The surface acidity of synthetic amorphous AI hydroxide was determined by acid/base titration with several complementary methods including solution analyses of the reacted solutions and XRD characterization of the rea...The surface acidity of synthetic amorphous AI hydroxide was determined by acid/base titration with several complementary methods including solution analyses of the reacted solutions and XRD characterization of the reacted solids. The synthetic specimen was characterized to be the amorphous material showing four broad peaks in XRD pattern. XRD analyses of reacted solids after the titration experiments showed that amorphous AI hydroxide rapidly transformed to crystalline bayerite at the alkaline condition (pH〉10). The solution analyses after and during the titration Ksp=^aAl^3+/aH^+^3 ,was 10^10.3. The amount of consumption of added acid or base during the titration experiment was attributed to both the protonation/deprotonation of dissolved AI species and surface hydroxyl group. The surface acidity constants, surface hydroxyl density and specific surface area were estimated by FITEQL 4.0.展开更多
The sorption of a triazol derivative, 1-(4-chlorophenyl)- 4,4-dimethyl-2-(1H-1,2,4-triazol-1-yl)penten-3-ol with a common name of S3307D, on fifteen soils and three H_2O_2-treated soils was investigated. The sorption ...The sorption of a triazol derivative, 1-(4-chlorophenyl)- 4,4-dimethyl-2-(1H-1,2,4-triazol-1-yl)penten-3-ol with a common name of S3307D, on fifteen soils and three H_2O_2-treated soils was investigated. The sorption isotherm for each untreated and treated soil was non-linear, and was best fitted to Freundlich sorption equation. Soils containing high amount of clay content or organic matter or both sorbed much higher amounts of the chemical than soils that had low contents of these soil constituents. H_2O_2-treated soils showed considerable sorptive affinity for S3307D. It was concluded that both organic matter and mineral fraction in natural soils contributed to the sorption of the basic compound. Sorption by the H_2O_2 treated soils increased as suspension pH decreased, but all suspension pHs exceeded the pKa of the compound by more than two units. This implies that organic base protonation can occur on surfaces of soil components, and surface acidity (exchangeable acidity ) is important in sorption process of the organic base rather than suspension pH.展开更多
Excellent catalysts with low-temperature activity and relatively wide temperature window for selective catalytic reduction of NO with ammonia(NH_(3)-SCR) are highly demanded in view of the practical treatment of NO.He...Excellent catalysts with low-temperature activity and relatively wide temperature window for selective catalytic reduction of NO with ammonia(NH_(3)-SCR) are highly demanded in view of the practical treatment of NO.Herein,we have designed a highly active VOx-MnOx/CeO_(2) material based on the intrinsic requirement of SCR reaction for catalyst,namely redox sites and surface acid sites.The vanadium oxide and manganese oxide are highly dispersed over the ceria mesosphere via simple incipient wetness impregnation.The loading of manganese could introduce acid sites and enhance the redox property remarkably,while the loading of vanadium increases acid sites and weakens redox property.Through tentatively controlling the appropriate loading ratio of the two components,the optimal catalyst achieves a balance between redox property and surface acidity.The work shed light on the development of new SCR catalyst with superior low temperature activity,wide work temperature window and good hydrothermal stability.展开更多
Galena(PbS)and chalcopyrite(CuFeS_(2))are sulfide minerals that exhibit good floatability characteristics.Thus,efficiently separating them via common flotation is challenging.Herein,a new method of surface sulfuric ac...Galena(PbS)and chalcopyrite(CuFeS_(2))are sulfide minerals that exhibit good floatability characteristics.Thus,efficiently separating them via common flotation is challenging.Herein,a new method of surface sulfuric acid corrosion in conjunction with flotation separation was proposed,and the efficient separation of galena and chalcopyrite was successfully realized.Contact angle test results showed a substantial decrease in surface contact angle and a selective inhibition of surface floatability for corroded galena.Meanwhile,the contact angle and floatability of corroded chalcopyrite remained almost unaffected.Scanning electron microscope results confirmed that sulfuric acid corrosion led to the formation of a dense oxide layer on the galena surface,whereas the chalcopyrite surface remained unaltered.X-ray photoelectron spectroscopy results showed that the chemical state of S^(2-)on the surface of corroded galena was oxidized to SO_(4)^(2-).A layer of hydrophilic PbSO4was formed on the surface,leading to a sharp decrease in galena floatability.Meanwhile,new hydrophobic CuS_(2),CuS,and Cu_(1-x)Fe_(1-y)S_(2-z)species exhibiting good floatability were generated on the chalcopyrite surface.Finally,theoretical analysis results were further verified by corrosion–flotation separation experiments.The galena–chalcopyrite mixture was completely separated via flotation separation under appropriate corrosion acidity,corrosion temperature,and corrosion time.A novel approach has been outlined in this study,providing potential applications in the efficient separation of refractory copper–lead sulfide ore.展开更多
NOx emission abatement catalysts V 2O 5 supported on various TiO 2 including anatase, rutile and mixture of both were investigated with various physico\|chemical measurements such as BET, NH\-3\|TPD, NARP, XRD and ...NOx emission abatement catalysts V 2O 5 supported on various TiO 2 including anatase, rutile and mixture of both were investigated with various physico\|chemical measurements such as BET, NH\-3\|TPD, NARP, XRD and so on, and the effect of TiO\-2 surface properties on the SCR(selective catalytic reduction) activity of V\-2O\-5/TiO\-2 catalysts was studied. It was found that the TiO\-2 surface properties had strong affect on the SCR activity of V\-2O\-5/TiO\-2 catalysts. The stronger acidic property resulted in the higher exposure of active sites as well as the higher SCR activity.展开更多
