In this study,high-gravity intensified heterogeneous catalytic ozonation is utilized for treatment of phenol-containing wastewater,and the kinetics of the direct reaction between ozone and phenol in the presence of ex...In this study,high-gravity intensified heterogeneous catalytic ozonation is utilized for treatment of phenol-containing wastewater,and the kinetics of the direct reaction between ozone and phenol in the presence of excess tertiary butanol(TBA)is investigated.It is revealed that the direct reaction between ozone and phenol in the rotating packed bed(RPB)follows the pseudo-first-order kinetics with a reaction rate constant higher than that in the conventional bubbling reactor(BR).Under different conditions of temperature,initial pH,high-gravity factor,and gaseous ozone concentration,the apparent reaction rate constant varies in the range of 0.0160–0.115 min-1.An empirical power-exponential model is established to characterize the effects of these parameters on the direct reaction between ozone and phenol by high-gravity intensified heterogeneous catalytic ozonation.展开更多
Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical capacity.Toward the broader implementation,the primary obstacle lies in the intricate multi-elec...Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical capacity.Toward the broader implementation,the primary obstacle lies in the intricate multi-electron,multi-step redox reaction associated with sluggish conversion kinetics,subsequently giving rise to a cascade of parasitic issues.In order to smooth reaction kinetics,catalysts are widely introduced to accelerate reaction rate via modulating the energy barrier.Over past decades,a large amount of research has been devoted to the catalyst design and catalytic mechanism exploration,and thus the great progress in electrochemical performance has been realized.Therefore,it is necessary to make a comprehensive review toward key progress in catalyst design and future development pathway.In this review,the basic mechanism of lithium metal batteries is provided along with corresponding advantages and existing challenges detailly described.The main catalysts employed to accelerate cathode reaction with emphasis on their catalytic mechanism are summarized as well.Finally,the rational design and innovative direction toward efficient catalysts are suggested for future application in metal-sulfur/gas battery and beyond.This review is expected to drive and benefit future research on rational catalyst design with multi-parameter synergistic impacts on the activity and stability of next-generation metal battery,thus opening new avenue for sustainable solution to climate change,energy and environmental issues,and the potential industrial economy.展开更多
As one of the most promising and practical advanced oxidation processes(AOPs),the catalytic ozonation is triggered by the active components of catalyst,which are usually derived from metals or metal oxides.To avoid th...As one of the most promising and practical advanced oxidation processes(AOPs),the catalytic ozonation is triggered by the active components of catalyst,which are usually derived from metals or metal oxides.To avoid the metal pollution from catalyst,here the amorphous boron(A-boron)is used as a metalfree catalyst for catalytic ozonation to produce free radicals for effective degradation of atrazine(ATZ),the world-widely used herbicide and also a widespread pollutant in environment.A-boron exhibits an outstanding performance for catalytic ozonation to remove ATZ from water.As A-boron is introduced into ozonation,the degradation efficiency in 10 min is promoted to 97.1%,much higher than that of 15.1%under ozonation.The mechanism is that the B-B bonds and internal suboxide B in A-boron serve as the main active sites to donate electrons to accelerate ozone decomposition to produce reactive oxygen species(ROS),including·O_(2)^(-)and^(1)O_(2),and further enhance ATZ degradation via ROS reactions.Moreover,the A-boron is still highly active with a degradation efficiency of ATZ over 95%in 10 min even after four successive cycles.This work shows A-boron could be an alternative for the active components of metal or metal oxide in catalytic ozonation.展开更多
In order to improve the ability of ozone to catalyze the degradation of phenolic pollutants in wastewater,the CuO/Al2O3 catalysts was prepared by the impregnation precipitation method and an ozone catalytic oxidation ...In order to improve the ability of ozone to catalyze the degradation of phenolic pollutants in wastewater,the CuO/Al2O3 catalysts was prepared by the impregnation precipitation method and an ozone catalytic oxidation system was constructed.The actual phenolic sewage was used as the treatment object.And the reaction conditions of the system were optimized,and the treatment effect was determined,while the non-catalytic system was used as a control group.At the same time,the influence of salt and ammonia nitrogen related water quality on the system was studied.The optimal reaction conditions for the treatment of phenolic wastewater covered:a catalyst dosage of 30 g/L,an ozone flow rate of 0.3 m3/h,a pH value of 8.80,and a reaction time of 15 minutes.Under these conditions,the phenol and COD removal rates of the system reached 98.7%and 49.4%,respectively,which were by 31.3 percentage points and 16.2 percentage points higher than that of the ozonation system alone.The salt and ammonia nitrogen in the sewage can reduce the oxidation effect of the system.When the salinity reached 10%and the ammonia nitrogen content reached 13 000 mg/L,the removal rate of phenol could be reduced by about 20%.The results of this paper have a reference value for phenol wastewater treatment engineering.展开更多
