Topochemical domain engineering to construct 2D mosaic heterostructure with internal electric field for high-performance overall water splitting

作者:Quan, Quan; Zhang, Yuxuan; Wang, Fei; Bu, Xiuming; Wang, Wei; Meng, You; Xie, Pengshan; Chen, Dong; Wang, Weijun; Li, Dengji; Liu, Chuntai; Yip, SenPo; Hoa, Johnny C.*
来源:Nano Energy, 2022, 101: 107566.
DOI:10.1016/j.nanoen.2022.107566

摘要

Rational design of bifunctional two-dimensional (2D) heterostructures with excellent activity and durability remains a great challenge for electrocatalytic water splitting. Herein, we propose a topochemical domain engineering to realize 2D mosaic heterostructures with ultrafine phosphide nanodomains highly dispersed on the surface of Ru doped CoMoO4 nanosheets (denoted as Ru-CMOP), which are vertically interconnected on the conductive skeleton assembling a 3D array structure. The as-prepared Ru-CMOP electrocatalyst exhibits excellent activity and long-term stability with the overpotentials of 114 and 286 mV at 100 mA cm-2 for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in 1.0 M KOH solution, respectively, outperforming most reported metal phosphide-based bifunctional heterostructures. Moreover, an assembled electrolyzer using the Ru-CMOP as anode and cathode simultaneously delivers cell voltages of 1.697 V and 1.828 V to achieve 100 mA cm-2 and 500 mA cm-2, respectively, with outstanding durability at 250 mA cm-2 for 120 h. Density functional theory calculations and experimental results indicate that the strongly coupled heterointerfaces with built-in electric field can facilitate electron transfer while multi-porous nanosheet arrays contribute to active sites exposure and mass/gas transport, thereby synergistically accelerating the reaction kinetics. Additionally, combining with a commercial silicon photovoltaic solar cell, the electrolyzer can be efficiently and robustly established, demonstrating the great potential for practical photovoltaic-electrolysis applications.