To optimize the CO_(2) adsorption performance of carbon materials,this study proposed a preparation method for biomass-based porous carbon through hydrothermal carbonization coupled with nitrogen source optimization a...To optimize the CO_(2) adsorption performance of carbon materials,this study proposed a preparation method for biomass-based porous carbon through hydrothermal carbonization coupled with nitrogen source optimization and K_(2)CO_(3) activation.The effects of different nitrogen sources(urea,piperazine,melamine,and polyaniline)and activation temperatures on the physicochemical features and CO_(2) adsorption characteristics of the porous carbons were systematically investigated.The results indicated that different nitrogen sources showed varying impacts on the CO_(2) uptake of porous carbons,and not all nitrogen sources enhanced the adsorption performance.The urea and piperazine doped porous carbons exhibited relatively low nitrogen contents and specific surface areas.Whereas the melamine doped carbons showed higher nitrogen contents and specific surface areas,but lacked narrow micropores,limiting their CO_(2) adsorption performance.In contrast,PAC-700,prepared using polyaniline as nitrogen source,featured a well-developed pore structure,abundant narrow micropores and pyrrolic-N groups,endowing it with enhanced CO_(2) adsorption capability.At 0℃/1 bar and 25℃/1 bar,the CO_(2) uptake of PAC-700 reached 6.85 and 4.64 mmol/g,respectively.Additionally,PAC-700 maintained a CO_(2) uptake retention ratio of 99%after 5 adsorption-desorption cycles and exhibited good CO_(2)/N_(2) selectivity of 22.4−51.6.These findings highlighted the advantageous CO_(2) adsorption performance of PAC-700,indicating its substantial application potential in the domain of carbon capture.展开更多
Sodium-ion batteries(SIBs)have emerged as a promising alternative to commercial lithium-ion batteries be-cause of the similar properties of Li and Na as well as the abundance and accessibility of sodium resources.The ...Sodium-ion batteries(SIBs)have emerged as a promising alternative to commercial lithium-ion batteries be-cause of the similar properties of Li and Na as well as the abundance and accessibility of sodium resources.The devel-opment of anode materials with a high capacity,excellent rate performance,and long cycle life is the key to the indus-trialization of SIBs.Biomass-derived carbon(BDC)anode materials synthesized from resource-rich,low-cost,and re-newable biomass have been extensively researched and their excellent sodium storage performance has been proven,making them the most promising new low-cost and high-performance anode material for SIBs.This review first intro-duces the sources of BDCs,including waste biomass such as plants,animals,and microorganisms,and then describes sev-eral methods for preparing BDC anode materials,including carbonization,chemical activation,and template methods.The storage mechanism and kinetic process of Na^(+)in BDCs are then considered as well as their structure control.The electrochemical properties of sodium-ion storage in BDCs with different structures are examined,and suggestions for future re-search are made.展开更多
The use of carbon from waste biomass has the potential to eliminate the drawbacks of Li-S batteries and improve their overall performance.Chrome-tanned-leather-shavings(CTLS)are a readily available waste product that ...The use of carbon from waste biomass has the potential to eliminate the drawbacks of Li-S batteries and improve their overall performance.Chrome-tanned-leather-shavings(CTLS)are a readily available waste product that can be transformed into porous carbon.We prepared an ac-tivated carbon by microwave pyrolysis combined with KOH activator using the CTLS as starting materials.The carbon had a specific surface area of 556 m^(2)g^(-1) and a honeycomb-like structure.Two kinds of N-doped activated carbons were then synthesized by thermal decomposition of the activated carbon,either combined with urea,or impregnated with eth-anolamine.Both N-doped activated carbons have an in-creased number of nitrogen and amine surface groups.However,only the urea treatment was effective in improv-ing the initial capacity of the cell(1363 mAh g^(-1)),which is probably linked to the sorption of long-chain polysulfides.This investigation confirms that it is possible to use the thermal de-composition of urea to obtain carbon materials from CTLS for use as the sulfur-host cathode in Li-S batteries and improve their performance.A radial basis function neural network was fitted to provide statistical support for the experimental results,which confirmed the importance of the nitrogen content of the carbons in determining the discharge capacity of the cells.展开更多
