Preparation and application of granular ZnOAl2O3 catalyst for the removal of

Preparation and application of granular ZnOAl2O3 catalyst for the removal of
Preparation and application of granular ZnOAl2O3 catalyst for the removal of

Journal of Hazardous Materials142(2007)

88–96

Preparation and application of granular ZnO/Al2O3catalyst

for the removal of hazardous trichloroethylene

Jyh-Cherng Chen?,Chun-Tien Tang

Department of Environmental Engineering,Hung-Kuang University,No.34,Chung-Chie Road,Shalu,Taichung County,Taiwan43302,ROC

Received9January2006;received in revised form26June2006;accepted27July2006

Available online31July2006

Abstract

Trichloroethylene(TCE)is a volatile and nerve-toxic liquid,which is widely used in many industries as an organic solvent.Without proper treatment,it will be volatilized into the atmosphere easily and hazardous to the human health and the environment.This study tries to prepare granular ZnO/Al2O3catalyst by a modi?ed oil-drop sol–gel process incorporated the incipient wetness impregnation method and estimates its performance on the catalytic decomposition of TCE.The effects of different preparation and operation conditions are also investigated. Experimental results show that the granular ZnO/Al2O3catalyst has good catalytic performance on TCE decomposition and the conversion of TCE is98%.ZnO/Al2O3(N)catalyst has better performance than ZnO/Al2O3(O)at high temperature.Five percent of active metal concentration and550?C calcination temperature are the better and economic preparation conditions,and the optimum operation temperature and space velocity are450?C and18,000h?1,respectively.The conversions of TCE are similar and all higher than90%as the oxygen concentration in feed gas is higher than5%.By Fourier transform infrared spectrography(FT-IR)analyses,the major reaction products in the catalytic decomposition of TCE are HCl and CO2.The Brunauer–Emmett–Teller(BET)surface areas of catalysts are signi?cantly decreased as the calcination temperature is higher than550?C due to the sintering of catalyst materials,as well as the reaction temperature is higher than150?C due to the accumulations of reaction residues on the surfaces of catalysts.These results are also demonstrated by the results of scanning electron micrography(SEM)and energy disperse spectrography(EDS).

?2006Elsevier B.V.All rights reserved.

Keywords:Catalysis;Trichloroethylene;Zinc oxide;Sol–gel;FT-IR

1.Introduction

The widespread presence of chlorinated volatile organic com-pounds(VOCs)in the environment poses a serious environmen-tal challenge because most of them are carcinogenic,toxic and extremely persistent in the environment.In this study,TCE is chosen as the probe contaminant because its emissions are asso-ciated to a wide range of industrial processes and its vapor is of great environmental concern,as it represents one of the most commonly detected pollutants in hazardous waste sites and land-?lls in many countries[1–4].

Heterogeneous catalytic oxidation has been demonstrated as an ef?cient abatement technology for the removal of VOCs [1–7].The activity and performance of catalyst are in?uenced

?Corresponding author.Tel.:+886426318652x4109;fax:+886426525245.

E-mail address:jcchen@https://www.360docs.net/doc/807368657.html,.tw(J.-C.Chen).by their chemical compositions and preparation method.Cat-alysts reported for destructive oxidation of chlorinated VOCs mostly consist of transition metal oxides(titanium,vanadium, manganese,ferric,nickel,copper and zinc)and noble metals (platinum,palladium and rhodium)on acidic supports[3,7,8]. Noble metals have better catalytic activities but they are expen-sive and easily poisoned by the acid gases(SO2and HCl)in the exhaust.On the other hand,the catalytic activities of transition metal oxides are lower but they are cheaper and have higher tol-erances to the acid gases[5,9].The supports of catalysts include alumina,silica,zeolite,activated carbon,molecular sieve and so on.Lu et al.[10]compared the activities of ZnO coated on differ-ent supports,the conversions of methylbenzene by ZnO/MCM-41was higher than that by ZnO/?-Al2O3at383?C,and also higher than that by ZnO/?-zeolite and ZnO/SiO2at361?C.Kim [11]also compared the activities of CuO coated on different sup-ports and their performances followed the sequence of CuO/?-Al2O3>CuO/TiO2(rutile)>CuO/TiO2(anatase)>CuO/SiO2.

