Ga-doped Cu/H-nanozeolite-Y catalyst for selective hydrogenation and hydrodeoxygenation of lignin-derived chemicals

被引:69
作者
Verma, Deepak [1 ,2 ,4 ]
Insyani, Rizki [1 ]
Cahyadi, Handi Setiadi [1 ]
Park, Jaeyong [2 ]
Kim, Seung Min [3 ]
Cho, Jae Min [4 ]
Bae, Jong Wook [4 ]
Kim, Jaehoon [1 ,2 ,4 ]
机构
[1] Sungkyunkwan Univ, SAINT, 2066 Seobu Ro, Suwon 16419, Gyeong Gi Do, South Korea
[2] Sungkyunkwan Univ, Sch Mech Engn, 2066 Seobu Ro, Suwon 16419, Gyeong Gi Do, South Korea
[3] Korea Inst Sci & Technol, Inst Adv Composite Mat, Chudong Ro 92, Wanju Gun, Jeonranbuk Do, South Korea
[4] Sungkyunkwan Univ, Sch Chem Engn, 2066 Seobu Ro, Suwon 16419, Gyeong Gi Do, South Korea
基金
新加坡国家研究基金会;
关键词
COPPER-BASED CATALYSTS; BIO-OIL; NIMO/GAMMA-AL2O3; CATALYSTS; SULFIDED COMO/GAMMA-AL2O3; AROMATIC-HYDROCARBONS; PHASE CARBONYLATION; DIMETHYL CARBONATE; CO2; HYDROGENATION; MODEL COMPOUNDS; ACTIVE-SITES;
D O I
10.1039/c8gc00629f
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The development of an efficient non-sulfided and non-precious catalyst for selective hydrogenation (HD) and hydrodeoxygenation (HDO) of biomass-derived feedstocks to produce fuels and chemicals is of great interest. In this study, a highly efficient bimetallic Ga-doped Cu/H-nanozeolite-Y (Cu/HNZY) catalyst was developed for selective HD and HDO of lignin-derived species (vanillin, acetovanillone, and cinnamaldehyde) under mild conditions (120-180 degrees C, 1 MPa H-2). The HNZY support exhibited a mesoporous structure with a large external surface area, which can facilitate reactant adsorption. Ga doping not only increased the Cu dispersion and Lewis acidity, but produced low coordinated Ga species (e.g., Ga+ and (GaH2)(+)), which could enhance the HDO activity. As a result, at 160 degrees C for 2 to 5 h, complete conversion of vanillin and acetovanillone into their decarbonylated species (creosol and 4-ethylguiuacol) with high selectivity (>99%) could be achieved at a low H-2 initial pressure of 1 MPa. In addition, when cinnamaldehyde was converted over Ga-doped Cu/HNZY at 180 degrees C, selective HD and HDO followed by cyclization formed high amounts of indane and its derivatives, which have a variety of applications in pharmaceutical and agricultural industries. This could open a new possibility for lignin-to-drug intermediates.
引用
收藏
页码:3253 / 3270
页数:18
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