Engineering the electronic structure of single atom Ru sites via compressive strain boosts acidic water oxidation electrocatalysis

Yancai Yao; Sulei Hu; Wenxing Chen; Zheng Qing Huang; Weichen Wei; Tao Yao; Ruirui Liu; Ketao Zang; Xiaoqian Wang; Geng Wu; Wenjuan Yuan; Tongwei Yuan; Baiquan Zhu; Wei Liu; Zhijun Li; Dongsheng He; Zhenggang Xue; Yu Wang; Xusheng Zheng; Juncai Dong; Chun Ran Chang; Yanxia Chen; Xun Hong; Jun Luo; Shiqiang Wei; Wei Xue Li; Peter Strasser; Yuen Wu; Yadong Li

doi:10.1038/s41929-019-0246-2

Engineering the electronic structure of single atom Ru sites via compressive strain boosts acidic water oxidation electrocatalysis

Yancai Yao, Sulei Hu, Wenxing Chen, Zheng Qing Huang, Weichen Wei, Tao Yao, Ruirui Liu, Ketao Zang, Xiaoqian Wang, Geng Wu, Wenjuan Yuan, Tongwei Yuan, Baiquan Zhu, Wei Liu, Zhijun Li, Dongsheng He, Zhenggang Xue, Yu Wang, Xusheng Zheng, Juncai DongChun Ran Chang, Yanxia Chen, Xun Hong, Jun Luo, Shiqiang Wei, Wei Xue Li^*, Peter Strasser, Yuen Wu, Yadong Li

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

858 Citations (Scopus)

Abstract

Single-atom precious metal catalysts hold the promise of perfect atom utilization, yet control of their activity and stability remains challenging. Here we show that engineering the electronic structure of atomically dispersed Ru ₁ on metal supports via compressive strain boosts the kinetically sluggish electrocatalytic oxygen evolution reaction (OER), and mitigates the degradation of Ru-based electrocatalysts in an acidic electrolyte. We construct a series of alloy-supported Ru ₁ using different PtCu alloys through sequential acid etching and electrochemical leaching, and find a volcano relation between OER activity and the lattice constant of the PtCu alloys. Our best catalyst, Ru ₁ –Pt ₃ Cu, delivers 90 mV lower overpotential to reach a current density of 10 mA cm ⁻² , and an order of magnitude longer lifetime over that of commercial RuO ₂ . Density functional theory investigations reveal that the compressive strain of the Pt _skin shell engineers the electronic structure of the Ru ₁ , allowing optimized binding of oxygen species and better resistance to over-oxidation and dissolution.

Original language	English
Pages (from-to)	304-313
Number of pages	10
Journal	Nature Catalysis
Volume	2
Issue number	4
DOIs	https://doi.org/10.1038/s41929-019-0246-2
Publication status	Published - 1 Apr 2019
Externally published	Yes

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Yao, Y., Hu, S., Chen, W., Huang, Z. Q., Wei, W., Yao, T., Liu, R., Zang, K., Wang, X., Wu, G., Yuan, W., Yuan, T., Zhu, B., Liu, W., Li, Z., He, D., Xue, Z., Wang, Y., Zheng, X., ... Li, Y. (2019). Engineering the electronic structure of single atom Ru sites via compressive strain boosts acidic water oxidation electrocatalysis. Nature Catalysis, 2(4), 304-313. https://doi.org/10.1038/s41929-019-0246-2

@article{5221e15f1a1e45378a3864cd72f55b45,

title = "Engineering the electronic structure of single atom Ru sites via compressive strain boosts acidic water oxidation electrocatalysis",

abstract = " Single-atom precious metal catalysts hold the promise of perfect atom utilization, yet control of their activity and stability remains challenging. Here we show that engineering the electronic structure of atomically dispersed Ru 1 on metal supports via compressive strain boosts the kinetically sluggish electrocatalytic oxygen evolution reaction (OER), and mitigates the degradation of Ru-based electrocatalysts in an acidic electrolyte. We construct a series of alloy-supported Ru 1 using different PtCu alloys through sequential acid etching and electrochemical leaching, and find a volcano relation between OER activity and the lattice constant of the PtCu alloys. Our best catalyst, Ru 1 –Pt 3 Cu, delivers 90 mV lower overpotential to reach a current density of 10 mA cm −2 , and an order of magnitude longer lifetime over that of commercial RuO 2 . Density functional theory investigations reveal that the compressive strain of the Pt skin shell engineers the electronic structure of the Ru 1 , allowing optimized binding of oxygen species and better resistance to over-oxidation and dissolution.",

author = "Yancai Yao and Sulei Hu and Wenxing Chen and Huang, {Zheng Qing} and Weichen Wei and Tao Yao and Ruirui Liu and Ketao Zang and Xiaoqian Wang and Geng Wu and Wenjuan Yuan and Tongwei Yuan and Baiquan Zhu and Wei Liu and Zhijun Li and Dongsheng He and Zhenggang Xue and Yu Wang and Xusheng Zheng and Juncai Dong and Chang, {Chun Ran} and Yanxia Chen and Xun Hong and Jun Luo and Shiqiang Wei and Li, {Wei Xue} and Peter Strasser and Yuen Wu and Yadong Li",

