Wu Tong, Xu Shumao, Zhang Zhuang, Luo Mengjia, Wang Ruiqi, Tang Yufeng, Wang Jiacheng, Huang Fuqiang
State Key Lab of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050, China.
Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, 100049, China.
Adv Sci (Weinh). 2022 Sep;9(25):e2202750. doi: 10.1002/advs.202202750. Epub 2022 Jul 11.
Large current-driven alkaline water splitting for large-scale hydrogen production generally suffers from the sluggish charge transfer kinetics. Commercial noble-metal catalysts are unstable in large-current operation, while most non-noble metal catalysts can only achieve high activity at low current densities <200 mA cm , far lower than industrially-required current densities (>500 mA cm ). Herein, a sulfide-based metallic heterostructure is designed to meet the industrial demand by regulating the electronic structure of phase transition coupling with interfacial defects from Mo and Ni incorporation. The modulation of metallic Mo S and in situ epitaxial growth of bifunctional Ni-based catalyst to construct metallic heterostructure can facilitate the charge transfer for fast Volmer H and Heyrovsky H generation. The Mo S @NiMo S electrolyzer requires an ultralow voltage of 1.672 V at a large current density of 1000 mA cm , with ≈100% retention over 100 h, outperforming the commercial RuO ||Pt/C, owing to the synergistic effect of the phase and interface electronic modulation. This work sheds light on the design of metallic heterostructure with an optimized interfacial electronic structure and abundant active sites for industrial water splitting.
用于大规模制氢的大电流驱动碱性水分解通常受限于缓慢的电荷转移动力学。商业贵金属催化剂在大电流运行中不稳定，而大多数非贵金属催化剂仅能在低于200 mA cm 的低电流密度下实现高活性，远低于工业所需电流密度（>500 mA cm ）。在此，通过调控相变耦合的电子结构以及引入Mo和Ni所产生的界面缺陷，设计了一种基于硫化物的金属异质结构以满足工业需求。金属Mo S 的调制以及双功能Ni基催化剂的原位外延生长以构建金属异质结构，可促进电荷转移，实现快速的伏尔默析氢（Volmer H ）和海洛夫斯基析氢（Heyrovsky H ）。Mo S @NiMo S 电解槽在1000 mA cm 的大电流密度下需要1.672 V的超低电压，在100小时内保持率约为100%，由于相和界面电子调制的协同效应，其性能优于商业RuO ||Pt/C。这项工作为设计具有优化界面电子结构和丰富活性位点的金属异质结构用于工业水分解提供了思路。
