Zeolite-encapsulated metal nanoclusters are at the heart of bifunctional catalysts,which hold great potential for petrochemical conversion and the emerging sustainable biorefineries.Nevertheless,efficient encapsulatio...Zeolite-encapsulated metal nanoclusters are at the heart of bifunctional catalysts,which hold great potential for petrochemical conversion and the emerging sustainable biorefineries.Nevertheless,efficient encapsulation of metal nanoclusters into a high-silica zeolite Y in particular with good structural integrity still remains a significant challenge.Herein,we have constructed Ru nanoclusters(~1 nm)encapsulated inside a high-silica zeolite Y(SY)with a SiO_(2)/Al_(2)O_(3) ratio(SAR)of 10 via a cooperative strategy for direct zeolite synthesis and a consecutive impregnation for metal encapsulation.Compared with the benchmark Ru/H-USY and other analogues,the as-prepared Ru/H-SY markedly boosts the yields of pentanoic biofuels and stability in the direct hydrodeoxygenation of biomass-derived levulinate even at a mild temperature of 180℃,which are attributed to the notable stabilization of transition states by the enhanced acid accessibility and properly sized constraints of zeolite cavities owing to the good structural integrity.展开更多
With the full growth of energy needs in the world, several studies are now focused on finding renewable sources. The aim of this work is to optimise biofuel formulation from a mixture design by studying physical prope...With the full growth of energy needs in the world, several studies are now focused on finding renewable sources. The aim of this work is to optimise biofuel formulation from a mixture design by studying physical properties, such as specific gravity and kinematic viscosity of various formulated mixtures. Optimization from the mixture plan revealed that in the chosen experimental domain, the optimal conditions are: 40% for used frying oil (UFO), 50% for bioethanol and 10% for diesel. These experimental conditions lead to a biofuel with a density of 0.84 and a kinematic viscosity of 2.97 cSt. These parameters are compliant with the diesel quality certificate in tropical areas. These density and viscosity values were determined according to respective desirability values of 0.68 and 0.75.展开更多
Over the last decade, the uptake rate of first-generation biofuels (ethanol and biodiesel) has decelerated as low blend limits have increased only slowly and extreme volatility in oil prices has limited investment in ...Over the last decade, the uptake rate of first-generation biofuels (ethanol and biodiesel) has decelerated as low blend limits have increased only slowly and extreme volatility in oil prices has limited investment in biofuels production infrastructure. Concerns over the environmental impacts of large-scale biofuels production combined with tariff barriers have greatly restricted the global trade in biofuels. First-generation biofuels produced either by fermentation of sugars from maize or sugarcane (ethanol) or transesterification of triglycerides (biodiesel) presently contribute less than 4% of terrestrial transportation fuel demand and techno-economic modelling foresees this only slowly increasing by 2035. With internal combustion and diesel engines widely anticipated as being phased out in favour of electric power for motor vehicles, a much-reduced market demand for biofuels is likely if global demand for all liquid fuels declines by 2050. However, second-generation, thermochemically produced and biomass-derived fuels (renewable diesel, marine oils and sustainable aviation fuel) have much higher blend limits;combined with policies to decarbonise the aviation and marine industries, major new markets for these products in terrestrial, marine and aviation sectors may emerge in the second half of the 21st century.展开更多
The chemical transformation of natural oils provides alternatives to limited fossil fuels and produces compounds with added value for the chemical industries.The selective deoxygenation of natural oils to diesel-range...The chemical transformation of natural oils provides alternatives to limited fossil fuels and produces compounds with added value for the chemical industries.The selective deoxygenation of natural oils to diesel-ranged hydrocarbons,bio-jet fuels,or fatty alcohols with controllable selectivity is especially attractive in natural oil feedstock biorefineries.This review presents recent progress in catalytic deoxygenation of natural oils or related model compounds(e.g.,fatty acids)to renewable liquid fuels(green diesel and bio-jet fuels)and valuable fatty alcohols(unsaturated and saturated fatty alcohols).Besides,it discusses and compares the existing and potential strategies to control the product selectivity over heterogeneous catalysts.Most research conducted and reviewed has only addressed the production of one