0304-3894/$–see front matter?2006Elsevier B.V.All rights reserved. doi:10.1016/j.jhazmat.2006.07.061

J.-C.Chen,C.-T.Tang/Journal of Hazardous Materials142(2007)88–9689

The performances of catalysts are not only in?uenced by their chemical compositions but also in?uenced by the oper-ation conditions such as operating temperature,space velocity, and the types and concentrations of air pollutants[9].Higher operating temperature promotes the decomposition ef?ciency of organic pollutants,but over temperature(>700?C)may cause the catalyst sintered or volatilized.Takemoto et al.[12]found that the conversion of CH2O by Cu–ZnO/Al2O3catalyst was increased with the increase of operating temperature.Nearly 100%CH2O was converted at150–200?C.Space velocity is the reciprocal of retention time of a pollutant?owing through the catalyst reactor.With small space velocity,the retention time of pollutant in the catalyst reactor is long and the conversions of VOCs are increased.The types and characteristics of pol-lutants also have signi?cant in?uences on the performances of catalysts.Kim[11]used a Cu/?-Al2O3catalyst to study the decompositions of different volatile organic compounds. The removal ef?ciency of toluene was the highest,the next was xylene,and benzene was the lowest.In addition,the per-formance of catalyst was decreased as the concentrations of pollutants were increased.Although TCE can be completely decomposed into CO2and HCl with the aids of catalysts,but some undesirable toxic byproducts may be formed in the cat-alytic reactions[1].Driessen et al.[2]addressed that phosgene, dichloroacetic acid(DCAA),monochloroacetic acid(MCAA), and dichloroacetylchloride(DCAC)can be formed in the cat-alytic decomposition of TCE.

ZnO is one of the photo catalysts with a similar band gap of TiO2,which has shown to be,in some cases,a more active catalyst.Even more importantly,ZnO possess the selectivity for complete mineralization of chlorinated waste[1].Moreover, ZnO can be used as a support and coated with copper to serve as a Cu–Zn catalyst for the synthesis of methanol[10].

Most researches reported the application of semiconductor metal oxide ZnO for the photo catalysis of organic pollutants; however,less study investigates the catalytic incinerations of chlorinated VOCs with ZnO/Al2O3catalyst.This study tries to prepare granular ZnO/Al2O3catalyst by modi?ed oil-drop sol–gel process incorporated with incipient wetness impreg-nation method and estimates its performance on the catalytic decomposition of TCE.The effects of different preparation and operation conditions are also investigated.

2.Experimental methods

2.1.Preparation of granular catalyst

The granular support?-Al2O3of catalyst was prepared by a modi?ed oil-drop sol–gel process[13,14].The starting material of?-Al2O3granules was high-concentration(1.8M)boehmite sol(from SASOL).The1.8M boehmite sol was?rst mixed with a small amount of1M HNO3(the volume ratio of acid/sol was 1:5).The modi?ed sol was stirred for15min at70?C by a mag-netic stirrer.A dramatic decrease of the pH of the sol by adding HNO3substantially accelerated the gelation process.After aging for half an hour at60–70?C,the pure1.8M boehmite sol became very viscous and it could not be stirred by the magnetic stirrer even at the maximum power.The very viscous sol was then trans-ferred to a dropper as the starting material for the granulation process.

The granulation process included the generation of sol droplets by the dropper,shaping,partially gelating the droplets into spherical wet-gel granules in a paraf?n oil layer(color: white;density:0.7864g/cm3;kinematic viscosity:34.5cs at 40?C,from J.T.Baker)and consolidating the structure of the wet-gel granules in a8wt.%ammonia solution layer.The paraf-?n oil layer and ammonia solution layer were kept at room temperature.The interface between the oil and ammonia solu-tion was slowly stirred to facilitate the transport of wet granules across the interface.After aging in the ammonia layer for at least45min,the spherical wet-gel granules(about1–2mm in diameter)were removed from the ammonia solution,carefully washed with water and alcohol sequentially,dried at40?C for 48h,and?nally calcined in air at450?C for6h.

The active metal ZnO was coated by incipient wetness impregnation method[9].The volume of impregnation solu-tion was estimated to equal to the volume of granular support. The precursors of zinc oxide were then weighed and mixed with distilled water to prepare the impregnation solution.The concen-tration of zinc in the catalyst was set at1,5and10%,respectively. The granular Al2O3support was then put into the impregnation solution and stirred at room temperature for8h.After the incip-ient wetness impregnation process,the granular catalysts were dried at120?C for12h and calcined in air at550?C for6h.Two types of zinc oxide precursors were used in this study to compare the differences.The?rst one was commercial zinc oxide pow-der with the average particle diameter of100nm.The second one was zinc nitride which is very soluble and can transform to zinc oxide by thermal calcinations.For easy expression,the cat-alysts prepared from different zinc oxide precursors are named as ZnO/Al2O3(O)and ZnO/Al2O3(N),respectively hereafter.It has to state that the precursor Zn(NO3)2for ZnO/Al2O3(N)cat-alyst can transform into ZnO completely after calcination in air at550?C for6h.There is no Zn3N2or Zn(NO3)2in the catalyst and that can be proved from the analyses results that no N peak was found in SEM/EDS spectra and no Zn3N2or Zn(NO3)2 peak was found in XRPD spectra.

