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The utilization of hydrazine in aiding water electrolysis presents a promising avenue for achieving highly efficient hydrogen production through energy conversion. Herein, bifunctional electrocatalyst of urchin‐like iron, nickle‐codoped cobalt phosphide supported on Ni foam (FeNi‐CoP/NF) is reported. Benefitting from the combined electronic structure and lattice strain engineering by Fe and Ni‐ codoping, the hydrazine‐assisted seawater electrolysis assembled with FeNi‐CoP/NF as both electrodes can achieve an industrial‐level current density of 1.5 A cm−2 at a record‐setting voltage of 163 mV at 70 °C and sustain stable operation for hundreds of hours in seawater environment. The existence of a potential coincidence region lends credibility to the feasibility of implementing self‐activated hydrazine‐assisted seawater electrolysis. Based on theoretical calculations, the separate and synergistic effects of electronic structure and lattice strain engineering are investigated and an integrated illustration of these two strategies on enhancing hydrogen evolution and hydrazine oxidation activity is provided. Moreover, an innovative multi‐powered hydrogen generation system featuring a direct hydrazine fuel cell, rechargeable Zn‐hydrazine battery, and hydrazine‐assisted seawater electrolysis is proposed, underscoring the unique advantages of hydrazine oxidation reaction and its prospective contribution to electrochemical energy conversion technologies powered by sustainable sources. [ABSTRACT FROM AUTHOR]

Water electrolysis, driven by renewable energy resources, is a promising energy conversion technology that has gained intensive interest in recent years. However, conventional water electrolysis faces a number of challenges, including large thermodynamic potential gaps, valueless anodic products, explosive hydrogen/oxygen mixtures, reactive oxygen species, and limited pure water. Hybrid water electrolysis, appending different electrolytes in the anode compartment to circumvent the above‐mentioned challenges in conventional water electrolysis, is a particularly attractive alternative. In this review, for the first time, a holistic and subtle description of hybrid water electrolysis is provided, focusing on the design of high‐activity/selectivity/stability anodic electrocatalysts for the electrochemical oxidation of various chemicals, such as alcohol, aldehyde, amine, urea and hydrazine, or the oxygen evolution reaction in seawater electrolytes. Comprehensive judging criteria for anodic oxidation reactions, electrocatalysts, and reaction parameters in hybrid water electrolysis are discussed. Some technoeconomic assessments, feasibility analyses, mechanism explorations, and correlation comparisons are involved. Finally, perspectives on and opportunities for future research directions in hybrid water electrolysis systems are outlined. [ABSTRACT FROM AUTHOR]

[Display omitted] • Interfacial heterogeneous Ni(OH) 2 /Ni 2 P microstructures are constructed on nickel foam. • Ni(OH) 2 /Ni 2 P/NF exhibits excellent HER, HzOR and hydrazine-assisted water splitting activity. • The heterogeneous interfaces contribute to the enhanced activity. • An innovative intermittent hydrazine-assisted water splitting electrolysis system is proposed. Hydrazine oxidation reaction (HzOR) has been proposed to replace the sluggish oxygen evolution reaction (OER) for energy-saving hydrogen generation. However, the rational design of bifunctional electrocatalysts that can simultaneously accelerate HER/HzOR kinetics and the source of the hydrazine chemical substrate are still challenging. Herein, interfacial heterogeneous nickel hydroxide/nickel phosphide microstructures are in-situ grown on nickel foam (Ni(OH) 2 /Ni 2 P/NF) via a combined electrodeposition-phosphorization-electrodeposition strategy. After Ni(OH) 2 modification, a charge redistribution is triggered between Ni(OH) 2 and Ni 2 P, reducing the charge-transfer resistance and optimizing the adsorption energy of reaction intermediates. Ni(OH) 2 /Ni 2 P/NF thus yields an impressive bifunctional electrocatalytic activity for HER and HzOR with potentials of −72 and −14 mV at 10 mA cm−2, respectively. When using Ni(OH) 2 /Ni 2 P/NF as both electrodes, decreased cell voltage of 0.357 V is required to drive a current density of 100 mA cm−2 in 0.5 M hydrazine-containing alkaline electrolyte. Furthermore, an intermittent hydrazine-assisted water electrolysis system is proposed to make the combination of hydrazine sewage purification and energy-saving hydrogen production realistic. [ABSTRACT FROM AUTHOR]