Sulphur modulated Ni3FeN supported on N/S co-doped graphene boosts rechargeable/flexible Zn-air battery performance

• Published in: Applied catalysis. B, Environmental Vol. 274; p. 119086
• Main Authors: Lai, Chenglong, Gong, Mingxing, Zhou, Yecheng, Fang, Jiayi, Huang, Li, Deng, Zhiping, Liu, Xupo, Zhao, Tonghui, Lin, Ruoqian, Wang, Kangli, Jiang, Kai, Xin, Huolin, Wang, Deli
• Format: Journal Article
• Language: English
• Published: Amsterdam Elsevier B.V 05.10.2020; Elsevier BV; Elsevier
• Subjects: Batteries; Bifunctional electrocatalyst; Catalysts; Decoration; Density functional theory; Durability; Electrocatalysts; Graphene; Intermediates; Intermetallic compounds; Iron compounds; Metal air batteries; NANOSCIENCE AND NANOTECHNOLOGY; Nickel compounds; Oxygen; Oxygen evolution reaction; Oxygen reduction reaction; Rechargeable batteries; Sulfur; Sulphur modulated; Water splitting; Zinc; Zinc-air battery; Zinc-oxygen batteries; Bifunctional electrocatalyst; Sulphur modulated; Oxygen evolution reaction; Oxygen reduction reaction; Zinc-air battery
• ISSN: 0926-3373; 1873-3883
• DOI: 10.1016/j.apcatb.2020.119086

Sulphur(S) modulated Ni3FeN supported on N/S co-doped graphene (S-Ni3FeN/NSG) is synthesized via controlling the nitriding process of NiFe disulfides, and delivers excellent bifunctional oxygen electrode reaction electrocatalyic performance, particularly exhibits practical application potential in rechargeable/flexible Zn-air battery. This work provides new insights into highly efficient and low-cost electrocatalyst designing strategies. [Display omitted] •The S-Ni3FeN/NSG-700 is synthesized by controlling the nitriding process of the NiFe disulfides.•The N/S co-doped graphene with porous structure provides a large number of ORR reactive sites.•The S residues in Ni3FeN nanoparticles expedite the rate-determination step of OER. Exploring feasible strategy for preparation of sulfur (S) modulated NiFe compounds and meanwhile clarifying the performance promoting mechanism of such catalysts has triggered numerous interest in rechargeable Zinc-air battery research field. Herein, S modulated Ni3FeN supported on N/S co-doped graphene (S-Ni3FeN/NSG) is synthesized via controlling the nitriding process of NiFe disulfides. The beneficial effect of the design strategy and S decoration on electrocatalytic activity are determined and analysed systematacially. The S-Ni3FeN/NSG-700 delivers excellent bifunctional oxygen electrocatalysis performance with half-wave potential of 0.878 V for ORR and low OER overpotential of 260 mV at 10 mA cm−2. Density Functional Theory (DFT) calculations demonstrate that S decoration effectively promotes the formation of OOH* intermediates and observably decreases the maximum of change of the Gibbs free energies for four primitive OER steps. Notably, when S-Ni3FeN/NSG-700 as air electrode applied in Zn-air battery test, the device shows superb durability for 1200 discharge/charge cycles at 10 mA cm-2. The corresponding all-solid Zinc-air battery exhibits excellent mechanical flexibility and a high power density of 140.1 mW cm-2. Two Zinc-air batteries in series can long-term stably power a self-made water-splitting device. This work provides new insights into highly efficient and low-cost bifunctional oxygen electrocatalyst designing.