Yu Kai, Yang Hongyuan, Zhang Hao, Huang Hui, Wang Zhaowu, Kang Zhenhui, Liu Yang, Menezes Prashanth W, Chen Ziliang
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.
Department of Chemistry: Metalorganics and Inorganic Materials, Technical University of Berlin, Straße Des 17 Juni 135. Sekr. C2, 10623, Berlin, Germany.
Nanomicro Lett. 2023 Jul 29;15(1):186. doi: 10.1007/s40820-023-01164-9.
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 LaOS 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 [Formula: see text] onto the surface of the deeply reconstructed porous heterostructure composed of confining NiOOH nanodomains by La(OH) 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.
高效且耐用的析氧反应(OER)要求电催化剂具有丰富的活性位点、优化的电子结构以及稳健的组分和机械稳定性。在此,基于LaOS原型制备了一种具有丰富氧空位的双金属氧硫化镧镍,作为用于碱性OER的无粘结剂预催化剂。先进的原位和非原位表征与理论计算相结合,揭示了OER过程中La、Ni、O和S物种之间的协同效应,这确保了氧阴离子[化学式:见原文]吸附并稳定在由La(OH)屏障限制NiOOH纳米域组成的深度重构多孔异质结构表面。这种耦合、限制、孔隙率和固定化能够显著改善活性位点的可及性、相稳定性、质量扩散能力以及含氧化合物中间体的固有吉布斯自由能。优化后的电催化剂展现出卓越的碱性OER活性和耐久性,优于大多数镍基基准OER电催化剂。