The global distributions of the air-sea CO2 transfer velocity and flux are retrieved from TOPEX/Poseidon and Jason altimeter data from October 1992 to December 2009 using a combined algorithm. The 17 a average global,...The global distributions of the air-sea CO2 transfer velocity and flux are retrieved from TOPEX/Poseidon and Jason altimeter data from October 1992 to December 2009 using a combined algorithm. The 17 a average global, area-weighted, Schmidt number-corrected mean gas transfer velocity is 21.26 cm/h, and the full exploration of the uncertainty of this estimate awaits further data. The average total CO2 flux (calculated by carbon) from atmosphere to ocean during the 17 a was 2.58 Pg/a. The highest transfer velocity is in the circumpolar current area, because of constant high wind speeds and currents there. This results in strong CO2 fluxes. CO2 fluxes are strong but opposite direction in the equatorial east Pacific Ocean, because the air-sea CO2 partial pressure difference is the largest in the global cceans. The results differ from the previous studies calculated using the wind speed. It is demonstrated that the air-sea transfer velocity is very important for estimating air-sea CO2 flux. It is critical to have an accurate estimation for improving calculation of CO2 flux within climate change studies.展开更多
Periodic density functional theory calculations have been performed to investigate the chemisorption behavior of COz molecule on a series of surface alloys that are built by dispersing individual middle-late transitio...Periodic density functional theory calculations have been performed to investigate the chemisorption behavior of COz molecule on a series of surface alloys that are built by dispersing individual middle-late transition metal (TM) atoms (TM = Fe, Co, Ni, Ru, Rh, Pd, Ag, Os, lr, Pt, Au) on the Cu(100) and Cu(lll) surfaces. The most stable configurations of CO2 chemisorbed on different TM/Cu surfaces are determined, and the results show that among the late transition metals, Co, Ru, and Os are potentially good dopants to enhance the chemisorption and activation of CO2 on copper surfaces. To obtain a deep understanding of the adsorption property, the bonding characteristics of the adsorption bonds are carefully examined by the crystal orbital Hamilton population technique, which reveals that the TM atom primarily provides d orbitals with z-component, namely dz2, dxz, and dvz orbitals to interact with the adsorbate.展开更多
In this letter ab initio electronic structure calculations are performed for extensive geometries Of CS2. A newly written program is used to fit the computed energies into the Sorbie-Murrel function, whose contour plo...In this letter ab initio electronic structure calculations are performed for extensive geometries Of CS2. A newly written program is used to fit the computed energies into the Sorbie-Murrel function, whose contour plots are illustrated.展开更多
The carbon layers on implanted steel surface have been studied by means of Auger spectra. It is shown that the thickness of the carbon layer is proportional to the dose of implanted ions. By comparison with the result...The carbon layers on implanted steel surface have been studied by means of Auger spectra. It is shown that the thickness of the carbon layer is proportional to the dose of implanted ions. By comparison with the results of friction and wear tests, the friction coefficient is smaller than 0.20 at the first part of the friction coefficient curve. It is considered that the graphitic carbon layer on the top of steel is helpful to reducing the surface friction coefficient of steel.展开更多
Surface functionalization of carbon nanofibers(CNFs) was carried out, i e, CNFs were firstly oxidized and then the surface was silanized by 3-Aminopropyltriethoxysilane(APTES) via an assembly method. A new kind of...Surface functionalization of carbon nanofibers(CNFs) was carried out, i e, CNFs were firstly oxidized and then the surface was silanized by 3-Aminopropyltriethoxysilane(APTES) via an assembly method. A new kind of high wear resistance s-CNFs/epoxy composite was fabricated by in-situ reaction. FTIR spectroscopy was used to detect the changes of the functional groups produced by silane on the surface of CNFs. The tribological properties and microstructures of modified and unmodified CNFs/epoxy composites were studied, respectively. The expremental results indicate that APTES is covalently linked to the surface of CNFs successfully and improves the dispersion of CNF in epoxy matrix. The friction coefficients and the wear rates of s-CNFs/epoxy composites are evidently lower than those of u-CNFs/epoxy composites under the same loads. Investigations also indicate that abrasive wear is the main wear mechanism for u-CNFs/epoxy composite, with slight adhesive wear for s-CNFs/epoxy composite under the same sliding wear condition.展开更多
Carbon deposition on nickel powders in methane involves three stages in different reaction temperature ranges. Temperature programing oxidation test and Raman spectrum results indicated the formation of complex and or...Carbon deposition on nickel powders in methane involves three stages in different reaction temperature ranges. Temperature programing oxidation test and Raman spectrum results indicated the formation of complex and ordered carbon structures at high deposition temperatures. The values of I(D)/I(G) of the deposited carbon reached 1.86, 1.30, and 1.22 in the first, second, and third stages, respectively. The structure of carbon in the second stage was similar to that in the third stage. Carbon deposited in the first stage rarely contained homogeneous pyrolytic deposit layers. A kinetic model was developed to analyze the carbon deposition behavior in the first stage. The rate-determining step of the first stage is supposed to be interfacial reaction. Based on the investigation of carbon deposition kinetics on nickel powders from different resources, carbon deposition rate is suggested to have a linear relation with the square of specific surface area of nickel particles.展开更多