The preparation of a synthetic pitch from aromatic monomers could easily regulate structure orientation at the molecu-lar level,which would be useful in fabrication.An isotropic synthetic pitch was prepared by a chlor...The preparation of a synthetic pitch from aromatic monomers could easily regulate structure orientation at the molecu-lar level,which would be useful in fabrication.An isotropic synthetic pitch was prepared by a chlorine-and/or nitrogen-induced sub-stitution polymerization reaction method using aromatic hydrocarbon precursors containing Cl and N,which for this study were chloromethyl naphthalene and quinoline.This method was verified by investigating the structural changes under different synthesis conditions,and the synthesis mechanism induced by aromatics containing Cl was also probed.The result shows that the pyridinic N in quinoline contains a lone pair of electrons,and is an effective active site to induce the polymerization reaction by coupling with aromatic hydrocarbons containing Cl.The reaction between such free radicals causes strong homopolymerization and oligomeriza-tion.A higher reaction temperature and longer reaction time significantly increased the degree of polymerization and thus increased the softening point of the pitch.A linear molecular structure was formed by the Cl substitution reaction,which produced a highly spinnable pitch with a softening point of 258.6℃,and carbon fibers with a tensile strength of 1163.82 MPa were obtained.This study provides a relatively simple and safe method for the preparation of high-quality spinnable pitch.展开更多
The template carbonization method was utilized for the production of mesoporous carbons using attapulgite as a template and sucrose as carbon precursor. Sucrose was polymerized and carbonized in the tubes of natural a...The template carbonization method was utilized for the production of mesoporous carbons using attapulgite as a template and sucrose as carbon precursor. Sucrose was polymerized and carbonized in the tubes of natural attapulgite using a sulfuric acid catalyst. The structure of the template and carbons were investigated by powder X-ray diffraction, transmission electron microscopy, and Nitrogen adsorption analysis techniques. At the micrometer level, the carbon material templated with the natural attapulgite had the similar morphology. Nitrogen adsorption analysis showed that the obtained porous carbons possess a wide pore size distribution and a large pore volume, especially in the range of mesopores.展开更多
Sodium fulvic acid based hierarchical porous carbons(SFA-HPCs) with a specific surface area of 1919 m^2·g^(–1) and total volume of 1.7 cm^3·g^(–1) has been synthesized by a simple self-template method. The...Sodium fulvic acid based hierarchical porous carbons(SFA-HPCs) with a specific surface area of 1919 m^2·g^(–1) and total volume of 1.7 cm^3·g^(–1) has been synthesized by a simple self-template method. The carbon skeleton can be formatted by the decomposition process of sodium fulvic acid(SFA) in a N_2 atmosphere. The sodium compund in SFA is used as a self-template to create the hierarchical porous structure. The unique hierarchical structure of SFA-HPCs provides an efficient pathway for electrolyte ions to be diffused into the internal surfaces of bulk electrode particles. It results in a high charge storage capacitance of 186 F·g^(–1) at current load of 40 A·g^(–1). The capacitance of 230 F·g^(–1) at 0.05 A·g^(–1) and 186 F·g^(–1) at 40 A·g^(–1) show its good rate capability. Besides, it also achieves desirable cycling stability, 99.4% capacitance remained after 10000 cycles at 40 A·g^(–1).展开更多
A process was proposed based on the combination of chemical and physical activation for the production of activated carbons used as the electrode material for electric double layer capacitor (EDLC). By material charac...A process was proposed based on the combination of chemical and physical activation for the production of activated carbons used as the electrode material for electric double layer capacitor (EDLC). By material characterization and electrochemical methods, the influences of the activitation process on the specific surface area, pore structure and electrochemical properties of the activated carbons were investigated. The results show that specific surface area, the mesopore volume, and the specific capacitance increase with the increase of the mass ratio of KOH to char (m(KOH)/m(char)) and the activation time, respectively. When m(KOH)/m(char) is 4.0, the specific surface area and the mesopore volume reach the maximum values, i.e. 1 960 m2/g and 0.308 4 cm3/g, and the specific capacitance is 120.7 F/g synchronously. Compared with the chemical activation, the activated carbons prepared by chemical-physical activation show a larger mesopore volume, a higher ratio of mesopore and a larger specific capacitance.展开更多
