A rational integration of multiple reactive centers into a combined unit to facilitate their cooperative effects is a smart approach for accelerating the catalytic activity.Here,to achieve this goal,linear imidazolium...A rational integration of multiple reactive centers into a combined unit to facilitate their cooperative effects is a smart approach for accelerating the catalytic activity.Here,to achieve this goal,linear imidazolium-based ionic polymers were confined into the nanopores of mesoporous silica nanospheres anchored with homogeneously distributed zinc salts.Owing to the flexible character and the reinforced cooperative effects of the ionic liquid(nucleophile)and zinc species(Lewis acid)in the confined mesoporous structure,the resultant composite exhibited dramatically improved catalytic performance in the cycloaddition of CO2 with epoxides to form cyclic carbonates.This was in contrast to that observed for the individual catalytic components.Moreover,such a solid catalyst could be easily recovered and reused four times without a significant loss of activity.展开更多
Silicon isotope analysis traditionally uses a standard-sample bracketing (SSB) method that relies upon greater instrument stability than can be consistently expected. The following proposed method reduces the level ...Silicon isotope analysis traditionally uses a standard-sample bracketing (SSB) method that relies upon greater instrument stability than can be consistently expected. The following proposed method reduces the level of instrumental stability required for the analysis process and provides a valid solution for high-precision and accurate studies of Si isotopic compositions. Rock samples were dissolved by using alkali fusion and acidification. Silicon isotopes were purified with an ion exchange resin. Interfering peaks for isotopes were separated by using a Nu Plasma 1700 multi-collector inductively coupled plasma mass spectrometry (MS) system in high-resolution mode (M/AM 〉 8000 RP). Two magnesium isotopes (25Mg and 26Mg) and three silicon isotopes (28Si, 29Si, and 3;Si) were analyzed in the same data collection cycle. Mg isotopes were used as an internal standard to calibrate the mass discrimination effects in MS analysis of Si isotopes in combination with the SSB method in order to reduce the effects of MS interference and instrumental mass dis- crimination on the accuracy of measurements. The conventional SSB method without the Mg internal standard and the proposed SSB method with Mg calibration delivered consistent results within two standard deviations. When Mg was used as an internal standard for calibration, the analysis precision was better than 0.05 %0 amu.展开更多
In recent years, the preservation of fruits and vegetables in cold storage has become an issue of increasing concern, ethylene plays a leading role among them. We found ZnO has the effect of degrading gaseous ethylene...In recent years, the preservation of fruits and vegetables in cold storage has become an issue of increasing concern, ethylene plays a leading role among them. We found ZnO has the effect of degrading gaseous ethylene, however its effect is not particularly satisfactory. Therefore, we used simple photo-deposition procedure and low-temperature calcination method to synthesize Au, Ag, and Au Ag alloy supported ZnO to improve the photocatalytic efficiency. Satisfactorily, after ZnO loaded with sole Au or Ag particles, the efficiency of ethylene degradation was 17.5 and 26.8 times than that of pure ZnO, showing a large increase in photocatalytic activity. However, the photocatalytic stability of Ag/ZnO was very poor, because Ag can be easily photooxidized to Ag2O. Surprisingly, when ZnO was successfully loaded with the Au Ag alloy, not only the photocatalytic activity was further improved to 94.8 times than that of pure ZnO, but also the photocatalytic stability was very good after 10 times of cycles. Characterization results explained that the Au-Ag alloy NPs modified ZnO showed great visible-light absorption because of the surface plasmon resonance(SPR) effect. Meanwhile, the higher photocurrent density showed the effective carrier separation ability in Au Ag/ZnO. Therefore, the cooperative action of plasmonic Au Ag bimetallic alloy NPs and efficient carrier separation capability result in the outstanding photoactivity of ethylene oxidation. At the same time, the formation of the alloy produced a new crystal structure different from Au and Ag, which overcomes the problem of poor stability of Ag/ZnO, and finally obtains Au Ag/ZnO photocatalyst with high activity and high stability. This work proposes a new concept of using metal alloys to remove ethylene in actual production.展开更多
