Mg-air batteries have attracted tremendous attention as a potential next-generation power source for portable electronics and e-transportation due to their remarkable high theoretical volumetric energy density,environ...Mg-air batteries have attracted tremendous attention as a potential next-generation power source for portable electronics and e-transportation due to their remarkable high theoretical volumetric energy density,environmental sustainability,and cost-effectiveness.However,the fast hydrogen evolution reaction(HER)in NaCl-based aqueous electrolytes impairs the performance of Mg-air batteries and leads to poor specific capacity,low energy density,and low utilization.Thus,the conventionally used NaCl solute was proposed to be replaced by NaNO_(3)and acetic acid additive as a corrosion inhibitor,therefore an electrolyte engineering for long-life time Mg-air batteries is reported.The resulting Mg-air batteries based on this optimized electrolyte demonstrate an improved discharge voltage reaching~1.8 V for initial 5 h at a current density of 0.5 mA/cm^(2) and significantly prolonged cells'operational lifetime to over 360 h,in contrast to only~17 h observed in NaCl electrolyte.X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry were employed to analyse the composition of surface film and scanning electron microscopy combined with transmission electron microscopy to clarify the morphology changes of the surface layer as a function of acetic acid addition.The thorough studies of chemical composition and morphology of corrosion products have allowed us to elucidate the working mechanism of Mg anode in this optimized electrolyte for Mg-air batteries.展开更多
The oxidative desulfurization of a real refinery feedstock (i.e.,non-hydrotreated kerosene with total sulfur mass content of 0.16%) with a mixture of hydrogen peroxide and acetic acid was studied.The influences of var...The oxidative desulfurization of a real refinery feedstock (i.e.,non-hydrotreated kerosene with total sulfur mass content of 0.16%) with a mixture of hydrogen peroxide and acetic acid was studied.The influences of various operating parameters including reaction temperature (T),acid to sulfur molar ratio (nacid/nS),and oxidant to sulfur molar ratio (nO/nS) on the sulfur removal of kerosene were investigated.The results revealed that an increase in the reaction temperature (T) and nacid/nS enhances the sulfur removal.Moreover,there is an optimum nO/nS related to the reaction temperature and the best sulfur removal could be obtained at nO/nS=8 and 23 for the reaction temperatures of 25 and 60°C,respectively.The maximum observed sulfur removal in the present oxidative desulfurization system was 83.3%.展开更多
The palladium complex of the molecular complex of poly(4 vinylpyridine) with acetic acid(PVP/ HAc Pd) was prepared. Its catalytic activity for the hydrogenation of nitrobenzene was found much higher than that of the c...The palladium complex of the molecular complex of poly(4 vinylpyridine) with acetic acid(PVP/ HAc Pd) was prepared. Its catalytic activity for the hydrogenation of nitrobenzene was found much higher than that of the corresponding palladium complex of poly(4 vinylpyridine). In the presence of a strong inorganic alkali, especially potassium hydroxide, the catalytic activity is greatly improved. The suitable hydrogenation condition for PVP/HAc Pd is to use 0 1 mol/L ethanol solution of potassium hydroxide as the hydrogenation medium and the hydrogenation is carried out at 45 ℃.展开更多
MIL-53(Fe)was synthesized using a“modulator approach”that utilizes acetic acid(HAc)as an additive to control the size and morphology of the resulting crystals.We demonstrate that after activation under vaccum at 100...MIL-53(Fe)was synthesized using a“modulator approach”that utilizes acetic acid(HAc)as an additive to control the size and morphology of the resulting crystals.We demonstrate that after activation under vaccum at 100℃,the MIL-53(Fe)functions well for H2S selective oxidation.The introduction of acetic acid in the presence of benzene-1,4-dicarboxylic acid(H2BDC)would result in a series of MIL-53(Fe)nanocrystals(denoted as MIL-53(Fe)-xH,x stands for the volume of added HAc with morphology evoluting from irregular particles to short hexagonal columns.The vacuum treatment facilitates the removal of acetate groups,thus generating Fe3+Lewis acid sites.Consequently,the resulted MIL-53(Fe)-xH exhibits good catalytic activity(98%H2S conversion and 92%sulfur selectivity)at moderate reaction temperatures(100–190℃).The MIL-53(Fe)-5H is superior to the traditional iron-based catalysts,showing stable performance in a test period of 55 h.展开更多
