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Construction of C-C bonds via photoreductive coupling of ketones and aldehydes in the metal-organic-framework MFM-300(Cr)

DOI: 10.1038/s41467-021-23302-w DOI Help

Authors: Tian Luo (University of Manchester) , Lili Li (University of Manchester) , Yinlin Chen (University of Manchester) , Jie An (China Agricultural University) , Chengcheng Liu (University of Manchester; Shandong University) , Zheng Yan (University of Manchester; Jiaxing University) , Joseph H. Carter (University of Manchester; Diamond Light Source) , Xue Han (University of Manchester) , Alena M. Sheveleva (University of Manchester) , Floriana Tuna (University of Manchester) , Eric J. L. Mcinnes (University of Manchester) , Chiu C. Tang (Diamond Light Source) , Martin Schroeder (University of Manchester) , Sihai Yang (University of Manchester)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Nature Communications , VOL 12

State: Published (Approved)
Published: June 2021
Diamond Proposal Number(s): 15972

Open Access Open Access

Abstract: Construction of C-C bonds via reductive coupling of aldehydes and ketones is hindered by the highly negative reduction potential of these carbonyl substrates, particularly ketones, and this renders the formation of ketyl radicals extremely endergonic. Here, we report the efficient activation of carbonyl compounds by the formation of specific host-guest interactions in a hydroxyl-decorated porous photocatalyst. MFM-300(Cr) exhibits a band gap of 1.75‚ÄČeV and shows excellent catalytic activity and stability towards the photoreductive coupling of 30 different aldehydes and ketones to the corresponding 1,2-diols at room temperature. Synchrotron X-ray diffraction and electron paramagnetic resonance spectroscopy confirm the generation of ketyl radicals via confinement within MFM-300(Cr). This protocol removes simultaneously the need for a precious metal-based photocatalyst or for amine-based sacrificial agents for the photochemical synthesis.

Journal Keywords: Heterogeneous catalysis; Photocatalysis

Diamond Keywords: Photocatalysis

Subject Areas: Chemistry, Materials


Instruments: I11-High Resolution Powder Diffraction

Added On: 14/06/2021 09:55

Documents:
s41467-021-23302-w.pdf

Discipline Tags:

Catalysis Physical Chemistry Materials Science Metallurgy Metal-Organic Frameworks Chemistry Organometallic Chemistry

Technical Tags:

Diffraction X-ray Powder Diffraction