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Nano Research 2023, 16(1): 181-188 https://doi.org/10.1007/s12274-022-4664-0
Issue | Published: 23 July 2022

Amorphous NH2-MIL-68 as an efficient electro- and photo-catalyst for CO2 conversion reactions

Show Author's Information Lifei Liu1,2,  Jianling Zhang1,2( ),  Xiuyan Cheng1,2,  Mingzhao Xu1,2,  Xinchen Kang1,2,  Qiang Wan1,2,  Buxing Han1,2,  Ningning Wu1,2,  Lirong Zheng3,  Chenyan Ma3
Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid, Interface and Chemical Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China
School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China
Beijing Synchrotron Radiation Facility (BSRF), Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
Keywords:
photocatalyst, electrocatalyst, defect engineering, amorphous metal-organic framework, missing ligand incorporation
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Liu L, Zhang J, Cheng X, et al. Amorphous NH2-MIL-68 as an efficient electro- and photo-catalyst for CO2 conversion reactions. Nano Research, 2023, 16(1): 181-188. https://doi.org/10.1007/s12274-022-4664-0
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Abstract Full text Electronic supplementary material About this article

To produce metal-organic framework (MOF) catalysts with both high activity and durability is interesting but challenging. We report an amorphous MOF (NH2-MIL-68), which combines the advantages of (1) a large number of open metal sites, (2) the basic building blocks and connectivity of crystalline NH2-MIL-68, and (3) hierarchically meso- and microporous structure. It exhibits high performances in electrocatalytic reduction of CO2 and photochemical cycloaddition of CO2 under mild conditions. For the former reaction, the maximum Faradaic efficiency for product formic acid (FEHCOOH) reaches 93.3% with a current density of 34.2 mA·cm−2 at −2.05 V vs. Ag/Ag+ catalyzed by amorphous NH2-MIL-68, while the crystalline NH2-MIL-68 shows FEHCOOH of 67.7% with considerable productions of CO and H2 at the same experimental conditions. For the photochemical cycloaddition of CO2 with styrene oxide, the yield by amorphous NH2-MIL-68 can reach 94.1% at 12 h, which is higher than the reported value under similar conditions. The structure–efficiency relationship of the catalyst for the two reactions was investigated. This work opens up new possibility for designing high-performance MOF and MOF-based catalysts.


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Electronic supplementary material
About this article

Amorphous NH2-MIL-68 as an efficient electro- and photo-catalyst for CO2 conversion reactions

Show Author's information Lifei Liu1,2, Jianling Zhang1,2( ), Xiuyan Cheng1,2, Mingzhao Xu1,2, Xinchen Kang1,2, Qiang Wan1,2, Buxing Han1,2, Ningning Wu1,2, Lirong Zheng3, Chenyan Ma3
Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid, Interface and Chemical Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China
School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China
Beijing Synchrotron Radiation Facility (BSRF), Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China

Abstract

To produce metal-organic framework (MOF) catalysts with both high activity and durability is interesting but challenging. We report an amorphous MOF (NH2-MIL-68), which combines the advantages of (1) a large number of open metal sites, (2) the basic building blocks and connectivity of crystalline NH2-MIL-68, and (3) hierarchically meso- and microporous structure. It exhibits high performances in electrocatalytic reduction of CO2 and photochemical cycloaddition of CO2 under mild conditions. For the former reaction, the maximum Faradaic efficiency for product formic acid (FEHCOOH) reaches 93.3% with a current density of 34.2 mA·cm−2 at −2.05 V vs. Ag/Ag+ catalyzed by amorphous NH2-MIL-68, while the crystalline NH2-MIL-68 shows FEHCOOH of 67.7% with considerable productions of CO and H2 at the same experimental conditions. For the photochemical cycloaddition of CO2 with styrene oxide, the yield by amorphous NH2-MIL-68 can reach 94.1% at 12 h, which is higher than the reported value under similar conditions. The structure–efficiency relationship of the catalyst for the two reactions was investigated. This work opens up new possibility for designing high-performance MOF and MOF-based catalysts.

Keywords: photocatalyst, electrocatalyst, defect engineering, amorphous metal-organic framework, missing ligand incorporation

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Publication history
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Acknowledgements

Publication history

Received: 04 May 2022
Revised: 01 June 2022
Accepted: 14 June 2022
Published: 23 July 2022
Issue date: January 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This research was made possible as a result of a generous grant from Ministry of Science and Technology of China (No. 2017YFA0403003) and the National Natural Science Foundation of China (No. 22033009).

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