The rapid synthesis of 3-bromocarbarole-N-acetic acid was performed using microwave irradiation. Under the optimal conditions the yield was 85.6% . The crystal structure showed that the carboxylic groups form bifurcat...The rapid synthesis of 3-bromocarbarole-N-acetic acid was performed using microwave irradiation. Under the optimal conditions the yield was 85.6% . The crystal structure showed that the carboxylic groups form bifurcated hydrogen bonds and the hydroxyl oxygen atoms serve as proton donors and also acceptor. Each carboxylic group was involved in four hydrogen bonds. The package of crystal was dominated by links of these hydrogen bonds.展开更多
The effect of thermal pretreatment on the active sites and catalytic performances of PtSn/SiO2 catalyst in acetic acid （AcOH） hydrogenation was investigated in this article. The catalysts were characterized by N2 ph...The effect of thermal pretreatment on the active sites and catalytic performances of PtSn/SiO2 catalyst in acetic acid （AcOH） hydrogenation was investigated in this article. The catalysts were characterized by N2 physical adsorption, X-ray diffraction, transmission electron microscopy, pyridine Fourier-transform infrared spectra, and H2-O2 titration on its physicochemical properties. The results showed that Pt species were formed primarily in crystalline structure and no PtSnx alloy was observed. Meanwhile, with the increment of thermal pretreatrnent temperature, Pt dispersion showed a decreas- ing trend due to the aggregation of Pt particles. Simultaneously, the amount of Lewis acid sites was remarkably influenced by such thermal pretreatment owning to the consequent physicochemical property variation of Sn species. Interestingly, the catalytic activity showed the similar variation trend with that of Lewis acid sites, confirming the important roles of Lewis acid sites in AcOH hydrogenation. Moreover, a balancing effect between exposed Pt and Lewis acid sites was obtained, resulting in the superior catalytic performance in AcOH hydrogenation.展开更多
In separation processes,hydrogen bonding has a very significant effect on the efficiency of isolation of acetic acid (HOAc) from HOAc/H2O mixtures. This intermolecular interaction on aggregates composed of a single HO...In separation processes,hydrogen bonding has a very significant effect on the efficiency of isolation of acetic acid (HOAc) from HOAc/H2O mixtures. This intermolecular interaction on aggregates composed of a single HOAc molecule and varying numbers of H2O molecules has been examined by using ab initio molecular dynamics simulations (AIMD) and quantum chemical calculations (QCC). Thermodynamic data in aqueous solution were obtained through the self-consistent reaction field calculations and the polarizable continuum model. The aggregation free energy of the aggregates in gas phase as well as in aqueous system shows that the 6-membered ring is the most favorable structure in both states. The relative stability of the ring structures inferred from the thermodynamic properties of the QCC is consistent with the ring distributions of the AIMD simulation. The study shows that in dilute aqueous solution of HOAc the more favorable molecular interaction is the hydrogen bonding between HOAc and H2O molecules,resulting in the separation of acetic acid from the HOAc/H2O mixtures with more difficulty than usual.展开更多
Hydrogen production from steam reforming of bio-oil and acetic acid using Ni/γ-Al2O3 catalyst was studied in a laboratory-scale fixed bed reactor.This study selected different Ni loadings(16.8%and 30.5%)in Ni/γ-Al2O...Hydrogen production from steam reforming of bio-oil and acetic acid using Ni/γ-Al2O3 catalyst was studied in a laboratory-scale fixed bed reactor.This study selected different Ni loadings(16.8%and 30.5%)in Ni/γ-Al2O3 catalysts and reaction temperatures(500°C,600°C and 700°C)as variables to optimize the hydrogen yield and selectivity of gases formed.Experiments were carried out in an isothermal manner.The catalysts were prepared on wet impregnation of aγ-Al2O3 which supported with two different Ni loadings.The principal gases generated were H2,CO,CO2 and CH4.The results from steam reforming of acetic acid showed that the yield and selectivity of hydrogen using the catalyst with 30.5%Ni were significantly higher than that with 16.8%Ni.The results showed that the most favorable temperature for hydrogen production was 600°C,and the steam reforming of bio-oil using Ni/γ-Al2O3 catalyst with 30.5%Ni showed that the yields and selectivity of H2 and CO2 increased with the temperature increasing while CH4 and CO selectivity decreased.These results showed that the most favorable temperature for hydrogen production from bio-oil using 30.5%Ni/γ-Al2O3 was 600°C,at which hydrogen yield was at its maximum of 65%.展开更多
