The production of?-valerolactone(GVL)from lignocellulosic biomass has become a focus of research owing to its potential applications in fuels and chemicals.In this study,(n)CuOx-CaCO3(where n is the molar ratio of Cu ...The production of?-valerolactone(GVL)from lignocellulosic biomass has become a focus of research owing to its potential applications in fuels and chemicals.In this study,(n)CuOx-CaCO3(where n is the molar ratio of Cu to Ca)compounds were prepared for the first time and shown to function as efficient bifunctional catalysts for the conversion of biomass-derived methyl levulinate(ML)into GVL,using methanol as the in-situ hydrogen source.Among the catalysts with varied Cu/Ca molar ratios,(3/2)CuOx-CaCO3 provided the highest GVL yield of 95.6% from ML.The incorporation of CaCO3 with CuO resulted in the formation of Cu+species in a CuOx-CaCO3 catalyst,which greatly facilitated the hydrogenation of ML.Notably,CuOx-CaCO3 also displayed excellent catalytic performance in the methanolysis products of cellulose,even in the presence of humins.Therefore,a facile two-step strategy for the production of GVL from cellulose could be developed over this robust and inexpensive catalyst,through the integration of cellulose methanolysis catalyzed by sulfuric acid,methanol reforming,and ML hydrogenation in methanol medium.展开更多
Au-Ir and Au-Ru on TiOz catalysts prepared by sequential deposition-precipitation technique were compared with the corresponding monometallics in the hydrogenation of levulinic acid to y-valero]actone. Interestingly t...Au-Ir and Au-Ru on TiOz catalysts prepared by sequential deposition-precipitation technique were compared with the corresponding monometallics in the hydrogenation of levulinic acid to y-valero]actone. Interestingly the addition of Ao to Ir/TiO2 showed a detrimental effect on the activity of Ir monometallic catalyst whereas a positive synergistic effect was shown in the case of Ru. Both catalysts were reduced under H2 to increase the M0-Au0 interaction, From previous DFT calculations and catalytic test, we addressed the lower activity of Au-lr/TiO2 than that of Ir/TiO2 to the interference of Au into the redox mechanism of lr atoms.展开更多
基金supported by the National Natural Science Foundation of China(21676223,21706223,21776234,21606188)the Fundamental Research Funds for the Central Universities(20720180084),the Energy development Foundation of Energy College,Xiamen University(2017NYFZ02)+1 种基金the Natural Science Foundation of Fujian Province of China(2018J01017)the Education Department of Fujian Province(JZ160398)~~
文摘The production of?-valerolactone(GVL)from lignocellulosic biomass has become a focus of research owing to its potential applications in fuels and chemicals.In this study,(n)CuOx-CaCO3(where n is the molar ratio of Cu to Ca)compounds were prepared for the first time and shown to function as efficient bifunctional catalysts for the conversion of biomass-derived methyl levulinate(ML)into GVL,using methanol as the in-situ hydrogen source.Among the catalysts with varied Cu/Ca molar ratios,(3/2)CuOx-CaCO3 provided the highest GVL yield of 95.6% from ML.The incorporation of CaCO3 with CuO resulted in the formation of Cu+species in a CuOx-CaCO3 catalyst,which greatly facilitated the hydrogenation of ML.Notably,CuOx-CaCO3 also displayed excellent catalytic performance in the methanolysis products of cellulose,even in the presence of humins.Therefore,a facile two-step strategy for the production of GVL from cellulose could be developed over this robust and inexpensive catalyst,through the integration of cellulose methanolysis catalyzed by sulfuric acid,methanol reforming,and ML hydrogenation in methanol medium.
基金financial support granted by project UNAM-PAPIIT IN105416
文摘Au-Ir and Au-Ru on TiOz catalysts prepared by sequential deposition-precipitation technique were compared with the corresponding monometallics in the hydrogenation of levulinic acid to y-valero]actone. Interestingly the addition of Ao to Ir/TiO2 showed a detrimental effect on the activity of Ir monometallic catalyst whereas a positive synergistic effect was shown in the case of Ru. Both catalysts were reduced under H2 to increase the M0-Au0 interaction, From previous DFT calculations and catalytic test, we addressed the lower activity of Au-lr/TiO2 than that of Ir/TiO2 to the interference of Au into the redox mechanism of lr atoms.