期刊
ACS APPLIED MATERIALS & INTERFACES
卷 12, 期 36, 页码 40236-40247出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c08001
关键词
carbon dioxide; copper catalyst; coupling reaction; hierarchical porosity; N-doped carbon
资金
- National Natural Science Foundation of China [U1810111, 21676089]
- Natural Science Foundation of Guangdong Province, China [2018B030311010]
- Youth Science and Technology Innovation Talent of Guangdong TeZhi Plan [2019TQ05L111]
- Key Laboratory of Biomass Chemical Engineering of Ministry of Education, Zhejiang University [2018BCE002]
Chemical transformation of carbon dioxide (CO2) into fine chemicals such as oxazolidinones and carbamates is mainly reported using transition-metal complexes as homogeneous catalysts. Herein, we demonstrate that a heterogeneous catalyst of highly dispersed Cu (Cu/NHPC) supported on hierarchically porous N-doped carbon (NHPC) can efficiently promote CO2 fixations to oxazolidinones and beta-oxopropylcarbamates. The obtained NHPC, assembled by ultrathin nitrogen-doped carbon nanosheets with a three-dimensional (3D) structure, is readily prepared by pyrolysis of a nitrogen-containing polymer gel (NPG) in the presence of an activator of potassium bicarbonate (KHCO3). The resulting NHPC shows specific Brunauer-Emmet-Teller (BET) surface areas up to 2054 m(2) g(-1) with a mean micro/ mesopore size of 0.55/3.2 nm and a broad macropore size distribution from 50 to 230 nm. The Cu/NHPC can efficiently promote three-component coupling of CO2, amines, and propargyl alcohols for syntheses of various oxazolidinones and beta-oxopropylcarbamates with yields up to 99% and a wide substrate scope. Moreover, the Cu/NHPC exhibits excellent recyclability in CO2-to-oxazolidinone transformation during nine-time recycling. The research thus develops an NHPC-based heterogeneous Cu catalyst for green transformation of CO2.
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