From June 2008 to August 2013,approximately 67 kt of CO_(2) was injected into a deep saline formation at the Ketzin pilot CO_(2) storage site.During injection,3D seismic surveys have been performed to monitor the migr...From June 2008 to August 2013,approximately 67 kt of CO_(2) was injected into a deep saline formation at the Ketzin pilot CO_(2) storage site.During injection,3D seismic surveys have been performed to monitor the migration of sequestered CO_(2).Seismic monitoring results are limited by the acquisition and signal-to-noise ratio of the acquired data.The multiphysical reservoir simulation provides information regarding the CO_(2) fluid behavior,and the approximated model should be calibrated with the monitoring results.In this work,property models are delivered from the multiphysical model during 3D repeated seismic surveys.The simulated seismic data based on the models are compared with the real data,and the results validate the effectiveness of the multiphysical inversion method.Time-lapse analysis shows the trend of CO_(2) migration during and after injection.展开更多
Considering that copper mine tailings(CMTs)are commonly mixed with ordinary Portland cement,fly ash(FA),and kaolin to produce geopolymers,to make full use of CMTs,the properties of geopolymers manufactured under diffe...Considering that copper mine tailings(CMTs)are commonly mixed with ordinary Portland cement,fly ash(FA),and kaolin to produce geopolymers,to make full use of CMTs,the properties of geopolymers manufactured under different material mass ratios and curing methods(standard curing,water bath curing,and 60℃curing)are evaluated with significantly increased dosage of CMTs.Porosity and unconfined compressive strength tests,X-ray diffraction,field emission scanning electron microscopy,and energy dispersive spectroscopy are used to determine the physical and mechanical properties,microstructure,and mineral composition of geopolymers.Finally,costs and CO 2 emissions of specimens with different material mass ratios during the preparation processes are compared.The results show that during the geopolymerization of low-calcium materials,various geopolymer gels,including calcium silicate,calcium silicoaluminate,and mainly sodium silicoaluminate gels,coexist.The solid waste,cost,and carbon dioxide emission reductions can reach 100%,166.3 yuan/t,and 73.3 kg/t,respectively.Under a curing condition of 60℃,the sample with a CMTs mass fraction of 70%and an FA mass fraction of 30%meets the requirements of porosity,compressive strength.The resource utilization of CMT and FA is realized in a more economical way.展开更多
Two major challenges,high cost and short lifespan,have been hindering the commercialization process of lowtemperature fuel cells.Professor Wei's group has been focusing on decreasing cathode Pt loadings without lo...Two major challenges,high cost and short lifespan,have been hindering the commercialization process of lowtemperature fuel cells.Professor Wei's group has been focusing on decreasing cathode Pt loadings without losses of activity and durability,and their research advances in this area over the past three decades are briefly reviewed herein.Regarding the Pt-based catalysts and the low Pt usage,they have firstly tried to clarify the degradation mechanism of Pt/C catalysts,and then demonstrated that the activity and stability could be improved by three strategies:regulating the nanostructures of the active sites,enhancing the effects of support materials,and optimizing structures of the three-phase boundary.For Pt-free catalysts,especialiy carbon-based ones,several strategies that they proposed to enhance the activity of nitrogen-/heteroatom-doped carbon catalysts are firstly presented.Then,an indepth understanding of the degradation mechanism for carbon-based catalysts is discussed,and followed by the corresponding stability enhancement strategies.Also,the carbon-based electrode at the micrometer-scale,faces the challenges such as low active-site density,thick catalytic layer,and the effect of hydrogen peroxide,which require rational structure design for the integral cathodic electrode.This review finally gives a brief conclusion and outlook about the low cost and long lifespan of cathodic oxygen reduction catalysts.展开更多
Graphene oxide(GO)with excellent dispersion ability can assist the dispersion of single-walled carbon nanotube(SWCNT)and promote the formation of uniform and stable GO/SWCNT coating liquid.The highly conductive polyet...Graphene oxide(GO)with excellent dispersion ability can assist the dispersion of single-walled carbon nanotube(SWCNT)and promote the formation of uniform and stable GO/SWCNT coating liquid.The highly conductive polyethylene terephthalate/reduced graphene oxide/SWCNT(PET/rGO/SWCNT)electromagnetic shielding composite fabric was successfully prepared by anchoring rGO/SWCNT on PET fabric via dip-coating piror to low-temperature thermal reduction.The results showed that the carboxyl groups and hydroxyl groups formed of hydrophilic-treated PET were conducive to the formation of hydrogen bonds with that of GO,which enhanced the interaction between PET fabric and GO/SWCNT coating;the loading of GO/SWCNT increased with the number of dip-coating,the unit area loading of rGO/SWCNT in the final composite fabric was 2.7 mg/cm^(2) after 10 dip-coating cycles and thermal reduction;the PET/rGO/SWCNT composite fabric had a continuous and dense conductive network,with a conductivity of up to 41.6 S/m and the average electromagnetic interference shielding effectiveness in X-band was 22 dB;the flexible PET/rGO/SWCNT composite fabric was not only easy to process,but also exhibited excellent conductivity and shielding efficiency,showing great potential in the application of electromagnetic shielding fabrics.展开更多