2.2.Test of catalyst activity

A catalysis reaction system was set up to measure the activ-ity of granular ZnO/Al2O3catalyst.As shown in Fig.1,the experimental equipments are composed of pure gas cylinders, mass?ow meters,a generator of volatile TCE gas,a quartz reaction tube,an electric heater,and a programmable tempera-ture controller.The on-line gas analyzers of Fourier transform infrared spectrograph(FT-IR,Perkin-Elmer:Spectrum One)and Gas chromatograph-?ame ionization detector(GC-FID,Varian: CP-3800)were used to monitor the concentrations of reac-tion produces in the ef?uent.The concentration and?ow rate of volatile TCE gas were accurately controlled by mass?ow meters.The total?ow rate and concentration of TCE gas were controlled at500ml min?1and450ppm,respectively.The?ow rates of air and N2were controlled at480and0ml min?1as the

90J.-C.Chen,C.-T.Tang /Journal of Hazardous Materials 142(2007)

88–96

Fig.1.Diagram of experimental apparatus.

in?uent O 2concentration was 21%.The other 20ml min ?1N 2was used to evaporate pure TCE liquid (from J.T.Baker)to gen-erate TCE gas.The temperature of water bath in the generator of TCE gas was controlled at 40?C.The concentration of gener-ated TCE gas was rechecked by FT-IR gas analyzer and required to keep steady at least for 5min before performing every test.After that,0.67g ZnO/Al 2O 3catalysts were put in the middle of quartz tube and ?xed from both sides by quartz ?bers.As the reaction temperature was preheated to the required value and kept steady for 25min,the generated TCE gas was introduced into the quartz tube and the gas analyzer FT-IR was turned on.The compositions and concentrations of reaction products in the ef?uent of catalyst reactor were continuously scanned and moni-tored.The scanning range of FT-IR spectra was 450–4000cm ?1and the instrument resolution was 4cm ?1.The concentrations of TCE and other compounds were also analyzed and rechecked by GC-FID.The operation temperatures of GC-FID were 200?C at injector,180?C at column (equity-5)and 200?C at detector.To con?rm the conversion of TCE was complete and stable,each test was performed for at least 50min.After the catalyst test was ?nished,the ?ow meters and electric heater were shut down and the reacted catalyst was taken out for further analyses.Table 1lists the experimental conditions of every test.

2.3.Characteristic analyses of catalyst

The surface areas of catalysts were measured at 77K by the gravimetric methods with a vacuum microbalance (Micromerit-ics:Gemini 2360).Theses results provide a comparison of the surface area between fresh and reacted catalysts.N 2adsorption–desorption procedure was used to determine the textural properties.The Brunauer–Emmett–Teller (BET)sur-face area was calculated from the adsorption isotherm.The average pore diameter was obtained from the pore size distri-bution.An X-ray powder diffractometer (XRPD,SIEMENS:D5000)with a Cu K ?radiation was used to identify the crys-talline species of zinc and aluminum on the catalyst.Diffraction patterns were manually analyzed with JCPDS card (standard patterns).The scanning range of 2θwas 20–80?in steps of 0.04?.The scanning speed was 4?min ?1.The surface struc-ture and the accumulation of contaminants on the surface of reacted catalyst were observed by a scanning electron micro-scope (SEM,TOPCON:ABT-150S)at the Regional Instrument Center in National Chung-Hsing University (Taichung City,Tai-wan).The acceleration voltage was 0.5–40kV and the resolution was 4nm.The samples used for SEM micrography needed dry-ing for 8h at 105?C in an oven and stored in a desiccator

Table 1

List of experimental conditions Run Catalyst Impregnation concentration of Zn (wt.%)Calcinations temperature (?C)Operation

temperature (?C)Oxygen

concentration (%)Space velocity (h ?1)

1–5–

––30,150,250,350,45021360006–10ZnO/Al 2O 3(N)1055030,150,250,350,450213600011–15ZnO/Al 2O 3(O)1055030,150,250,350,45021

3600016–18ZnO/Al 2O 3(N)105504505,10,1536000

19–21ZnO/Al 2O 3(N)105504502112000,18000,7200022–24ZnO/Al 2O 3(N)1,5,10550

450213600025–27

ZnO/Al 2O 3(N)

10

450,650,750

450

21

36000

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to prevent the interference of moisture.The compositions and relative amounts of elements on the surface of catalyst were determined by an energy dispersive spectroscopy(EDS,LINK: exLII)with a Kevex superdry detector.In addition,the prepared catalysts were also analyzed by the electron spectroscopy for chemical analysis system(ESCA,VG Scienti?c:ESCALAB 250)using Mg K?(hν=1253.6eV)as the radiation source to con?rm their chemical compositions.

