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
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
Vanadium redox flow batteries(VRFBs)are one of the most promising energy storage systems owing to their safety,efficiency,flexibility and scalability.However,the commercial viability of VRFBs is still hindered by the ...Vanadium redox flow batteries(VRFBs)are one of the most promising energy storage systems owing to their safety,efficiency,flexibility and scalability.However,the commercial viability of VRFBs is still hindered by the low electrochemical performance of the available carbon-based electrodes.Defect engineering is a powerful strategy to enhance the redox catalytic activity of carbon-based electrodes for VRFBs.In this paper,uniform carbon defects are introduced on the surfaces of carbon felt(CF)electrode by Ar plasma etching.Together with a higher specific surface area,the Ar plasma treated CF offers additional catalytic sites,allowing faster and more reversible oxidation/reduction reactions of vanadium ions.As a result,the VRFB using plasma treated electrode shows a power density of 1018.3 mW/cm^(2),an energy efficiency(EE)of 84.5%,and the EE remains stable over 1000 cycles.展开更多
Redox flow batteries offer a potential solution to an increase in renewable energy generation on the grid by offering long-term, large-scale storage and regulation of power. However, they are currently un- derutilised...Redox flow batteries offer a potential solution to an increase in renewable energy generation on the grid by offering long-term, large-scale storage and regulation of power. However, they are currently un- derutilised due to cost and performance issues, many of which are linked to the microstructure of the porous carbon electrodes used. Here, for the first time, we offer a detailed study of the in situ effects of compression on a commercially available carbon felt electrode. Visualisation of electrode structure us- ing X-ray computed tomography shows the non-linear way that these materials compress and various metrics are used to elucidate the changes in porosity, pore size distribution and tortuosity factor under compressions from 0%-90%.展开更多
Nickel hexacyanoferrate (NiHCF) film was synthesized on porous three-dimensional carbon felt (PTCF) substrate by repetitious batch chemical depositions, and the NiHCF/PTCF electrode was used as electrochemically switc...Nickel hexacyanoferrate (NiHCF) film was synthesized on porous three-dimensional carbon felt (PTCF) substrate by repetitious batch chemical depositions, and the NiHCF/PTCF electrode was used as electrochemically switched ion exchange (ESIX) electrode in a packed bed for continuous separation for cesium ions. The morphologies of the prepared electrodes were characterized by scanning electron microscopy and the effects of solution concentration on the ion-exchange capacity of the electrodes were investigated by cyclic voltammetry technique. Cycling stability and long-term storage stability of NiHCF/PTCF electrodes were also studied. The NiHCF/PTCF electrodes with excellent ion-exchange ability were used to assemble a diaphragm-isolated ESIX reactor for cesium separation. Continuous separation of cesium and regeneration of NiHCF/PTCF electrode based on the diaphragm-isolated reactor were performed in a laboratory-scale two-electrode system.展开更多
Advanced zinc-cerium redox flow battery(ZCRFB) is a large-scale energy storage system which plays a significant role in the application of new energy sources. The requirement of superior cathode with high acitivity ...Advanced zinc-cerium redox flow battery(ZCRFB) is a large-scale energy storage system which plays a significant role in the application of new energy sources. The requirement of superior cathode with high acitivity and fast ion diffusion is a hierarchical porous structure, which was synthesized in this work by a method in which both hard template and soft template were used. The structure and the performance of the cathode prepared here were characterized and evaluated by a variety of techniques such as scanning electron microscopy(SEM), transmission electron microscopy(TEM), X-ray photoelectron spectroscopy(XPS), cyclic voltammetry(CV), linear sweep voltammetry(LSV), and chronoamperometry(CA). There were mainly three types of pore size within the hierarchical porous carbon: 2 μm, 80 nm, and 10 nm. The charge capacity of the cell using hierarchical porous carbon(HPC) as positive electrode was obviously larger than that using carbon felt; the former was 665.5 mAh with a coulombic efficiency of 89.0% and an energy efficiency of 79.0%, whereas the latter was 611.1 mAh with a coulombic efficiency of 81.5% and an energy efficiency of 68.6%. In addition, performance of the ZCRFB using HPC as positive electrode showed a good stability over 50 cycles.These results showed that the hierarchical porous carbon was superior over the carbon felt for application in ZCRFB.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
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