category;therefore,a new integrative vision exploring how to direct the process toward fuel and/or chemicals is urgently needed.Thus,work conducted to date addressing the development of new catalysts and studying the influence of the reaction parameters(e.g.,temperature,time and hydrogen pressure)is summarized and critically discussed from a green and sustainable perspective using efficiency indicators(e.g.,yields,selectivity,turnover frequencies and catalysts lifetime).Special attention has been given to the chemical transformations occurring to identify key descriptors to tune the selectivity toward target products by manipulating the reaction conditions and the structures of the catalysts.Finally,the challenges and future research goals to develop novel and holistic natural oil biorefineries are proposed.As a result,this critical review provides the readership with appropriate information to selectively control the transformation of natural oils into either biofuels and/or value-added chemicals.This new flexible vision can help pave the wave to suit the present and future market needs.展开更多
Aviation biofuels have the potential to reduce greenhouse gas emissions and improve engine performance. Theaim of this study was to assess the suitability of various jet biofuel blends for use in a ZF850 jet engine. T...Aviation biofuels have the potential to reduce greenhouse gas emissions and improve engine performance. Theaim of this study was to assess the suitability of various jet biofuel blends for use in a ZF850 jet engine. The effects of theblends on engine performance were assessed under various thrust output settings with respect to the thrust, thrust-specificfuel consumption, emission characteristics, exhaust gas temperature, acceleration and deceleration performance. Blendingwith catalytic hydrothermolysis jet (CHJ) fuel improved the combustion efficiency by reducing carbon monoxide andunburned hydrocarbon emissions and markedly reducing PM2.5 emissions. However, a slight reduction in thrust output wasobserved. Throughout the entire range of thrust output settings, the 10% CHJ fuel blend provided higher thrust, lower thrustspecificfuel consumption, and lower exhaust gas temperature. The CHJ fuel blends exhibited no significant effects on thedeceleration performance, while the 5% and 15% blends caused a 0.4 s delay in the time required for complete acceleration.Global sensitivity analysis was conducted to better understand the effects of the fuel blends on engine performance andemission characteristics. This analysis identified the critical parameters of engine performance as engine-influence and fuelinfluenceparameters and engine-influence and fuel-less influence parameters. The overall engine efficiency benefit was nonlinearlyrelated to the blend ratio and thrust output. The results indicate that the use of CHJ fuel blends can improve engineefficiency if they comply with the engine design and control regulations.展开更多
Lignin is the most abundant naturally phenolic biomass,and the synthesis of high-performance renewable fuel from lignin has attracted significant attention.We propose the efficient synthesis of high-density fuels usin...Lignin is the most abundant naturally phenolic biomass,and the synthesis of high-performance renewable fuel from lignin has attracted significant attention.We propose the efficient synthesis of high-density fuels using simulated lignin cracked oil in tandem with hydroalkylation and deoxygenation reactions.First,we investigated the reaction pathway for the hydroalkylation of phenol,which competes with the hydrodeoxygenation form cyclohexane.And then,we investigated the effects of metal catalyst types,the loading amount of metallic,acid dosage,and reactant ratio on the reaction results.The phenol hydroalkylation and hydrodeoxygenation were balanced when 180℃ and 5 MPa H_(2)with the alkanes yield of 95%.By extending the substrate to other lignin-derived phenolics and simulated lignin cracked oil,we obtained the polycyclic alkane fuel with high density of 0.918 g·ml^(-1)and calorific value of41.2 MJ·L^(-1).Besides,the fuel has good low-temperature properties(viscosity of 9.3 mm^(2)·s^(-1)at 20℃ and freezing point below-55℃),which is expected to be used as jet fuel.This work provides a promising way for the easy and green production of high-density fuel directly from real lignin oil.展开更多
