Lithium–sulfur(Li–S)batteries are promisingcandidates for next-generation energy storagegiven their high energy density and potential low cost.Chemically activated carbon(CAC)is often used fortheir cathodes,because ...Lithium–sulfur(Li–S)batteries are promisingcandidates for next-generation energy storagegiven their high energy density and potential low cost.Chemically activated carbon(CAC)is often used fortheir cathodes,because it has a high specific surfacearea for sulfur loading.We have developed a pressurizedphysical activation(PPA)method that producedan activated carbon(PPAC)with a high specific surfacearea comparable to that of CAC.The pore structure of PPAC could be changed and its use as a cathode material for Li–Sbatteries was investigated.Battery tests at different capacity rates(C-rates)showed that it had a much improved high-rate performancewith a discharge capacity of 900 mAh/(g of sulfur)at 1 C,in contrast to only 600 mAh/(g of sulfur)for CAC.Porestructure analyses showed that PPAC prepared at a high activation temperature(1000℃)had unusual channel-like mesoporesbetween the microdomains that are the basic structural units of artificial carbon materials.These are connected to microporesdeveloped in each microdomain,and deliver ions from the surroundings to the internal pores and vice versa.The well-developedmicropores and mesopores of PPAC respectively ensured the high adsorption of lithium polysulfides and a high rate ofion diffusion.Compared to CAC,PPAC is a high-performance,low-cost cathode material that is promising for use in futureLi–S batteries.展开更多
Aqueous zincion capacitors(ZICs)have significant potential as energy storage systems because of their high specific capacity and superior reliability.Heteroatom-doped carbon materials were known to substantially incre...Aqueous zincion capacitors(ZICs)have significant potential as energy storage systems because of their high specific capacity and superior reliability.Heteroatom-doped carbon materials were known to substantially increase the capacitance of ZICs,however the mechanism remains poorly understood.Coal-based activated carbon was functionalized with B and N to serve as the cathode material in ZICs.This modification gave the material a high specific capacity of 371.4 mAh g^(-1)at 1 A g^(-1)and it retained 74%of its initial capacity after 10000 cycles.Experimental results and density functional theory calculations revealed that pyridinic N plays a crucial role in increasing Zn^(2+)storage,demonstrating superior electrochemical reversibility.This work gives valuable insight into the design of high-capacity and ultrafast pseudocapacitive carbon cathodes for ZICs.展开更多
To elucidate the effect of calcite-regulated activated carbon(AC)structure on low-temperature denitrification performance of SCR catalysts,this work prepared a series of Mn-Ce/De-AC-xCaCO_(3)(x is the calcite content ...To elucidate the effect of calcite-regulated activated carbon(AC)structure on low-temperature denitrification performance of SCR catalysts,this work prepared a series of Mn-Ce/De-AC-xCaCO_(3)(x is the calcite content in coal)catalysts were prepared by the incipient wetness impregnation method,followed by acid washing to remove calcium-containing minerals.Comprehensive characterization and low-temperature denitrification tests revealed that calcite-induced structural modulation of coal-derived AC significantly enhances catalytic activity.Specifically,NO conversion increased from 88.3%of Mn-Ce/De-AC to 91.7%of Mn-Ce/De-AC-1CaCO_(3)(210℃).The improved SCR denitrification activity results from the enhancement of physicochemical properties including higher Mn^(4+)content and Ce^(4+)/Ce^(3+)ratio,an abundance of chemisorbed oxygen and acidic sites,which could strengthen the SCR reaction pathways(richer NH_(3)activated species and bidentate nitrate active species).Therefore,NO removal is enhanced.展开更多
The reduction of 4-nitrophenol(4-NP)to 4-aminophenol(4-AP)in wastewater faces challenges in terms of conversion rate and stability.We used coal tar pitch-based activated carbon fibers(ACFs)as an support material for l...The reduction of 4-nitrophenol(4-NP)to 4-aminophenol(4-AP)in wastewater faces challenges in terms of conversion rate and stability.We used coal tar pitch-based activated carbon fibers(ACFs)as an support material for loading transition metal catalysts to catalyze the reaction.Fe-Ni nanoparticles were loaded onto the coal tar pitch-based ACF through a simple hydrothermal-calcination method.The results showed that the coal tar pitch-based ACFs had a high specific surface area(1847 m^(2)/g)and a unique microporous structure,and the metals were loaded onto them.The average diameter of the nanoparticles formed was approximately 100 nm.By changing the metal loading it was shown that the performance was best when the reaction temperature was 45℃,the 4-NP concentration was 2.5 mmol L^(-1),and the molar concentration ratio of Fe^(3+)to Ni^(2+)was 1∶2(total 7.5 mmol L^(-1)).Under these conditions the conversion efficiency reached 99.88%.Fe2.5/Ni5-ACF exhibited excellent catalytic activity and recyclability for 4-NP after five cycles.The inherent advantages of nanomaterials increase the catalytic efficiency of 4-NP,which expands the use of coal tar pitch-based ACFs as supporting materials in the field of catalysis.展开更多