Reference materials for quantitative determination of regulated heavy metals, such as Pb and Cd in electronic components, were designed and investigated in terms of stability and homogeneity. Reference materials with ...Reference materials for quantitative determination of regulated heavy metals, such as Pb and Cd in electronic components, were designed and investigated in terms of stability and homogeneity. Reference materials with two concentration levels of heavy metals were prepared by spiking Pb and Cd compounds to epoxy molding compounds made by mixing silica powders and epoxy resin. The concentration changes of the reference materials during stability test for 1 a were not observed. In the homogeneity assessment, the as-prepared reference materials were studied by using three different analytical tools, inductively coupled plasma atomic emission spectrometry (ICP-AES), X-ray fluoroescence spectrometry (XRF) and laser ablation ICP mass. The results show different homogeneities by the characteristics of analytical tools and the materials.展开更多
An in-situ microanalysis of Pb isotopic compositions in sulfide minerals is carried out by using femtosecond laser-ablation multi-collector inductively coupled plasma mass spectrometry (fsLA-MC-ICP-MS). High-tempera...An in-situ microanalysis of Pb isotopic compositions in sulfide minerals is carried out by using femtosecond laser-ablation multi-collector inductively coupled plasma mass spectrometry (fsLA-MC-ICP-MS). High-temperature-activated carbon was used to filter Hg contained in the carrier gas, which reduced the Hg background signal by 48% and also lowered the detection limit of the analysis. Fractionation and mass discrimination effects existing in the ICP-MS analytical processes were corrected using an internal reference T1 in conjunction with an external reference NIST SRM 610. The proposed method was used to an- alyze the Pb isotopic compositions of chalcopyrite, pyrite, and sphalerite from the Dulong Sn-Zn-In polymetallic ore district. The results showed that in this ore district, the sulfide minerals and different grains of the same sulfide mineral show a large variation in Pb content up to 1000-fold. The studied pyrites show relatively higher Pb contents and homogeneous Pb isotopic compositions, whereas the sphalerites have low Pb contents but most variable Pb isotopic compositions. It is suggested that the large variation of Pb isotopic composition may reflect a late hydrothermal superimposition on the primary sulfide formation. In addition, radiogenic Pb accumulated by radioactive decay of trace amounts of U over time in the host minerals may also be one of the causes for the large variation range of Pb content and Pb isotopic composition of those low-Pb sphalerites. Chalcopyrite and sphalerite grains with Pb content greater than 10 ppm presented a consistent Pb isotopic distribution, whereas all the sulfide grains with Pb content greater than 100 ppm had consistent Pb isotopic composition within 2s measurement uncertainties. The in-situ analysis of Pb isotopic composition agreed well with the results obtained by conventional chemical methods within 2s measurement uncertainties, indicating that the data obtained by fsLA-MC-ICP-MS are reliable. Additionally, this study indicates that the Pb isotopic composition could truthfully record the source of ore-forming minerals only for sulfide minerals with high Pb content. On the contrary, the Pb isotopic composition of low-Pb sulfide minerals may be affected by trace amounts of U in the host minerals that may lead to a highly radiogenic Pb isotope ratio. Alternatively, it is also possible that late fluid metasomatic overprinting may alter the Pb isotopic compositions.展开更多
LiNi_(1/3)Co_(1/3)Mn_(1/3)O_2, LiMn_2O_4 and LiCoO_2 are paired to make the blended materials for the cathode of lithium-ion batteries. The factors impacting on the characteristics of blended materials are studied usi...LiNi_(1/3)Co_(1/3)Mn_(1/3)O_2, LiMn_2O_4 and LiCoO_2 are paired to make the blended materials for the cathode of lithium-ion batteries. The factors impacting on the characteristics of blended materials are studied using constant current charge/discharge measurement and electrochemical impedance spectroscopy. The results show that the three pairs of blended materials exhibit very different synergetic effects in high C-rate discharging. The mechanism of particle synergetic effect has a physical root on the compensating material property of blending components, which fundamentally correlates with their similarity and difference in crystalline and electronic structures. The AC impedance show the obvious changes that alternate the high C-rate performance, due to reduced particle impedance in blended materials. The pairs of LiNi_(1/3)Co_(1/3)Mn_(1/3)O_2-LiMn_2O and LiCoO_2-LiMn_2O_4 present obvious increases in high C-rate reversible capacities than does the pair LiCoO_2-LiNi_(1/3)Co_(1/3)Mn_(1/3)O_2.展开更多
