Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 12, Issue 49, Pages 54851-54861Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c17612
Keywords
copper phyllosilicate; hydrogenation; hydrophobicity; levulinic acid; gamma-valerolactone
Funding
- Ministry of Science and Technology [106-2221-E-006-188-MY3]
- Taiwan's Deep Decarbonization Pathways toward a Sustainable Society [AS-KPQ-106-DDPP]
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A reduction-silylation-reduction method was developed to synthesize hydrophobic Cu catalysts derived from Cu phyllosilicates (CuPS). Triethoxy(octyl)silane (OTS) was used as the coupling agent. The OTS-grafted, reduced CuPS catalysts were applied in the hydrogenation of levulinic acid (LA) to gamma-valerolactone (GVL). The most promising catalyst was synthesized by reducing CuPS at a high temperature (350 degrees C for 3 h), followed by OTS grafting, and then by repeating the previous reduction step. High LA conversion (95.7%), GVL yield (85.2%), and stability (3 cycles with a 7.5% loss of initial activity) were obtained at a mild reaction condition (130 degrees C with a H-2 pressure of 12 bar). A high reduction temperature not only leads to a low oxidation state of Cu species but also suppresses the formation of silylation-induced acids. Moreover, the intrinsic activity of a reduced CuPS catalyst was nearly intact after subjecting to silylation and the second reduction treatment.
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