Noble-Metal-Free Ni-W-O-Derived Catalysts for High-Capacity Hydrogen Production from Hydrazine Monohydrate

作者：Shi, Qing; Zhang, Deng-Xue; Yin, Hui; Qu, Yu-Ping; Zhou, Liang-Liang; Chen, Chen; Wu, Hui; Wang, Ping^*

来源：ACS Sustainable Chemistry & Engineering, 2020, 8(14): 5595-5603.

DOI：10.1021/acssuschemeng.9b07782

• Hydrogen storage
• Hydrazine monohydrate
• Noble-metalfree catalyst
• Ni-W alloy
• Phase evolution

Development of active and earth-abundant catalysts is pivotal to render hydrazine monohydrate (N2H4-H2O) viable as a hydrogen carrier. Herein, we report the synthesis of noble-metalfree Ni-W-O-derived catalysts using a hydrothermal method in combination with reductive annealing treatment. Interestingly, the thus-prepared Ni-based catalysts exhibit remarkably distinct catalytic properties toward N2H4-H2O decomposition depending upon the annealing temperature. From a systematic phase/ microstructure/chemical state characterization and the first-principles calculations, we found that the variation of the apparent catalytic properties of these Ni-based catalysts should stem from the formation of different Ni-W alloys with distinct intrinsic activity, selectivity, and distribution state. The thereby chosen Ni- W alloy nanocomposite catalyst prepared under an optimized condition showed high activity, nearly 100% selectivity, and excellent stability toward N2H4-H2O decomposition for hydrogen production. Furthermore, this noble-metal-free catalyst enables rapid hydrogen production from commercially available N2H4-H2O solution with an intriguingly high hydrogen capacity of 6.28 wt % and a satisfactory dynamic response property. These results are inspiring and momentous for promoting the use of the N2H4-H2O-based H-2 source systems.