Cu(I)‐Glutathione Assembly Supported on ZIF‐8 as Robust and Efficient Catalyst for Mild CO2 Conversions

The Cu‐glutathione (GSH) redox system, essential in biology, is designed here as a supramacromolecular assembly in which the tetrahedral 18e Cu(I) center loses a thiol ligand upon adsorption onto ZIF‐8, as shown by EXAFS and DFT calculation, to generate a very robust 16e planar trigonal single‐atom...

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Published inAngewandte Chemie International Edition Vol. 63; no. 37; pp. e202407430 - n/a
Main Authors Wang, Wenjuan, Wang, Tiansheng, Chen, Shuang, Lv, Ying, Salmon, Lionel, Espuche, Bruno, Moya, Sergio, Morozova, Oksana, Yun, Yapei, Di Silvio, Desiré, Daro, Nathalie, Berlande, Murielle, Hapiot, Philippe, Pozzo, Jean‐Luc, Yu, Haizhu, Hamon, Jean‐René, Astruc, Didier
Format Journal Article
LanguageEnglish
Published Germany Wiley Subscription Services, Inc 09.09.2024
Wiley-VCH Verlag
EditionInternational ed. in English
Subjects
alkyne
Alkynes
Amines
Assembly
Carbon dioxide
carboxylation
Catalysts
Catalytic converters
Chemical Sciences
CO2
Copper
Glutathione
heterogeneous catalysis
Robustness
Substrates
ZIF-8
carboxylation
alkyne
ZIF-8
glutathione
CO2
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Summary:The Cu‐glutathione (GSH) redox system, essential in biology, is designed here as a supramacromolecular assembly in which the tetrahedral 18e Cu(I) center loses a thiol ligand upon adsorption onto ZIF‐8, as shown by EXAFS and DFT calculation, to generate a very robust 16e planar trigonal single‐atom Cu(I) catalyst. Synergy between Cu(I) and ZIF‐8, revealed by catalytic experiments and DFT calculation, affords CO2 conversion into high‐value‐added chemicals with a wide scope of substrates by reaction with terminal alkynes or propargyl amines in excellent yields under mild conditions and reuse at least 10 times without significant decrease in catalytic efficiency. The Cu(I)‐glutathione polymer supported on ZIF‐8 is a robust catalyst for the efficient carboxylation of terminal alkynes and the cyclization of propargylamine with CO2 under atmospheric pressure and mild conditions with a wide range of substrates, converting them into high value‐added chemicals, with strong positive synergy between Cu(I) and ZIF‐8. This catalyst is reused at least 10 times without significant reduction in catalytic efficiency.
Bibliography:Both authors (WW and TW) contributed equally to this work.
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ISSN:1433-7851
1521-3773
1521-3773
DOI:10.1002/anie.202407430