The porous cubic yttrium oxides with high specific surface area were prepared yttrium nitrate and its complex formed with methyl salicylate. The specific surface area by the explosive decomposition of and properties o...The porous cubic yttrium oxides with high specific surface area were prepared yttrium nitrate and its complex formed with methyl salicylate. The specific surface area by the explosive decomposition of and properties of powders synthesized at various temperatures were characterized using BET, X-ray diffraction （XRD）, infrared spectra （IR）, and scanning electron microscopy （SEM）. The results indicate that the highest specific surface area is found to be 65.37 m^2·g^-1 at the calcination temperature of 600 ℃, and then decreases to 20.33 m2· g^- 1 with the calcination temperature rising from 600 to 900 ℃. The powders show strong surface activity for adsorping water and carbon dioxide in air, which also decreases with the rising calcination temperature. The drop both on the surface area and surface activity of samples at higher temperatures may be due to pore-narrowing（sintering） effects.展开更多
Zirconia-ceria mixed oxide powders were prepared by high temperature aging method.The effects of the temperature and the time of aging, cerium content and calcination on powder performance were studied.The result show...Zirconia-ceria mixed oxide powders were prepared by high temperature aging method.The effects of the temperature and the time of aging, cerium content and calcination on powder performance were studied.The result shows that high temperature aging is an efficient way of preparation of ZrO2-CeO2 mixed oxide powders with high specific surface area and good thermal stability, and that addition of a small amount of cerium to hydrous zirconia can promote the preparation of high specific surface area powders.展开更多
The electrochemical reduction of CO2(CO2 RR) can substantially contribute to the production of useful chemicals and reduction of global CO2 emissions. Herein, we presented N and S dual-doped high-surface-area carbon m...The electrochemical reduction of CO2(CO2 RR) can substantially contribute to the production of useful chemicals and reduction of global CO2 emissions. Herein, we presented N and S dual-doped high-surface-area carbon materials(SZ-HCN) as CO2 RR catalysts. N and S were doped by one-step pyrolysis of a N-containing polymer and S powder. ZnCl2 was applied as a volatile porogen to prepare porous SZ-HCN. SZ-HCN with a high specific surface area(1510 m2 g–1) exhibited efficient electrocatalytic activity and selectivity for CO2 RR. Electrochemical measurements demonstrated that SZ-HCN showed excellent catalytic performance for CO2-to-CO reduction with a high CO Faradaic efficiency(~93%) at-0.6 V. Furthermore, SZ-HCN offered a stable current density and high CO selectivity over at least 20 h continuous operation, revealing remarkable electrocatalytic durability. The experimental results and density functional theory calculations indicated that N and S dual-doped carbon materials required lower Gibbs free energy to form the COOH* intermediate than that for single-N-doped carbon for CO2-to-CO reduction, thereby enhancing CO2 RR activity.展开更多
Silica gels with a high specific surface area and high adsorption activity ,which have high selectivity and high adsorption capacity for zirconium in acidic high level radioactive liquid waste (HLLW), have been prepar...Silica gels with a high specific surface area and high adsorption activity ,which have high selectivity and high adsorption capacity for zirconium in acidic high level radioactive liquid waste (HLLW), have been prepared from water-glass and hydrochloric acid through adding surfactants. The surfactant modifies the surface of the primary sol particles, thus suppresses the growth of the primary particle,but accelerates their agglomeration. The action of the surfactant is similar to that of the organic structure-directing agent and makes the sol cluster cross-linkage ring-like network in short order. The specific surface area of the silica gel is 998 m 2/g; the static adsorption capacity and the adsorption distribution coefficient for zirconium in HLLW are 32.6 mg/g and 56.1 mL/g, respectively.展开更多