A series of high surface area graphitic carbon materials (HSGCs) were prepared by ball-milling method. Effect of the graphitic degree of HSGCs on the catalytic performance of Ba-Ru-K/HSGC-x (x is the ball-milling t...A series of high surface area graphitic carbon materials (HSGCs) were prepared by ball-milling method. Effect of the graphitic degree of HSGCs on the catalytic performance of Ba-Ru-K/HSGC-x (x is the ball-milling time in hour) catalysts was studied using ammonia synthesis as a probe reaction. The graphitic degree and pore structure of HSGC-x supports could be successfully tuned via the variation of ball-milling time. Ru nanoparticles of different Ba-Ru-K/HSGC-x catalysts are homogeneously distributed on the supports with the particle sizes ranging from 1.6 to 2.0 nm. The graphitic degree of the support is closely related to its facile electron transfer capability and so plays an important role in improving the intrinsic catalytic performance of Ba-Ru-K/HSGC-x catalyst.展开更多
A series of activated carbons from Taixi anthracite were prepared by steam activation in the presence of KOH and then they were modified by different methods. The regulation of porosity and the modification of surface...A series of activated carbons from Taixi anthracite were prepared by steam activation in the presence of KOH and then they were modified by different methods. The regulation of porosity and the modification of surface chemistry were carried out with the aim to improve the benzene adsorption capacity of activated carbon. The influences of KOH and activation process parameters including activation temperature, activation time and steam flow rate on porosity of activated carbon were evaluated, and the effect of modification methods on surface chemistry was investigated. Also, the relationship between benzene adsorption capacity and porosity and surface chemistry was analyzed. Results show that activation temperature is the dominant factor in the activation process; the introduction of KOH into the raw material can enhance the reactivity of char in activation process, meanwhile it shows a negative effect on the porosity development, especially on the mesopore development. Results of FTIR analysis indicate that anthracite-based activated carbon with condensed aromatics and chemically inert oxygen does not present the nature to be surface modified. Besides, benzene adsorption capacity has an approximate linear relationship with surface area and in our preparation, benzene adsorption capacity and surface area of activated carbon are up to 1210 m 2 /g and 423 mg/g, respectively.展开更多
Facile production of high quality activated carbons from biomass materials has greatly triggered much attention presently. In this paper, a series of interconnected porous carbon materials from lotus root shells bioma...Facile production of high quality activated carbons from biomass materials has greatly triggered much attention presently. In this paper, a series of interconnected porous carbon materials from lotus root shells biomass are prepared via simple pyrolysis and followed by a KOH activation process. The prepared carbons exhibit high specific surface areas of up to 2961 m^2/g and large pore volume~1.47 cm3/g. In addition, the resultant porous carbons served as electrode materials in supercapacitor exhibit high specific capacitance and outstanding recycling stability and high energy density. In particular, their specific capacitance retention was almost 100% after 10500 cycles at a current density of 2 A/g. Remarkabely, the impact of the tailored specific surface areas of various carbon samples on their capacitive performances is systematically investigated.Generally, it was believed that the highly-developed porosity features(including surface areas and pore volume and pore size-distributions), together with the good conductivity of activated carbon species, play a key role in effectively improving the storage energy performances of the porous carbon electrode materials in supercapacitor.展开更多
Taming the electron transfer across metal–support interfaces appears to be an attractive yet challenging methodology to boost catalytic properties.Herein,we demonstrate a precise engineering strategy for the carbon s...Taming the electron transfer across metal–support interfaces appears to be an attractive yet challenging methodology to boost catalytic properties.Herein,we demonstrate a precise engineering strategy for the carbon surface chemistry of Pt/C catalysts—that is,for the electron-withdrawing/donating oxygencontaining groups on the carbon surface—to fine-tune the electrons of the supported metal nanoparticles.Taking the ammonia borane hydrolysis as an example,a combination of density functional theory(DFT)calculations,advanced characterizations,and kinetics and isotopic analyses reveals quantifiable relationships among the carbon surface chemistry,Pt charge state and binding energy,activation entropy/enthalpy,and resultant catalytic activity.After decoupling the influences of other factors,the Pt charge is unprecedentedly identified as an experimentally measurable descriptor of the Pt active site,contributing to a 15-fold increment in the hydrogen generation rate.Further incorporating the Pt charge with the number of Pt active sites,a mesokinetics model is proposed for the first time that can individually quantify the contributions of the electronic and geometric properties to precisely predict the catalytic performance.Our results demonstrate a potentially groundbreaking methodology to design and manipulate metal–carbon catalysts with desirable properties.展开更多
A novel carbon-sulfur nano-composite material was synthesized by heating sublimed sulfur and high surface area activated carbon (HSAAC) under certain conditions. The physical and chemical per- formances of the novel...A novel carbon-sulfur nano-composite material was synthesized by heating sublimed sulfur and high surface area activated carbon (HSAAC) under certain conditions. The physical and chemical per- formances of the novel carbon-sulfur nano-composite were characterized by scanning electron microscopy (SEM), Brunauer-Emmett-Teller (BET) and X-ray diffraction (XRD). The electrochemical performances of nano-composite were characterized by charge-discharge characteristic, cyclic voltammetry and electrochemical impendence spectroscopy (EIS). The experimental results indicate that the electrochemical capability of nano- composite material was superior to that of traditional S-containing composite material. The cathode made by carbon-sulfur nano-composite material shows a good cycle ability and a high specific charge-discharge capacity. The HSAAC shows a vital role in adsorbing sublimed sulfur and the polysulfides within the cathode and is an excellent electric conductor for a sulfur cathode and prevents the shuttle behavior of the lithium-sulfur battery.展开更多