The influences of molar ratio of KOH to C and activated temperature on the pore structure and electrochemical property of porous activated carbon from mesophase pitch activated by KOH were investigated. The surface ar...The influences of molar ratio of KOH to C and activated temperature on the pore structure and electrochemical property of porous activated carbon from mesophase pitch activated by KOH were investigated. The surface areas and the pore structures of activated carbons were analyzed by nitrogen adsorption, and the electrochemical properties of the activated carbons were studied using two-electrode capacitors in organic electrolyte. The results indicate that the maximum surface area of 3 190 m2/g is obtained at molar ratio of KOH to C of 5:1, the maximum specific capacitance of 122 F/g is attained at molar ratio of KOH to C of 4:1, and 800 ℃ is the proper temperature to obtain the maximum surface area and capacitance.展开更多
Fuel cell stacks as the automotive power source can be severely poisoned by a trace amount of NOx in atmosphere,which makes it necessary to provide clean air for fuel cell vehicles.In this work,activating commercial a...Fuel cell stacks as the automotive power source can be severely poisoned by a trace amount of NOx in atmosphere,which makes it necessary to provide clean air for fuel cell vehicles.In this work,activating commercial activated carbons with K2CO3 for the large enhancement of NO capture was studied.K2CO3 modified activated carbons(K2CO3 ACs)were prepared by impregnating activate carbons in K2CO3 solution under ultrasound treatment,followed by temperature programmed baking at 800 oC.The dynamic NO flow tests on K2CO3 ACs at room temperature indicated that NO adsorption capacity reached the maximum(96 mg/g)when K2CO3 loading was 19.5 wt%,which corresponded to a specific surface area of 1196.1 m2/g and total pore volume of 0.70 cm3/g.The ten-fold enhancement of NO adsorption on K2CO3 ACs compared to the unimpregnated activated carbon was mainly attributed to the formation of potassium nitrite,which was confirmed by FTIR and temperature programmed desorption measurements.Regeneration tests of NO adsorption on the optimum sample revealed that 76%of the NO adsorption capacity could be remained after the fourth cycle.展开更多
A novel type of metal oxide/activated carbon catalyst was prepared by sol-gel method for the hydrolysis of carbonyl sulfide （COS）. The influences of the calcination temperature, additive content （2.5%-10.0% Fe2O3, ...A novel type of metal oxide/activated carbon catalyst was prepared by sol-gel method for the hydrolysis of carbonyl sulfide （COS）. The influences of the calcination temperature, additive content （2.5%-10.0% Fe2O3, mass fraction） and the basic density of the activation process were thoroughly investigated. The surface of catalysts was characterized by Boehm titration. The products were characterized by scanning electron microscopy （SEM）, X-ray diffractometry （XRD） and X-ray photoelectron spectroscopy （XPS）. The results show that catalysts with 2.5%-5.0% Fe2O3 after calcining at 500 ℃ have superior activity. The conversion rate of COS increases with increasing the relative density of basic capacity loaded onto activated carbon（AC）, and the activity follows the order： KOH〉Na2CO3 〉NaHCO3. Boehm titration data clearly show that the total acidity increases （from 0.06 to 0.48 mmol/g） and the basic groups decrease （from 0.78 to 0.56 mmol/g） after COS hydrolysis and H2S adsorption. The XPS results show that the product of HzS may be absorbed by the interaction with metal compounds and 02 to form sulfate （171.28 eV） and element sulfur （164.44 eV）, which lead to catalysts poisoning.展开更多
Oxygen reduction reaction(ORR)plays a crucial role in many energy storage and conversion devices.Currently,the development of inexpensive and high-performance carbon-based non-precious-metal ORR catalysts in alkaline ...Oxygen reduction reaction(ORR)plays a crucial role in many energy storage and conversion devices.Currently,the development of inexpensive and high-performance carbon-based non-precious-metal ORR catalysts in alkaline media still gains a wide attention.In this paper,the mesoporous Fe-N/C catalysts were synthesized through SiO2-mediated templating method using biomass soybeans as the nitrogen and carbon sources.The SiO2 templates create a simultaneous optimization of both the surface functionalities and porous structures of Fe-N/C catalysts.Detailed investigations indicate that the Fe-N/C3 catalyst prepared with the mass ratio of SiO2 to soybean being 3:4 exhibits brilliant electrocatalytic performance,excellent long-term stability and methanol tolerance for the ORR,with the onset potential and the half-wave potential of the ORR being about 0.890 V and 0.783 V(vs RHE),respectively.Meanwhile,the desired 4-electron transfer pathway of the ORR on the catalysts can be observed.It is significantly proposed that the high BET specific surface area and the appropriate pore-size,as well as the high pyridinic-N and total nitrogen loadings may play key roles in enhancing the ORR performance for the Fe-N/C3 catalyst.These results suggest a feasible route based on the economical and sustainable soybean biomass to develop inexpensive and highly efficient non-precious metal electrochemical catalysts for the ORR.展开更多
