The reactions of anionic zirconium oxide clusters ZrxOy- with C2H6 and C4H10 are investi-gated by a time of flight mass spectrometer coupled with a laser vaporization cluster source.Hydrogen containing products Zr2O5H...The reactions of anionic zirconium oxide clusters ZrxOy- with C2H6 and C4H10 are investi-gated by a time of flight mass spectrometer coupled with a laser vaporization cluster source.Hydrogen containing products Zr2O5H- and Zr3O7H- are observed after the reaction. Den-sity functional theory calculations indicate that the hydrogen abstraction is favorable in the reaction of Zr2O5- with C2H6, which supports that the observed Zr2O5H- and Zr3O7H- are due to hydrogen atom abstraction from the alkane molecules. This work shows a newpossible pathway in the reaction of zirconium oxide cluster anions with alkane molecules.展开更多
Objective To evaluate the associations between the serum anion gap （AG） with the severity and prognosis of coronary artery disease （CAD）. Methods We measured serum electrolytes in 18,115 CAD patients indicated by ...Objective To evaluate the associations between the serum anion gap （AG） with the severity and prognosis of coronary artery disease （CAD）. Methods We measured serum electrolytes in 18,115 CAD patients indicated by coronary angiography. The serum AG was calculated according to the equation： AG = Na^＋ [（mmol/L） ＋ K^＋ （mmol/L）] - [Cl^- （mmol/L） ＋ HCO3^- （mmol/L）]. Results A total of 4510 （24.9%） participants had their AG levels greater than 16 mmol/L. The serum AG was independently associated with measures of CAD severity, including more severe clinical types of CAD （P 〈 0.001） and worse cardiac function （P = 0.004）. Patients in the 4th quartile of serum AG （≥ 15.92 mmol/L） had a 5.171-fold increased risk of 30 days all-cause death （P 〈 0.001）. This association was robust, even after adjustment for age, sex, evaluated glomerular filtration rate [hazard ratio （HR）： 4.861, 95% confidence interval （CI）： 2.150–10.993, P 〈 0.001], clinical diagnosis, severity of coronary artery stenosis, cardiac function grades, and other confounders （HR： 3.318, 95% CI： 1.76–2.27, P = 0.009）. Conclusion In this large population-based study, our findings reveal a high percentage of increased serum AG in CAD. Higher AG is associated with more severe clinical types of CAD and worse cardiac function. Furthermore, the increased serum AG is an independent, significant, and strong predictor of all-cause mortality. These findings support a role for the serum AG in the risk-stratification of CAD.展开更多
Dissociation of molecular hydrogen （H2） is extensively studied to understand the mechanism of hydrogenation reactions. In this study, H2 dissociation by Aul-doped closed-shell titanium oxide cluster anions AuTi3O7 a...Dissociation of molecular hydrogen （H2） is extensively studied to understand the mechanism of hydrogenation reactions. In this study, H2 dissociation by Aul-doped closed-shell titanium oxide cluster anions AuTi3O7 and AuTi3O8 has been identified by mass spectrometry and quantum chemistry calculations. The clusters were generated by laser ablation and mass- selected to react with H2 in art ion trap reactor. In the reaction of AuTi3O8 with H2, the ion pair Au＋-O22 rather than Au＋-O2 is the active site to promote H2 dissociation. This finding is in contrast with the previous result that the lattice oxygen is usually the reactive oxygen species in H2 dissociation. The higher reactivity of the peroxide species is further supported by frontier molecular orbital analysis. This study provides new insights into gold catalysis involving H2 activation and dissociation.展开更多
A new method for the determination of Fe by thin layer resin phase spectrophotometry in alkali condition was reported. The complex anion formed by Fe（Ⅱ） and VA was absorbed on the 717w resin and Fe was determined b...A new method for the determination of Fe by thin layer resin phase spectrophotometry in alkali condition was reported. The complex anion formed by Fe（Ⅱ） and VA was absorbed on the 717w resin and Fe was determined by making thin layer. This method had a high sensitivity （ε620= 3.0×10^5L/mol.cm）, which was 15 times higher than that of liquid phase spectrophotometry. It had been proved a satisfactory precision （5.01μg Fe, n=6, RSD=1.8%）. The trace Fe in natural water was determined and the recovery was 97%.展开更多
