Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 286, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2020.119870
Keywords
High-efficient S vacancies; 1T-MoS2 phase; SV-1T-MoS2@MoO3 electrocatalyst; Electrocatalytic nitrogen reduction reaction
Funding
- Fundamental Research Funds for the Central Universities [0301005202017, 2018CDQYFXCS0017, 106112017CDJXSYY0001]
- Thousand Young Talents Program of the Chinese Central Government [0220002102003]
- National Natural Science Foundation of China (NSFC) [U19A20100, 21971027, 21373280, 21403019]
- Beijing National Laboratory for Molecular Sciences (BNLMS)
- Hundred Talents Program at Chongqing University [0903005203205]
- State Key Laboratory of Mechanical Transmissions Project [SKLMTZZKT-2017M11]
- Natural Science Foundation of Chongqing [cstc2019jcyj-msxmX0426]
- Science and Technology Research Project of Education Agency in Chongqing [KJZD-K201800102]
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In this study, a novel electrocatalyst for nitrogen reduction, SV-1 T-MoS2@MoO3, was successfully synthesized via an interfacial engineering strategy. The catalyst exhibited outstanding electrocatalytic performance, with high NH3 yield rate and optimized Faradaic efficiency, compared to previously reported MoS2-based counterparts. The design of SV-1 T-MoS2@MoO3 with a hybrid structure provides a reference and enlightenment for better envisagement of efficient nitrogen fixing catalysts in the future.
Electrochemical reduction of nitrogen into ammonia has received attentions as an alternative to the industrial process of Haber-Bosch. Profited from the biomimetic inorganic structure, MoS2 has been proven to be a promising catalyst for electrocatalytic nitrogen reduction reaction (ENRR). However, it suffers from deficient active sites and sluggish kinetics. Herein, a novel ENRR electrocatalyst was synthesized via an interfacial engineering strategy, in which the single-layered 1 T-MoS2 with high density of active sites (S vacancies) is uniformly grown on the supporting MoO3 matrix (denoted as SV-1 T-MoS2@MoO3). Benefiting from the functional S vacancies, well-designed structure and the comparative advantages of metallic 1 T-MoS2 phase, the as-synthesized SV-1 T-MoS2@MoO3 exhibits outstanding electrocatalytic performance with highest NH3 yield rate (116.1 mu g h(-1) mg(-1) ea p and optimized Faradaic efficiency (18.9 %), compared to other previously reported MoS2 -based counterparts in acid electrolyte. Density functional theory calculations revealed that the S vacancies can regulate the electronic structure of SV-1 T-MoS2@MoO3 and lead to the antibonding 2 pi* orbital of N-2 molecule moving close to the Fermi level, which greatly promoted the catalytic process towards a more favorable direction for ENRR. The design of SV-1 T-MoS2@MoO3 with hybrid structure in this work provides a reference and enlightenment for better envisagement of efficient nitrogen fixing catalysts.
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