Simultaneously preparing sodium silicate solution with high modulus and obtaining aluminum concentrate with high Al/Si ratio from activated roasting clinker is the key to a new method for clean utilization of coal fly...Simultaneously preparing sodium silicate solution with high modulus and obtaining aluminum concentrate with high Al/Si ratio from activated roasting clinker is the key to a new method for clean utilization of coal fly ash.This study systematically investigates the leaching mechanism of SiO_(2) from activated roasting clinker in sodium silicate solution and proposes an optimized leaching process.The colloidal particles formed by the condensation of siloxane groups increase the diffusion resistance of the leaching agent in the capillary pores,and the SiO_(2) deep inside the pores is difficult to contact with the leaching agent,which is an important reason for the insufficient leaching of SiO_(2) in high modulus sodium silicate solution.A two-stage countercurrent leaching process proposed can simultaneously prepare sodium silicate solution with modulus greater than 2.5 and aluminum concentrate with high Al/Si ratio exceeding 11.This work provides a potential application solution for the development of clean and economically feasible technologies for the utilization of fly ash.展开更多
A series of blue and blue‑green Ir(Ⅲ)complexes has been investigated theoretically to explore their electronic structures,photophysical properties,efficiency roll‑off effect,and thermal activation delayed fluorescenc...A series of blue and blue‑green Ir(Ⅲ)complexes has been investigated theoretically to explore their electronic structures,photophysical properties,efficiency roll‑off effect,and thermal activation delayed fluorescence(TADF)properties.All calculations were performed using density functional theory(DFT)and time‑dependent density functional theory(TDDFT).Calculations for electronic structures,frontier molecular orbital characteristics(which determine the efficiency roll‑off effect of the complexes),and photophysical properties were conducted using the Gaussian 09 software package.The calculation of spin‑orbit coupling matrix elements<T|HSOC|S>,which determine the TADF properties of the complexes,was performed using the ORCA software package.The calculation results show that the auxiliary ligand tetraphenylimidodiphosphinate(tpip),a strong electron‑withdrawing group,can mitigate the efficiency roll‑off effect of the complex.Furthermore,TADF is observed in one of the designed complexes,(F_(3)Phppy)_(2)Ir(tpip),where F_(3)Phppy=2‑[4‑(2,4,6‑trifluorophenyl)phenyl]pyridine.展开更多
Lithium-ion capacitors(LICs)combine the high power dens-ity of electrical double-layer capacitors with the high energy density of lithium-ion batteries.However,they face practical limitations due to the narrow operati...Lithium-ion capacitors(LICs)combine the high power dens-ity of electrical double-layer capacitors with the high energy density of lithium-ion batteries.However,they face practical limitations due to the narrow operating voltage window of their activated carbon(AC)cathodes.We report a scalable thermal treatment strategy to develop high-voltage-tolerant AC cathodes.Through controlled thermal treatment of commer-cial activated carbon(Raw-AC)under a H_(2)/Ar atmosphere at 400-800℃,the targeted reduction of degradation-prone functional groups can be achieved while preserving the critical pore structure and increasing graph-itic microcrystalline ordering.The AC treated at 400℃(HAC-400)had a significant increase in specific capacity(96.0 vs.75.1 mAh/g at 0.05 A/g)and better rate capability(61.1 vs.36.1 mAh/g at 5 A/g)in half-cell LICs,along with an 83.5%capacity retention over 7400 cycles within an extended voltage range of 2.0-4.2 V in full-cell LICs.Scalability was demonstrated by a 120 g batch production,enabling fabrication of pouch-type LICs with commercial hard carbon anodes that delivered a higher energy density of 28.3 Wh/kg at 1 C,and a peak power density of 12.1 kW/kg compared to devices using raw AC.This simple,industry-compatible approach may be used for producing ad-vanced cathode materials for practical high-performance LICs.展开更多
Chemical warfare agents(CWAs)are extremely lethal substances used in warfare and terrorism,capable of causing permanent damage even in small doses,despite medical intervention.Therefore,detection,protection,and detoxi...Chemical warfare agents(CWAs)are extremely lethal substances used in warfare and terrorism,capable of causing permanent damage even in small doses,despite medical intervention.Therefore,detection,protection,and detoxification of CWAs are vital for the safety of first responders,military personnel,and civilians,driving significant research in this area.Herein,we designed and synthesized a poly(-diallyldimethylammonium chloride)(PDDA)mediated cupric oxide(CuO)functionalized activated carbon fabric(ACF),termed ACF@PDDA-CuO,as an adsorbent filter material for self-detoxifying chemical protective clothing.PDDA,a positively charged polyelectrolyte,effectively binds in-situ synthesized CuO to the negatively charged ACF surface,serving as a suitable binder.This study demonstrates the synergistic effects of PDDA-CuO functionalization on ACF,where PDDA treatment enhanced mechanical and comfort properties,and CuO crystal growth significantly improved detoxification efficacy against the CWA Nerve Agent Sarin.Comprehensive analyses,including FTIR,BET surface area analysis,SEM,EDS,TEM,STEM,TGA,XPS,and XRD,confirmed the uniform deposition of CuO and PDDA on the ACF surface.The Cu content on ACF@PDDA-CuO samples was measured via iodometric titration.The materials were evaluated for tensile strength,air permeability,water vapor permeability,nerve agent(Sarin)detoxification,and blister agent(Sulfur Mustard)breakthrough time to assess their applicability for protective clothing.The optimized PDDA-CuO on ACF detoxified 82.04%of Sarin within 18 h,compared to 25.22%by ACF alone,and enhanced tensile strength by 23.67%,air permeability by 24.63%,and water vapor permeability by 3.94%,while maintaining protection against Sulfur Mustard for 24 h.These findings indicate that ACF@PDDA-CuO is a promising candidate for CWA protective clothing,offering robust protection with enhanced comfort.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
