The conversion of carbon dioxide to chemicals by the electrochemical reactions(ERC)is an efficient solution to the current energy crisis and excess CO_(2) emissions.It is still a great challenge and of significance to...The conversion of carbon dioxide to chemicals by the electrochemical reactions(ERC)is an efficient solution to the current energy crisis and excess CO_(2) emissions.It is still a great challenge and of significance to synthesize a highly selective,efficient,and non-noble metal electrocatalyst that facilitates the ERC reaction.A novel triton X-100(C_(14)H_(22)O(C_(2)H_(4)O)n)assisted electrodeposition method was developed to synthesize the ordered cone-structured tin(OCSn)electrocatalysts with controllable morphology and structure.The results suggest that Triton X-100 plays an important role in directing the structure of the Sn electrocatalysts during the electrodeposition process.The OCSn synthesized at 60 m A cm^(-2) achieves the best performances.It selectively catalyzes the ERC on the onset potential about 110 m V lower than Sn synthesized without Triton X-100.In 0.5 M Na HCO_(3),high faradaic efficiency(92%)for formate product on OCSn has been achieved.More prominently,the catalyst presents excellent stability,showing no performance deterioration during 30 h electrolysis.This work provides an efficient,green,and scalable synthesis method of the electrocatalyst for CO_(2) reduction to formate.展开更多
A novel ion-imprinted polymer, lead ion-imprinted micro-beads with combination of two functional monomers, was synthesized using the W/O/W polymerization method. Two functional monomers, 1,12-dodecanediol-O,O’-diphen...A novel ion-imprinted polymer, lead ion-imprinted micro-beads with combination of two functional monomers, was synthesized using the W/O/W polymerization method. Two functional monomers, 1,12-dodecanediol-O,O’-diphenyl-phosphonic acid (DDDPA) and 4-vinylpyridine, were used to form a suitable construction with micro-pores fitting the template and recognition sites. The eflects of adsorbent dosage, solution pH and the competitive ions on the adsorption and separation eflciency of lead ions were investigated. The lead ion-imprinted micro-beads were eflcient for lead ions removal from aqueous solution in a broad pH range (4–9), when the adsorbent dosage was above 0.1 g/L. The adsorption process obeyed the pseudo second-order kinetics model and it only took half an hour to reach the equilibrium. The adsorption isotherm of lead ion was described by the Langmuir model (R2 0.99) with a maximum adsorption capacity of 116.9 mg/g. In the presence of competitive ions Co2+ and Cd2+, the lead ion-imprinted micro-beads showed a high selectivity for lead ions. The selectivity coeficient of Pb2+/Cd2+ and Pb2+/Co2+are 99.3 and 114.7, respectively.展开更多
The effects of ferric ion, pH, and bromide on the formation and distribution of disinfection byproducts (DBPs) during chlorination were studied. Two raw water samples from Huangpu River and Yangtze River, two typica...The effects of ferric ion, pH, and bromide on the formation and distribution of disinfection byproducts (DBPs) during chlorination were studied. Two raw water samples from Huangpu River and Yangtze River, two typical drinking water sources of Shanghai, were used for the investigation. Compared with the samples from Huangpu River, the raw water samples from Yangtze River had lower content of total organic carbon (TOC) and ferric ions, but higher bromide concentrations. Under controlled chlorination conditions, four trihalomethanes (THMs), nine haloacetic acids (HAAs), total organic halogen (TOX) and its halogen species fractions, including total organic chlorine (TOC1) and total organic bromide (TOBr), were determined. The results showed that co-existent ferric and bromide ions significantly promoted the formation of total THMs and HAAs for both raw water samples. Higher concentration of bromide ions significantly changed the speciation of the formed THMs and HAAs. There was an obvious shift to brominated species, which might result in a more adverse influence on the safety of drinking water. The results also indicated that high levels of bromide ions in raw water samples produced higher percentages of unknown TOBr.展开更多