The pore structures of two activated carbons from sawdust with KOH activation and coconut-shell with steam activation for supercapacitor were analyzed by N2 adsorption method. The electrochemical properties of both ac...The pore structures of two activated carbons from sawdust with KOH activation and coconut-shell with steam activation for supercapacitor were analyzed by N2 adsorption method. The electrochemical properties of both activated carbons in 6 mol/L KOH solution and 1 mol/L EtgNPF4/PC were compared, and the effect of pore structure on the capacitance was investigated by cyclic voltammetry, AC impedance and charge-discharge measurements. The results indicate that the capacitance mainly depends on effective surface area, but the power property mainly depends on mesoporosity. At low specific current （1 A/g）, the maximum specific Capacitances of 276.3 F/g in aqueous system and 123.9 F/g in nonaqueous system can be obtained from sawdust activated carbon with a larger surface area of 1 808 m^2/g, butat a high specific current, the specific capacitance of coconut-shell activated carbon with a higher mesoporosity of 75.1% is more excellent. Activated carbon by KOH activation is fitter for aqueous system and that by steam activation is fitter for nonaqueous system.展开更多
Carbon materials are a key component in energy storage and conversion devices and their microstructure plays a crucial role in determining device performance.However,traditional carbon materials are unable to meet the...Carbon materials are a key component in energy storage and conversion devices and their microstructure plays a crucial role in determining device performance.However,traditional carbon materials are unable to meet the requirements for applications in emerging fields such as renewable energy and electric vehicles due to limitations including a disordered structure and uncontrolled defects.With an aim of realizing devisable structures,adjustable functions,and performance breakthroughs,superstructured carbons is proposed and represent a category of carbon-based materials,characterized by precisely-built pores,networks,and interfaces.Superstructured carbons can overcome the limitations of traditional carbon materials and improve the performance of energy storage and conversion devices.We review the structure-activity relationships of superstructured carbons and recent research advances from three aspects including a precisely customized pore structure,a dense carbon network framework,and a multi-component highly coupled interface between the different components.Finally,we provide an outlook on the future development of and practical challenges in energy storage and conversion devices.展开更多
基金supported by the National Key R&D Program(2022YFC3902403)Fundamental Research Funds for the Central Universities(2024JC001,2019JG002)Technology Innovation Special Fund of Jiangsu Province for Carbon Dioxide Emission Peaking and Carbon Neutrality(BE2022307)。
文摘To optimize the CO_(2) adsorption performance of carbon materials,this study proposed a preparation method for biomass-based porous carbon through hydrothermal carbonization coupled with nitrogen source optimization and K_(2)CO_(3) activation.The effects of different nitrogen sources(urea,piperazine,melamine,and polyaniline)and activation temperatures on the physicochemical features and CO_(2) adsorption characteristics of the porous carbons were systematically investigated.The results indicated that different nitrogen sources showed varying impacts on the CO_(2) uptake of porous carbons,and not all nitrogen sources enhanced the adsorption performance.The urea and piperazine doped porous carbons exhibited relatively low nitrogen contents and specific surface areas.Whereas the melamine doped carbons showed higher nitrogen contents and specific surface areas,but lacked narrow micropores,limiting their CO_(2) adsorption performance.In contrast,PAC-700,prepared using polyaniline as nitrogen source,featured a well-developed pore structure,abundant narrow micropores and pyrrolic-N groups,endowing it with enhanced CO_(2) adsorption capability.At 0℃/1 bar and 25℃/1 bar,the CO_(2) uptake of PAC-700 reached 6.85 and 4.64 mmol/g,respectively.Additionally,PAC-700 maintained a CO_(2) uptake retention ratio of 99%after 5 adsorption-desorption cycles and exhibited good CO_(2)/N_(2) selectivity of 22.4−51.6.These findings highlighted the advantageous CO_(2) adsorption performance of PAC-700,indicating its substantial application potential in the domain of carbon capture.
