A series of(Ce,Cr)xO2/Nb2O5 catalysts with different(Ce,Cr)xO2 to Nb2O5 mass ratios were synthesized by the deposition-precipitation method for use in deep catalytic oxidation of 1,2-dichloroethane(DCE), which is one ...A series of(Ce,Cr)xO2/Nb2O5 catalysts with different(Ce,Cr)xO2 to Nb2O5 mass ratios were synthesized by the deposition-precipitation method for use in deep catalytic oxidation of 1,2-dichloroethane(DCE), which is one of the typical chlorinated volatile organic compound pollutants. The textural properties were characterized by X-ray diffraction, N2 adsorption/desorption isotherms, UV-Raman spectroscopy, and scanning electron microscopy. The surface acidity and the redox properties were characterized by ammonia temperature-programmed desorption and H2 temperature-programmed reduction, respectively. The results show that the addition of a proper amount of(Ce,Cr)xO2 over Nb2O5 significantly improves the intrinsic catalytic activity towards the deep oxidation of DCE, and only a very small amount of C2H3Cl is detected as the byproduct of the oxidation process. Further study reveals the existence of an obvious synergistic effect between Nb2O5, with abundant strong acid sites, and(Ce,Cr)xO2, with strong oxidation sites, as the strong acid sites of Nb2O5 promote the adsorption and dehydrochlorination of DCE, while the strong oxidation sites of(Ce,Cr)xO2 contribute to the deep oxidation of the reactant, intermediates, and byproducts.展开更多
An idea on interfacial equilibrium-potential differences () which are generated for the extraction of univalent metal picrate (MPic) and divalent ones (MPic2) by crown ethers (L) into high-polar diluents was improved....An idea on interfacial equilibrium-potential differences () which are generated for the extraction of univalent metal picrate (MPic) and divalent ones (MPic2) by crown ethers (L) into high-polar diluents was improved. These potentials were clarified with some experimental extraction-data reported before on the M = Ag(I), Ca(II), Sr(II) and Ba(II) extraction with 18-crown-6 ether (18C6) and benzo-18C6 into 1,2-dichloroethane (DCE) and nitrobenzene (NB). Consequently, it was demonstrated that the? values from the extraction-experimentally obtained logKD,Pic ones are in agreement with or close to those calculated from charge balance equations in many cases, where the symbol, KD,Pic, denotes an individual distribution constant of Pic﹣ into the DCE or NB phase. Also, it was experimentally shown that extraction constants based on the overall extraction equilibria do not virtually contain the? terms in their functional expressions.展开更多
HZSM-5, Al_2O_3, TiO_2 and SiO_2 supported CeO_2-ZrO_2-CrO_x catalysts were prepared by deposition-precipitation method and tested for deep catalytic oxidation of 1,2-dichloroethane（DCE）, as one of the common chlori...HZSM-5, Al_2O_3, TiO_2 and SiO_2 supported CeO_2-ZrO_2-CrO_x catalysts were prepared by deposition-precipitation method and tested for deep catalytic oxidation of 1,2-dichloroethane（DCE）, as one of the common chlorinated organic pollutants. All the catalysts were characterized by means of N_2 adsorption-desorption, X-ray photoelectron spectroscopy（XPS）, ammonia-temperatureprogrammed desorption（NH_3-TPD） and hydrogen temperature-programmed reduction（H2-TPR）. The characterization results revealed that there was strongly synergistic effect between the oxidizability of CZCr species and the acidity of supports, which obviously promoted the catalytic activity for DCE degradation. 20% CZCr/HZSM-5 showed the highest activity and good durability during the long-term continuous test. The catalytic activity decreased in the order： 20%CZCr/HZSM-5〉CZCr〉20%CZCr/TiO_2〉20%CZCr/Al_2O_3〉20%CZCr/SiO_2.展开更多
The electrochemical behavior of ionizable drugs (Amitriptyline, Diphenhydramine and Trihexyphene- dyl) at the water/1,2-dichloroethane interface with the phase volume ratio (r = Vo/Vw) equal to 1 are investigated by c...The electrochemical behavior of ionizable drugs (Amitriptyline, Diphenhydramine and Trihexyphene- dyl) at the water/1,2-dichloroethane interface with the phase volume ratio (r = Vo/Vw) equal to 1 are investigated by cyclic voltammetry. The system is composed of an aqueous droplet supported at an Ag/AgCl disk electrode and it was covered with an organic solution. In this manner, a conventional three-electrode potentiostat can be used to study the ioni-zable drugs transfer process at a liquid/liquid interface. Physicochemical parameters such as the formal transfer potential, the Gibbs energy of transfer and the standard par-tition coefficients of the ionized forms of these drugs can be evaluated from cyclic voltammograms obtained. The ob-tained results have been summarized in ionic partition dia-grams, which are a useful tool for predicting and interpret-ing the transfer mechanisms of ionizable drugs at the liq-uid/liquid interfaces and biological membranes.展开更多
The faradaic ion transfer of protonated 1,10-phenanthrolino [H(Phen)^+] across the interface between unbuffered aqueous and 1,2-dichloroethane(DCE)solutions was inves- tigated by means of current scan polarography at ...The faradaic ion transfer of protonated 1,10-phenanthrolino [H(Phen)^+] across the interface between unbuffered aqueous and 1,2-dichloroethane(DCE)solutions was inves- tigated by means of current scan polarography at ascending aqueous electrolyte electrode, as well as chronopotentiometry.It follows from the splitting of the waves observed at the pH of aqueous phase(sodium sulfate solution)between 2.5—3.8 that neutral reagent(Phen) distributes into the aqueous phase,where it is protonated.The positive wave is associated with the mass transfer controlled by the H^+ influx,whereas the negative one is by the Phen influx.The reverse chronopotentiometry indicated that all the protonated transfer processes were reversible.A good agreement between experimental results and theoretical treatment was achieved.The aqueous acid dissociation constant of protonated Phen,K_a,can be evalu- ated from the dependence of the wave heights on the pH in the base of the equilibrium.展开更多
