Abstract
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 N2 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 N2 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)2MoS4 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 µg h−1 mg −1cat 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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12 December 2022
An Erratum to this paper has been published: https://doi.org/10.1007/s11426-022-1481-4
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Acknowledgements
This work was supported by the National Natural Science Foundation of China (21773163, 21531006, 22001021), the 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, and the Project of Scientific and Technologic Infrastructure of Suzhou (SZS201905). We are grateful to the useful comments and suggestions of the editor and the reviewers.
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A hybrid catalyst for efficient electrochemical N2 fixation formed by decorating amorphous MoS3 nanosheets with MIL-101(Fe) nanodots
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Xu, WY., Li, C., Li, FL. et al. A hybrid catalyst for efficient electrochemical N2 fixation formed by decorating amorphous MoS3 nanosheets with MIL-101(Fe) nanodots. Sci. China Chem. 65, 885–891 (2022). https://doi.org/10.1007/s11426-021-1206-2
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DOI: https://doi.org/10.1007/s11426-021-1206-2