镍
催化作用
硫化镍
阳离子聚合
硫化物
过电位
材料科学
活动站点
无机化学
吸附
光化学
化学
电化学
物理化学
有机化学
高分子化学
电极
冶金
作者
Pengyan Wang,Tingting Wang,Rui Qin,Zonghua Pu,Chengtian Zhang,Jiawei Zhu,Ding Chen,Dong Feng,Zongkui Kou,Shichun Mu,John Wang
标识
DOI:10.1002/aenm.202103359
摘要
Abstract Tuning active sites in catalyst design is the key to boosting the intrinsic activity of hydrogen evolution reaction (HER). Cationic Ni has been widely established as an active site in nickel sulfide due to the relatively low Gibbs free energy of hydrogen adsorption ( Δ G H* ). However, one of the big unsettled issues is whether S can be activated as a more active site than Ni in NiS 2 . Herein, the swapping of catalytic active sites from cationic Ni to anionic S in a hierarchical structure consisting of NiS 2 nanoflowers grown on dual‐phased NiS 2 ‐NiS foam (denoted as NiS 2 /NiS 2 ‐NiS) is shown. A combined study of theoretical calculations and X‐ray photoelectron spectroscopy analysis demonstrate the remarkably antidromic electron transfer from Ni to S sites, therefore relieving the adsorption of hydrogen species and endowing a higher intrinsic activity at the S site over the Ni site. The new catalyst therefore exhibits superior HER performance, identified by doubling in the intrinsic activity and a twofold increased turnover frequency value compared to its pure NiS 2 counterpart (0.028 s −1 vs 0.015 s −1 at the applied overpotential of 200 mV). The NiS 2 /NiS 2 ‐NiS electrode also demonstrates outstanding activity toward the oxygen evolution reaction and overall water splitting.
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