One new polymer [Co(L)(H2O)2]n(1) was synthesized by 4-(ethoxycarbonyl)-5-methyl-1H-1,2,3-triazole-1-carboxylic acid(Emtc) under the in situ solvent thermal reaction(H2L = 1-(carboxymethyl)-5-methyl-1H-1,...One new polymer [Co(L)(H2O)2]n(1) was synthesized by 4-(ethoxycarbonyl)-5-methyl-1H-1,2,3-triazole-1-carboxylic acid(Emtc) under the in situ solvent thermal reaction(H2L = 1-(carboxymethyl)-5-methyl-1H-1,2,3-triazole-4-carboxylic acid). The title complex performs a wave-like 2D framework and the ligand H2L demonstrates the coordination mode as μ4-η-2:η-1η-1:η-1. The crystal structure has been established by single-crystal X-ray diffraction, and characterized by FT-IR. Fluorescent property was investigated in this work. Hirshfeld surface analysis has also been carried out on 1, and obvious main intermolecular interactions are observed.展开更多
Since 2-aminonicotinic acid is a zwitterionic molecule,the salt or co-crystal strategy was used for the precipitation under identical conditions and obtained two novel salts: salt 1 with 2:1:2 stoichiometry of 2-am...Since 2-aminonicotinic acid is a zwitterionic molecule,the salt or co-crystal strategy was used for the precipitation under identical conditions and obtained two novel salts: salt 1 with 2:1:2 stoichiometry of 2-aminonicotinic acid:perchloric acid:H2O and salt 2 with 2:1:3 stoichiometry of 2-aminonicotinic acid:sulfuric acid:H2O. Their crystal structures were characterized by single-crystal X-ray diffraction,differential scanning calorimetry(DSC) and thermogravimetric analyses(TGA). The structure determination shows that two salts are both primarily stabilized by the strong N–H…O hydrogen bonding interaction between 2-aminonicotinic acid and its corresponding acids. Constituents of the salt-crystalline phase were also investigated in terms of Hirshfeld surfaces. In the crystal lattice,a three-dimensional hydrogen-bonded network is observed,including the formation of a two-dimensional molecular scaffolding motif. Hirshfeld surfaces and fingerprint plots of two salts show that the structures are stabilized by H…H,O–H…O and C–O…π intermolecular interactions.展开更多
This article discussed the benzoic acid activated carbons which have changed the types and content of acid oxygen-function groups on the surface of activated carbons and their effect on the adsorption for Hg^0 in simu...This article discussed the benzoic acid activated carbons which have changed the types and content of acid oxygen-function groups on the surface of activated carbons and their effect on the adsorption for Hg^0 in simulated flue gas at 140 ℃. These surface acid oxygen function groups were identified by Boehm titration, Fourier transformation infrared spectrum, temperature programmed desorption and X-ray photoelectron spectroscopy. It indicates that the carboxyl, lactone and phenolic were formed when the benzoic acid is loaded on the surface of activated carbons. Among the surface acid oxygen function groups, the carboxyl groups enhance the adsorption capacities of Hg^0 for activated carbons to a greater extent.展开更多
Fibrous brucite,a kind of brucite with unique structure and physical properties,was modified with stearic acid as a surface modifier.In order to investigate the mechanism of surface modification,the fixation of steari...Fibrous brucite,a kind of brucite with unique structure and physical properties,was modified with stearic acid as a surface modifier.In order to investigate the mechanism of surface modification,the fixation of stearic acid on fibrous brucite and the induced changes in surface properties were studied by using X-ray diffraction(XRD),scanning electron microscopy(SEM),infrared spectroscopy(IR),Raman spectroscopy and thermo-gravimetric analysis(TGA).XRD analysis indicates that the modification of fibrous brucite with stearic acid does not cause any changes in the structure of fibrous brucite mineral.Spectroscopy and thermal analysis show that the surfactant molecules are not only directly adsorbed on the surface of the mineral,but also chemisorbed on mineral surface by forming chemical bonds between the modifier and magnesium hydroxide.展开更多
Tuning the surface acidity of ZSM-5 catalyst is essential to achieve desired propene selectivity and yield.Here several ratios of Zr were utilized to modify ZSM-5 via flame spray pyrolysis technique coupled with a pul...Tuning the surface acidity of ZSM-5 catalyst is essential to achieve desired propene selectivity and yield.Here several ratios of Zr were utilized to modify ZSM-5 via flame spray pyrolysis technique coupled with a pulse spray evaporation system.The interaction between Zr and ZSM-5 in the flame influenced the physicochemical and acidity properties of the Zr/ZSM-5.The increasing Zr ratio in ZSM-5 shows coated layers of irregular nano-sized Zr with an increase in crystallite sizes due to the synergetic effect between Zr and ZSM-5.The surface chemical analysis revealed increased lattice oxygen on the Zr modified ZSM-5(1:4) sample compared to other catalysts.The acidity analysis revealed the Lewis and Br?nsted acid distribution in the weak and medium acid sites on the catalyst surface.However,the increase in Zr loading decreased the concentration of Br?nsted acid sites and tuned the catalyst surface to more Lewis acidity,promoting propene selectivity and hindering the over-oxidation of propene.The modified ZSM-5 catalysts were examined in a fixed bed reactor within 300℃-700℃ at a gas hourly space velocity(GHSV) of 6000 mL·g(catalysts)^(-1)·h^(-1) for the oxidative dehydrogenation of propane(ODHP) to propene.Among the catalysts,Zr/ZSM-5(1:4) exhibited the best propene yield, with 57.19% propane conversion and 75.54% selectivity to propene and the highest stability.This work provides a promising strategy for tuning the surface acidity of ZSM-5 with Zr for ODHP applications.展开更多
Alkaline earth metal (Mg,Ca,Sr and Ba)-doped Mo-V-Sb-O x catalysts,prepared by a dry-up method,have been investigated for their catalytic performance in the oxidation of propane under different reaction conditions.T...Alkaline earth metal (Mg,Ca,Sr and Ba)-doped Mo-V-Sb-O x catalysts,prepared by a dry-up method,have been investigated for their catalytic performance in the oxidation of propane under different reaction conditions.The catalysts have been characterized by N2 adsorption-desorption,temperature-programmed desorption (TPD) of NH3,SEM and XRD.Influence of water vapor on the catalytic performance,particularly on the selectivities to acetic acid and acrylic acid,has also been studied.The selectivity to acrylic acid was improved significantly by the doping of alkaline earth metals to Mo-V-Sb-O x catalysts.The surface acidic sites of the catalyst decreased with the doping of the catalyst with alkaline earth metals,which ultimately was found to be beneficial for obtaining high selectivity to acrylic acid.The catalytic activity and product selectivities were found to be influenced by the reaction temperature,C3H8/O2 ratio and space velocity.A significant improvement in the selectivity to acrylic acid has also been observed by the addition of water vapor in the feed of propane and oxygen in the oxidation of propane.展开更多