The catalytic hydrogenation of carboxylic acid to alcohols is one of the important strategies for the conversion of biomass.Herein,a series of Ni-doped PtSn catalysts were prepared,characterized and studied in the hyd...The catalytic hydrogenation of carboxylic acid to alcohols is one of the important strategies for the conversion of biomass.Herein,a series of Ni-doped PtSn catalysts were prepared,characterized and studied in the hydrogenation of acetic acid.The Ni dopant has a strong interaction with Pt,which promotes the hydrogen adsorption,providing an activated hydrogen-rich environment for the hydrogenation.Meanwhile,the presence of Ni also improves the Pt dispersion,giving more accessible active sites for hydrogen activation.The cooperation of Pt and Ni significantly promotes the catalytic activity of the hydrogenation of acetic acid to ethanol.As a result,the catalyst with 0.1%Ni exhibits the best reaction activity,and its space time yield is twice as that of the PtSn/SiO2 catalyst.It provides a meaningful instruction on the catalyst design for the carboxylic acid hydrogenation.展开更多
Fluorescence spectra of acetic acid-water solution excited by ultraviolet （UV） light are studied, and the relationship between fluorescence spectra and molecular association of acetic acid is discussed. The results ...Fluorescence spectra of acetic acid-water solution excited by ultraviolet （UV） light are studied, and the relationship between fluorescence spectra and molecular association of acetic acid is discussed. The results indicate that when the exciting light wavelength is longer than 246 nm, there are two fluorescence peaks located at 305 and 334 nm, respectively. By measuring the excitation spectra, the optimal wavelengths of the two fluorescence peaks are obtained, which are 258 and 284 nm, respectively. Fluorescence spectra of acetic acid-water solution change with concentrations, which is primarily attributed to changes of molecular association of acetic acid in aqueous solution. Through theoretical analysis, three variations of molecular association have been obtained in acetic acid-water solution, which are the hydrated monomers, the linear dimers, and the water separated dimers. This research can provide references to studies of molecular association of acetic acid-water, especiMly studies of hydrogen bonds.展开更多
基金the China Scholarship Council(CSC)for funding(no.201806310116)。
文摘Mg-air batteries have attracted tremendous attention as a potential next-generation power source for portable electronics and e-transportation due to their remarkable high theoretical volumetric energy density,environmental sustainability,and cost-effectiveness.However,the fast hydrogen evolution reaction(HER)in NaCl-based aqueous electrolytes impairs the performance of Mg-air batteries and leads to poor specific capacity,low energy density,and low utilization.Thus,the conventionally used NaCl solute was proposed to be replaced by NaNO_(3)and acetic acid additive as a corrosion inhibitor,therefore an electrolyte engineering for long-life time Mg-air batteries is reported.The resulting Mg-air batteries based on this optimized electrolyte demonstrate an improved discharge voltage reaching~1.8 V for initial 5 h at a current density of 0.5 mA/cm^(2) and significantly prolonged cells'operational lifetime to over 360 h,in contrast to only~17 h observed in NaCl electrolyte.X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry were employed to analyse the composition of surface film and scanning electron microscopy combined with transmission electron microscopy to clarify the morphology changes of the surface layer as a function of acetic acid addition.The thorough studies of chemical composition and morphology of corrosion products have allowed us to elucidate the working mechanism of Mg anode in this optimized electrolyte for Mg-air batteries.
基金Supported by the R&D center of Esfahan refinery (Esfahan,Iran)the technical supports of central laboratory of Esfahan Refinery for total sulfur analysis
文摘The oxidative desulfurization of a real refinery feedstock (i.e.,non-hydrotreated kerosene with total sulfur mass content of 0.16%) with a mixture of hydrogen peroxide and acetic acid was studied.The influences of various operating parameters including reaction temperature (T),acid to sulfur molar ratio (nacid/nS),and oxidant to sulfur molar ratio (nO/nS) on the sulfur removal of kerosene were investigated.The results revealed that an increase in the reaction temperature (T) and nacid/nS enhances the sulfur removal.Moreover,there is an optimum nO/nS related to the reaction temperature and the best sulfur removal could be obtained at nO/nS=8 and 23 for the reaction temperatures of 25 and 60°C,respectively.The maximum observed sulfur removal in the present oxidative desulfurization system was 83.3%.
