Black phosphorus-hosted single-atom catalyst for electrocatalytic nitrogen reduction

作     者：Xiaoyun Lin Lulu Li Xin Chang Chunlei Pei Zhi-Jian Zhao Jinlong Gong 林晓韵;李璐璐;常鑫;裴春雷;赵志坚;巩金龙

作者机构：Key Laboratory for Green Chemical Technology of Ministry of EducationSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China Collaborative Innovation Center of Chemical Science and EngineeringTianjin 300350China Joint School of National University of Singapore and Tianjin UniversityInternational Campus of Tianjin UniversityFuzhou 350207China 

基　　金：supported by the National Natural Science Foundation of China (21525626 and 21761132023) the Program of Introducing Talents of Discipline to Universities (BP0618007) 

出 版 物：《Science China Materials》 (中国科学（材料科学（英文版）)

年 卷 期：2021年第64卷第5期

页      码：1173-1181页

摘      要：Designing highly selective and efficient singleatom electrocatalysts is essential for ammonia production under ambient conditions. This paper describes a density functional theory study on exploring the performance trends of transition metal complexes with P-based ligands in nitrogen reduction reaction(NRR) and further develops a design principle for high-performance single-atom catalysts(SACs)of NRR. Among the explored catalysts, W@BP(0.40 eV),Ta@BP(0.47 eV), and Nb@BP(0.53 eV) are identified as remarkable candidates with low free energy change in the potential-limiting step, high stability and high electrical conductivity for NRR. It is worth noting that almost all SACs with P-based ligands exhibit high NRR selectivity, due to the fact that they adsorb *N_(2) more strongly than *H. The adsorption free energy of *N_(2) H can be considered as a descriptor for the intrinsic activity trends in NRR. Furthermore, by constructing a volcano plot of the activity against the electronic charge on metal centers, it is demonstrated that the metal center with a moderate amount of positive charge can promote the catalytic performance of NRR.

主 题 词：nitrogen reduction reaction electrocatalysts singleatom catalysts density functional theory(DFT) black phosphorus 

学科分类：081702[081702] 081705[081705] 08[工学] 0817[工学-轻工类] 080502[080502] 0805[工学-能源动力学] 

核心收录：

D　O　I：10.1007/s40843-020-1522-y

馆 藏 号：203102485...