Different series of transition metal catalysts supported on Al2O3 were prepared by the impregnation method. The catalytic activity was measured in a batch reactor with ozone as the oxidizing reagent. The experimental ...Different series of transition metal catalysts supported on Al2O3 were prepared by the impregnation method. The catalytic activity was measured in a batch reactor with ozone as the oxidizing reagent. The experimental results indicate that Cu/Al2O3 has a very effective catalytic activity during the ozonation of organic pollutants in water. The optimum conditions for preparing Cu/Al2O3 were systematically investigated with the orthogonal testing method. Furthermore, the results also show that the surface properties of catalyst are not compulsory for effective oxidation.展开更多
A novel heterogeneous catalytic ozonation process in water treatment was studied,with a copper-loaded activated carbon(Cu/AC) that was prepared by an incipient wetness impregnation method at low temperature and tested...A novel heterogeneous catalytic ozonation process in water treatment was studied,with a copper-loaded activated carbon(Cu/AC) that was prepared by an incipient wetness impregnation method at low temperature and tested as a catalyst in the ozonation of phenol and oxalic acid.Cu/AC was characterized using XRD,BET and SEM techniques.Compared with ozonation alone,the presence of Cu/AC in the ozonation processes significantly improves the degradation of phenol or oxalic acid.With the introduction of the hydroxyl radical scavenger,i.e.,turt-butanol alcohol(t-BuOH),the degradation efficiency of both phenol and oxalic acid in the Cu/AC catalyzed ozonation process decreases by 22% at 30 min.This indicates that Cu/AC accelerates ozone decomposition into certain concentration of hydroxyl radicals.The amount of Cu(Ⅱ) produced during the reaction of Cu/AC-catalyzed ozonation of phenol or oxalic acid is very small,which shows that the two processes are both heterogeneous catalytic ozonation reactions.展开更多
Pd/LaxPbyMnOz, Pd/C, Pd/molecular sieve and Pd-heteropoly acid catalysts for direct synthesis of diphenyl carbonate (DPC) by heterogeneous catalytic reaction were compared and the results of DPC synthesis indicated th...Pd/LaxPbyMnOz, Pd/C, Pd/molecular sieve and Pd-heteropoly acid catalysts for direct synthesis of diphenyl carbonate (DPC) by heterogeneous catalytic reaction were compared and the results of DPC synthesis indicated that the catalyst Pd/LaxPbyMnOz had higher activity. The Pd/LaxPbyMnOz catalyst and the support was characterized by XRD, SEM and TEM, the main phase was La0.62Pb0.38MnO3 and the average diameter could be about 25.4 nm. The optimum conditions for synthesis of DPC with Pd/LaxPbyMnOz were determined by orthogonal experiments and the experimental results showed that reaction temperature was the first factor of effect on the selectivity and yield of DPC, and the concentration of O2 in gas phase also had significant effect on selectivity of DPC. The optimum reaction conditions were catMyst/phenol mass ratio 1 to 50, pressure 4.5 MPa,volume concentration of O2 25%, reaction temperature 60° and reaction time 4 h. The maximum yield and average selectivity could reach 13% and 97% respectively in the batch operation.展开更多
Catalytic treatments of VOCs at normal temperature can greatly reduce the cost and temperature of processing,and improve the safety factor in line with the requirements of green chemistry.Activated carbon fiber(ACF)wa...Catalytic treatments of VOCs at normal temperature can greatly reduce the cost and temperature of processing,and improve the safety factor in line with the requirements of green chemistry.Activated carbon fiber(ACF)was pretreated with 10%H_(2)SO_(4)by single factor optimization to increase specific surface area and pore volume obviously.The catalytic ozonation performance of ACF loaded with Au,Ag,Pt and Pd noble metals on ethyl acetate was investigated and Pd/ACF was selected as the optimal catalyst which had certain stability.Pd is uniformly distributed on the surface of ACF,and Palladium mainly exists in the form of Pd0 with a amount of Pd+2.The specific surface area of the catalysts gradually decreases as the loading increases.The activation energy of ethyl acetate calculated by Arrhenius equation is 113 kJ mol 1.With 1%Pd loading and the concentration ratio of ozone to ethyl acetate is 3:1,catalytic ozonation performance is maximized and the conversion rate of ethyl acetate reached to 60%in 3050℃Cat 15,00030,000 h^1.展开更多
