期刊
MATERIALS ADVANCES
卷 1, 期 5, 页码 1285-1292出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0ma00348d
关键词
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资金
- Research Grants Council of the Hong Kong Special Administrative Region, China [PolyU152140/19E]
- Hong Kong Polytechnic University [Q54V, RH9G]
- National Natural Science Foundation of China [11804286]
- Fundamental Research Funds for the Central Universities [19lgpy263]
- Scientific and Technical Innovation Action Plan (Hong Kong, Macao and Taiwan Science & Technology Cooperation Project of Shanghai Science and Technology Committee) [19160760600]
Converting earth-abundant nitrogen into value-added chemical ammonia is a significant yet challenging topic. The electrocatalytic nitrogen reduction reaction (NRR), compared with the conventional Haber-Bosch process, is an energy-saving and environmentally friendly approach. Finding electrocatalysts which can activate nitrogen effectively and exhibit high selectivity and stability for the electrocatalytic NRR is a major task. Single-atom catalysts can act as a good solution. In this work, by means of first-principles density functional theory, molecular dynamics calculations, and a two-step screening process, we have studied 17 transition metal single atoms supported on tetracyanoquinodimethane monolayers (TM-TCNQ), and among them, Sc-TCNQ and Ti-TCNQ are found to be excellent candidates for NRR electrocatalysts. N-2 adsorption and activation are effective due to the 'acceptance-donation' mechanism and suitable electronic structure of TM-TCNQ. The Gibbs free energy diagram shows that Sc-TCNQ and Ti-TCNQ exhibit a low NRR overpotential of 0.33 and 0.22 V, respectively, through an enzymatic-consecutive mixed pathway. In addition, the selectivity of the NRR over the HER and stability of the Sc-/Ti-TCNQ monolayers are also validated. This work opens a new avenue for designing novel single-atom catalysts for the NRR as well as other catalytic applications.
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