Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 285, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2020.119810
Keywords
Atomic layered MoS2; Activation; Density functional theory; Electrocatalytic nitrogen fixation; Adjacent Mo atom sites
Funding
- National Key Research and Development Program of China [2018YFB1502700]
- Provincial Nature Science Foundation of Sichuan [2017CC0017, 2018FZ0105, 2019YJ0025]
- Research and Development Program of Chengdu [2019-YF05-01193-SN]
- Fundamental Research Funds for the Central Universities [YJ201746]
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Porous atomic layered 2H-MoS2 (PAL-MoS2) prepared by one-step calcination treatment shows excellent performance in nitrogen reduction reaction, with high Faradic efficiency and significant NH3 yield.
MoS2 has been proven to be an efficient NRR electrocatalyst, the activation of inert basal plane and rational utilization of basal plane have become the key to further increasing the activity. The defects of basal plane help to expose active sites, however, they cannot activate basal plane to promote NRR. Herein, based on the calculation results, we designed porous atomic layered 2H-MoS2(PAL-MoS2) by one-step calcination treatment. The porosity of the basal plane effectively utilizes basal plane atoms while the presence of adjacent Mo atom pairs improves the NRR performance. A high Faradic efficiency of 44.36 % and a sizeable NH3 yield of 3405.55 mu g h(-1) mg(cat)(-1) (1.98 mu g h(-1) cm(-2)) at -0.1 V vs. reversible hydrogen electrode are obtained in 0.1 M HCl under ambient conditions, as far as we know, outperforming most of Mo-based NRR electrocatalysts reported before. Furthermore, this catalyst also exhibits high selectivity, electrochemical stability and good performance characterization.
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