The aim of "green chemistry" and "atom economy" is to utilize carbon dioxide and replace harmful reactants such as CO and phosgene for the production of cyclic carbonates. In this paper, metal-free catalysts inclu...The aim of "green chemistry" and "atom economy" is to utilize carbon dioxide and replace harmful reactants such as CO and phosgene for the production of cyclic carbonates. In this paper, metal-free catalysts including organic bases, ionic liquids, supported catalysts, organic copolymers and carbon materials for the synthesis of cyclic carbonates by the cycloaddition of carbon dioxide to epoxides are reviewed. Recent advances in the design of the catalysts and the understanding of the reaction mechanism are summarized and discussed. The synergistic effects of organic bases and hydrogen bond donors, organic bases and nucleophilic anions, hydrogen bond donors and nucleophilic anions and active components and supports are highlighted. The challenge is to develop metal-free catalysts suitable for carbon dioxide capture and fixation. The ultimate goal is to synthesize cyclic carbonates in a flow reactor directly using carbon dioxide from industrial flue gas at ambient temperature and atmospheric pressure. By using synergetic effects, a multi-functional approach can meet the design strategy of metal-free catalysts for carbon dioxide adsorption and activation as well as epoxide ring opening.展开更多
Low‐temperature CO oxidation is important for both fundamental studies and practical applica‐tions. Supported gold catalysts are generally regarded as the most active catalysts for low‐temperature CO oxidation. The...Low‐temperature CO oxidation is important for both fundamental studies and practical applica‐tions. Supported gold catalysts are generally regarded as the most active catalysts for low‐temperature CO oxidation. The active sites are traditionally believed to be Au nanoclusters or nanoparticles in the size range of 0.5–5 nm. Only in the last few years have single‐atom Au catalysts been proved to be active for CO oxidation. Recent advances in both experimental and theoretical studies on single‐atom Au catalysts unambiguously demonstrated that when dispersed on suitable oxide supports the Au single atoms can be extremely active for CO oxidation. In this mini‐review, recent advances in the development of Au single‐atom catalysts are discussed, with the aim of illus‐trating their unique catalytic features during CO oxidation.展开更多
The preparation of fine TiC powders by carbothermal reduction of TiO2 in vacuum was investigated by XRD,SEM,XRF and laser particle sizer.Thermodynamic analysis indicates that it is easy to prepare TiC in vacuum and th...The preparation of fine TiC powders by carbothermal reduction of TiO2 in vacuum was investigated by XRD,SEM,XRF and laser particle sizer.Thermodynamic analysis indicates that it is easy to prepare TiC in vacuum and the formation sequence of products are Ti4O7(Magneli phase),Ti3O5,Ti2O3,TiCxO1-x and TiC with the increase of reaction temperature.Experimental results demonstrate that TiC powders with single phase are obtained with molar ratio of TiO2 to C ranging from 1:3.2 to 1:6 at 1 550 ℃ for 4 h when the system pressure is 50 Pa,and TiC1.0 is gained when the molar ratio of TiO2 to C is 1:4 and 1:5.In addition,fine TiC1.0 powders(D50 equals 3.04 μm) with single phase and low impurities are obtained when the molar ratio of TiO2 to C is 1:4.SEM observation shows that uniform shape,low agglomeration,and loose structure are observed on the surface of block product.展开更多
CO oxidation is probably the most studied reaction in heterogeneous catalysis.This reaction has become a hot topic with the discovery of nanogold catalysts,which are active at low temperatures(at or below room temper...CO oxidation is probably the most studied reaction in heterogeneous catalysis.This reaction has become a hot topic with the discovery of nanogold catalysts,which are active at low temperatures(at or below room temperature).Au catalysts are the benchmark for judging the activities of other metals in CO oxidation.Pt-group metals(PGMs) that give comparable performances are of particular interest.In this mini-review,we summarize the advances in various PGM(Pt,Pd,Ir,Rh,Ru)catalysts that have high catalytic activities in low-temperature CO oxidation arising from reducible supports or the presence of OH species.The effects of the size of the metal species and the importance of the interface between the metal and the reducible support are covered and discussed in terms of their promotional role in CO oxidation at low temperatures.展开更多
The structure and catalytic desulfurization characteristics of CeO2-TiO2 mixed oxides were investigated by means ofX-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and catalytic activity tests. Acco...The structure and catalytic desulfurization characteristics of CeO2-TiO2 mixed oxides were investigated by means ofX-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and catalytic activity tests. According to the results, a CeO2-TiO2solid solution is formed when the mole ratio of cerium to titanium n(Ce):n(Ti) is 5:5 or greater, and the most suitable n(Ce):n(Ti) isdetermined as 7:3, over which the conversion rate of SO2 and the yield of sulfur at 500℃ reach 93% and 99%, respectively.According to the activity testing curve, Ce0.7Ti0.3O2 (n(Ce):n(Ti)=7:3) without any pretreatment can be gradually activated by reagentgas after about 10 min, and reaches a steady activation status 60 min later. The XPS results of Ce0.7Ti0.3O2 after different time ofSO2+CO reaction show that CeO2 is the active component that offers the redox couple Ce4+/Ce3+ and the labile oxygen vacancies, andTiO2 only functions as a catalyst structure stabilizer during the catalytic reaction process. After 48 h of catalytic reaction at 500℃,Ce0.7Ti0.3O2 still maintains a stable structure without being vulcanized, demonstrating its good anti-sulfur poisoning performance.展开更多
