A variety of spherical and structured activated charcoal supported Pt/Fe3O4 composites with an average particle size of ~100 nm have been synthesized by a self-assembly method using the difference of reduction potenti...A variety of spherical and structured activated charcoal supported Pt/Fe3O4 composites with an average particle size of ~100 nm have been synthesized by a self-assembly method using the difference of reduction potential between Pt (Ⅳ) and Fe (Ⅱ) precursors as driving force. The formed Fe3O4 nanoparticles (NPs) effectively prevent the aggregation of Pt nanocrystallites and promote the dispersion of Pt NPs on the surface of catalyst, which will be favorable for the exposure of Pt active sites for high-efficient adsorption and contact of substrate and hydrogen donor. The electron-enrichment state of Pt NPs donated by Fe304 nanocrystallites is corroborated by XPS measurement, which is responsible for promoting and activating the terminal C=O bond of adsorbed substrate via a vertical configuration. The experimental results show that the activated charcoal supported Pt/Fe3O4 catalyst exhibits 94.8% selectivity towards cinnamyl alcohol by the transfer hydrogenation of einnamaldehyde with Pt loading of 2.46% under the optimum conditions of 120 ℃ for 6 h, and 2-propanol as a hydrogen donor. Additionally, the present study demonstrates that a high-efficient and recyclable catalyst can be rapidly separated from the mixture due to its natural magnetism upon the application of magnetic field.展开更多
The catalytic performance of co mmonly used heteropolyacids (H3PW12O40, H4SiW12O40 and H3PMO12O40 synthesis of 4,4'-methylenedianiline (4,4'-MDA) from aniline and formaldehyde was evaluated and the result showed ...The catalytic performance of co mmonly used heteropolyacids (H3PW12O40, H4SiW12O40 and H3PMO12O40 synthesis of 4,4'-methylenedianiline (4,4'-MDA) from aniline and formaldehyde was evaluated and the result showed that H4SiW12O40 with moderate acid strength exhibited the best catalytic performance. Then HaSiW12O40@MIL-100(Fe) was prepared by encapsulating H4SiW12O40 within the pores of MIL-100(Fe) to facilitate its recovery and reuse. The prepared H4SiW12O40@MIL-100(Fe) was characterized by means of FT-IR, N2 adsorption-desorption, XRD, TG and then the catalytic performance was evaluated. The result showed that H4SiW12O40 was highly dispersed in the pores of MIL-100(Fe), and both the Keggin structure of HaSiW12O40 and the crystal skeleton structure of MIL-100(Fe) could be effectively/preserved. Furthermore, H4SiW12O40@ MIL-100(Fe) showed excellent catalytic performance under the following reaction conditions: a molar ratio of aniline to formaldehyde = 5, a mass ratio of catalyst to formaldehyde = 1.2, a reaction temperature of 120 ℃ and a reaction time of 6 h. Under the above reaction conditions, the conversion of aniline was 41.1%, and the yield and selectivity of 4,4'-MDA were 81,6% and 79.2%, respectively. Unfortunately, an appreciable loss in the catalytic activity of the recovered H4SiW12O40@MIL-100(Fe) was observed because of the blocking of the pores and the change of the acidity resulted from the adsorption of alkaline organics such as aniline and 4,4'-MDA. The adsorbed alkaline organics could be cleaned up when the recovered catalyst was washed by methanol and DMF. Then the catalyst was effectively reused up to three cycles without much loss in its activity.展开更多
The study on the behaviourof potassium, phosphate and trace elements, Fe, Mn, Cu and Zn, in the rhizosphere of different varieties of flue-cured tobacco (Nicotiana tabacum L.) with high and low potassium application r...The study on the behaviourof potassium, phosphate and trace elements, Fe, Mn, Cu and Zn, in the rhizosphere of different varieties of flue-cured tobacco (Nicotiana tabacum L.) with high and low potassium application rate with rhizobag technique showed that soil available K, soil available P, and slow available K was in depletion status, whereas DTPA extractable Fe, Mn, Zn and Cu accumulated obviously in rhizosphere. The depletion and accumulation rates of mineral nutrients differed in degree with K application rate, soil type, and tobacco variety. The content of a vailable K in both rhizosphere and bulk soil and K concentration in tobacco leaf increased significantly, and the available P in rhizosphere dropped with more K applicatin. The DTPA-Fe content of red soil much lower in pH was higher than that of calcareous soil in bulk soil. But the DTPA-Fe content of calcareous soil was much higher than that of red soil in rhizosphere, which was considered perhaps to be mainly related to releasing of Fe phytosiderophore. Nitrate could increase depletion of available K in rhizosphere and also soil pH in comparison with ammonium.展开更多
