In this paper, methane coupling at ambient temperature, under atmospheric pressure and in the presence of hydrogen was firstly investigated by using pulse corona plasma and Pt/g-Al2O3 catalyst. Experimental results s...In this paper, methane coupling at ambient temperature, under atmospheric pressure and in the presence of hydrogen was firstly investigated by using pulse corona plasma and Pt/g-Al2O3 catalyst. Experimental results showed that Pt/g-Al2O3 catalyst has catalytic activity for methane coupling to C2H4. Over sixty percent of outcomes of C2 hydrocarbons were detected to be ethylene.展开更多
The catalytic performance of oxidative coupling of methane(OCM) over Eu 2O 3 catalysts promoted by alkaline earth fluorides was studied The results showed that C 2 hydrocarbon selectivity and yield over the fluor...The catalytic performance of oxidative coupling of methane(OCM) over Eu 2O 3 catalysts promoted by alkaline earth fluorides was studied The results showed that C 2 hydrocarbon selectivity and yield over the fluoride promoted Eu 2O 3 catalysts were apparently higher than those over pure Eu 2O 3; the OCM performance increased according to the sequence of CaF 2 Eu 2O 3≈BaF 2 Eu 2O 3<SrF 2 Eu 2O 3 under the same conditions XRD experiment indicated that rhombohedral EuOF phase formed in the fresh BaF 2 Eu 2O 3 catalyst, while the exchange of F - and O 2- did not apparently happen in the fresh CaF 2 Eu 2O 3 and SrF 2 Eu 2O 3 catalysts Pyridine TPD and CO 2 TPD measurements found that, after adding SrF 2 to Eu 2O 3, the catalyst surface acidity decreased, whereas the surface basic strength increased slightly, resulting in an improvement in C 2 selectivity and yield展开更多
The oxidation of 2-naphthol and 2-naphthalenethiol to 1,1'-bi-2-naphthol and bis-2-naphthyl disulfide respectively has been carried out in excellent yields in solid state in the presence of Fe3+-montmorillonite or...The oxidation of 2-naphthol and 2-naphthalenethiol to 1,1'-bi-2-naphthol and bis-2-naphthyl disulfide respectively has been carried out in excellent yields in solid state in the presence of Fe3+-montmorillonite or alumina-supported FeCl3.展开更多
The dehydrogenation of isobutane （IB） to produce isobutene coupled with reverse water gas shift in the presence of carbon dioxide was investigated over the catalyst Cr2O3 supported on active carbon （Cr2O3/AC）. The...The dehydrogenation of isobutane （IB） to produce isobutene coupled with reverse water gas shift in the presence of carbon dioxide was investigated over the catalyst Cr2O3 supported on active carbon （Cr2O3/AC）. The results illustrated that isobutane conversion and isobutene yield can be enhanced through the reaction coupling in the presence of carbon dioxide. Moreover, carbon dioxide can partially eliminate carbonaceous deposition on the catalyst and keep the active phase （Cr2O3）, which are then helpful to alleviate the catalyst deactivation.展开更多
Herein,a bottom-down design is presented to successfully fabricate ZIF-derived Co3O4,grown in situ on a one-dimensional(1D)α-MnO2 material,denoted as α-MnO2@Co3O4.The synergistic effect derived from the coupled inte...Herein,a bottom-down design is presented to successfully fabricate ZIF-derived Co3O4,grown in situ on a one-dimensional(1D)α-MnO2 material,denoted as α-MnO2@Co3O4.The synergistic effect derived from the coupled interface constructed betweenα-MnO2 and Co3O4 is responsible for the enhanced catalytic activity.The resultantα-MnO2@Co3O4 catalyst exhibits excellent catalytic activity at a T90%(temperature required to achieve a toluene conversion of 90%)of approximately 229℃,which is 47 and 28℃ lower than those of the pureα-MnO2 nanowire and Co3O4-b obtained via pyrolysis of ZIF-67,respectively.This activity is attributed to the increase in the number of surface-adsorbed oxygen species,which accelerate the oxygen mobility and enhance the redox pairs of Mn^4+/Mn^3+ and Co^2+/Co^3+.Moreover,the result of in situ diffuse reflectance infrared Fourier transform spectroscopy suggests that the gaseous oxygen could be more easily activated to adsorbed oxygen species on the surface of α-MnO2@Co3O4 than on that of α-MnO2.The catalytic reaction route of toluene oxidation over theα-MnO2@Co3O4 catalyst is as follows:toluene→benzoate species→alkanes containing oxygen functional group→CO2 and H2O.In addition,the α-MnO2@Co3O4 catalyst shows excellent stability and good water resistance for toluene oxidation.Furthermore,the preparation method can be extended to other 1D MnO2 materials.A new strategy for the development of high-performance catalysts of practical significance is provided.展开更多