Two acidic carbon materials (H-PRC and HS-C) were used as catalysts for the condensation reaction of methanol with formaldehyde to produce dimethoxymethane (DMM) in aqueous solution (hydrophilic system) and for ...Two acidic carbon materials (H-PRC and HS-C) were used as catalysts for the condensation reaction of methanol with formaldehyde to produce dimethoxymethane (DMM) in aqueous solution (hydrophilic system) and for the etherification of isopentene with methanol to produce tert amyl methyl ether (TAME) in toluene solution (lipophilic system). Microcalorimetric adsorptions of water and benzene showed that the HS-C was highly hydrophilic without the lipophilicity, while the H-PRC exhibited both the hydrophilicity and lipophilicity. Thus, the HS-C was well dispersed in aqueous solution and difficult to separate from it. On the other hand, the H-PRC was highly active, more active than the acidic resin (D008) and sulfuric acid, for the synthesis of DMM in aqueous solution. The H-PRC was also highly active, more active than the HS-C, for the etherification of isopentene with methanol to produce TAME in toluene solution, probably owing to its amphiphilic surface property as well as its strong surface acidity as measured by the microcalorirnetric adsorption of NH3.展开更多
A new zinc acetate catalyst which was prepared from modified activated carbon exhibited extreme activity towards the synthesis of vinyl acetate. The activated carbon was modified by nitric acid, vitriol and peroxyacet...A new zinc acetate catalyst which was prepared from modified activated carbon exhibited extreme activity towards the synthesis of vinyl acetate. The activated carbon was modified by nitric acid, vitriol and peroxyacetic acid (PAA). The effect on specific area, structure, pH and surface acidity groups of carders by modification was discussed. Amount of carbonyl and carboxyl groups in activated carbon was increased by peroxyacetic acid treatment. The productivity of the new catalyst was 14.58% higher than that of catalyst prepared using untreated activated carbon. The relationship between amount of carbonyl and carboxyl groups (m) and catalyst productivity (P) was P = 1.83 + 2.26 × 10^-3*e^3.17m. Reaction mechanism was proposed. C 2009 Liang Rong Feng. Published by Elsevier B.V. on behalf of Chinese Chemical Society. All rights reserved.展开更多
The decomposition of copper anode slime heated by microwave energy in a sulfuric acid medium was investigated. Leaching experiments were carried out in a multi-mode cavity with microwave assistance. The leaching proce...The decomposition of copper anode slime heated by microwave energy in a sulfuric acid medium was investigated. Leaching experiments were carried out in a multi-mode cavity with microwave assistance. The leaching process parameters were optimized using response surface methodology(RSM). Under the optimized conditions, the leaching efficiencies of copper and tellurium were 99.56% ± 0.16% and 98.68% ± 0.12%, respectively. Meanwhile, a conventional leaching experiment was performed in order to evaluate the influence of microwave radiation. The mechanism of microwave-assisted leaching of copper anode slime was also investigated. In the results, the microwave technology is demonstrated to have a great potential to improve the leaching efficiency and reduce the leaching time. The enhanced recoveries of copper and tellurium are believed to result from the presence of a temperature gradient due to the shallow microwave penetration depth and the superheating at the solid-liquid interface.展开更多
The cation exchange and the chemical weathering are two important processes for sedi-ments to buffer the acidification of surface water. In this paper, for sediments these two processeshave been studied. The relations...The cation exchange and the chemical weathering are two important processes for sedi-ments to buffer the acidification of surface water. In this paper, for sediments these two processeshave been studied. The relationship between BFC of sediments and ANC of the surface waters andthe weathering characteristics of sediments were discussed. The buffering effect and mechanism of sedi-ments against acidic deposition have also been studied. The results show that BFC of sediments arepositively correlative to ANC of the surface waters. the chemical weathering rate of sediments can beexpressed as R=k×[H ̄ +] ̄m.展开更多
In the study,the catalyst precursors of Ce-modifiedγ-MnO2 were washed with deionized water until the pH value of the supernatant was 1,2,4 and 7,and the obtained catalysts were named accordingly.Under space velocity ...In the study,the catalyst precursors of Ce-modifiedγ-MnO2 were washed with deionized water until the pH value of the supernatant was 1,2,4 and 7,and the obtained catalysts were named accordingly.Under space velocity of 300,000 hr-1,the ozone conversion over the pH=7 catalyst under dry conditions and relative humidity of 65%over a period of 6 hr was 100%and 96%,respectively.However,the ozone decomposition activity of the pH=2 and 4 catalysts distinctly decreased under relative humidity of 65%compared to that under dry conditions.Detailed physical and chemical characterization demonstrated that the residual sulfate ions on the pH=2 and 4 catalysts decreased their hydrophobicity and then restrained humid ozone decomposition activity.The pH=2 and 4 catalysts had inferior resistance to high space velocity under dry conditions,because the residual sulfate ion on their surface reduced their adsorption capacity for ozone molecules and increased their apparent activation energies,which was proved by temperature programmed desorption of O2 and kinetic experiments.Long-term activity testing,X-ray photoelectron spectroscopy and density functional theory calculations revealed that there were two kinds of oxygen vacancies on the manganese dioxide catalysts,one of which more easily adsorbed oxygen species and then became deactivated.This study revealed the detrimental effect of surface acid ions on the activity of catalysts under humid and dry atmospheres,and provided guidance for the development of highly efficient catalysts for ozone decomposition.展开更多
