Electro-oxidation of Ce ( Ⅲ ) to Ce ( Ⅳ ) in parallel plate flow type electrolyzer divided with cation exchange membrane was carried out in nitric acid media at carbon felt anode under galvanostatic conditions. ...Electro-oxidation of Ce ( Ⅲ ) to Ce ( Ⅳ ) in parallel plate flow type electrolyzer divided with cation exchange membrane was carried out in nitric acid media at carbon felt anode under galvanostatic conditions. Carbon felt was used as an anode for its high specific surface area and high oxygen evolution overpotential. Pt coated Ti plates were used as cathode and anode current feeder. The oxidation of 1 mol· L^-1 Ce( Ⅲ ) solution in 2 mol· L^- 1 HNO3 was proceeding with a high current efficiency (92%) until about 80% of Ce( Ⅲ ) was oxidized. Then, oxygen evolution, accompanied by terminal voltage jump, took place, lowering current efficiency. Ce( Ⅲ ) was oxidized up to 90% with current efficiency of 62%. In this mode, strong carbon felt anode oxidation was observed. The wear out of carbon felt was 46% in six consequent runs (6 h of operation). After each run, carbon felt surface had to be renewed with slightly alkaline solution to remove carbon oxidation products and ensure regular operational conditions. When anode surface was blocked, oxygen evolution took place from the beginning of electrolysis due to higher actual current density. The wear out of carbon felt anode could be minimized by means of oxygen evolution prevention. In the case when electrolysis had been stopped before oxygen evolution started (at Ce( Ⅳ ) conversion of about 80% ), the wear out of anode was less than 2% during 6 consequent runs (4 h of operation).展开更多
Surface electropositivity and low internal resistance are important factors to improve the anode performance in microbial fuel cells (MFCs). Nitrogen doping is an effective way for the modification of traditional carb...Surface electropositivity and low internal resistance are important factors to improve the anode performance in microbial fuel cells (MFCs). Nitrogen doping is an effective way for the modification of traditional carbon materials. In this work, heat treatment and melamine were used to modify carbon felts to enhance electrogenesis capacity of MFCs. The modified carbon felts were characterized using X-ray photoelectron spectroscopy (XPS), scanning electron microscope (SEM), atomic force microscopy (AFM) and malvern zeta potentiometer. Results show that the maximum power densities under heat treatment increase from 276.1 to 423.4 mW/m(2) (700 degrees C) and 461.5 mW/m(2) (1200 degrees C) and further increase to 472.5 mW/m(2) (700 degrees C) and 515.4 mW/m(2) (1200 degrees C) with the co-carbonization modification of melamine. The heat treatment reduces the material resistivity, improves the zeta potential which is beneficial to microbial adsorption and electron transfer. The addition of melamine leads to the higher content of surface pyridinic and quaternary nitrogen and higher zeta potential. It is related to higher MFCs performance. Generally, the melamine modification at high temperature increases the feasibility of carbon felt as MFCs's anode materials. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.展开更多
Prussian blue (PB) modified carbon felt electrodes were prepared. The electrochemical behavior was investigated by cyclic voltammetry, electrochemical impedance spectroscopy and charge-discharge experiments. In order ...Prussian blue (PB) modified carbon felt electrodes were prepared. The electrochemical behavior was investigated by cyclic voltammetry, electrochemical impedance spectroscopy and charge-discharge experiments. In order to distinguish the mechanism of the PB modified carbon felt electrode, the electrochemical quartz crystal microbalance (EQCM) was employed. The results of cyclic voltammetry show that the modification can improve the reversibility and the suitable PB deposition is the amount of 10 circles deposition. PB modified carbon felt electrode can effectively decrease the charge transfer resistance. The voltage efficiency of VRB employing PB modified carbon felt electrode can be increased by 12%. The mass change of the PB modified Pt crystal electrode in the process of the potential scan is obvious. The reaction of substitution of VO2+ for high-spin Fe ion in PB is probable to happen and the possible reaction equation is given. The preliminary exploration shows that PB modified carbon felt is electrochemically promising for redox flow battery.展开更多