Allelochemicals of Chinese-fir root was extracted by technology ofsupercritical CO_2 extraction under orthogonal experiment design, and it was used to analyzeallelopathic activity of Chinese-fir through bioassay of se...Allelochemicals of Chinese-fir root was extracted by technology ofsupercritical CO_2 extraction under orthogonal experiment design, and it was used to analyzeallelopathic activity of Chinese-fir through bioassay of seed germination. The results showed thatas to the available rate of allelochemicals, the pressure and temperature of extraction were themost important factors. The allelochemicals of Chinese-fir root extracted by pure CO_2 and ethanolmixed with CO_2 have different allelopathic activities to seed germination, and the allelochemicalsextracted by ethanol mixed with CO_2 had stronger inhibitory effects on seed germination than thatextracted by pure CO_2.展开更多
Ruthenium (Ru)‐based catalysts are widely employed in several types of gas‐solid reactions because of their high catalytic activities. This review provides theoretical research on Ru‐based catalysts and an analys...Ruthenium (Ru)‐based catalysts are widely employed in several types of gas‐solid reactions because of their high catalytic activities. This review provides theoretical research on Ru‐based catalysts and an analysis of their basic properties and oxidation behavior. There is particular emphasis on Ru‐catalyzed gas‐solid catalytic reactions, including the catalytic oxidation of VOCs, preferential oxidation of CO, synthesis of ammonia, oxidation of HCl and partial oxidation of CH4. Recent litera‐ture on catalysis is summarized and compared. Finally, we describe current challenges in the field and propose approaches for future development of Ru‐based catalysts.展开更多
TiO2/γ-Al2O3 supported In/Ag catalysts were prepared by impregnation method,and investigated for NO reduction with CO as the reducing agent under lean burn conditions.The microscopic structure and surface properties ...TiO2/γ-Al2O3 supported In/Ag catalysts were prepared by impregnation method,and investigated for NO reduction with CO as the reducing agent under lean burn conditions.The microscopic structure and surface properties of the catalysts were studied by N2 adsorption-desorption,X-ray diffraction,transmission electron microscopy,X-ray photoelectron spectroscopy,ultraviolet-visible spectroscopy,H2 temperature-programmed reduction and Fourier transform infrared spectroscopy.TiO2/γ-Al2O3 supported In/Ag is a good catalyst for the reduction of NO to N2.It displayed high dispersion,large amounts of surface active components and high NO adsorption capacity,which gave good catalytic performance and stability for the reduction of NO with CO under lean burn conditions.The silver species stabilized and improved the dispersion of the indium species.The introduction of TiO2 into the γ-Al2O3 support promoted NO adsorption and improved the dispersion of the indium species and silver species.展开更多
Selective oxidation of glycerol is a hot topic.Increased biodiesel production has led to glycerol oxidation over Au- and Pt-based catalysts being widely studied.However,Pt catalysts suffer from deactivation because of...Selective oxidation of glycerol is a hot topic.Increased biodiesel production has led to glycerol oxidation over Au- and Pt-based catalysts being widely studied.However,Pt catalysts suffer from deactivation because of weak metal-support interactions.In this study,multi-walled carbon nanotube(MWCNTs)-pillared nitrogen-doped graphene(NG) was prepared by direct pyrolysis of melamine on MWCNTs,and the synthesized NG-MWCNT composite was used as the support for Pt.Characterization results showed that the surface area(173 m^2/g) and pore volume of the NG-MWCNT composite were greater than those of bare MWCNTs and the separated melamine pyrolysis product(CH_x).Pt(1.4±0.4 nm) dispersion on the NG-MWCNTs was favorable and the Pt/NG-MWCNT catalyst was highly active and selective in the oxidation of glycerol to glyceric acid(GLYA) in base-free aqueous solution.For example,the conversion of glycerol reached 64.4% with a GLYA selectivity of 81.0%,whereas the conversions of glycerol over Pt/MWCNTs and Pt/CN_x were 29.0% and 31.6%,respectively.The unique catalytic activity of the Pt/NG-MWCNTs is attributed to well-dispersed Pt clusters on the NG-MWCNTs and the electron-donating effect of the nitrogen dopant in the NG-MWCNTs.展开更多