Potassium-ion hybrid capacitors(PIHCs)are widely regarded as highly promising energy storage devices,due to their exceptional energy density,impressive power density,and abundant potassium resources.Unfortunately,rest...Potassium-ion hybrid capacitors(PIHCs)are widely regarded as highly promising energy storage devices,due to their exceptional energy density,impressive power density,and abundant potassium resources.Unfortunately,restricted by the inherent capacitive storage mechanism,the carbon cathodes possess a much lower specific capacity than battery-type anodes.Therefore,designing high-performance carbon cathodes is extremely urgent for the development of PIHCs.Herein,N,O codoped porous carbon(NOPC)was fabricated through the NaCl hard template method and combined KOH/melamine chemical activation technique,displaying the characteristics of abundant N/O content(4.7 at%/16.9 at%),ultrahigh specific surface area(3092 m^(2)g^(-1))and hierarchical pore network.The designed NOPC cathode delivers a high specific capacity(164.4 mAh.g^(-1)at 0.05 A.g^(-1))and superior cyclability(95.1%retention ratio at 2 A·g^(-1)over 2500 cycles).Notably,the adjustable ratio of micropores to mesopores facilitates the achievement of the optimal bal-ance between capacity and rate capability.Moreover,the pseudocapacitance can be further augmented through the incorporation of N/O functional groups.As expected,the graphite//NOPC based PIHC possesses a high energy density of 113 Wh·kg-at 747 W·kg^(-1)and excellent capacity retention of 84.4% fter 400 cycles at 1.0 A·g^(-1).This work introduces a novel strategy for designing carbon cathodes that enhances the electrochemical performance of PIHCs.展开更多
In this work,a facile"carbonization-activation"strategy is developed to synthesize N,P-codoped hierarchical porous carbon.Phosphoric acid is innovatively introduced during the hydrothermal process to achieve...In this work,a facile"carbonization-activation"strategy is developed to synthesize N,P-codoped hierarchical porous carbon.Phosphoric acid is innovatively introduced during the hydrothermal process to achieve in-situ P doping as well as create abundant pores,and the employment of sodamide is of vital importance to simultaneously serve as activating agent and N-source to succeed a high-level N doping.Thus,the obtained samples exhibit a unique three-dimensional hierarchical structure with an ultra-high specific surface area(3646 m^(2)g^(-1))and ultra-high N-doping level(9.81 at.%).Computational analyses confirm that N,P co-doping and higher N content can enhance active sites and widen potential differences of carbon materials to improve their capacitance.The as-prepared carbon materials demonstrate superior electrochemical performances,such as an ultra-high capacitance of 586 Fg^(-1)at 1 Ag^(-1),a superior rate capability of 409 Fg^(-1)at 20 Ag^(-1),and excellent long-term stability of 97%capacitance retention after10,000 cycles in 6 M KOH.Moreover,an assembled symmetric supercapacitor delivers a high energy density of 28.1 Wh kg^(-1)at the power density of 450 W kg^(-1)in 1 M Na_(2)SO_(4),demonstrating a great potential for applications in supercapacitors.展开更多
Orderly mesoporous CuFe2O4spinel-type mixed oxide with high specific surface area was prepared successfully by a hard-template method in which KIT-6mesoporous silica was selected as the hard template.The KIT-6 hard te...Orderly mesoporous CuFe2O4spinel-type mixed oxide with high specific surface area was prepared successfully by a hard-template method in which KIT-6mesoporous silica was selected as the hard template.The KIT-6 hard template and CuFe2O4samples were characterized by X-ray diffraction,X-ray photoelectron spectroscopy,X-ray fluorescence,transmission electron microscopy,scanning electron microscopy,nitrogen physisorption,and hydrogen-temperature programmed reduction.The KIT-6 hard template had perfect crystallization and ordered mesoporous structure with a probable pore distribution of about 9.1 nm,large enough to be filled by the spinel precursor.The mesoporous CuFe2O4spinel oxide synthesized inside the KIT-6 mesopores had a relatively small pore size(4.3 nm),orderly arrangement,and high specific area(194 m2/g).The catalytic activity of the mesoporous CuFe2O4was tested for the selective oxidation of ammonia to nitrogen.The conversion of ammonia reached nearly 100%at 300°C with a nitrogen selectivity as high as 96%.The nitrogen selectivity remained high with increasing temperature and even maintained a value of80%at 600°C.展开更多