This paper describes the potential of heterogeneous catalytic ozonization of sulfo-salicylic acid (SSal). It was found that catalytic ozonization in the presence of Mn-Zr-O (a modified manganese dioxide supported on s...This paper describes the potential of heterogeneous catalytic ozonization of sulfo-salicylic acid (SSal). It was found that catalytic ozonization in the presence of Mn-Zr-O (a modified manganese dioxide supported on silica gel) had significantly enhanced the removal rate (72%) of total organic carbon (TOC) compared with that of ozonization alone (19%). The efficient removal rate of TOC was probably due to increasing the adsorption ability of catalyst and accelerating decomposition of ozone to produce more powerful oxidants than ozone. .展开更多
CuO particles were attempted to fill in the channel of multi-walled carbon nanotubes (MWCNTs) as novel catalytic materials CuO@MWCNTs used for ozonation of humic acids (HA) in aqueous solution.Catalyst samples were ch...CuO particles were attempted to fill in the channel of multi-walled carbon nanotubes (MWCNTs) as novel catalytic materials CuO@MWCNTs used for ozonation of humic acids (HA) in aqueous solution.Catalyst samples were characterized by transmission electron microscopy (TEM),X-ray diffraction (XRD),thermogravimetric analysis (TG) and X-ray photoelectron spectroscopy (XPS).The removal efficiency of HA was promoted in the presence of CuO@MWCNTs compared with that of Al2O3-supported CuO catalyst (CuO/Al2O3) and CuO-coating MWCNTs catalyst (CuO/MWCNTs).The strong synergetic effect in the confinement environment on CuO nanoparticles can attribute to the locally higher pressure due to the lower potential energy of reactants in the channels.Strong interaction happened between the catalyst and reactants,which promoted the decomposition of ozone and the generation of OH.The results of experimental and theoretical investigation confirmed that CuO@MWCNTs promotes the initiation and generation of OH,hence accelerating the degradation of organic pollutants.展开更多
In order to improve the catalytic ozonation effect of resorcinol, the spinel CuFe_2O_4 was modified by doped CeO_2, and X-ray diffraction(XRD) and scanning electron microscopy(SEM) were used for characterization analy...In order to improve the catalytic ozonation effect of resorcinol, the spinel CuFe_2O_4 was modified by doped CeO_2, and X-ray diffraction(XRD) and scanning electron microscopy(SEM) were used for characterization analysis. The effects of composite catalyst CeO_2/CuFe_2O_4 dosage, ozone dosage, initial pH and reaction temperature on degradation were studied, and the stability of the catalyst was tested. The results showed that the composite effect of CeO_2/CuFe_2O_4 prepared by combustion method was good, and the catalyst presented a laminated structure, in which 30 wt% CeO_2/CuFe_2O_4 degradation effect was significant. The removal rate of resorcinol using CeO_2/CuFe_2O_4 composite catalyst was higher than that using ozone or CuFe_2O_4 separately by 41.8% and 11.9%, respectively. In a reaction with resorcinol concentration of 100 mg/L, the catalyst dosage of 1.0 g/L, the ozone dosage of 2.5 mg/(L·min), at pH=9, temperature of 20 ℃, for reaction time of 40 min, the resorcinol removal rate was 88.5%. The catalyst CeO_2/CuFe_2O_4 still showed good degradation effect after repeatedly using for 10 times, and the dissolution rate of metal ions was lower than that of CuFe_2O_4.展开更多
During textile manufacturing, huge amounts of wastewaters characterized by removed impurities and high concentrations of dye are produced. These wastewaters cause several problems when they are discharged to the envir...During textile manufacturing, huge amounts of wastewaters characterized by removed impurities and high concentrations of dye are produced. These wastewaters cause several problems when they are discharged to the environment. The use of ozone in wastewater treatment results of interest. In this work we propose to assess the discoloration rate of different synthetic wastewaters as a function of pH, dye concentration (methylene blue (MB)) and reaction time. A comparison of discoloration rate between conventional ozonation and catalytic ozonation salts of copper, zinc, silver and nickel was also performed. For the optimization of the ozonation process of colored solutions, it was used a central composite experimental design with five replicates of the center point resulting to evaluate the influence of the independent variables at different ranges of pH, [MB] and time. In the catalyst-assisted ozonation, [MB], pH and the reaction time were fixed to 100 mg/L, 5.5 and 15 min, respectively. The optimized experimental conditions to provide maximum discoloration were pH=3.3;[MB]=8.6 mg/L and time=74.3 min. Regarding the catalyst-assisted ozonation, it was found that CuSO4 catalyst gave better color reduction if compared with other catalysts assayed.展开更多
A combined process of catalytic ozonation in the presence of a novel heterogeneous catalyst and biological activated carbon was investigated for the removal of priority control organic pollutants, the reduction of gen...A combined process of catalytic ozonation in the presence of a novel heterogeneous catalyst and biological activated carbon was investigated for the removal of priority control organic pollutants, the reduction of genotoxicity, and the improvement of biodegradable dissolved organic carbon (BDOC). Results confirm that the catalytic ozonation has higher effectiveness for the removal of refractory harmful organic pollutants, the reduction of genotoxicity and the increase of bio-degradability of organics than ozonation alone, which results in lower pollution load for subsequent biological activated carbon process, and then leads to less organic pollutants penetrating biological activated carbon. The novel catalytic ozonation with this combined process exhibits excellent performance to guarantee the safety of drinking water.展开更多