A study was conducted to determine the effects of elevated CO2 on soil N process at Changbai Mountain in Jilin Province, northeastern China (42°24"N, 128°06"E, and 738 m elevation). A randomized complete...A study was conducted to determine the effects of elevated CO2 on soil N process at Changbai Mountain in Jilin Province, northeastern China (42°24"N, 128°06"E, and 738 m elevation). A randomized complete block design of ambient and elevated CO2 was established in an open-top chamber facility in the spring of 1999. Changpai Scotch pine (Pinus sylvestris var. sylvestriformis seeds were sowed in May, 1999 and CO2 fumigation treatments began after seeds germination. In each year, the exposure started at the end of April and stopped at the end of October. Soil samples were collected in June and August 2006 and in June 2007, and soil nitrifying, denitrifying and N2-fixing enzyme activities were measured. Results show that soil nitrifying enzyme activities (NEA) in the 5-10 cm soil layer were significantly increased at elevated CO2 by 30.3% in June 2006, by 30.9% in August 2006 and by 11.3% in June 2007. Soil denitrifying enzyme activities (DEA) were significantly decreased by elevated CO2 treatment in June 2006 (P 〈 0.012) and August 2006 (P 〈 0.005) samplings in our study; no significant difference was detected in June 2007, and no significant changes in N2-fixing enzyme activity were found. This study suggests that elevated CO2 can alter soil nitrifying enzyme and denitrifying enzyme activities.展开更多
The impacts of elevated atmospheric CO2 concentrations (500 靘olmol-1and 700 靘olmol-1) on total soil respiration and the contribution of root respiration of Pinus koraiensis seedlings were investigated from May to Oc...The impacts of elevated atmospheric CO2 concentrations (500 靘olmol-1and 700 靘olmol-1) on total soil respiration and the contribution of root respiration of Pinus koraiensis seedlings were investigated from May to October in 2003 at the Research Station of Changbai Mountain Forest Ecosystems, Chinese Academy of Sciences, Jilin Province, China. After four growing seasons in top-open chambers exposed to elevated CO2, the total soil respiration and roots respiration of Pinus koraiensis seedlings were measured by a LI-6400-09 soil CO2 flux chamber. Three PVC cylinders in each chamber were inserted about 30 cm into the soil in-stantaneously to terminate the supply of current photosynthates from the tree canopy to roots for separating the root respiration from total soil respiration. Soil respirations both inside and outside of the cylinders were measured on June 16, August 20 and October 8, respectively. The results indicated that: there was a marked diurnal change in air temperature and soil temperature at depth of 5 cm on June 16, the maximum of soil temperature at depth of 5 cm lagged behind that of air temperature, no differences in temperature between treatments were found (P>0.05). The total soil respiration and soil respiration with roots severed showed strong diurnal and seasonal patterns. There was marked difference in total soil respiration and soil respiration with roots severed between treatments (P<0.01); Mean total soil respiration and contribution of root under different treatments were 3.26, 4.78 and 1.47 靘olm 2s-1, 11.5%, 43.1% and 27.9% on June 16, August 20 and October 8, respectively.展开更多
Behaviors of TiO2 in the alumina carbothermic reduction and chlorination process in vacuum at different temperatures were investigated experimentally by means of XRD,SEM and EDS.In the preparation of materials,the mol...Behaviors of TiO2 in the alumina carbothermic reduction and chlorination process in vacuum at different temperatures were investigated experimentally by means of XRD,SEM and EDS.In the preparation of materials,the molar ratio of Al2O3 to C was 1:4,and 10% TiO2 and excess AlCl3 were added.The results show that TiC is produced by C and TiO2 after TiO2 transforms from anatase into rutile gradually.In the temperature range of 1 763?1 783 K,the compounds of Ti and Al are not found in slags and condensate.The purity of aluminum reaches 98.35%,and TiO2 does not participate in alumina carbothermic reduction process and chlorination process in vacuum.展开更多
CO2 concentrations at different heights in a broadleaved/Korean forest (with a mean height of 26 m) were measured with infrared gas analyzer IRGA (model 2250D, LI-COR Inc. and LI-COR, 820) from Aug. to Oct. of 1999, A...CO2 concentrations at different heights in a broadleaved/Korean forest (with a mean height of 26 m) were measured with infrared gas analyzer IRGA (model 2250D, LI-COR Inc. and LI-COR, 820) from Aug. to Oct. of 1999, Apr. to Jul. of 2000, and from Aug. 2002 to Sept. 2003. Based on the collected dada, the diurnal and seasonal dynamics of profiles and storage of carbon dioxide in the forest were analyzed. The diurnal CO2 profiles showed that the vertical distribution of CO2 concentration were different for daytime and nighttime, and the CO2 concentration was highest close to forest floor, no matter at daytime and nighttime. The seasonal profiles of CO2 showed that stratification in the canopy was evident during growth season. CO2 concentrations at different heights (60 m to 2.5 m) had a little change in March, with a difference of 10 mmolmol-1, but had a significant change in July, with a difference of 60 mmolmol-1. In July, there also existed a greater gradient of CO2 concentrations at canopy (22, 26 and 32 m), with a difference of 8 mmolmol-1. The calculated total storage (ΔC/Δt ) of CO2 in the air column with height of 40 m beneath eddy covariance instrument was negative, and made a little contribution to NEE.展开更多
基金"中央高校基本科研业务费专项资金资助"(Supported by the Fundamental Research Fundsfor the Central Universities)重大项目"提升区域发展能力:继续推进西部大开发战略的路径选择的对策研究"(项目编号:12LZUJBWZZ002)2011年甘肃省社科规划项目"甘肃省区域和行业碳减排问题研究"
基金supported by the National Natural Science Foundation of China(Grant No.42025403)the Youth Innovation Promotion Association,Chinese Academy of Sciences(Grant No.2023074).
