Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 9, Pages 10925-10932Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c22276
Keywords
metal-organic framework; metal-carbene; photocatalysis; C-H bond functionalization; heterogeneous catalysis
Funding
- National Natural Science Foundation of China [21890381, 21820102001, 21531001]
- Fundamental Research Funds for the Central Universities [DUT20TD101]
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By stabilizing highly active carbenes in metal-organic frameworks, efficient acceleration of carbene migratory insertion and C-H bond activation was achieved, leading to inert alkane functionalization. The first-time isolation and structural characterization of Ir-III-carbene intermediates were successfully conducted.
The activation and transformation of inert alkyl C(sp(3))-H bonds to obtain high-value fine chemicals by sustainable solar energy are of great significance. Herein, by incorporating Ir-III-porphyrin into metal-organic frameworks (MOFs) to stabilize the highly active carbene, we reported a new approach to combining metallo- and photocatalysis to efficiently accelerate carbene migratory insertion and C-H bond activation via the radical coupling pathway for inert alkane functionalization. The in situ-formed carbene was restricted into the pores of MOFs to produce Ir-III-carbene, allowing the first-time isolation and structural characterization of the Ir-III-carbene intermediate which are not stabilized by a heteroatom. The product of the reaction, especially the cyclic ethers as substrates, suggested that the functionalization of the a position of the alkoxy group was favored. Additionally, the new approach could be extended to stabilize the metal carbene intermediates to realize C(sp(3))-H bond alkylation and arylation.
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