Techno-economic potentials of thermal and catalytic pyrolysis plants for the conversion of waste plastics to liquid fuels have been widely studied, but it is not obvious which of the two plants is more profitable, as ...Techno-economic potentials of thermal and catalytic pyrolysis plants for the conversion of waste plastics to liquid fuels have been widely studied, but it is not obvious which of the two plants is more profitable, as the existing studies used different assumptions and cost bases in their analyses, thereby making it difficult to compare the economic potentials of the two plants. In this study, industrial-scale thermal and catalytic waste plastics pyrolysis plants were designed and economically analyzed using ASPEN PLUS. Amorphous silica-alumina was considered the optimum catalyst, with 3:1 feed to catalyst ratio. Based on 20,000 tons/year of feed and 20% interest rate, the catalytic plant, having a net present value (NPV) of � million, was found to be economically less attractive than the thermal plant, having the NPV of �.4 million. On the contrary, sensitivity analyses of the two plants at a feed rate of 50,000 tons/year gave rise to a slightly higher NPV for the catalytic plant (� million) than the thermal plant having NPV of � million, thereby making the former more economically attractive for processing large amounts of waste plastics into liquid fuels. Consequently, as the catalytic plant showed a better scale economy and would produce higher quality liquid fuels than the thermal plant, it is recommended for commercialization in Nigeria.展开更多
In this account,highly ordered mesoporous MnO_x/TiO_2composite catalysts with efficient catalytic ozonation of phenol degradation were synthesized by the sol–gel method.The surface morphology and properties of the ca...In this account,highly ordered mesoporous MnO_x/TiO_2composite catalysts with efficient catalytic ozonation of phenol degradation were synthesized by the sol–gel method.The surface morphology and properties of the catalysts were characterized by several analytical methods,including SEM,TEM,BET,XRD,FTIR,and XPS.Interestingly,Mn doping was found to improve the degree of order,and the ordered mesoporous structure was optimized at 3%doping.Meanwhile,MnO_xwas highly dispersed in the ordered mesoporous materials to yield good catalytic ozonation performance.Phenol could completely be degraded in 20 min and mineralized at 79%in 60 min.Thus,the catalyst greatly improved the efficiency of degradation and mineralization of phenol when compared to single O_3or O_3+TiO_2.Finally,the reaction mechanism of the catalyst was discussed and found to conform to pseudo-first-order reaction dynamics.展开更多
Since the discovery of mesoporous silica in 1990s,there have been numerous mesoporous silica-based nanomaterials developed for catalytic applications,aiming at enhanced catalytic activity and stability.Recently,there ...Since the discovery of mesoporous silica in 1990s,there have been numerous mesoporous silica-based nanomaterials developed for catalytic applications,aiming at enhanced catalytic activity and stability.Recently,there have also been considerable interests in endowing them with hierarchical porosities to overcome the diffusional limitation for those with long unimodal channels.Present processes of making mesoporous silica largely rely on chemical sources which are relatively expensive and impose environmental concerns on their processes.In this regard,it is desirable to develop hierarchical silica supports from natural minerals.Herein,we present a series of work on surface reconstruction,modification,and functionalization to produce diatomite-based catalysts with original morphology and macro-meso-micro porosities and to test their suitability as catalyst supports for both liquid-and gas-phase reactions.Two wet-chemical routes were developed to introduce mesoporosity to both amorphous and crystalline diatomites.Importantly,we have used computational modeling to affirm that the diatomite morphology can improve catalytic performance based on fluid dynamics simulations.Thus,one could obtain this type of catalysts from numerous natural diatoms that have inherently intricate morphologies and shapes in micrometer scale.In principle,such catalytic nanocomposites acting as miniaturized industrial catalysts could be employed in microfluidic reactors for process intensification.展开更多
基金supported by the Fund for Shanxi Province Higher Education“1331 Project”for Improving Quality and Efficiency Construction(nuc2021-006)Key Research&Development Plan of Shanxi Province(201903D321059)+1 种基金Scientific Activities of Selected Returned Overseas Professionals in Shanxi Province(20200004)Transformation and Cultivation Projects of Scientific and Technological Achievements in Universities of Shanxi Province Institutions(2020CG040).