文摘From June 2008 to August 2013,approximately 67 kt of CO_(2) was injected into a deep saline formation at the Ketzin pilot CO_(2) storage site.During injection,3D seismic surveys have been performed to monitor the migration of sequestered CO_(2).Seismic monitoring results are limited by the acquisition and signal-to-noise ratio of the acquired data.The multiphysical reservoir simulation provides information regarding the CO_(2) fluid behavior,and the approximated model should be calibrated with the monitoring results.In this work,property models are delivered from the multiphysical model during 3D repeated seismic surveys.The simulated seismic data based on the models are compared with the real data,and the results validate the effectiveness of the multiphysical inversion method.Time-lapse analysis shows the trend of CO_(2) migration during and after injection.
基金The National Natural Science Foundation of China(No.41877240)Scientific Research Foundation of Graduate School of Southeast University(No.YBPY1930).
文摘Considering that copper mine tailings(CMTs)are commonly mixed with ordinary Portland cement,fly ash(FA),and kaolin to produce geopolymers,to make full use of CMTs,the properties of geopolymers manufactured under different material mass ratios and curing methods(standard curing,water bath curing,and 60℃curing)are evaluated with significantly increased dosage of CMTs.Porosity and unconfined compressive strength tests,X-ray diffraction,field emission scanning electron microscopy,and energy dispersive spectroscopy are used to determine the physical and mechanical properties,microstructure,and mineral composition of geopolymers.Finally,costs and CO 2 emissions of specimens with different material mass ratios during the preparation processes are compared.The results show that during the geopolymerization of low-calcium materials,various geopolymer gels,including calcium silicate,calcium silicoaluminate,and mainly sodium silicoaluminate gels,coexist.The solid waste,cost,and carbon dioxide emission reductions can reach 100%,166.3 yuan/t,and 73.3 kg/t,respectively.Under a curing condition of 60℃,the sample with a CMTs mass fraction of 70%and an FA mass fraction of 30%meets the requirements of porosity,compressive strength.The resource utilization of CMT and FA is realized in a more economical way.
基金supported by the National Key Research and Development Program of China(No.2020YFB1506002,2019YFB1504503,2016YFB0101202)National 973 Program of China(No.2012CB215501)National Natural Science Foundation of China(No.52021004,22022502(2021),21822803(2019),21576031(2016),51272297(2013),20936008(2010),20676156(2007),20376088(2004),20176066(2002),29976047(2000)).
文摘Two major challenges,high cost and short lifespan,have been hindering the commercialization process of lowtemperature fuel cells.Professor Wei's group has been focusing on decreasing cathode Pt loadings without losses of activity and durability,and their research advances in this area over the past three decades are briefly reviewed herein.Regarding the Pt-based catalysts and the low Pt usage,they have firstly tried to clarify the degradation mechanism of Pt/C catalysts,and then demonstrated that the activity and stability could be improved by three strategies:regulating the nanostructures of the active sites,enhancing the effects of support materials,and optimizing structures of the three-phase boundary.For Pt-free catalysts,especialiy carbon-based ones,several strategies that they proposed to enhance the activity of nitrogen-/heteroatom-doped carbon catalysts are firstly presented.Then,an indepth understanding of the degradation mechanism for carbon-based catalysts is discussed,and followed by the corresponding stability enhancement strategies.Also,the carbon-based electrode at the micrometer-scale,faces the challenges such as low active-site density,thick catalytic layer,and the effect of hydrogen peroxide,which require rational structure design for the integral cathodic electrode.This review finally gives a brief conclusion and outlook about the low cost and long lifespan of cathodic oxygen reduction catalysts.
文摘Graphene oxide(GO)with excellent dispersion ability can assist the dispersion of single-walled carbon nanotube(SWCNT)and promote the formation of uniform and stable GO/SWCNT coating liquid.The highly conductive polyethylene terephthalate/reduced graphene oxide/SWCNT(PET/rGO/SWCNT)electromagnetic shielding composite fabric was successfully prepared by anchoring rGO/SWCNT on PET fabric via dip-coating piror to low-temperature thermal reduction.The results showed that the carboxyl groups and hydroxyl groups formed of hydrophilic-treated PET were conducive to the formation of hydrogen bonds with that of GO,which enhanced the interaction between PET fabric and GO/SWCNT coating;the loading of GO/SWCNT increased with the number of dip-coating,the unit area loading of rGO/SWCNT in the final composite fabric was 2.7 mg/cm^(2) after 10 dip-coating cycles and thermal reduction;the PET/rGO/SWCNT composite fabric had a continuous and dense conductive network,with a conductivity of up to 41.6 S/m and the average electromagnetic interference shielding effectiveness in X-band was 22 dB;the flexible PET/rGO/SWCNT composite fabric was not only easy to process,but also exhibited excellent conductivity and shielding efficiency,showing great potential in the application of electromagnetic shielding fabrics.