Highly efficient synthesis of clean biofuels using the bio-syngas obtained from biomass gasi- fication was performed over Fel.5CulZnlAllK0.117 catalyst. The maximum biofuel yield from the bio-syngas reaches about 1.59...Highly efficient synthesis of clean biofuels using the bio-syngas obtained from biomass gasi- fication was performed over Fel.5CulZnlAllK0.117 catalyst. The maximum biofuel yield from the bio-syngas reaches about 1.59 kg biofuels/（kgcat·rh） with a contribution of 0.57 kg alcohols/（kgcat·rh） and 1.02 kg liquid hydrocarbons/（kgcat·rh）. The alcohol products in the resulting biofuels were dominated by the C2＋ alcohols （mainly C2-C6 alcohols） with a content of 73.55%-89.98%. The selectivity .of the liquid hydrocarbons （C5＋） in the hydrocarbon products ranges from 60.37% to 70.94%. The synthesis biofuels also possess a higher heat value of 40.53-41.49 MJ/kg. The effects of the synthesis conditions, including temperature, pressure, and gas hourly space velocity, on the biofuel synthesis were investigated in detail. The catalyst features were characterized by inductively coupled plasma and atomic emission spectroscopy, X-ray diffraction, temperature programmed reduction, and the N2 adsorption-desorption isotherms measurements. The present biofuel synthesis with a higher biofuel yield and a higher selectivity of liquid hydrocarbons and C2＋ alcohols may be a potentially useful route to produce clean biofuels and chemicals from biomass.展开更多
Excessive mining and utilization fossil fuels has led to drastic environmental consequences,which will contribute to global warming and cause further climate change with severe consequences for the human population.Th...Excessive mining and utilization fossil fuels has led to drastic environmental consequences,which will contribute to global warming and cause further climate change with severe consequences for the human population.The magnitude of these challenges requires several approaches to develop sustainable alternatives for chemicals and fuels production.In this context,biological processes,mainly microbial fermentation,have gained particular interest.For example,autotrophic gas-fermenting acetogenic bacteria are capable of converting CO,CO_(2) and H_(2) into biomass and multiple metabolites through Wood-Ljungdahl pathway,which can be exploited for large-scale fermentation processes to sustainably produce bulk biochemicals and biofuels(e.g.acetate and ethanol)from syngas.Clostridium autoethanogenum is one representative of these chemoautotrophic bacteria and considered as the model for the gas fermentation.Recently,the development of synthetic biology toolbox for this strain has enabled us to study and genetically improve their metabolic capability in gas fermentation.In this review,we will summarize the recent progress involved in the understanding of physiological mechanism and strain engineering for C.autoethanogenum,and provide our perspectives on the future development about the basic biology and engineering biology of this strain.展开更多
基金supported by the National Natural Science Foundation of China (22288101,21991090,21991091,22078316,22272171 and 22109167)the Sino-French International Research Network (Zeolites)+2 种基金the BL01B1 beamline of SPring-8 and the 1W1B station of Beijing Synchrotron Radiation Facility (BSRF)for the support of XAS measurementsthe Division of Energy Research Resources of Dalian Institute of Chemical Physics for the support of iDPC-STEM measurementsthe support of the Alexander von Humboldt Foundation (CHN 1220532 HFST-P)。
文摘Zeolite-encapsulated metal nanoclusters are at the heart of bifunctional catalysts,which hold great potential for petrochemical conversion and the emerging sustainable biorefineries.Nevertheless,efficient encapsulation of metal nanoclusters into a high-silica zeolite Y in particular with good structural integrity still remains a significant challenge.Herein,we have constructed Ru nanoclusters(~1 nm)encapsulated inside a high-silica zeolite Y(SY)with a SiO_(2)/Al_(2)O_(3) ratio(SAR)of 10 via a cooperative strategy for direct zeolite synthesis and a consecutive impregnation for metal encapsulation.Compared with the benchmark Ru/H-USY and other analogues,the as-prepared Ru/H-SY markedly boosts the yields of pentanoic biofuels and stability in the direct hydrodeoxygenation of biomass-derived levulinate even at a mild temperature of 180℃,which are attributed to the notable stabilization of transition states by the enhanced acid accessibility and properly sized constraints of zeolite cavities owing to the good structural integrity.
文摘With the full growth of energy needs in the world, several studies are now focused on finding renewable sources. The aim of this work is to optimise biofuel formulation from a mixture design by studying physical properties, such as specific gravity and kinematic viscosity of various formulated mixtures. Optimization from the mixture plan revealed that in the chosen experimental domain, the optimal conditions are: 40% for used frying oil (UFO), 50% for bioethanol and 10% for diesel. These experimental conditions lead to a biofuel with a density of 0.84 and a kinematic viscosity of 2.97 cSt. These parameters are compliant with the diesel quality certificate in tropical areas. These density and viscosity values were determined according to respective desirability values of 0.68 and 0.75.
