Atomic-level Ru-Ir mixing in rutile-type (RuIr)O2 for efficient and durable oxygen evolution catalysis

IF 14.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Yeji Park, Ho Yeon Jang, Tae Kyung Lee, Taekyung Kim, Doyeop Kim, Dongjin Kim, Hionsuck Baik, Jinwon Choi, Taehyun Kwon, Sung Jong Yoo, Seoin Back, Kwangyeol Lee
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Abstract

The success of proton exchange membrane water electrolysis (PEMWE) depends on active and robust electrocatalysts to facilitate oxygen evolution reaction (OER). Heteroatom-doped-RuOx has emerged as a promising electrocatalysts because heteroatoms suppress lattice oxygen participation in the OER, thereby preventing the destabilization of surface Ru and catalyst degradation. However, identifying suitable heteroatoms and achieving their atomic-scale coupling with Ru atoms are nontrivial tasks. Herein, to steer the reaction pathway away from the involvement of lattice oxygen, we integrate OER-active Ir atoms into the RuO2 matrix, which maximizes the synergy between stable Ru and active Ir centers, by leveraging the changeable growth behavior of Ru/Ir atoms on lattice parameter-modulated templates. In PEMWE, the resulting (RuIr)O2/C electrocatalysts demonstrate notable current density of 4.96 A cm−2 and mass activity of 19.84 A mgRu+Ir−1 at 2.0 V. In situ spectroscopic analysis and computational calculations highlight the importance of the synergistic coexistence of Ru/Ir-dual-OER-active sites for mitigating Ru dissolution via the optimization of the binding energy with oxygen intermediates and stabilization of Ru sites.

Abstract Image

原子级Ru-Ir在金红石型(RuIr)O2中的混合,用于高效持久的析氧催化
质子交换膜水电解(PEMWE)的成功取决于活性和稳健的电催化剂来促进析氧反应(OER)。杂原子掺杂的钌已经成为一种很有前途的电催化剂,因为杂原子抑制了OER中晶格氧的参与,从而防止了表面钌的不稳定和催化剂的降解。然而,寻找合适的杂原子并实现它们与钌原子的原子尺度耦合是一项艰巨的任务。为了使反应途径远离晶格氧的参与,我们利用Ru/Ir原子在晶格参数调制模板上的可变生长行为,将oer活性Ir原子集成到RuO2矩阵中,从而最大限度地发挥稳定Ru和活性Ir中心之间的协同作用。在PEMWE中,得到的(RuIr)O2/C电催化剂在2.0 V时具有4.96 A cm−2的电流密度和19.84 A mgRu+Ir−1的质量活性。原位光谱分析和计算计算强调了Ru/ ir -双oer活性位点协同共存的重要性,通过优化与氧中间体的结合能和稳定Ru位点来减轻Ru的溶解。
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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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