Ni-O4 as Active Sites for Efficient Oxygen Evolution Reaction with Electronic Metal-Support Interactions

Zhang-Hong Zhou; Wei-Hang Li; Zhen Zhang; Qing-Song Huang; Xiao-Chong Zhao; Wei Cao

doi:10.1021/acsami.2c11201

Ni-O₄ as Active Sites for Efficient Oxygen Evolution Reaction with Electronic Metal-Support Interactions

ACS Appl Mater Interfaces. 2022 Oct 26;14(42):47542-47548. doi: 10.1021/acsami.2c11201. Epub 2022 Oct 13.

Authors

Zhang-Hong Zhou^{1

2}, Wei-Hang Li², Zhen Zhang², Qing-Song Huang¹, Xiao-Chong Zhao², Wei Cao²

Affiliations

¹ School of Chemical Engineering, Sichuan University, Chengdu610065, P.R. China.
² Institute of Materials, China Academy of Engineering Physics, Jiangyou621908, China.

PMID: 36228176
DOI: 10.1021/acsami.2c11201

Abstract

Precise adjustment of the metal site structure in single-atom catalysts (SACs) plays a key role in addressing the oxygen evolution reaction (OER). Herein, we report the synthesis of O-doped Ni SACs anchored on porous graphene-like carbon (Ni-O-G) using molten salts (ZnCl₂ and NaCl) as templates, in which the unique Ni-O₄ structure serves as the active sites. Ni-O-G, with an overpotential of only 238 mV (@ 10 mA cm^-2), is one of the more advanced catalysts. An array of characterizations and density functional theory calculations show that the Ni-O₄ coordination enables Ni to be closer to the Fermi level compared to traditional Ni-N₄, enhancing the electronic metal-support interaction to facilitate OER kinetics. Thus, this work offers an alternative strategy for the structural modulation of Ni SACs and the effect of different coordination elements with the same atomic coordination structure on the intrinsic OER activity.

Keywords: Ni−O4 coordination structure; O-doped Ni single-atom catalysis; electronic metal−support interaction; molten salt templates; oxygen evolution reaction; porous carbon support.