文摘Sodium-ion batteries(SIBs)have emerged as a promising alternative to commercial lithium-ion batteries be-cause of the similar properties of Li and Na as well as the abundance and accessibility of sodium resources.The devel-opment of anode materials with a high capacity,excellent rate performance,and long cycle life is the key to the indus-trialization of SIBs.Biomass-derived carbon(BDC)anode materials synthesized from resource-rich,low-cost,and re-newable biomass have been extensively researched and their excellent sodium storage performance has been proven,making them the most promising new low-cost and high-performance anode material for SIBs.This review first intro-duces the sources of BDCs,including waste biomass such as plants,animals,and microorganisms,and then describes sev-eral methods for preparing BDC anode materials,including carbonization,chemical activation,and template methods.The storage mechanism and kinetic process of Na^(+)in BDCs are then considered as well as their structure control.The electrochemical properties of sodium-ion storage in BDCs with different structures are examined,and suggestions for future re-search are made.
文摘The use of carbon from waste biomass has the potential to eliminate the drawbacks of Li-S batteries and improve their overall performance.Chrome-tanned-leather-shavings(CTLS)are a readily available waste product that can be transformed into porous carbon.We prepared an ac-tivated carbon by microwave pyrolysis combined with KOH activator using the CTLS as starting materials.The carbon had a specific surface area of 556 m^(2)g^(-1) and a honeycomb-like structure.Two kinds of N-doped activated carbons were then synthesized by thermal decomposition of the activated carbon,either combined with urea,or impregnated with eth-anolamine.Both N-doped activated carbons have an in-creased number of nitrogen and amine surface groups.However,only the urea treatment was effective in improv-ing the initial capacity of the cell(1363 mAh g^(-1)),which is probably linked to the sorption of long-chain polysulfides.This investigation confirms that it is possible to use the thermal de-composition of urea to obtain carbon materials from CTLS for use as the sulfur-host cathode in Li-S batteries and improve their performance.A radial basis function neural network was fitted to provide statistical support for the experimental results,which confirmed the importance of the nitrogen content of the carbons in determining the discharge capacity of the cells.
文摘The preparation of a synthetic pitch from aromatic monomers could easily regulate structure orientation at the molecu-lar level,which would be useful in fabrication.An isotropic synthetic pitch was prepared by a chlorine-and/or nitrogen-induced sub-stitution polymerization reaction method using aromatic hydrocarbon precursors containing Cl and N,which for this study were chloromethyl naphthalene and quinoline.This method was verified by investigating the structural changes under different synthesis conditions,and the synthesis mechanism induced by aromatics containing Cl was also probed.The result shows that the pyridinic N in quinoline contains a lone pair of electrons,and is an effective active site to induce the polymerization reaction by coupling with aromatic hydrocarbons containing Cl.The reaction between such free radicals causes strong homopolymerization and oligomeriza-tion.A higher reaction temperature and longer reaction time significantly increased the degree of polymerization and thus increased the softening point of the pitch.A linear molecular structure was formed by the Cl substitution reaction,which produced a highly spinnable pitch with a softening point of 258.6℃,and carbon fibers with a tensile strength of 1163.82 MPa were obtained.This study provides a relatively simple and safe method for the preparation of high-quality spinnable pitch.
文摘The template carbonization method was utilized for the production of mesoporous carbons using attapulgite as a template and sucrose as carbon precursor. Sucrose was polymerized and carbonized in the tubes of natural attapulgite using a sulfuric acid catalyst. The structure of the template and carbons were investigated by powder X-ray diffraction, transmission electron microscopy, and Nitrogen adsorption analysis techniques. At the micrometer level, the carbon material templated with the natural attapulgite had the similar morphology. Nitrogen adsorption analysis showed that the obtained porous carbons possess a wide pore size distribution and a large pore volume, especially in the range of mesopores.
