Microalgae biomass is an ideal precursor to prepare renewable carbon materials,which has broad application.The bioaccumulation efficiency(lipids,proteins,carbohydrates)and biomass productivity of microalgae are influe...Microalgae biomass is an ideal precursor to prepare renewable carbon materials,which has broad application.The bioaccumulation efficiency(lipids,proteins,carbohydrates)and biomass productivity of microalgae are influenced by spectroscopy during the culture process.In this study,a bilayer plate-type photobioreactor was designed to cultivate Chlorella protothecoides with spectral selectivity by nanofluids.Compared to culture without spectral selectivity,the spectral selectivity of Ag/CoSO_(4)nanofluids increased microalgae biomass by 5.76%,and the spectral selectivity of CoSO_(4)solution increased by 17.14%.In addition,the spectral selectivity of Ag/CoSO_(4)nanofluids was more conducive to the accumulation of nutrients(29.46%lipids,50.66%proteins,and 17.86%carbohydrates)in microalgae.Further cultured chlorella was utilized to prepare bioelectrode materials,it was found that algal based biochar had a good pore structure(micro specific surface area:1627.5314 m^(2)/g,average pore size:0.21294 nm).As the current density was 1 A/g,the specific capacitance reached 230 F/g,appearing good electrochemical performance.展开更多
Double-perovskite type oxide LaSrFeCoO(LSFCO) was used as oxygen carrier for chemical looping steam methane reforming(CL-SMR) due to its unique structure and reactivity. Two different oxidation routes,steam-oxidat...Double-perovskite type oxide LaSrFeCoO(LSFCO) was used as oxygen carrier for chemical looping steam methane reforming(CL-SMR) due to its unique structure and reactivity. Two different oxidation routes,steam-oxidation and steam-air-stepwise-oxidation, were applied to investigate the recovery behaviors of the lattice oxygen in the oxygen carrier. The characterizations of the oxide were determined by X-ray diffraction(XRD), X-ray photoelectron spectroscopy(XPS), hydrogen temperature-programmed reduction(H-TPR) and scanning electron microscopy(SEM). The fresh sample LSFCO exhibits a monocrystalline perovskite structure with cubic symmetry and high crystallinity, except for a little impurity phase due to the antisite defect of Fe/Co disorder. The deconvolution distribution of XPS patterns indicated that Co,and Fe are predominantly in an oxidized state(Feand Fe) and(Coand Co), while O 1s exists at three species of lattice oxygen, chemisorbed oxygen and physical adsorbed oxygen. The double perovskite structure and chemical composition recover to the original state after the steam and air oxidation, while the Co ion cannot incorporate into the double perovskite structure and thus form the CoO just via individual steam oxidation. In comparison to the two different oxidation routes, the sample obtained by steam-oxidation exhibits even higher CHconversion, CO and Hselectivity and stronger hydrogen generation capacity.展开更多
Chemical looping dry reforming(CLDR) is an innovative technology for CO2 utilization using the chemical looping principle.The CLDR process consists of three stages,i.e.CH4 reduction,CO2 reforming,and air oxidation.S...Chemical looping dry reforming(CLDR) is an innovative technology for CO2 utilization using the chemical looping principle.The CLDR process consists of three stages,i.e.CH4 reduction,CO2 reforming,and air oxidation.Spinel nickel ferrite(NiFe2O4) was prepared and its multi-cycle performance as an oxygen carrier for CLDR was experimentally investigated.X-ray diffraction(XRD) and Laser Raman spectroscopy showed that a pure spinel crystalline phase(NiFe2O4) was obtained by a parallel flow co-precipitating method.NiFe2O4was reduced into Fe-Ni alloy and wustite(FexO) during the CH4 reduction process.Subsequent oxidation of the reduced oxygen carrier was performed with CO2 as an oxidant to form an intermediate state:a mixture of spinel Ni(1-x)Fe(2+x)O4,Fe(2+y)O4 and metallic Ni.And CO was generated in parallel during this stage.Approximate 185 mL of CO was generated for 1 g spinel NiFe2O4 in a single cycle.The intermediate oxygen carrier was fully oxidized in the air oxidation stage to form a mixture of Ni(1+x)Fe(2-x)O4 and Fe2O3.Although the original state of oxygen carrier(NiFe2O4) was not fully regenerated and agglomeration was observed,a good recyclability was shown in 10 successive redox cycles.展开更多
Thermodynamic parameters of chemical reactions in the system were carried out through thermodynamic analysis. According to the Gibbs free energy minimization principle of the system, equilibrium composition of the rea...Thermodynamic parameters of chemical reactions in the system were carried out through thermodynamic analysis. According to the Gibbs free energy minimization principle of the system, equilibrium composition of the reactions of chemical-looping gasification (CLG) of biomass with natural hematite (Fe2O3) as oxygen carrier were analyzed using commercial software of HSC Chemistry 5.1. The feasibility of the CLG of biomass with hematite was experimental verified in a lab-scale bubbling fluidized bed reactor using argon as fluidizing gas. It was indicated the experimental results were consistent with the theoretical analysis. The presence of oxygen carrier gave a significant effect on the biomass conversion and improved the synthesis gas yield obviously. It was observed that the gas content of CO and H2 was over 70% in CLG of biomass. The reduced hematite particles mainly existed in form of FeO. It was showed that the reduction of natural hematite with biomass proceeds in a stepwise manner from Fe2O3 →Fe3O4→ FeO. Reduction product of natural hematite can be restored the lattice oxygen by oxidation with air.展开更多