A novel anode material for all-vanadium redox flow battery was synthesized by dispersion coating of sol-gel processed(resorcinol-furaldehyde) mesoporous carbon(MPC) onto the surface of polyacrylonitrile carbon felt(CF...A novel anode material for all-vanadium redox flow battery was synthesized by dispersion coating of sol-gel processed(resorcinol-furaldehyde) mesoporous carbon(MPC) onto the surface of polyacrylonitrile carbon felt(CF).The coated samples were then annealed at 900℃ and1100℃ and the subsequent morphology,surface chemistry,and electrochemical properties of the MPC coated CF were characterized and compared with an uncoated CF.Addition of the MPC coating is shown to dramatically increase surface area while also increasing the number of active surface oxygen groups particularly for samples annealed at 1100℃.MPC coating shows a mixed effect on electrochemical properties.Characterization with cyclic voltammetry reveals the introduction of MPC coating provides roughly 30%increase in peak current density for the oxidation and reduction reactions of the V(IV)/V(V) redox couple,which is attributed to the significantly increased number of active reaction sites.However,MPC coating seems to be accompanied by a reduction in conductivity as demonstrated by increased redox peak separation and charge transfer resistance.This negative effect on conductivity can be mitigated by heat treatment(at or above 1100℃) which improves surface graphitization reducing redox peak separation and charge transfer resistance such that it is comparable with uncoated samples.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
Polysulfide/ferricyanide flow batteries(S/Fe RFBs),with the advantages of abundant earth reservation low cost,high safety,and environmental friendliness,have attracted significant interest and demonstrated noteworthy ...Polysulfide/ferricyanide flow batteries(S/Fe RFBs),with the advantages of abundant earth reservation low cost,high safety,and environmental friendliness,have attracted significant interest and demonstrated noteworthy potential for practical applications.However,the battery performance,including the energy efficiency(EE),voltage efficiency(VE),and power density of the S/Fe RFBs remains low owing to the slow redox kinetics of polysulfide ions.To address these concerns,WS_(2)was selected as the booster and deposited on a commercial carbon felt electrode(WS_(2)-CF)to stimulate the redox reactions of polysulfide ions.With better hydrophilicity and smaller charge-transfer resistance,WS_(2)-CF exhibits enhanced electrochemical activity toward polysulfide redox reactions.Consequently,the battery performance of S/Fe RFB with WS_(2)-CF as the anode has been improved,with EE of 84%,VE of 84%,and a peak power density of 175.7 mW·cm^(-2),which are all higher than the cell only with the bare carbon felt(CF)as electrodes(76%,77%and 155.8 mW·cm^(-2),respectively).Furthermore,the cycling life of the S/Fe RFB with WS_(2)-CF has been prolonged to 2200 cycles with a capacity retention of 96% a 40 mA·cm^(-2)because of the good stability of WS_(2)-CF as the anode.Contrarily,under the same conditions,the S/Fe RFB without WS_(2)-CF terminated after 1500 cycles with a fast capacity decay.The successful utilization of WS_(2)as a booster on an electrode provides an efficient strategy for obtaining advanced S/Fe RFBs for practical applications.展开更多
Green hydrogen production via seawater electrolysis holds a great promise for carbon-neutral energy production. However, the development of efficient and low-cost bifunctional electrocatalysts for seawater electrolysi...Green hydrogen production via seawater electrolysis holds a great promise for carbon-neutral energy production. However, the development of efficient and low-cost bifunctional electrocatalysts for seawater electrolysis at an industrial level remains a significant challenge. Herein, we report a facile approach based on one-dimensional (1D) cobalt carbonate hydroxide (CCH) nanoneedles (NNs) as skeleton and zeolitic imidazolate framework-67 (ZIF-67) as a sacrificial template to construct a self-supported NiCo layered double hydroxide (NiCo LDH) heterostructure nanocage (CCH@NiCo LDH) anchoring on the carbon felt (CF). The NiCo LDHs have hollow features, consisting of ultrathin layered hydroxide nanosheets. Benefiting from the structural advantages, unique carbon substrate and desirable composition, three-dimensional (3D) NiCo LDH nanocages exhibit superior performance as a bifunctional catalyst for overall seawater splitting at an industrial level and good corrosion resistance in alkaline media. In the alkaline seawater (1 M KOH + 0.5 M NaCl), it exhibits low overpotentials of 356 mV for hydrogen evolution reaction (HER) and 433 mV for oxygen evolution reaction (OER) at 400 mA·cm^(−2), much better than most of reported non-noble metal catalysts. Consequently, the obtained CF electrode loading of CCH@NiCo LDH exhibits outstanding performance as anodes and cathodes for overall alkaline seawater splitting, with remarkably low cell voltages of 1.56 and 1.89 V at current densities of 10 and 400 mA·cm^(−2), respectively. Moreover, the robust stability of 100 h is also demonstrated at above 200 mA·cm^(−2) in alkaline seawater. Our present work demonstrates significant potential for constructing effective cost-efficient and non-noble-metal bifunctional electrocatalyst and electrode for industrial seawater splitting.展开更多
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.
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).
