Electrochemical ammonia synthesis under ambient conditions using TM-embedded porphine-fused sheets as single-atom catalysts.
Ying YaoSheng-Yao LvGuoliang LiLi-Ming YangPublished in: Physical chemistry chemical physics : PCCP (2023)
In this research, we systematically investigated the reaction mechanism and electrocatalytic properties of transition metal anchored two-dimensional (2D) porphine-fused sheets (TM-Por) as novel single-atom catalysts (SACs) for the electrochemical nitrogen reduction reaction (eNRR) under ambient conditions. Using high-throughput screening and first-principles calculations based on the density functional theory (DFT) method, three eNRR catalyst candidates, i.e. Mo-Por, Tc-Por, and Nb-Por, were screened out, with the eNRR onset potentials on them being -0.36, -0.53, and -0.74 V, respectively. Furthermore, these catalyst candidates all have good stability and selectivity. Analyzing the band structures found that these catalyst candidates all are metallic, which is needed for good electrocatalysts. Ab initio molecular dynamics (AIMD) simulations show that these catalyst candidates have good stability at 500 K. It is hoped that our work will open up new possibilities for the experimental synthesis of electrochemical ammonia catalysts.
Keyphrases
- molecular dynamics
- density functional theory
- highly efficient
- ionic liquid
- transition metal
- room temperature
- metal organic framework
- reduced graphene oxide
- gold nanoparticles
- air pollution
- particulate matter
- molecularly imprinted
- electron transfer
- label free
- carbon dioxide
- minimally invasive
- anaerobic digestion
- visible light
- high resolution
- single molecule
- molecular docking
- crystal structure