文摘In this study,high-gravity intensified heterogeneous catalytic ozonation is utilized for treatment of phenol-containing wastewater,and the kinetics of the direct reaction between ozone and phenol in the presence of excess tertiary butanol(TBA)is investigated.It is revealed that the direct reaction between ozone and phenol in the rotating packed bed(RPB)follows the pseudo-first-order kinetics with a reaction rate constant higher than that in the conventional bubbling reactor(BR).Under different conditions of temperature,initial pH,high-gravity factor,and gaseous ozone concentration,the apparent reaction rate constant varies in the range of 0.0160–0.115 min-1.An empirical power-exponential model is established to characterize the effects of these parameters on the direct reaction between ozone and phenol by high-gravity intensified heterogeneous catalytic ozonation.
基金supported by the National Natural Science Foundation of China(52272194)Liaoning Revitalization Talents Program(XLYC2007155)。
文摘Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical capacity.Toward the broader implementation,the primary obstacle lies in the intricate multi-electron,multi-step redox reaction associated with sluggish conversion kinetics,subsequently giving rise to a cascade of parasitic issues.In order to smooth reaction kinetics,catalysts are widely introduced to accelerate reaction rate via modulating the energy barrier.Over past decades,a large amount of research has been devoted to the catalyst design and catalytic mechanism exploration,and thus the great progress in electrochemical performance has been realized.Therefore,it is necessary to make a comprehensive review toward key progress in catalyst design and future development pathway.In this review,the basic mechanism of lithium metal batteries is provided along with corresponding advantages and existing challenges detailly described.The main catalysts employed to accelerate cathode reaction with emphasis on their catalytic mechanism are summarized as well.Finally,the rational design and innovative direction toward efficient catalysts are suggested for future application in metal-sulfur/gas battery and beyond.This review is expected to drive and benefit future research on rational catalyst design with multi-parameter synergistic impacts on the activity and stability of next-generation metal battery,thus opening new avenue for sustainable solution to climate change,energy and environmental issues,and the potential industrial economy.
基金Financial support is provided by the Key Research and Development Program of Zhejiang Province(No.2021C03179)the National Key Research and Development Program of China(No.2019YFC0408802)。
文摘As one of the most promising and practical advanced oxidation processes(AOPs),the catalytic ozonation is triggered by the active components of catalyst,which are usually derived from metals or metal oxides.To avoid the metal pollution from catalyst,here the amorphous boron(A-boron)is used as a metalfree catalyst for catalytic ozonation to produce free radicals for effective degradation of atrazine(ATZ),the world-widely used herbicide and also a widespread pollutant in environment.A-boron exhibits an outstanding performance for catalytic ozonation to remove ATZ from water.As A-boron is introduced into ozonation,the degradation efficiency in 10 min is promoted to 97.1%,much higher than that of 15.1%under ozonation.The mechanism is that the B-B bonds and internal suboxide B in A-boron serve as the main active sites to donate electrons to accelerate ozone decomposition to produce reactive oxygen species(ROS),including·O_(2)^(-)and^(1)O_(2),and further enhance ATZ degradation via ROS reactions.Moreover,the A-boron is still highly active with a degradation efficiency of ATZ over 95%in 10 min even after four successive cycles.This work shows A-boron could be an alternative for the active components of metal or metal oxide in catalytic ozonation.