基金supported by the Ningbo’s Industrial Technology Innovation and Industrialization of Scientific and Technological Achievements Program(2013B6003)
文摘Sodium fulvic acid based hierarchical porous carbons(SFA-HPCs) with a specific surface area of 1919 m^2·g^(–1) and total volume of 1.7 cm^3·g^(–1) has been synthesized by a simple self-template method. The carbon skeleton can be formatted by the decomposition process of sodium fulvic acid(SFA) in a N_2 atmosphere. The sodium compund in SFA is used as a self-template to create the hierarchical porous structure. The unique hierarchical structure of SFA-HPCs provides an efficient pathway for electrolyte ions to be diffused into the internal surfaces of bulk electrode particles. It results in a high charge storage capacitance of 186 F·g^(–1) at current load of 40 A·g^(–1). The capacitance of 230 F·g^(–1) at 0.05 A·g^(–1) and 186 F·g^(–1) at 40 A·g^(–1) show its good rate capability. Besides, it also achieves desirable cycling stability, 99.4% capacitance remained after 10000 cycles at 40 A·g^(–1).
基金Project(2007BAE12B01) supported by the National Key Technology Research and Development Program of China
文摘A process was proposed based on the combination of chemical and physical activation for the production of activated carbons used as the electrode material for electric double layer capacitor (EDLC). By material characterization and electrochemical methods, the influences of the activitation process on the specific surface area, pore structure and electrochemical properties of the activated carbons were investigated. The results show that specific surface area, the mesopore volume, and the specific capacitance increase with the increase of the mass ratio of KOH to char (m(KOH)/m(char)) and the activation time, respectively. When m(KOH)/m(char) is 4.0, the specific surface area and the mesopore volume reach the maximum values, i.e. 1 960 m2/g and 0.308 4 cm3/g, and the specific capacitance is 120.7 F/g synchronously. Compared with the chemical activation, the activated carbons prepared by chemical-physical activation show a larger mesopore volume, a higher ratio of mesopore and a larger specific capacitance.
基金Project(06FJ4059) supported by Hunan Provincial Academician Foundation
文摘The influences of molar ratio of KOH to C and activated temperature on the pore structure and electrochemical property of porous activated carbon from mesophase pitch activated by KOH were investigated. The surface areas and the pore structures of activated carbons were analyzed by nitrogen adsorption, and the electrochemical properties of the activated carbons were studied using two-electrode capacitors in organic electrolyte. The results indicate that the maximum surface area of 3 190 m2/g is obtained at molar ratio of KOH to C of 5:1, the maximum specific capacitance of 122 F/g is attained at molar ratio of KOH to C of 4:1, and 800 ℃ is the proper temperature to obtain the maximum surface area and capacitance.
基金Project(2018YFB0105303)supported by the Ministry of Science and Technology of ChinaProject(17DZ1200702)supported by the Shanghai Science and Technology Committee,China
文摘Fuel cell stacks as the automotive power source can be severely poisoned by a trace amount of NOx in atmosphere,which makes it necessary to provide clean air for fuel cell vehicles.In this work,activating commercial activated carbons with K2CO3 for the large enhancement of NO capture was studied.K2CO3 modified activated carbons(K2CO3 ACs)were prepared by impregnating activate carbons in K2CO3 solution under ultrasound treatment,followed by temperature programmed baking at 800 oC.The dynamic NO flow tests on K2CO3 ACs at room temperature indicated that NO adsorption capacity reached the maximum(96 mg/g)when K2CO3 loading was 19.5 wt%,which corresponded to a specific surface area of 1196.1 m2/g and total pore volume of 0.70 cm3/g.The ten-fold enhancement of NO adsorption on K2CO3 ACs compared to the unimpregnated activated carbon was mainly attributed to the formation of potassium nitrite,which was confirmed by FTIR and temperature programmed desorption measurements.Regeneration tests of NO adsorption on the optimum sample revealed that 76%of the NO adsorption capacity could be remained after the fourth cycle.
