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
Owing to an environment-friendly utilization of resources, increased attention has been focused on fuels and chemicals from biomass as an alternative to fossil resources. In addition, supercritical fluid technology ha...Owing to an environment-friendly utilization of resources, increased attention has been focused on fuels and chemicals from biomass as an alternative to fossil resources. In addition, supercritical fluid technology has been considered to be an environmentally-benign treatment. Therefore, its technology was applied for a conversion of biomass to useful fuels and chemicals in order to mitigate environmental loading. For example, supercritical water treatment has demonstrated that lignocellulosics can be hydrolyzed to become lignin-derived products for useful aromatic chemicals and carbohydrate-derived products, such as polysaccharides, oligosaccharides and monosaccharides of glucose, mannose and xylose used for subsequent ethanol fermentation. If this treatment is prolonged, lignocellulosics were found to be converted to organic acids such as formic, acetic, glycolic and lactic acids which can be converted to methane for biofuel. When alcohols, such as methanol and ethanol, were used instead of water, some other useful products were achieved, and its liquefied products were found to have a potential for liquid biofuel. In this study, therefore, our research achievements in supercritical fluid science of woody biomass will be introduced for clean and green chemistry for a sustainable environment.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
Transgenic trees as a new source for biofuel have brought a great interest in tree biotechnology. Genetically modifying forest trees for ethanol production have advantages in technical challenges, costs, environmental...Transgenic trees as a new source for biofuel have brought a great interest in tree biotechnology. Genetically modifying forest trees for ethanol production have advantages in technical challenges, costs, environmental concerns, and financial problems over some of crops. Genetic engineering of forest trees can be used to reduce the level of lignin, to produce the fast-growing trees, to develop trees with higher cellulose, and to allow the trees to be grown more widely. Trees can establish themselves in the field with less care of farmers, compared to most of crops. Transgenic crops as a new source for biofuel have been recently reviewed in several reviews. Here, we overview transgenic woody plants as a new source for biofuel including genetically modified woody plants and environment; main focus of woody plants genetic modifications; solar to chemical energy transfer; cellulose biosynthesis; lignin biosynthesis; and cellulosic ethanol as biofuel.展开更多
In this article, the aptitude of natural gas as feedstock in steam reforming process for hydrogen production is compared with that of different liquid fuels (pure compounds and commercial fuels), with the aim to inv...In this article, the aptitude of natural gas as feedstock in steam reforming process for hydrogen production is compared with that of different liquid fuels (pure compounds and commercial fuels), with the aim to investigate the potentialities of biofuels to overcome the CO2 emission problems deriving from fossil fuel processing. The performances of a nickel based catalyst (commercially used in steam reforming of natural gas) were evaluated in terms of feed conversion and yield to the different products as function of temperature, space velocity and water/fuel ratio. Furthermore, a preliminary evaluation of catalyst durability was effected by monitoring yield to H2 versus time on stream and measuring coke formation at the end of experimental tests. High yields to hydrogen were obtained with all fuels investigated, whereas the deactivation phenomena, which are correlated to carbon deposition on the catalyst, were observed with all tested fuels, except for methane and biofuel.展开更多
Zeolite-supported metal catalysts containing hydrogenation centers and acid sites are promising in the chemoselective hydrogenation of biomass platform molecules into value-added chemicals and fuels.The primary challe...Zeolite-supported metal catalysts containing hydrogenation centers and acid sites are promising in the chemoselective hydrogenation of biomass platform molecules into value-added chemicals and fuels.The primary challenge of employing such bifunctional catalysts for biomass conversion lies in catalyst stability in the liquid phase under harsh conditions. Herein, we have prepared a Ni/La-Y nanocatalyst via an improved wet impregnation method. Compared with Ni nanoparticles on H-Y, La addition shows a significantly enhanced stability and performance in the continuous liquid-phase hydrogenation of γ-valerolactone(GVL) into ethyl pentanoate(EP) at 200 ℃ for 1000 h. Complementary characterization studies reveal that La addition in the metal/zeolite catalyst not only efficiently modulates the acid property of the zeolite to alleviate coke formation, but also suppresses zeolite dealumination and metal agglomeration and leaching upon catalysis over a 1000 h period. These findings provide an efficient approach for improving the stability of zeolite-supported bifunctional catalysts, leading to potential application in hydrogen-assisted biomass valorization under the liquid-phase conditions.展开更多
