Journal
CHEMSUSCHEM
Volume 10, Issue 23, Pages 4748-4755Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.201701607
Keywords
alcohols; iridium; mesoporous carbon; metal clusters; methylation
Funding
- National Natural Science Foundation of China [21273260, 201403265, 21433001]
- Shandong Provincial Natural Science Foundation for Distinguished Young Scholar [JQ201305]
- Taishan Scholars Climbing Program of Shandong [tspd20150210]
- Young Taishan Scholars Program of Shandong Province [tsqn20161052]
- Youth Innovation Promotion Association CAS [2015168]
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C-H methylation is an attractive chemical transformation for C-C bonds construction in organic chemistry, yet efficient methylation of readily available (bio)alcohols in water using methanol as sustainable C1 feedstock is limited. Herein, iridium nanocatalysts encapsulated in yolk-shell-structured mesoporous carbon nanospheres (Ir@YSMCNs) were synthesized for this transformation. Monodispersed Ir clusters (ca. 1.0nm) were encapsulated insitu and spatially isolated within YSMCNs by a silica-assisted sol-gel emulsion strategy. A selection of (bio)alcohols (19examples) was selectively methylated in aqueous phase with good-to-high yields over the developed Ir@YSMCNs. The improved catalytic efficiencies in terms of activity and selectivity together with the good stability and recyclability were contributable to the ultrasmall Ir clusters with oxidation chemical state as a consequence of the confinement effect of YSMCNs with interconnected nanostructures.
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