A cobalt-free perovskite-type Ba0.5Sr0.5A10.1Fe0.9O3-δ （BSAF） chemically studied as solid oxide fuel cell （SOFC） cathode. The ductivity, and electrode polarizations in symmetrical cell based is developed and elec...A cobalt-free perovskite-type Ba0.5Sr0.5A10.1Fe0.9O3-δ （BSAF） chemically studied as solid oxide fuel cell （SOFC） cathode. The ductivity, and electrode polarizations in symmetrical cell based is developed and electro- structures, electrical con- on mixed ion conducting electrolyte were investigated, respectively. The temperature dependence of conductivity of BSAF in air shows a typical semiconductor behavior with positive temperature coefficient up to 450℃ where the conductivity reaches 14.0 S/cm while above this temperature the negative temperature coefficient dominates the total conductivity. Electrochemical charac- terizations show desirable polarization resistance of BSAF cathode in a symmetric cell based on mixed ion conducting electrolyte at 650-700℃, A single SOFC with BSAF cathode shows OCV of 1.0 V and maximum output of 420 mW/cm2 at 700 ℃ with humidified hydrogen fuel and static air oxidant.展开更多
The structural changes of silicate anions in the desilication process with the addition of calcium hydrate alumino-carbonate were studied by measuring Raman spectra, infrared spectra and corresponding second derivativ...The structural changes of silicate anions in the desilication process with the addition of calcium hydrate alumino-carbonate were studied by measuring Raman spectra, infrared spectra and corresponding second derivative spectra. The results show that the desilication ratio in the solution prepared by the addition of sodium silicate(solution-SS) is much greater than that in the solution by the addition of green liquor(solution-GL), and low alumina concentration in the sodium aluminate solutions facilitates the desilication process. It is also shown that alumino-silicate anions in the solution-GL, and Q^3 polymeric silicate anions in solution-SS are predominant, respectively. In addition, increasing the concentration of silica favors respectively the formation of the alumino-silicate or the Q^3 silicate anions in the solution-GL or the solution-SS. Therefore, it can be inferred that the low desilication ratio in the silicate-bearing aluminate solution is mainly attributed to the existence of alumino-silicate anions.展开更多
Micellar enhanced ultrafiltration （MEUF） is a new effective treatment technology for the filtration removal of organic pollutants through solubilization. The present paper is aimed to study the solubilization of org...Micellar enhanced ultrafiltration （MEUF） is a new effective treatment technology for the filtration removal of organic pollutants through solubilization. The present paper is aimed to study the solubilization of organic compounds such as chlorobenzene （CB）, pyrene and phenol by anionic, cationic and mixed anionic-nonionic surfactants such as sodium dodecyl sulfate （SDS）, cetyltrimethylammonium bromide （CTMAB） and Tween-80 （TW80） and the mixed SDS-TW80 with a batch equilibrium method. This study enables us to supply deeper investigation for MEUF. The results showed that solubilization capacity was not obvious below the critical micellar concentration （CMC）. The apparent solubilities of organic compounds were linearly related to surfactant concentrations over their CMCs. Solubilization capacity by single surfactants follow the order of TW80 〉 CTMAB 〉 SDS. The results also proved that the solubilization of the organic contaminants by the mixed surfactants can significantly be enhanced compared with the single anionic surfactant SDS. Whereas the CMC can be decreased, the solubility can be increased as long as the mass ratio of nonionic surfactant increases. The solubility enhancement efficiency of the different organic compounds follow the order of phenol 〉 CB 〉 pyrene. In addition, the solubilization ratio appears to be positively relative to the intrinsic water solubility of the organic contaminants and negatively correlates to octanol-water coefficients （Kow） of organic compounds and the hydrophile-lypophile balance values （HLB） of the surfactants.展开更多
