Abstract
Splitting hydrazine into H2 and N2 by electro-catalyzing hydrogen evolution and hydrazine oxidation reactions is promising for replacing fossil energy with H2. However, current hydrazine splitting is achieved using external powers to drive the two reactions, which is inapplicable to outdoor use. Here, Fe-doped CoS2 nanosheets are developed as a bifunctional electrocatalyst for the two reactions, by which direct hydrazine fuel cells and overall-hydrazine-splitting units are realized and integrated to form a self-powered H2 production system. Without external powers, this system employs hydrazine bifunctionally as the fuel of direct hydrazine fuel cell and the splitting target, namely a sole consumable, and exhibits an H2 evolution rate of 9.95 mmol h−1, a 98% Faradaic efficiency and a 20-h stability, all comparable to the best reported for self-powered water splitting. These performances are due to that Fe doping decreases the free-energy changes of H adsorption and adsorbed NH2NH2 dehydrogenation on CoS2.
Highlights
Splitting hydrazine into H2 and N2 by electro-catalyzing hydrogen evolution and hydrazine oxidation reactions is promising for replacing fossil energy with H2
Electrocatalytic water and hydrazine splittings have been developed as two green approaches to produce H2, each of which consists of two reactions, hydrogen evolution reaction (HER) and water oxidation reaction (WOR) for water splitting and HER and hydrazine oxidation reaction (HzOR) for hydrazine splitting
The synthesis procedure for the Fedoped CoS2 (Fe-CoS2) nanosheets is presented in Methods and Supplementary Fig. 1: Firstly, layered Fe-doped Co (OH)[2] precipitates, which were intercalated with dodecyl sulfate ions, were synthesized by performing hexamethylenetetramine hydrolysis in an aqueous solution containing Co2+, Fe2+, and sodium dodecyl sulfate[8]
Summary
Splitting hydrazine into H2 and N2 by electro-catalyzing hydrogen evolution and hydrazine oxidation reactions is promising for replacing fossil energy with H2. Fe-doped CoS2 nanosheets are developed as a bifunctional electrocatalyst for the two reactions, by which direct hydrazine fuel cells and overallhydrazine-splitting units are realized and integrated to form a self-powered H2 production system Without external powers, this system employs hydrazine bifunctionally as the fuel of direct hydrazine fuel cell and the splitting target, namely a sole consumable, and exhibits an H2 evolution rate of 9.95 mmol h−1, a 98% Faradaic efficiency and a 20-h stability, all comparable to the best reported for self-powered water splitting. This system employs hydrazine bifunctionally as the fuel of direct hydrazine fuel cell and the splitting target, namely a sole consumable, and exhibits an H2 evolution rate of 9.95 mmol h−1, a 98% Faradaic efficiency and a 20-h stability, all comparable to the best reported for self-powered water splitting These performances are due to that Fe doping decreases the free-energy changes of H adsorption and adsorbed NH2NH2 dehydrogenation on CoS2. These results demonstrate that the DHzFC-driven OHzS is a promising strategy for real-time hydrogen generation without any external power supplies
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