5 years ago

3D Nitrogen-Anion-Decorated Nickel Sulfides for Highly Efficient Overall Water Splitting

3D Nitrogen-Anion-Decorated Nickel Sulfides for Highly Efficient Overall Water Splitting
Pengzuo Chen, Lidong Zhang, Tianpei Zhou, Nan Zhang, Chengan Zhong, Yi Xie, Yun Tong, Mengxing Zhang, Changzheng Wu
Developing non-noble-metal electrocatalysts with high activity and low cost for both the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is of paramount importance for improving the generation of H2 fuel by electrocatalytic water-splitting. This study puts forward a new N-anion-decorated Ni3S2 material synthesized by a simple one-step calcination route, acting as a superior bifunctional electrocatalyst for the OER/HER for the first time. The introduction of N anions significantly modifies the morphology and electronic structure of Ni3S2, bringing high surface active sites exposure, enhanced electrical conductivity, optimal HER Gibbs free-energy (ΔGH*), and water adsorption energy change (ΔGH2O*). Remarkably, the obtained N-Ni3S2/NF 3D electrode exhibits extremely low overpotentials of 330 and 110 mV to reach a current density of 100 and 10 mA cm−2 for the OER and HER in 1.0 m KOH, respectively. Moreover, an overall water-splitting device comprising this electrode delivers a current density of 10 mA cm−2 at a very low cell voltage of 1.48 V. Our finding introduces a new way to design advanced bifunctional catalysts for water splitting. Metallic N-anion decorated Ni3S2 brings high surface active site exposure, enhanced conductivity, optimal hydrogen evolution reaction (HER) Gibbs free-energy, and water adsorption energy change, acting as superior bifunctional electrocatalysts for the HER/oxygen evolution reaction (OER). The metallic N-Ni3S2/NF 3D electrode only needs a low cell voltage of 1.48 V to reach the current density of 10 mA cm−2, which is superior to most Ni-based electrode materials.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/adma.201701584

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