The hydrogenation reaction characteristics and the properties of its hydrides for the magnetic regenerative material HoCu_2(CeCu_2-type) of a cryocooler were investigated. The XRD testing reveals that the hydrides of ...The hydrogenation reaction characteristics and the properties of its hydrides for the magnetic regenerative material HoCu_2(CeCu_2-type) of a cryocooler were investigated. The XRD testing reveals that the hydrides of HoCu_2 were a mixture of Cu, unknown hydride Ⅰ, and unknown hydride Ⅱ. Based on the PCT(pressure-concentration-temperature) curves under different reaction temperatures, the relationships among reaction temperature, equilibrium pressure, and maximum hydrogen absorption capacity were analyzed and discussed. The enthalpy change ΔH and entropy change ΔS as a result of the whole hydrogenation process were also calculated from the PCT curves. The magnetization and volumetric specific heat capacity of the hydride were also measured by SQUID magnetometer and PPMS, respectively.展开更多
The efficient and selective electrocatalytic hydrogenation(ECH)of furfural is considered a green strategy for achieving biomass-derived high-value chemicals.Regulating an aqueous electrolytic environment,a green hydro...The efficient and selective electrocatalytic hydrogenation(ECH)of furfural is considered a green strategy for achieving biomass-derived high-value chemicals.Regulating an aqueous electrolytic environment,a green hydrogen energy source of water,is significant for improving the selectivity of products and reducing energy consumption.In this study,we systematically investigated the mechanism of pH dependence of product selectivity in the ECH of furfural on Cu electrodes.Under acidic conditions,the oxygen atom dissociated directly from hydrogenated furfural-derived alkoxyl intermediates,followed by stepwise hydrogenation until H_(2)O formation via a thermodynamically favorable proton-coupled electron transfer process,thereby inducing a high proportion of the hydrogenolysis product(2-methylfuran).However,under partial alkaline conditions,furfural could be directly hydrogenated to furfuryl alcohol(selectivity~98%)due to the high-energy barrier of the deoxidation process via a surface hydride(Had)transfer.Our results highlight the vital role of the electrolytic environment in furfural selective conversion and broaden our fundamental understanding of hydrodeoxygenation reactions in ECH.展开更多
Selective propylene epoxidation to propylene oxide(PO) with hydrogen peroxide(H_2O_2) was carried out in a catalytic semi-batch reactor.High propylene epoxidation activity(44 h^(-1)) was observed over Nb based mesopor...Selective propylene epoxidation to propylene oxide(PO) with hydrogen peroxide(H_2O_2) was carried out in a catalytic semi-batch reactor.High propylene epoxidation activity(44 h^(-1)) was observed over Nb based mesoporous silicate materials Nb-TUD-1 under mild operating conditions.The physical and chemical properties of the Nb based silicates characterized using BET,FTIR,TPD,TEM and UV–Vis revealed that the site isolation and surface acidity are crucial for PO production.Catalyst synthesis methods were investigated for their effects on PO productivity,PO selectivity and H_2O_2 utilization efficiency.It is found that Nb-TUD-1 material synthesized by the sol–gel method is more active and selective than impregnated materials for liquid phase propylene epoxidation.Surface characterization confirms that thus synthesized Nb-TUD-1 catalysts have more Lewis acidity and less Bronsted acidity compared to the catalysts by impregnation.展开更多
Co-intensification was researched to accelerate gold leaching with regards to its electrochemical nature by using anodic intensifiers of heavy metal ions (Pb2+,Bi3+,Tl+,Hg2+ and Ag+) on the basis of hydrogen peroxide ...Co-intensification was researched to accelerate gold leaching with regards to its electrochemical nature by using anodic intensifiers of heavy metal ions (Pb2+,Bi3+,Tl+,Hg2+ and Ag+) on the basis of hydrogen peroxide assistant leaching on three different types of materials which were classified as a refractory sulphide gold concentrate,an easily leachable sulphide gold concentrate,and a low grade oxide gold ore according to their leaching characteristics.The results showed that,favorable co-intensification effects on the three materials were obtained and leaching time of gold was effectively shortened to no longer than 12 h from 16 to 24 h for hydrogen peroxide assistant leaching.For the five tested heavy metal ions,Bi3+and Tl+ presented co-intensifying effect on all the three materials,and Hg2+ caused co-intensifying effect on both refractory and easily leachable sulphide gold concentrates,and Pb2+ and Ag+ only had co-intensifying effect on the easily leachable sulphide gold concentrate.展开更多