Fe_(2)O_(3)/Al_(2)O_(3) and Fe_(2)O_(3)/Al_(2)O_(3) modified by low content of Ni(below 2%in weight)oxygen carriers were prepared by mechanical mixing and impregnation method.The synthesized oxygen carriers were chara...Fe_(2)O_(3)/Al_(2)O_(3) and Fe_(2)O_(3)/Al_(2)O_(3) modified by low content of Ni(below 2%in weight)oxygen carriers were prepared by mechanical mixing and impregnation method.The synthesized oxygen carriers were characterized by means of X-ray diffraction(XRD),X-ray fluorescence(XRF),scanning electron microscopy(SEM),BET-surface area and temperature programmed reduction(TPR).Besides,redox cyclic reactivity and the performance of chemical looping reforming of methane of the oxygen carriers were studied in a thermal gravimetrical analysis(TGA)and fixed bed at 850℃.It was observed that the redox reactivity of the oxygen carriers is improved by Ni addition because synergic effect may occur between NiO and Fe_(2)O_(3)/Al_(2)O_(3) to form NiFe_(2)O_(4) and NiAl_(2)O_(4) spinel phases.However,the improvement was not apparent as Ni addition reached 1 wt%or more because more nickel loaded resulted in methane decomposition into H2 and carbon leading to carbon deposition.The SEM and BET analysis showed that NiFe_(2)O_(4) and NiAl_(2)O_(4) particles dispersed into the pores of the Fe_(2)O_(3)/Al_(2)O_(3) particles in the course of preparation.In addition,the resistance to sintering of the modified samples increased with the Ni addition increasing.The results of successive redox cycles showed that the Ni modified Fe_(2)O_(3)/Al_(2)O_(3) oxygen carriers have good regenerability.With integration of reactivity and carbon deposition,the content 1.04 wt%of nickel doping was an optimal amount in the three modified samples.展开更多
基金This work was supported by the Key Research and Development Project of Jiangsu Province(BE2019009-4)the National Natural Science Foundation of China(52106091)the Qing Lan Project of Jiangsu Province。
文摘Microalgae biomass is an ideal precursor to prepare renewable carbon materials,which has broad application.The bioaccumulation efficiency(lipids,proteins,carbohydrates)and biomass productivity of microalgae are influenced by spectroscopy during the culture process.In this study,a bilayer plate-type photobioreactor was designed to cultivate Chlorella protothecoides with spectral selectivity by nanofluids.Compared to culture without spectral selectivity,the spectral selectivity of Ag/CoSO_(4)nanofluids increased microalgae biomass by 5.76%,and the spectral selectivity of CoSO_(4)solution increased by 17.14%.In addition,the spectral selectivity of Ag/CoSO_(4)nanofluids was more conducive to the accumulation of nutrients(29.46%lipids,50.66%proteins,and 17.86%carbohydrates)in microalgae.Further cultured chlorella was utilized to prepare bioelectrode materials,it was found that algal based biochar had a good pore structure(micro specific surface area:1627.5314 m^(2)/g,average pore size:0.21294 nm).As the current density was 1 A/g,the specific capacitance reached 230 F/g,appearing good electrochemical performance.
基金The financial support of the National Natural Science Foundation of China(51406208,51406214)supported by the Science&Technology Research Project of Guangdong Province(2015A010106009)the support of Key Laboratory of Renewable Energy,Chinese Academy of Sciences(Y607j51001)
文摘Double-perovskite type oxide LaSrFeCoO(LSFCO) was used as oxygen carrier for chemical looping steam methane reforming(CL-SMR) due to its unique structure and reactivity. Two different oxidation routes,steam-oxidation and steam-air-stepwise-oxidation, were applied to investigate the recovery behaviors of the lattice oxygen in the oxygen carrier. The characterizations of the oxide were determined by X-ray diffraction(XRD), X-ray photoelectron spectroscopy(XPS), hydrogen temperature-programmed reduction(H-TPR) and scanning electron microscopy(SEM). The fresh sample LSFCO exhibits a monocrystalline perovskite structure with cubic symmetry and high crystallinity, except for a little impurity phase due to the antisite defect of Fe/Co disorder. The deconvolution distribution of XPS patterns indicated that Co,and Fe are predominantly in an oxidized state(Feand Fe) and(Coand Co), while O 1s exists at three species of lattice oxygen, chemisorbed oxygen and physical adsorbed oxygen. The double perovskite structure and chemical composition recover to the original state after the steam and air oxidation, while the Co ion cannot incorporate into the double perovskite structure and thus form the CoO just via individual steam oxidation. In comparison to the two different oxidation routes, the sample obtained by steam-oxidation exhibits even higher CHconversion, CO and Hselectivity and stronger hydrogen generation capacity.