Rice planting decreased total iron but increased active iron.Iron activation varied greatly among different paddy soils but not in woodland soils.Paddy soil iron was mainly affected by pH,SOC and particle composition....Rice planting decreased total iron but increased active iron.Iron activation varied greatly among different paddy soils but not in woodland soils.Paddy soil iron was mainly affected by pH,SOC and particle composition.The decrease of soil Fe was mainly in the form of Fec and was closely related to SOC.展开更多
Walnut-shell activated carbon(WSAC) supported ferric oxide was modified by non-thermal plasma(NTP), and the removal efficiency for hydrogen sulfide over Fe/WSAC modified by dielectric barrier discharge(DBD) was ...Walnut-shell activated carbon(WSAC) supported ferric oxide was modified by non-thermal plasma(NTP), and the removal efficiency for hydrogen sulfide over Fe/WSAC modified by dielectric barrier discharge(DBD) was significantly promoted. The sample modified for10 min and 6.8 k V output(30 V input voltage) maintained 100% H2 S conversion over a long reaction time of 390 min. The surface properties of adsorbents modified by NTP under different conditions were evaluated by the methods of X-ray photoelectron spectroscopy(XPS), Brunauer–Emmett–Teller(BET) analysis and in-situ Fourier transform infrared spectroscopy(FTIR), to help understand the effect of the NTP treatment. NTP treatment enhanced the adsorption capacity of Fe/WSAC, which could due to the formation of micro-pores with sizes of0.4, 0.5 and 0.75 nm. XPS revealed that chemisorbed oxygen changed into lattice oxygen after NTP treatment, and lattice oxygen is beneficial for H2 S oxidation. From the in-situ FTIR result,transformation of the reaction path on Fe/WSAC was observed after NTP modification. The research results indicate that NTP is an effective method to improve the surface properties of the Fe/WSAC catalyst for H2 S adsorption-oxidation.展开更多
A theoretical model concerning active Q-switching of an Fe:ZnSe laser pumped by a continuous-wave(CW)2.8μm fiber laser is developed.Calculations are compared with the recently reported experiment results,and good agr...A theoretical model concerning active Q-switching of an Fe:ZnSe laser pumped by a continuous-wave(CW)2.8μm fiber laser is developed.Calculations are compared with the recently reported experiment results,and good agreement is achieved.Effects of principal parameters,including pump power,output reflectivity,ion concentration and temperature of crystal,on the laser output performance are investigated and analyzed.Numerical results demonstrate that similar to highly efficient CWFe:ZnSe laser,low temperature of the crystal is significant to obtain high peak power Q-switched pulses.The numerical simulation results are useful for optimizing the design of actively Q-switched Fe:ZnSe laser.展开更多
ZrC nanoparticles in the matrix of Fe were produced by the mechanically activated self-propagating hightemperature method using ZrO2/C/Mg/Fe powder mixtures. The effects of milling time, Fe content, and combustion tem...ZrC nanoparticles in the matrix of Fe were produced by the mechanically activated self-propagating hightemperature method using ZrO2/C/Mg/Fe powder mixtures. The effects of milling time, Fe content, and combustion temperature as well as the formation route for synthesizing ZrC powder particles were studied. The samples were characterized by XRD, SEM, TEM, and DTA. The XRD results revealed that, after 18 h of mechanical activation, ZrO2/ZC/Mg/Fe reacted with the self-propagating combustion(SHS) mode at 870 °C producing the ZrC–Fe nanocomposite. It was also found that both mechanical activation and Fe content played key roles in the ZrC synthesis temperature. With a Fe content of(5–40) wt%, the SHS reaction proceeded favorably and both the ZrC formation temperature and the adiabatic temperature(Tad) decreased. The Mg O content was removed from the final products using a leaching test process by dissolving in hydrochloric and acetic acids.展开更多