Fe304 was supported on mesoporous A12O3 or SiO2 (50 wt.%) using an incipient wetness impregnation method, and Fe304/A12O3 exhibited higher catalytic efficiency for the degradation of 2,4-dichlorophenoxyace- tic acid...Fe304 was supported on mesoporous A12O3 or SiO2 (50 wt.%) using an incipient wetness impregnation method, and Fe304/A12O3 exhibited higher catalytic efficiency for the degradation of 2,4-dichlorophenoxyace- tic acid andpara-chlorobenzoic acid aqueous solution with ozone. The effect and morphology of supported Fe304 on catalytic ozonation performance were investigated based on the characterization results of X-ray diffraction, X-ray photoelectron spectroscopy, BET analysis and Fourier transform infrared spectroscopy. The results indicated that the physical and chemical properties of the catalyst supports especially their Lewis acid sites had a significant influence on the catalytic activity. In comparison with SiO2, more Lewis acid sites existed on the surface of A12O3, resulting in higher catalytic ozonation activity. During the reaction process, no significant Fe ions release was observed. Moreover, Fe304/A12O3 exhibited stable structure and activity after successive cyclic experiments. The results indicated that the catalyst is a promising ozonation catalyst with magnetic separation in drinking water treatment.展开更多
In this study,the cytotoxicity of two different crystal phases of TiO2 nanoparticles,with surface modification by humic acid(HA),to Escherichia coli,was assessed.The physicochemical properties of TiO2 nanoparticles ...In this study,the cytotoxicity of two different crystal phases of TiO2 nanoparticles,with surface modification by humic acid(HA),to Escherichia coli,was assessed.The physicochemical properties of TiO2 nanoparticles were thoroughly characterized.Three different initial concentrations,namely 50,100,and 200 ppm,of HA were used for synthesis of HA coated TiO2 nanoparticles(denoted as A/RHA50,A/RHA100,and A/RHA200,respectively).Results indicate that rutile(LC50(concentration that causes 50%mortality compared the control group)=6.5)was more toxic than anatase(LC50=278.8)under simulated sunlight(SSL)irradiation,possibly due to an extremely narrow band gap.It is noted that HA coating increased the toxicity of anatase,but decreased that of rutile.Additionally,AHA50 and RHA50had the biggest differences compared to uncoated anatase and rutile with LC50of 201.9 and21.6,respectively.We then investigated the formation of reactive oxygen species(ROS)by TiO2 nanoparticles in terms of hydroxyl radicals(OH)and superoxide anions(O2^-).Data suggested that O2^- was the main ROS that accounted for the higher toxicity of rutile upon SSL irradiation.We also observed that HA coating decreased the generation of OH and O2^- on rutile,but increased O2^- formation on anatase.Results from TEM analysis also indicated that HA coated rutile tended to be attached to the surface of E.coli more than anatase.展开更多
Polypeptide brushes are attractive platforms to generate functional and responsive interfaces that are of potential interest due to their possible biodegradability, biocompatibility and tunable secondary structures. S...Polypeptide brushes are attractive platforms to generate functional and responsive interfaces that are of potential interest due to their possible biodegradability, biocompatibility and tunable secondary structures. Surface-initiated ringopening polymerization(SI-ROP) of α-amino acid N-carboxyanhydrides represents a powerful and versatile strategy to generate polypeptide brushes. This review is an attempt to capture the state-of-the-art in this field and highlights the latest developments in several selected areas. In addition to presenting an overview of the synthetic methods that have been used to generate polypeptide brushes via SI-ROP, this article will discuss the preparation of patterned polypeptide brushes, the conformational properties of surface-tethered polypeptides, ways to control chain orientation at surfaces as well as properties and applications of these thin polymer films.展开更多
Complex organics contained in dye wastewater are difficult to degrade and often require electrochemical advanced oxidation processes(EAOPs) to treat it. Surface activation of the electrode used in such treatment is ...Complex organics contained in dye wastewater are difficult to degrade and often require electrochemical advanced oxidation processes(EAOPs) to treat it. Surface activation of the electrode used in such treatment is an important factor determining the success of the process.The performance of boron-doped nanocrystalline diamond(BD-NCD) film electrode for decolorization of Acid Yellow(AY-36) azo dye with respect to the surface activation by electrochemical polarization was studied. Anodic polarization found to be more suitable as electrode pretreatment compared to cathodic one. After anodic polarization, the originally H-terminated surface of BD-NCD was changed into O-terminated, making it more hydrophilic.Due to the oxidation of surface functional groups and some portion of sp2 carbon in the BD-NCD film during anodic polarization, the electrode was successfully being activated showing lower background current, wider potential window and considerably less surface activity compared to the non-polarized one. Consequently, electrooxidation(EO) capability of the anodically-polarized BD-NCD to degrade AY-36 dye was significantly enhanced, capable of nearly total decolorization and chemical oxygen demand(COD) removal even after several times of re-using. The BD-NCD film electrode favored acidic condition for the dye degradation; and the presence of chloride ion in the solution was found to be more advantageous than sulfate active species.展开更多
文摘The surface acidity of synthetic amorphous AI hydroxide was determined by acid/base titration with several complementary methods including solution analyses of the reacted solutions and XRD characterization of the reacted solids. The synthetic specimen was characterized to be the amorphous material showing four broad peaks in XRD pattern. XRD analyses of reacted solids after the titration experiments showed that amorphous AI hydroxide rapidly transformed to crystalline bayerite at the alkaline condition (pH〉10). The solution analyses after and during the titration Ksp=^aAl^3+/aH^+^3 ,was 10^10.3. The amount of consumption of added acid or base during the titration experiment was attributed to both the protonation/deprotonation of dissolved AI species and surface hydroxyl group. The surface acidity constants, surface hydroxyl density and specific surface area were estimated by FITEQL 4.0.
