Single-atom Co dispersed on polyoxometalate derivatives confined in bamboo-like carbon nanotubes enabling efficient dual-site lattice oxygen mediated oxygen evolution electrocatalysis for acidic water electrolyzers

Jianyun Liu; Tanyuan Wang; Zijie Lin; Mengyi Liao; Shuxia Liu; Shiyu Wang; Zhao Cai; Hao Sun; Yue Shen; Yunhui Huang; Qing Li

doi:10.1039/D4EE00173G

Single-atom Co dispersed on polyoxometalate derivatives confined in bamboo-like carbon nanotubes enabling efficient dual-site lattice oxygen mediated oxygen evolution electrocatalysis for acidic water electrolyzers†

Jianyun Liu,^a Tanyuan Wang,

*^a Zijie Lin,^a Mengyi Liao,^a Shuxia Liu,^a Shiyu Wang,^a Zhao Cai,

^b Hao Sun,^c Yue Shen,

^a Yunhui Huang

^a and Qing Li

*^a

Author affiliations

* Corresponding authors

^a State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei 430074, China
E-mail: wangty@hust.edu.cn, qing_li@hust.edu.cn

^b Faculty of Materials Science and Chemistry, China University of Geosciences (Wuhan), Wuhan 430074, China

^c Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, and Zhangjiang Institute for Advanced Study, Shanghai Jiao Tong University, Shanghai 200240, China

Abstract

The development of efficient and durable earth-abundant electrocatalysts for the acidic oxygen evolution reaction (OER) is crucial for the large-scale application of proton exchange membrane water electrolyzers (PEMWEs). Here, we report a novel amorphous Mo–Ce oxide supported single-atom Co (Co_SA-MoCeO_x) encapsulated in bamboo-like carbon nanotubes (BCTs) catalysts for the acidic OER. Operando X-ray absorption spectroscopy confirms that the Mo–Ce oxide can promote the transformation of Co²⁺ sites into Co³⁺–O sites with lower coordination number and abundant oxygen vacancies at a low voltage, leading to a dual-metal-site lattice oxygen-mediated (LOM) pathway with fast OER kinetics. Moreover, the confinement effect of BCTs on Co_SA-MoCeO_x can reduce the direct contact between the catalyst and the acid, thus improving its corrosion resistance. The optimized catalyst exhibits a low overpotential of 239 mV for the OER at 10 mA cm⁻² in 0.5 M H₂SO₄ and maintains exceptional stability for more than 60 hours in PEMWEs, representing one of the best non-noble metal catalysts. Density functional theory calculations show that the strong interaction between single-atom Co sites and Mo–Ce oxide reduces the adsorption energy barrier of the LOM pathway from 1.60 eV to 1.08 eV, and inhibits the dissolution of the support with the increased vacancy formation energy of Mo, thus improving the OER activity and stability of the catalyst in acid.

Energy & Environmental Science

Single-atom Co dispersed on polyoxometalate derivatives confined in bamboo-like carbon nanotubes enabling efficient dual-site lattice oxygen mediated oxygen evolution electrocatalysis for acidic water electrolyzers†

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Single-atom Co dispersed on polyoxometalate derivatives confined in bamboo-like carbon nanotubes enabling efficient dual-site lattice oxygen mediated oxygen evolution electrocatalysis for acidic water electrolyzers

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