A novel heterogeneous catalytic ozonation process in water treatment was studied, with a copper-loaded activated carbon （Cu/AC） that was prepared by an incipient wetness impregnation method at low temperature and te...A novel heterogeneous catalytic ozonation process in water treatment was studied, with a copper-loaded activated carbon （Cu/AC） that was prepared by an incipient wetness impregnation method at low temperature and tested as a catalyst in the ozonation of phenol and oxalic acid. Cu/AC was characterized using XRD, BET and SEM techniques. Compared with ozonation alone, the presence of Cu/AC in the ozonation processes significantly improves the degradation of phenol or oxalic acid. With the introduction of the hydroxyl radical scavenger, i.e., turt-butanol alcohol （t-BuOH）, the degradation efficiency of both phenol and oxalic acid in the Cu/AC catalyzed ozonation process decreases by 22% at 30 min. This indicates that Cu/AC accelerates ozone decomposition into certain concentration of hydroxyl radicals. The amount of Cu（II ） produced during the reaction of Cu/AC-catalyzed ozonation of phenol or oxalic acid is very small, which shows that the two processes are both heterogeneous catalytic ozonation reactions.展开更多
To investigate the influence of the activated carbon pore structure on the adsorption of volatile organic compounds （VOCs）, three commercial activated carbon samples were chosen. The fixed-bed thermostatic adsorptio...To investigate the influence of the activated carbon pore structure on the adsorption of volatile organic compounds （VOCs）, three commercial activated carbon samples were chosen. The fixed-bed thermostatic adsorption experiments were conducted under certain conditions, where toluene, acetone, and 1, 2-dichloroethane acted as adsorbents. Then, the incidence relation between the experimental results and the activated carbon pore structure was analyzed. After that, the results of the correlation analysis were verified in accordance with fractal theory and adsorption characteristic curve analysis. The results show that the pore diameter gradient is helpful for strengthening the intemal diffusion. Under the same condition, the adsorption of organic gases tends to be selective, and the positions of toluene, acetone and 1, 2-dichloroethane adsorbed on the activated carbon are mainly in the ranges of 1.27-1.49 nm, 0.67-0.84 nm and 1.39-1.75 nm, respectively. The relationship between adsorption capacity and activated carbon pore volume can accurately explain the spreading process of the adsorbents in the activated carbon.展开更多
A laboratory scale up-flow biological activated carbon(BAC) reactor was constructed for the advanced treatment of synthetic flotation wastewater. Biodegradation of a common collector(i.e., ethyl xanthate) for non-ferr...A laboratory scale up-flow biological activated carbon(BAC) reactor was constructed for the advanced treatment of synthetic flotation wastewater. Biodegradation of a common collector(i.e., ethyl xanthate) for non-ferrous metallic ore flotation was evaluated. The results show that the two stages of domestication can improve microbial degradation ability. The BAC reactor obtains a chemical oxygen demand(COD) reduction rate of 82.5% for ethyl xanthate and its effluent COD concentration lowers to below 20 mg/L. The kinetics equation of the BAC reactor proves that the activated carbon layers at the height of 0 mm to 70 mm play a key role in the removal of flotation reagents. Ultraviolet spectral analysis indicates that most of the ethyl xanthate are degraded by microorganisms after advanced treatment by the BAC reactor.展开更多
The time-dependent rheological behaviors of alkali-activated cement(AAC)are expected to be precisely controlled,in order to meet the requirements of modern engineering practices.In this paper,the effects of activator,...The time-dependent rheological behaviors of alkali-activated cement(AAC)are expected to be precisely controlled,in order to meet the requirements of modern engineering practices.In this paper,the effects of activator,including the Na_(2)O concentration and SiO_(2)/Na_(2)O(S/N)molar ratio,on the rheological behavior of alkali-activated slag fly ash pastes were investigated.The small amplitude oscillatory shear(SAOS)and shear test were used to evaluate the structural build-up and flowability of pastes.Besides,zeta potential measurement,calorimetric test and thermogravimetric analysis(TGA)were carried out to reveal the physico-chemical mechanisms behind the rheological evolution of fresh pastes.It was found that high Na_(2)O concentration and low S/N molar ratio improved the flowability and structural build-up rate of paste.Moreover,the structural build-up of alkali-activated slag-fly ash pastes consists of two stages,which is controlled by the dissolution of solid reactants and formation of C-(A)-S-H gels,respectively.展开更多
