氧原子补偿缺陷对Ni_(3)S_(2)(101)晶面析氧反应性能的影响

Effect of oxygen atom compensating the defect to enhance electrocatalytic oxygen evolution reaction on Ni_(3)S_(2)(101)facet

为深入了解催化剂中晶体缺陷对析氧反应(oxygen evolution reaction,OER)催化性能的影响,运用第一性原理研究S空位对Ni_(3)S_(2)(101)晶面的影响,并通过O原子补偿空位提高催化剂的催化活性.计算结果表明:空位的引入有利于OER过程中含氧中间体的吸附,但却严重阻碍了其解吸附,导致催化活性降低;当O原子通过替位掺杂对S空位进行补偿时,可有效改善催化剂活性位点的解吸附能力,使缺陷体系的催化活性得到大幅提高.本文所得结果为设计高效的Ni_(3)S_(2)基二维电催化剂提供了参考.

In order to understand the effect of crystal defects on the catalytic performance of oxygen evolution reaction(OER),the effect of S vacancies on the crystalline surface of Ni_(3)S_(2)(101)is investigated by first principles,and the catalytic activity of the catalyst is improved by compensating the vacancies with O atoms.The calculated results show that the introduction of vacancy is beneficial to the adsorption of oxygen-containing intermediates in OER process,but it seriously hinders the desorption and lands to the decrease of catalytic activity;when the S vacancies are compensated by O-atom substitution doping,the desorption capacity of the active sites of the catalyst can be effectively improved,resulting in a substantial increase in the catalytic activity of the defective system.The result obtained in this paper provides an important reference for the design of efficient Ni_(3)S_(2)-based two-dimensional electrocatalysts.