Constructing abundant 5d electron buffering interfaces for enhancing acidic water oxidation†

IF 9.5 2区 材料科学 Q1 CHEMISTRY, PHYSICAL
Jingqiu Shang, Xiuxiu Zhang, Youcai Che, Xupeng Qin, Yuhao Zhang, Jing Zhang, Baojie Li, Chenyu Yang, Yaling Jiang, Xiangang Lin and Qinghua Liu
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Abstract

The development of Ru-based acidic oxygen evolution reaction (OER) catalysts is crucial for enhancing the efficiency of electric-driven water electrolysis, yet their stability remains constrained by the susceptibility of Ru active centers to dissolution and over-oxidation. In this work, a Ru/Ta2O5(V) catalyst with abundant 5d electron buffering interfaces was fabricated by an oxide defect separation strategy. Through strong metal–support interactions to modulate the electronic structure of Ru active sites, we effectively balance the trade-off between catalytic activity and stability. The optimized Ru/Ta2O5(V) demonstrates a low overpotential of 272 mV at 10 mA cm−2 and maintains stable operation for 190 hours with an ultralow voltage increment rate. In situ infrared spectroscopy and X-ray photoelectron spectroscopy reveal that the anchoring of Ru on the support surface modulates the electron cloud density around Ru sites via Ta 5d electrons, which not only optimizes the reaction pathway but also significantly improves the corrosion resistance in acidic environments, effectively mitigating the dissolution and excessive oxidation of active sites during the OER process. This work proposes a novel structural design strategy for achieving stable acidic OER catalysis through rational Ru immobilization on inert supports.

Abstract Image

构建丰富的5d电子缓冲界面,增强酸性水的氧化作用
钌基酸性析氧反应(OER)催化剂的开发对于提高电驱动水电解效率至关重要,但其稳定性仍然受到钌活性中心对溶解和过度氧化的敏感性的限制。本文采用氧化物缺陷分离策略制备了具有丰富5d电子缓冲界面的Ru/Ta2O5(V)催化剂。通过强大的金属支持相互作用来调节Ru活性位点的电子结构,我们有效地平衡了催化活性和稳定性之间的权衡。优化后的Ru/Ta2O5(V)在10 mA cm−2下具有272 mV的低过电位,并能以超低的电压增量率稳定工作190小时。原位红外光谱和x射线光电子能谱分析表明,Ru在载体表面的锚定通过Ta 5d电子调节了Ru位点周围的电子云密度,不仅优化了反应途径,而且显著提高了酸性环境下的耐腐蚀性,有效减轻了OER过程中活性位点的溶解和过度氧化。这项工作提出了一种新的结构设计策略,通过在惰性载体上合理地固定Ru来实现稳定的酸性OER催化。
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来源期刊
Journal of Materials Chemistry A
Journal of Materials Chemistry A CHEMISTRY, PHYSICAL-ENERGY & FUELS
CiteScore
19.50
自引率
5.00%
发文量
1892
审稿时长
1.5 months
期刊介绍: The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.
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