Sodium carbonate and carboxymethyl cellulose powders are compressed into two-component tablets with three mass ratios,97%:3%,95%:5% and 93%:7%.The dissolution tests for two-component tablets and reference pure sodium ...Sodium carbonate and carboxymethyl cellulose powders are compressed into two-component tablets with three mass ratios,97%:3%,95%:5% and 93%:7%.The dissolution tests for two-component tablets and reference pure sodium carbonate tablets are carried out at various temperatures.The dissolution process of each tablet is measured by electrical conductivity tracking method and the concentration of dissolved sodium carbonate is quanti fied with calibrated conductivity-concentration converting equation of sodium carbonate.The quanti fied dissolution data is fitted with both surface reaction model and diffusion layer model and the results clearly show that surface reaction model is suggested as the appropriate dissolution model for all measured tablets.Therefore,it is determined that carboxymethyl cellulose is a stable element to remain the dissolution mechanism of tablet unchanged.The dissolution rate constant quanti fied with surface reaction model presents that carboxymethyl cellulose-sodium carbonate two-component tablets obtain signi ficant higher dissolution rate constant than pure sodium carbonate tablet and higher proportion of carboxymethyl cellulose leads to apparent higher dissolution rate constant.The results prove for the usage of carboxymethyl cellulose in most practical applications at a relative low-level,the effect of carboxymethyl cellulose is effective and positive for two-component tablet to enhance the dissolution process and improve dissolution rate constant and this effect is speculated coming from its dynamic physical transforming process in water including dilation and conglutination.展开更多
Different oxygen and nitrogen containing functional groups were created on the surface of the multiwalled carbon nanotubes. The multi-walled carbon nanotubes were treated in ultrasonic bath with sulfuric or nitric aci...Different oxygen and nitrogen containing functional groups were created on the surface of the multiwalled carbon nanotubes. The multi-walled carbon nanotubes were treated in ultrasonic bath with sulfuric or nitric acid. Furthermore the surface texture was modified by increase of the roughness. In particular after treatment with the oxidizing nitric acid, in comparison to the H2SO4 or ultra-sonic treated samples,craters and edges are dominating the surface structures. Manganese oxide was deposited on the multiwalled carbon nanotubes by precipitation mechanism. Various manganese oxides are formed during the deposition process. The samples were characterized by elemental analysis, microscopy, thermal analysis,Raman spectroscopy, and by the zeta potential as well as X-ray diffraction measurements. It was shown that the deposited manganese oxides are stabilized rather by surface texture of the multi-walled carbon nanotubes than by created functional groups.展开更多
Composites of carbon aerogel and graphite oxide(GO) were synthesized using a self-assembly method based on dispersive forces. Their surface was modified by treatment in hydrogen sulfide at 650 and800 ℃. The samples...Composites of carbon aerogel and graphite oxide(GO) were synthesized using a self-assembly method based on dispersive forces. Their surface was modified by treatment in hydrogen sulfide at 650 and800 ℃. The samples obtained were characterized by adsorption of nitrogen, TA-MS, XPS, potentiometric titration, and HRTEM and tested as catalysts for oxygen reduction reactions(ORR) in an alkaline medium.The synergistic effect of the composite(electrical conductivity, porosity and surface chemistry) leads to a good ORR catalytic activity. The onset potential for the composite of carbon aerogel heated at 800 ℃ is shifted to a more positive value and the number of electron transfer was 2e-at the potential 0.68 V versus RHE and it increased to 4e-with an increase in the negative values of the potential. An excellent tolerance to methanol crossover was also recorded.展开更多
The purpose of this study was to investigate the effect of preadsorbed CO at different temperatures, calcination temperatures, the combined influence of reduction temperature and time, and pretreatment using hydrogen ...The purpose of this study was to investigate the effect of preadsorbed CO at different temperatures, calcination temperatures, the combined influence of reduction temperature and time, and pretreatment using hydrogen or syngas as reduction agents on the F-T synthesis (FTS) activity and selectivity of Co/Al2O3 catalyst. The reactivity of the carbon species at higher preadsorption temperature with H2 in TPSR decreased, whereas the carbon-containing species showed higher reactivity over Co/Al2O3 catalyst with low calcination temperature. This agreed well with the order of catalytic activity for F-T synthesis on this catalyst. The catalytic activity of the catalyst varied with reduction temperature and time remarkably. CODEX optimization gave an optimum reduction temperature of 756 K and reduction time of 6.2 h and estimated C5+ yield perfectly. The pretreatment of Co/Al2O3 catalyst with different reduction agents (hydrogen or syngas) showed important influences on the catalytic performance. A high CO conversion and C5+ yield were obtained on the catalyst reduced by hydrogen, whereas methane selectivity on the catalyst reduced by syngas was much higher than that on the catalyst reduced by hydrogen.展开更多
