期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 126, 期 32, 页码 13629-13639出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.2c03776
关键词
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资金
- NSFC [52001172, 21925503, 22121005]
- MOE [B12015]
- Research Funds for the Central Government
- Reform of Local Universities [10000-22311201/006]
- Fundamental Re- search Funds for the Central Universities
This study reports efficient electrocatalytic nitrogen reduction reaction (NRR) on few-layer antimonene in an aqueous K2SO4 electrolyte. The research reveals that active edges and surface-adsorbed hydrated potassium cations enhance NRR kinetics, while K+ increases the energy barrier of proton migration, suppressing the competitive hydrogen evolution reaction (HER) and improving NRR selectivity.
The electrochemical nitrogen reduction reaction (NRR) is an eco-friendly route for ambient N2 fixation with renewable energy but still suffers from low selectivity and sluggish kinetics owing to formidable N2 activation and the competitive hydrogen evolution reaction (HER). Herein, efficient electrocatalytic NRR is reported on few-layer antimonene in an aqueous K2SO4 electrolyte. Density functional theory (DFT) calculations reveal enhancement of NRR kinetics on antimonene with active edges and surface-adsorbed hydrated potassium cations. Combined DFT and comparative ab initio molecular dynamics simulations on antimonene in alkali cation-containing electrolytes indicate that K+ increases the proton migration energy barrier in an interfacial water layer, thus suppressing the HER and improving the NRR selectivity. Experimentally, the prepared few-layer antimonene exhibits a high NH3 yield rate of 44.6 mu g h-1 mg-1 with a Faradaic efficiency of 29.6% in 0.5 M K2SO4. This work suggests the promising use of a group-VA elementary two-dimensional (2D) layered material for nitrogen fixation and provides a new insight into the role of alkali cations in modulating NRR electrocatalysis.
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