文摘The sorption of a triazol derivative, 1-(4-chlorophenyl)- 4,4-dimethyl-2-(1H-1,2,4-triazol-1-yl)penten-3-ol with a common name of S3307D, on fifteen soils and three H_2O_2-treated soils was investigated. The sorption isotherm for each untreated and treated soil was non-linear, and was best fitted to Freundlich sorption equation. Soils containing high amount of clay content or organic matter or both sorbed much higher amounts of the chemical than soils that had low contents of these soil constituents. H_2O_2-treated soils showed considerable sorptive affinity for S3307D. It was concluded that both organic matter and mineral fraction in natural soils contributed to the sorption of the basic compound. Sorption by the H_2O_2 treated soils increased as suspension pH decreased, but all suspension pHs exceeded the pKa of the compound by more than two units. This implies that organic base protonation can occur on surfaces of soil components, and surface acidity (exchangeable acidity ) is important in sorption process of the organic base rather than suspension pH.
基金Project supported by the National Natural Science Foundation of China (21576054)Science and Technology Planning of Guangdong Province (2016B020241003)+1 种基金Natural Science Foundation of Guangdong Province(2018A030310563)Foundation of Higher Education of Guangdong Province(2018KZDXM031)。
文摘Excellent catalysts with low-temperature activity and relatively wide temperature window for selective catalytic reduction of NO with ammonia(NH_(3)-SCR) are highly demanded in view of the practical treatment of NO.Herein,we have designed a highly active VOx-MnOx/CeO_(2) material based on the intrinsic requirement of SCR reaction for catalyst,namely redox sites and surface acid sites.The vanadium oxide and manganese oxide are highly dispersed over the ceria mesosphere via simple incipient wetness impregnation.The loading of manganese could introduce acid sites and enhance the redox property remarkably,while the loading of vanadium increases acid sites and weakens redox property.Through tentatively controlling the appropriate loading ratio of the two components,the optimal catalyst achieves a balance between redox property and surface acidity.The work shed light on the development of new SCR catalyst with superior low temperature activity,wide work temperature window and good hydrothermal stability.
基金financially supported by the National Natural Science Foundation of China(No.52064027)Yunnan Major Scientific and Technological Projects,China(No.202202AG050015)。
文摘Galena(PbS)and chalcopyrite(CuFeS_(2))are sulfide minerals that exhibit good floatability characteristics.Thus,efficiently separating them via common flotation is challenging.Herein,a new method of surface sulfuric acid corrosion in conjunction with flotation separation was proposed,and the efficient separation of galena and chalcopyrite was successfully realized.Contact angle test results showed a substantial decrease in surface contact angle and a selective inhibition of surface floatability for corroded galena.Meanwhile,the contact angle and floatability of corroded chalcopyrite remained almost unaffected.Scanning electron microscope results confirmed that sulfuric acid corrosion led to the formation of a dense oxide layer on the galena surface,whereas the chalcopyrite surface remained unaltered.X-ray photoelectron spectroscopy results showed that the chemical state of S^(2-)on the surface of corroded galena was oxidized to SO_(4)^(2-).A layer of hydrophilic PbSO4was formed on the surface,leading to a sharp decrease in galena floatability.Meanwhile,new hydrophobic CuS_(2),CuS,and Cu_(1-x)Fe_(1-y)S_(2-z)species exhibiting good floatability were generated on the chalcopyrite surface.Finally,theoretical analysis results were further verified by corrosion–flotation separation experiments.The galena–chalcopyrite mixture was completely separated via flotation separation under appropriate corrosion acidity,corrosion temperature,and corrosion time.A novel approach has been outlined in this study,providing potential applications in the efficient separation of refractory copper–lead sulfide ore.