note = "Publisher Copyright: {\textcopyright} 2019, The Author(s), under exclusive licence to Springer Nature Limited.",

year = "2019",

month = apr,

day = "1",

doi = "10.1038/s41929-019-0246-2",

language = "English",

volume = "2",

pages = "304--313",

journal = "Nature Catalysis",

issn = "2520-1158",

publisher = "Nature Publishing Group",

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Yao, Y, Hu, S, Chen, W, Huang, ZQ, Wei, W, Yao, T, Liu, R, Zang, K, Wang, X, Wu, G, Yuan, W, Yuan, T, Zhu, B, Liu, W, Li, Z, He, D, Xue, Z, Wang, Y, Zheng, X, Dong, J, Chang, CR, Chen, Y, Hong, X, Luo, J, Wei, S, Li, WX, Strasser, P, Wu, Y & Li, Y 2019, 'Engineering the electronic structure of single atom Ru sites via compressive strain boosts acidic water oxidation electrocatalysis', Nature Catalysis, vol. 2, no. 4, pp. 304-313. https://doi.org/10.1038/s41929-019-0246-2

TY - JOUR

T1 - Engineering the electronic structure of single atom Ru sites via compressive strain boosts acidic water oxidation electrocatalysis

AU - Yao, Yancai

AU - Hu, Sulei

AU - Chen, Wenxing

AU - Huang, Zheng Qing

AU - Wei, Weichen

AU - Yao, Tao

AU - Liu, Ruirui

AU - Zang, Ketao

AU - Wang, Xiaoqian

AU - Wu, Geng

AU - Yuan, Wenjuan

AU - Yuan, Tongwei

AU - Zhu, Baiquan

AU - Liu, Wei

AU - Li, Zhijun

AU - He, Dongsheng

AU - Xue, Zhenggang

AU - Wang, Yu

AU - Zheng, Xusheng

AU - Dong, Juncai

AU - Chang, Chun Ran

AU - Chen, Yanxia

AU - Hong, Xun

AU - Luo, Jun

AU - Wei, Shiqiang

AU - Li, Wei Xue

AU - Strasser, Peter

AU - Wu, Yuen

AU - Li, Yadong

PY - 2019/4/1

Y1 - 2019/4/1

N2 - Single-atom precious metal catalysts hold the promise of perfect atom utilization, yet control of their activity and stability remains challenging. Here we show that engineering the electronic structure of atomically dispersed Ru 1 on metal supports via compressive strain boosts the kinetically sluggish electrocatalytic oxygen evolution reaction (OER), and mitigates the degradation of Ru-based electrocatalysts in an acidic electrolyte. We construct a series of alloy-supported Ru 1 using different PtCu alloys through sequential acid etching and electrochemical leaching, and find a volcano relation between OER activity and the lattice constant of the PtCu alloys. Our best catalyst, Ru 1 –Pt 3 Cu, delivers 90 mV lower overpotential to reach a current density of 10 mA cm −2 , and an order of magnitude longer lifetime over that of commercial RuO 2 . Density functional theory investigations reveal that the compressive strain of the Pt skin shell engineers the electronic structure of the Ru 1 , allowing optimized binding of oxygen species and better resistance to over-oxidation and dissolution.

AB - Single-atom precious metal catalysts hold the promise of perfect atom utilization, yet control of their activity and stability remains challenging. Here we show that engineering the electronic structure of atomically dispersed Ru 1 on metal supports via compressive strain boosts the kinetically sluggish electrocatalytic oxygen evolution reaction (OER), and mitigates the degradation of Ru-based electrocatalysts in an acidic electrolyte. We construct a series of alloy-supported Ru 1 using different PtCu alloys through sequential acid etching and electrochemical leaching, and find a volcano relation between OER activity and the lattice constant of the PtCu alloys. Our best catalyst, Ru 1 –Pt 3 Cu, delivers 90 mV lower overpotential to reach a current density of 10 mA cm −2 , and an order of magnitude longer lifetime over that of commercial RuO 2 . Density functional theory investigations reveal that the compressive strain of the Pt skin shell engineers the electronic structure of the Ru 1 , allowing optimized binding of oxygen species and better resistance to over-oxidation and dissolution.

UR - http://www.scopus.com/inward/record.url?scp=85062831689&partnerID=8YFLogxK

U2 - 10.1038/s41929-019-0246-2

DO - 10.1038/s41929-019-0246-2

M3 - Article

AN - SCOPUS:85062831689

SN - 2520-1158

VL - 2

SP - 304

EP - 313

JO - Nature Catalysis

JF - Nature Catalysis

IS - 4

ER -

Engineering the electronic structure of single atom Ru sites via compressive strain boosts acidic water oxidation electrocatalysis

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