The preparation of activated carbon from Chinese fir sawdust by zinc chloride activation under both nitrogen atmosphere and vacuum conditions was carded out in a self-manufactured vacuum pyrolysis reactor. The effects...The preparation of activated carbon from Chinese fir sawdust by zinc chloride activation under both nitrogen atmosphere and vacuum conditions was carded out in a self-manufactured vacuum pyrolysis reactor. The effects of the system pressure and the activation condition （nitrogen or vacuum） on pore development were investigated. The results show that both high quality activated carbon and high added-value bio-oil can be obtained simultaneously via vacuum chemical activation. The characteristics of the activated carbons produced under vacuum conditions are better than those prepared under nitrogen atmosphere. The performance parameters of the activated carbon obtained under vacuum conditions are as follows： the pore size distribution is mainly microporous, the Brunauer-Emmett-Teller （BET） surface area is 1 070.59 m^2/g, the microporous volume is 0.502 4 cm^3/g, the average pore size is 2.085 nm, and the iodine adsorption value and the methylene blue adsorption value are 1 142.92 and 131.34 mg/g, respectively. The activated carbon from vacuum chemical activation has developed micropores, and the N2 adsorption equilibrium constant of the corresponding activated carbon gradually increases with the decrease of reaction system pressure.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 isotherm,mechanism and kinetics of carbon tetrachloride(CT) adsorption by polyacrylonitrile-based activated carbon fiber(PAN-ACF) were investigated in batch reactors and a continuous flow reactor,and the regenerat...The isotherm,mechanism and kinetics of carbon tetrachloride(CT) adsorption by polyacrylonitrile-based activated carbon fiber(PAN-ACF) were investigated in batch reactors and a continuous flow reactor,and the regeneration of PAN-ACF was also studied.Freundlich and Dubinin-Radushkevich(D-R) adsorption equations can well describe the adsorption isotherm.CT is mainly adsorbed on the exterior surface of PAN-ACF with low boundary layer effect and rate-controlling step of intra-particle diffusion.The adsorption dynamics in the batch reactor well fits with the pseudo-first-order model,and the breakthrough curves in the continuous flow reactor can be well described by the Yoon-Nelson model.The ACF can be recycled through thermal regeneration,whereas the adsorption capacity decreases from 7.87 to 4.98 mg/g after the fourth regeneration.78%-94%of CT can be removed from the wastewater of a fluorine chemical plant on a pilot scale,which confirms the efficacy of ACF under industrial conditions.The results indicate that PAN-ACF is applicable to CT removal from wastewater.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
Activated carbon was prepared from bamboo by mechanochemical process with phosphoric acid as activating agent.The effects of milling time on the adsorption property and porous structure of the obtained activated car-b...Activated carbon was prepared from bamboo by mechanochemical process with phosphoric acid as activating agent.The effects of milling time on the adsorption property and porous structure of the obtained activated car-bon were discussed.The results showed that phosphoric acid activation assisted by mechanochemical process can slightly improve the adsorption performance of the prepared activated carbon.The iodine,methylene blue adsorption value and the specific surface area of the prepared activated carbons increased from 840.16 mg/g,168 mg/g and 1229.246 m/g to 947.51 mg/g,195 mg/g,and 1265.373 m2/g,respectively.Compared with conventional phosphoric acid activation,the activated carbon produced by mechanochemical process has greater adsorption capacity.展开更多
A five steps pressure swing adsorption process was designed for acetone and toluene mixtures separation and recovery. Dynamic distributions of gas phase content and temperature were investigated. Based on the theory o...A five steps pressure swing adsorption process was designed for acetone and toluene mixtures separation and recovery. Dynamic distributions of gas phase content and temperature were investigated. Based on the theory of Soret and Dufour, a non-isothermal mathematical model was developed to simulate the PSA process. Effects of heat and mass transfer coefficients were studied. The coupled Soret and Dufour effects were also evaluated. It is found that the heat transfer coefficient has little effect on mass transfer in adsorption stage. However, it has some impacts in desorption stage. The maximum value of C/C0 increases by about 25% as heat transfer coefficient decreases. The temperature variation is less than 0.05 K with the change of mass transfer coefficient, so that the effect of mass transfer coefficient on heat transfer can be ignored. It is also concluded that the Soret and Dufour coupled effects are not obvious in pressure swing adsorption compared with fixed-bed adsorption.展开更多
The removal efficiencies of heavy metals(As, Cr, Cu, Ni, Pb and Zn) were investigated in the 17 operating municipal wastewater treatment plants(WWTPs) and compared with those in four main activated sludge processes. S...The removal efficiencies of heavy metals(As, Cr, Cu, Ni, Pb and Zn) were investigated in the 17 operating municipal wastewater treatment plants(WWTPs) and compared with those in four main activated sludge processes. Significant differences of heavy metal removal efficiencies were observed among four activated sludge processes. The removal efficiency for As(75.5%) in the oxidation ditch(OD) process is significantly higher than that in the conventional activated sludge(CAS) process(38.6%) or sequencing batch reactor(SBR) process(51.4%). The mean removal efficiencies for Cu and Ni in the OD process are 90.5% and 46.7%, respectively, while low mean removal efficiencies are observed for Cu(69.9%) and Ni(16.5%), respectively, in the SBR process. The removal efficiencies for Cu and Ni in the OD process are significantly higher than those in the anaerobic-anoxic-oxic(A2-O) process. These results highlight the differences of removal efficiencies for heavy metals in different processes and should be considered when selecting a wastewater treatment process.展开更多