文摘NOx emission abatement catalysts V 2O 5 supported on various TiO 2 including anatase, rutile and mixture of both were investigated with various physico\|chemical measurements such as BET, NH\-3\|TPD, NARP, XRD and so on, and the effect of TiO\-2 surface properties on the SCR(selective catalytic reduction) activity of V\-2O\-5/TiO\-2 catalysts was studied. It was found that the TiO\-2 surface properties had strong affect on the SCR activity of V\-2O\-5/TiO\-2 catalysts. The stronger acidic property resulted in the higher exposure of active sites as well as the higher SCR activity.
基金Supported by the financial support of Fundamental Research Funds for the Central Universities(3207045420)Jiangsu Ainaji Neoenergy Science&Technology Co.,Ltd.(8507040091)
文摘One new polymer [Co(L)(H2O)2]n(1) was synthesized by 4-(ethoxycarbonyl)-5-methyl-1H-1,2,3-triazole-1-carboxylic acid(Emtc) under the in situ solvent thermal reaction(H2L = 1-(carboxymethyl)-5-methyl-1H-1,2,3-triazole-4-carboxylic acid). The title complex performs a wave-like 2D framework and the ligand H2L demonstrates the coordination mode as μ4-η-2:η-1η-1:η-1. The crystal structure has been established by single-crystal X-ray diffraction, and characterized by FT-IR. Fluorescent property was investigated in this work. Hirshfeld surface analysis has also been carried out on 1, and obvious main intermolecular interactions are observed.
基金supported by the prospective joint research project of Jiangsu province(BY20122193)the Fundamental Research Funds for the Central Universities(CXZZ12_0119)
文摘Since 2-aminonicotinic acid is a zwitterionic molecule,the salt or co-crystal strategy was used for the precipitation under identical conditions and obtained two novel salts: salt 1 with 2:1:2 stoichiometry of 2-aminonicotinic acid:perchloric acid:H2O and salt 2 with 2:1:3 stoichiometry of 2-aminonicotinic acid:sulfuric acid:H2O. Their crystal structures were characterized by single-crystal X-ray diffraction,differential scanning calorimetry(DSC) and thermogravimetric analyses(TGA). The structure determination shows that two salts are both primarily stabilized by the strong N–H…O hydrogen bonding interaction between 2-aminonicotinic acid and its corresponding acids. Constituents of the salt-crystalline phase were also investigated in terms of Hirshfeld surfaces. In the crystal lattice,a three-dimensional hydrogen-bonded network is observed,including the formation of a two-dimensional molecular scaffolding motif. Hirshfeld surfaces and fingerprint plots of two salts show that the structures are stabilized by H…H,O–H…O and C–O…π intermolecular interactions.
文摘This article discussed the benzoic acid activated carbons which have changed the types and content of acid oxygen-function groups on the surface of activated carbons and their effect on the adsorption for Hg^0 in simulated flue gas at 140 ℃. These surface acid oxygen function groups were identified by Boehm titration, Fourier transformation infrared spectrum, temperature programmed desorption and X-ray photoelectron spectroscopy. It indicates that the carboxyl, lactone and phenolic were formed when the benzoic acid is loaded on the surface of activated carbons. Among the surface acid oxygen function groups, the carboxyl groups enhance the adsorption capacities of Hg^0 for activated carbons to a greater extent.
基金Funded by National Natural Science Foundation of China(No.51274015)
文摘Fibrous brucite,a kind of brucite with unique structure and physical properties,was modified with stearic acid as a surface modifier.In order to investigate the mechanism of surface modification,the fixation of stearic acid on fibrous brucite and the induced changes in surface properties were studied by using X-ray diffraction(XRD),scanning electron microscopy(SEM),infrared spectroscopy(IR),Raman spectroscopy and thermo-gravimetric analysis(TGA).XRD analysis indicates that the modification of fibrous brucite with stearic acid does not cause any changes in the structure of fibrous brucite mineral.Spectroscopy and thermal analysis show that the surfactant molecules are not only directly adsorbed on the surface of the mineral,but also chemisorbed on mineral surface by forming chemical bonds between the modifier and magnesium hydroxide.
基金financial support from the National Natural Science Foundation of China (No. 52161145105/51888103/51976216)Ministry of Science and Technology of China (2017YFA0402800)+5 种基金Beijing Municipal Natural Science Foundation (JQ20017)K.C. Wong Education Foundation (GJTD-2020-07)Recruitment of Global Youth Expertsthe financial support of the Belt and Road scholarshipthe financial support of the ANSO scholarshipthe support of the Chinese Academy of Sciences for the CAS project (Grant No.2018/43)。
文摘Tuning the surface acidity of ZSM-5 catalyst is essential to achieve desired propene selectivity and yield.Here several ratios of Zr were utilized to modify ZSM-5 via flame spray pyrolysis technique coupled with a pulse spray evaporation system.The interaction between Zr and ZSM-5 in the flame influenced the physicochemical and acidity properties of the Zr/ZSM-5.The increasing Zr ratio in ZSM-5 shows coated layers of irregular nano-sized Zr with an increase in crystallite sizes due to the synergetic effect between Zr and ZSM-5.The surface chemical analysis revealed increased lattice oxygen on the Zr modified ZSM-5(1:4) sample compared to other catalysts.The acidity analysis revealed the Lewis and Br?nsted acid distribution in the weak and medium acid sites on the catalyst surface.However,the increase in Zr loading decreased the concentration of Br?nsted acid sites and tuned the catalyst surface to more Lewis acidity,promoting propene selectivity and hindering the over-oxidation of propene.The modified ZSM-5 catalysts were examined in a fixed bed reactor within 300℃-700℃ at a gas hourly space velocity(GHSV) of 6000 mL·g(catalysts)^(-1)·h^(-1) for the oxidative dehydrogenation of propane(ODHP) to propene.Among the catalysts,Zr/ZSM-5(1:4) exhibited the best propene yield, with 57.19% propane conversion and 75.54% selectivity to propene and the highest stability.This work provides a promising strategy for tuning the surface acidity of ZSM-5 with Zr for ODHP applications.