Identification of chemical oxygen demand(COD)in municipal solid waste(MSW)landfill leachates is a challenging problem.This paper investigated the feasibility of using sodium persulfate(PS),a strong oxidant,as a permea...Identification of chemical oxygen demand(COD)in municipal solid waste(MSW)landfill leachates is a challenging problem.This paper investigated the feasibility of using sodium persulfate(PS),a strong oxidant,as a permeable reactive barrier(PRB)filling material.Firstly,sustained-release persulfate balls were manufactured to adjust the release rate of persulfate,the oxidation agent.In addition,Fe(II)-loaded activated carbon(Fe-AC)was used to help with an even distribution of Fe(II)in the porous medium(PRB in this case).Then,the oxidation efficiency and kinetic rate of COD removal by the sustained-release balls were subjected to batch tests.A mass ratio of 1:1.4:0.24:0.7 for PS:cement:sand:water was the most efficient for COD removal(95%).The breakthrough curve for a 5 mm sustained-release ball revealed that the retardation factor was 1.27 and that the hydrodynamic dispersion coefficient was 15.6 cm^(2)/d.The corresponding half-life of COD oxidation was 0.43 d,which was comparable with the half-life of PS release from sustained-release balls(0.56 d).The sustained-release persulfate balls were shown to be an economical material with a simple recipe and production method when catalyzed by Fe-AC.Compared with cutting-edge methods,sustained-release balls used in PRBs offer significant advantages in terms of both effectiveness and economy for the preparation of sustained-release and catalytic materials.These results verified the feasibility of using sustained-release persulfate balls as a PRB material for COD removal.展开更多
Weak magnetic field(WMF) was employed to improve the removal of Cr(VI) by zero-valent iron(ZVI) for the first time. The removal rate of Cr(VI) was elevated by a factor of 1.12-5.89 due to the application of a ...Weak magnetic field(WMF) was employed to improve the removal of Cr(VI) by zero-valent iron(ZVI) for the first time. The removal rate of Cr(VI) was elevated by a factor of 1.12-5.89 due to the application of a WMF, and the WMF-induced improvement was more remarkable at higher Cr(VI) concentration and higher p H. Fe2+was not detected until Cr(VI) was exhausted, and there was a positive correlation between the WMF-induced promotion factor of Cr(VI) removal rate and that of Fe2+release rate in the absence of Cr(VI) at pH 4.0-5.5. These phenomena imply that ZVI corrosion with Fe2+release was the limiting step in the process of Cr(VI) removal. The superimposed WMF had negligible influence on the apparent activation energy of Cr(VI) removal by ZVI, indicating that WMF accelerated Cr(VI)removal by ZVI but did not change the mechanism. The passive layer formed with WMF was much more porous than without WMF, thereby facilitating mass transport. Therefore,WMF could accelerate ZVI corrosion and alleviate the detrimental effects of the passive layer, resulting in more rapid removal of Cr(VI) by ZVI. Exploiting the magnetic memory of ZVI, a two-stage process consisting of a small reactor with WMF for ZVI magnetization and a large reactor for removing contaminants by magnetized ZVI can be employed as a new method of ZVI-mediated remediation.展开更多
基金This work is supported by the National Natural Science Foundation of China (No.51372248, No.51432009 and No.51502297), Instrument Developing Project of the Chinese Academy of Sciences (No.yz201421), the CAS/SAFEA International Partnership Program for Creative Research Teams of Chinese Academy of Sciences, China.
文摘A variety of spherical and structured activated charcoal supported Pt/Fe3O4 composites with an average particle size of ~100 nm have been synthesized by a self-assembly method using the difference of reduction potential between Pt (Ⅳ) and Fe (Ⅱ) precursors as driving force. The formed Fe3O4 nanoparticles (NPs) effectively prevent the aggregation of Pt nanocrystallites and promote the dispersion of Pt NPs on the surface of catalyst, which will be favorable for the exposure of Pt active sites for high-efficient adsorption and contact of substrate and hydrogen donor. The electron-enrichment state of Pt NPs donated by Fe304 nanocrystallites is corroborated by XPS measurement, which is responsible for promoting and activating the terminal C=O bond of adsorbed substrate via a vertical configuration. The experimental results show that the activated charcoal supported Pt/Fe3O4 catalyst exhibits 94.8% selectivity towards cinnamyl alcohol by the transfer hydrogenation of einnamaldehyde with Pt loading of 2.46% under the optimum conditions of 120 ℃ for 6 h, and 2-propanol as a hydrogen donor. Additionally, the present study demonstrates that a high-efficient and recyclable catalyst can be rapidly separated from the mixture due to its natural magnetism upon the application of magnetic field.
