期刊
FUEL PROCESSING TECHNOLOGY
卷 213, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.fuproc.2020.106709
关键词
Cellulose; Lignocellulosic biomass; Polyoxometalate; Alkyl levulinate; Kinetics
资金
- National Natural Science Foundation of China [21965018]
- Yunan Ten Thousand Talents Plan Young & Elite Talents Project
The study focused on designing metal-modified heteropolyacids as multifunctional catalysts for efficient conversion of cellulose and lignocellulosic biomass into fuels and chemicals, specifically alkyl levulinate. The introduction of Al3+ was found to significantly promote cellulose depolymerization and reaction processes, leading to improved efficiency in product formation.
Efficient production of fuels and chemicals from lignocellulosic biomass is the main goal of biorefinery processes. Herein, the metal-modified heteropolyacids with tunable Lewis and Bronsted acid sites were designed as the monolithic multifunctional catalyst for valorizing cellulose and lignocellulosic biomass to alkyl levulinate, a versatile platform molecule. Among them, Al-exchanged two protons of H4SiW12O40 (Al2/3H2SiW12O40) was found to be uniquely effective. The kinetic behavior describing the conversion of cellulose to ethyl levulinate was investigated to monitor the process, and compared between parent H4SiW12O40 and Al2/3H2SiW12O40 to understand the mechanistic role of Al3+. The introduction of Al3+ substantially facilitated cellulose depolymerization and glucose-to-fructose isomerization, leading to a high rate and product selectivity. The estimated activation energies for cellulose degradation and glucopyraoside alcoholysis decreased by 50.6 kJ/mol and 40.9 kJ/mol, respectively. 50-72% yields of ethyl levulinate were accomplished from cellulosic biomasses such as pine wood, eucalyptus, bamboo, bagasse and Napier grass. Al2/3H2SiW12O40 allowed cellulose conversion in various linear alcohols producing high-yield alkyl levulinate, and could be reused multiple times with a good stability. This study opens a reliable and promising avenue for one-pot transformation of cellulose and raw lignocellulosic biomass to ester compounds.
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