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Vol. 15 (2023)

Immobilization of Oxyanions on the Reconstructed Heterostructure Evolved from a Bimetallic Oxysulfide for the Promotion of Oxygen Evolution Reaction

https://doi.org/10.1007/s40820-023-01164-9
Kai Yu
Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon‑Based Functional Materials and Devices, Joint International Research Laboratory of Carbon‑Based Functional Materials and Devices, Soochow University, Suzhou 215123, People’s Republic of China
Hongyuan Yang
Department of Chemistry: Metalorganics and Inorganic Materials, Technical University of Berlin, Straße Des 17 Juni 135. Sekr. C2, 10623 Berlin, Germany
Hao Zhang
Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon‑Based Functional Materials and Devices, Joint International Research Laboratory of Carbon‑Based Functional Materials and Devices, Soochow University, Suzhou 215123, People’s Republic of China
Hui Huang
Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon‑Based Functional Materials and Devices, Joint International Research Laboratory of Carbon‑Based Functional Materials and Devices, Soochow University, Suzhou 215123, People’s Republic of China
Zhaowu Wang
School of Physics and Engineering, Longmen Laboratory, Henan University of Science and Technology, Luoyang 471023, People’s Republic of China
Zhenhui Kang
Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon‑Based Functional Materials and Devices, Joint International Research Laboratory of Carbon‑Based Functional Materials and Devices, Soochow University, Suzhou 215123, People’s Republic of China
Yang Liu
Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon‑Based Functional Materials and Devices, Joint International Research Laboratory of Carbon‑Based Functional Materials and Devices, Soochow University, Suzhou 215123, People’s Republic of China
Prashanth W. Menezes
Department of Chemistry: Metalorganics and Inorganic Materials, Technical University of Berlin, Straße Des 17 Juni 135. Sekr. C2, 10623 Berlin, Germany
Ziliang Chen
Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon‑Based Functional Materials and Devices, Joint International Research Laboratory of Carbon‑Based Functional Materials and Devices, Soochow University, Suzhou 215123, People’s Republic of China

Corresponding Author: Ziliang Chen

zlchen@suda.edu.cn

Nano-Micro Letters, Vol. 15 (2023), Article Number: 186

Abstract

Efficient and durable oxygen evolution reaction (OER) requires the electrocatalyst to bear abundant active sites, optimized electronic structure as well as robust component and mechanical stability. Herein, a bimetallic lanthanum-nickel oxysulfide with rich oxygen vacancies based on the La2O2S prototype is fabricated as a binder-free precatalyst for alkaline OER. The combination of advanced in situ and ex situ characterizations with theoretical calculation uncovers the synergistic effect among La, Ni, O, and S species during OER, which assures the adsorption and stabilization of the oxyanion (SO42−) onto the surface of the deeply reconstructed porous heterostructure composed of confining NiOOH nanodomains by La(OH)3 barrier. Such coupling, confinement, porosity and immobilization enable notable improvement in active site accessibility, phase stability, mass diffusion capability and the intrinsic Gibbs free energy of oxygen-containing intermediates. The optimized electrocatalyst delivers exceptional alkaline OER activity and durability, outperforming most of the Ni-based benchmark OER electrocatalysts.


Highlights:
1 A bimetallic lanthanum-nickel oxysulfide based on a La2O2S prototype was developed as a precatalyst for the electrochemical alkaline oxygen evolution reaction (OER).
2 The in situ, ex situ, and theoretical investigations demonstrated that the precatalyst underwent a deep OER-driven reconstruction into a porous heterostructure where NiOOH nanodomains were uniformly separated and confined by La(OH)3 barrier.
3 Oxyanion (SO42−) was steadily adsorbed on the surface of this in situ reconstructed NiOOH/La(OH)3 heterostructure, enabling it for enhanced OER activity and durability.

Keywords

Lanthanum-nickel oxysulfide Rare earth metal Immobilization of oxyanions Structural reconstruction Oxygen evolution catalysis
Yu, Kai, Hongyuan Yang, Hao Zhang, Hui Huang, Zhaowu Wang, Zhenhui Kang, Yang Liu, Prashanth W. Menezes, and Ziliang Chen. 2023. “Immobilization of Oxyanions on the Reconstructed Heterostructure Evolved from a Bimetallic Oxysulfide for the Promotion of Oxygen Evolution Reaction”. Nano-Micro Letters 15 (July):186. https://doi.org/10.1007/s40820-023-01164-9.
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