Journal
CHEMICAL ENGINEERING JOURNAL
Volume 433, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.134504
Keywords
Non-noble metal; MoS2; Screw-like; Electrocatalytic nitrogen fixation
Categories
Funding
- National Natural Science Foundation of China [51872173]
- Hong Kong Scholars Program [XJ2019042]
- Innovation and Technology Commission of the Hong Kong Special Administrative Region [ITC-CNERC14EG03]
- Taishan Scholars Program of Shandong Province [tsqn201812068]
- Higher School Youth Innovation Team of Shandong Province [2019KJA013]
- Science and Technology Special Project of Qingdao City [20-3-4-3-nsh]
- Opening Fund of State Key Laboratory of Heavy Oil Processing [SKLOP202002006]
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This study synthesized one-dimensional screw-like MoS2 nanosheets with oxygen partially replacing sulfur as an efficient non-noble metal electrocatalyst for NRR, achieving excellent performance in a 0.1 M HCl solution. The unique structure and oxygen substitution show promising potential for the rational design of non-precious metal-based NRR electrocatalysts.
Electrocatalytic nitrogen reduction reaction (NRR) is considered to be an energy-saving method for the production of NH3. However, it is still very challenging to achieve a high NH3 yield and efficiency under ambient conditions. Herein, we for the first time synthesize one-dimensional screw-like MoS2 with oxygen partially replacing sulfur (1D-MoS2-xOy) nanosheets by a one-step solvothermal method as an efficient non-noble metal electrocatalyst for NRR. In a 0.1 M HCl solution, 1D-MoS2-xOy exhibits excellent NRR performance, with a remarkable average ammonia yield rate of 5.56 x 10(-8) mols(-1) cm(-2) at-0.35 V, and a high Faradaic efficiency of 9.86% at-0.3 V. The isotope labeling experiment proves that the generation of NH3 is completely derived from the feed-in N-2. Density functional theory calculations show that MoS2 with oxygen partially replacing sulfur can reduce the Gibbs free energy of the potential determination step (PDS). Besides, the unique screw-like structure can provide more N-2 adsorption sites for NRR. This work proposes a promising strategy for the reasonable design of non-precious metal-based NRR electrocatalysts.
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