基金financially supported by the Ministry of Science and Technology of the People’s Republic of China [Grant No. 2017YFC1404605]
文摘In order to improve the ability of ozone to catalyze the degradation of phenolic pollutants in wastewater,the CuO/Al2O3 catalysts was prepared by the impregnation precipitation method and an ozone catalytic oxidation system was constructed.The actual phenolic sewage was used as the treatment object.And the reaction conditions of the system were optimized,and the treatment effect was determined,while the non-catalytic system was used as a control group.At the same time,the influence of salt and ammonia nitrogen related water quality on the system was studied.The optimal reaction conditions for the treatment of phenolic wastewater covered:a catalyst dosage of 30 g/L,an ozone flow rate of 0.3 m3/h,a pH value of 8.80,and a reaction time of 15 minutes.Under these conditions,the phenol and COD removal rates of the system reached 98.7%and 49.4%,respectively,which were by 31.3 percentage points and 16.2 percentage points higher than that of the ozonation system alone.The salt and ammonia nitrogen in the sewage can reduce the oxidation effect of the system.When the salinity reached 10%and the ammonia nitrogen content reached 13 000 mg/L,the removal rate of phenol could be reduced by about 20%.The results of this paper have a reference value for phenol wastewater treatment engineering.
基金Supported by the National Natural Science Foundation of China(No20476019)
文摘Different series of transition metal catalysts supported on Al2O3 were prepared by the impregnation method. The catalytic activity was measured in a batch reactor with ozone as the oxidizing reagent. The experimental results indicate that Cu/Al2O3 has a very effective catalytic activity during the ozonation of organic pollutants in water. The optimum conditions for preparing Cu/Al2O3 were systematically investigated with the orthogonal testing method. Furthermore, the results also show that the surface properties of catalyst are not compulsory for effective oxidation.
基金Project(40973074) supported by the National Natural Science Foundation of China
文摘A novel heterogeneous catalytic ozonation process in water treatment was studied,with a copper-loaded activated carbon(Cu/AC) that was prepared by an incipient wetness impregnation method at low temperature and tested as a catalyst in the ozonation of phenol and oxalic acid.Cu/AC was characterized using XRD,BET and SEM techniques.Compared with ozonation alone,the presence of Cu/AC in the ozonation processes significantly improves the degradation of phenol or oxalic acid.With the introduction of the hydroxyl radical scavenger,i.e.,turt-butanol alcohol(t-BuOH),the degradation efficiency of both phenol and oxalic acid in the Cu/AC catalyzed ozonation process decreases by 22% at 30 min.This indicates that Cu/AC accelerates ozone decomposition into certain concentration of hydroxyl radicals.The amount of Cu(Ⅱ) produced during the reaction of Cu/AC-catalyzed ozonation of phenol or oxalic acid is very small,which shows that the two processes are both heterogeneous catalytic ozonation reactions.
基金National Natural Science Foundation of China(No.20076036Tianjin University C1 National Laboratory Project
文摘Pd/LaxPbyMnOz, Pd/C, Pd/molecular sieve and Pd-heteropoly acid catalysts for direct synthesis of diphenyl carbonate (DPC) by heterogeneous catalytic reaction were compared and the results of DPC synthesis indicated that the catalyst Pd/LaxPbyMnOz had higher activity. The Pd/LaxPbyMnOz catalyst and the support was characterized by XRD, SEM and TEM, the main phase was La0.62Pb0.38MnO3 and the average diameter could be about 25.4 nm. The optimum conditions for synthesis of DPC with Pd/LaxPbyMnOz were determined by orthogonal experiments and the experimental results showed that reaction temperature was the first factor of effect on the selectivity and yield of DPC, and the concentration of O2 in gas phase also had significant effect on selectivity of DPC. The optimum reaction conditions were catMyst/phenol mass ratio 1 to 50, pressure 4.5 MPa,volume concentration of O2 25%, reaction temperature 60° and reaction time 4 h. The maximum yield and average selectivity could reach 13% and 97% respectively in the batch operation.
基金the National Key R&D Program of the Ministry of Science and Technology,China(Grant No.2018YFC0705304)and the Key Scientific and Technological Support Projects,Tianjin City,China(Grant No.19YFZCSF01090).
文摘Catalytic treatments of VOCs at normal temperature can greatly reduce the cost and temperature of processing,and improve the safety factor in line with the requirements of green chemistry.Activated carbon fiber(ACF)was pretreated with 10%H_(2)SO_(4)by single factor optimization to increase specific surface area and pore volume obviously.The catalytic ozonation performance of ACF loaded with Au,Ag,Pt and Pd noble metals on ethyl acetate was investigated and Pd/ACF was selected as the optimal catalyst which had certain stability.Pd is uniformly distributed on the surface of ACF,and Palladium mainly exists in the form of Pd0 with a amount of Pd+2.The specific surface area of the catalysts gradually decreases as the loading increases.The activation energy of ethyl acetate calculated by Arrhenius equation is 113 kJ mol 1.With 1%Pd loading and the concentration ratio of ozone to ethyl acetate is 3:1,catalytic ozonation performance is maximized and the conversion rate of ethyl acetate reached to 60%in 3050℃Cat 15,00030,000 h^1.