The hafnium isotopic analysis using laser ablation has been widely conducted on Hf-rich minerals (zircon/baddeleyite/ calzirtite/eudialyte), however, little work has been reported on Hf-poor (〈100 ppm) minerals. ...The hafnium isotopic analysis using laser ablation has been widely conducted on Hf-rich minerals (zircon/baddeleyite/ calzirtite/eudialyte), however, little work has been reported on Hf-poor (〈100 ppm) minerals. This work presents a detailed procedure of in situ hafnium isotopic analysis from ruffle using laser ablation multiple collector inductively coupled plasma mass spectrometry (LA-MC-ICP-MS). The rutile U-Pb dating reference material JDX shows homogeneous hafnium isotopic ratios, with 176Hf/177Hf=0.281795±0.000015 (2SD, n=33) and176Lu/177Hf=0.000018±0.000004 (2SD, n=17) that suggest the possibility of using JDX as a new reference material hafnium isotopic measurement. We also measure hafnium isotopic compositions of other rutile U-Pb dating reference material (R10, Sugluk-4 and PCA-S207) and the 176Hf/177Hf values are similar to previously reported results, which confirms that we can acquire accurate and precise hafnium isotopic compositions using our developed analytical protocol. We analyzed hafnium isotopic compositions and U-Pb ages of rutile in high-temperature and ultrahigh-temperature granulites from various terrains of the Khondalite Belt from the North China Craton, combined with zircon results in the same area, suggesting that the metamorphic evolution history of the granulite is much more complicated than previously thought.展开更多
基金supported by the National Natural Science Foundation of China(201573136,21603128,U1510105)the Natural Science Foundation for Young Scientists of Shanxi Province(2016021034)the Scientific Research Start-up Funds of Shanxi University(RSC723)~~
文摘A rational integration of multiple reactive centers into a combined unit to facilitate their cooperative effects is a smart approach for accelerating the catalytic activity.Here,to achieve this goal,linear imidazolium-based ionic polymers were confined into the nanopores of mesoporous silica nanospheres anchored with homogeneously distributed zinc salts.Owing to the flexible character and the reinforced cooperative effects of the ionic liquid(nucleophile)and zinc species(Lewis acid)in the confined mesoporous structure,the resultant composite exhibited dramatically improved catalytic performance in the cycloaddition of CO2 with epoxides to form cyclic carbonates.This was in contrast to that observed for the individual catalytic components.Moreover,such a solid catalyst could be easily recovered and reused four times without a significant loss of activity.
基金funded by the National Natural Science Foundation of China(Grant Nos.41427804,41421002,41373004)Beijing SHRIMP Center Open Foundation,and Program for Changjiang Scholars and Innovative Research Team in University(Grant No.IRT1281)the MOST Research Foundation from the State Key Laboratory of Continental Dynamics(BJ08132-1)
文摘Silicon isotope analysis traditionally uses a standard-sample bracketing (SSB) method that relies upon greater instrument stability than can be consistently expected. The following proposed method reduces the level of instrumental stability required for the analysis process and provides a valid solution for high-precision and accurate studies of Si isotopic compositions. Rock samples were dissolved by using alkali fusion and acidification. Silicon isotopes were purified with an ion exchange resin. Interfering peaks for isotopes were separated by using a Nu Plasma 1700 multi-collector inductively coupled plasma mass spectrometry (MS) system in high-resolution mode (M/AM 〉 8000 RP). Two magnesium isotopes (25Mg and 26Mg) and three silicon isotopes (28Si, 29Si, and 3;Si) were analyzed in the same data collection cycle. Mg isotopes were used as an internal standard to calibrate the mass discrimination effects in MS analysis of Si isotopes in combination with the SSB method in order to reduce the effects of MS interference and instrumental mass dis- crimination on the accuracy of measurements. The conventional SSB method without the Mg internal standard and the proposed SSB method with Mg calibration delivered consistent results within two standard deviations. When Mg was used as an internal standard for calibration, the analysis precision was better than 0.05 %0 amu.