文摘Alkaline earth metal (Mg,Ca,Sr and Ba)-doped Mo-V-Sb-O x catalysts,prepared by a dry-up method,have been investigated for their catalytic performance in the oxidation of propane under different reaction conditions.The catalysts have been characterized by N2 adsorption-desorption,temperature-programmed desorption (TPD) of NH3,SEM and XRD.Influence of water vapor on the catalytic performance,particularly on the selectivities to acetic acid and acrylic acid,has also been studied.The selectivity to acrylic acid was improved significantly by the doping of alkaline earth metals to Mo-V-Sb-O x catalysts.The surface acidic sites of the catalyst decreased with the doping of the catalyst with alkaline earth metals,which ultimately was found to be beneficial for obtaining high selectivity to acrylic acid.The catalytic activity and product selectivities were found to be influenced by the reaction temperature,C3H8/O2 ratio and space velocity.A significant improvement in the selectivity to acrylic acid has also been observed by the addition of water vapor in the feed of propane and oxygen in the oxidation of propane.
文摘Two acidic carbon materials (H-PRC and HS-C) were used as catalysts for the condensation reaction of methanol with formaldehyde to produce dimethoxymethane (DMM) in aqueous solution (hydrophilic system) and for the etherification of isopentene with methanol to produce tert amyl methyl ether (TAME) in toluene solution (lipophilic system). Microcalorimetric adsorptions of water and benzene showed that the HS-C was highly hydrophilic without the lipophilicity, while the H-PRC exhibited both the hydrophilicity and lipophilicity. Thus, the HS-C was well dispersed in aqueous solution and difficult to separate from it. On the other hand, the H-PRC was highly active, more active than the acidic resin (D008) and sulfuric acid, for the synthesis of DMM in aqueous solution. The H-PRC was also highly active, more active than the HS-C, for the etherification of isopentene with methanol to produce TAME in toluene solution, probably owing to its amphiphilic surface property as well as its strong surface acidity as measured by the microcalorirnetric adsorption of NH3.
文摘A new zinc acetate catalyst which was prepared from modified activated carbon exhibited extreme activity towards the synthesis of vinyl acetate. The activated carbon was modified by nitric acid, vitriol and peroxyacetic acid (PAA). The effect on specific area, structure, pH and surface acidity groups of carders by modification was discussed. Amount of carbonyl and carboxyl groups in activated carbon was increased by peroxyacetic acid treatment. The productivity of the new catalyst was 14.58% higher than that of catalyst prepared using untreated activated carbon. The relationship between amount of carbonyl and carboxyl groups (m) and catalyst productivity (P) was P = 1.83 + 2.26 × 10^-3*e^3.17m. Reaction mechanism was proposed. C 2009 Liang Rong Feng. Published by Elsevier B.V. on behalf of Chinese Chemical Society. All rights reserved.
基金financially supported by the National Science and Technology Support Program of China during the 12th Five-Year Plan Period (No. 2012BAE06B05)the Fundamental Research Funds for the Central Universities of China (No. N130602004)
文摘The decomposition of copper anode slime heated by microwave energy in a sulfuric acid medium was investigated. Leaching experiments were carried out in a multi-mode cavity with microwave assistance. The leaching process parameters were optimized using response surface methodology(RSM). Under the optimized conditions, the leaching efficiencies of copper and tellurium were 99.56% ± 0.16% and 98.68% ± 0.12%, respectively. Meanwhile, a conventional leaching experiment was performed in order to evaluate the influence of microwave radiation. The mechanism of microwave-assisted leaching of copper anode slime was also investigated. In the results, the microwave technology is demonstrated to have a great potential to improve the leaching efficiency and reduce the leaching time. The enhanced recoveries of copper and tellurium are believed to result from the presence of a temperature gradient due to the shallow microwave penetration depth and the superheating at the solid-liquid interface.
文摘The cation exchange and the chemical weathering are two important processes for sedi-ments to buffer the acidification of surface water. In this paper, for sediments these two processeshave been studied. The relationship between BFC of sediments and ANC of the surface waters andthe weathering characteristics of sediments were discussed. The buffering effect and mechanism of sedi-ments against acidic deposition have also been studied. The results show that BFC of sediments arepositively correlative to ANC of the surface waters. the chemical weathering rate of sediments can beexpressed as R=k×[H ̄ +] ̄m.
基金supported by the National Key R&D Program of China(Nos.2016YFC0207104 and 2017YFC0211802)the National Natural Science Foundation of China(NSFC)(No.21876191)the Youth Innovation Promotion Association,CAS(No.2017064)
文摘In the study,the catalyst precursors of Ce-modifiedγ-MnO2 were washed with deionized water until the pH value of the supernatant was 1,2,4 and 7,and the obtained catalysts were named accordingly.Under space velocity of 300,000 hr-1,the ozone conversion over the pH=7 catalyst under dry conditions and relative humidity of 65%over a period of 6 hr was 100%and 96%,respectively.However,the ozone decomposition activity of the pH=2 and 4 catalysts distinctly decreased under relative humidity of 65%compared to that under dry conditions.Detailed physical and chemical characterization demonstrated that the residual sulfate ions on the pH=2 and 4 catalysts decreased their hydrophobicity and then restrained humid ozone decomposition activity.The pH=2 and 4 catalysts had inferior resistance to high space velocity under dry conditions,because the residual sulfate ion on their surface reduced their adsorption capacity for ozone molecules and increased their apparent activation energies,which was proved by temperature programmed desorption of O2 and kinetic experiments.Long-term activity testing,X-ray photoelectron spectroscopy and density functional theory calculations revealed that there were two kinds of oxygen vacancies on the manganese dioxide catalysts,one of which more easily adsorbed oxygen species and then became deactivated.This study revealed the detrimental effect of surface acid ions on the activity of catalysts under humid and dry atmospheres,and provided guidance for the development of highly efficient catalysts for ozone decomposition.