The mesoporous Cu/Mg/Fe layered double hydroxide(Cu/Mg/Fe-LDH) with carbonate intercalation was synthesized and used for the removal of arsenate from aqueous solutions.The Cu/Mg/Fe-LDH was characterized by Fourier t...The mesoporous Cu/Mg/Fe layered double hydroxide(Cu/Mg/Fe-LDH) with carbonate intercalation was synthesized and used for the removal of arsenate from aqueous solutions.The Cu/Mg/Fe-LDH was characterized by Fourier transform infrared spectrometry,X-ray diffraction crystallography,scanning electron microscopy,X-ray photoelectron spectroscopy and Brunauer-Emmett-Teller.Effects of various physico-chemical parameters such as pH,adsorbent dosage,contact time and initial arsenate concentration on the adsorption of arsenate onto Cu/Mg/Fe-LDH were investigated.Results showed that it was efficient for the removal of arsenate,and the removal efficiency of arsenate increased with the increment of the adsorbent dosage,while the arsenate adsorption capacity decreased with increase of initial pH from 3 to 11.The adsorption isotherms can be well described by the Langmuir model with R 2 〉 0.99.Its adsorption kinetics followed the pseudo second-order kinetic model.Coexisting ions such as HPO42-,CO32-,SO42and NO3could compete with arsenate for adsorption sites on the Cu/Mg/Fe-LDH.The adsorption of arsenate on the adsorbent can be mainly attributed to the ion exchange process.It was found that the synthesized Cu/Mg/Fe-LDH can reduce the arsenate concentration down to a final level of 〈 10 μg/L under the experimental conditions,and makes it a potential material for the decontamination of arsenate polluted water.展开更多
For the system of water samples collected from Yangtze River,the effects of seasonal variation and Fe(III) concentrations on the formation and distribution of trihalomethanes (THMs) during chlorination have been i...For the system of water samples collected from Yangtze River,the effects of seasonal variation and Fe(III) concentrations on the formation and distribution of trihalomethanes (THMs) during chlorination have been investigated.The corresponding lifetime cancer risk of the formed THMs to human beings was estimated using the parameters and procedure issued by the US EPA.The results indicated that the average concentration of THMs (100.81 μg/L) in spring was significantly higher than that in other seasons,which was related to the higher bromide ion concentration resulted from the intrusion of tidal saltwater.The total cancer risk in spring reached 8.23 × 10 ?5 and 8.86 × 10 ?5 for males and females,respectively,which were about two times of those in summer under the experimental conditions.Furthermore,it was found that the presence of Fe(III) resulted in the increased level of THMs and greater cancer risk from exposure to humans.Under weak basic conditions,about 10% of the increment of THMs from the water samples in spring was found in the presence of 0.5 mg/L Fe(III) compared with the situation without Fe(III).More attention should be given to the effect of the coexistence of Fe(III) and bromide ions on the risk assessment of human intake of THMs from drinking water should be paid more attention,especially in the coastland and estuaries.展开更多
Natural zeolite was modified by loading cetylpyridinium bromide (CPB) to create more efficient sites for humic acid (HA) adsorption. The natural and CPB modified zeolites were characterized with X-ray diffraction,...Natural zeolite was modified by loading cetylpyridinium bromide (CPB) to create more efficient sites for humic acid (HA) adsorption. The natural and CPB modified zeolites were characterized with X-ray diffraction, field emission scanning electron microscopy, Fourier transform infrared spectroscopy and elemental analysis. The effects of various experimental parameters such as contact time, initial HA concentration, solution pH and coexistent Ca^2+, upon HA adsorption onto CPB modified zeolites were evaluated. The results showed that natural zeolite had negligible affinity for HA in aqueous solutions, but CPB modified zeolites exhibited high adsorption efficiency for HA. A higher CPB loading on natural zeolites exhibited a larger HA adsorption capacity. Acidic pH and coexistent Ca^2+ were proved to be favorable for HA adsorption onto CPB modified zeolite. The kinetic process was well described by pseudo second-order model. The experimental isotherm data fitted well to Langmuir and Sips models. The maximum monolayer adsorption capacity of CPB modified zeolite with surfactant bilayer coverage was found to be 92.0 mg/g.展开更多