Terpenoids have drawn much attention to scientists in synthesizing high-performance bio-jet fuels due to their ring structures,which feature potential high densities.Here,a facile biphasic catalytic process has been d...Terpenoids have drawn much attention to scientists in synthesizing high-performance bio-jet fuels due to their ring structures,which feature potential high densities.Here,a facile biphasic catalytic process has been developed for the production of high-density tricyclic hydrocarbon biofuels from a monoterpenoid,1,8-cineole,using sulfuric acid(H2SO4)as the homogeneous catalyst.A^100%conversion of 1,8-cineole and a>40%carbon yield of cyclic dimers were achieved at 100℃within two hours.The mechanism for the acid-catalyzed conversion of 1,8-cineole to cyclic hydrocarbon dimers were explored.In particular,the formation of the diene intermediates and the following dimerization of dienes was essential to synthesize tricyclic terpene dimers.The biphasic catalytic process accelerated the deoxygenation rate and enabled the dimerization with the aid of organic solvent while controlling the reaction rates to avoid the formation of solid residues.Moreover,this process also facilitated the product separation by organic solvent extraction while enabling easy recycle of the homogenous catalysts.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
The effect of ethanedioic acid(Ed A) functionalization on Al2O3 supported Ni catalyst was studied on the hydrodeoxygenation(HDO), isomerization, kinetics and Arrhenius parameters of octadec-9-enoic acid(OA) into...The effect of ethanedioic acid(Ed A) functionalization on Al2O3 supported Ni catalyst was studied on the hydrodeoxygenation(HDO), isomerization, kinetics and Arrhenius parameters of octadec-9-enoic acid(OA) into biofuel in this report. This was achieved via synthesis of two catalysts; the first, nickel alumina catalyst(Ni/Al2O3) was via the incorporation of inorganic Ni precursor into Al2O3; the second was via the incorporation nickel oxalate(Ni Ox) prepared by functionalization of Ni with Ed A into Al2O3 to obtain organometallic Ni Ox/Al2O3 catalyst. Their characterization results showed that Ni species present in Ni/Al2O3 and Ni Ox/Al2O3 were 8.2% and 9.3%, respectively according to the energy dispersive X-ray result. Ni Ox/Al2O3 has comparably higher Ni content due to the Ed A functionalization which also increases its acidity and guarantees high Ni dispersion with weaker metal-support-interaction leading to highly reducible Ni as seen in the X-ray diffraction, X-ray photoelectron spectroscopy, TPR and Raman spectroscopy results. Their activities tested on the HDO of OA showed that Ni Ox/Al2O3 did not only display the best catalytic and reusability abilities, but it also possesses isomerization ability due to its increased acidity. The Ni Ox/Al2O3 also has the highest rate constants evaluated using pseudo-first-order kinetics,but the least activation energy of 176 k J/mol in the biofuel formation step compared to 244 k J/mol evaluated when using Ni/Al2O3. The result is promising for future feasibility studies toward commercialization of catalytic HDO of OA into useful biofuel using organometallic catalysts.展开更多
In sub-Saharan Africa(SSA), the main goals behind the development of a biofuel industry are employment creation and income generation. Jatropha(Jatropha curcas L.) has emerged as a candidate for biodiesel producti...In sub-Saharan Africa(SSA), the main goals behind the development of a biofuel industry are employment creation and income generation. Jatropha(Jatropha curcas L.) has emerged as a candidate for biodiesel production. It is a non-edible oil producing, drought-resistant plant that can be grown on marginal land with limited water and low soil fertility. However, these are also attributes that typify weedy and invasive plant species. Adding to these concerns are the general questioning of whether biofuel production will reduce Greenhouse gas(GHG)emissions globally. Currently, there is limited information on the potential invasiveness of many biofuel crops, and in particular, the potential risks of cultivating Jatropha. This paper aims to assess the benefits and risks, especially risks,of growing Jatropha for biodiesel production. Jatropha should be screened through a science-based risk-assessment procedure to predict the risk of becoming invasive before it is released for large-scale commercial cultivation.The net GHG savings can be achieved through the cultivation of Jatropha, considering two main factors: no landuse change and crop management without chemical fertilization.展开更多