The density,viscosity and refractive index of aqueous solutions of tetrabutylammonium hydroxide(TBAOH),piperazine(PZ) and their aqueous blends are determined at several temperatures(303.15 to 333.15 K).All these measu...The density,viscosity and refractive index of aqueous solutions of tetrabutylammonium hydroxide(TBAOH),piperazine(PZ) and their aqueous blends are determined at several temperatures(303.15 to 333.15 K).All these measured physicochemical properties decreases with an increase in temperature.The density data is used to calculate the coefficient of thermal expansion and excess molar volume of all aqueous binary and ternary solutions.The coefficient of thermal expansion increases with increase in temperatures and concentrations.The negativity of excess molar volume for all the aqueous solution decreased with increase in temperature.Each physical property is correlated with temperature by least square method and the corresponding coefficients for each property are presented.The prediction values from correlations for the physical properties are in good agreement with the experimental values.展开更多
Many minerals in nature have self-purification capacity to hold and stabilize deleterious contaminants into their lattice structures,which can be used for treatment of heavy metals-bearing contaminants. Hydrotalcite L...Many minerals in nature have self-purification capacity to hold and stabilize deleterious contaminants into their lattice structures,which can be used for treatment of heavy metals-bearing contaminants. Hydrotalcite Layer Double Hydroxide (LDH),tobermorite Calcium Silicate Hydrate (CSH) and apatite are ubiquitous minerals in nature,having higher geochemical stability and potential for binding and stabilizing heavy metals. Based on the elucidation of crystal structure property and self-purification principles of the three minerals above,this article discussed how to design the self-purification system of heavy metal-bearing contaminants.展开更多
Conversion of waste biomass to valuable carbonaceous material is a sustainable and environmental benign method for energy and reduction of greenhouse gas emission. Herein, a two-step hydrothermal method was developed ...Conversion of waste biomass to valuable carbonaceous material is a sustainable and environmental benign method for energy and reduction of greenhouse gas emission. Herein, a two-step hydrothermal method was developed to fabricate high performance electrode material from pomelo peels. In the first step, the pomelo peels were transformed to carbonaceous aerogel (CA), which constructed of three- dimensional, sponge-like brown monolith with hierarchical pores, low-density (0.032 g]cm3) and excel- lent mechanical flexibility. Then, the cobalt nickel aluminum layered double hydroxide (CoNiAI-LDH) was in situ loaded on the surface of CA to form exquisite core-shell structure (CoNiAI-LDH@CA) through the second hydrothermal step. When used as an electrode material for supercapacitor, CoNiA1-LDHOCA exhibited high specific capacitances of 1,134F/g at 1A/g and 902Fig at 10A/g, respectively. Furthermore, they displayed an excellent cycling stability without an obvious capacitance decrease after 4,000 cycles.展开更多
Light weight and mechanically strong α-chitin aerogels were fabricated using the sol-gel/self-assembly method from α-chitin in different aqueous alkali hydroxide(KOH, Na OH and Li OH)/urea solutions. All of the α-c...Light weight and mechanically strong α-chitin aerogels were fabricated using the sol-gel/self-assembly method from α-chitin in different aqueous alkali hydroxide(KOH, Na OH and Li OH)/urea solutions. All of the α-chitin solutions exhibited temperature-induced rapid gelation behavior. 13 C nuclear magnetic resonance(NMR) spectra revealed that the aqueous alkali hydroxide/urea solutions are non-derivatizing solvents for α-chitin. Fourier transform infrared(FT-IR), X-ray diffraction(XRD) and cross-polarization magic angle spinning(CP/MAS) 13 C NMR confirmed that α-chitin has a stable aggregate structure after undergoing dissolution and regeneration. Subsequently, nanostructured α-chitin aerogels were fabricated by regeneration from the chitin solutions in ethanol and then freeze-drying from t-Bu OH. These α-chitin aerogels exhibited high porosity(87% to 94%), low density(0.09 to 0.19 g/cm^3), high specific surface area(419 to 535 m^2/g) and large pore volume(2.7 to 3.8 cm^3/g). Moreover, the α-chitin aerogels exhibited good mechanical properties under compression and tension models. In vitro studies showed that m BMSCs cultured on chitin hydrogels have good biocompatibility. These nanostructured α-chitin aerogels may be useful for various applications, such as catalyst supports, carbon aerogel precursors and biomedical materials.展开更多
基金Project(51276154)supported by the National Natural Science Foundation of ChinaProject(2012010111014)supported by the University Doctoral Subject Special Foundation of China
文摘The hydrogenation reaction characteristics and the properties of its hydrides for the magnetic regenerative material HoCu_2(CeCu_2-type) of a cryocooler were investigated. The XRD testing reveals that the hydrides of HoCu_2 were a mixture of Cu, unknown hydride Ⅰ, and unknown hydride Ⅱ. Based on the PCT(pressure-concentration-temperature) curves under different reaction temperatures, the relationships among reaction temperature, equilibrium pressure, and maximum hydrogen absorption capacity were analyzed and discussed. The enthalpy change ΔH and entropy change ΔS as a result of the whole hydrogenation process were also calculated from the PCT curves. The magnetization and volumetric specific heat capacity of the hydride were also measured by SQUID magnetometer and PPMS, respectively.