基金Supported by the Outstanding Youngs Science Foudation of Henan Province(1999)
文摘The palladium complex of the molecular complex of poly(4 vinylpyridine) with acetic acid(PVP/ HAc Pd) was prepared. Its catalytic activity for the hydrogenation of nitrobenzene was found much higher than that of the corresponding palladium complex of poly(4 vinylpyridine). In the presence of a strong inorganic alkali, especially potassium hydroxide, the catalytic activity is greatly improved. The suitable hydrogenation condition for PVP/HAc Pd is to use 0 1 mol/L ethanol solution of potassium hydroxide as the hydrogenation medium and the hydrogenation is carried out at 45 ℃.
文摘MIL-53(Fe)was synthesized using a“modulator approach”that utilizes acetic acid(HAc)as an additive to control the size and morphology of the resulting crystals.We demonstrate that after activation under vaccum at 100℃,the MIL-53(Fe)functions well for H2S selective oxidation.The introduction of acetic acid in the presence of benzene-1,4-dicarboxylic acid(H2BDC)would result in a series of MIL-53(Fe)nanocrystals(denoted as MIL-53(Fe)-xH,x stands for the volume of added HAc with morphology evoluting from irregular particles to short hexagonal columns.The vacuum treatment facilitates the removal of acetate groups,thus generating Fe3+Lewis acid sites.Consequently,the resulted MIL-53(Fe)-xH exhibits good catalytic activity(98%H2S conversion and 92%sulfur selectivity)at moderate reaction temperatures(100–190℃).The MIL-53(Fe)-5H is superior to the traditional iron-based catalysts,showing stable performance in a test period of 55 h.
文摘The rapid synthesis of 3-bromocarbarole-N-acetic acid was performed using microwave irradiation. Under the optimal conditions the yield was 85.6% . The crystal structure showed that the carboxylic groups form bifurcated hydrogen bonds and the hydroxyl oxygen atoms serve as proton donors and also acceptor. Each carboxylic group was involved in four hydrogen bonds. The package of crystal was dominated by links of these hydrogen bonds.
基金Acknowledgements We are grateful to the financial support from the National Natural Science Foundation of China （Grant Nos. 21276186, 21325626, 91434127, U1510203） and the Tianjin Natural Science Foundation （13JCZDJC33000）.
文摘The effect of thermal pretreatment on the active sites and catalytic performances of PtSn/SiO2 catalyst in acetic acid （AcOH） hydrogenation was investigated in this article. The catalysts were characterized by N2 physical adsorption, X-ray diffraction, transmission electron microscopy, pyridine Fourier-transform infrared spectra, and H2-O2 titration on its physicochemical properties. The results showed that Pt species were formed primarily in crystalline structure and no PtSnx alloy was observed. Meanwhile, with the increment of thermal pretreatrnent temperature, Pt dispersion showed a decreas- ing trend due to the aggregation of Pt particles. Simultaneously, the amount of Lewis acid sites was remarkably influenced by such thermal pretreatment owning to the consequent physicochemical property variation of Sn species. Interestingly, the catalytic activity showed the similar variation trend with that of Lewis acid sites, confirming the important roles of Lewis acid sites in AcOH hydrogenation. Moreover, a balancing effect between exposed Pt and Lewis acid sites was obtained, resulting in the superior catalytic performance in AcOH hydrogenation.