Surfactant-modified natural zeolites(SMNZ)with different coverage types were prepared by loading hexadecyltrimethyl ammonium bromide(HTAB)onto the surface of a natural zeolite.The adsorption behavior of humic acid(HA)...Surfactant-modified natural zeolites(SMNZ)with different coverage types were prepared by loading hexadecyltrimethyl ammonium bromide(HTAB)onto the surface of a natural zeolite.The adsorption behavior of humic acid(HA)on SMNZ was investigated.Results indicate that the adsorbent SMNZ exhibited a higher affinity toward HA than the natural zeolite.HA removal efficiency by SMNZ increased with HTAB loading.Coexisting Ca2+in solution favored HA adsorption onto SMNZ.Adsorption capacity decreased with an increasing solution pH.For typical SMNZ with bilayer HTAB coverage,HA adsorption process is well described by a pseudo-second-order kinetic model.The experimental isotherm data fitted well with the Langmuir model.Calculated maximum HA adsorption capacities for SMNZ with bilayer HTAB coverage at pH 5.5 and 7.5 were 63 and 41 mg·g^(-1),respectively.E2/E3(absorbance at 250 nm to that at 365 nm)and E4/E6(absorbance at 465 nm to that at 665 nm)ratios of the residual HA in solution were lower than that of the original HA solution.This indicates that the HA fractions with high polar functional groups,low molecular weight(MW),and aromaticity had a stronger tendency for adsorption onto SMNZ with bilayer HTAB coverage.Results show that HTABmodified natural zeolite is a promising adsorbent for removal of HA from aqueous solution.展开更多
The dissociation constants of polyepoxysuccinic acid(PESA)were investigated in this study.Based on the potentiometric titration and the BEST program,the dissociation constants of PESA were determined.Considering the c...The dissociation constants of polyepoxysuccinic acid(PESA)were investigated in this study.Based on the potentiometric titration and the BEST program,the dissociation constants of PESA were determined.Considering the complexity of the dissociation of PESA in aqueous solution,several models were constructed to simulate the dissociation process of PESA.By comparison,the dissociation constants of PESA were obtained with model 4.The species distribution of PESA in aqueous solution as a function of pH was also presented according to the experimental and calculation results.It showed that the H_(2)L model with five basic structure units to describe the dissociation of PESA was reasonable,and the relevant constants had less error and better matching between the experimental and calculation data.The corresponding values of pK_(ai) were 4.68 and 4.92,respectively,for H2L at 35℃ with ionic strength of 0.1 mol/L.展开更多
A novel composite adsorbent, hydroxyapatite/ manganese dioxide (HAp/MnO2), has been developed for the purpose of removing lead ions from aqueous solutions. The combination of HAp with MnO2 is meant to increase its a...A novel composite adsorbent, hydroxyapatite/ manganese dioxide (HAp/MnO2), has been developed for the purpose of removing lead ions from aqueous solutions. The combination of HAp with MnO2 is meant to increase its adsorption capacity. Various factors that may affect the adsorption efficiency, including solution pH, coexistent substances such as humic acid and competing cations (Ca2+, Mg2+), initial solute concentration, and the duration of the reaction, have been investigated. Using this composite adsorbent, solution pH and coexistent calcium or magnesium cations were found to have no significant influence on the removal of lead ions under the experi- mental conditions. The adsorption equilibrium was described well by the Langmuir isotherm model, and the calculated maximum adsorption capacity was 769 mg. gl. The sorption processes obeyed the pseudo-second-order kinetics model. The experimental results indicate that HAp/MnO2 composite may be an effective adsorbent for the removal of lead ions from aqueous solutions.展开更多