基金Project(Xiang Zu [2016] 91) supported by the “100 Talented Teams” of Hunan Province,ChinaProject(2018RS3077) supported by the Huxiang High-level Talents Program,China+2 种基金Project(22002009) supported by the National Natural Science Foundation of ChinaProject(2021JJ40565) supported by the Natural Science Foundation of Hunan Province,ChinaProject(19C0054) supported by the Scientific Research Foundation of Hunan Provincial Education Department,China。
文摘Vanadium redox flow batteries(VRFBs)are one of the most promising energy storage systems owing to their safety,efficiency,flexibility and scalability.However,the commercial viability of VRFBs is still hindered by the low electrochemical performance of the available carbon-based electrodes.Defect engineering is a powerful strategy to enhance the redox catalytic activity of carbon-based electrodes for VRFBs.In this paper,uniform carbon defects are introduced on the surfaces of carbon felt(CF)electrode by Ar plasma etching.Together with a higher specific surface area,the Ar plasma treated CF offers additional catalytic sites,allowing faster and more reversible oxidation/reduction reactions of vanadium ions.As a result,the VRFB using plasma treated electrode shows a power density of 1018.3 mW/cm^(2),an energy efficiency(EE)of 84.5%,and the EE remains stable over 1000 cycles.
基金support from the EPSRC under grants EP/L014289/1 EP/N032888/1 and EP/M014045/1the STFC Global Challenges Network in Batteries and Electrochemical Energy Devices under the grant ST/N002385/1 for facilitation of travelfunding from the Royal Academy of Engineering
文摘Redox flow batteries offer a potential solution to an increase in renewable energy generation on the grid by offering long-term, large-scale storage and regulation of power. However, they are currently un- derutilised due to cost and performance issues, many of which are linked to the microstructure of the porous carbon electrodes used. Here, for the first time, we offer a detailed study of the in situ effects of compression on a commercially available carbon felt electrode. Visualisation of electrode structure us- ing X-ray computed tomography shows the non-linear way that these materials compress and various metrics are used to elucidate the changes in porosity, pore size distribution and tortuosity factor under compressions from 0%-90%.
基金Supported by the National Natural Science Foundation of China (21276173)the National Science Foundation of Shanxi Province (2012011020-5, 2012011006-1)the International Joint Research Project of Shanxi Province (2011081028)
文摘Nickel hexacyanoferrate (NiHCF) film was synthesized on porous three-dimensional carbon felt (PTCF) substrate by repetitious batch chemical depositions, and the NiHCF/PTCF electrode was used as electrochemically switched ion exchange (ESIX) electrode in a packed bed for continuous separation for cesium ions. The morphologies of the prepared electrodes were characterized by scanning electron microscopy and the effects of solution concentration on the ion-exchange capacity of the electrodes were investigated by cyclic voltammetry technique. Cycling stability and long-term storage stability of NiHCF/PTCF electrodes were also studied. The NiHCF/PTCF electrodes with excellent ion-exchange ability were used to assemble a diaphragm-isolated ESIX reactor for cesium separation. Continuous separation of cesium and regeneration of NiHCF/PTCF electrode based on the diaphragm-isolated reactor were performed in a laboratory-scale two-electrode system.
基金supported by National Program on Key Basic Research Project of China(973 Program,2012CB215500)National Natural Science Foundation of China(21361010)
文摘Advanced zinc-cerium redox flow battery(ZCRFB) is a large-scale energy storage system which plays a significant role in the application of new energy sources. The requirement of superior cathode with high acitivity and fast ion diffusion is a hierarchical porous structure, which was synthesized in this work by a method in which both hard template and soft template were used. The structure and the performance of the cathode prepared here were characterized and evaluated by a variety of techniques such as scanning electron microscopy(SEM), transmission electron microscopy(TEM), X-ray photoelectron spectroscopy(XPS), cyclic voltammetry(CV), linear sweep voltammetry(LSV), and chronoamperometry(CA). There were mainly three types of pore size within the hierarchical porous carbon: 2 μm, 80 nm, and 10 nm. The charge capacity of the cell using hierarchical porous carbon(HPC) as positive electrode was obviously larger than that using carbon felt; the former was 665.5 mAh with a coulombic efficiency of 89.0% and an energy efficiency of 79.0%, whereas the latter was 611.1 mAh with a coulombic efficiency of 81.5% and an energy efficiency of 68.6%. In addition, performance of the ZCRFB using HPC as positive electrode showed a good stability over 50 cycles.These results showed that the hierarchical porous carbon was superior over the carbon felt for application in ZCRFB.
