In this work,a“cyclopentanone-vanillin”strategy was proposed for the preparation of jet fuel range cycloalkanes from lignocellulose-derived ketones and lignin-derived aldehydes via aldol condensation and hydrodeoxyg...In this work,a“cyclopentanone-vanillin”strategy was proposed for the preparation of jet fuel range cycloalkanes from lignocellulose-derived ketones and lignin-derived aldehydes via aldol condensation and hydrodeoxygenation(HDO).Ethanolamine lactate ionic liquid(LAIL)exhibited excellent catalytic activity in the aldol condensation of cyclopentanone and vanillin.Desired mono-condensation and bicondensation products were obtained with yield of 95.2%at 100℃.It is found that the synergy effects between amino group of ethanolamine and hydroxyl group of lactic acid play a key role in the aldol condensation.The condensation products were converted into cycloalkanes by HDO over 5%Pd/Nb_(2)O_(5)catalyst.The density of the obtained HDO products is 0.89 g/cm^(3)and the freezing point is lower than-60℃.These results suggest that the resulted cycloalkanes can be used as additives to improve the density and low-temperature fluidity of the jet fuels.展开更多
Direct conversion of syngas to aromatics has great potential to decrease fossil fuel dependence.Here,a unique structured hybrid catalyst composed of Fe_(3)O_(4) nanoparticles intimately dispersed inside an acidic zeol...Direct conversion of syngas to aromatics has great potential to decrease fossil fuel dependence.Here,a unique structured hybrid catalyst composed of Fe_(3)O_(4) nanoparticles intimately dispersed inside an acidic zeolite is developed.1 to 4 nm sized Fe_(3)O_(4) nanoparticles end up evenly dispersed in an acidic and slightly mesoporous Al-ZSM-5 based on Fe_(3)O_(4) restructuring during co-hydro thermal synthesis using organosilane modification.A very high aromatic productivity of 214 mmolaromatics h^(-1) gFe^(-1) can be obtained with a remarkable 62%aromatic selectivity in hydrocarbons.This catalyst has excellent sintering resistance ability and maintains stable aromatics production over 570 h.The synthetic insights that postulate a mechanism for the metastable oxide-zeolite reorganization during hydrothermal synthesis could serve as a generic route to sinter-resistant oxide-zeolite composite materials with uniform,well-dispersed oxide nanoparticles in close intimacy with-and partially confined in-a zeolite matrix.展开更多
Herein,we reported in situ synthesis of biomass-derived Ni/C catalyst by self-reduction with pomelo peel.Compared with the conventional method, which includes carbonization, activation, impregnation and reduction, the...Herein,we reported in situ synthesis of biomass-derived Ni/C catalyst by self-reduction with pomelo peel.Compared with the conventional method, which includes carbonization, activation, impregnation and reduction, the entire preparation process was simplified to two steps, which was more straightforward. This synthesis method was green as Ni/C can be prepared without any additional chemical and the self-reduction process was realized in N2, which can avoid using H2 thus averting some problems such as storage, transportation and safety of H2. Meanwhile, the size and dispersion of Ni particles can be controlled by changing carbonization temperature.The synthesis mechanism of Ni/C catalyst with selfreduction was investigated, which was mainly attributed to the carbon and reducing gas produced during the carbonization process.For the catalytic performance of GVL synthesis, a high yield (94.5%) can be obtained and it exhibited good stability up to 5 cycles without obvious loss of catalytic activity.展开更多
Limited by single function,it is difficult for the traditional stirred vessels to meet the requirements of mixing system in biomass wastewater treatment processes.The estimation of biomass wastewater stirring reactor ...Limited by single function,it is difficult for the traditional stirred vessels to meet the requirements of mixing system in biomass wastewater treatment processes.The estimation of biomass wastewater stirring reactor performance by computational fluid dynamics(CFD)during multiphase reactions is important,due to the uncertainty in the numerical results.In this study,a novel double-partition stirred vessel with eccentrically located impellers was developed for the special subject.In addition,many simulations were carried out with the wastewater from biomass ethanol production as the medium to ensure the high reactor performance.The fluid flow was simulated and analyzed using the turbulent RNG k-ε model and multi reference frames.A good agreement is found between the simulation results and the confirmatory experiment.Moreover,the weir crest and interconnected pore were specially designed for the establishment of the circulation of fluid to maintain different technological conditions in the two regions.The distributions of radial velocities and tangential velocities were concentrated near the stirring blade.From the velocity profile,it is deduced that the flow pattern in the stirred vessel is insensitive to Reynolds number.Finally,this simulation study could contribute to the improvement and optimization of the structure,as well as the operation of the novel stirred vessel.展开更多
基金funded by grants from the National Natural Science Foundation of China(No.52236010,51876210)the Fundamental Research Funds for the Central Universities(No.2242022R10058)。
文摘In this work,a“cyclopentanone-vanillin”strategy was proposed for the preparation of jet fuel range cycloalkanes from lignocellulose-derived ketones and lignin-derived aldehydes via aldol condensation and hydrodeoxygenation(HDO).Ethanolamine lactate ionic liquid(LAIL)exhibited excellent catalytic activity in the aldol condensation of cyclopentanone and vanillin.Desired mono-condensation and bicondensation products were obtained with yield of 95.2%at 100℃.It is found that the synergy effects between amino group of ethanolamine and hydroxyl group of lactic acid play a key role in the aldol condensation.The condensation products were converted into cycloalkanes by HDO over 5%Pd/Nb_(2)O_(5)catalyst.The density of the obtained HDO products is 0.89 g/cm^(3)and the freezing point is lower than-60℃.These results suggest that the resulted cycloalkanes can be used as additives to improve the density and low-temperature fluidity of the jet fuels.