基金the financially support of the National Natural Science Foundation of China(No.21576255 and No.21577141)Dalian Science Fund for Distinguished Young Scholars(2018RJ09)。
文摘The conversion of carbon dioxide to chemicals by the electrochemical reactions(ERC)is an efficient solution to the current energy crisis and excess CO_(2) emissions.It is still a great challenge and of significance to synthesize a highly selective,efficient,and non-noble metal electrocatalyst that facilitates the ERC reaction.A novel triton X-100(C_(14)H_(22)O(C_(2)H_(4)O)n)assisted electrodeposition method was developed to synthesize the ordered cone-structured tin(OCSn)electrocatalysts with controllable morphology and structure.The results suggest that Triton X-100 plays an important role in directing the structure of the Sn electrocatalysts during the electrodeposition process.The OCSn synthesized at 60 m A cm^(-2) achieves the best performances.It selectively catalyzes the ERC on the onset potential about 110 m V lower than Sn synthesized without Triton X-100.In 0.5 M Na HCO_(3),high faradaic efficiency(92%)for formate product on OCSn has been achieved.More prominently,the catalyst presents excellent stability,showing no performance deterioration during 30 h electrolysis.This work provides an efficient,green,and scalable synthesis method of the electrocatalyst for CO_(2) reduction to formate.
基金supported by the National Natural Science Foundation of China (No. 41072173)the National Science & Technology Pillar Program in the Eleventh Five-year Plan Period of China (No. 2006BAJ04A07)
文摘A novel ion-imprinted polymer, lead ion-imprinted micro-beads with combination of two functional monomers, was synthesized using the W/O/W polymerization method. Two functional monomers, 1,12-dodecanediol-O,O’-diphenyl-phosphonic acid (DDDPA) and 4-vinylpyridine, were used to form a suitable construction with micro-pores fitting the template and recognition sites. The eflects of adsorbent dosage, solution pH and the competitive ions on the adsorption and separation eflciency of lead ions were investigated. The lead ion-imprinted micro-beads were eflcient for lead ions removal from aqueous solution in a broad pH range (4–9), when the adsorbent dosage was above 0.1 g/L. The adsorption process obeyed the pseudo second-order kinetics model and it only took half an hour to reach the equilibrium. The adsorption isotherm of lead ion was described by the Langmuir model (R2 0.99) with a maximum adsorption capacity of 116.9 mg/g. In the presence of competitive ions Co2+ and Cd2+, the lead ion-imprinted micro-beads showed a high selectivity for lead ions. The selectivity coeficient of Pb2+/Cd2+ and Pb2+/Co2+are 99.3 and 114.7, respectively.
基金supported by the National Mega-Project of Science and Technology of China (No.2008ZX07421-002)the National Eleventh Five-Year Pillar Program of Sciencethe Technology of China (No.2006BAJ04A07)
文摘The effects of ferric ion, pH, and bromide on the formation and distribution of disinfection byproducts (DBPs) during chlorination were studied. Two raw water samples from Huangpu River and Yangtze River, two typical drinking water sources of Shanghai, were used for the investigation. Compared with the samples from Huangpu River, the raw water samples from Yangtze River had lower content of total organic carbon (TOC) and ferric ions, but higher bromide concentrations. Under controlled chlorination conditions, four trihalomethanes (THMs), nine haloacetic acids (HAAs), total organic halogen (TOX) and its halogen species fractions, including total organic chlorine (TOC1) and total organic bromide (TOBr), were determined. The results showed that co-existent ferric and bromide ions significantly promoted the formation of total THMs and HAAs for both raw water samples. Higher concentration of bromide ions significantly changed the speciation of the formed THMs and HAAs. There was an obvious shift to brominated species, which might result in a more adverse influence on the safety of drinking water. The results also indicated that high levels of bromide ions in raw water samples produced higher percentages of unknown TOBr.