基金the financial support by the National Natural Science Foundation of China(51406214 and51406208)supported by the Natural science Foundation of Guangdong Province(2015A030313719)the Science&Technology Research Project of Guangdong Province(2013B050800008)
文摘Chemical looping dry reforming(CLDR) is an innovative technology for CO2 utilization using the chemical looping principle.The CLDR process consists of three stages,i.e.CH4 reduction,CO2 reforming,and air oxidation.Spinel nickel ferrite(NiFe2O4) was prepared and its multi-cycle performance as an oxygen carrier for CLDR was experimentally investigated.X-ray diffraction(XRD) and Laser Raman spectroscopy showed that a pure spinel crystalline phase(NiFe2O4) was obtained by a parallel flow co-precipitating method.NiFe2O4was reduced into Fe-Ni alloy and wustite(FexO) during the CH4 reduction process.Subsequent oxidation of the reduced oxygen carrier was performed with CO2 as an oxidant to form an intermediate state:a mixture of spinel Ni(1-x)Fe(2+x)O4,Fe(2+y)O4 and metallic Ni.And CO was generated in parallel during this stage.Approximate 185 mL of CO was generated for 1 g spinel NiFe2O4 in a single cycle.The intermediate oxygen carrier was fully oxidized in the air oxidation stage to form a mixture of Ni(1+x)Fe(2-x)O4 and Fe2O3.Although the original state of oxygen carrier(NiFe2O4) was not fully regenerated and agglomeration was observed,a good recyclability was shown in 10 successive redox cycles.
文摘Thermodynamic parameters of chemical reactions in the system were carried out through thermodynamic analysis. According to the Gibbs free energy minimization principle of the system, equilibrium composition of the reactions of chemical-looping gasification (CLG) of biomass with natural hematite (Fe2O3) as oxygen carrier were analyzed using commercial software of HSC Chemistry 5.1. The feasibility of the CLG of biomass with hematite was experimental verified in a lab-scale bubbling fluidized bed reactor using argon as fluidizing gas. It was indicated the experimental results were consistent with the theoretical analysis. The presence of oxygen carrier gave a significant effect on the biomass conversion and improved the synthesis gas yield obviously. It was observed that the gas content of CO and H2 was over 70% in CLG of biomass. The reduced hematite particles mainly existed in form of FeO. It was showed that the reduction of natural hematite with biomass proceeds in a stepwise manner from Fe2O3 →Fe3O4→ FeO. Reduction product of natural hematite can be restored the lattice oxygen by oxidation with air.
基金The financial support of the National Natural Science Foundation of China(No.51076154)is gratefully acknowledgedThis work was also supported by the National Key Technology R&D Program of 12^(th) Five-Year Plan of China(No.2011BAD15B05)the Science&Technology Research Project of Guangdong Province(No.2010B010900047).
文摘Fe_(2)O_(3)/Al_(2)O_(3) and Fe_(2)O_(3)/Al_(2)O_(3) modified by low content of Ni(below 2%in weight)oxygen carriers were prepared by mechanical mixing and impregnation method.The synthesized oxygen carriers were characterized by means of X-ray diffraction(XRD),X-ray fluorescence(XRF),scanning electron microscopy(SEM),BET-surface area and temperature programmed reduction(TPR).Besides,redox cyclic reactivity and the performance of chemical looping reforming of methane of the oxygen carriers were studied in a thermal gravimetrical analysis(TGA)and fixed bed at 850℃.It was observed that the redox reactivity of the oxygen carriers is improved by Ni addition because synergic effect may occur between NiO and Fe_(2)O_(3)/Al_(2)O_(3) to form NiFe_(2)O_(4) and NiAl_(2)O_(4) spinel phases.However,the improvement was not apparent as Ni addition reached 1 wt%or more because more nickel loaded resulted in methane decomposition into H2 and carbon leading to carbon deposition.The SEM and BET analysis showed that NiFe_(2)O_(4) and NiAl_(2)O_(4) particles dispersed into the pores of the Fe_(2)O_(3)/Al_(2)O_(3) particles in the course of preparation.In addition,the resistance to sintering of the modified samples increased with the Ni addition increasing.The results of successive redox cycles showed that the Ni modified Fe_(2)O_(3)/Al_(2)O_(3) oxygen carriers have good regenerability.With integration of reactivity and carbon deposition,the content 1.04 wt%of nickel doping was an optimal amount in the three modified samples.