A DFT screening of single transition atoms supported on MoS2 as highly efficient electrocatalysts for the nitrogen reduction reaction
A DFT screening of single transition atoms supported on MoS2 as highly efficient electrocatalysts for the nitrogen reduction reaction
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DFT 筛选 MoS2 负载的单过渡原子作为氮还原反应的高效电催化剂
DOI：
10.1039/d0nr00030b
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发表时间：
2020
期刊：
影响因子：
6.7
通讯作者：
Ge Guixian
中科院分区：
文献类型：
--
作者：
Zhai Xingwu;Li Lei;Liu Xiaoyue;Li Yafei;Yang Jueming;Yang Dezheng;Zhang Jinli;Yan Hongxia;Ge Guixian
开发低成本、高效率的电催化氮还原反应（NRR）材料是一个极具吸引力和挑战性的课题。采用密度泛函理论（DFT）方法，系统研究了一系列过渡金属（TM）原子负载于MoS 2纳米片（TM@MoS2）上的电催化性能.发现负载在MoS 2上的Re（Re@MoS2）具有最好的NRR催化活性，其极限电位为-0.43 V，沿着对竞争析氢反应（HER）具有高选择性。此外，在500 K下的从头算分子动力学（AIMD）模拟和态密度（DOS）计算表明，Re@MoS2的高热力学稳定性和优异的导电性。单原子催化剂（SAC）的几个参数与NH物种的吸附吉布斯自由能变化（ΔG*NH）之间存在线性关系，表明后者是一个简单的描述新SAC筛选的描述符。这些结果为在环境条件下探索新型高效的电化学NRR电催化剂铺平了道路。
The development of low-cost and highly efficient materials for the electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions is an attractive and challenging topic in chemistry. In this study, the electrocatalytic performance of a series of transition metal (TM) atoms supported on MoS2 nanosheets (TM@MoS2) was systematically investigated using density functional theory (DFT) calculations. It was found that Re supported on MoS2 (Re@MoS2) has the best NRR catalytic activity with a limiting potential of −0.43 V, along with high selectivity over the competing hydrogen evolution reaction (HER). Moreover, the ab initio molecular dynamics (AIMD) simulations at 500 K and density of states (DOS) calculations indicated the high thermodynamic stability and excellent electrical conductivity of Re@MoS2. A linear trend between several parameters of single atom catalysts (SACs) and the adsorption Gibbs free energy change of the NH species (ΔG*NH) was observed, indicating the later as a simple descriptor for the facilitated screening of novel SACs. These results pave the way for exploring novel, highly efficient electrocatalysts for the electrochemical NRR under ambient conditions.