Silica aerogels were prepared at ambient drying by using ethanol/trimethylchlorosilane （TMCS）/heptane solution as pore water exchange and surface modification of the wet gel before drying. The obtained silica aeroge...Silica aerogels were prepared at ambient drying by using ethanol/trimethylchlorosilane （TMCS）/heptane solution as pore water exchange and surface modification of the wet gel before drying. The obtained silica aerogels exhibit a sponge-like structure with uniform pore size distribution. The effects of heat-treatment on the hydrophobicity, specific surface area and other properties were investigated. The results indicated that the hydrophobicity of silica aerogels could be maintained up to 350℃. With increasing heating temperature, hydrophobicity decreased, and became completely hydrophilic after heat-treatment at 500℃. Brunaueremmitt-teller （BET） surface area results indicated that the specific surface area of silica aerogels increased with increasing heating temperature in the range of 150-500℃. The effects of heat-treatment on the morphology and chemical bonding state of silica aerogels were investigated by scanning electron microscopy （SEM）, differential temperature analysis （DTA） and Fourier-transform infrared spectroscopy （FT-IR）.展开更多
The mechanism of high pressure roll grinding on improvement of compression strength of oxidized hematite pellets was researched by considering their roasting properties. The results indicate that oxidized hematite pel...The mechanism of high pressure roll grinding on improvement of compression strength of oxidized hematite pellets was researched by considering their roasting properties. The results indicate that oxidized hematite pellets require higher preheating temperature and longer preheating time to attain required compression strength of pellets compared with the common magnetite oxidized pellets. It is found that when the hematite concentrates are pretreated by high pressure roll grinding （HPRG）, the compression strengths of preheated and roasted oxidized hematite pellets get improved even with lower preheating and roasting temperatures and shorter preheating and roasting time. The mechanism for HPRG to improve roasting properties of oxidized pellets were investigated and the cause mainly lies in the increase of micro-sized particles and the decrease of dispersion degree for hematite concentrates, which promotes the hematite concentrate particles to be compacted, the solid-phase crystallization, and finally the formation of Fe203 bonding bridges during subsequent high temperature roasting process.展开更多
文摘The porous cubic yttrium oxides with high specific surface area were prepared yttrium nitrate and its complex formed with methyl salicylate. The specific surface area by the explosive decomposition of and properties of powders synthesized at various temperatures were characterized using BET, X-ray diffraction （XRD）, infrared spectra （IR）, and scanning electron microscopy （SEM）. The results indicate that the highest specific surface area is found to be 65.37 m^2·g^-1 at the calcination temperature of 600 ℃, and then decreases to 20.33 m2· g^- 1 with the calcination temperature rising from 600 to 900 ℃. The powders show strong surface activity for adsorping water and carbon dioxide in air, which also decreases with the rising calcination temperature. The drop both on the surface area and surface activity of samples at higher temperatures may be due to pore-narrowing（sintering） effects.
文摘Zirconia-ceria mixed oxide powders were prepared by high temperature aging method.The effects of the temperature and the time of aging, cerium content and calcination on powder performance were studied.The result shows that high temperature aging is an efficient way of preparation of ZrO2-CeO2 mixed oxide powders with high specific surface area and good thermal stability, and that addition of a small amount of cerium to hydrous zirconia can promote the preparation of high specific surface area powders.