文摘The efficient and selective electrocatalytic hydrogenation(ECH)of furfural is considered a green strategy for achieving biomass-derived high-value chemicals.Regulating an aqueous electrolytic environment,a green hydrogen energy source of water,is significant for improving the selectivity of products and reducing energy consumption.In this study,we systematically investigated the mechanism of pH dependence of product selectivity in the ECH of furfural on Cu electrodes.Under acidic conditions,the oxygen atom dissociated directly from hydrogenated furfural-derived alkoxyl intermediates,followed by stepwise hydrogenation until H_(2)O formation via a thermodynamically favorable proton-coupled electron transfer process,thereby inducing a high proportion of the hydrogenolysis product(2-methylfuran).However,under partial alkaline conditions,furfural could be directly hydrogenated to furfuryl alcohol(selectivity~98%)due to the high-energy barrier of the deoxidation process via a surface hydride(Had)transfer.Our results highlight the vital role of the electrolytic environment in furfural selective conversion and broaden our fundamental understanding of hydrodeoxygenation reactions in ECH.
基金Supported by the China Postdoctoral Science Foundation(2017 M612374)the Natural Science Foundation of Shandong Province(ZR2017BB007)+5 种基金the Postdoctoral Research Funding of Shandong Province(201703016)the Qingdao Postdoctoral Research Funding(BY20170210)the Fundamental Research Funding of Qingdao(17-1-1-67-jch,17-1-1-80-jch)the Fundamental Research Funds for the Central Universities(18CX02145A,17CX02017A)the New Faculty Start-up Funding from China University of Petroleum(YJ201601058)the Natural Science Foundation of China(21606254)
文摘Selective propylene epoxidation to propylene oxide(PO) with hydrogen peroxide(H_2O_2) was carried out in a catalytic semi-batch reactor.High propylene epoxidation activity(44 h^(-1)) was observed over Nb based mesoporous silicate materials Nb-TUD-1 under mild operating conditions.The physical and chemical properties of the Nb based silicates characterized using BET,FTIR,TPD,TEM and UV–Vis revealed that the site isolation and surface acidity are crucial for PO production.Catalyst synthesis methods were investigated for their effects on PO productivity,PO selectivity and H_2O_2 utilization efficiency.It is found that Nb-TUD-1 material synthesized by the sol–gel method is more active and selective than impregnated materials for liquid phase propylene epoxidation.Surface characterization confirms that thus synthesized Nb-TUD-1 catalysts have more Lewis acidity and less Bronsted acidity compared to the catalysts by impregnation.
基金Project(50725416) supported by the National Natural Science Foundation for Distinguished Young Scholars of China
文摘Co-intensification was researched to accelerate gold leaching with regards to its electrochemical nature by using anodic intensifiers of heavy metal ions (Pb2+,Bi3+,Tl+,Hg2+ and Ag+) on the basis of hydrogen peroxide assistant leaching on three different types of materials which were classified as a refractory sulphide gold concentrate,an easily leachable sulphide gold concentrate,and a low grade oxide gold ore according to their leaching characteristics.The results showed that,favorable co-intensification effects on the three materials were obtained and leaching time of gold was effectively shortened to no longer than 12 h from 16 to 24 h for hydrogen peroxide assistant leaching.For the five tested heavy metal ions,Bi3+and Tl+ presented co-intensifying effect on all the three materials,and Hg2+ caused co-intensifying effect on both refractory and easily leachable sulphide gold concentrates,and Pb2+ and Ag+ only had co-intensifying effect on the easily leachable sulphide gold concentrate.
