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用于高效析氧的异质单原子中的位点特异性协同作用。

Site-specific synergy in heterogeneous single atoms for efficient oxygen evolution.

作者信息

Ma Peiyu, Xue Jiawei, Li Ji, Cao Heng, Wang Ruyang, Zuo Ming, Zhang Zhirong, Bao Jun

机构信息

National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui, PR China.

Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, PR China.

出版信息

Nat Commun. 2025 Mar 15;16(1):2573. doi: 10.1038/s41467-025-57864-w.

Abstract

Heterogeneous single-atom systems demonstrate potential to break performance limitations of single-atom catalysts through synergy interactions. The synergy in heterogeneous single atoms strongly dependes on their anchoring sites. Herein, we reveal the site-specific synergy in heterogeneous single atoms for oxygen evolution. The RuIr/CoOOH is fabricated by anchoring Ru single atoms onto three-fold facial center cubic hollow sites and Ir single atoms onto oxygen vacancy sites on CoOOH. Moreover, IrRu/CoOOH is also prepared by switching the anchoring sites of single atoms. Electrochemical measurements demonstrate the RuIr/CoOOH exhibits enhanced OER performance compared to IrRu/CoOOH. In-situ spectroscopic and mechanistic studies indicate that Ru single atoms at three-fold facial center cubic hollow sites serve as adsorption sites for key reaction intermediates, while Ir single atoms at oxygen vacancy sites stabilize the *OOH intermediates via hydrogen bonding interactions. This work discloses the correlation between the synergy in heterogeneous single atoms and their anchoring sites.

摘要

异质单原子体系显示出通过协同相互作用打破单原子催化剂性能限制的潜力。异质单原子中的协同作用在很大程度上取决于它们的锚定位点。在此,我们揭示了异质单原子在析氧过程中的位点特异性协同作用。通过将Ru单原子锚定在面心立方中空三位点上,以及将Ir单原子锚定在CoOOH的氧空位上,制备了RuIr/CoOOH。此外,还通过切换单原子的锚定位点制备了IrRu/CoOOH。电化学测量表明,与IrRu/CoOOH相比,RuIr/CoOOH表现出增强的析氧反应性能。原位光谱和机理研究表明,面心立方中空三位点上的Ru单原子作为关键反应中间体的吸附位点,而氧空位上的Ir单原子通过氢键相互作用稳定*OOH中间体。这项工作揭示了异质单原子中的协同作用与其锚定位点之间的相关性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6587/11910543/503abb3296d3/41467_2025_57864_Fig1_HTML.jpg

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