期刊
SCIENCE CHINA-CHEMISTRY
卷 65, 期 5, 页码 885-891出版社
SCIENCE PRESS
DOI: 10.1007/s11426-021-1206-2
关键词
nitrogen reduction reaction; MIL-101(Fe) nanodots; amorphous MoS3; precursor-transformation; hybrid electrocatalysts
资金
- National Natural Science Foundation of China [21773163, 21531006, 22001021]
- State Key Laboratory of Organometallic Chemistry of Shanghai Institute of Organic Chemistry [KF2021005]
- Natural Science Foundation of Jiangsu Province [BK20201048]
- Natural Science Research Project of Higher Education Institutions in Jiangsu Province [20KJB150008]
- Collaborative Innovation Center of Suzhou Nano Science and Technology
- Project of Scientific and Technologic Infrastructure of Suzhou [SZS201905]
In this study, a MIL-101(Fe)/MoS3 hybrid catalyst was successfully synthesized and showed excellent electrocatalytic activity and durability for the reduction of N-2 to NH3. The transformation of micro-sized MIL-101(Fe) precursors into ultra-small nanodots and anchoring them on MoS3 resulted in improved exposure of active centers and mass transfer, leading to enhanced catalytic activity and stability.
Metal-organic frameworks possessing relatively large pores, high surface areas, and unsaturated metal sites are attractive materials for use as electrocatalysts in the reduction of N-2 to NH3. In this work, a MIL-101(Fe)/MoS3 hybrid catalyst, prepared by using a precursor-transformation strategy, is shown to be an effective electrocatalyst for the N-2 reduction reaction (NRR). Under solvothermal conditions, micro-sized octahedral MIL-101(Fe) precursors are converted into ultra-small nanodots, while amorphous MoS3 derived from (NH4)(2)MoS4 provides a surface suitable for anchoring the MIL-101(Fe) nanodots. The as-prepared composite exhibits excellent electrocatalytic activity and durability for the NRR with a Faraday efficiency of 36.71% and an NH3 yield of 25.7 mu g h(-1) mg(cat)(-1) at -0.1 V vs. RHE in 0.1 M HCl. The results show that the dispersion and adherence of MIL-101(Fe) nanodots on amorphous MoS3 improves the exposure of active centers and aids mass transfer, resulting in greatly enhanced catalytic activity and stability.
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