Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 142, Issue 26, Pages 11521-11527Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c04144
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Funding
- Singapore Ministry of Education [RG11/18, MOE2016-T2-1-043]
- Max Planck Institute-Nanyang Technological University Joint Lab
- Boston College
- NSF [CHE 1566445]
- Nanyang Technological University
- Ministry of Education, Singapore
- Nanyang Technological University, Singapore
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Here we design an interface between a metal nanoparticle (NP) and a metal-organic framework (MOF) to activate an inert CO2 carboxylation reaction and in situ monitor its unconventional regioselectivity at the molecular level. Using a Kolbe-Schmitt reaction as model, our strategy exploits the NP@MOF interface to create a pseudo high-pressure CO2 microenvironment over the phenolic substrate to drive its direct C-H carboxylation at ambient conditions. Conversely, Kolbe-Schmitt reactions usually demand high reaction temperature (>125 degrees C) and pressure (>80 atm). Notably, we observe an unprecedented CO2 meta-carboxylation of an arene that was previously deemed impossible in traditional Kolbe-Schmitt reactions. While the phenolic substrate in this study is fixed at the NP@MOF interface to facilitate spectroscopic investigations, free reactants could be activated the same way by the local pressurized CO2 microenvironment. These valuable insights create enormous opportunities in diverse applications including synthetic chemistry, gas valorization, and greenhouse gas remediation.
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