NiCoS x@Cobalt Carbonate Hydroxide Obtained by Surface Sulfurization for Efficient and Stable Hydrogen Evolution at Large Current Densities

Xian Zhang; Renji Zheng; Mengtian Jin; Run Shi; Zhong Ai; Abbas Amini; Qing Lian; Chun Cheng; Shaoxian Song

doi:10.1021/acsami.1c07504

NiCoS _x@Cobalt Carbonate Hydroxide Obtained by Surface Sulfurization for Efficient and Stable Hydrogen Evolution at Large Current Densities

ACS Appl Mater Interfaces. 2021 Aug 4;13(30):35647-35656. doi: 10.1021/acsami.1c07504. Epub 2021 Jul 20.

Authors

Xian Zhang¹, Renji Zheng^{1

2}, Mengtian Jin³, Run Shi³, Zhong Ai¹, Abbas Amini⁴, Qing Lian³, Chun Cheng^{3

5

6}, Shaoxian Song¹

Affiliations

¹ School of Resources and Environmental Engineering and Hubei Key Laboratory of Mineral Resources Processing and Environment, Wuhan University of Technology, Luoshi Road 122, Wuhan, Hubei 430070, China.
² School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China.
³ Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, P. R. China.
⁴ Center for Infrastructure Engineering, Western Sydney University, Kingswood, New South Wales 2751, Australia.
⁵ Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Southern University of Science and Technology, Shenzhen 518055, P. R. China.
⁶ Key Laboratory of Energy Conversion and Storage Technologies (Southern University of Science and Technology), Ministry of Education, Shenzhen 518055, China.

PMID: 34283575
DOI: 10.1021/acsami.1c07504

Abstract

Developing earth-abundant, active, and stable electrocatalysts for hydrogen evolution reactions (HERs) at large current densities has remained challenging. Herein, heterostructured nickel foam-supported cobalt carbonate hydroxide nanoarrays embellished with NiCoS_x nanoflakes (NiCoS_x@CoCH NAs/NF) are designed via room-temperature sulfurization, which can drive 10 and 1000 mA cm^-2 at low overpotentials of 55 and 438 mV for HER and exhibit impressive long-term stability at the industrial-level current density. Surprisingly, NiCoS_x@CoCH NAs/NF after a 500 h stability test at 500 mA cm^-2 exhibit better catalytic performance than the initial one at high current densities. Simulations showed that NiCoS_x@CoCH NAs have an optimized hydrogen adsorption free energy (ΔG_H*) of 0.02 eV, owing to the synergistic effect of CoCH (ΔG_H* = 1.36 eV) and NiCoS_x (ΔG_H* = 0.03 eV). The electric field at the heterostructure interface leads to electron transport from CoCH to NiCoS_x, which enhances HER dynamics. The hierarchical nanostructure has a large specific area and a superaerophobic surface, which are beneficial to hydrogen generation/release for efficient and stable HER.

Keywords: cobalt carbonate hydroxide; hydrogen evolution reaction; large current density; long-term stability; surface sulfurization.