Upcycling CO2 and bio-derived furan into degradable plastic monomer via coupling of photocatalysis and thermocatalysis

被引:0
作者
Liu, Qi [1 ,2 ]
Li, Chengyang [1 ,2 ]
Wang, Tingting [1 ,2 ]
Sun, Peng [1 ,3 ]
Wang, Jia [1 ]
Xi, Yongjie [1 ]
Gao, Guang [1 ]
Nie, Mengnan [1 ,2 ]
Huang, Li [1 ,2 ]
Wang, Guofeng [1 ]
Zhao, Zelun [1 ]
Huang, Zhiwei [1 ]
Li, Fuwei [1 ,2 ]
机构
[1] Chinese Acad Sci, Lanzhou Inst Chem Phys, State Key Lab Low Carbon Catalysis & Carbon Dioxid, State Key Lab Oxo Synth & Select Oxidat, Lanzhou 730000, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Suzhou Kehua Low Carbon Technol Res Co LTD, Xiamen, Peoples R China
关键词
Carbon dioxide; Biomass conversion; Photocatalysis; Oxygen vacancy; C -O bond hydrogenolysis; Degradable plastic monomer; TOTAL-ENERGY CALCULATIONS; CARBOXYLIC-ACIDS; CARBON-DIOXIDE; CATALYSTS; HYDROGENATION; OXIDATION; BIOMASS; HYDROGENOLYSIS; DISPERSION; SUPPORT;
D O I
10.1016/j.cej.2024.157519
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Coupling of CO2 with biomass-derived molecules into degradable plastic monomer provides a promising strategy to address the increasing problems of carbon recycle and carbon neutrality. Herein, we develop a sustainable route to produce 6-hydroxycaproate (6-HMC) by coupling photocatalytic carboxylation of biomass-derived furfuryl alcohol with CO2 to 2-furanacetic acid (FA), and the thermocatalytic hydrogenolysis of methyl 2-tetrahydrofuranyl acetate (MTFA) derived from FA, wherein Pd/CeO2 exhibit the highest productivity of 6-HMC (505 mmol(6-HMC) mmol(metal)(-1) h(-1)), much higher than its counterparts of precious- and non-precious-metal catalysts. Moreover, Pd/CeO2 also presents good stability for 6 recycles without remarkable decrease in 6-HMC yield. Systematic experiments and computational studies suggest that higher concentration of oxygen vacancies and strong metal-support interactions account for enhanced catalytic performance of Pd/CeO2. The work employs CO2 and lignocellulosic-derived platform molecule as feedstocks to produce valuable degradable plastic monomer, providing a promising route to access pure-CO2 originated high-carbon oxygen-containing compounds.
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页数:10
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