基金supported by the National Science and Technology Support Project of China(2013BAC11B03)the National Natural Science Foundation of China(21401054,21476065,21273067)the Graduate Student Scientific Research Innovation Fund Project of Hunan Province(CX2015B082)~~
文摘The aim of "green chemistry" and "atom economy" is to utilize carbon dioxide and replace harmful reactants such as CO and phosgene for the production of cyclic carbonates. In this paper, metal-free catalysts including organic bases, ionic liquids, supported catalysts, organic copolymers and carbon materials for the synthesis of cyclic carbonates by the cycloaddition of carbon dioxide to epoxides are reviewed. Recent advances in the design of the catalysts and the understanding of the reaction mechanism are summarized and discussed. The synergistic effects of organic bases and hydrogen bond donors, organic bases and nucleophilic anions, hydrogen bond donors and nucleophilic anions and active components and supports are highlighted. The challenge is to develop metal-free catalysts suitable for carbon dioxide capture and fixation. The ultimate goal is to synthesize cyclic carbonates in a flow reactor directly using carbon dioxide from industrial flue gas at ambient temperature and atmospheric pressure. By using synergetic effects, a multi-functional approach can meet the design strategy of metal-free catalysts for carbon dioxide adsorption and activation as well as epoxide ring opening.
文摘Low‐temperature CO oxidation is important for both fundamental studies and practical applica‐tions. Supported gold catalysts are generally regarded as the most active catalysts for low‐temperature CO oxidation. The active sites are traditionally believed to be Au nanoclusters or nanoparticles in the size range of 0.5–5 nm. Only in the last few years have single‐atom Au catalysts been proved to be active for CO oxidation. Recent advances in both experimental and theoretical studies on single‐atom Au catalysts unambiguously demonstrated that when dispersed on suitable oxide supports the Au single atoms can be extremely active for CO oxidation. In this mini‐review, recent advances in the development of Au single‐atom catalysts are discussed, with the aim of illus‐trating their unique catalytic features during CO oxidation.
基金Project(u0837604)supported by the Natural Science Foundation of Yunnan Province,ChinaProject(51004058)supported by the National Natural Science Foundation of ChinaProject(20095314110003)supported by Specialized Research Fund for the Doctoral Program of Higher Education
文摘The preparation of fine TiC powders by carbothermal reduction of TiO2 in vacuum was investigated by XRD,SEM,XRF and laser particle sizer.Thermodynamic analysis indicates that it is easy to prepare TiC in vacuum and the formation sequence of products are Ti4O7(Magneli phase),Ti3O5,Ti2O3,TiCxO1-x and TiC with the increase of reaction temperature.Experimental results demonstrate that TiC powders with single phase are obtained with molar ratio of TiO2 to C ranging from 1:3.2 to 1:6 at 1 550 ℃ for 4 h when the system pressure is 50 Pa,and TiC1.0 is gained when the molar ratio of TiO2 to C is 1:4 and 1:5.In addition,fine TiC1.0 powders(D50 equals 3.04 μm) with single phase and low impurities are obtained when the molar ratio of TiO2 to C is 1:4.SEM observation shows that uniform shape,low agglomeration,and loose structure are observed on the surface of block product.
基金supported by the National Natural Science Foundation of China(21076211,21203181,21576251,21676269)the "Strategic Priority Research Program" of the Chinese Academy of Sciences(XDB17020100)+1 种基金the National Key projects for Fundamental Research and Development of China(2016YFA0202801)Department of Science and Technology of Liaoning Province under contract of 2015020086-101~~
文摘CO oxidation is probably the most studied reaction in heterogeneous catalysis.This reaction has become a hot topic with the discovery of nanogold catalysts,which are active at low temperatures(at or below room temperature).Au catalysts are the benchmark for judging the activities of other metals in CO oxidation.Pt-group metals(PGMs) that give comparable performances are of particular interest.In this mini-review,we summarize the advances in various PGM(Pt,Pd,Ir,Rh,Ru)catalysts that have high catalytic activities in low-temperature CO oxidation arising from reducible supports or the presence of OH species.The effects of the size of the metal species and the importance of the interface between the metal and the reducible support are covered and discussed in terms of their promotional role in CO oxidation at low temperatures.