文摘In recent years, the preservation of fruits and vegetables in cold storage has become an issue of increasing concern, ethylene plays a leading role among them. We found ZnO has the effect of degrading gaseous ethylene, however its effect is not particularly satisfactory. Therefore, we used simple photo-deposition procedure and low-temperature calcination method to synthesize Au, Ag, and Au Ag alloy supported ZnO to improve the photocatalytic efficiency. Satisfactorily, after ZnO loaded with sole Au or Ag particles, the efficiency of ethylene degradation was 17.5 and 26.8 times than that of pure ZnO, showing a large increase in photocatalytic activity. However, the photocatalytic stability of Ag/ZnO was very poor, because Ag can be easily photooxidized to Ag2O. Surprisingly, when ZnO was successfully loaded with the Au Ag alloy, not only the photocatalytic activity was further improved to 94.8 times than that of pure ZnO, but also the photocatalytic stability was very good after 10 times of cycles. Characterization results explained that the Au-Ag alloy NPs modified ZnO showed great visible-light absorption because of the surface plasmon resonance(SPR) effect. Meanwhile, the higher photocurrent density showed the effective carrier separation ability in Au Ag/ZnO. Therefore, the cooperative action of plasmonic Au Ag bimetallic alloy NPs and efficient carrier separation capability result in the outstanding photoactivity of ethylene oxidation. At the same time, the formation of the alloy produced a new crystal structure different from Au and Ag, which overcomes the problem of poor stability of Ag/ZnO, and finally obtains Au Ag/ZnO photocatalyst with high activity and high stability. This work proposes a new concept of using metal alloys to remove ethylene in actual production.
基金Project(2010-0008-276) supported by NCRC (National Core Research Center) program through the National Research Foundation of Korea funded by the Ministry of Education, Science and Technology
文摘Reference materials for quantitative determination of regulated heavy metals, such as Pb and Cd in electronic components, were designed and investigated in terms of stability and homogeneity. Reference materials with two concentration levels of heavy metals were prepared by spiking Pb and Cd compounds to epoxy molding compounds made by mixing silica powders and epoxy resin. The concentration changes of the reference materials during stability test for 1 a were not observed. In the homogeneity assessment, the as-prepared reference materials were studied by using three different analytical tools, inductively coupled plasma atomic emission spectrometry (ICP-AES), X-ray fluoroescence spectrometry (XRF) and laser ablation ICP mass. The results show different homogeneities by the characteristics of analytical tools and the materials.
基金supported by the National Natural Science Foundation of China(Grant Nos.41427804,41421002,41373004)Program for Changjiang Scholars and Innovative Research Team in University(Grant No.IRT1281)the MOST Research Foundation from the State Key Laboratory of Continental Dynamics(Grant No.BJ08132-1)
文摘An in-situ microanalysis of Pb isotopic compositions in sulfide minerals is carried out by using femtosecond laser-ablation multi-collector inductively coupled plasma mass spectrometry (fsLA-MC-ICP-MS). High-temperature-activated carbon was used to filter Hg contained in the carrier gas, which reduced the Hg background signal by 48% and also lowered the detection limit of the analysis. Fractionation and mass discrimination effects existing in the ICP-MS analytical processes were corrected using an internal reference T1 in conjunction with an external reference NIST SRM 610. The proposed method was used to an- alyze the Pb isotopic compositions of chalcopyrite, pyrite, and sphalerite from the Dulong Sn-Zn-In polymetallic ore district. The results showed that in this ore district, the sulfide minerals and different grains of the same sulfide mineral show a large variation in Pb content up to 1000-fold. The studied pyrites show relatively higher Pb contents and homogeneous Pb isotopic compositions, whereas the sphalerites have low Pb contents but most variable Pb isotopic compositions. It is