基金The project was supported by the National Natural Science Foundation of China(No.29877024)
文摘This paper describes the potential of heterogeneous catalytic ozonization of sulfo-salicylic acid (SSal). It was found that catalytic ozonization in the presence of Mn-Zr-O (a modified manganese dioxide supported on silica gel) had significantly enhanced the removal rate (72%) of total organic carbon (TOC) compared with that of ozonization alone (19%). The efficient removal rate of TOC was probably due to increasing the adsorption ability of catalyst and accelerating decomposition of ozone to produce more powerful oxidants than ozone. .
基金Sponsored by the State Key Lab of Urban Water Resource and Environment (Grant No.ESK200801)
文摘CuO particles were attempted to fill in the channel of multi-walled carbon nanotubes (MWCNTs) as novel catalytic materials CuO@MWCNTs used for ozonation of humic acids (HA) in aqueous solution.Catalyst samples were characterized by transmission electron microscopy (TEM),X-ray diffraction (XRD),thermogravimetric analysis (TG) and X-ray photoelectron spectroscopy (XPS).The removal efficiency of HA was promoted in the presence of CuO@MWCNTs compared with that of Al2O3-supported CuO catalyst (CuO/Al2O3) and CuO-coating MWCNTs catalyst (CuO/MWCNTs).The strong synergetic effect in the confinement environment on CuO nanoparticles can attribute to the locally higher pressure due to the lower potential energy of reactants in the channels.Strong interaction happened between the catalyst and reactants,which promoted the decomposition of ozone and the generation of OH.The results of experimental and theoretical investigation confirmed that CuO@MWCNTs promotes the initiation and generation of OH,hence accelerating the degradation of organic pollutants.
基金Supported by the National Natural Science Foundation of China(41772240)
文摘In order to improve the catalytic ozonation effect of resorcinol, the spinel CuFe_2O_4 was modified by doped CeO_2, and X-ray diffraction(XRD) and scanning electron microscopy(SEM) were used for characterization analysis. The effects of composite catalyst CeO_2/CuFe_2O_4 dosage, ozone dosage, initial pH and reaction temperature on degradation were studied, and the stability of the catalyst was tested. The results showed that the composite effect of CeO_2/CuFe_2O_4 prepared by combustion method was good, and the catalyst presented a laminated structure, in which 30 wt% CeO_2/CuFe_2O_4 degradation effect was significant. The removal rate of resorcinol using CeO_2/CuFe_2O_4 composite catalyst was higher than that using ozone or CuFe_2O_4 separately by 41.8% and 11.9%, respectively. In a reaction with resorcinol concentration of 100 mg/L, the catalyst dosage of 1.0 g/L, the ozone dosage of 2.5 mg/(L·min), at pH=9, temperature of 20 ℃, for reaction time of 40 min, the resorcinol removal rate was 88.5%. The catalyst CeO_2/CuFe_2O_4 still showed good degradation effect after repeatedly using for 10 times, and the dissolution rate of metal ions was lower than that of CuFe_2O_4.
文摘During textile manufacturing, huge amounts of wastewaters characterized by removed impurities and high concentrations of dye are produced. These wastewaters cause several problems when they are discharged to the environment. The use of ozone in wastewater treatment results of interest. In this work we propose to assess the discoloration rate of different synthetic wastewaters as a function of pH, dye concentration (methylene blue (MB)) and reaction time. A comparison of discoloration rate between conventional ozonation and catalytic ozonation salts of copper, zinc, silver and nickel was also performed. For the optimization of the ozonation process of colored solutions, it was used a central composite experimental design with five replicates of the center point resulting to evaluate the influence of the independent variables at different ranges of pH, [MB] and time. In the catalyst-assisted ozonation, [MB], pH and the reaction time were fixed to 100 mg/L, 5.5 and 15 min, respectively. The optimized experimental conditions to provide maximum discoloration were pH=3.3;[MB]=8.6 mg/L and time=74.3 min. Regarding the catalyst-assisted ozonation, it was found that CuSO4 catalyst gave better color reduction if compared with other catalysts assayed.