文摘Over the last decade, the uptake rate of first-generation biofuels (ethanol and biodiesel) has decelerated as low blend limits have increased only slowly and extreme volatility in oil prices has limited investment in biofuels production infrastructure. Concerns over the environmental impacts of large-scale biofuels production combined with tariff barriers have greatly restricted the global trade in biofuels. First-generation biofuels produced either by fermentation of sugars from maize or sugarcane (ethanol) or transesterification of triglycerides (biodiesel) presently contribute less than 4% of terrestrial transportation fuel demand and techno-economic modelling foresees this only slowly increasing by 2035. With internal combustion and diesel engines widely anticipated as being phased out in favour of electric power for motor vehicles, a much-reduced market demand for biofuels is likely if global demand for all liquid fuels declines by 2050. However, second-generation, thermochemically produced and biomass-derived fuels (renewable diesel, marine oils and sustainable aviation fuel) have much higher blend limits;combined with policies to decarbonise the aviation and marine industries, major new markets for these products in terrestrial, marine and aviation sectors may emerge in the second half of the 21st century.
基金financially supported by the National Natural Science Foundation of China (No.21536007)the 111 Project (B17030)+1 种基金support from China Scholarship Council (CSC No.202006240156)the Spanish Ministry of Science,Innovation and Universities for the Juan de la Cierva (JdC)fellowships (Grant Numbers FJCI-2016-30847 and IJC2018-037110-I)awarded.
文摘The chemical transformation of natural oils provides alternatives to limited fossil fuels and produces compounds with added value for the chemical industries.The selective deoxygenation of natural oils to diesel-ranged hydrocarbons,bio-jet fuels,or fatty alcohols with controllable selectivity is especially attractive in natural oil feedstock biorefineries.This review presents recent progress in catalytic deoxygenation of natural oils or related model compounds(e.g.,fatty acids)to renewable liquid fuels(green diesel and bio-jet fuels)and valuable fatty alcohols(unsaturated and saturated fatty alcohols).Besides,it discusses and compares the existing and potential strategies to control the product selectivity over heterogeneous catalysts.Most research conducted and reviewed has only addressed the production of one category;therefore,a new integrative vision exploring how to direct the process toward fuel and/or chemicals is urgently needed.Thus,work conducted to date addressing the development of new catalysts and studying the influence of the reaction parameters(e.g.,temperature,time and hydrogen pressure)is summarized and critically discussed from a green and sustainable perspective using efficiency indicators(e.g.,yields,selectivity,turnover frequencies and catalysts lifetime).Special attention has been given to the chemical transformations occurring to identify key descriptors to tune the selectivity toward target products by manipulating the reaction conditions and the structures of the catalysts.Finally,the challenges and future research goals to develop novel and holistic natural oil biorefineries are proposed.As a result,this critical review provides the readership with appropriate information to selectively control the transformation of natural oils into either biofuels and/or value-added chemicals.This new flexible vision can help pave the wave to suit the present and future market needs.
基金the National Key Research and Development Program of China(2018YFB1501505).
文摘Aviation biofuels have the potential to reduce greenhouse gas emissions and improve engine performance. Theaim of this study was to assess the suitability of various jet biofuel blends for use in a ZF850 jet engine. The effects of theblends on engine performance were assessed under various thrust output settings with respect to the thrust, thrust-specificfuel consumption, emission characteristics, exhaust gas temperature, acceleration and deceleration performance. Blendingwith catalytic hydrothermolysis jet (CHJ) fuel improved the combustion efficiency by reducing carbon monoxide andunburned hydrocarbon emissions and markedly reducing PM2.5 emissions. However, a slight reduction in thrust output wasobserved. Throughout the entire range of thrust output settings, the 10% CHJ fuel blend provided higher thrust, lower thrustspecificfuel consumption, and lower exhaust gas temperature. The CHJ fuel blends exhibited no significant effects on thedeceleration performance, while the 5% and 15% blends caused a 0.4 s delay in the time required for complete acceleration.Global sensitivity analysis was conducted to better understand the effects of the fuel blends on engine performance andemission characteristics. This analysis identified the critical parameters of engine performance as engine-influence and fuelinfluenceparameters and engine-influence and fuel-less influence parameters. The overall engine efficiency benefit was nonlinearlyrelated to the blend ratio and thrust output. The results indicate that the use of CHJ fuel blends can improve engineefficiency if they comply with the engine design and control regulations.