Silver coatings on the exterior surface of monolithic activated carbon(MAC) with different morphology were prepared by directly immersing MAC into [Ag(NH3)2]NO3 solution. Acid and base treatments were employed to ...Silver coatings on the exterior surface of monolithic activated carbon(MAC) with different morphology were prepared by directly immersing MAC into [Ag(NH3)2]NO3 solution. Acid and base treatments were employed to modify the surface oxygenic groups of MAC, respectively. The MACs' Brunauer-EmmettTeller(BET) surface area, surface groups, and silver coating morphology were characterized by N2 adsorption, elemental analysis(EA), X-ray photoelectron spectroscopy(XPS), and scanning electron microscopy(SEM), respectively. The coating morphology was found to be closely related to the surface area and surface functional groups of MAC. For a raw MAC which contained a variety of oxygenic groups, HNO3 treatment enhanced the relative amount of highly oxidized groups such as carboxyl and carbonates, which disfavored the deposition of silver particles. By contrast, Na OH treatment significantly improved the amount of carbonyl groups, which in turn improved the deposition amount of silver. Importantly, lamella silver was produced on raw MAC while Na OH treatment resulted in granular particles because of the capping effect of carbonyl groups. At appropriate [Ag(NH3)2]NO3 concentrations, silver nanoparticles smaller than 100 nm were homogeneously dispersed on Na OH-treated MAC. The successful tuning of the size and morphology of silver coatings on MAC is promising for novel applications in air purification and for antibacterial or aesthetic purposes.展开更多
Carbon-sulfur nano-composite cathodes for lithium rechargeable batteries were investigated by electrochemical impedance spectroscopy (EIS). The novel carbon-sulfur nano-composite material was synthesized by heating su...Carbon-sulfur nano-composite cathodes for lithium rechargeable batteries were investigated by electrochemical impedance spectroscopy (EIS). The novel carbon-sulfur nano-composite material was synthesized by heating sublimed sulfur and high surface area activated carbon (HSAAC) in certain conditions. Equivalent circuits were used to fit the spectra at different discharge states. The variations of impedance spectra, charge-transfer resistance and double layer capacitance were discussed. The changes of EIS with potential were analyzed based on a plausible electrical equivalent circuit model, and some parameters were measured and analyzed about electrochemical performance and state of charge and discharge of the electrode. The good accuracy in fitting values of the model to the experimental data indicates that the mathematical model gives out a satisfying description upon the mechanism of high rate of capacity fade in lithium-sulfur battery.展开更多
Polypropylene(PP) composites that contain silver micro-particles(MILLION KILLER, denoted as Ag-Ms) and conductive carbon black(CB) have both antibacterial and antistatic properties. In the present study, the ant...Polypropylene(PP) composites that contain silver micro-particles(MILLION KILLER, denoted as Ag-Ms) and conductive carbon black(CB) have both antibacterial and antistatic properties. In the present study, the antibacterial and antistatic PP/Ag-Ms/CB composites were prepared by melt blending. The results showed that when the content was 0.8 wt%, Ag-Ms could be uniformly dispersed in the PP matrix and the mechanical properties of the composites remained stable. And the reduction percentages of Staphylococcus aureus and Escherichia coli were more than 80% which showed the good antibacterial behavior. In addition, conductive carbon black had reinforcing and toughening effects on the mechanical properties of PP/Ag-Ms/CB composites. When the content of CB was beyond 30 wt%, the surface resistance of the composite was reduced to less than 108 Ω which showed a remarkable antistatic property. According to the different filling content of conductive carbon black, it can flexibly regulate the resistivity of PP, and the conductive effect is durable and stable. We thus can produce permanent antistatic materials.展开更多
This study presents the use of chicken eggshells waste utilizing palm kernel shell based activated carbon(PKSAC) through the modification of their surface to enhance the adsorption capacity of H2S. Response surface ...This study presents the use of chicken eggshells waste utilizing palm kernel shell based activated carbon(PKSAC) through the modification of their surface to enhance the adsorption capacity of H2S. Response surface methodology technique was used to optimize the process conditions and they were found to be: 500 mg/L for H2S initial concentration, 540 min for contact time and 1 g for adsorbent mass. The impacts of three arrangement factors(calcination temperature of impregnated activated carbon(IAC), the calcium solution concentration and contact time of calcination) on the H2S removal efficiency and impregnated AC yield were investigated. Both responses IAC yield(IACY, %) and removal efficiency(RE, %) were maximized to optimize the IAC preparation conditions. The optimum preparation conditions for IACY and RE were found as follows: calcination temperature of IAC of 880 ℃, calcium solution concentration of 49.3% and calcination contact time of 57.6 min, which resulted in 35.8% of IACY and 98.2% RE. In addition, the equilibrium and kinetics of the process were investigated. The adsorbent was characterized using TGA, XRD, FTIR, SEM/EDX, and BET. The maximum monolayer adsorption capacity was found to be 543.47 mg/g. The results recommended that the composite of PKSAC and Ca O could be a useful material for H2S containing wastewater treatment.展开更多
基金The Public Science and Technology Research Funds Projects of Ocean of State Oceanic Administration People’s Republic of China under contract No.200905012a project funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions of China
文摘The global distributions of the air-sea CO2 transfer velocity and flux are retrieved from TOPEX/Poseidon and Jason altimeter data from October 1992 to December 2009 using a combined algorithm. The 17 a average global, area-weighted, Schmidt number-corrected mean gas transfer velocity is 21.26 cm/h, and the full exploration of the uncertainty of this estimate awaits further data. The average total CO2 flux (calculated by carbon) from atmosphere to ocean during the 17 a was 2.58 Pg/a. The highest transfer velocity is in the circumpolar current area, because of constant high wind speeds and currents there. This results in strong CO2 fluxes. CO2 fluxes are strong but opposite direction in the equatorial east Pacific Ocean, because the air-sea CO2 partial pressure difference is the largest in the global cceans. The results differ from the previous studies calculated using the wind speed. It is demonstrated that the air-sea transfer velocity is very important for estimating air-sea CO2 flux. It is critical to have an accurate estimation for improving calculation of CO2 flux within climate change studies.