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support of UniEnergy Technologies and the University of Washington Clean Energy Institute
文摘A novel anode material for all-vanadium redox flow battery was synthesized by dispersion coating of sol-gel processed(resorcinol-furaldehyde) mesoporous carbon(MPC) onto the surface of polyacrylonitrile carbon felt(CF).The coated samples were then annealed at 900℃ and1100℃ and the subsequent morphology,surface chemistry,and electrochemical properties of the MPC coated CF were characterized and compared with an uncoated CF.Addition of the MPC coating is shown to dramatically increase surface area while also increasing the number of active surface oxygen groups particularly for samples annealed at 1100℃.MPC coating shows a mixed effect on electrochemical properties.Characterization with cyclic voltammetry reveals the introduction of MPC coating provides roughly 30%increase in peak current density for the oxidation and reduction reactions of the V(IV)/V(V) redox couple,which is attributed to the significantly increased number of active reaction sites.However,MPC coating seems to be accompanied by a reduction in conductivity as demonstrated by increased redox peak separation and charge transfer resistance.This negative effect on conductivity can be mitigated by heat treatment(at or above 1100℃) which improves surface graphitization reducing redox peak separation and charge transfer resistance such that it is comparable with uncoated samples.
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financially supported by the NationalNatural Science Foundation of China(No.22209015)Scientific Research Foundation of Hunan Provincial Education Department(Nos.21A0195 and 21C0215)100 Talented Team of Hunan Province(No.XiangZu[2016]91)。
文摘Polysulfide/ferricyanide flow batteries(S/Fe RFBs),with the advantages of abundant earth reservation low cost,high safety,and environmental friendliness,have attracted significant interest and demonstrated noteworthy potential for practical applications.However,the battery performance,including the energy efficiency(EE),voltage efficiency(VE),and power density of the S/Fe RFBs remains low owing to the slow redox kinetics of polysulfide ions.To address these concerns,WS_(2)was selected as the booster and deposited on a commercial carbon felt electrode(WS_(2)-CF)to stimulate the redox reactions of polysulfide ions.With better hydrophilicity and smaller charge-transfer resistance,WS_(2)-CF exhibits enhanced electrochemical activity toward polysulfide redox reactions.Consequently,the battery performance of S/Fe RFB with WS_(2)-CF as the anode has been improved,with EE of 84%,VE of 84%,and a peak power density of 175.7 mW·cm^(-2),which are all higher than the cell only with the bare carbon felt(CF)as electrodes(76%,77%and 155.8 mW·cm^(-2),respectively).Furthermore,the cycling life of the S/Fe RFB with WS_(2)-CF has been prolonged to 2200 cycles with a capacity retention of 96% a 40 mA·cm^(-2)because of the good stability of WS_(2)-CF as the anode.Contrarily,under the same conditions,the S/Fe RFB without WS_(2)-CF terminated after 1500 cycles with a fast capacity decay.The successful utilization of WS_(2)as a booster on an electrode provides an efficient strategy for obtaining advanced S/Fe RFBs for practical applications.
基金supported by the National Natural Science Foundation of China(Nos.51908408 and 21872104)Natural Science Foundation of Tianjin for Distinguished Young Scholar,China(No.20JCJQJC00150).
文摘Green hydrogen production via seawater electrolysis holds a great promise for carbon-neutral energy production. However, the development of efficient and low-cost bifunctional electrocatalysts for seawater electrolysis at an industrial level remains a significant challenge. Herein, we report a facile approach based on one-dimensional (1D) cobalt carbonate hydroxide (CCH) nanoneedles (NNs) as skeleton and zeolitic imidazolate framework-67 (ZIF-67) as a sacrificial template to construct a self-supported NiCo layered double hydroxide (NiCo LDH) heterostructure nanocage (CCH@NiCo LDH) anchoring on the carbon felt (CF). The NiCo LDHs have hollow features, consisting of ultrathin layered hydroxide nanosheets. Benefiting from the structural advantages, unique carbon substrate and desirable composition, three-dimensional (3D) NiCo LDH nanocages exhibit superior performance as a bifunctional catalyst for overall seawater splitting at an industrial level and good corrosion resistance in alkaline media. In the alkaline seawater (1 M KOH + 0.5 M NaCl), it exhibits low overpotentials of 356 mV for hydrogen evolution reaction (HER) and 433 mV for oxygen evolution reaction (OER) at 400 mA·cm^(−2), much better than most of reported non-noble metal catalysts. Consequently, the obtained CF electrode loading of CCH@NiCo LDH exhibits outstanding performance as anodes and cathodes for overall alkaline seawater splitting, with remarkably low cell voltages of 1.56 and 1.89 V at current densities of 10 and 400 mA·cm^(−2), respectively. Moreover, the robust stability of 100 h is also demonstrated at above 200 mA·cm^(−2) in alkaline seawater. Our present work demonstrates significant potential for constructing effective cost-efficient and non-noble-metal bifunctional electrocatalyst and electrode for industrial seawater splitting.