文摘The structure and catalytic desulfurization characteristics of CeO2-TiO2 mixed oxides were investigated by means ofX-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and catalytic activity tests. According to the results, a CeO2-TiO2solid solution is formed when the mole ratio of cerium to titanium n(Ce):n(Ti) is 5:5 or greater, and the most suitable n(Ce):n(Ti) isdetermined as 7:3, over which the conversion rate of SO2 and the yield of sulfur at 500℃ reach 93% and 99%, respectively.According to the activity testing curve, Ce0.7Ti0.3O2 (n(Ce):n(Ti)=7:3) without any pretreatment can be gradually activated by reagentgas after about 10 min, and reaches a steady activation status 60 min later. The XPS results of Ce0.7Ti0.3O2 after different time ofSO2+CO reaction show that CeO2 is the active component that offers the redox couple Ce4+/Ce3+ and the labile oxygen vacancies, andTiO2 only functions as a catalyst structure stabilizer during the catalytic reaction process. After 48 h of catalytic reaction at 500℃,Ce0.7Ti0.3O2 still maintains a stable structure without being vulcanized, demonstrating its good anti-sulfur poisoning performance.
基金This paper was supported by Natural Science Foundation of Fujian Province (B0010020)
文摘Allelochemicals of Chinese-fir root was extracted by technology ofsupercritical CO_2 extraction under orthogonal experiment design, and it was used to analyzeallelopathic activity of Chinese-fir through bioassay of seed germination. The results showed thatas to the available rate of allelochemicals, the pressure and temperature of extraction were themost important factors. The allelochemicals of Chinese-fir root extracted by pure CO_2 and ethanolmixed with CO_2 have different allelopathic activities to seed germination, and the allelochemicalsextracted by ethanol mixed with CO_2 had stronger inhibitory effects on seed germination than thatextracted by pure CO_2.
基金supported by Beijing Natural Science Foundation (8164063)the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB05050100)~~
文摘Ruthenium (Ru)‐based catalysts are widely employed in several types of gas‐solid reactions because of their high catalytic activities. This review provides theoretical research on Ru‐based catalysts and an analysis of their basic properties and oxidation behavior. There is particular emphasis on Ru‐catalyzed gas‐solid catalytic reactions, including the catalytic oxidation of VOCs, preferential oxidation of CO, synthesis of ammonia, oxidation of HCl and partial oxidation of CH4. Recent litera‐ture on catalysis is summarized and compared. Finally, we describe current challenges in the field and propose approaches for future development of Ru‐based catalysts.
基金supported by the National Science & Technology Pillar Program(2012BAF03B02)National Natural Science Foundation of China(21101085,U1162203)+3 种基金Natural Science Foundation of Liaoning Province(2015020196)Doctoral Fund of Shandong Province(BS2015HZ003)Fushun Science & Technology Program(FSKJHT 201423)Liaoning Excellent Talents Program in University(LJQ2012031)~~
文摘TiO2/γ-Al2O3 supported In/Ag catalysts were prepared by impregnation method,and investigated for NO reduction with CO as the reducing agent under lean burn conditions.The microscopic structure and surface properties of the catalysts were studied by N2 adsorption-desorption,X-ray diffraction,transmission electron microscopy,X-ray photoelectron spectroscopy,ultraviolet-visible spectroscopy,H2 temperature-programmed reduction and Fourier transform infrared spectroscopy.TiO2/γ-Al2O3 supported In/Ag is a good catalyst for the reduction of NO to N2.It displayed high dispersion,large amounts of surface active components and high NO adsorption capacity,which gave good catalytic performance and stability for the reduction of NO with CO under lean burn conditions.The silver species stabilized and improved the dispersion of the indium species.The introduction of TiO2 into the γ-Al2O3 support promoted NO adsorption and improved the dispersion of the indium species and silver species.
基金financially supported by the National Natural Science Foundation of China(21473155,21273198,21073159)Natural Science Foundation of Zhejiang Province(L12B03001)the foundation from State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology(GCTKF2014009)~~
文摘Selective oxidation of glycerol is a hot topic.Increased biodiesel production has led to glycerol oxidation over Au- and Pt-based catalysts being widely studied.However,Pt catalysts suffer from deactivation because of weak metal-support interactions.In this study,multi-walled carbon nanotube(MWCNTs)-pillared nitrogen-doped graphene(NG) was prepared by direct pyrolysis of melamine on MWCNTs,and the synthesized NG-MWCNT composite was used as the support for Pt.Characterization results showed that the surface area(173 m^2/g) and pore volume of the NG-MWCNT composite were greater than those of bare MWCNTs and the separated melamine pyrolysis product(CH_x).Pt(1.4±0.4 nm) dispersion on the NG-MWCNTs was favorable and the Pt/NG-MWCNT catalyst was highly active and selective in the oxidation of glycerol to glyceric acid(GLYA) in base-free aqueous solution.For example,the conversion of glycerol reached 64.4% with a GLYA selectivity of 81.0%,whereas the conversions of glycerol over Pt/MWCNTs and Pt/CN_x were 29.0% and 31.6%,respectively.The unique catalytic activity of the Pt/NG-MWCNTs is attributed to well-dispersed Pt clusters on the NG-MWCNTs and the electron-donating effect of the nitrogen dopant in the NG-MWCNTs.