3.Results and discussions

3.1.Characteristics of granular ZnO/Al2O3catalyst

The characteristics of granular ZnO/Al2O3catalyst prepared by modi?ed oil-drop sol–gel process and incipient wetness impregnation method was measured before the activity test. Table2indicates that the BET surface areas of fresh Al2O3 support,ZnO/Al2O3(O)and ZnO/Al2O3(N)catalysts are386.8, Table2

BET surface area of ZnO/Al2O3catalyst

Catalyst BET surface area(m2/g) Al2O3(support)386.8

ZnO/Al2O3(O)(fresh)297.0

1%ZnO/Al2O3(N)(fresh)209.3

5%ZnO/Al2O3(N)(fresh)201.0

ZnO/Al2O3(N)(30?C reacted)368.0

ZnO/Al2O3(N)(150?C reacted)173.3

ZnO/Al2O3(N)(250?C reacted)187.5

ZnO/Al2O3(N)(350?C reacted)187.9

ZnO/Al2O3(N)(450?C reacted)171.3297and209.3m2g?1,respectively.The surface area of fresh Al2O3support is greater than that of general commercial sup-port,but is decreased after the impregnation of active metal ZnO. The surface area of ZnO/Al2O3(O)catalyst is greater than that of ZnO/Al2O3(N),implying that using nano-ZnO powder as the precursor of active metal is better than Zn(NO3)2for the preparation of ZnO/Al2O3catalyst.This result can be illus-trated by the SEM micrographs of fresh ZnO/Al2O3(N)and ZnO/Al2O3(O)catalysts(Fig.2).The surface and pore distribu-tions of fresh ZnO/Al2O3(N)catalyst are smooth and clogged, while the surface of fresh ZnO/Al2O3(O)catalyst is porous and uniform.Fig.3shows the EDS spectra of fresh Al2O3support, ZnO/Al2O3(N)and ZnO/Al2O3(O)catalysts.The result illus-trates that aluminum and zinc are the major elements in the ZnO/Al2O3(N)and ZnO/Al2O3(O)catalysts,and indicates that the catalysts are not contaminated with other elements during the preparation processes.

To con?rm the chemical composition of active metals in the ZnO/Al2O3catalyst,the electron spectroscopy spectra of gran-ular catalysts are provided in Fig.4.The binding energies of Zn2p3/2,Zn2p1/2and O1s are1019.9,1042.70and530.5eV, respectively.They are identical to the standard spectra of Zn2+ and O2?[15–17].ZnO is therefore proved to be the major active species in the catalyst.There is no peaks for N1s(398.8eV)and Zn3N2observed in the XPS spectra of ZnO/Al2O3(N)catalyst, because the catalyst is prepared at low nitride concentrations(1, 5and10%)and the corresponding N concentrations are very low (0.34,1.7and3.4%)and the catalyst is calcined in air at550?C for6h to completely convert the zinc nitride into zinc oxide. This can be proved from the analyses results that no N peak is found in SEM/EDS spectra and no Zn3N2or Zn(NO3)2

peak Fig.2.SEM micrographs of ZnO/Al2O3(N)and ZnO/Al2O3(O)catalysts(fresh and reacted).

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88–96

Fig.3.EDS spectra of fresh Al 2O 3support and ZnO/Al 2O 3catalysts.

is found in XRPD spectra.On the other hand,the O 1s peak in the XPS spectra is smooth,symmetrical and locates at 530.5eV for ZnO/Al 2O 3(O)and 531.0eV for ZnO/Al 2O 3(N).The O 1s peak at 530.5eV for ZnO/Al 2O 3(O)is attributed to Zn–O bonds because this value is in good agreement with previous refer-ences [16–18].The O 1s peak at 531.0eV for ZnO/Al 2O 3(N)shifts 0.5eV toward higher binging energy side from the O 1s peak for Zn–O bonds.This shows that few O–H bonds may be formed due to absorbed H 2O molecules on the catalyst [18].3.2.Effect of different catalyst preparation conditions 3.2.1.Different active metal precursors

Fig.5shows the conversions of TCE by different ZnO/Al 2O 3(N)and ZnO/Al 2O 3(O)catalysts at different oper-ation temperature.The other operation conditions were identi-cal:TCE 450ppm,oxygen 21%,operation temperature 450?C and space velocity 36,000h ?1.Without catalyst (blank test),the conversion of TCE is slightly increased with the increase of operation temperature and is only 13%at 450?C.As the