基金Project(50908110) supported by the National Natural Science Foundation of ChinaProject(2008AA062602) supported by the National High-Tech Research and Development Program of China+1 种基金Project(20090451431) supported by China Postdoctoral Science FoundationProject(2007PY01-10) supported by Young and Middle-aged Academic and Technical Back-up Personnel Program of Yunnan Province,China
文摘A novel type of metal oxide/activated carbon catalyst was prepared by sol-gel method for the hydrolysis of carbonyl sulfide （COS）. The influences of the calcination temperature, additive content （2.5%-10.0% Fe2O3, mass fraction） and the basic density of the activation process were thoroughly investigated. The surface of catalysts was characterized by Boehm titration. The products were characterized by scanning electron microscopy （SEM）, X-ray diffractometry （XRD） and X-ray photoelectron spectroscopy （XPS）. The results show that catalysts with 2.5%-5.0% Fe2O3 after calcining at 500 ℃ have superior activity. The conversion rate of COS increases with increasing the relative density of basic capacity loaded onto activated carbon（AC）, and the activity follows the order： KOH〉Na2CO3 〉NaHCO3. Boehm titration data clearly show that the total acidity increases （from 0.06 to 0.48 mmol/g） and the basic groups decrease （from 0.78 to 0.56 mmol/g） after COS hydrolysis and H2S adsorption. The XPS results show that the product of HzS may be absorbed by the interaction with metal compounds and 02 to form sulfate （171.28 eV） and element sulfur （164.44 eV）, which lead to catalysts poisoning.
基金Project(21406273)supported by the National Natural Science Foundation of China
文摘Oxygen reduction reaction(ORR)plays a crucial role in many energy storage and conversion devices.Currently,the development of inexpensive and high-performance carbon-based non-precious-metal ORR catalysts in alkaline media still gains a wide attention.In this paper,the mesoporous Fe-N/C catalysts were synthesized through SiO2-mediated templating method using biomass soybeans as the nitrogen and carbon sources.The SiO2 templates create a simultaneous optimization of both the surface functionalities and porous structures of Fe-N/C catalysts.Detailed investigations indicate that the Fe-N/C3 catalyst prepared with the mass ratio of SiO2 to soybean being 3:4 exhibits brilliant electrocatalytic performance,excellent long-term stability and methanol tolerance for the ORR,with the onset potential and the half-wave potential of the ORR being about 0.890 V and 0.783 V(vs RHE),respectively.Meanwhile,the desired 4-electron transfer pathway of the ORR on the catalysts can be observed.It is significantly proposed that the high BET specific surface area and the appropriate pore-size,as well as the high pyridinic-N and total nitrogen loadings may play key roles in enhancing the ORR performance for the Fe-N/C3 catalyst.These results suggest a feasible route based on the economical and sustainable soybean biomass to develop inexpensive and highly efficient non-precious metal electrochemical catalysts for the ORR.
基金Project(2007BAE12B01-2) supported by the National Key Project Scientific and Technical Supporting Programs Funded by Ministry of Science and Technology of China
文摘The pore structures of two activated carbons from sawdust with KOH activation and coconut-shell with steam activation for supercapacitor were analyzed by N2 adsorption method. The electrochemical properties of both activated carbons in 6 mol/L KOH solution and 1 mol/L EtgNPF4/PC were compared, and the effect of pore structure on the capacitance was investigated by cyclic voltammetry, AC impedance and charge-discharge measurements. The results indicate that the capacitance mainly depends on effective surface area, but the power property mainly depends on mesoporosity. At low specific current （1 A/g）, the maximum specific Capacitances of 276.3 F/g in aqueous system and 123.9 F/g in nonaqueous system can be obtained from sawdust activated carbon with a larger surface area of 1 808 m^2/g, butat a high specific current, the specific capacitance of coconut-shell activated carbon with a higher mesoporosity of 75.1% is more excellent. Activated carbon by KOH activation is fitter for aqueous system and that by steam activation is fitter for nonaqueous system.
文摘Carbon materials are a key component in energy storage and conversion devices and their microstructure plays a crucial role in determining device performance.However,traditional carbon materials are unable to meet the requirements for applications in emerging fields such as renewable energy and electric vehicles due to limitations including a disordered structure and uncontrolled defects.With an aim of realizing devisable structures,adjustable functions,and performance breakthroughs,superstructured carbons is proposed and represent a category of carbon-based materials,characterized by precisely-built pores,networks,and interfaces.Superstructured carbons can overcome the limitations of traditional carbon materials and improve the performance of energy storage and conversion devices.We review the structure-activity relationships of superstructured carbons and recent research advances from three aspects including a precisely customized pore structure,a dense carbon network framework,and a multi-component highly coupled interface between the different components.Finally,we provide an outlook on the future development of and practical challenges in energy storage and conversion devices.