文摘Lithium–sulfur(Li–S)batteries are promisingcandidates for next-generation energy storagegiven their high energy density and potential low cost.Chemically activated carbon(CAC)is often used fortheir cathodes,because it has a high specific surfacearea for sulfur loading.We have developed a pressurizedphysical activation(PPA)method that producedan activated carbon(PPAC)with a high specific surfacearea comparable to that of CAC.The pore structure of PPAC could be changed and its use as a cathode material for Li–Sbatteries was investigated.Battery tests at different capacity rates(C-rates)showed that it had a much improved high-rate performancewith a discharge capacity of 900 mAh/(g of sulfur)at 1 C,in contrast to only 600 mAh/(g of sulfur)for CAC.Porestructure analyses showed that PPAC prepared at a high activation temperature(1000℃)had unusual channel-like mesoporesbetween the microdomains that are the basic structural units of artificial carbon materials.These are connected to microporesdeveloped in each microdomain,and deliver ions from the surroundings to the internal pores and vice versa.The well-developedmicropores and mesopores of PPAC respectively ensured the high adsorption of lithium polysulfides and a high rate ofion diffusion.Compared to CAC,PPAC is a high-performance,low-cost cathode material that is promising for use in futureLi–S batteries.
文摘Aqueous zincion capacitors(ZICs)have significant potential as energy storage systems because of their high specific capacity and superior reliability.Heteroatom-doped carbon materials were known to substantially increase the capacitance of ZICs,however the mechanism remains poorly understood.Coal-based activated carbon was functionalized with B and N to serve as the cathode material in ZICs.This modification gave the material a high specific capacity of 371.4 mAh g^(-1)at 1 A g^(-1)and it retained 74%of its initial capacity after 10000 cycles.Experimental results and density functional theory calculations revealed that pyridinic N plays a crucial role in increasing Zn^(2+)storage,demonstrating superior electrochemical reversibility.This work gives valuable insight into the design of high-capacity and ultrafast pseudocapacitive carbon cathodes for ZICs.
基金Supported by the Science and Technology Cooperation and Exchange special project of Cooperation of Shanxi Province(202404041101014)the Fundamental Research Program of Shanxi Province(202403021212333)+3 种基金the Joint Funds of the National Natural Science Foundation of China(U24A20555)the Lvliang Key R&D of University-Local Cooperation(2023XDHZ10)the Initiation Fund for Doctoral Research of Taiyuan University of Science and Technology(20242026)the Outstanding Doctor Funding Award of Shanxi Province(20242080).
文摘To elucidate the effect of calcite-regulated activated carbon(AC)structure on low-temperature denitrification performance of SCR catalysts,this work prepared a series of Mn-Ce/De-AC-xCaCO_(3)(x is the calcite content in coal)catalysts were prepared by the incipient wetness impregnation method,followed by acid washing to remove calcium-containing minerals.Comprehensive characterization and low-temperature denitrification tests revealed that calcite-induced structural modulation of coal-derived AC significantly enhances catalytic activity.Specifically,NO conversion increased from 88.3%of Mn-Ce/De-AC to 91.7%of Mn-Ce/De-AC-1CaCO_(3)(210℃).The improved SCR denitrification activity results from the enhancement of physicochemical properties including higher Mn^(4+)content and Ce^(4+)/Ce^(3+)ratio,an abundance of chemisorbed oxygen and acidic sites,which could strengthen the SCR reaction pathways(richer NH_(3)activated species and bidentate nitrate active species).Therefore,NO removal is enhanced.
文摘The reduction of 4-nitrophenol(4-NP)to 4-aminophenol(4-AP)in wastewater faces challenges in terms of conversion rate and stability.We used coal tar pitch-based activated carbon fibers(ACFs)as an support material for loading transition metal catalysts to catalyze the reaction.Fe-Ni nanoparticles were loaded onto the coal tar pitch-based ACF through a simple hydrothermal-calcination method.The results showed that the coal tar pitch-based ACFs had a high specific surface area(1847 m^(2)/g)and a unique microporous structure,and the metals were loaded onto them.The average diameter of the nanoparticles formed was approximately 100 nm.By changing the metal loading it was shown that the performance was best when the reaction temperature was 45℃,the 4-NP concentration was 2.5 mmol L^(-1),and the molar concentration ratio of Fe^(3+)to Ni^(2+)was 1∶2(total 7.5 mmol L^(-1)).Under these conditions the conversion efficiency reached 99.88%.Fe2.5/Ni5-ACF exhibited excellent catalytic activity and recyclability for 4-NP after five cycles.The inherent advantages of nanomaterials increase the catalytic efficiency of 4-NP,which expands the use of coal tar pitch-based ACFs as supporting materials in the field of catalysis.