Thermodynamic models of calculating mass action concentrations for structural units or ion couples in RbCl-H2O binary and RbCl-RbNO3-H2O ternary strong electrolyte aqueous solutions were developed based on the ion and...Thermodynamic models of calculating mass action concentrations for structural units or ion couples in RbCl-H2O binary and RbCl-RbNO3-H2O ternary strong electrolyte aqueous solutions were developed based on the ion and molecule coexistence theory at 298.15 K.A transformation coefficient is needed to compare the calculated mass action concentration and the reported activity because they are obtained at different standard states and concentration units.The results show that the transformation coefficients between the calculated mass action concentrations and the reported activities of the same structural units or ion couples in RbCl-H2O binary and RbCl-RbNO3-H2O ternary strong electrolyte aqueous solutions change in a very narrow range.The transformed mass action concentrations of structural units or ion couples in RbCl-H2O binary system are in good agreement with the reported activities. The transformed mass action concentrations of RbCl and RbNO3 in RbCl-RbNO3-H2O ternary solution are also in good agreement with the reported activities,aRbCl and 3RbNOa,with different total ionic strengths as 0.01,0.05,0.1,0.5,1.0,1.5,2.0,3.0 and 3.5 mol/kg,respectively.All those results mean the developed thermodynamic model of strong electrolyte aqueous solutions can reflect structural characteristics of RbCl-H2O binary and RbCl-RbNO3-H2O ternary strong electrolyte aqueous solutions and the mass action concentration also strictly follows the mass action law.展开更多
Vapor phase catalytic hydrogen peroxide production by oxidation of water is possible by coupling the reaction with oxidation of an organic sacrificial reductant. It is potentially a safer process than direct synthesis...Vapor phase catalytic hydrogen peroxide production by oxidation of water is possible by coupling the reaction with oxidation of an organic sacrificial reductant. It is potentially a safer process than direct synthesis from H2 and O2. Based on mechanistic information available mostly for liquid phase catalytic processes, feasible reaction mechanisms for such coupled reactions are proposed based on which desirable catalyst properties are identified. It is found that the surface-adsorbed oxygen bond is an important parameter for identifying desirable catalysts. Thermodynamics can be used to identify the types of organic oxidation reactions that can couple with water oxidation such that H2O2 formation becomes thermodynamically favorable. Reactions such as epoxidation of alkenes and selective oxidation of alkanes to alcohols cannot provide sufficient thermodynamic driving force, whereas oxidation of alcohols to aldehydes and to acids can. Finally, further research is suggested to identify catalytic properties important for H2O2 decomposition and for coupling selective oxidation of organic compounds to oxidation of H2O in order to facilitate development of H2O2 production coupled with selective organic oxidation.展开更多
The 0.8Pb(Zr0.48Ti0.52)O3 – 0.125Pb(Zn1/3Nb2/3)O3 – 0.075Pb(Mn1/3Nb2/3)O3 + x wt% Fe2O3 ceramics (PZT-PZN-PMnN), where x = 0 ÷?0.35, has been prepared by two-stage calcination method. The effect of Fe2O3 conten...The 0.8Pb(Zr0.48Ti0.52)O3 – 0.125Pb(Zn1/3Nb2/3)O3 – 0.075Pb(Mn1/3Nb2/3)O3 + x wt% Fe2O3 ceramics (PZT-PZN-PMnN), where x = 0 ÷?0.35, has been prepared by two-stage calcination method. The effect of Fe2O3 content on the crystal structure and electrical properties of ceramics has been investigated. The results of X-ray diffraction (XRD) show that all samples have pure perovskite phase with tetragonal structure, the c/a ratio increases with increasing Fe2O3 content. At x = 0.25, electrical properties of ceramics are best: the density (r) of 7.86 g/cm3, the electromechanical coupling factor (kp) of 0.64, the dielectric constant (εr) of 1400, the dielectric loss (tand) of 0.003, the mechanical quality factor (Qm) of 1450, the piezoelectric constant (d31) of 155 pC/N, and the remanent polarization (Pr) of 37 μC/cm2, which makes it as a promising material for high power piezoelectric devices.展开更多
Developing efficient electrocatalysts for hydrogen evolution reaction(HER) is of great importance in contemporary water electrolysis technology. Here, a novel hierarchically sea urchin-like electrocatalyst(Mo_(4)O_(11...Developing efficient electrocatalysts for hydrogen evolution reaction(HER) is of great importance in contemporary water electrolysis technology. Here, a novel hierarchically sea urchin-like electrocatalyst(Mo_(4)O_(11)-MoS_(2)-VO_(2)) is synthesized by hydrothermal deposition and post-annealing strategy. The optimized electrocatalyst behaves as a high active hydrogen evolution electrode in 0.5 mol/L H_(2)SO_(4). This electrode needs overpotential of only 43 m V to achieve 10 m A/cm^(2)with a Tafel slope of 37 m V/dec and maintains its catalytic activity for at least 36 h. Better than most previously reported non-noble metal electrocatalysts anchored on carbon cloth. It is worth mentioning that the hierarchical sea urchin-like structure promotes the redistribution of electrons and provides more catalytic active sites. This strategy shows a way for the construction of inexpensive non-noble metal electrocatalysts in the future.展开更多
文摘In this paper, methane coupling at ambient temperature, under atmospheric pressure and in the presence of hydrogen was firstly investigated by using pulse corona plasma and Pt/g-Al2O3 catalyst. Experimental results showed that Pt/g-Al2O3 catalyst has catalytic activity for methane coupling to C2H4. Over sixty percent of outcomes of C2 hydrocarbons were detected to be ethylene.
