Gong Feilong, Chen Zhilin, Chang Chaoqun, Song Min, Zhao Yang, Li Haitao, Gong Lihua, Zhang Yali, Zhang Jie, Zhang Yonghui, Wei Shizhong, Liu Jian
Key Laboratory of Surface and Interface Science and Technology of Henan Province, College of Material and Chemical Engineering, Zhengzhou University of Light Industry, Zhengzhou, Henan, 450000, P. R. China.
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning, 116023, P. R. China.
Adv Mater. 2025 Feb;37(5):e2415269. doi: 10.1002/adma.202415269. Epub 2024 Dec 8.
Constructing built-in electric field (BIEF) in heterojunction catalyst is an effective way to optimize adsorption/desorption of reaction intermediates, while its precise tailor to achieve efficient bifunctional electrocatalysis remains great challenge. Herein, the hollow Mo/MoS nanoreactors with tunable BIEFs are elaborately prepared to simultaneously promote hydrogen evolution reaction (HER) and urea oxidation reaction (UOR) for sustainable hydrogen production. The BIEF induced by sulfur vacancies can be modulated from 0.79 to 0.57 to 0.42 mV nm, and exhibits a parabola-shaped relationship with HER and UOR activities, the Mo/MoS nanoreactor with moderate BIEF presents the best bifunctional activity. Theoretical calculations reveal that the moderate BIEF can evidently facilitate the hydrogen adsorption/desorption in the HER and the breakage of N─H bond in the UOR. The electrolyzer assembled with Mo/MoS delivers a cell voltage of 1.49 V at 100 mA cm, which is 437 mV lower than that of traditional water electrolysis, and also presents excellent durability at 200 mA cm for 200 h. Life cycle assessment indicates the HER||UOR system possesses notable superiority across various environment impact and energy consumption. This work can provide theoretical and experimental direction on the rational design of advanced materials for energy-saving and eco-friendly hydrogen production.
在异质结催化剂中构建内建电场（BIEF）是优化反应中间体吸附/解吸的有效方法，然而精确调控以实现高效双功能电催化仍然是巨大挑战。在此，精心制备了具有可调BIEF的空心Mo/MoS纳米反应器，以同时促进析氢反应（HER）和尿素氧化反应（UOR），实现可持续制氢。由硫空位诱导的BIEF可从0.79调制到0.57再到0.42 mV nm，并与HER和UOR活性呈现抛物线关系，具有适度BIEF的Mo/MoS纳米反应器表现出最佳的双功能活性。理论计算表明，适度的BIEF能显著促进HER中的氢吸附/解吸以及UOR中N─H键的断裂。由Mo/MoS组装的电解槽在100 mA cm时的电池电压为1.49 V，比传统水电解低437 mV，并且在200 mA cm下持续200 h也表现出优异的耐久性。生命周期评估表明，HER||UOR系统在各种环境影响和能源消耗方面具有显著优势。这项工作可为合理设计节能和环保制氢的先进材料提供理论和实验指导。