In this contribution, one-pot tandem conversion of fructose into biofuel components, including 5-ethoxymethylfurfural(EMF), 2,5-(bis(ethoxymethyl)furan(BEMF) and ethyl levulinate(EL), was performed in an in-s...In this contribution, one-pot tandem conversion of fructose into biofuel components, including 5-ethoxymethylfurfural(EMF), 2,5-(bis(ethoxymethyl)furan(BEMF) and ethyl levulinate(EL), was performed in an in-situ generated catalyst system through consecutive dehydration, etherification, and transfer hydrogenation. Specifically, ZrOCl2·8H2O was in-situ decomposed into HCl and ZrO(OH)2 in ethanol, which effectively catalyzed the dehydration/etherification of fructose to 5-ethoxymethylfurfural(EMF) and subsequent reductive etherification of EMF using ethanol as H-donor, respectively. EMF, BEMF and EL were detected as the main products, and total yield of detectable products of up to 65.4% was obtained at 200 ℃ in only 2 h.展开更多
In this study,an amine-coordinated cobalt phthalocyanine(CoPc)-based anodic catalyst was fabricated by a facile process,to enhance the performance of hydrogen peroxide fuel cells(HPFCs) and enzymatic biofuel cells(EBC...In this study,an amine-coordinated cobalt phthalocyanine(CoPc)-based anodic catalyst was fabricated by a facile process,to enhance the performance of hydrogen peroxide fuel cells(HPFCs) and enzymatic biofuel cells(EBCs).For this purpose,polyethyleneimine(PEI) was added onto the reduced graphene oxide and CoPc composite(RGO/CoPc) to create abundant NH2 axial ligand groups,for anchoring the Co core within the CoPc.Owing to the PEI addition,the onset potential of the hydrogen peroxide oxidation reaction was shifted by 0.13 V in the negative direction(0.02 V) and the current density was improved by 1.92 times(1.297 mA cm^(-2)),compared to those for RGO/CoPc(0.15 V and 0.676 mA cm^(-2),respectively),due to the formation of donor-acceptor dyads and the prevention of CoPc from leaching out.The biocatalyst using glucose oxidase(GOx)([RGO/CoPc]/PEI/GOx) showed a better onset potential and catalytic activity(0.15 V and 318.7 μA cm^(-2)) than comparable structures,as well as significantly improved operational durability and long-term stability.This is also attributed to PEI,which created a favorable microenvironment for the enzyme.The maximum power densities(MPDs) and open-circuit voltages(OCVs) obtained for HPFCs and EBCs using the suggested catalyst were 105.2±1.3 μW cm^(-2)(0.317±0.003 V) and 25.4±0.9 μW cm^(-2)(0.283±0.007 V),respectively.This shows that the amine axial ligand effectively improves the performance of the actual driving HPFCs and EBCs.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Owing to an environment-friendly utilization of resources, increased attention has been focused on fuels and chemicals from biomass as an alternative to fossil resources. In addition, supercritical fluid technology has been considered to be an environmentally-benign treatment. Therefore, its technology was applied for a conversion of biomass to useful fuels and chemicals in order to mitigate environmental loading. For example, supercritical water treatment has demonstrated that lignocellulosics can be hydrolyzed to become lignin-derived products for useful aromatic chemicals and carbohydrate-derived products, such as polysaccharides, oligosaccharides and monosaccharides of glucose, mannose and xylose used for subsequent ethanol fermentation. If this treatment is prolonged, lignocellulosics were found to be converted to organic acids such as formic, acetic, glycolic and lactic acids which can be converted to methane for biofuel. When alcohols, such as methanol and ethanol, were used instead of water, some other useful products were achieved, and its liquefied products were found to have a potential for liquid biofuel. In this study, therefore, our research achievements in supercritical fluid science of woody biomass will be introduced for clean and green chemistry for a sustainable environment.
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supported by the East Carolina Christmas Tree Program
文摘Transgenic trees as a new source for biofuel have brought a great interest in tree biotechnology. Genetically modifying forest trees for ethanol production have advantages in technical challenges, costs, environmental concerns, and financial problems over some of crops. Genetic engineering of forest trees can be used to reduce the level of lignin, to produce the fast-growing trees, to develop trees with higher cellulose, and to allow the trees to be grown more widely. Trees can establish themselves in the field with less care of farmers, compared to most of crops. Transgenic crops as a new source for biofuel have been recently reviewed in several reviews. Here, we overview transgenic woody plants as a new source for biofuel including genetically modified woody plants and environment; main focus of woody plants genetic modifications; solar to chemical energy transfer; cellulose biosynthesis; lignin biosynthesis; and cellulosic ethanol as biofuel.
