5-Hydroxymethylfurfural(5-HMF)is one of the important bio-based platform compounds,and the catalytic conversion of glucose to 5-HMF is a highly desirable approach that is receiving increasing attention.Herein,we repor...5-Hydroxymethylfurfural(5-HMF)is one of the important bio-based platform compounds,and the catalytic conversion of glucose to 5-HMF is a highly desirable approach that is receiving increasing attention.Herein,we reported the synthesis of lignin-derived carbon supported tin oxides(SnOx/LC)catalyst via a two-step hydrothermal-pyrolytic method using wheat straw alkali lignin as a cost-effective carbon source with high carbon content.The key preparation conditions of the catalyst and its catalytic conditions for the conversion of glucose to 5-HMF were investigated,respectively.Results show that under the preparation conditions of tin tetrachloride dosage of 3.0 mmol and pyrolysis temperature of 500 ℃,the optimized catalyst(3.0-SnOx/LC-500)with a high yield of 63.4%exhibits good catalytic performance of 5-HMF yield of 50.1%and reaction selectivity of 86.0%under the optimum conditions of reaction temperature and time of 190 ℃ and 3 h,initial glucose concentration of 10%(mass),3.0-SnOx/LC-500 dosage of 100 mg in a biphasic solvent system of volume ratio of water to tetrahydrofuran of 1:4.In addition,3.0-SnOx/LC-500 exerts an excellent reusability in a five-cycle experiment.Furthermore,SnOx/LC was characterized in detail using X-ray diffraction patterns(XRD),X-ray photoelectron spectroscopy(XPS),Brunauer-Emmett-Teller(BET),ammonia temperature-programmed-desorption(NH3-TPD),pyridine adsorption infrared spectroscopy(Py-FTIR),scanning electron microscope(SEM)and thermal gravimetric analysis(TGA).Results indicate that Brønsted acid sites and Lewis acid sites coexist on 3.0-SnOx/LC-500,and more Sn^(4+),as well as a proper ratio of weak acidity to medium acidity,are conductive to its catalytic performance in glucose-to-5-HMF reaction.展开更多
Two kinds of mesoporous carbon solid acids(LDMCE-SO3H and LDMCS-SO3H)were successfully prepared using masson pine alkali lignin as carbon source by evaporation-induced self-assembly(EISA)and salt-induced selfassembly(...Two kinds of mesoporous carbon solid acids(LDMCE-SO3H and LDMCS-SO3H)were successfully prepared using masson pine alkali lignin as carbon source by evaporation-induced self-assembly(EISA)and salt-induced selfassembly(SISA)followed by sulfonation,respectively.In terms of preparation process,SISA(self-assembly in water and preparation time of 2 days)is greener and simpler than EISA(self-assembly in ethanol and preparation time of 7 days).The prepared LDMCE-SO3H and LDMCS-SO3H exhibit obvious differences in structural characteristics such as pore channel structure,specific surface area,mesopore volume and the density of-SO3H groups.Furthermore,the catalytic performances of LDMCE-SO3H and LDMCS-SO3H were investigated in the hydrolysis of microcrystalline cellulose in water,and the glucose yields of 48.99%and 54.42%were obtained under the corresponding optimal reaction conditions.More importantly,the glucose yields still reached 28.85%and 30.35%after five runs,and restored to 39.02%and 45.98%through catalysts regeneration,respectively,demonstrating that LDMCE-SO3H and LDMCS-SO3H have excellent recyclability and regenerability.展开更多
1A solid acid catalyst was prepared from masson pine alkali lignin in waste liquor of soda pulping by a combined process of chemical activation,carbonization,and sulfonation.The lignin-derived solid acid(LDSA)was char...1A solid acid catalyst was prepared from masson pine alkali lignin in waste liquor of soda pulping by a combined process of chemical activation,carbonization,and sulfonation.The lignin-derived solid acid(LDSA)was characterized by FESEM,XRD,FTIR,TGA,XPS,BET analyses,and acid-base back titration.The carbonaceous material had high thermal stability and large specific surface area(488.4 m^(2)/g),and the structural analyses showed that it was composed of amorphous carbon bearing-SO_(3)H,-COOH,and phenolic-OH groups.The lignin-derived catalyst was then applied to the hydrolysis of a microcrystalline cellulose(MCC)in aqueous system,and the yield of total reducing sugars was found to be 46.1%.It was proposed that good adsorption capacities of cellulose and desorption property of glucose on LDSA probably contributed to efficient catalytic hydrolysis.展开更多
