An activated carbon with ash content less than 10% and specific surface area more than 1 600 m 2 /g was prepared from coal and the effect of K containing compounds in preparation of coal based activated carbon was inv...An activated carbon with ash content less than 10% and specific surface area more than 1 600 m 2 /g was prepared from coal and the effect of K containing compounds in preparation of coal based activated carbon was investigated in detail in this paper. KOH was used in co carbonization with coal, changes in graphitic crystallites in chars derived from carbonization of coal with and without KOH were analyzed by X ray diffraction (XRD) technique, activation rates of chars with different contents of K containing compounds were deduced, and resulting activated carbons were characterized by nitrogen adsorption isotherms at 77 K and iodine numbers. The results showed that the addition of KOH to the coal before carbonization can realize the intensive removal of inorganic matters from chars under mild conditions, especially the efficient removal of dispersive quartz, an extremely difficult separated mineral component in other processes else. Apart from this, KOH demonstrates a favorable effect in control over coal carbonization with the goal to form nongraphitizable isotropic carbon precursor, which is a necessary prerequisite for the formation and development of micro pores. However, the K containing compounds such as K 2 CO 3 and K 2 O remaining in chars after carbonization catalyze the reaction between carbon and steam in activation, which leads to the formation of macro pores. In the end an innovative method, in which KOH is added to coal before carbonization and K containing compounds are removed by acid washing after carbonization, was proposed for the synthesis of quality coal based activated carbon.展开更多
Activated carbons(ACs) with a wide range of surface areas were made from petroleum coke by means of KOH activation. The electrochemical characterization was carried out for several activated carbons used as polarizabl...Activated carbons(ACs) with a wide range of surface areas were made from petroleum coke by means of KOH activation. The electrochemical characterization was carried out for several activated carbons used as polarizable electrodes of electric double-layer capacitors(EDLCs) in an aqueous electrolytic solution. The porous structures and electrochemical double-layer capacitance of the activated carbons were investigated by virtue of nitrogen gas adsorption and constant current cycling(CCC) methods. The relationship among the surface area, pore volume of the activated carbons and specific double-layer capacitance was discussed. It was found that the specific capacitance of ACs increased linearly with the increase of surface area. The presence of mesopores in the activated carbons with very high surface area(>2000 m\+2/g) was not very effective for them to be used as EDLCs. The influence of chemical characteristics of the activated carbons on the double layer formation could be considered to be negligible.展开更多
We report here the activated carbon and cobalt hexacyanoferrate composite,which is applied as the electrode materials in symmetric supercapacitors containing a 1.0 M Na_(2)SO_(4) aqueous electrolyte.This novel materia...We report here the activated carbon and cobalt hexacyanoferrate composite,which is applied as the electrode materials in symmetric supercapacitors containing a 1.0 M Na_(2)SO_(4) aqueous electrolyte.This novel material combines high specific surface area and electrochemical stability of activated carbon with the redox properties of cobalt hexacyanoferrate,resulting in maximum specific capacitance of 329 F g^(-1) with large voltage working window of 2.0 V.Electrochemical studies indicated that cobalt hexacyanoferrate introduces important pseudocapacitive properties accounting for the overall charge-storage process,especially when I<0.5 A g^(-1).At lower gravimetric currents(e.g.,0.05 A g^(-1))and up to 1.0 V,the presence of cobalt hexacyanoferrate improves the specific energy for more than 300%.In addition,to better understanding the energy storage process we also provided a careful investigation of the electrode materials under dynamic polarization conditions using the in situ Raman spectroscopy and synchrotron light Xray diffraction techniques.Interesting complementary findings were obtained in these studies.We believe that this novel electrode material is promising for applications regarding the energy-storage process in pseudocapacitors with long lifespan properties.展开更多
