Journal
JOURNAL OF COLLOID AND INTERFACE SCIENCE
Volume 609, Issue -, Pages 815-824Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcis.2021.11.087
Keywords
Polyoxometalates; Molybdenum disulfide; Cobalt disulfide; Electrocatalyst; Nitrogen reduction reaction
Categories
Funding
- Major Research Plan National Natural Science Foundation of China [92061102]
- National Science Foundation of China [22171059]
- Outstanding Youth Project of Natural Science Foundation in Heilongjiang Province [YQ2020B005]
- Postdoctoral Science Foundation, China [2017 M611380]
- University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province [UNPYSCT-2018213]
- Opening Foundation of Key Laboratory of Functional Inorganic Material Chemistry (Heilongjiang University, Ministry of Education)
- Specialized Fund for the Doctoral Research of Jilin Engineering Normal University [BSKJ201916]
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This study successfully prepared an efficient non-precious bimetallic sulfide catalyst CoS2/MoS2 through a one-step method, which exhibits high yield, selectivity, and excellent stability in electrochemical nitrogen reduction reaction (NRR).
Electrochemical nitrogen reduction reaction (NRR) has been identified as a prospective alternative for sustainable ammonia production. Developing cost-effective and highly efficient electrocatalysts is critical for NRR under ambient conditions. Herein, the hierarchical cobalt-molybdenum bimetallic sulfide (CoS2/MoS2) flower-like heterostructure assembled from well-aligned nanosheets has been easily fabricated through a one-step strategy. The efficient synergy between different components and the formation of heterostructure in CoS2/MoS2 nanosheets with abundant active sites makes the non-noble metal catalyst CoS2/MoS2 highly effective in NRR, with a high NH3 yield rate (38.61 mu g h(-1) mg(cat).(-1)), Faradaic efficiency (34.66%), high selectivity (no formation of hydrazine) and excellent long-term stability in 1.0 mol L-1 K2SO4 electrolyte (pH = 3.5) at -0.25 V versus the reversible hydrogen electrode (vs. RHE) under ambient conditions, exceeding much recently reported cobalt- and molybdenum-based materials, even catch up with some noble-metal-based catalyst. Density functional theory (DFT) calculation indicates that the formation of N2H* species on CoS2(200)/MoS2(002) is the rate-determining step via both the alternating and distal pathways with the maximum DG values (1.35 eV). These results open up opportunities for the development of efficient non-precious bimetal-based catalysts for NRR. (C) 2021 Elsevier Inc. All rights reserved.
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