基金supported by the National Natural Science Foundation of China (No.90411020)Major State Basic Research Development Program of China (973 Program)(2002CB412502).
文摘A study was conducted to determine the effects of elevated CO2 on soil N process at Changbai Mountain in Jilin Province, northeastern China (42°24"N, 128°06"E, and 738 m elevation). A randomized complete block design of ambient and elevated CO2 was established in an open-top chamber facility in the spring of 1999. Changpai Scotch pine (Pinus sylvestris var. sylvestriformis seeds were sowed in May, 1999 and CO2 fumigation treatments began after seeds germination. In each year, the exposure started at the end of April and stopped at the end of October. Soil samples were collected in June and August 2006 and in June 2007, and soil nitrifying, denitrifying and N2-fixing enzyme activities were measured. Results show that soil nitrifying enzyme activities (NEA) in the 5-10 cm soil layer were significantly increased at elevated CO2 by 30.3% in June 2006, by 30.9% in August 2006 and by 11.3% in June 2007. Soil denitrifying enzyme activities (DEA) were significantly decreased by elevated CO2 treatment in June 2006 (P 〈 0.012) and August 2006 (P 〈 0.005) samplings in our study; no significant difference was detected in June 2007, and no significant changes in N2-fixing enzyme activity were found. This study suggests that elevated CO2 can alter soil nitrifying enzyme and denitrifying enzyme activities.
文摘The impacts of elevated atmospheric CO2 concentrations (500 靘olmol-1and 700 靘olmol-1) on total soil respiration and the contribution of root respiration of Pinus koraiensis seedlings were investigated from May to October in 2003 at the Research Station of Changbai Mountain Forest Ecosystems, Chinese Academy of Sciences, Jilin Province, China. After four growing seasons in top-open chambers exposed to elevated CO2, the total soil respiration and roots respiration of Pinus koraiensis seedlings were measured by a LI-6400-09 soil CO2 flux chamber. Three PVC cylinders in each chamber were inserted about 30 cm into the soil in-stantaneously to terminate the supply of current photosynthates from the tree canopy to roots for separating the root respiration from total soil respiration. Soil respirations both inside and outside of the cylinders were measured on June 16, August 20 and October 8, respectively. The results indicated that: there was a marked diurnal change in air temperature and soil temperature at depth of 5 cm on June 16, the maximum of soil temperature at depth of 5 cm lagged behind that of air temperature, no differences in temperature between treatments were found (P>0.05). The total soil respiration and soil respiration with roots severed showed strong diurnal and seasonal patterns. There was marked difference in total soil respiration and soil respiration with roots severed between treatments (P<0.01); Mean total soil respiration and contribution of root under different treatments were 3.26, 4.78 and 1.47 靘olm 2s-1, 11.5%, 43.1% and 27.9% on June 16, August 20 and October 8, respectively.
基金Project (u0837604) supported by the Joint Funds of the National Natural Science Foundation of China and Yunnan ProvinceProject (20095314110003) supported by the Special Research Funds of the Doctor Subject of Higher School,China
文摘Behaviors of TiO2 in the alumina carbothermic reduction and chlorination process in vacuum at different temperatures were investigated experimentally by means of XRD,SEM and EDS.In the preparation of materials,the molar ratio of Al2O3 to C was 1:4,and 10% TiO2 and excess AlCl3 were added.The results show that TiC is produced by C and TiO2 after TiO2 transforms from anatase into rutile gradually.In the temperature range of 1 763?1 783 K,the compounds of Ti and Al are not found in slags and condensate.The purity of aluminum reaches 98.35%,and TiO2 does not participate in alumina carbothermic reduction process and chlorination process in vacuum.
基金This study is supported by The Development Plan of State Key Fundamental Research of China (973) (contract No. 2002CB412502),by Knowledge Innovation Project of CAS (KZCX1-SW-01-03) and by Natural Science Foundation of China (30170167).
文摘CO2 concentrations at different heights in a broadleaved/Korean forest (with a mean height of 26 m) were measured with infrared gas analyzer IRGA (model 2250D, LI-COR Inc. and LI-COR, 820) from Aug. to Oct. of 1999, Apr. to Jul. of 2000, and from Aug. 2002 to Sept. 2003. Based on the collected dada, the diurnal and seasonal dynamics of profiles and storage of carbon dioxide in the forest were analyzed. The diurnal CO2 profiles showed that the vertical distribution of CO2 concentration were different for daytime and nighttime, and the CO2 concentration was highest close to forest floor, no matter at daytime and nighttime. The seasonal profiles of CO2 showed that stratification in the canopy was evident during growth season. CO2 concentrations at different heights (60 m to 2.5 m) had a little change in March, with a difference of 10 mmolmol-1, but had a significant change in July, with a difference of 60 mmolmol-1. In July, there also existed a greater gradient of CO2 concentrations at canopy (22, 26 and 32 m), with a difference of 8 mmolmol-1. The calculated total storage (ΔC/Δt ) of CO2 in the air column with height of 40 m beneath eddy covariance instrument was negative, and made a little contribution to NEE.