文摘Fe304 was supported on mesoporous A12O3 or SiO2 (50 wt.%) using an incipient wetness impregnation method, and Fe304/A12O3 exhibited higher catalytic efficiency for the degradation of 2,4-dichlorophenoxyace- tic acid andpara-chlorobenzoic acid aqueous solution with ozone. The effect and morphology of supported Fe304 on catalytic ozonation performance were investigated based on the characterization results of X-ray diffraction, X-ray photoelectron spectroscopy, BET analysis and Fourier transform infrared spectroscopy. The results indicated that the physical and chemical properties of the catalyst supports especially their Lewis acid sites had a significant influence on the catalytic activity. In comparison with SiO2, more Lewis acid sites existed on the surface of A12O3, resulting in higher catalytic ozonation activity. During the reaction process, no significant Fe ions release was observed. Moreover, Fe304/A12O3 exhibited stable structure and activity after successive cyclic experiments. The results indicated that the catalyst is a promising ozonation catalyst with magnetic separation in drinking water treatment.
基金supported in part by the NSF-REU program(National Science Foundation-Research Experiences for Undergraduates,No.#CHE-1156111)the NSF-CREST program(National Science Foundation-Centers of Research Excellencein Science and Technology,No.#HRD-0833178)
文摘In this study,the cytotoxicity of two different crystal phases of TiO2 nanoparticles,with surface modification by humic acid(HA),to Escherichia coli,was assessed.The physicochemical properties of TiO2 nanoparticles were thoroughly characterized.Three different initial concentrations,namely 50,100,and 200 ppm,of HA were used for synthesis of HA coated TiO2 nanoparticles(denoted as A/RHA50,A/RHA100,and A/RHA200,respectively).Results indicate that rutile(LC50(concentration that causes 50%mortality compared the control group)=6.5)was more toxic than anatase(LC50=278.8)under simulated sunlight(SSL)irradiation,possibly due to an extremely narrow band gap.It is noted that HA coating increased the toxicity of anatase,but decreased that of rutile.Additionally,AHA50 and RHA50had the biggest differences compared to uncoated anatase and rutile with LC50of 201.9 and21.6,respectively.We then investigated the formation of reactive oxygen species(ROS)by TiO2 nanoparticles in terms of hydroxyl radicals(OH)and superoxide anions(O2^-).Data suggested that O2^- was the main ROS that accounted for the higher toxicity of rutile upon SSL irradiation.We also observed that HA coating decreased the generation of OH and O2^- on rutile,but increased O2^- formation on anatase.Results from TEM analysis also indicated that HA coated rutile tended to be attached to the surface of E.coli more than anatase.
基金financially supported by the Sino-Swiss Science and Technology Cooperation(No.EG41-092011)as well as the Chinese Academy of Sciences(Visiting Professorship for Senior International Scientists to H.A.K.)
文摘Polypeptide brushes are attractive platforms to generate functional and responsive interfaces that are of potential interest due to their possible biodegradability, biocompatibility and tunable secondary structures. Surface-initiated ringopening polymerization(SI-ROP) of α-amino acid N-carboxyanhydrides represents a powerful and versatile strategy to generate polypeptide brushes. This review is an attempt to capture the state-of-the-art in this field and highlights the latest developments in several selected areas. In addition to presenting an overview of the synthetic methods that have been used to generate polypeptide brushes via SI-ROP, this article will discuss the preparation of patterned polypeptide brushes, the conformational properties of surface-tethered polypeptides, ways to control chain orientation at surfaces as well as properties and applications of these thin polymer films.
基金financially supported by "National" Science Council of Taiwan by Grant NSC 99-2221-E-009-042Ministry of Economic Affairs of Taiwan by Grant 101-EC-17-A-08-S1-208
文摘Complex organics contained in dye wastewater are difficult to degrade and often require electrochemical advanced oxidation processes(EAOPs) to treat it. Surface activation of the electrode used in such treatment is an important factor determining the success of the process.The performance of boron-doped nanocrystalline diamond(BD-NCD) film electrode for decolorization of Acid Yellow(AY-36) azo dye with respect to the surface activation by electrochemical polarization was studied. Anodic polarization found to be more suitable as electrode pretreatment compared to cathodic one. After anodic polarization, the originally H-terminated surface of BD-NCD was changed into O-terminated, making it more hydrophilic.Due to the oxidation of surface functional groups and some portion of sp2 carbon in the BD-NCD film during anodic polarization, the electrode was successfully being activated showing lower background current, wider potential window and considerably less surface activity compared to the non-polarized one. Consequently, electrooxidation(EO) capability of the anodically-polarized BD-NCD to degrade AY-36 dye was significantly enhanced, capable of nearly total decolorization and chemical oxygen demand(COD) removal even after several times of re-using. The BD-NCD film electrode favored acidic condition for the dye degradation; and the presence of chloride ion in the solution was found to be more advantageous than sulfate active species.