Journal
NATURE CHEMISTRY
Volume 11, Issue 10, Pages 940-947Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41557-019-0313-y
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Funding
- Global Climate and Energy Project
- TomKat Center for Sustainable Energy
- Camille and Henry Dreyfus Foundation
- Arnold and Mabel Beckman Foundation
- NASA Space Technology Research Fellowship
- National Science Foundation [ECCS-1542152]
- Office of Science, Office of Basic Energy Sciences of the US DOE [DE-AC02-05CH11231]
- US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
- Office of Biological and Environmental Research
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The ability to functionalize hydrocarbons with CO2 could create opportunities for high-volume CO2 utilization. However, current methods to form carbon-carbon bonds between hydrocarbons and CO2 require stoichiometric consumption of very resource-intensive reagents to overcome the low reactivity of these substrates. Here, we report a simple semi-continuous cycle that converts aromatic hydrocarbons, CO2 and alcohol into aromatic esters without consumption of stoichiometric reagents. Our strategy centres on the use of solid bases composed of an alkali carbonate (M2CO3, where M+ = K+ or Cs+) dispersed over a mesoporous support. Nanoscale confinement disrupts the crystallinity of M2CO3 and engenders strong base reactivity at intermediate temperatures. The overall cycle involves two distinct steps: (1) CO32--promoted C-H carboxylation, in which the hydrocarbon substrate is deprotonated by the supported M2CO3 and reacts with CO2 to form a supported carboxylate (RCO2M); and (2) methylation, in which RCO2M reacts with methanol and CO2 to form an isolable methyl ester with concomitant regeneration of M2CO3.
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