基金supported by the National Natural Science Foundation of China (No. 41072173)the National High Technology Research and Development Program(863) of China (No. 2009AA062905)
文摘The mesoporous Cu/Mg/Fe layered double hydroxide(Cu/Mg/Fe-LDH) with carbonate intercalation was synthesized and used for the removal of arsenate from aqueous solutions.The Cu/Mg/Fe-LDH was characterized by Fourier transform infrared spectrometry,X-ray diffraction crystallography,scanning electron microscopy,X-ray photoelectron spectroscopy and Brunauer-Emmett-Teller.Effects of various physico-chemical parameters such as pH,adsorbent dosage,contact time and initial arsenate concentration on the adsorption of arsenate onto Cu/Mg/Fe-LDH were investigated.Results showed that it was efficient for the removal of arsenate,and the removal efficiency of arsenate increased with the increment of the adsorbent dosage,while the arsenate adsorption capacity decreased with increase of initial pH from 3 to 11.The adsorption isotherms can be well described by the Langmuir model with R 2 〉 0.99.Its adsorption kinetics followed the pseudo second-order kinetic model.Coexisting ions such as HPO42-,CO32-,SO42and NO3could compete with arsenate for adsorption sites on the Cu/Mg/Fe-LDH.The adsorption of arsenate on the adsorbent can be mainly attributed to the ion exchange process.It was found that the synthesized Cu/Mg/Fe-LDH can reduce the arsenate concentration down to a final level of 〈 10 μg/L under the experimental conditions,and makes it a potential material for the decontamination of arsenate polluted water.
基金financially supported by National Mega-Project of Science and Technology of China (No.2008ZX07421-002)the National Eleventh Five-Year Pillar Program of Science and Technology of China (No.2006BAJ04A07)
文摘For the system of water samples collected from Yangtze River,the effects of seasonal variation and Fe(III) concentrations on the formation and distribution of trihalomethanes (THMs) during chlorination have been investigated.The corresponding lifetime cancer risk of the formed THMs to human beings was estimated using the parameters and procedure issued by the US EPA.The results indicated that the average concentration of THMs (100.81 μg/L) in spring was significantly higher than that in other seasons,which was related to the higher bromide ion concentration resulted from the intrusion of tidal saltwater.The total cancer risk in spring reached 8.23 × 10 ?5 and 8.86 × 10 ?5 for males and females,respectively,which were about two times of those in summer under the experimental conditions.Furthermore,it was found that the presence of Fe(III) resulted in the increased level of THMs and greater cancer risk from exposure to humans.Under weak basic conditions,about 10% of the increment of THMs from the water samples in spring was found in the presence of 0.5 mg/L Fe(III) compared with the situation without Fe(III).More attention should be given to the effect of the coexistence of Fe(III) and bromide ions on the risk assessment of human intake of THMs from drinking water should be paid more attention,especially in the coastland and estuaries.
基金supported by the National Major Project of Science & Technology Ministry of China (No.2008ZX07421-002)the National Natural Science Foundation of China (No. 50908142)
文摘Natural zeolite was modified by loading cetylpyridinium bromide (CPB) to create more efficient sites for humic acid (HA) adsorption. The natural and CPB modified zeolites were characterized with X-ray diffraction, field emission scanning electron microscopy, Fourier transform infrared spectroscopy and elemental analysis. The effects of various experimental parameters such as contact time, initial HA concentration, solution pH and coexistent Ca^2+, upon HA adsorption onto CPB modified zeolites were evaluated. The results showed that natural zeolite had negligible affinity for HA in aqueous solutions, but CPB modified zeolites exhibited high adsorption efficiency for HA. A higher CPB loading on natural zeolites exhibited a larger HA adsorption capacity. Acidic pH and coexistent Ca^2+ were proved to be favorable for HA adsorption onto CPB modified zeolite. The kinetic process was well described by pseudo second-order model. The experimental isotherm data fitted well to Langmuir and Sips models. The maximum monolayer adsorption capacity of CPB modified zeolite with surfactant bilayer coverage was found to be 92.0 mg/g.