基金supported financially by the National Natural Science Foundation of China(51776206)the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(2017BT01N092)+4 种基金the National Key R&D Program of China(2018YFB1501504)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX20_0095)the Fundamental Research Funds for the Central Universities(3203002104D)the Research Foundation-Flanders(FWO,grant 12E8617N)for funding and KU Leuven grant C14/20/086visiting scholar(2017-20202)at the Guangzhou Institute of Energy Conversion,Chinese Academy of Sciences。
文摘Direct conversion of syngas to aromatics has great potential to decrease fossil fuel dependence.Here,a unique structured hybrid catalyst composed of Fe_(3)O_(4) nanoparticles intimately dispersed inside an acidic zeolite is developed.1 to 4 nm sized Fe_(3)O_(4) nanoparticles end up evenly dispersed in an acidic and slightly mesoporous Al-ZSM-5 based on Fe_(3)O_(4) restructuring during co-hydro thermal synthesis using organosilane modification.A very high aromatic productivity of 214 mmolaromatics h^(-1) gFe^(-1) can be obtained with a remarkable 62%aromatic selectivity in hydrocarbons.This catalyst has excellent sintering resistance ability and maintains stable aromatics production over 570 h.The synthetic insights that postulate a mechanism for the metastable oxide-zeolite reorganization during hydrothermal synthesis could serve as a generic route to sinter-resistant oxide-zeolite composite materials with uniform,well-dispersed oxide nanoparticles in close intimacy with-and partially confined in-a zeolite matrix.
基金funded by the National Key R&D Program of China (2018YFB1501504)the National Natural Science Foundation of China (Nos. 51776206 and 21878290)+1 种基金the Natural Science Foundation of Guangdong province (2017A030313073)CAS Pioneer Hundred Talents Program
文摘Herein,we reported in situ synthesis of biomass-derived Ni/C catalyst by self-reduction with pomelo peel.Compared with the conventional method, which includes carbonization, activation, impregnation and reduction, the entire preparation process was simplified to two steps, which was more straightforward. This synthesis method was green as Ni/C can be prepared without any additional chemical and the self-reduction process was realized in N2, which can avoid using H2 thus averting some problems such as storage, transportation and safety of H2. Meanwhile, the size and dispersion of Ni particles can be controlled by changing carbonization temperature.The synthesis mechanism of Ni/C catalyst with selfreduction was investigated, which was mainly attributed to the carbon and reducing gas produced during the carbonization process.For the catalytic performance of GVL synthesis, a high yield (94.5%) can be obtained and it exhibited good stability up to 5 cycles without obvious loss of catalytic activity.
基金supported by the National Natural Science Foundation of China(Grant No.21868014)Low-carbon Development Guidance Project of Yunnan Province in 2021(No.135)+5 种基金Key Sci-Tech Project of China Tobacco Yunnan Industrial Co.,Ltd.,(Grant No.2022GY03)Key Project of Yunnan Fundamental Research Program(Grant No.2019FA004)Yunnan Academician and Expert Workstation(Grant No.202205 AF150024)Kunming International Sci-Tech Cooperation Base,China(Grant No.GHJD-2020026)Yunnan Sci-Tech Talents and Platform Program(Grant No.202105AC160058)Scientific research project of Yunnan Environmental Science Society,China(No.XHKYKT006).
文摘Limited by single function,it is difficult for the traditional stirred vessels to meet the requirements of mixing system in biomass wastewater treatment processes.The estimation of biomass wastewater stirring reactor performance by computational fluid dynamics(CFD)during multiphase reactions is important,due to the uncertainty in the numerical results.In this study,a novel double-partition stirred vessel with eccentrically located impellers was developed for the special subject.In addition,many simulations were carried out with the wastewater from biomass ethanol production as the medium to ensure the high reactor performance.The fluid flow was simulated and analyzed using the turbulent RNG k-ε model and multi reference frames.A good agreement is found between the simulation results and the confirmatory experiment.Moreover,the weir crest and interconnected pore were specially designed for the establishment of the circulation of fluid to maintain different technological conditions in the two regions.The distributions of radial velocities and tangential velocities were concentrated near the stirring blade.From the velocity profile,it is deduced that the flow pattern in the stirred vessel is insensitive to Reynolds number.Finally,this simulation study could contribute to the improvement and optimization of the structure,as well as the operation of the novel stirred vessel.