Effect of activated carbon and electrolyte on electrochemical properties of organic supercapacitor was investigated. The results show that specific surface area and mesoporosity of activated carbon influence specific ...Effect of activated carbon and electrolyte on electrochemical properties of organic supercapacitor was investigated. The results show that specific surface area and mesoporosity of activated carbon influence specific capacitance. If specific surface area is larger and mesoporosity is higher, the specific capacitance will become bigger. Specific surface area influences resistance of carbon electrode and consequently influences power property and pore size distribution. If specific surface area is smaller and mesoporosity is higher, the power property will become better. Ash influences leakage current and electrochemical cycling stability. If ash content is lower, the performance will become better. The properties of supercapacitor highly depend on the electrolyte. The compatibility of electrolyte and activated carbon is a determining factor of supercapacitor’s working voltage. LiPF6/(EC+EMC+DMC) is inappropriate for double layer capacitor. MeEt3NPF4/PC has higher specific capacitance than Et4NPF4/PC because methyl’s electronegativity value is lower than ethyl and MeEt3N+ has more positive charges and stronger polarizability than Et4N+ when an ethyl is substituted by methyl.展开更多
Activated carbon aerogels(ACAs) derived from sol-gel polycondensation of resorcinol (R) and formaldehyde (F) were pyrolyzed under Ar flow and activated in CO2 atmosphere. The morphology of ACAs was characterized...Activated carbon aerogels(ACAs) derived from sol-gel polycondensation of resorcinol (R) and formaldehyde (F) were pyrolyzed under Ar flow and activated in CO2 atmosphere. The morphology of ACAs was characterized by scanning electron microscopy (SEM) and the structural properties were determined by N2 adsorption at 77 K. The results show that ACAs have a typical three-dimensional nanonetwork structure composing of cross-linking of carbon nanoparticles. The specific surface area and the total pore volume remarkably increase with increasing activation time while the previous porous structure still remains. The specific capacitance of the 950-10-ACA electrode can reach up to 212.3 F/g in 6 mol/L KOH electrolyte. The results of constant-current charge-discharge testing indicate that the ACAs electrodes present fast charge- discharge rate and long cycle life (about 98% capacitance retained after 3000 charge-discharge cycles at 1.25 mA/cm2). Lower internal resistances can be achieved for 950-10-ACA electrode in KOH electrolyte. Our investigations are very important to improve the wettability and electrochemical performance of electrode for supercapacitors.展开更多
The purpose of this work is to prepare better activated carbons from the shells of Ricinodendron Heudelotii by chemical activation with sulfuric acid (H<sub>2</sub>SO<sub>4</sub>) and sodium hy...The purpose of this work is to prepare better activated carbons from the shells of Ricinodendron Heudelotii by chemical activation with sulfuric acid (H<sub>2</sub>SO<sub>4</sub>) and sodium hydroxide (NaOH). The process was optimized by a full factorial design (2<sup>K</sup>) based on the analysis of the external specific surface area of sixteen (16) activated carbons prepared according to the parameters of the preparation. This active analysis reveals that under the preparation conditions, good carbons are obtained for a sodium hydroxide concentration equal to 1 M, an impregnation time of 24 h and carbonization at 500˚C for 1 h. The external specific surface of this carbon is 358 m<sup>2</sup><sup> </sup>•<sup></sup> g<sup>-1</sup>. The characteristics of this prepared carbon are as follows: a pH at zero point charge (pHpzc) of 8.2, a predominantly amorphous structure, a basic character and a low ash content (4.2%). It also has surface functions;the lactonic and carbonyl groups (C=O) at 1600 cm<sup>-1</sup> and the carboxylate groups (O-H or C-O) at 1340 cm<sup>-1</sup>.展开更多
The catalytic pyrolyses of rayon have been studied respectively by thermo-gravimetric analysis (TGA) when rayon was treated with phosphoric acid (PA), three ammonium phosphate salts and ammonium sulfate (AS). The air ...The catalytic pyrolyses of rayon have been studied respectively by thermo-gravimetric analysis (TGA) when rayon was treated with phosphoric acid (PA), three ammonium phosphate salts and ammonium sulfate (AS). The air is favorable to the catalysis of dibasic ammonium phosphate (DAP), but not to those of ADP, PA, AP, and AS obviously. It is put forward that a peak’s shape character can be described with the ratio of height to half-height-width (H/W /2) of the peak on a differential thermo-gravimetric (DTG) curve. A flat cracking peak, presenting a more moderate dehydration reaction, has a smaller ratio and could lead to higher carbonization and activation yields. The experimental results prove this view. According to expectation, the order of catalysis is: DAP≥ADP>PA> APAS no catalyst.展开更多