Poly(pheniothiazine) films were prepared on a porous carbon felt(CF) electrode surface by an electrooxidative polymerization of three phenothiazine derivatives(i.e.,Tthionine(TN),Toluidine Blue(TB) and Methyl...Poly(pheniothiazine) films were prepared on a porous carbon felt(CF) electrode surface by an electrooxidative polymerization of three phenothiazine derivatives(i.e.,Tthionine(TN),Toluidine Blue(TB) and Methylene Blue(MB)) from 0.1 mol/L phosphate buffer solution(pH 7.0).Among the three phenothiazies,the poly(TB) film-modified CF exhibited an excellent electrocatalytic activity for the oxidation of nicotinamide adenine dinucleotide reduced form(NADH) at +0.2 V vs.Ag/AgCl.The poly(TB) film-modified CF was successfully used as working electrode unit of highly sensitive amperometric flow-through detector for NADH.The peak currents(peak heights) were almost unchanged,irrespective of a carrier flow rate ranging from 2.0 to 4.1 mL/min,resulting in the measurement of NADH(ca.30 samples/hr) at 4.1 mL/min.The peak current responses of NADH showed linear relationship over the concentration range from 1 to 30 μmol/L(sensitivity:0.318 μA/(μmol/L);correlation coefficient:0.997).The lower detection limit was found to be 0.3 μmol/L(S/N = 3).展开更多
Tyrosinase(TYR) was covalently immobilized onto amino-functionalized carbon felt surface via glutaraldehyde-coupling under ultrasonic treatment for 10 min.The resulting TYR-immobilized carbon felt was used as a work...Tyrosinase(TYR) was covalently immobilized onto amino-functionalized carbon felt surface via glutaraldehyde-coupling under ultrasonic treatment for 10 min.The resulting TYR-immobilized carbon felt was used as a working electrode unit of bioelectrocatalytic flow-through detector for TYR substrates(catechol,p-chlorophenol(p-CP),p-cresol,phenol etc.).Cathodic peak currents based on the electroreduction of enzymatically produced o-quinones were detected at-50 mV vs.Ag/AgCl.Compared with previous work in which TYR was immobilized onto amino-functionalized carbon felt for 16 hr without the ultrasonic treatment,we succeeded in(1) shortening the enzyme immobilization time from 16 hr to 10 min,(2) enhancing the sensitivity of p-CP,and(3) improving the operational stability of p-CP.The ultrasonic treatment during the TYR immobilization step would lead to certain changes in the structure of the immobilized TYR and the morphology of the immobilized TYR-layer on the carbon felt surface.展开更多
TiO2-coated carbon felt(TCF)composite catalysts have been prepared via a supercritical treatment of titanium tetraisopropoxide(TTIP)as the precursor.The physical properties of the catalysts were characterized by means...TiO2-coated carbon felt(TCF)composite catalysts have been prepared via a supercritical treatment of titanium tetraisopropoxide(TTIP)as the precursor.The physical properties of the catalysts were characterized by means of thermogravimetric and differential thermal analysis(TG–DTA),X-ray diffraction(XRD),fluorescence spectroscopy,scanning electron microscopy (SEM),and BET surface areas techniques.The photocatalytic activities of the materials were evaluated using the degradation of Congo red(CR)as a probe reaction.All the composites showed much higher photocatalytic activity than commercial P25 due to significant synergistic effects.Reused TCF retained high photocatalytic activity for degradation of CR.The photocatalytic efficiency in CR degradation was found to be strongly dependent on the TiO2-coating ratio and calcination temperature.A possible mechanism for the enhanced reactivity involves shuttling of electrons from TiO2 particles to the carbon felt(CF)as a result of an optimal arrangement in TCF that stabilizes charge separation and reduces charge recombination.In addition to the significant synergistic effects,the abundant spaces between adjacent carbon fibers allow UV light to penetrate into the felt-like photocatalyst to a considerable depth,so that a three-dimensional environment is available for the photocatalytic reaction.展开更多