文摘The catalytic performance of oxidative coupling of methane(OCM) over Eu 2O 3 catalysts promoted by alkaline earth fluorides was studied The results showed that C 2 hydrocarbon selectivity and yield over the fluoride promoted Eu 2O 3 catalysts were apparently higher than those over pure Eu 2O 3; the OCM performance increased according to the sequence of CaF 2 Eu 2O 3≈BaF 2 Eu 2O 3<SrF 2 Eu 2O 3 under the same conditions XRD experiment indicated that rhombohedral EuOF phase formed in the fresh BaF 2 Eu 2O 3 catalyst, while the exchange of F - and O 2- did not apparently happen in the fresh CaF 2 Eu 2O 3 and SrF 2 Eu 2O 3 catalysts Pyridine TPD and CO 2 TPD measurements found that, after adding SrF 2 to Eu 2O 3, the catalyst surface acidity decreased, whereas the surface basic strength increased slightly, resulting in an improvement in C 2 selectivity and yield
文摘The oxidation of 2-naphthol and 2-naphthalenethiol to 1,1'-bi-2-naphthol and bis-2-naphthyl disulfide respectively has been carried out in excellent yields in solid state in the presence of Fe3+-montmorillonite or alumina-supported FeCl3.
基金the State Key Fundamental Research Project(No.2006CB202504)the National Natural Science Foundation of China(No.20676140)Natural Science Foundation of Shanxi Province.
文摘The dehydrogenation of isobutane （IB） to produce isobutene coupled with reverse water gas shift in the presence of carbon dioxide was investigated over the catalyst Cr2O3 supported on active carbon （Cr2O3/AC）. The results illustrated that isobutane conversion and isobutene yield can be enhanced through the reaction coupling in the presence of carbon dioxide. Moreover, carbon dioxide can partially eliminate carbonaceous deposition on the catalyst and keep the active phase （Cr2O3）, which are then helpful to alleviate the catalyst deactivation.
文摘Herein,a bottom-down design is presented to successfully fabricate ZIF-derived Co3O4,grown in situ on a one-dimensional(1D)α-MnO2 material,denoted as α-MnO2@Co3O4.The synergistic effect derived from the coupled interface constructed betweenα-MnO2 and Co3O4 is responsible for the enhanced catalytic activity.The resultantα-MnO2@Co3O4 catalyst exhibits excellent catalytic activity at a T90%(temperature required to achieve a toluene conversion of 90%)of approximately 229℃,which is 47 and 28℃ lower than those of the pureα-MnO2 nanowire and Co3O4-b obtained via pyrolysis of ZIF-67,respectively.This activity is attributed to the increase in the number of surface-adsorbed oxygen species,which accelerate the oxygen mobility and enhance the redox pairs of Mn^4+/Mn^3+ and Co^2+/Co^3+.Moreover,the result of in situ diffuse reflectance infrared Fourier transform spectroscopy suggests that the gaseous oxygen could be more easily activated to adsorbed oxygen species on the surface of α-MnO2@Co3O4 than on that of α-MnO2.The catalytic reaction route of toluene oxidation over theα-MnO2@Co3O4 catalyst is as follows:toluene→benzoate species→alkanes containing oxygen functional group→CO2 and H2O.In addition,the α-MnO2@Co3O4 catalyst shows excellent stability and good water resistance for toluene oxidation.Furthermore,the preparation method can be extended to other 1D MnO2 materials.A new strategy for the development of high-performance catalysts of practical significance is provided.