文摘In this article, the aptitude of natural gas as feedstock in steam reforming process for hydrogen production is compared with that of different liquid fuels (pure compounds and commercial fuels), with the aim to investigate the potentialities of biofuels to overcome the CO2 emission problems deriving from fossil fuel processing. The performances of a nickel based catalyst (commercially used in steam reforming of natural gas) were evaluated in terms of feed conversion and yield to the different products as function of temperature, space velocity and water/fuel ratio. Furthermore, a preliminary evaluation of catalyst durability was effected by monitoring yield to H2 versus time on stream and measuring coke formation at the end of experimental tests. High yields to hydrogen were obtained with all fuels investigated, whereas the deactivation phenomena, which are correlated to carbon deposition on the catalyst, were observed with all tested fuels, except for methane and biofuel.
基金The National Key R&D Program of China(2018YFB1501602)the National Natural Science Foundation of China(21721004 and 22078316)are acknowledged for financial support。
文摘Zeolite-supported metal catalysts containing hydrogenation centers and acid sites are promising in the chemoselective hydrogenation of biomass platform molecules into value-added chemicals and fuels.The primary challenge of employing such bifunctional catalysts for biomass conversion lies in catalyst stability in the liquid phase under harsh conditions. Herein, we have prepared a Ni/La-Y nanocatalyst via an improved wet impregnation method. Compared with Ni nanoparticles on H-Y, La addition shows a significantly enhanced stability and performance in the continuous liquid-phase hydrogenation of γ-valerolactone(GVL) into ethyl pentanoate(EP) at 200 ℃ for 1000 h. Complementary characterization studies reveal that La addition in the metal/zeolite catalyst not only efficiently modulates the acid property of the zeolite to alleviate coke formation, but also suppresses zeolite dealumination and metal agglomeration and leaching upon catalysis over a 1000 h period. These findings provide an efficient approach for improving the stability of zeolite-supported bifunctional catalysts, leading to potential application in hydrogen-assisted biomass valorization under the liquid-phase conditions.
文摘Terpenoids have drawn much attention to scientists in synthesizing high-performance bio-jet fuels due to their ring structures,which feature potential high densities.Here,a facile biphasic catalytic process has been developed for the production of high-density tricyclic hydrocarbon biofuels from a monoterpenoid,1,8-cineole,using sulfuric acid(H2SO4)as the homogeneous catalyst.A^100%conversion of 1,8-cineole and a>40%carbon yield of cyclic dimers were achieved at 100℃within two hours.The mechanism for the acid-catalyzed conversion of 1,8-cineole to cyclic hydrocarbon dimers were explored.In particular,the formation of the diene intermediates and the following dimerization of dienes was essential to synthesize tricyclic terpene dimers.The biphasic catalytic process accelerated the deoxygenation rate and enabled the dimerization with the aid of organic solvent while controlling the reaction rates to avoid the formation of solid residues.Moreover,this process also facilitated the product separation by organic solvent extraction while enabling easy recycle of the homogenous catalysts.
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financial support from Higher Impact Research-Ministry of Higher Education project no D000011-16001 of the Faculty of Engineering,University of Malaya,Malaysia and the Mitsubishi Corporation Education Trust Fund,University Teknologi PETRONAS,Malaysia
文摘The effect of ethanedioic acid(Ed A) functionalization on Al2O3 supported Ni catalyst was studied on the hydrodeoxygenation(HDO), isomerization, kinetics and Arrhenius parameters of octadec-9-enoic acid(OA) into biofuel in this report. This was achieved via synthesis of two catalysts; the first, nickel alumina catalyst(Ni/Al2O3) was via the incorporation of inorganic Ni precursor into Al2O3; the second was via the incorporation nickel oxalate(Ni Ox) prepared by functionalization of Ni with Ed A into Al2O3 to obtain organometallic Ni Ox/Al2O3 catalyst. Their characterization results showed that Ni species present in Ni/Al2O3 and Ni Ox/Al2O3 were 8.2% and 9.3%, respectively according to the energy dispersive X-ray result. Ni Ox/Al2O3 has comparably higher Ni content due to the Ed A functionalization which also increases its acidity and guarantees high Ni dispersion with weaker metal-support-interaction leading to highly reducible Ni as seen in the X-ray diffraction, X-ray photoelectron spectroscopy, TPR and Raman spectroscopy results. Their activities tested on the HDO of OA showed that Ni Ox/Al2O3 did not only display the best catalytic and reusability abilities, but it also possesses isomerization ability due to its increased acidity. The Ni Ox/Al2O3 also has the highest rate constants evaluated using pseudo-first-order kinetics,but the least activation energy of 176 k J/mol in the biofuel formation step compared to 244 k J/mol evaluated when using Ni/Al2O3. The result is promising for future feasibility studies toward commercialization of catalytic HDO of OA into useful biofuel using organometallic catalysts.
