Single transition metal atom embedded into a MoS2 nanosheet as a promising catalyst for electrochemical ammonia synthesis.
Jia ZhaoJingxiang ZhaoQinghai CaiPublished in: Physical chemistry chemical physics : PCCP (2018)
The electrochemical reduction of N2 to NH3 (NRR) under ambient conditions is significant for sustainable agriculture. Here, by means of density functional theory (DFT) computations, the potential of a series of single transition metal (TM) atoms embedded into a MoS2 monolayer with an S-vacancy (TM/MoS2) as electrocatalysts for NRR was systematically investigated. Our DFT results revealed that among all these considered candidate catalysts, the single Mo atom embedded into the MoS2 nanosheet was found to be the most active catalyst for NRR with an onset potential of -0.53 V, in which the hydrogenation of the adsorbed N2* to N2H* is the potential-determining step. The high stabilization of the N2H* species is responsible for the superior performance of the embedded Mo atom for the NRR, which is well consistent with its d-band center. Our findings may facilitate the further design of single-atom electrocatalysts with high efficiency for NH3 synthesis at room temperature.
Keyphrases
- room temperature
- transition metal
- density functional theory
- ionic liquid
- molecular dynamics
- high efficiency
- gold nanoparticles
- electron transfer
- climate change
- highly efficient
- particulate matter
- human health
- quantum dots
- reduced graphene oxide
- risk assessment
- molecular docking
- molecularly imprinted
- mass spectrometry
- crystal structure
- atomic force microscopy