基金Project(52374362)supported by the National Natural Science Foundation of ChinaProject(2022YFC3900901)supported by the National Key Research and Development Program of China。
文摘Simultaneously preparing sodium silicate solution with high modulus and obtaining aluminum concentrate with high Al/Si ratio from activated roasting clinker is the key to a new method for clean utilization of coal fly ash.This study systematically investigates the leaching mechanism of SiO_(2) from activated roasting clinker in sodium silicate solution and proposes an optimized leaching process.The colloidal particles formed by the condensation of siloxane groups increase the diffusion resistance of the leaching agent in the capillary pores,and the SiO_(2) deep inside the pores is difficult to contact with the leaching agent,which is an important reason for the insufficient leaching of SiO_(2) in high modulus sodium silicate solution.A two-stage countercurrent leaching process proposed can simultaneously prepare sodium silicate solution with modulus greater than 2.5 and aluminum concentrate with high Al/Si ratio exceeding 11.This work provides a potential application solution for the development of clean and economically feasible technologies for the utilization of fly ash.
文摘A series of blue and blue‑green Ir(Ⅲ)complexes has been investigated theoretically to explore their electronic structures,photophysical properties,efficiency roll‑off effect,and thermal activation delayed fluorescence(TADF)properties.All calculations were performed using density functional theory(DFT)and time‑dependent density functional theory(TDDFT).Calculations for electronic structures,frontier molecular orbital characteristics(which determine the efficiency roll‑off effect of the complexes),and photophysical properties were conducted using the Gaussian 09 software package.The calculation of spin‑orbit coupling matrix elements<T|HSOC|S>,which determine the TADF properties of the complexes,was performed using the ORCA software package.The calculation results show that the auxiliary ligand tetraphenylimidodiphosphinate(tpip),a strong electron‑withdrawing group,can mitigate the efficiency roll‑off effect of the complex.Furthermore,TADF is observed in one of the designed complexes,(F_(3)Phppy)_(2)Ir(tpip),where F_(3)Phppy=2‑[4‑(2,4,6‑trifluorophenyl)phenyl]pyridine.
文摘Lithium-ion capacitors(LICs)combine the high power dens-ity of electrical double-layer capacitors with the high energy density of lithium-ion batteries.However,they face practical limitations due to the narrow operating voltage window of their activated carbon(AC)cathodes.We report a scalable thermal treatment strategy to develop high-voltage-tolerant AC cathodes.Through controlled thermal treatment of commer-cial activated carbon(Raw-AC)under a H_(2)/Ar atmosphere at 400-800℃,the targeted reduction of degradation-prone functional groups can be achieved while preserving the critical pore structure and increasing graph-itic microcrystalline ordering.The AC treated at 400℃(HAC-400)had a significant increase in specific capacity(96.0 vs.75.1 mAh/g at 0.05 A/g)and better rate capability(61.1 vs.36.1 mAh/g at 5 A/g)in half-cell LICs,along with an 83.5%capacity retention over 7400 cycles within an extended voltage range of 2.0-4.2 V in full-cell LICs.Scalability was demonstrated by a 120 g batch production,enabling fabrication of pouch-type LICs with commercial hard carbon anodes that delivered a higher energy density of 28.3 Wh/kg at 1 C,and a peak power density of 12.1 kW/kg compared to devices using raw AC.This simple,industry-compatible approach may be used for producing ad-vanced cathode materials for practical high-performance LICs.
基金Defence Research and Development Establishment(DRDE),DRDO,Gwalior-474002,(India)for his keen interestencouragement.The DRDE accession number for this manuscript is DRDE-IREC-130-28/03/2024.