文摘In sub-Saharan Africa(SSA), the main goals behind the development of a biofuel industry are employment creation and income generation. Jatropha(Jatropha curcas L.) has emerged as a candidate for biodiesel production. It is a non-edible oil producing, drought-resistant plant that can be grown on marginal land with limited water and low soil fertility. However, these are also attributes that typify weedy and invasive plant species. Adding to these concerns are the general questioning of whether biofuel production will reduce Greenhouse gas(GHG)emissions globally. Currently, there is limited information on the potential invasiveness of many biofuel crops, and in particular, the potential risks of cultivating Jatropha. This paper aims to assess the benefits and risks, especially risks,of growing Jatropha for biodiesel production. Jatropha should be screened through a science-based risk-assessment procedure to predict the risk of becoming invasive before it is released for large-scale commercial cultivation.The net GHG savings can be achieved through the cultivation of Jatropha, considering two main factors: no landuse change and crop management without chemical fertilization.
基金financial support from the National Natural Science Foundation of China (Grant Nos.21706223 21776234+7 种基金 21676223 21506177)the Fundamental Research Funds for the Central Universities (Grant Nos. 20720160087 20720160077)the Natural Science Foundation of Fujian Province of China (Grant Nos. 2016J01077 2015J05034 2014J01209)the Education Department of Fujian Province (Grant No. JZ160398)
文摘In this contribution, one-pot tandem conversion of fructose into biofuel components, including 5-ethoxymethylfurfural(EMF), 2,5-(bis(ethoxymethyl)furan(BEMF) and ethyl levulinate(EL), was performed in an in-situ generated catalyst system through consecutive dehydration, etherification, and transfer hydrogenation. Specifically, ZrOCl2·8H2O was in-situ decomposed into HCl and ZrO(OH)2 in ethanol, which effectively catalyzed the dehydration/etherification of fructose to 5-ethoxymethylfurfural(EMF) and subsequent reductive etherification of EMF using ethanol as H-donor, respectively. EMF, BEMF and EL were detected as the main products, and total yield of detectable products of up to 65.4% was obtained at 200 ℃ in only 2 h.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(Nos.2017R1D1A1B03032033 and 2020R1C1C1010386)“Leaders in INdustry-university Cooperation+”project supported by the Ministry of Education and National Research Foundation of Korea。
文摘In this study,an amine-coordinated cobalt phthalocyanine(CoPc)-based anodic catalyst was fabricated by a facile process,to enhance the performance of hydrogen peroxide fuel cells(HPFCs) and enzymatic biofuel cells(EBCs).For this purpose,polyethyleneimine(PEI) was added onto the reduced graphene oxide and CoPc composite(RGO/CoPc) to create abundant NH2 axial ligand groups,for anchoring the Co core within the CoPc.Owing to the PEI addition,the onset potential of the hydrogen peroxide oxidation reaction was shifted by 0.13 V in the negative direction(0.02 V) and the current density was improved by 1.92 times(1.297 mA cm^(-2)),compared to those for RGO/CoPc(0.15 V and 0.676 mA cm^(-2),respectively),due to the formation of donor-acceptor dyads and the prevention of CoPc from leaching out.The biocatalyst using glucose oxidase(GOx)([RGO/CoPc]/PEI/GOx) showed a better onset potential and catalytic activity(0.15 V and 318.7 μA cm^(-2)) than comparable structures,as well as significantly improved operational durability and long-term stability.This is also attributed to PEI,which created a favorable microenvironment for the enzyme.The maximum power densities(MPDs) and open-circuit voltages(OCVs) obtained for HPFCs and EBCs using the suggested catalyst were 105.2±1.3 μW cm^(-2)(0.317±0.003 V) and 25.4±0.9 μW cm^(-2)(0.283±0.007 V),respectively.This shows that the amine axial ligand effectively improves the performance of the actual driving HPFCs and EBCs.