文摘The electrochemical reduction of CO2(CO2 RR) can substantially contribute to the production of useful chemicals and reduction of global CO2 emissions. Herein, we presented N and S dual-doped high-surface-area carbon materials(SZ-HCN) as CO2 RR catalysts. N and S were doped by one-step pyrolysis of a N-containing polymer and S powder. ZnCl2 was applied as a volatile porogen to prepare porous SZ-HCN. SZ-HCN with a high specific surface area(1510 m2 g–1) exhibited efficient electrocatalytic activity and selectivity for CO2 RR. Electrochemical measurements demonstrated that SZ-HCN showed excellent catalytic performance for CO2-to-CO reduction with a high CO Faradaic efficiency(~93%) at-0.6 V. Furthermore, SZ-HCN offered a stable current density and high CO selectivity over at least 20 h continuous operation, revealing remarkable electrocatalytic durability. The experimental results and density functional theory calculations indicated that N and S dual-doped carbon materials required lower Gibbs free energy to form the COOH* intermediate than that for single-N-doped carbon for CO2-to-CO reduction, thereby enhancing CO2 RR activity.
文摘Silica gels with a high specific surface area and high adsorption activity ,which have high selectivity and high adsorption capacity for zirconium in acidic high level radioactive liquid waste (HLLW), have been prepared from water-glass and hydrochloric acid through adding surfactants. The surfactant modifies the surface of the primary sol particles, thus suppresses the growth of the primary particle,but accelerates their agglomeration. The action of the surfactant is similar to that of the organic structure-directing agent and makes the sol cluster cross-linkage ring-like network in short order. The specific surface area of the silica gel is 998 m 2/g; the static adsorption capacity and the adsorption distribution coefficient for zirconium in HLLW are 32.6 mg/g and 56.1 mL/g, respectively.
基金financially supported by the National Natural Science Foundation of China(Nos.22179123 and52002138)Taishan Scholar Program of Shandong Province+1 种基金China(No.tsqn202211048)the Fundamental Research Funds for the Central Universities(Nos.202262010 and 862201013190)。
文摘Potassium-ion hybrid capacitors(PIHCs)are widely regarded as highly promising energy storage devices,due to their exceptional energy density,impressive power density,and abundant potassium resources.Unfortunately,restricted by the inherent capacitive storage mechanism,the carbon cathodes possess a much lower specific capacity than battery-type anodes.Therefore,designing high-performance carbon cathodes is extremely urgent for the development of PIHCs.Herein,N,O codoped porous carbon(NOPC)was fabricated through the NaCl hard template method and combined KOH/melamine chemical activation technique,displaying the characteristics of abundant N/O content(4.7 at%/16.9 at%),ultrahigh specific surface area(3092 m^(2)g^(-1))and hierarchical pore network.The designed NOPC cathode delivers a high specific capacity(164.4 mAh.g^(-1)at 0.05 A.g^(-1))and superior cyclability(95.1%retention ratio at 2 A·g^(-1)over 2500 cycles).Notably,the adjustable ratio of micropores to mesopores facilitates the achievement of the optimal bal-ance between capacity and rate capability.Moreover,the pseudocapacitance can be further augmented through the incorporation of N/O functional groups.As expected,the graphite//NOPC based PIHC possesses a high energy density of 113 Wh·kg-at 747 W·kg^(-1)and excellent capacity retention of 84.4% fter 400 cycles at 1.0 A·g^(-1).This work introduces a novel strategy for designing carbon cathodes that enhances the electrochemical performance of PIHCs.
基金financially supported by the National Natural Science Foundation of China(Nos.21776147,21606140,61604086,and 21905153)the Qingdao Municipal Science and Technology Bureau,China(19-6-1-91-nsh)+2 种基金the International Science&Technology Cooperation Program of China(No.2014DFA60150)the Department of Science and Technology of Shandong Province(Nos.ZR2018BB066 and 2016GGX104010)the Chemcloudcomputing of National Supercomputing Center in Shenzhen(Shenzhen CloudComputing Center)。
文摘In this work,a facile"carbonization-activation"strategy is developed to synthesize N,P-codoped hierarchical porous carbon.Phosphoric acid is innovatively introduced during the hydrothermal process to achieve in-situ P doping as well as create abundant pores,and the employment of sodamide is of vital importance to simultaneously serve as activating agent and N-source to succeed a high-level N doping.Thus,the obtained samples exhibit a unique three-dimensional hierarchical structure with an ultra-high specific surface area(3646 m^(2)g^(-1))and ultra-high N-doping level(9.81 at.%).Computational analyses confirm that N,P co-doping and higher N content can enhance active sites and widen potential differences of carbon materials to improve their capacitance.The as-prepared carbon materials demonstrate superior electrochemical performances,such as an ultra-high capacitance of 586 Fg^(-1)at 1 Ag^(-1),a superior rate capability of 409 Fg^(-1)at 20 Ag^(-1),and excellent long-term stability of 97%capacitance retention after10,000 cycles in 6 M KOH.Moreover,an assembled symmetric supercapacitor delivers a high energy density of 28.1 Wh kg^(-1)at the power density of 450 W kg^(-1)in 1 M Na_(2)SO_(4),demonstrating a great potential for applications in supercapacitors.