基金supported by the independent research major project of Key Laboratory of Biomass Energy and Materials of Jiangsu Province, China (JSBEM-S-202202)the key project of Science and Technology Plan of Nanping, China (N2022B002)the Open Research Fund of Academy of Advanced Carbon Conversion Technology, Huaqiao University, China
文摘5-Hydroxymethylfurfural(5-HMF)is one of the important bio-based platform compounds,and the catalytic conversion of glucose to 5-HMF is a highly desirable approach that is receiving increasing attention.Herein,we reported the synthesis of lignin-derived carbon supported tin oxides(SnOx/LC)catalyst via a two-step hydrothermal-pyrolytic method using wheat straw alkali lignin as a cost-effective carbon source with high carbon content.The key preparation conditions of the catalyst and its catalytic conditions for the conversion of glucose to 5-HMF were investigated,respectively.Results show that under the preparation conditions of tin tetrachloride dosage of 3.0 mmol and pyrolysis temperature of 500 ℃,the optimized catalyst(3.0-SnOx/LC-500)with a high yield of 63.4%exhibits good catalytic performance of 5-HMF yield of 50.1%and reaction selectivity of 86.0%under the optimum conditions of reaction temperature and time of 190 ℃ and 3 h,initial glucose concentration of 10%(mass),3.0-SnOx/LC-500 dosage of 100 mg in a biphasic solvent system of volume ratio of water to tetrahydrofuran of 1:4.In addition,3.0-SnOx/LC-500 exerts an excellent reusability in a five-cycle experiment.Furthermore,SnOx/LC was characterized in detail using X-ray diffraction patterns(XRD),X-ray photoelectron spectroscopy(XPS),Brunauer-Emmett-Teller(BET),ammonia temperature-programmed-desorption(NH3-TPD),pyridine adsorption infrared spectroscopy(Py-FTIR),scanning electron microscope(SEM)and thermal gravimetric analysis(TGA).Results indicate that Brønsted acid sites and Lewis acid sites coexist on 3.0-SnOx/LC-500,and more Sn^(4+),as well as a proper ratio of weak acidity to medium acidity,are conductive to its catalytic performance in glucose-to-5-HMF reaction.
基金financial support from the National Natural Science Foundation of China(grant No.21706085)Subsidized Project for Postgraduates’Innovative Fund in Scientific Research of Huaqiao Universitythe Foundation of Key Laboratory of Pulp and Paper Science and Technology of Ministry of Education/Shandong Province of China(grant No.KF201804)。
文摘Two kinds of mesoporous carbon solid acids(LDMCE-SO3H and LDMCS-SO3H)were successfully prepared using masson pine alkali lignin as carbon source by evaporation-induced self-assembly(EISA)and salt-induced selfassembly(SISA)followed by sulfonation,respectively.In terms of preparation process,SISA(self-assembly in water and preparation time of 2 days)is greener and simpler than EISA(self-assembly in ethanol and preparation time of 7 days).The prepared LDMCE-SO3H and LDMCS-SO3H exhibit obvious differences in structural characteristics such as pore channel structure,specific surface area,mesopore volume and the density of-SO3H groups.Furthermore,the catalytic performances of LDMCE-SO3H and LDMCS-SO3H were investigated in the hydrolysis of microcrystalline cellulose in water,and the glucose yields of 48.99%and 54.42%were obtained under the corresponding optimal reaction conditions.More importantly,the glucose yields still reached 28.85%and 30.35%after five runs,and restored to 39.02%and 45.98%through catalysts regeneration,respectively,demonstrating that LDMCE-SO3H and LDMCS-SO3H have excellent recyclability and regenerability.
基金the financial support from the Natural Science Foundation of Fujian Province,China(2015J01055)the Scientific Research Allowance of Huaqiao University of China(13BS417)the Open Foundation of Guangdong Provincial Engineering Research Center of Green Fine Chemicals of China.
文摘1A solid acid catalyst was prepared from masson pine alkali lignin in waste liquor of soda pulping by a combined process of chemical activation,carbonization,and sulfonation.The lignin-derived solid acid(LDSA)was characterized by FESEM,XRD,FTIR,TGA,XPS,BET analyses,and acid-base back titration.The carbonaceous material had high thermal stability and large specific surface area(488.4 m^(2)/g),and the structural analyses showed that it was composed of amorphous carbon bearing-SO_(3)H,-COOH,and phenolic-OH groups.The lignin-derived catalyst was then applied to the hydrolysis of a microcrystalline cellulose(MCC)in aqueous system,and the yield of total reducing sugars was found to be 46.1%.It was proposed that good adsorption capacities of cellulose and desorption property of glucose on LDSA probably contributed to efficient catalytic hydrolysis.