基金supported by the National Natural Science Foundation of China(21373048,21203027,and 21371034)
文摘Periodic density functional theory calculations have been performed to investigate the chemisorption behavior of COz molecule on a series of surface alloys that are built by dispersing individual middle-late transition metal (TM) atoms (TM = Fe, Co, Ni, Ru, Rh, Pd, Ag, Os, lr, Pt, Au) on the Cu(100) and Cu(lll) surfaces. The most stable configurations of CO2 chemisorbed on different TM/Cu surfaces are determined, and the results show that among the late transition metals, Co, Ru, and Os are potentially good dopants to enhance the chemisorption and activation of CO2 on copper surfaces. To obtain a deep understanding of the adsorption property, the bonding characteristics of the adsorption bonds are carefully examined by the crystal orbital Hamilton population technique, which reveals that the TM atom primarily provides d orbitals with z-component, namely dz2, dxz, and dvz orbitals to interact with the adsorbate.
文摘In this letter ab initio electronic structure calculations are performed for extensive geometries Of CS2. A newly written program is used to fit the computed energies into the Sorbie-Murrel function, whose contour plots are illustrated.
文摘The carbon layers on implanted steel surface have been studied by means of Auger spectra. It is shown that the thickness of the carbon layer is proportional to the dose of implanted ions. By comparison with the results of friction and wear tests, the friction coefficient is smaller than 0.20 at the first part of the friction coefficient curve. It is considered that the graphitic carbon layer on the top of steel is helpful to reducing the surface friction coefficient of steel.
基金Funded by the National Young Top Talents Plan of China(2013042)the National Science Foundation of China(21676052,21606042)+1 种基金the Science Foundation for Distinguished Young Scholars of Heilongjiang Province(JC201403)the Natural Science Foundation of Heilongjiang Province(E2015034)
文摘Surface functionalization of carbon nanofibers(CNFs) was carried out, i e, CNFs were firstly oxidized and then the surface was silanized by 3-Aminopropyltriethoxysilane(APTES) via an assembly method. A new kind of high wear resistance s-CNFs/epoxy composite was fabricated by in-situ reaction. FTIR spectroscopy was used to detect the changes of the functional groups produced by silane on the surface of CNFs. The tribological properties and microstructures of modified and unmodified CNFs/epoxy composites were studied, respectively. The expremental results indicate that APTES is covalently linked to the surface of CNFs successfully and improves the dispersion of CNF in epoxy matrix. The friction coefficients and the wear rates of s-CNFs/epoxy composites are evidently lower than those of u-CNFs/epoxy composites under the same loads. Investigations also indicate that abrasive wear is the main wear mechanism for u-CNFs/epoxy composite, with slight adhesive wear for s-CNFs/epoxy composite under the same sliding wear condition.
基金financially supported by the National Program on Key Basic Research Project of China (973 Program, No. 2012CB215405)the National Natural Science Foundation of China (No. 51174022)
文摘Carbon deposition on nickel powders in methane involves three stages in different reaction temperature ranges. Temperature programing oxidation test and Raman spectrum results indicated the formation of complex and ordered carbon structures at high deposition temperatures. The values of I(D)/I(G) of the deposited carbon reached 1.86, 1.30, and 1.22 in the first, second, and third stages, respectively. The structure of carbon in the second stage was similar to that in the third stage. Carbon deposited in the first stage rarely contained homogeneous pyrolytic deposit layers. A kinetic model was developed to analyze the carbon deposition behavior in the first stage. The rate-determining step of the first stage is supposed to be interfacial reaction. Based on the investigation of carbon deposition kinetics on nickel powders from different resources, carbon deposition rate is suggested to have a linear relation with the square of specific surface area of nickel particles.