suggested that the large variation of Pb isotopic composition may reflect a late hydrothermal superimposition on the primary sulfide formation. In addition, radiogenic Pb accumulated by radioactive decay of trace amounts of U over time in the host minerals may also be one of the causes for the large variation range of Pb content and Pb isotopic composition of those low-Pb sphalerites. Chalcopyrite and sphalerite grains with Pb content greater than 10 ppm presented a consistent Pb isotopic distribution, whereas all the sulfide grains with Pb content greater than 100 ppm had consistent Pb isotopic composition within 2s measurement uncertainties. The in-situ analysis of Pb isotopic composition agreed well with the results obtained by conventional chemical methods within 2s measurement uncertainties, indicating that the data obtained by fsLA-MC-ICP-MS are reliable. Additionally, this study indicates that the Pb isotopic composition could truthfully record the source of ore-forming minerals only for sulfide minerals with high Pb content. On the contrary, the Pb isotopic composition of low-Pb sulfide minerals may be affected by trace amounts of U in the host minerals that may lead to a highly radiogenic Pb isotope ratio. Alternatively, it is also possible that late fluid metasomatic overprinting may alter the Pb isotopic compositions.
基金supported by the National Research Program of China (Grant No. 2013AA050901)the National Young Scholar Natural Science Foundation of China (Grant No. 201303235)+3 种基金the Public Projects of Zhejiang Province (Grant No. 2015C31122)Zhejiang Natural Science Foundation(Grant No. LY16B030007)Ningbo Natural Science Foundation (Grant No.2015A610240)Zhejiang Province Key Science and Technology InnovationTeam (Grant No. 2013PT16)
文摘LiNi_(1/3)Co_(1/3)Mn_(1/3)O_2, LiMn_2O_4 and LiCoO_2 are paired to make the blended materials for the cathode of lithium-ion batteries. The factors impacting on the characteristics of blended materials are studied using constant current charge/discharge measurement and electrochemical impedance spectroscopy. The results show that the three pairs of blended materials exhibit very different synergetic effects in high C-rate discharging. The mechanism of particle synergetic effect has a physical root on the compensating material property of blending components, which fundamentally correlates with their similarity and difference in crystalline and electronic structures. The AC impedance show the obvious changes that alternate the high C-rate performance, due to reduced particle impedance in blended materials. The pairs of LiNi_(1/3)Co_(1/3)Mn_(1/3)O_2-LiMn_2O and LiCoO_2-LiMn_2O_4 present obvious increases in high C-rate reversible capacities than does the pair LiCoO_2-LiNi_(1/3)Co_(1/3)Mn_(1/3)O_2.
基金supported by the National Natural Science Foundation of China(Grants Nos.41130313&41525012)
文摘The hafnium isotopic analysis using laser ablation has been widely conducted on Hf-rich minerals (zircon/baddeleyite/ calzirtite/eudialyte), however, little work has been reported on Hf-poor (〈100 ppm) minerals. This work presents a detailed procedure of in situ hafnium isotopic analysis from ruffle using laser ablation multiple collector inductively coupled plasma mass spectrometry (LA-MC-ICP-MS). The rutile U-Pb dating reference material JDX shows homogeneous hafnium isotopic ratios, with 176Hf/177Hf=0.281795±0.000015 (2SD, n=33) and176Lu/177Hf=0.000018±0.000004 (2SD, n=17) that suggest the possibility of using JDX as a new reference material hafnium isotopic measurement. We also measure hafnium isotopic compositions of other rutile U-Pb dating reference material (R10, Sugluk-4 and PCA-S207) and the 176Hf/177Hf values are similar to previously reported results, which confirms that we can acquire accurate and precise hafnium isotopic compositions using our developed analytical protocol. We analyzed hafnium isotopic compositions and U-Pb ages of rutile in high-temperature and ultrahigh-temperature granulites from various terrains of the Khondalite Belt from the North China Craton, combined with zircon results in the same area, suggesting that the metamorphic evolution history of the granulite is much more complicated than previously thought.