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Realizing the Synergy of Interface Engineering and Chemical Substitution for Ni3N Enables its Bifunctionality Toward Hydrazine Oxidation Assisted Energy-Saving Hydrogen Production
Advanced Functional Materials  (IF18.808),  Pub Date : 2021-06-23, DOI: 10.1002/adfm.202103673
Yi Liu, Jihua Zhang, Yapeng Li, Qizhu Qian, Ziyun Li, Genqiang Zhang

Hydrazine oxidation assisted water electrolysis offers a unique rationale for energy-saving hydrogen production, yet the lack of effective non-noble-metal bifunctional catalysts is still a grand challenge at the current stage. Here, the Mo doped Ni3N and Ni heterostructure porous nanosheets grow on Ni foam (denoted as MoNi3N/Ni/NF) are successfully constructed, featuring simultaneous interface engineering and chemical substitution, which endow the outstanding bifunctional electrocatalytic performances toward both hydrazine oxidation reaction (HzOR) and hydrogen evolution reaction (HER), demanding a working potential of −0.3 mV to reach 10 mA cm−2 for HzOR and −45 mV for that of HER. Impressively, the overall hydrazine splitting (OHzS) system requires an ultralow cell voltage of 55 mV to deliver 10 mA cm−2 with remarkable long-term durability. Moreover, as a proof-of-concept, economical H2 production systems utilizing OHzS unit powered by a waste AAA battery, a commercial solar cell, and a homemade direct hydrazine fuel cell (DHzFC) are investigated to inspire future practical applications. The density functional theory calculations demonstrate that the synergy of Mo substitution and abundant Ni3N/Ni interface owns a more thermoneutral value for H* absorption ability toward HER and optimized dehydrogenation process for HzOR.