基金Supported by the National Natural Science Foundation of China(21236001,21476058,21506046)
文摘The catalytic performance of co mmonly used heteropolyacids (H3PW12O40, H4SiW12O40 and H3PMO12O40 synthesis of 4,4'-methylenedianiline (4,4'-MDA) from aniline and formaldehyde was evaluated and the result showed that H4SiW12O40 with moderate acid strength exhibited the best catalytic performance. Then HaSiW12O40@MIL-100(Fe) was prepared by encapsulating H4SiW12O40 within the pores of MIL-100(Fe) to facilitate its recovery and reuse. The prepared H4SiW12O40@MIL-100(Fe) was characterized by means of FT-IR, N2 adsorption-desorption, XRD, TG and then the catalytic performance was evaluated. The result showed that H4SiW12O40 was highly dispersed in the pores of MIL-100(Fe), and both the Keggin structure of HaSiW12O40 and the crystal skeleton structure of MIL-100(Fe) could be effectively/preserved. Furthermore, H4SiW12O40@ MIL-100(Fe) showed excellent catalytic performance under the following reaction conditions: a molar ratio of aniline to formaldehyde = 5, a mass ratio of catalyst to formaldehyde = 1.2, a reaction temperature of 120 ℃ and a reaction time of 6 h. Under the above reaction conditions, the conversion of aniline was 41.1%, and the yield and selectivity of 4,4'-MDA were 81,6% and 79.2%, respectively. Unfortunately, an appreciable loss in the catalytic activity of the recovered H4SiW12O40@MIL-100(Fe) was observed because of the blocking of the pores and the change of the acidity resulted from the adsorption of alkaline organics such as aniline and 4,4'-MDA. The adsorbed alkaline organics could be cleaned up when the recovered catalyst was washed by methanol and DMF. Then the catalyst was effectively reused up to three cycles without much loss in its activity.
基金Project supported by the National Natural Science Foundation of ChinaChina National Tobacco Corporation.
文摘The study on the behaviourof potassium, phosphate and trace elements, Fe, Mn, Cu and Zn, in the rhizosphere of different varieties of flue-cured tobacco (Nicotiana tabacum L.) with high and low potassium application rate with rhizobag technique showed that soil available K, soil available P, and slow available K was in depletion status, whereas DTPA extractable Fe, Mn, Zn and Cu accumulated obviously in rhizosphere. The depletion and accumulation rates of mineral nutrients differed in degree with K application rate, soil type, and tobacco variety. The content of a vailable K in both rhizosphere and bulk soil and K concentration in tobacco leaf increased significantly, and the available P in rhizosphere dropped with more K applicatin. The DTPA-Fe content of red soil much lower in pH was higher than that of calcareous soil in bulk soil. But the DTPA-Fe content of calcareous soil was much higher than that of red soil in rhizosphere, which was considered perhaps to be mainly related to releasing of Fe phytosiderophore. Nitrate could increase depletion of available K in rhizosphere and also soil pH in comparison with ammonium.
基金financially supported by Scientific Research Fund of Hunan Provincial Education Department(Grant No.20A234)San’an Nie thanks the National Natural Science Foundation of China(Grant No.42177288)as well as the National Natural Science Foundation of Hunan Province,China(Grant No.2023JJ30307).
文摘Rice planting decreased total iron but increased active iron.Iron activation varied greatly among different paddy soils but not in woodland soils.Paddy soil iron was mainly affected by pH,SOC and particle composition.The decrease of soil Fe was mainly in the form of Fec and was closely related to SOC.
基金supported by National Natural Science Foundation of China(Nos.21667015,51408282 and 21367016)
文摘Walnut-shell activated carbon(WSAC) supported ferric oxide was modified by non-thermal plasma(NTP), and the removal efficiency for hydrogen sulfide over Fe/WSAC modified by dielectric barrier discharge(DBD) was significantly promoted. The sample modified for10 min and 6.8 k V output(30 V input voltage) maintained 100% H2 S conversion over a long reaction time of 390 min. The surface properties of adsorbents modified by NTP under different conditions were evaluated by the methods of X-ray photoelectron spectroscopy(XPS), Brunauer–Emmett–Teller(BET) analysis and in-situ Fourier transform infrared spectroscopy(FTIR), to help understand the effect of the NTP treatment. NTP treatment enhanced the adsorption capacity of Fe/WSAC, which could due to the formation of micro-pores with sizes of0.4, 0.5 and 0.75 nm. XPS revealed that chemisorbed oxygen changed into lattice oxygen after NTP treatment, and lattice oxygen is beneficial for H2 S oxidation. From the in-situ FTIR result,transformation of the reaction path on Fe/WSAC was observed after NTP modification. The research results indicate that NTP is an effective method to improve the surface properties of the Fe/WSAC catalyst for H2 S adsorption-oxidation.
基金the 2021 Annual Instructional Science and Technology Program of Yongzhou(No.2021YZKJ09)the Science Research Project of Hunan Institute of Science and Technology(No.21xky040)。
文摘A theoretical model concerning active Q-switching of an Fe:ZnSe laser pumped by a continuous-wave(CW)2.8μm fiber laser is developed.Calculations are compared with the recently reported experiment results,and good agreement is achieved.Effects of principal parameters,including pump power,output reflectivity,ion concentration and temperature of crystal,on the laser output performance are investigated and analyzed.Numerical results demonstrate that similar to highly efficient CWFe:ZnSe laser,low temperature of the crystal is significant to obtain high peak power Q-switched pulses.The numerical simulation results are useful for optimizing the design of actively Q-switched Fe:ZnSe laser.
