期刊
SCIENCE
卷 351, 期 6280, 页码 1424-1427出版社
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.aad9730
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资金
- University of Pennsylvania
- Ministry of Education of Spain
- Institute for Basic Science in Korea [IBS-R10-D1]
- NIH [GM63188]
Despite steady progress in catalytic methods for the borylation of hydrocarbons, methane has not yet been subject to this transformation. Here we report the iridium-catalyzed borylation of methane using bis(pinacolborane) in cyclohexane solvent. Initially, trace amounts of borylated products were detected with phenanthroline-coordinated Ir complexes. A combination of experimental high-pressure and high-throughput screening, and computational mechanism discovery techniques helped to rationalize the foundation of the catalysis and identify improved phosphine-coordinated catalytic complexes. Optimized conditions of 150 degrees C and 3500-kilopascal pressure led to yields as high as similar to 52%, turnover numbers of 100, and improved chemoselectivity for monoborylated versus diborylated methane.
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