The recent development of portable electronics promotes the growing demand for flexible energy storage devices. Supercapacitors are promising candidates due to their high power density. Therefore, flexible supercapaci...The recent development of portable electronics promotes the growing demand for flexible energy storage devices. Supercapacitors are promising candidates due to their high power density. Therefore, flexible supercapacitors are desired. Here, the porous activated carbon felts(ACFs) with exfoliated graphene nanosheets and rich oxygen-containing groups were fabricated by a facile thermal treatment strategy.Such ACFs can act as the flexible electrodes of all-solid-state supercapacitors directly without the use of binder and conductive materials. They exhibit excellent electrochemical properties, such as high specific areal capacitance, superior rate ability and long-term cycling stability. Moreover, the fabricated flexible all-solid-state supercapacitors based on ACFs deliver stable electrochemical performance under different bending states.展开更多
文摘Electro-oxidation of Ce ( Ⅲ ) to Ce ( Ⅳ ) in parallel plate flow type electrolyzer divided with cation exchange membrane was carried out in nitric acid media at carbon felt anode under galvanostatic conditions. Carbon felt was used as an anode for its high specific surface area and high oxygen evolution overpotential. Pt coated Ti plates were used as cathode and anode current feeder. The oxidation of 1 mol· L^-1 Ce( Ⅲ ) solution in 2 mol· L^- 1 HNO3 was proceeding with a high current efficiency (92%) until about 80% of Ce( Ⅲ ) was oxidized. Then, oxygen evolution, accompanied by terminal voltage jump, took place, lowering current efficiency. Ce( Ⅲ ) was oxidized up to 90% with current efficiency of 62%. In this mode, strong carbon felt anode oxidation was observed. The wear out of carbon felt was 46% in six consequent runs (6 h of operation). After each run, carbon felt surface had to be renewed with slightly alkaline solution to remove carbon oxidation products and ensure regular operational conditions. When anode surface was blocked, oxygen evolution took place from the beginning of electrolysis due to higher actual current density. The wear out of carbon felt anode could be minimized by means of oxygen evolution prevention. In the case when electrolysis had been stopped before oxygen evolution started (at Ce( Ⅳ ) conversion of about 80% ), the wear out of anode was less than 2% during 6 consequent runs (4 h of operation).
文摘Surface electropositivity and low internal resistance are important factors to improve the anode performance in microbial fuel cells (MFCs). Nitrogen doping is an effective way for the modification of traditional carbon materials. In this work, heat treatment and melamine were used to modify carbon felts to enhance electrogenesis capacity of MFCs. The modified carbon felts were characterized using X-ray photoelectron spectroscopy (XPS), scanning electron microscope (SEM), atomic force microscopy (AFM) and malvern zeta potentiometer. Results show that the maximum power densities under heat treatment increase from 276.1 to 423.4 mW/m(2) (700 degrees C) and 461.5 mW/m(2) (1200 degrees C) and further increase to 472.5 mW/m(2) (700 degrees C) and 515.4 mW/m(2) (1200 degrees C) with the co-carbonization modification of melamine. The heat treatment reduces the material resistivity, improves the zeta potential which is beneficial to microbial adsorption and electron transfer. The addition of melamine leads to the higher content of surface pyridinic and quaternary nitrogen and higher zeta potential. It is related to higher MFCs performance. Generally, the melamine modification at high temperature increases the feasibility of carbon felt as MFCs's anode materials. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.
基金Project (2008ZX07313-005) supported by the National Water Pollution Control and Management of Major Special Science and Technology Foundation
文摘Prussian blue (PB) modified carbon felt electrodes were prepared. The electrochemical behavior was investigated by cyclic voltammetry, electrochemical impedance spectroscopy and charge-discharge experiments. In order to distinguish the mechanism of the PB modified carbon felt electrode, the electrochemical quartz crystal microbalance (EQCM) was employed. The results of cyclic voltammetry show that the modification can improve the reversibility and the suitable PB deposition is the amount of 10 circles deposition. PB modified carbon felt electrode can effectively decrease the charge transfer resistance. The voltage efficiency of VRB employing PB modified carbon felt electrode can be increased by 12%. The mass change of the PB modified Pt crystal electrode in the process of the potential scan is obvious. The reaction of substitution of VO2+ for high-spin Fe ion in PB is probable to happen and the possible reaction equation is given. The preliminary exploration shows that PB modified carbon felt is electrochemically promising for redox flow battery.
