Effective electronic tuning of Pt single atoms via heterogeneous atomic coordination of (Co,Ni)(OH)2 for efficient hydrogen evolution

An Pei; Ruikuan Xie; Yun Zhang; Yingliang Feng; Weizhen Wang; Sifan Zhang; Zinan Huang; Lihua Zhu; Guoliang Chai; Zhiqing Yang; Qingsheng Gao; Hengqiang Ye; Congxiao Shang; Bing Hui Chen; Zhengxiao Guo

doi:10.1039/D2EE02785B

Effective electronic tuning of Pt single atoms via heterogeneous atomic coordination of (Co,Ni)(OH)₂ for efficient hydrogen evolution†

An Pei,‡^a Ruikuan Xie,

‡^c Yun Zhang,‡^a Yingliang Feng,‡^a Weizhen Wang,^d Sifan Zhang,^a Zinan Huang,^e Lihua Zhu,

*^ab Guoliang Chai,

*^cg Zhiqing Yang,*^d Qingsheng Gao,

^e Hengqiang Ye,^d Congxiao Shang,^b Bing Hui Chen

^f and Zhengxiao Guo

*^b

Author affiliations

* Corresponding authors

^a Jiangxi Provincial Key Laboratory of Functional Molecular Materials Chemistry, College of Chemistry and Chemical Engineering, Faculty of Materials Metallurgy and Chemistry, Jiangxi University of Science and Technology, Ganzhou 341000, Jiang Xi, China
E-mail: zhulihua@jxust.edu.cn

^b HKU-CAS Joint Laboratory on New Materials and Department of Chemistry, The University of Hong Kong, Hong Kong SAR, China
E-mail: zxguo@hku.hk

^c State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences (CAS), Fuzhou, 350002 Fujian, China
E-mail: g.chai@fjirsm.ac.cn

^d Ji Hua Laboratory, Foshan 528200, China
E-mail: yangzhq@jihualab.ac.cn

^e College of Chemistry and Materials Science, and Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications, Jinan University, Guangzhou 510632, China

^f College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China

^g Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou, Fujian 350108, P. R. China

Abstract

Hydroxide-supported atomic structures, particularly single atoms, offer a wide scope for active microenvironmental tuning to enhance the catalytic performance, but little has been explored on the electronic synergy between mono- and dual-hydroxides. Here, we propose a way of constructing a Pt₁/(Co,Ni)(OH)₂/C single-atom catalyst (SAC), with Pt single-atoms, Pt₁, stabilized and anchored on the surface of defective (Co,Ni)(OH)₂, which is further supported on carbon black. This catalyst exhibits a far superior hydrogen evolution reaction (HER) activity to Pt₁/Co(OH)₂/C, Pt₁/Ni(OH)₂/C, Pt₁/C, and the commercial 20 wt% Pt/C. Particularly, it shows an almost zero onset overpotential and an outstanding electrocatalytic mass activity for the HER, 29.7 times higher than that of Pt₁/C and 115.9 times higher than that of the commercial 20 wt% Pt/C at −0.09 V vs. RHE, respectively. There is negligible attenuation after the chronopotentiometry test at 100 mA cm⁻² for 24 h and cyclic voltammetry for 20 000 cycles. Operando Raman spectra clarified that the Volmer step for water decomposition (the H–OH bond breaking) takes place around the defective sites of (Co,Ni)(OH)₂. Density functional theory (DFT) calculations confirmed the electronic synergy between the Pt single atoms and bimetallic (Co,Ni)(OH)₂, which leads to stable anchoring of Pt and yields an appropriate adsorption energy of *H, leading to rapid H₂ generation.

Energy & Environmental Science

Effective electronic tuning of Pt single atoms via heterogeneous atomic coordination of (Co,Ni)(OH)₂ for efficient hydrogen evolution†

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Effective electronic tuning of Pt single atoms via heterogeneous atomic coordination of (Co,Ni)(OH)₂ for efficient hydrogen evolution

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