Strongly acidic soils （pH 〈 5.0） are detrimental to tea （Camellia sinensis） production and quality. Little information exists on the ability of surface amendments to ameliorate subsoil acidity in the tea garden s...Strongly acidic soils （pH 〈 5.0） are detrimental to tea （Camellia sinensis） production and quality. Little information exists on the ability of surface amendments to ameliorate subsoil acidity in the tea garden soils. A 120-d glasshouse column leaching experiment was conducted using commonly available soil ameliorants. Alkaline slag （AS） and organic residues, pig manure （PM） and rapeseed cake （RC） differing in ash alkalinity and C/N ratio were incorporated alone and in combination into the surface （0-15 cm） of soil columns （10 cm internal diameter x 50 cm long） packed with soil from the acidic soil layer （15-30 cm） of an Ultisol （initial pH -- 4.4）. During the 120-d experiment, the soil columns were watered （about 127 mm over 9 applications） according to the long-term mean annual rainfall （1 143 mm） and the leachates were collected and analyzed. At the end of the experiment, soil columns were partitioned into various depths and the chemical properties of soil were measured. The PM with a higher C/N ratio increased subsoil pH, whereas the RC with a lower C/N ratio decreased subsoil pH. However, combined amendments had a greater ability to reduce subsoil acidity than either of the amendments alone. The increases in pH of the subsoil were mainly ascribed to decreased base cation concentrations and the decomposition of organic anions present in dissolved organic carbon （DOC） and immobilization of nitrate that had been leached down from the amended layer. A significant （P 〈 0.05） correlation between alkalinity production （reduced exchangeable acidity - N-cycle alkalinity） and alkalinity balance （net alkalinity production - N-cycle alkalinity） was observed at the end of the experiment. Additionally, combined amendments significantly increased （P ~ 0.05） subsoil cation concentrations and decreased subsoil A1 saturation （P 〈 0.05）. Combined applications of AS with organic amendments to surface soils are effective in reducing subsoil acidity in high-rainfall areas. Further investigations under field conditions and over longer timeframes are needed to fully understand their practical effectiveness in ameliorating acidity of deeper soil layers under naturally occurring leaching regimes.展开更多
In recent years, a great deal of interest has been focused on nitrogen-containing extractants for the separation of actinides from lanthanides. In this study, we synthesized a polyazamacrocycle-type C8-cyclen ligand c...In recent years, a great deal of interest has been focused on nitrogen-containing extractants for the separation of actinides from lanthanides. In this study, we synthesized a polyazamacrocycle-type C8-cyclen ligand comprising four tertiary alkyl amino groups, for the extraction of Am3+ and Eu3+. The C8-cyclen demonstrated a weak ability to extract and separate Am3+ and Eu3+ that increased with the increasing "softness" of the aqueous anions. The extraction behavior of Am3+ and Eu3+ indicated coordination interactions between the C8-cyclen and the Am3+ and Eu3+ ions. The suppression of Am3+ or Eu3+ extraction by acid depended on the media anions involved.展开更多
基金This work was supported by the Chinese Academy of Sciences （Hundred Talents Fund）, the National Natural Science Foundation of China （No.20703048 and No.20803083）, and the Center of Molecular Science Foundation of Institute of Chemistry, Chinese Academy of Sciences （No.CMS-LX200902）.
文摘The reactions of anionic zirconium oxide clusters ZrxOy- with C2H6 and C4H10 are investi-gated by a time of flight mass spectrometer coupled with a laser vaporization cluster source.Hydrogen containing products Zr2O5H- and Zr3O7H- are observed after the reaction. Den-sity functional theory calculations indicate that the hydrogen abstraction is favorable in the reaction of Zr2O5- with C2H6, which supports that the observed Zr2O5H- and Zr3O7H- are due to hydrogen atom abstraction from the alkane molecules. This work shows a newpossible pathway in the reaction of zirconium oxide cluster anions with alkane molecules.
基金Acknowledgement This work was supported by the Beijing Nova Program （No. Z121107002512053）, the Beijing Health System High Level Health Technology Talent Cultivation Plan （No. 2013-3-013）, the Beijing Outstanding Talent Training Program （No. 2014000021223ZK32）, and the National Natural Science Foundation of China （No. 81100143） to S.W.Y., and the Beijing Municipal Administration of Hospitals Clinical Medicine Development of Special Funding Support （No. ZYLX201303） to Y.J.Z.