文摘Chemical warfare agents(CWAs)are extremely lethal substances used in warfare and terrorism,capable of causing permanent damage even in small doses,despite medical intervention.Therefore,detection,protection,and detoxification of CWAs are vital for the safety of first responders,military personnel,and civilians,driving significant research in this area.Herein,we designed and synthesized a poly(-diallyldimethylammonium chloride)(PDDA)mediated cupric oxide(CuO)functionalized activated carbon fabric(ACF),termed ACF@PDDA-CuO,as an adsorbent filter material for self-detoxifying chemical protective clothing.PDDA,a positively charged polyelectrolyte,effectively binds in-situ synthesized CuO to the negatively charged ACF surface,serving as a suitable binder.This study demonstrates the synergistic effects of PDDA-CuO functionalization on ACF,where PDDA treatment enhanced mechanical and comfort properties,and CuO crystal growth significantly improved detoxification efficacy against the CWA Nerve Agent Sarin.Comprehensive analyses,including FTIR,BET surface area analysis,SEM,EDS,TEM,STEM,TGA,XPS,and XRD,confirmed the uniform deposition of CuO and PDDA on the ACF surface.The Cu content on ACF@PDDA-CuO samples was measured via iodometric titration.The materials were evaluated for tensile strength,air permeability,water vapor permeability,nerve agent(Sarin)detoxification,and blister agent(Sulfur Mustard)breakthrough time to assess their applicability for protective clothing.The optimized PDDA-CuO on ACF detoxified 82.04%of Sarin within 18 h,compared to 25.22%by ACF alone,and enhanced tensile strength by 23.67%,air permeability by 24.63%,and water vapor permeability by 3.94%,while maintaining protection against Sulfur Mustard for 24 h.These findings indicate that ACF@PDDA-CuO is a promising candidate for CWA protective clothing,offering robust protection with enhanced comfort.
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.
基金Project(40973074) supported by the National Natural Science Foundation of China
文摘A novel heterogeneous catalytic ozonation process in water treatment was studied, with a copper-loaded activated carbon （Cu/AC） that was prepared by an incipient wetness impregnation method at low temperature and tested as a catalyst in the ozonation of phenol and oxalic acid. Cu/AC was characterized using XRD, BET and SEM techniques. Compared with ozonation alone, the presence of Cu/AC in the ozonation processes significantly improves the degradation of phenol or oxalic acid. With the introduction of the hydroxyl radical scavenger, i.e., turt-butanol alcohol （t-BuOH）, the degradation efficiency of both phenol and oxalic acid in the Cu/AC catalyzed ozonation process decreases by 22% at 30 min. This indicates that Cu/AC accelerates ozone decomposition into certain concentration of hydroxyl radicals. The amount of Cu（II ） produced during the reaction of Cu/AC-catalyzed ozonation of phenol or oxalic acid is very small, which shows that the two processes are both heterogeneous catalytic ozonation reactions.
基金Projects(20976200)supported by the National Natural Science Foundation of China
文摘To investigate the influence of the activated carbon pore structure on the adsorption of volatile organic compounds （VOCs）, three commercial activated carbon samples were chosen. The fixed-bed thermostatic adsorption experiments were conducted under certain conditions, where toluene, acetone, and 1, 2-dichloroethane acted as adsorbents. Then, the incidence relation between the experimental results and the activated carbon pore structure was analyzed. After that, the results of the correlation analysis were verified in accordance with fractal theory and adsorption characteristic curve analysis. The results show that the pore diameter gradient is helpful for strengthening the intemal diffusion. Under the same condition, the adsorption of organic gases tends to be selective, and the positions of toluene, acetone and 1, 2-dichloroethane adsorbed on the activated carbon are mainly in the ranges of 1.27-1.49 nm, 0.67-0.84 nm and 1.39-1.75 nm, respectively. The relationship between adsorption capacity and activated carbon pore volume can accurately explain the spreading process of the adsorbents in the activated carbon.
基金Project(201209013)supported by Special Fund for Environmental Scientific Research in the Public Interest,China
文摘A laboratory scale up-flow biological activated carbon(BAC) reactor was constructed for the advanced treatment of synthetic flotation wastewater. Biodegradation of a common collector(i.e., ethyl xanthate) for non-ferrous metallic ore flotation was evaluated. The results show that the two stages of domestication can improve microbial degradation ability. The BAC reactor obtains a chemical oxygen demand(COD) reduction rate of 82.5% for ethyl xanthate and its effluent COD concentration lowers to below 20 mg/L. The kinetics equation of the BAC reactor proves that the activated carbon layers at the height of 0 mm to 70 mm play a key role in the removal of flotation reagents. Ultraviolet spectral analysis indicates that most of the ethyl xanthate are degraded by microorganisms after advanced treatment by the BAC reactor.
基金Project(2017 YFB 0310100)supported by National Key R&D Program of ChinaProjects(51778629,51922109)supported by the National Natural Science Foundation of ChinaProjects(2020 zzts 617,2020 CX 011)supported by the Innovation-Driven Project of Central South University,China。
文摘The time-dependent rheological behaviors of alkali-activated cement(AAC)are expected to be precisely controlled,in order to meet the requirements of modern engineering practices.In this paper,the effects of activator,including the Na_(2)O concentration and SiO_(2)/Na_(2)O(S/N)molar ratio,on the rheological behavior of alkali-activated slag fly ash pastes were investigated.The small amplitude oscillatory shear(SAOS)and shear test were used to evaluate the structural build-up and flowability of pastes.Besides,zeta potential measurement,calorimetric test and thermogravimetric analysis(TGA)were carried out to reveal the physico-chemical mechanisms behind the rheological evolution of fresh pastes.It was found that high Na_(2)O concentration and low S/N molar ratio improved the flowability and structural build-up rate of paste.Moreover,the structural build-up of alkali-activated slag-fly ash pastes consists of two stages,which is controlled by the dissolution of solid reactants and formation of C-(A)-S-H gels,respectively.