基金the CO2 Management (MOR) research group of Universiti TeknologiPETRONAS for providing the financial support and facilities
文摘The density,viscosity and refractive index of aqueous solutions of tetrabutylammonium hydroxide(TBAOH),piperazine(PZ) and their aqueous blends are determined at several temperatures(303.15 to 333.15 K).All these measured physicochemical properties decreases with an increase in temperature.The density data is used to calculate the coefficient of thermal expansion and excess molar volume of all aqueous binary and ternary solutions.The coefficient of thermal expansion increases with increase in temperatures and concentrations.The negativity of excess molar volume for all the aqueous solution decreased with increase in temperature.Each physical property is correlated with temperature by least square method and the corresponding coefficients for each property are presented.The prediction values from correlations for the physical properties are in good agreement with the experimental values.
文摘Many minerals in nature have self-purification capacity to hold and stabilize deleterious contaminants into their lattice structures,which can be used for treatment of heavy metals-bearing contaminants. Hydrotalcite Layer Double Hydroxide (LDH),tobermorite Calcium Silicate Hydrate (CSH) and apatite are ubiquitous minerals in nature,having higher geochemical stability and potential for binding and stabilizing heavy metals. Based on the elucidation of crystal structure property and self-purification principles of the three minerals above,this article discussed how to design the self-purification system of heavy metal-bearing contaminants.
基金supported by the National Natural Science Foundation of China(21333009,21273244,21573245)the Youth Innovation Promotion Association of Chinese Academy of Sciences(2017049)
文摘Conversion of waste biomass to valuable carbonaceous material is a sustainable and environmental benign method for energy and reduction of greenhouse gas emission. Herein, a two-step hydrothermal method was developed to fabricate high performance electrode material from pomelo peels. In the first step, the pomelo peels were transformed to carbonaceous aerogel (CA), which constructed of three- dimensional, sponge-like brown monolith with hierarchical pores, low-density (0.032 g]cm3) and excel- lent mechanical flexibility. Then, the cobalt nickel aluminum layered double hydroxide (CoNiAI-LDH) was in situ loaded on the surface of CA to form exquisite core-shell structure (CoNiAI-LDH@CA) through the second hydrothermal step. When used as an electrode material for supercapacitor, CoNiA1-LDHOCA exhibited high specific capacitances of 1,134F/g at 1A/g and 902Fig at 10A/g, respectively. Furthermore, they displayed an excellent cycling stability without an obvious capacitance decrease after 4,000 cycles.
基金supported by the National Natural Science Foundation of China (21422405, 51373125)the Major Program of National Natural Science Foundation of China (21334005)+1 种基金the facility support of the Natural Science Foundation of Hubei Provincethe Fundamental Research Funds for the Central Universities
文摘Light weight and mechanically strong α-chitin aerogels were fabricated using the sol-gel/self-assembly method from α-chitin in different aqueous alkali hydroxide(KOH, Na OH and Li OH)/urea solutions. All of the α-chitin solutions exhibited temperature-induced rapid gelation behavior. 13 C nuclear magnetic resonance(NMR) spectra revealed that the aqueous alkali hydroxide/urea solutions are non-derivatizing solvents for α-chitin. Fourier transform infrared(FT-IR), X-ray diffraction(XRD) and cross-polarization magic angle spinning(CP/MAS) 13 C NMR confirmed that α-chitin has a stable aggregate structure after undergoing dissolution and regeneration. Subsequently, nanostructured α-chitin aerogels were fabricated by regeneration from the chitin solutions in ethanol and then freeze-drying from t-Bu OH. These α-chitin aerogels exhibited high porosity(87% to 94%), low density(0.09 to 0.19 g/cm^3), high specific surface area(419 to 535 m^2/g) and large pore volume(2.7 to 3.8 cm^3/g). Moreover, the α-chitin aerogels exhibited good mechanical properties under compression and tension models. In vitro studies showed that m BMSCs cultured on chitin hydrogels have good biocompatibility. These nanostructured α-chitin aerogels may be useful for various applications, such as catalyst supports, carbon aerogel precursors and biomedical materials.