Nano-Micro Letters ( IF 31.6 ) Pub Date : 2023-07-29 , DOI: 10.1007/s40820-023-01164-9 Kai Yu 1 , Hongyuan Yang 2 , Hao Zhang 1 , Hui Huang 1 , Zhaowu Wang 3 , Zhenhui Kang 1 , Yang Liu 1 , Prashanth W Menezes 2, 4 , Ziliang Chen 1, 2, 4
|
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 \(\left( {{\text{SO}}_{4}^{{2 - }} } \right)\) 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.
Graphical Abstract
中文翻译：
氧阴离子在双金属硫氧化物重构异质结构上的固定化促进析氧反应
摘要
高效持久的析氧反应（OER）需要电催化剂具有丰富的活性位点、优化的电子结构以及坚固的组件和机械稳定性。在此，基于La 2 O 2 S原型制备了具有丰富氧空位的双金属镧镍氧硫化物作为碱性OER的无粘合剂预催化剂。先进的原位和异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，确保了氧阴离子的吸附和稳定 \(\ left( {{\text{SO }}_{4}^{{2 - }} } \right)\)到由 La(OH) 3势垒限制 NiOOH 纳米域组成的深度重建的多孔异质结构的表面上。这种偶联、限制、孔隙率和固定化能够显着改善活性位点的可及性、相稳定性、质量扩散能力和含氧中间体的固有吉布斯自由能。经过优化的电催化剂具有卓越的碱性 OER 活性和耐用性，优于大多数镍基基准 OER 电催化剂。
京公网安备 11010802027423号