基金Supported by the Jiangsu Planned Projects for Postdoctoral Research Funds (No. 0901001C)the National Natural Science Foundation of China (Grant No. 20876072)the Natural Science Foundation of Jiangsu Province (No. KB2008023)
文摘In separation processes,hydrogen bonding has a very significant effect on the efficiency of isolation of acetic acid (HOAc) from HOAc/H2O mixtures. This intermolecular interaction on aggregates composed of a single HOAc molecule and varying numbers of H2O molecules has been examined by using ab initio molecular dynamics simulations (AIMD) and quantum chemical calculations (QCC). Thermodynamic data in aqueous solution were obtained through the self-consistent reaction field calculations and the polarizable continuum model. The aggregation free energy of the aggregates in gas phase as well as in aqueous system shows that the 6-membered ring is the most favorable structure in both states. The relative stability of the ring structures inferred from the thermodynamic properties of the QCC is consistent with the ring distributions of the AIMD simulation. The study shows that in dilute aqueous solution of HOAc the more favorable molecular interaction is the hydrogen bonding between HOAc and H2O molecules,resulting in the separation of acetic acid from the HOAc/H2O mixtures with more difficulty than usual.
基金The authors gratefully thank the support for this research from the Major State Basic Research Development Program of China(2012AA101808)Project 51206100 and 51276103 supported by National Natural Science Foundation of China,Project ZR2012EEQ018 supported by Shandong Provincial Natural Science Foundation,China,A Project of Shandong Province Higher Educational Science and Technology Program(J12LF12)Project 4072-112007 supported by Shandong University of Science and Technology Young Teachers Program.
文摘Hydrogen production from steam reforming of bio-oil and acetic acid using Ni/γ-Al2O3 catalyst was studied in a laboratory-scale fixed bed reactor.This study selected different Ni loadings(16.8%and 30.5%)in Ni/γ-Al2O3 catalysts and reaction temperatures(500°C,600°C and 700°C)as variables to optimize the hydrogen yield and selectivity of gases formed.Experiments were carried out in an isothermal manner.The catalysts were prepared on wet impregnation of aγ-Al2O3 which supported with two different Ni loadings.The principal gases generated were H2,CO,CO2 and CH4.The results from steam reforming of acetic acid showed that the yield and selectivity of hydrogen using the catalyst with 30.5%Ni were significantly higher than that with 16.8%Ni.The results showed that the most favorable temperature for hydrogen production was 600°C,and the steam reforming of bio-oil using Ni/γ-Al2O3 catalyst with 30.5%Ni showed that the yields and selectivity of H2 and CO2 increased with the temperature increasing while CH4 and CO selectivity decreased.These results showed that the most favorable temperature for hydrogen production from bio-oil using 30.5%Ni/γ-Al2O3 was 600°C,at which hydrogen yield was at its maximum of 65%.
基金The National Natural Science Foundation of China are acknowledged for the financial support on this work(Grant No.21878227).
文摘The catalytic hydrogenation of carboxylic acid to alcohols is one of the important strategies for the conversion of biomass.Herein,a series of Ni-doped PtSn catalysts were prepared,characterized and studied in the hydrogenation of acetic acid.The Ni dopant has a strong interaction with Pt,which promotes the hydrogen adsorption,providing an activated hydrogen-rich environment for the hydrogenation.Meanwhile,the presence of Ni also improves the Pt dispersion,giving more accessible active sites for hydrogen activation.The cooperation of Pt and Ni significantly promotes the catalytic activity of the hydrogenation of acetic acid to ethanol.As a result,the catalyst with 0.1%Ni exhibits the best reaction activity,and its space time yield is twice as that of the PtSn/SiO2 catalyst.It provides a meaningful instruction on the catalyst design for the carboxylic acid hydrogenation.
基金supported by the Natural Science Foundation of Jiangsu Province (No. BK2007204)the Natural Science Foundation of Jiangsu Province Educational Committee (No. 07KJD140208).
文摘Fluorescence spectra of acetic acid-water solution excited by ultraviolet （UV） light are studied, and the relationship between fluorescence spectra and molecular association of acetic acid is discussed. The results indicate that when the exciting light wavelength is longer than 246 nm, there are two fluorescence peaks located at 305 and 334 nm, respectively. By measuring the excitation spectra, the optimal wavelengths of the two fluorescence peaks are obtained, which are 258 and 284 nm, respectively. Fluorescence spectra of acetic acid-water solution change with concentrations, which is primarily attributed to changes of molecular association of acetic acid in aqueous solution. Through theoretical analysis, three variations of molecular association have been obtained in acetic acid-water solution, which are the hydrated monomers, the linear dimers, and the water separated dimers. This research can provide references to studies of molecular association of acetic acid-water, especiMly studies of hydrogen bonds.