文摘Objective To evaluate the associations between the serum anion gap （AG） with the severity and prognosis of coronary artery disease （CAD）. Methods We measured serum electrolytes in 18,115 CAD patients indicated by coronary angiography. The serum AG was calculated according to the equation： AG = Na^＋ [（mmol/L） ＋ K^＋ （mmol/L）] - [Cl^- （mmol/L） ＋ HCO3^- （mmol/L）]. Results A total of 4510 （24.9%） participants had their AG levels greater than 16 mmol/L. The serum AG was independently associated with measures of CAD severity, including more severe clinical types of CAD （P 〈 0.001） and worse cardiac function （P = 0.004）. Patients in the 4th quartile of serum AG （≥ 15.92 mmol/L） had a 5.171-fold increased risk of 30 days all-cause death （P 〈 0.001）. This association was robust, even after adjustment for age, sex, evaluated glomerular filtration rate [hazard ratio （HR）： 4.861, 95% confidence interval （CI）： 2.150–10.993, P 〈 0.001], clinical diagnosis, severity of coronary artery stenosis, cardiac function grades, and other confounders （HR： 3.318, 95% CI： 1.76–2.27, P = 0.009）. Conclusion In this large population-based study, our findings reveal a high percentage of increased serum AG in CAD. Higher AG is associated with more severe clinical types of CAD and worse cardiac function. Furthermore, the increased serum AG is an independent, significant, and strong predictor of all-cause mortality. These findings support a role for the serum AG in the risk-stratification of CAD.
基金supported by the National Natural Science Foundation of China(No.21573246,No.21773253,and No.21773254)the Beijing Natural Science Foundation(2172059)the Youth Innovation Promotion Association,Chinese Academy of Sciences(2016030)
文摘Dissociation of molecular hydrogen （H2） is extensively studied to understand the mechanism of hydrogenation reactions. In this study, H2 dissociation by Aul-doped closed-shell titanium oxide cluster anions AuTi3O7 and AuTi3O8 has been identified by mass spectrometry and quantum chemistry calculations. The clusters were generated by laser ablation and mass- selected to react with H2 in art ion trap reactor. In the reaction of AuTi3O8 with H2, the ion pair Au＋-O22 rather than Au＋-O2 is the active site to promote H2 dissociation. This finding is in contrast with the previous result that the lattice oxygen is usually the reactive oxygen species in H2 dissociation. The higher reactivity of the peroxide species is further supported by frontier molecular orbital analysis. This study provides new insights into gold catalysis involving H2 activation and dissociation.
文摘A new method for the determination of Fe by thin layer resin phase spectrophotometry in alkali condition was reported. The complex anion formed by Fe（Ⅱ） and VA was absorbed on the 717w resin and Fe was determined by making thin layer. This method had a high sensitivity （ε620= 3.0×10^5L/mol.cm）, which was 15 times higher than that of liquid phase spectrophotometry. It had been proved a satisfactory precision （5.01μg Fe, n=6, RSD=1.8%）. The trace Fe in natural water was determined and the recovery was 97%.
文摘A cobalt-free perovskite-type Ba0.5Sr0.5A10.1Fe0.9O3-δ （BSAF） chemically studied as solid oxide fuel cell （SOFC） cathode. The ductivity, and electrode polarizations in symmetrical cell based is developed and electro- structures, electrical con- on mixed ion conducting electrolyte were investigated, respectively. The temperature dependence of conductivity of BSAF in air shows a typical semiconductor behavior with positive temperature coefficient up to 450℃ where the conductivity reaches 14.0 S/cm while above this temperature the negative temperature coefficient dominates the total conductivity. Electrochemical charac- terizations show desirable polarization resistance of BSAF cathode in a symmetric cell based on mixed ion conducting electrolyte at 650-700℃, A single SOFC with BSAF cathode shows OCV of 1.0 V and maximum output of 420 mW/cm2 at 700 ℃ with humidified hydrogen fuel and static air oxidant.
基金Project(51274242)supported by the National Natural Science Foundation of ChinaProject(2015CX001)supported by the Innovation-driven Plan in Central South University,China
文摘The structural changes of silicate anions in the desilication process with the addition of calcium hydrate alumino-carbonate were studied by measuring Raman spectra, infrared spectra and corresponding second derivative spectra. The results show that the desilication ratio in the solution prepared by the addition of sodium silicate(solution-SS) is much greater than that in the solution by the addition of green liquor(solution-GL), and low alumina concentration in the sodium aluminate solutions facilitates the desilication process. It is also shown that alumino-silicate anions in the solution-GL, and Q^3 polymeric silicate anions in solution-SS are predominant, respectively. In addition, increasing the concentration of silica favors respectively the formation of the alumino-silicate or the Q^3 silicate anions in the solution-GL or the solution-SS. Therefore, it can be inferred that the low desilication ratio in the silicate-bearing aluminate solution is mainly attributed to the existence of alumino-silicate anions.