基金supported by the Natural Science Foundation of China(NSFC Grant No.20803064)the Natural Science Foundation of Zhejiang Provence(Y4090348 and LY12B03007)Qianjiang Talent Project in Zhejiang Province(2010R10039 and 2013R10056)
文摘A series of high surface area graphitic carbon materials (HSGCs) were prepared by ball-milling method. Effect of the graphitic degree of HSGCs on the catalytic performance of Ba-Ru-K/HSGC-x (x is the ball-milling time in hour) catalysts was studied using ammonia synthesis as a probe reaction. The graphitic degree and pore structure of HSGC-x supports could be successfully tuned via the variation of ball-milling time. Ru nanoparticles of different Ba-Ru-K/HSGC-x catalysts are homogeneously distributed on the supports with the particle sizes ranging from 1.6 to 2.0 nm. The graphitic degree of the support is closely related to its facile electron transfer capability and so plays an important role in improving the intrinsic catalytic performance of Ba-Ru-K/HSGC-x catalyst.
基金the financial support by the Special Fund for Basic Scientific Research of Central Colleges (No.2009KH10)the Beijing Postdoctoral Fund (No. B148)the Green Shoots Plan of Beijing Academy of Science and Technology of China (No. B142)
文摘A series of activated carbons from Taixi anthracite were prepared by steam activation in the presence of KOH and then they were modified by different methods. The regulation of porosity and the modification of surface chemistry were carried out with the aim to improve the benzene adsorption capacity of activated carbon. The influences of KOH and activation process parameters including activation temperature, activation time and steam flow rate on porosity of activated carbon were evaluated, and the effect of modification methods on surface chemistry was investigated. Also, the relationship between benzene adsorption capacity and porosity and surface chemistry was analyzed. Results show that activation temperature is the dominant factor in the activation process; the introduction of KOH into the raw material can enhance the reactivity of char in activation process, meanwhile it shows a negative effect on the porosity development, especially on the mesopore development. Results of FTIR analysis indicate that anthracite-based activated carbon with condensed aromatics and chemically inert oxygen does not present the nature to be surface modified. Besides, benzene adsorption capacity has an approximate linear relationship with surface area and in our preparation, benzene adsorption capacity and surface area of activated carbon are up to 1210 m 2 /g and 423 mg/g, respectively.
基金National Science Foundation of China(No.21173167)the Science and Technology Committee of Shaanxi Province(Grant No.2014KW09-03)+1 种基金Program for New Century Excellent Talents in University(NCET-13-0953)the Research Fund of the State Key Lab of Solidification Processing(NWPU),China(Grant No.15-BZ-2015)
文摘Facile production of high quality activated carbons from biomass materials has greatly triggered much attention presently. In this paper, a series of interconnected porous carbon materials from lotus root shells biomass are prepared via simple pyrolysis and followed by a KOH activation process. The prepared carbons exhibit high specific surface areas of up to 2961 m^2/g and large pore volume~1.47 cm3/g. In addition, the resultant porous carbons served as electrode materials in supercapacitor exhibit high specific capacitance and outstanding recycling stability and high energy density. In particular, their specific capacitance retention was almost 100% after 10500 cycles at a current density of 2 A/g. Remarkabely, the impact of the tailored specific surface areas of various carbon samples on their capacitive performances is systematically investigated.Generally, it was believed that the highly-developed porosity features(including surface areas and pore volume and pore size-distributions), together with the good conductivity of activated carbon species, play a key role in effectively improving the storage energy performances of the porous carbon electrode materials in supercapacitor.
基金the Natural Science Foundation of China(21922803,92034301,22008066,and 21776077)the China Postdoctoral Science Foundation(BX20190116)+1 种基金the Innovation Program of Shanghai Municipal Education Commission,the Program of Shanghai Academic/Tech-nology Research Leader(21XD1421000)111 Project of the Min-istry of Education of China(B08021)。
文摘Taming the electron transfer across metal–support interfaces appears to be an attractive yet challenging methodology to boost catalytic properties.Herein,we demonstrate a precise engineering strategy for the carbon surface chemistry of Pt/C catalysts—that is,for the electron-withdrawing/donating oxygencontaining groups on the carbon surface—to fine-tune the electrons of the supported metal nanoparticles.Taking the ammonia borane hydrolysis as an example,a combination of density functional theory(DFT)calculations,advanced characterizations,and kinetics and isotopic analyses reveals quantifiable relationships among the carbon surface chemistry,Pt charge state and binding energy,activation entropy/enthalpy,and resultant catalytic activity.After decoupling the influences of other factors,the Pt charge is unprecedentedly identified as an experimentally measurable descriptor of the Pt active site,contributing to a 15-fold increment in the hydrogen generation rate.Further incorporating the Pt charge with the number of Pt active sites,a mesokinetics model is proposed for the first time that can individually quantify the contributions of the electronic and geometric properties to precisely predict the catalytic performance.Our results demonstrate a potentially groundbreaking methodology to design and manipulate metal–carbon catalysts with desirable properties.