Fe/C-based magnetically activated carbon(MAC) was obtained by carbonizing and activating its precursor, that was prepared by co-precipitation of anthracite coal impregnated in ferric chloride solution. The effect of t...Fe/C-based magnetically activated carbon(MAC) was obtained by carbonizing and activating its precursor, that was prepared by co-precipitation of anthracite coal impregnated in ferric chloride solution. The effect of the concentrations of FeCl3 and pH of solution on BET surface area, pore volume and magnetic properties of the MAC was studied by BET N2 adsorption and VSM method. The results indicated that the magnetization of MAC gradually increases with increasing concentration of FeCl3 and pH value of solution, and BET surface area was inclined to fluctuation. The largest BET surface area and magnetization of MAC were 1327.5 m2/g and 35.56 emu/g, respectively. The form of magnetic matter in the magnetically activated carbon was mainly Fe3C by X-ray powder diffraction(XRD) and magnetic attraction test.展开更多
Taking the selection of coal-tar pitch as precursor and KOH as activated agent, the activated carbon electrode material was fabricated for supercapacitor.The surface area and the pore structure of activated carbon wer...Taking the selection of coal-tar pitch as precursor and KOH as activated agent, the activated carbon electrode material was fabricated for supercapacitor.The surface area and the pore structure of activated carbon were analyzed by Nitro adsorption method. The electrochemical properties of the activated carbons were determined using two-electrode capacitors in 6 mol/L KOH aqueous electrolytes. The influences of activated temperature and mass ratio of KOH to C on the pore structure and electrochemical property of porous activated carbon were investigated in detail. The reasons for the changes of pore structure and electrochemical performance of activated carbon prepared under different conditions were also discussed theoretically. The results indicate that the maximum specific capacitance of 240 F/g can be obtained in alkaline medium, and the surface area, the pore structure and the specific capacitance of activated carbon depend on the treatment methods; the capacitance variation of activated carbon cannot be interpreted only by the change of surface area and pore structure, the lattice order and the electrolyte wetting effect of the activated carbon should also be taken into account.展开更多
Using the mesophase pitch as precursor, KOH and CO2 as activated agents, the activated carbon electrode material was fabricated by physical-chemical combined activated technique for supercapacitor. The influence of ac...Using the mesophase pitch as precursor, KOH and CO2 as activated agents, the activated carbon electrode material was fabricated by physical-chemical combined activated technique for supercapacitor. The influence of activated process on the pore structure of activated carbon was analyzed and 14 F supercapacitor with working voltage of 2.5 V was prepared. The charge and discharge behaviors, the properties of cyclic voltammetry, specific capacitance, equivalent serials resistance (ESR), cycle properties, and temperature properties of prepared supercapacitor were examined. The cyclic voltammetry curve results indicate that the carbon based supercapacitor using the self-made activated carbon as electrode materials shows the desired capacitance properties. In 1 mol/L Et4NBF4/AN electrolyte, the capacitance and ESR of the supercapacitor are 14.7 F and 60 m?, respectively. The specific capacitance of activated carbon electrode materials is 99.6 F/g; its energy density can reach 2.96 W·h/kg under the large current discharge condition. There is no obvious capacitance decay that can be observed after 5000 cycles. The leakage current is below 0.2 mA after keeping the voltage at 2.5 V for 1 h. Meanwhile, the supercapacitor shows desired temperature property; it can be operated normally in the temperature ranging from -40 ℃ to 70 ℃.展开更多
锌离子电容器(ZICs)具有能量密度高、倍率性能好、循环寿命长、成本低等优点,近年来得到了广泛的研究。在碳基阴极表面引入氧官能团是提高水系ZICs电容性能的有效策略。然而,氧官能团的存在是否有利于提高乙醇(EtOH)基ZICs的电容性能,...锌离子电容器(ZICs)具有能量密度高、倍率性能好、循环寿命长、成本低等优点,近年来得到了广泛的研究。在碳基阴极表面引入氧官能团是提高水系ZICs电容性能的有效策略。然而,氧官能团的存在是否有利于提高乙醇(EtOH)基ZICs的电容性能,目前还没有被深入研究。本文采用硝酸氧化和进一步热处理的方法对阴极活性炭表面的氧官能团进行了优化。在ZnCl2/EtOH电解液中,优化后的样品在电流密度为1 A g^(−1)时比电容达到195 F g^(−1),比未改性的样品(125 F g^(−1))提高了56%。同时,ZICs也表现出良好的循环稳定性,在3 A g^(−1)下的稳定循环次数超过16000次,并且保持100%的库仑效率。这是因为氧官能团,特别是羧基和酯基(―COO)的存在,为Zn2+氧化还原反应提供了丰富的电化学活性位点。因此,本研究通过优化氧官能团增强了炭阴极的电容性能,并为EtOH基ZICs的商业应用提供了研究基础。展开更多