基金supported by the National Key R&D Program of China(2016YFC0204300)the National Natural Science Foundation of China(21477109)~~
文摘A series of(Ce,Cr)xO2/Nb2O5 catalysts with different(Ce,Cr)xO2 to Nb2O5 mass ratios were synthesized by the deposition-precipitation method for use in deep catalytic oxidation of 1,2-dichloroethane(DCE), which is one of the typical chlorinated volatile organic compound pollutants. The textural properties were characterized by X-ray diffraction, N2 adsorption/desorption isotherms, UV-Raman spectroscopy, and scanning electron microscopy. The surface acidity and the redox properties were characterized by ammonia temperature-programmed desorption and H2 temperature-programmed reduction, respectively. The results show that the addition of a proper amount of(Ce,Cr)xO2 over Nb2O5 significantly improves the intrinsic catalytic activity towards the deep oxidation of DCE, and only a very small amount of C2H3Cl is detected as the byproduct of the oxidation process. Further study reveals the existence of an obvious synergistic effect between Nb2O5, with abundant strong acid sites, and(Ce,Cr)xO2, with strong oxidation sites, as the strong acid sites of Nb2O5 promote the adsorption and dehydrochlorination of DCE, while the strong oxidation sites of(Ce,Cr)xO2 contribute to the deep oxidation of the reactant, intermediates, and byproducts.
文摘An idea on interfacial equilibrium-potential differences () which are generated for the extraction of univalent metal picrate (MPic) and divalent ones (MPic2) by crown ethers (L) into high-polar diluents was improved. These potentials were clarified with some experimental extraction-data reported before on the M = Ag(I), Ca(II), Sr(II) and Ba(II) extraction with 18-crown-6 ether (18C6) and benzo-18C6 into 1,2-dichloroethane (DCE) and nitrobenzene (NB). Consequently, it was demonstrated that the? values from the extraction-experimentally obtained logKD,Pic ones are in agreement with or close to those calculated from charge balance equations in many cases, where the symbol, KD,Pic, denotes an individual distribution constant of Pic﹣ into the DCE or NB phase. Also, it was experimentally shown that extraction constants based on the overall extraction equilibria do not virtually contain the? terms in their functional expressions.
基金Project supports from National Nature Science Foundation of China(21177110)
文摘HZSM-5, Al_2O_3, TiO_2 and SiO_2 supported CeO_2-ZrO_2-CrO_x catalysts were prepared by deposition-precipitation method and tested for deep catalytic oxidation of 1,2-dichloroethane（DCE）, as one of the common chlorinated organic pollutants. All the catalysts were characterized by means of N_2 adsorption-desorption, X-ray photoelectron spectroscopy（XPS）, ammonia-temperatureprogrammed desorption（NH_3-TPD） and hydrogen temperature-programmed reduction（H2-TPR）. The characterization results revealed that there was strongly synergistic effect between the oxidizability of CZCr species and the acidity of supports, which obviously promoted the catalytic activity for DCE degradation. 20% CZCr/HZSM-5 showed the highest activity and good durability during the long-term continuous test. The catalytic activity decreased in the order： 20%CZCr/HZSM-5〉CZCr〉20%CZCr/TiO_2〉20%CZCr/Al_2O_3〉20%CZCr/SiO_2.
文摘The electrochemical behavior of ionizable drugs (Amitriptyline, Diphenhydramine and Trihexyphene- dyl) at the water/1,2-dichloroethane interface with the phase volume ratio (r = Vo/Vw) equal to 1 are investigated by cyclic voltammetry. The system is composed of an aqueous droplet supported at an Ag/AgCl disk electrode and it was covered with an organic solution. In this manner, a conventional three-electrode potentiostat can be used to study the ioni-zable drugs transfer process at a liquid/liquid interface. Physicochemical parameters such as the formal transfer potential, the Gibbs energy of transfer and the standard par-tition coefficients of the ionized forms of these drugs can be evaluated from cyclic voltammograms obtained. The ob-tained results have been summarized in ionic partition dia-grams, which are a useful tool for predicting and interpret-ing the transfer mechanisms of ionizable drugs at the liq-uid/liquid interfaces and biological membranes.
基金Project supported by the National Natural Science Foundation of China.
文摘The faradaic ion transfer of protonated 1,10-phenanthrolino [H(Phen)^+] across the interface between unbuffered aqueous and 1,2-dichloroethane(DCE)solutions was inves- tigated by means of current scan polarography at ascending aqueous electrolyte electrode, as well as chronopotentiometry.It follows from the splitting of the waves observed at the pH of aqueous phase(sodium sulfate solution)between 2.5—3.8 that neutral reagent(Phen) distributes into the aqueous phase,where it is protonated.The positive wave is associated with the mass transfer controlled by the H^+ influx,whereas the negative one is by the Phen influx.The reverse chronopotentiometry indicated that all the protonated transfer processes were reversible.A good agreement between experimental results and theoretical treatment was achieved.The aqueous acid dissociation constant of protonated Phen,K_a,can be evalu- ated from the dependence of the wave heights on the pH in the base of the equilibrium.