基金the Science and Technique Key Foundation of Guangdong Province(No.2003A1100101,2003C105006)
文摘A novel carbon-sulfur nano-composite material was synthesized by heating sublimed sulfur and high surface area activated carbon (HSAAC) under certain conditions. The physical and chemical per- formances of the novel carbon-sulfur nano-composite were characterized by scanning electron microscopy (SEM), Brunauer-Emmett-Teller (BET) and X-ray diffraction (XRD). The electrochemical performances of nano-composite were characterized by charge-discharge characteristic, cyclic voltammetry and electrochemical impendence spectroscopy (EIS). The experimental results indicate that the electrochemical capability of nano- composite material was superior to that of traditional S-containing composite material. The cathode made by carbon-sulfur nano-composite material shows a good cycle ability and a high specific charge-discharge capacity. The HSAAC shows a vital role in adsorbing sublimed sulfur and the polysulfides within the cathode and is an excellent electric conductor for a sulfur cathode and prevents the shuttle behavior of the lithium-sulfur battery.
基金the Institute of Particle and Science Engineering,University of Leeds and Procter & Gamble Newcastle Innovation Centre(UK) for partially funding the project
文摘Sodium carbonate and carboxymethyl cellulose powders are compressed into two-component tablets with three mass ratios,97%:3%,95%:5% and 93%:7%.The dissolution tests for two-component tablets and reference pure sodium carbonate tablets are carried out at various temperatures.The dissolution process of each tablet is measured by electrical conductivity tracking method and the concentration of dissolved sodium carbonate is quanti fied with calibrated conductivity-concentration converting equation of sodium carbonate.The quanti fied dissolution data is fitted with both surface reaction model and diffusion layer model and the results clearly show that surface reaction model is suggested as the appropriate dissolution model for all measured tablets.Therefore,it is determined that carboxymethyl cellulose is a stable element to remain the dissolution mechanism of tablet unchanged.The dissolution rate constant quanti fied with surface reaction model presents that carboxymethyl cellulose-sodium carbonate two-component tablets obtain signi ficant higher dissolution rate constant than pure sodium carbonate tablet and higher proportion of carboxymethyl cellulose leads to apparent higher dissolution rate constant.The results prove for the usage of carboxymethyl cellulose in most practical applications at a relative low-level,the effect of carboxymethyl cellulose is effective and positive for two-component tablet to enhance the dissolution process and improve dissolution rate constant and this effect is speculated coming from its dynamic physical transforming process in water including dilation and conglutination.
文摘Different oxygen and nitrogen containing functional groups were created on the surface of the multiwalled carbon nanotubes. The multi-walled carbon nanotubes were treated in ultrasonic bath with sulfuric or nitric acid. Furthermore the surface texture was modified by increase of the roughness. In particular after treatment with the oxidizing nitric acid, in comparison to the H2SO4 or ultra-sonic treated samples,craters and edges are dominating the surface structures. Manganese oxide was deposited on the multiwalled carbon nanotubes by precipitation mechanism. Various manganese oxides are formed during the deposition process. The samples were characterized by elemental analysis, microscopy, thermal analysis,Raman spectroscopy, and by the zeta potential as well as X-ray diffraction measurements. It was shown that the deposited manganese oxides are stabilized rather by surface texture of the multi-walled carbon nanotubes than by created functional groups.
基金supported by the Spanish Ministry of Economy and Competitiveness (Project CTQ2012-37925-C03-03)FEDER fundsby the Hungarian National Fund OTKA K109558
文摘Composites of carbon aerogel and graphite oxide(GO) were synthesized using a self-assembly method based on dispersive forces. Their surface was modified by treatment in hydrogen sulfide at 650 and800 ℃. The samples obtained were characterized by adsorption of nitrogen, TA-MS, XPS, potentiometric titration, and HRTEM and tested as catalysts for oxygen reduction reactions(ORR) in an alkaline medium.The synergistic effect of the composite(electrical conductivity, porosity and surface chemistry) leads to a good ORR catalytic activity. The onset potential for the composite of carbon aerogel heated at 800 ℃ is shifted to a more positive value and the number of electron transfer was 2e-at the potential 0.68 V versus RHE and it increased to 4e-with an increase in the negative values of the potential. An excellent tolerance to methanol crossover was also recorded.
基金The National Basic Research Program of China (973 Program) (No. 2005CB221402)China National Petroleum Corporation
文摘The purpose of this study was to investigate the effect of preadsorbed CO at different temperatures, calcination temperatures, the combined influence of reduction temperature and time, and pretreatment using hydrogen or syngas as reduction agents on the F-T synthesis (FTS) activity and selectivity of Co/Al2O3 catalyst. The reactivity of the carbon species at higher preadsorption temperature with H2 in TPSR decreased, whereas the carbon-containing species showed higher reactivity over Co/Al2O3 catalyst with low calcination temperature. This agreed well with the order of catalytic activity for F-T synthesis on this catalyst. The catalytic activity of the catalyst varied with reduction temperature and time remarkably. CODEX optimization gave an optimum reduction temperature of 756 K and reduction time of 6.2 h and estimated C5+ yield perfectly. The pretreatment of Co/Al2O3 catalyst with different reduction agents (hydrogen or syngas) showed important influences on the catalytic performance. A high CO conversion and C5+ yield were obtained on the catalyst reduced by hydrogen, whereas methane selectivity on the catalyst reduced by syngas was much higher than that on the catalyst reduced by hydrogen.