文摘An activated carbon with ash content less than 10% and specific surface area more than 1 600 m 2 /g was prepared from coal and the effect of K containing compounds in preparation of coal based activated carbon was investigated in detail in this paper. KOH was used in co carbonization with coal, changes in graphitic crystallites in chars derived from carbonization of coal with and without KOH were analyzed by X ray diffraction (XRD) technique, activation rates of chars with different contents of K containing compounds were deduced, and resulting activated carbons were characterized by nitrogen adsorption isotherms at 77 K and iodine numbers. The results showed that the addition of KOH to the coal before carbonization can realize the intensive removal of inorganic matters from chars under mild conditions, especially the efficient removal of dispersive quartz, an extremely difficult separated mineral component in other processes else. Apart from this, KOH demonstrates a favorable effect in control over coal carbonization with the goal to form nongraphitizable isotropic carbon precursor, which is a necessary prerequisite for the formation and development of micro pores. However, the K containing compounds such as K 2 CO 3 and K 2 O remaining in chars after carbonization catalyze the reaction between carbon and steam in activation, which leads to the formation of macro pores. In the end an innovative method, in which KOH is added to coal before carbonization and K containing compounds are removed by acid washing after carbonization, was proposed for the synthesis of quality coal based activated carbon.
基金Supported by the Young Teacher Scientific Research Foundation of BU CT(No.QN0 2 4 9) and National Natural ScienceFoundation(No.5 0 2 72 0 70 )
文摘Activated carbons(ACs) with a wide range of surface areas were made from petroleum coke by means of KOH activation. The electrochemical characterization was carried out for several activated carbons used as polarizable electrodes of electric double-layer capacitors(EDLCs) in an aqueous electrolytic solution. The porous structures and electrochemical double-layer capacitance of the activated carbons were investigated by virtue of nitrogen gas adsorption and constant current cycling(CCC) methods. The relationship among the surface area, pore volume of the activated carbons and specific double-layer capacitance was discussed. It was found that the specific capacitance of ACs increased linearly with the increase of surface area. The presence of mesopores in the activated carbons with very high surface area(>2000 m\+2/g) was not very effective for them to be used as EDLCs. The influence of chemical characteristics of the activated carbons on the double layer formation could be considered to be negligible.
基金the financial support from the Brazilian funding agencies CNPq(301486/2016-6)FAPESP(2014/02163-7,2017/11958-1,2018/20756-6)+2 种基金FAPEMIG(Financial support for the LMMA/UFVJM Laboratory)CNPq(PQ-2 grant:Process 301095/2018-3)the support from Shell and the strategic importance of the support given by ANP(Brazil’s National Oil,Natural Gas and Biofuels Agency)through the R&D levy regulation。
文摘We report here the activated carbon and cobalt hexacyanoferrate composite,which is applied as the electrode materials in symmetric supercapacitors containing a 1.0 M Na_(2)SO_(4) aqueous electrolyte.This novel material combines high specific surface area and electrochemical stability of activated carbon with the redox properties of cobalt hexacyanoferrate,resulting in maximum specific capacitance of 329 F g^(-1) with large voltage working window of 2.0 V.Electrochemical studies indicated that cobalt hexacyanoferrate introduces important pseudocapacitive properties accounting for the overall charge-storage process,especially when I<0.5 A g^(-1).At lower gravimetric currents(e.g.,0.05 A g^(-1))and up to 1.0 V,the presence of cobalt hexacyanoferrate improves the specific energy for more than 300%.In addition,to better understanding the energy storage process we also provided a careful investigation of the electrode materials under dynamic polarization conditions using the in situ Raman spectroscopy and synchrotron light Xray diffraction techniques.Interesting complementary findings were obtained in these studies.We believe that this novel electrode material is promising for applications regarding the energy-storage process in pseudocapacitors with long lifespan properties.
