Heteroatom dopants overcome the activity-stability trade-off in RuO2 for acidic oxygen evolution

IF 14.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Wei Zheng, Yang Zhao, Kang Jiang, Feng Xie, Linghu Meng, Shanqiang Gao, Jilong Li, Jiao Lan, Min Luo, Lifeng Liu, Yongwen Tan
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Abstract

The pursuit of RuO2 as an alternative acidic oxygen evolution reaction electrocatalyst to IrO2 holds great promise, yet simultaneously achieving highly active and stable RuO2 remains an urgent challenge, as conventional strategies often boost one property at the expense of the other. Here, we successfully construct Ta and B co-doped nanoporous RuO2 with Ru-O-Ta frameworks and Ru-O-B active sites to overcome the activity-stability trade-off. The Ru-O-Ta frameworks stabilize the Ru sites by mediating bridging oxygen and preferentially replenishing oxygen vacancies, thereby facilitating the oxygen evolution reaction through the adsorbate evolution mechanism. Concurrently, the Ru-O-Ta/B sites not only switch the rate-determining step but also lower the energy barriers, thereby enhancing catalytic activity. The Ta/B-RuO2 exhibits a low overpotential of 170 mV at 10 mA cm2, a favorable Tafel slope of 44 mV dec−1, and an outstanding durability. We demonstrate that proton-exchange membrane water electrolyzers equipped with Ta/B-RuO2 achieves a current density of 1.0 A cm−2 at a low voltage of 1.6 V and maintains stable operation for 120 h at 200 mA cm−2.

Abstract Image

杂原子掺杂物克服了RuO2中酸性析氧的活性-稳定性权衡
追求RuO2作为IrO2的酸性氧演化反应的替代电催化剂具有很大的前景,但同时实现高活性和稳定的RuO2仍然是一个紧迫的挑战,因为传统的策略往往以牺牲另一种性质为代价来提高一种性质。在这里,我们成功地构建了具有Ru-O-Ta框架和Ru-O-B活性位点的Ta和B共掺杂的纳米孔RuO2,以克服活性-稳定性的权衡。Ru- o - ta框架通过介导桥接氧和优先补充氧空位来稳定Ru位点,从而通过吸附物演化机制促进析氧反应。同时,Ru-O-Ta/B位点不仅改变了速率决定步骤,而且降低了能垒,从而提高了催化活性。Ta/B-RuO2在10 mA cm−2下的过电位为170 mV, Tafel斜率为44 mV dec−1,并且具有优异的耐久性。结果表明,在1.6 V的低电压下,Ta/B-RuO2的质子交换膜水电解槽电流密度可达1.0 a cm - 2,在200 mA cm - 2下可稳定运行120小时。
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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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