Dai Jiajun, Wang Kangli, Voloshina Elena, Dedkov Yuriy, Paulus Beate
Institut für Chemie und Biochemie, Freie Universität Berlin, Arnimallee 22, Berlin 14195, Germany.
Physikalisch-Chemisches Institut, Justus-Liebig-Universität Gießen, Heinrich-Buff-Ring 17, Gießen 35392, Germany.
ACS Omega. 2023 Sep 5;8(37):33920-33927. doi: 10.1021/acsomega.3c04677. eCollection 2023 Sep 19.
The state-of-the-art density functional theory approach was used to study the structural and electronic properties of pristine and defective MnPX monolayers as well as their activity toward water and hydrogen evolution reaction (HER) catalytic performance. The adsorption behavior of HO on a pristine MnPX structure is of physisorption nature, whereas the adsorption energy is significantly increased for the defective structures. At the same time, the water dissociation process is more energetically favorable, and the reactivity of MnPX is determined by the vacancy configuration. Following Nørskov's approach, the HER catalytic performance is evaluated by calculating the hydrogen adsorption free energy on the respective MnPX surface. Our calculation results demonstrate that defective 2D MnPX with low coordinated P shows significantly higher HER performance compared to the pristine counterpart.
采用最先进的密度泛函理论方法研究了原始和有缺陷的MnPX单层的结构和电子性质，以及它们对水和析氢反应（HER）催化性能的活性。HO在原始MnPX结构上的吸附行为具有物理吸附性质，而对于有缺陷的结构，吸附能显著增加。同时，水离解过程在能量上更有利，并且MnPX的反应性由空位构型决定。按照诺尔施科夫的方法，通过计算相应MnPX表面上的氢吸附自由能来评估HER催化性能。我们的计算结果表明，与原始的MnPX相比，低配位P的有缺陷二维MnPX表现出明显更高的HER性能。
