Dynamic rhenium dopant boosts ruthenium oxide for durable oxygen evolution

Huanyu Jin; Xinyan Liu; Pengfei An; Cheng Tang; Huimin Yu; Qinghua Zhang; Hong-Jie Peng; Lin Gu; Yao Zheng; Taeseup Song; Kenneth Davey; Ungyu Paik; Juncai Dong; Shi-Zhang Qiao

doi:10.1038/s41467-023-35913-6

Dynamic rhenium dopant boosts ruthenium oxide for durable oxygen evolution

Nat Commun. 2023 Jan 21;14(1):354. doi: 10.1038/s41467-023-35913-6.

Authors

Huanyu Jin^#^{1

2}, Xinyan Liu^#³, Pengfei An⁴, Cheng Tang¹, Huimin Yu⁵, Qinghua Zhang⁶, Hong-Jie Peng³, Lin Gu⁶, Yao Zheng¹, Taeseup Song⁷, Kenneth Davey¹, Ungyu Paik⁷, Juncai Dong⁸, Shi-Zhang Qiao⁹

Affiliations

¹ School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA, 5005, Australia.
² Institute for Sustainability, Energy and Resources, The University of Adelaide, Adelaide, SA, 5005, Australia.
³ Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu, 611731, Sichuan, China.
⁴ Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, China.
⁵ Future Industries Institute, University of South Australia, Mawson Lakes Campus, Adelaide, SA, 5095, Australia.
⁶ Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, China.
⁷ Department of Energy Engineering, Hanyang University, Seoul, 04763, Republic of Korea.
⁸ Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, China. dongjc@ihep.ac.cn.
⁹ School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA, 5005, Australia. s.qiao@adelaide.edu.au.

^# Contributed equally.

Abstract

Heteroatom-doping is a practical means to boost RuO₂ for acidic oxygen evolution reaction (OER). However, a major drawback is conventional dopants have static electron redistribution. Here, we report that Re dopants in Re_0.06Ru_0.94O₂ undergo a dynamic electron accepting-donating that adaptively boosts activity and stability, which is different from conventional dopants with static dopant electron redistribution. We show Re dopants during OER, (1) accept electrons at the on-site potential to activate Ru site, and (2) donate electrons back at large overpotential and prevent Ru dissolution. We confirm via in situ characterizations and first-principle computation that the dynamic electron-interaction between Re and Ru facilitates the adsorbate evolution mechanism and lowers adsorption energies for oxygen intermediates to boost activity and stability of Re_0.06Ru_0.94O₂. We demonstrate a high mass activity of 500 A g_cata.^-1 (7811 A g_Re-Ru^-1) and a high stability number of S-number = 4.0 × 10⁶ n_oxygen n_Ru^-1 to outperform most electrocatalysts. We conclude that dynamic dopants can be used to boost activity and stability of active sites and therefore guide the design of adaptive electrocatalysts for clean energy conversions.

MeSH terms

Adsorption
Oxides
Oxygen
Rhenium*
Ruthenium*

Substances

Rhenium
Ruthenium
Oxides
Oxygen