furthermore, the IrMoO_x || IrMoO_x catalyst delivers the current density of 10 mV cm⁻² at ultralow voltage of 1.55 V, outperforming the commercial Pt/C || IrO₂ (1.76 V).

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在IrMoOx中通过非晶化诱导缺氧：一种高效酸水氧化和水分解的途径

尽管酸性质子交换膜水电解槽（PEMWEs）在经济高效制氢方面具有相当大的潜力，但其酸性析氧反应（OER）动力学显著低于碱性，导致活性和稳定性较差。本文中，我们成功地合成了无定形的IrMoOx催化剂，与商业IrO2相比，它具有结构无序、氧缺乏和Ir物种氧化态增加的特点。无定形IrMoOx催化剂在酸中析氢反应（HER）和析氢反应（OER）中表现出优异的双功能催化活性和耐久性，并在10 mA cm−2下分别具有超低过电位（29和235 mV）。理论计算表明，在非晶imoox中存在特殊的IrO4平面结构，并说明引入的Mo和富氧空位优化了金属物种的d波段，从而调整了速率决定步骤，与商业IrO2相比提高了OER性能。此外，IrMoOx || IrMoOx催化剂在1.55 V的超低电压下可提供10 mV cm - 2的电流密度，优于商用Pt/C || IrO2 （1.76 V）。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

International Journal of Hydrogen Energy 工程技术-环境科学

CiteScore

13.50

自引率

25.00%

发文量

3502

审稿时长

60 days

期刊介绍： The objective of the International Journal of Hydrogen Energy is to facilitate the exchange of new ideas, technological advancements, and research findings in the field of Hydrogen Energy among scientists and engineers worldwide. This journal showcases original research, both analytical and experimental, covering various aspects of Hydrogen Energy. These include production, storage, transmission, utilization, enabling technologies, environmental impact, economic considerations, and global perspectives on hydrogen and its carriers such as NH3, CH4, alcohols, etc. The utilization aspect encompasses various methods such as thermochemical (combustion), photochemical, electrochemical (fuel cells), and nuclear conversion of hydrogen, hydrogen isotopes, and hydrogen carriers into thermal, mechanical, and electrical energies. The applications of these energies can be found in transportation (including aerospace), industrial, commercial, and residential sectors.