基金This work was supported by the National Major Project of Science and Technology Ministry of China(Grant No.2008ZX07421-002)the National Natural Science Foundation of China(Grant No.50908142)the National Science and Technology Infrastructure Program of China(Grant No.2006BAJ08B02).
文摘Surfactant-modified natural zeolites(SMNZ)with different coverage types were prepared by loading hexadecyltrimethyl ammonium bromide(HTAB)onto the surface of a natural zeolite.The adsorption behavior of humic acid(HA)on SMNZ was investigated.Results indicate that the adsorbent SMNZ exhibited a higher affinity toward HA than the natural zeolite.HA removal efficiency by SMNZ increased with HTAB loading.Coexisting Ca2+in solution favored HA adsorption onto SMNZ.Adsorption capacity decreased with an increasing solution pH.For typical SMNZ with bilayer HTAB coverage,HA adsorption process is well described by a pseudo-second-order kinetic model.The experimental isotherm data fitted well with the Langmuir model.Calculated maximum HA adsorption capacities for SMNZ with bilayer HTAB coverage at pH 5.5 and 7.5 were 63 and 41 mg·g^(-1),respectively.E2/E3(absorbance at 250 nm to that at 365 nm)and E4/E6(absorbance at 465 nm to that at 665 nm)ratios of the residual HA in solution were lower than that of the original HA solution.This indicates that the HA fractions with high polar functional groups,low molecular weight(MW),and aromaticity had a stronger tendency for adsorption onto SMNZ with bilayer HTAB coverage.Results show that HTABmodified natural zeolite is a promising adsorbent for removal of HA from aqueous solution.
基金This work was supported by the Key Technologies Research and Development Program of the Eleventh-Five Year Plan of China(Grant No.2006BAJ08B02)the Innovation Project of Talented Scientific Youth of Fujian Province in 2008 Year(No.2008F3096).
文摘The dissociation constants of polyepoxysuccinic acid(PESA)were investigated in this study.Based on the potentiometric titration and the BEST program,the dissociation constants of PESA were determined.Considering the complexity of the dissociation of PESA in aqueous solution,several models were constructed to simulate the dissociation process of PESA.By comparison,the dissociation constants of PESA were obtained with model 4.The species distribution of PESA in aqueous solution as a function of pH was also presented according to the experimental and calculation results.It showed that the H_(2)L model with five basic structure units to describe the dissociation of PESA was reasonable,and the relevant constants had less error and better matching between the experimental and calculation data.The corresponding values of pK_(ai) were 4.68 and 4.92,respectively,for H2L at 35℃ with ionic strength of 0.1 mol/L.
基金This work was supported by the National Natural Science Foundation of China (Grant No. 41372241).
文摘A novel composite adsorbent, hydroxyapatite/ manganese dioxide (HAp/MnO2), has been developed for the purpose of removing lead ions from aqueous solutions. The combination of HAp with MnO2 is meant to increase its adsorption capacity. Various factors that may affect the adsorption efficiency, including solution pH, coexistent substances such as humic acid and competing cations (Ca2+, Mg2+), initial solute concentration, and the duration of the reaction, have been investigated. Using this composite adsorbent, solution pH and coexistent calcium or magnesium cations were found to have no significant influence on the removal of lead ions under the experi- mental conditions. The adsorption equilibrium was described well by the Langmuir isotherm model, and the calculated maximum adsorption capacity was 769 mg. gl. The sorption processes obeyed the pseudo-second-order kinetics model. The experimental results indicate that HAp/MnO2 composite may be an effective adsorbent for the removal of lead ions from aqueous solutions.