文摘ZrC nanoparticles in the matrix of Fe were produced by the mechanically activated self-propagating hightemperature method using ZrO2/C/Mg/Fe powder mixtures. The effects of milling time, Fe content, and combustion temperature as well as the formation route for synthesizing ZrC powder particles were studied. The samples were characterized by XRD, SEM, TEM, and DTA. The XRD results revealed that, after 18 h of mechanical activation, ZrO2/ZC/Mg/Fe reacted with the self-propagating combustion(SHS) mode at 870 °C producing the ZrC–Fe nanocomposite. It was also found that both mechanical activation and Fe content played key roles in the ZrC synthesis temperature. With a Fe content of(5–40) wt%, the SHS reaction proceeded favorably and both the ZrC formation temperature and the adiabatic temperature(Tad) decreased. The Mg O content was removed from the final products using a leaching test process by dissolving in hydrochloric and acetic acids.
基金Ministry of Science and Technology of China(Nos.2019YFC1805002 and 2018YFC1802300)National Natural Science Foundation of China(Nos.42177118 and 51779219)+1 种基金Basic Science Center Program for Multiphase Evolution in Hypergravity of the National Natural Science Foundation of China(No.51988101)Overseas Expertise Introduction Center for Discipline Innovation(No.B18047),China.
文摘Identification of chemical oxygen demand(COD)in municipal solid waste(MSW)landfill leachates is a challenging problem.This paper investigated the feasibility of using sodium persulfate(PS),a strong oxidant,as a permeable reactive barrier(PRB)filling material.Firstly,sustained-release persulfate balls were manufactured to adjust the release rate of persulfate,the oxidation agent.In addition,Fe(II)-loaded activated carbon(Fe-AC)was used to help with an even distribution of Fe(II)in the porous medium(PRB in this case).Then,the oxidation efficiency and kinetic rate of COD removal by the sustained-release balls were subjected to batch tests.A mass ratio of 1:1.4:0.24:0.7 for PS:cement:sand:water was the most efficient for COD removal(95%).The breakthrough curve for a 5 mm sustained-release ball revealed that the retardation factor was 1.27 and that the hydrodynamic dispersion coefficient was 15.6 cm^(2)/d.The corresponding half-life of COD oxidation was 0.43 d,which was comparable with the half-life of PS release from sustained-release balls(0.56 d).The sustained-release persulfate balls were shown to be an economical material with a simple recipe and production method when catalyzed by Fe-AC.Compared with cutting-edge methods,sustained-release balls used in PRBs offer significant advantages in terms of both effectiveness and economy for the preparation of sustained-release and catalytic materials.These results verified the feasibility of using sustained-release persulfate balls as a PRB material for COD removal.
基金supported by the National Natural Science Foundation of China (Nos. 21277095, 51478329)the Specialized Research Fund for the Doctoral Program of Higher Education (20130072110026)the Tongji University Open Funding for Materials Characterization (No. 2013080)
文摘Weak magnetic field(WMF) was employed to improve the removal of Cr(VI) by zero-valent iron(ZVI) for the first time. The removal rate of Cr(VI) was elevated by a factor of 1.12-5.89 due to the application of a WMF, and the WMF-induced improvement was more remarkable at higher Cr(VI) concentration and higher p H. Fe2+was not detected until Cr(VI) was exhausted, and there was a positive correlation between the WMF-induced promotion factor of Cr(VI) removal rate and that of Fe2+release rate in the absence of Cr(VI) at pH 4.0-5.5. These phenomena imply that ZVI corrosion with Fe2+release was the limiting step in the process of Cr(VI) removal. The superimposed WMF had negligible influence on the apparent activation energy of Cr(VI) removal by ZVI, indicating that WMF accelerated Cr(VI)removal by ZVI but did not change the mechanism. The passive layer formed with WMF was much more porous than without WMF, thereby facilitating mass transport. Therefore,WMF could accelerate ZVI corrosion and alleviate the detrimental effects of the passive layer, resulting in more rapid removal of Cr(VI) by ZVI. Exploiting the magnetic memory of ZVI, a two-stage process consisting of a small reactor with WMF for ZVI magnetization and a large reactor for removing contaminants by magnetized ZVI can be employed as a new method of ZVI-mediated remediation.