基金the support from National Key Research and Development Program of China(2021YFC2104400)the Tianjin Science and Technology Plan Project(21JCQNJC00340)the Haihe Laboratory of Sustainable Chemical Transformations for financial support。
文摘Lignin is the most abundant naturally phenolic biomass,and the synthesis of high-performance renewable fuel from lignin has attracted significant attention.We propose the efficient synthesis of high-density fuels using simulated lignin cracked oil in tandem with hydroalkylation and deoxygenation reactions.First,we investigated the reaction pathway for the hydroalkylation of phenol,which competes with the hydrodeoxygenation form cyclohexane.And then,we investigated the effects of metal catalyst types,the loading amount of metallic,acid dosage,and reactant ratio on the reaction results.The phenol hydroalkylation and hydrodeoxygenation were balanced when 180℃ and 5 MPa H_(2)with the alkanes yield of 95%.By extending the substrate to other lignin-derived phenolics and simulated lignin cracked oil,we obtained the polycyclic alkane fuel with high density of 0.918 g·ml^(-1)and calorific value of41.2 MJ·L^(-1).Besides,the fuel has good low-temperature properties(viscosity of 9.3 mm^(2)·s^(-1)at 20℃ and freezing point below-55℃),which is expected to be used as jet fuel.This work provides a promising way for the easy and green production of high-density fuel directly from real lignin oil.
基金This work was supported by the National Basic Research Program of Ministry of Science and Technology of China （No.2007CB210206）, the National High Tech Research and Development Program （No.2009AA05Z435）, and the National Natural Science Foundation of China （No.50772107）.
文摘Highly efficient synthesis of clean biofuels using the bio-syngas obtained from biomass gasi- fication was performed over Fel.5CulZnlAllK0.117 catalyst. The maximum biofuel yield from the bio-syngas reaches about 1.59 kg biofuels/（kgcat·rh） with a contribution of 0.57 kg alcohols/（kgcat·rh） and 1.02 kg liquid hydrocarbons/（kgcat·rh）. The alcohol products in the resulting biofuels were dominated by the C2＋ alcohols （mainly C2-C6 alcohols） with a content of 73.55%-89.98%. The selectivity .of the liquid hydrocarbons （C5＋） in the hydrocarbon products ranges from 60.37% to 70.94%. The synthesis biofuels also possess a higher heat value of 40.53-41.49 MJ/kg. The effects of the synthesis conditions, including temperature, pressure, and gas hourly space velocity, on the biofuel synthesis were investigated in detail. The catalyst features were characterized by inductively coupled plasma and atomic emission spectroscopy, X-ray diffraction, temperature programmed reduction, and the N2 adsorption-desorption isotherms measurements. The present biofuel synthesis with a higher biofuel yield and a higher selectivity of liquid hydrocarbons and C2＋ alcohols may be a potentially useful route to produce clean biofuels and chemicals from biomass.
基金supported by the Shenzhen Science and Technology Program(Grant No.JCYJ20210324101014036).
文摘Excessive mining and utilization fossil fuels has led to drastic environmental consequences,which will contribute to global warming and cause further climate change with severe consequences for the human population.The magnitude of these challenges requires several approaches to develop sustainable alternatives for chemicals and fuels production.In this context,biological processes,mainly microbial fermentation,have gained particular interest.For example,autotrophic gas-fermenting acetogenic bacteria are capable of converting CO,CO_(2) and H_(2) into biomass and multiple metabolites through Wood-Ljungdahl pathway,which can be exploited for large-scale fermentation processes to sustainably produce bulk biochemicals and biofuels(e.g.acetate and ethanol)from syngas.Clostridium autoethanogenum is one representative of these chemoautotrophic bacteria and considered as the model for the gas fermentation.Recently,the development of synthetic biology toolbox for this strain has enabled us to study and genetically improve their metabolic capability in gas fermentation.In this review,we will summarize the recent progress involved in the understanding of physiological mechanism and strain engineering for C.autoethanogenum,and provide our perspectives on the future development about the basic biology and engineering biology of this strain.