基金Sponsored by the National High Technology Research and Development Program (863) of China(Grant No. 2006AA06Z306)the National Natural Science Foundation of China(Grant No.50578051)
文摘A combined process of catalytic ozonation in the presence of a novel heterogeneous catalyst and biological activated carbon was investigated for the removal of priority control organic pollutants, the reduction of genotoxicity, and the improvement of biodegradable dissolved organic carbon (BDOC). Results confirm that the catalytic ozonation has higher effectiveness for the removal of refractory harmful organic pollutants, the reduction of genotoxicity and the increase of bio-degradability of organics than ozonation alone, which results in lower pollution load for subsequent biological activated carbon process, and then leads to less organic pollutants penetrating biological activated carbon. The novel catalytic ozonation with this combined process exhibits excellent performance to guarantee the safety of drinking water.
文摘Techno-economic potentials of thermal and catalytic pyrolysis plants for the conversion of waste plastics to liquid fuels have been widely studied, but it is not obvious which of the two plants is more profitable, as the existing studies used different assumptions and cost bases in their analyses, thereby making it difficult to compare the economic potentials of the two plants. In this study, industrial-scale thermal and catalytic waste plastics pyrolysis plants were designed and economically analyzed using ASPEN PLUS. Amorphous silica-alumina was considered the optimum catalyst, with 3:1 feed to catalyst ratio. Based on 20,000 tons/year of feed and 20% interest rate, the catalytic plant, having a net present value (NPV) of � million, was found to be economically less attractive than the thermal plant, having the NPV of �.4 million. On the contrary, sensitivity analyses of the two plants at a feed rate of 50,000 tons/year gave rise to a slightly higher NPV for the catalytic plant (� million) than the thermal plant having NPV of � million, thereby making the former more economically attractive for processing large amounts of waste plastics into liquid fuels. Consequently, as the catalytic plant showed a better scale economy and would produce higher quality liquid fuels than the thermal plant, it is recommended for commercialization in Nigeria.
基金Supported by the National Natural Science Foundation of China(21676139)the Higher Education Natural Science Foundation of Jiangsu Province(15KJA530001)+1 种基金Research Fund of State Key Laboratory of Materials-Oriented Chemical Engineering(ZK201604)the Project of Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)
文摘In this account,highly ordered mesoporous MnO_x/TiO_2composite catalysts with efficient catalytic ozonation of phenol degradation were synthesized by the sol–gel method.The surface morphology and properties of the catalysts were characterized by several analytical methods,including SEM,TEM,BET,XRD,FTIR,and XPS.Interestingly,Mn doping was found to improve the degree of order,and the ordered mesoporous structure was optimized at 3%doping.Meanwhile,MnO_xwas highly dispersed in the ordered mesoporous materials to yield good catalytic ozonation performance.Phenol could completely be degraded in 20 min and mineralized at 79%in 60 min.Thus,the catalyst greatly improved the efficiency of degradation and mineralization of phenol when compared to single O_3or O_3+TiO_2.Finally,the reaction mechanism of the catalyst was discussed and found to conform to pseudo-first-order reaction dynamics.
基金the financial support provided by the National Research Foundation (NRF), Prime Minister’s Office, Singapore, under its Campus for Research Excellence and Technological Enterprise (CREATE) programpartially funded by the National University of Singapore under its Flagship Green Energy Program (GEP), Agency for Science, Technology and Research (A*STAR) under its Low Carbon Energy Research Funding Initiative (LCER-FI)Chongqing Science and Technology Research and Development Base Construction Project (cstc2013gjhz0029)
文摘Since the discovery of mesoporous silica in 1990s,there have been numerous mesoporous silica-based nanomaterials developed for catalytic applications,aiming at enhanced catalytic activity and stability.Recently,there have also been considerable interests in endowing them with hierarchical porosities to overcome the diffusional limitation for those with long unimodal channels.Present processes of making mesoporous silica largely rely on chemical sources which are relatively expensive and impose environmental concerns on their processes.In this regard,it is desirable to develop hierarchical silica supports from natural minerals.Herein,we present a series of work on surface reconstruction,modification,and functionalization to produce diatomite-based catalysts with original morphology and macro-meso-micro porosities and to test their suitability as catalyst supports for both liquid-and gas-phase reactions.Two wet-chemical routes were developed to introduce mesoporosity to both amorphous and crystalline diatomites.Importantly,we have used computational modeling to affirm that the diatomite morphology can improve catalytic performance based on fluid dynamics simulations.Thus,one could obtain this type of catalysts from numerous natural diatoms that have inherently intricate morphologies and shapes in micrometer scale.In principle,such catalytic nanocomposites acting as miniaturized industrial catalysts could be employed in microfluidic reactors for process intensification.