基金Project(2007CB613607) supported by the National Basic Research Program of China
文摘Effect of activated carbon and electrolyte on electrochemical properties of organic supercapacitor was investigated. The results show that specific surface area and mesoporosity of activated carbon influence specific capacitance. If specific surface area is larger and mesoporosity is higher, the specific capacitance will become bigger. Specific surface area influences resistance of carbon electrode and consequently influences power property and pore size distribution. If specific surface area is smaller and mesoporosity is higher, the power property will become better. Ash influences leakage current and electrochemical cycling stability. If ash content is lower, the performance will become better. The properties of supercapacitor highly depend on the electrolyte. The compatibility of electrolyte and activated carbon is a determining factor of supercapacitor’s working voltage. LiPF6/(EC+EMC+DMC) is inappropriate for double layer capacitor. MeEt3NPF4/PC has higher specific capacitance than Et4NPF4/PC because methyl’s electronegativity value is lower than ethyl and MeEt3N+ has more positive charges and stronger polarizability than Et4N+ when an ethyl is substituted by methyl.
基金Funded by the National Science Foundation of China(Nos.11074176 and 10976019)the Research Fund for the Doctoral Program of Higher Education of China(No.20100181110080)
文摘Activated carbon aerogels(ACAs) derived from sol-gel polycondensation of resorcinol (R) and formaldehyde (F) were pyrolyzed under Ar flow and activated in CO2 atmosphere. The morphology of ACAs was characterized by scanning electron microscopy (SEM) and the structural properties were determined by N2 adsorption at 77 K. The results show that ACAs have a typical three-dimensional nanonetwork structure composing of cross-linking of carbon nanoparticles. The specific surface area and the total pore volume remarkably increase with increasing activation time while the previous porous structure still remains. The specific capacitance of the 950-10-ACA electrode can reach up to 212.3 F/g in 6 mol/L KOH electrolyte. The results of constant-current charge-discharge testing indicate that the ACAs electrodes present fast charge- discharge rate and long cycle life (about 98% capacitance retained after 3000 charge-discharge cycles at 1.25 mA/cm2). Lower internal resistances can be achieved for 950-10-ACA electrode in KOH electrolyte. Our investigations are very important to improve the wettability and electrochemical performance of electrode for supercapacitors.
文摘The purpose of this work is to prepare better activated carbons from the shells of Ricinodendron Heudelotii by chemical activation with sulfuric acid (H<sub>2</sub>SO<sub>4</sub>) and sodium hydroxide (NaOH). The process was optimized by a full factorial design (2<sup>K</sup>) based on the analysis of the external specific surface area of sixteen (16) activated carbons prepared according to the parameters of the preparation. This active analysis reveals that under the preparation conditions, good carbons are obtained for a sodium hydroxide concentration equal to 1 M, an impregnation time of 24 h and carbonization at 500˚C for 1 h. The external specific surface of this carbon is 358 m<sup>2</sup><sup> </sup>•<sup></sup> g<sup>-1</sup>. The characteristics of this prepared carbon are as follows: a pH at zero point charge (pHpzc) of 8.2, a predominantly amorphous structure, a basic character and a low ash content (4.2%). It also has surface functions;the lactonic and carbonyl groups (C=O) at 1600 cm<sup>-1</sup> and the carboxylate groups (O-H or C-O) at 1340 cm<sup>-1</sup>.
文摘The catalytic pyrolyses of rayon have been studied respectively by thermo-gravimetric analysis (TGA) when rayon was treated with phosphoric acid (PA), three ammonium phosphate salts and ammonium sulfate (AS). The air is favorable to the catalysis of dibasic ammonium phosphate (DAP), but not to those of ADP, PA, AP, and AS obviously. It is put forward that a peak’s shape character can be described with the ratio of height to half-height-width (H/W /2) of the peak on a differential thermo-gravimetric (DTG) curve. A flat cracking peak, presenting a more moderate dehydration reaction, has a smaller ratio and could lead to higher carbonization and activation yields. The experimental results prove this view. According to expectation, the order of catalysis is: DAP≥ADP>PA> APAS no catalyst.
