@article{Wang2022, 
author = {Guojing Wang and Yuzhuo Sun and Yidan Zhao and Yang Zhang and Xiaohong Li and Louzhen Fan and Yunchao Li},
title = {Phosphorus-induced electronic structure reformation of hollow NiCo2Se4 nanoneedle arrays enabling highly efficient and durable hydrogen evolution in all-pH media},
year = {2022},
journal = {Nano Research},
volume = {15},
number = {10},
pages = {8771-8782},
keywords = {P-doped NiCo2Se4 nanoarrays, local electronic structure, hydrogen evolution reaction (HER), pH-universal electrocatalysis, density functional theory (DFT) calculation},
url = {https://www.sciopen.com/article/10.1007/s12274-022-4534-9},
doi = {10.1007/s12274-022-4534-9},
abstract = {With practical electrocatalytic hydrogen production frequently involving the splitting of water in various pH media, there is an urgent need but still a technical challenge to develop low-cost, highly active, and stable electrocatalysts for pH-universal hydrogen evolution reaction (HER). We report herein the adoption of a hydrothermal reaction combined with a post gas-phase doping strategy to fabricate P-doped NiCo2Se4 hollow nanoneedle arrays on carbon fiber paper (i.e., P-NiCo2Se4/CFP). Notably, the optimal arrays (P8.71-NiCo2Se4/CFP) can afford an outstanding pH-universal HER performance, with an overpotential as low as 33, 57, and 69 mV at 10 mA·cm−2 and corresponding Tafel slopes down to 52, 61, and 72 mV·dec−1 in acidic, alkaline, and neutral media, respectively, outperforming most state-of-the-art nonprecious catalysts and even the commercial Pt/C catalyst in both neutral and alkaline media at large current densities. Impressively, P8.71-NiCo2Se4/CFP also displays good durability toward long-time stability testing in harsh acidic and alkaline electrolytes. Experimental and theoretical studies further reveal that the doping of P atoms into NiCo2Se4 can simultaneously optimize its H* adsorption/desorption energy, water adsorption energy, and water dissociation energy by adjusting the local electronic states of various active sites, thus accelerating the rate-determining step of HER in different pH media to endow P-NiCo2Se4 with an outstanding pH-universal HER performance. This work provides atomic-level insights into the roles of active sites in various electrolysis environments, thereby shedding new light on the rational design of highly efficient pH-universal nonprecious catalysts for HER and beyond.}
}