文摘Micellar enhanced ultrafiltration （MEUF） is a new effective treatment technology for the filtration removal of organic pollutants through solubilization. The present paper is aimed to study the solubilization of organic compounds such as chlorobenzene （CB）, pyrene and phenol by anionic, cationic and mixed anionic-nonionic surfactants such as sodium dodecyl sulfate （SDS）, cetyltrimethylammonium bromide （CTMAB） and Tween-80 （TW80） and the mixed SDS-TW80 with a batch equilibrium method. This study enables us to supply deeper investigation for MEUF. The results showed that solubilization capacity was not obvious below the critical micellar concentration （CMC）. The apparent solubilities of organic compounds were linearly related to surfactant concentrations over their CMCs. Solubilization capacity by single surfactants follow the order of TW80 〉 CTMAB 〉 SDS. The results also proved that the solubilization of the organic contaminants by the mixed surfactants can significantly be enhanced compared with the single anionic surfactant SDS. Whereas the CMC can be decreased, the solubility can be increased as long as the mass ratio of nonionic surfactant increases. The solubility enhancement efficiency of the different organic compounds follow the order of phenol 〉 CB 〉 pyrene. In addition, the solubilization ratio appears to be positively relative to the intrinsic water solubility of the organic contaminants and negatively correlates to octanol-water coefficients （Kow） of organic compounds and the hydrophile-lypophile balance values （HLB） of the surfactants.
基金This study was supported by the National Natural Science Foundation of China （No. 41401336）, the Na- tural Science Foundation of Jiangsu Province, China （No. BK20130105）, the State Key Laboratory of Soil and Sustainable Agriculture, Chinese Academy of Sci-ence （No. Y412201452）, and the Environmental Pro- tection Public Benefit Research Foundation of China （No. 201309036）. We thank the three anonymous refe- rees for their helpful comments.
文摘Strongly acidic soils （pH 〈 5.0） are detrimental to tea （Camellia sinensis） production and quality. Little information exists on the ability of surface amendments to ameliorate subsoil acidity in the tea garden soils. A 120-d glasshouse column leaching experiment was conducted using commonly available soil ameliorants. Alkaline slag （AS） and organic residues, pig manure （PM） and rapeseed cake （RC） differing in ash alkalinity and C/N ratio were incorporated alone and in combination into the surface （0-15 cm） of soil columns （10 cm internal diameter x 50 cm long） packed with soil from the acidic soil layer （15-30 cm） of an Ultisol （initial pH -- 4.4）. During the 120-d experiment, the soil columns were watered （about 127 mm over 9 applications） according to the long-term mean annual rainfall （1 143 mm） and the leachates were collected and analyzed. At the end of the experiment, soil columns were partitioned into various depths and the chemical properties of soil were measured. The PM with a higher C/N ratio increased subsoil pH, whereas the RC with a lower C/N ratio decreased subsoil pH. However, combined amendments had a greater ability to reduce subsoil acidity than either of the amendments alone. The increases in pH of the subsoil were mainly ascribed to decreased base cation concentrations and the decomposition of organic anions present in dissolved organic carbon （DOC） and immobilization of nitrate that had been leached down from the amended layer. A significant （P 〈 0.05） correlation between alkalinity production （reduced exchangeable acidity - N-cycle alkalinity） and alkalinity balance （net alkalinity production - N-cycle alkalinity） was observed at the end of the experiment. Additionally, combined amendments significantly increased （P ~ 0.05） subsoil cation concentrations and decreased subsoil A1 saturation （P 〈 0.05）. Combined applications of AS with organic amendments to surface soils are effective in reducing subsoil acidity in high-rainfall areas. Further investigations under field conditions and over longer timeframes are needed to fully understand their practical effectiveness in ameliorating acidity of deeper soil layers under naturally occurring leaching regimes.
基金supported by the National Natural Science Foundation of China(91226110)the Program for Changjiang Scholars and Innovative Research Team in University
文摘In recent years, a great deal of interest has been focused on nitrogen-containing extractants for the separation of actinides from lanthanides. In this study, we synthesized a polyazamacrocycle-type C8-cyclen ligand comprising four tertiary alkyl amino groups, for the extraction of Am3+ and Eu3+. The C8-cyclen demonstrated a weak ability to extract and separate Am3+ and Eu3+ that increased with the increasing "softness" of the aqueous anions. The extraction behavior of Am3+ and Eu3+ indicated coordination interactions between the C8-cyclen and the Am3+ and Eu3+ ions. The suppression of Am3+ or Eu3+ extraction by acid depended on the media anions involved.