基金Funded by the Interdisciplinary Program of Shanghai Jiao Tong University(YG2016MS24)
文摘Silver coatings on the exterior surface of monolithic activated carbon(MAC) with different morphology were prepared by directly immersing MAC into [Ag(NH3)2]NO3 solution. Acid and base treatments were employed to modify the surface oxygenic groups of MAC, respectively. The MACs' Brunauer-EmmettTeller(BET) surface area, surface groups, and silver coating morphology were characterized by N2 adsorption, elemental analysis(EA), X-ray photoelectron spectroscopy(XPS), and scanning electron microscopy(SEM), respectively. The coating morphology was found to be closely related to the surface area and surface functional groups of MAC. For a raw MAC which contained a variety of oxygenic groups, HNO3 treatment enhanced the relative amount of highly oxidized groups such as carboxyl and carbonates, which disfavored the deposition of silver particles. By contrast, Na OH treatment significantly improved the amount of carbonyl groups, which in turn improved the deposition amount of silver. Importantly, lamella silver was produced on raw MAC while Na OH treatment resulted in granular particles because of the capping effect of carbonyl groups. At appropriate [Ag(NH3)2]NO3 concentrations, silver nanoparticles smaller than 100 nm were homogeneously dispersed on Na OH-treated MAC. The successful tuning of the size and morphology of silver coatings on MAC is promising for novel applications in air purification and for antibacterial or aesthetic purposes.
文摘Carbon-sulfur nano-composite cathodes for lithium rechargeable batteries were investigated by electrochemical impedance spectroscopy (EIS). The novel carbon-sulfur nano-composite material was synthesized by heating sublimed sulfur and high surface area activated carbon (HSAAC) in certain conditions. Equivalent circuits were used to fit the spectra at different discharge states. The variations of impedance spectra, charge-transfer resistance and double layer capacitance were discussed. The changes of EIS with potential were analyzed based on a plausible electrical equivalent circuit model, and some parameters were measured and analyzed about electrochemical performance and state of charge and discharge of the electrode. The good accuracy in fitting values of the model to the experimental data indicates that the mathematical model gives out a satisfying description upon the mechanism of high rate of capacity fade in lithium-sulfur battery.
基金Funded by National Natural Science Funds of China(No.51173141)Natural Science Funds of Hubei Province,China(No.2014CFC1152)+1 种基金Science and Technology Research Program of Department of Education of Hubei Province,China(No.Q20122305)Funds of Hubei Key Laboratory of Automotive Power Train and Electronic Control(No.ZDK1201405)
文摘Polypropylene(PP) composites that contain silver micro-particles(MILLION KILLER, denoted as Ag-Ms) and conductive carbon black(CB) have both antibacterial and antistatic properties. In the present study, the antibacterial and antistatic PP/Ag-Ms/CB composites were prepared by melt blending. The results showed that when the content was 0.8 wt%, Ag-Ms could be uniformly dispersed in the PP matrix and the mechanical properties of the composites remained stable. And the reduction percentages of Staphylococcus aureus and Escherichia coli were more than 80% which showed the good antibacterial behavior. In addition, conductive carbon black had reinforcing and toughening effects on the mechanical properties of PP/Ag-Ms/CB composites. When the content of CB was beyond 30 wt%, the surface resistance of the composite was reduced to less than 108 Ω which showed a remarkable antistatic property. According to the different filling content of conductive carbon black, it can flexibly regulate the resistivity of PP, and the conductive effect is durable and stable. We thus can produce permanent antistatic materials.
基金Funded by the Faculty of Chemical&Natural Resources Engineering,Universiti Malaysia Pahang through a Local Research Grant Scheme
文摘This study presents the use of chicken eggshells waste utilizing palm kernel shell based activated carbon(PKSAC) through the modification of their surface to enhance the adsorption capacity of H2S. Response surface methodology technique was used to optimize the process conditions and they were found to be: 500 mg/L for H2S initial concentration, 540 min for contact time and 1 g for adsorbent mass. The impacts of three arrangement factors(calcination temperature of impregnated activated carbon(IAC), the calcium solution concentration and contact time of calcination) on the H2S removal efficiency and impregnated AC yield were investigated. Both responses IAC yield(IACY, %) and removal efficiency(RE, %) were maximized to optimize the IAC preparation conditions. The optimum preparation conditions for IACY and RE were found as follows: calcination temperature of IAC of 880 ℃, calcium solution concentration of 49.3% and calcination contact time of 57.6 min, which resulted in 35.8% of IACY and 98.2% RE. In addition, the equilibrium and kinetics of the process were investigated. The adsorbent was characterized using TGA, XRD, FTIR, SEM/EDX, and BET. The maximum monolayer adsorption capacity was found to be 543.47 mg/g. The results recommended that the composite of PKSAC and Ca O could be a useful material for H2S containing wastewater treatment.