空位缺陷
催化作用
二硒醚
选择性
材料科学
拉曼光谱
化学
光化学
硒
结晶学
有机化学
光学
物理
冶金
作者
Ying‐Ming Wang,Hui Huang,Jie Wu,Hongyuan Yang,Zhenhui Kang,Yang Liu,Zhaowu Wang,Prashanth W. Menezes,Ziliang Chen
标识
DOI:10.1002/advs.202205347
摘要
Vacancy engineering is deemed as one of the powerful protocols to tune the catalytic activity of electrocatalysts. Herein, Se-vacancy with charge polarization is created in the NiSe2 structure (NiSe2 -VSe ) via a sequential phase conversion strategy. By a combined analysis of the Rietveld method, transient photovoltage spectra (TPV), in situ Raman and density functional theory (DFT) calculation, it is unequivocally discovered that the presence of charge-polarized Se-vacancy is beneficial for stabilizing the structure, decreasing the electron transfer kinetics, as well as optimizing the free adsorption energy of reaction intermediate during two-electron oxygen reduction reaction (2e- ORR). Benefiting from these merits, the as-prepared NiSe2 -VSe delivered the highest selectivity of 96% toward H2 O2 in alkaline media, together with a selectivity higher than 90% over the wide potential range from 0.25 to 0.55 V, ranking it in the top level among the previously reported transition metal-based electrocatalysts. Most notably, it also displayed admirable stability with only a slight selectivity decay after 5000 cycles of accelerated degradation test (ADT).
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