基金Project supported by Publication Foundation of National Science and Technology Academic Books of China
文摘Thermodynamic models of calculating mass action concentrations for structural units or ion couples in RbCl-H2O binary and RbCl-RbNO3-H2O ternary strong electrolyte aqueous solutions were developed based on the ion and molecule coexistence theory at 298.15 K.A transformation coefficient is needed to compare the calculated mass action concentration and the reported activity because they are obtained at different standard states and concentration units.The results show that the transformation coefficients between the calculated mass action concentrations and the reported activities of the same structural units or ion couples in RbCl-H2O binary and RbCl-RbNO3-H2O ternary strong electrolyte aqueous solutions change in a very narrow range.The transformed mass action concentrations of structural units or ion couples in RbCl-H2O binary system are in good agreement with the reported activities. The transformed mass action concentrations of RbCl and RbNO3 in RbCl-RbNO3-H2O ternary solution are also in good agreement with the reported activities,aRbCl and 3RbNOa,with different total ionic strengths as 0.01,0.05,0.1,0.5,1.0,1.5,2.0,3.0 and 3.5 mol/kg,respectively.All those results mean the developed thermodynamic model of strong electrolyte aqueous solutions can reflect structural characteristics of RbCl-H2O binary and RbCl-RbNO3-H2O ternary strong electrolyte aqueous solutions and the mass action concentration also strictly follows the mass action law.
基金support by Northwestern University through a gift from Dr.Warren Haug is greatly appreciated
文摘Vapor phase catalytic hydrogen peroxide production by oxidation of water is possible by coupling the reaction with oxidation of an organic sacrificial reductant. It is potentially a safer process than direct synthesis from H2 and O2. Based on mechanistic information available mostly for liquid phase catalytic processes, feasible reaction mechanisms for such coupled reactions are proposed based on which desirable catalyst properties are identified. It is found that the surface-adsorbed oxygen bond is an important parameter for identifying desirable catalysts. Thermodynamics can be used to identify the types of organic oxidation reactions that can couple with water oxidation such that H2O2 formation becomes thermodynamically favorable. Reactions such as epoxidation of alkenes and selective oxidation of alkanes to alcohols cannot provide sufficient thermodynamic driving force, whereas oxidation of alcohols to aldehydes and to acids can. Finally, further research is suggested to identify catalytic properties important for H2O2 decomposition and for coupling selective oxidation of organic compounds to oxidation of H2O in order to facilitate development of H2O2 production coupled with selective organic oxidation.
文摘The 0.8Pb(Zr0.48Ti0.52)O3 – 0.125Pb(Zn1/3Nb2/3)O3 – 0.075Pb(Mn1/3Nb2/3)O3 + x wt% Fe2O3 ceramics (PZT-PZN-PMnN), where x = 0 ÷?0.35, has been prepared by two-stage calcination method. The effect of Fe2O3 content on the crystal structure and electrical properties of ceramics has been investigated. The results of X-ray diffraction (XRD) show that all samples have pure perovskite phase with tetragonal structure, the c/a ratio increases with increasing Fe2O3 content. At x = 0.25, electrical properties of ceramics are best: the density (r) of 7.86 g/cm3, the electromechanical coupling factor (kp) of 0.64, the dielectric constant (εr) of 1400, the dielectric loss (tand) of 0.003, the mechanical quality factor (Qm) of 1450, the piezoelectric constant (d31) of 155 pC/N, and the remanent polarization (Pr) of 37 μC/cm2, which makes it as a promising material for high power piezoelectric devices.
基金supported by the National Natural Science Foundation of China (No. 51802177)Independent Cultivation Program of Innovation Team of Ji nan City (No. 2019GXRC011)Introduction and Cultivation Plan of Young Innovative Talents in Colleges and Universities of Shandong Province,Shandong Provincial Natural Science Foundation (No. ZR^(2)020ME052)。
文摘Developing efficient electrocatalysts for hydrogen evolution reaction(HER) is of great importance in contemporary water electrolysis technology. Here, a novel hierarchically sea urchin-like electrocatalyst(Mo_(4)O_(11)-MoS_(2)-VO_(2)) is synthesized by hydrothermal deposition and post-annealing strategy. The optimized electrocatalyst behaves as a high active hydrogen evolution electrode in 0.5 mol/L H_(2)SO_(4). This electrode needs overpotential of only 43 m V to achieve 10 m A/cm^(2)with a Tafel slope of 37 m V/dec and maintains its catalytic activity for at least 36 h. Better than most previously reported non-noble metal electrocatalysts anchored on carbon cloth. It is worth mentioning that the hierarchical sea urchin-like structure promotes the redistribution of electrons and provides more catalytic active sites. This strategy shows a way for the construction of inexpensive non-noble metal electrocatalysts in the future.