基金financially supported in part by the Open Research Center Project of the Ministry of Education,Science and Culture of Japan
文摘Poly(pheniothiazine) films were prepared on a porous carbon felt(CF) electrode surface by an electrooxidative polymerization of three phenothiazine derivatives(i.e.,Tthionine(TN),Toluidine Blue(TB) and Methylene Blue(MB)) from 0.1 mol/L phosphate buffer solution(pH 7.0).Among the three phenothiazies,the poly(TB) film-modified CF exhibited an excellent electrocatalytic activity for the oxidation of nicotinamide adenine dinucleotide reduced form(NADH) at +0.2 V vs.Ag/AgCl.The poly(TB) film-modified CF was successfully used as working electrode unit of highly sensitive amperometric flow-through detector for NADH.The peak currents(peak heights) were almost unchanged,irrespective of a carrier flow rate ranging from 2.0 to 4.1 mL/min,resulting in the measurement of NADH(ca.30 samples/hr) at 4.1 mL/min.The peak current responses of NADH showed linear relationship over the concentration range from 1 to 30 μmol/L(sensitivity:0.318 μA/(μmol/L);correlation coefficient:0.997).The lower detection limit was found to be 0.3 μmol/L(S/N = 3).
基金supported in part by the Open Research Center Project of the Ministry of Education,Science and Culture of Japan
文摘Tyrosinase(TYR) was covalently immobilized onto amino-functionalized carbon felt surface via glutaraldehyde-coupling under ultrasonic treatment for 10 min.The resulting TYR-immobilized carbon felt was used as a working electrode unit of bioelectrocatalytic flow-through detector for TYR substrates(catechol,p-chlorophenol(p-CP),p-cresol,phenol etc.).Cathodic peak currents based on the electroreduction of enzymatically produced o-quinones were detected at-50 mV vs.Ag/AgCl.Compared with previous work in which TYR was immobilized onto amino-functionalized carbon felt for 16 hr without the ultrasonic treatment,we succeeded in(1) shortening the enzyme immobilization time from 16 hr to 10 min,(2) enhancing the sensitivity of p-CP,and(3) improving the operational stability of p-CP.The ultrasonic treatment during the TYR immobilization step would lead to certain changes in the structure of the immobilized TYR and the morphology of the immobilized TYR-layer on the carbon felt surface.
基金supported by the Natural Science Foundation of Hunan Province (09JJ6101)the National Natural Science Foundation of China (50802034)
文摘TiO2-coated carbon felt(TCF)composite catalysts have been prepared via a supercritical treatment of titanium tetraisopropoxide(TTIP)as the precursor.The physical properties of the catalysts were characterized by means of thermogravimetric and differential thermal analysis(TG–DTA),X-ray diffraction(XRD),fluorescence spectroscopy,scanning electron microscopy (SEM),and BET surface areas techniques.The photocatalytic activities of the materials were evaluated using the degradation of Congo red(CR)as a probe reaction.All the composites showed much higher photocatalytic activity than commercial P25 due to significant synergistic effects.Reused TCF retained high photocatalytic activity for degradation of CR.The photocatalytic efficiency in CR degradation was found to be strongly dependent on the TiO2-coating ratio and calcination temperature.A possible mechanism for the enhanced reactivity involves shuttling of electrons from TiO2 particles to the carbon felt(CF)as a result of an optimal arrangement in TCF that stabilizes charge separation and reduces charge recombination.In addition to the significant synergistic effects,the abundant spaces between adjacent carbon fibers allow UV light to penetrate into the felt-like photocatalyst to a considerable depth,so that a three-dimensional environment is available for the photocatalytic reaction.
基金supported by National Natural Science Foundation of China (Nos. 21573116, 51822205 and 21875121)Ministry of Science and Technology of China (No. 2017YFA0206701)+1 种基金Ministry of Education of China (No. B12015)the Young Thousand Talents Program
文摘The recent development of portable electronics promotes the growing demand for flexible energy storage devices. Supercapacitors are promising candidates due to their high power density. Therefore, flexible supercapacitors are desired. Here, the porous activated carbon felts(ACFs) with exfoliated graphene nanosheets and rich oxygen-containing groups were fabricated by a facile thermal treatment strategy.Such ACFs can act as the flexible electrodes of all-solid-state supercapacitors directly without the use of binder and conductive materials. They exhibit excellent electrochemical properties, such as high specific areal capacitance, superior rate ability and long-term cycling stability. Moreover, the fabricated flexible all-solid-state supercapacitors based on ACFs deliver stable electrochemical performance under different bending states.