文摘Fe/C-based magnetically activated carbon(MAC) was obtained by carbonizing and activating its precursor, that was prepared by co-precipitation of anthracite coal impregnated in ferric chloride solution. The effect of the concentrations of FeCl3 and pH of solution on BET surface area, pore volume and magnetic properties of the MAC was studied by BET N2 adsorption and VSM method. The results indicated that the magnetization of MAC gradually increases with increasing concentration of FeCl3 and pH value of solution, and BET surface area was inclined to fluctuation. The largest BET surface area and magnetization of MAC were 1327.5 m2/g and 35.56 emu/g, respectively. The form of magnetic matter in the magnetically activated carbon was mainly Fe3C by X-ray powder diffraction(XRD) and magnetic attraction test.
基金Project(2005CB623703) supported by the National Basic Research Program of China project(5JJ30103) supported bythe Natural Science Foundation of Hunan Province
文摘Taking the selection of coal-tar pitch as precursor and KOH as activated agent, the activated carbon electrode material was fabricated for supercapacitor.The surface area and the pore structure of activated carbon were analyzed by Nitro adsorption method. The electrochemical properties of the activated carbons were determined using two-electrode capacitors in 6 mol/L KOH aqueous electrolytes. The influences of activated temperature and mass ratio of KOH to C on the pore structure and electrochemical property of porous activated carbon were investigated in detail. The reasons for the changes of pore structure and electrochemical performance of activated carbon prepared under different conditions were also discussed theoretically. The results indicate that the maximum specific capacitance of 240 F/g can be obtained in alkaline medium, and the surface area, the pore structure and the specific capacitance of activated carbon depend on the treatment methods; the capacitance variation of activated carbon cannot be interpreted only by the change of surface area and pore structure, the lattice order and the electrolyte wetting effect of the activated carbon should also be taken into account.
基金Project(2007BAE12800) supported by the National Supported Plan for Science and TechnologyProject(06FJ4059) supported by the Hunan Provincial Academician Foundation
文摘Using the mesophase pitch as precursor, KOH and CO2 as activated agents, the activated carbon electrode material was fabricated by physical-chemical combined activated technique for supercapacitor. The influence of activated process on the pore structure of activated carbon was analyzed and 14 F supercapacitor with working voltage of 2.5 V was prepared. The charge and discharge behaviors, the properties of cyclic voltammetry, specific capacitance, equivalent serials resistance (ESR), cycle properties, and temperature properties of prepared supercapacitor were examined. The cyclic voltammetry curve results indicate that the carbon based supercapacitor using the self-made activated carbon as electrode materials shows the desired capacitance properties. In 1 mol/L Et4NBF4/AN electrolyte, the capacitance and ESR of the supercapacitor are 14.7 F and 60 m?, respectively. The specific capacitance of activated carbon electrode materials is 99.6 F/g; its energy density can reach 2.96 W·h/kg under the large current discharge condition. There is no obvious capacitance decay that can be observed after 5000 cycles. The leakage current is below 0.2 mA after keeping the voltage at 2.5 V for 1 h. Meanwhile, the supercapacitor shows desired temperature property; it can be operated normally in the temperature ranging from -40 ℃ to 70 ℃.
文摘锌离子电容器(ZICs)具有能量密度高、倍率性能好、循环寿命长、成本低等优点,近年来得到了广泛的研究。在碳基阴极表面引入氧官能团是提高水系ZICs电容性能的有效策略。然而,氧官能团的存在是否有利于提高乙醇(EtOH)基ZICs的电容性能,目前还没有被深入研究。本文采用硝酸氧化和进一步热处理的方法对阴极活性炭表面的氧官能团进行了优化。在ZnCl2/EtOH电解液中,优化后的样品在电流密度为1 A g^(−1)时比电容达到195 F g^(−1),比未改性的样品(125 F g^(−1))提高了56%。同时,ZICs也表现出良好的循环稳定性,在3 A g^(−1)下的稳定循环次数超过16000次,并且保持100%的库仑效率。这是因为氧官能团,特别是羧基和酯基(―COO)的存在,为Zn2+氧化还原反应提供了丰富的电化学活性位点。因此,本研究通过优化氧官能团增强了炭阴极的电容性能,并为EtOH基ZICs的商业应用提供了研究基础。