基金supported by the National High Technology Research and Development Program of China (2013AA065900)the National Natural Science Foundation of China (21177008,21121064)
文摘Orderly mesoporous CuFe2O4spinel-type mixed oxide with high specific surface area was prepared successfully by a hard-template method in which KIT-6mesoporous silica was selected as the hard template.The KIT-6 hard template and CuFe2O4samples were characterized by X-ray diffraction,X-ray photoelectron spectroscopy,X-ray fluorescence,transmission electron microscopy,scanning electron microscopy,nitrogen physisorption,and hydrogen-temperature programmed reduction.The KIT-6 hard template had perfect crystallization and ordered mesoporous structure with a probable pore distribution of about 9.1 nm,large enough to be filled by the spinel precursor.The mesoporous CuFe2O4spinel oxide synthesized inside the KIT-6 mesopores had a relatively small pore size(4.3 nm),orderly arrangement,and high specific area(194 m2/g).The catalytic activity of the mesoporous CuFe2O4was tested for the selective oxidation of ammonia to nitrogen.The conversion of ammonia reached nearly 100%at 300°C with a nitrogen selectivity as high as 96%.The nitrogen selectivity remained high with increasing temperature and even maintained a value of80%at 600°C.
文摘Silica aerogels were prepared at ambient drying by using ethanol/trimethylchlorosilane （TMCS）/heptane solution as pore water exchange and surface modification of the wet gel before drying. The obtained silica aerogels exhibit a sponge-like structure with uniform pore size distribution. The effects of heat-treatment on the hydrophobicity, specific surface area and other properties were investigated. The results indicated that the hydrophobicity of silica aerogels could be maintained up to 350℃. With increasing heating temperature, hydrophobicity decreased, and became completely hydrophilic after heat-treatment at 500℃. Brunaueremmitt-teller （BET） surface area results indicated that the specific surface area of silica aerogels increased with increasing heating temperature in the range of 150-500℃. The effects of heat-treatment on the morphology and chemical bonding state of silica aerogels were investigated by scanning electron microscopy （SEM）, differential temperature analysis （DTA） and Fourier-transform infrared spectroscopy （FT-IR）.
基金Project(50725416) supported by the National Natural Science Funds for Distinguished Young Scholars of China
文摘The mechanism of high pressure roll grinding on improvement of compression strength of oxidized hematite pellets was researched by considering their roasting properties. The results indicate that oxidized hematite pellets require higher preheating temperature and longer preheating time to attain required compression strength of pellets compared with the common magnetite oxidized pellets. It is found that when the hematite concentrates are pretreated by high pressure roll grinding （HPRG）, the compression strengths of preheated and roasted oxidized hematite pellets get improved even with lower preheating and roasting temperatures and shorter preheating and roasting time. The mechanism for HPRG to improve roasting properties of oxidized pellets were investigated and the cause mainly lies in the increase of micro-sized particles and the decrease of dispersion degree for hematite concentrates, which promotes the hematite concentrate particles to be compacted, the solid-phase crystallization, and finally the formation of Fe203 bonding bridges during subsequent high temperature roasting process.