文摘The preparation of activated carbon from Chinese fir sawdust by zinc chloride activation under both nitrogen atmosphere and vacuum conditions was carded out in a self-manufactured vacuum pyrolysis reactor. The effects of the system pressure and the activation condition （nitrogen or vacuum） on pore development were investigated. The results show that both high quality activated carbon and high added-value bio-oil can be obtained simultaneously via vacuum chemical activation. The characteristics of the activated carbons produced under vacuum conditions are better than those prepared under nitrogen atmosphere. The performance parameters of the activated carbon obtained under vacuum conditions are as follows： the pore size distribution is mainly microporous, the Brunauer-Emmett-Teller （BET） surface area is 1 070.59 m^2/g, the microporous volume is 0.502 4 cm^3/g, the average pore size is 2.085 nm, and the iodine adsorption value and the methylene blue adsorption value are 1 142.92 and 131.34 mg/g, respectively. The activated carbon from vacuum chemical activation has developed micropores, and the N2 adsorption equilibrium constant of the corresponding activated carbon gradually increases with the decrease of reaction system pressure.
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(2004C33068) supported by the Science and Technology Programs of Zhejiang Province,ChinaProject(20100933B17) supported by the Social Development and Science Research Program of Hangzhou,China
文摘The isotherm,mechanism and kinetics of carbon tetrachloride(CT) adsorption by polyacrylonitrile-based activated carbon fiber(PAN-ACF) were investigated in batch reactors and a continuous flow reactor,and the regeneration of PAN-ACF was also studied.Freundlich and Dubinin-Radushkevich(D-R) adsorption equations can well describe the adsorption isotherm.CT is mainly adsorbed on the exterior surface of PAN-ACF with low boundary layer effect and rate-controlling step of intra-particle diffusion.The adsorption dynamics in the batch reactor well fits with the pseudo-first-order model,and the breakthrough curves in the continuous flow reactor can be well described by the Yoon-Nelson model.The ACF can be recycled through thermal regeneration,whereas the adsorption capacity decreases from 7.87 to 4.98 mg/g after the fourth regeneration.78%-94%of CT can be removed from the wastewater of a fluorine chemical plant on a pilot scale,which confirms the efficacy of ACF under industrial conditions.The results indicate that PAN-ACF is applicable to CT removal from wastewater.
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.
文摘Activated carbon was prepared from bamboo by mechanochemical process with phosphoric acid as activating agent.The effects of milling time on the adsorption property and porous structure of the obtained activated car-bon were discussed.The results showed that phosphoric acid activation assisted by mechanochemical process can slightly improve the adsorption performance of the prepared activated carbon.The iodine,methylene blue adsorption value and the specific surface area of the prepared activated carbons increased from 840.16 mg/g,168 mg/g and 1229.246 m/g to 947.51 mg/g,195 mg/g,and 1265.373 m2/g,respectively.Compared with conventional phosphoric acid activation,the activated carbon produced by mechanochemical process has greater adsorption capacity.
基金Projects(20976200,20676154) supported by the National Natural Science Foundation of China
文摘A five steps pressure swing adsorption process was designed for acetone and toluene mixtures separation and recovery. Dynamic distributions of gas phase content and temperature were investigated. Based on the theory of Soret and Dufour, a non-isothermal mathematical model was developed to simulate the PSA process. Effects of heat and mass transfer coefficients were studied. The coupled Soret and Dufour effects were also evaluated. It is found that the heat transfer coefficient has little effect on mass transfer in adsorption stage. However, it has some impacts in desorption stage. The maximum value of C/C0 increases by about 25% as heat transfer coefficient decreases. The temperature variation is less than 0.05 K with the change of mass transfer coefficient, so that the effect of mass transfer coefficient on heat transfer can be ignored. It is also concluded that the Soret and Dufour coupled effects are not obvious in pressure swing adsorption compared with fixed-bed adsorption.
基金Project(2012AA06A202)supported by Hi-tech Research and Development Project of China
文摘The removal efficiencies of heavy metals(As, Cr, Cu, Ni, Pb and Zn) were investigated in the 17 operating municipal wastewater treatment plants(WWTPs) and compared with those in four main activated sludge processes. Significant differences of heavy metal removal efficiencies were observed among four activated sludge processes. The removal efficiency for As(75.5%) in the oxidation ditch(OD) process is significantly higher than that in the conventional activated sludge(CAS) process(38.6%) or sequencing batch reactor(SBR) process(51.4%). The mean removal efficiencies for Cu and Ni in the OD process are 90.5% and 46.7%, respectively, while low mean removal efficiencies are observed for Cu(69.9%) and Ni(16.5%), respectively, in the SBR process. The removal efficiencies for Cu and Ni in the OD process are significantly higher than those in the anaerobic-anoxic-oxic(A2-O) process. These results highlight the differences of removal efficiencies for heavy metals in different processes and should be considered when selecting a wastewater treatment process.