ZnO/Al 2O 3(N)and ZnO/Al 2O 3(O)catalysts are present,the conversions of TCE are improved,especially at the opera-tion temperature of 450?C.The performance of ZnO/Al 2O 3(N)catalyst is slightly better than that of ZnO/Al 2O 3(O)as the operation temperature is higher than 250?C.The best con-version of TCE by ZnO/Al 2O 3(N)catalyst is 94%at 450?C.From the FT-IR spectra of reaction products (Fig.6),the peaks of CO and HCl can be observed besides the major compound TCE.The peak of CO emitted from the catalytic incineration of TCE at 450?C by ZnO/Al 2O 3(O)is higher than that by ZnO/Al 2O 3(N).Because CO is a major byprod-uct of incomplete oxidation of hydrocarbons,the higher con-centration of CO means a lower catalytic activity.Therefore,both ZnO/Al 2O 3(N)and ZnO/Al 2O 3(O)catalysts have catalytic activities for TCE decomposition and ZnO/Al 2O 3(N)is better than ZnO/Al 2O 3(O).

3.2.2.Different concentrations of active metal

Fig.7shows the conversions of TCE by ZnO/Al 2O 3(N)cata-lyst with different concentrations of active metal (1,5and 10%).

J.-C.Chen,C.-T.Tang /Journal of Hazardous Materials 142(2007)88–96

93

Fig.4.ESCA spectra of ZnO/Al 2O 3(O)catalyst:(a)Zn 2p and (b)O

1s.

Fig.5.Conversions of TCE by ZnO/Al 2O 3(O)catalysts at different operation

temperatures.

Fig.6.FT-IR spectra for the ef?uent reaction

products.

Fig.7.Conversions of TCE by ZnO/Al 2O 3(N)catalysts with different concen-trations of active metal.

The operation temperature and space velocity were all controlled at 450?C and 36,000h ?1,respectively.The conversions of TCE by granular catalysts coated with 5and 10%active metal (ZnO)are similar and both are higher than 96%.The conversion of TCE by the catalyst coated with 1%ZnO is lower than 60%.More active metal coated on the support of catalyst is supposed to pro-vide more reaction sites for catalytic decomposition of TCE gas.On the other hand,the BET surface areas of the ZnO/Al 2O 3(N)catalysts coated with 1,5and 10%ZnO are 209.3,201and 195.5m 2g ?1,respectively.The BET surface area of catalyst is slightly decreased as the concentration of active metal increased.Catalyst coated with too much active metal will block its sur-face area and is more expensive.Therefore,the granular catalyst coated with 5%active metal is considered to be the effective and economic one in our experiment.

3.2.3.Different calcination temperatures

Fig.8shows the conversions of TCE by ZnO/Al 2O 3(N)cat-alyst prepared at different calcination temperatures (450,550,650and 750?C).The other operation conditions are identical.ZnO/Al 2O 3(N)catalyst prepared at the calcination temperature of 550?C has better performance.Calcination temperature can in?uence the characteristic of active metal,and the porosity and surface areas of catalysts [10,13,14,17].This result can also be illustrated by the SEM micrographs in Fig.9.The surface mor-phology of ZnO/Al 2O 3(N)catalyst calcined at 550?C has more and uniform porosity than that at 450and 650?C.Moreover,the surface of ZnO/Al 2O 3(N)catalyst is sintered and melted at higher calcination temperatures 650and 750?

C.

Fig.8.Conversions of TCE by ZnO/Al 2O 3(N)catalysts prepared at different calcination temperatures.

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88–96

Fig.9.SEM micrographs of ZnO/Al 2O 3(N)catalysts prepared at different calcinations temperatures.

3.3.Effect of different catalytic reaction conditions

3.3.1.Different reaction temperatures

Fig.10shows the conversions of TCE by ZnO/Al 2O 3(N)catalyst at different reaction temperatures.The conversion of TCE is increased from 18to 33%as the reaction temperature is increased from 30to 350?C.A signi?cant increase of TCE conversion (94%)can be observed as the reaction temperature rises to 450?C.As a result,the performance of ZnO/Al 2O 3(N)catalyst is outstanding at high operation temperature 450?C.This ?nding is also identical to the studies of Liu et al.[19]and Takemoto et al.[12];both indicated that the activities of catalysts for the decomposition of organic pollutants were increased with the temperature.

From the EDS analyses,some peaks of elemental chlorine can be found on the reacted ZnO/Al 2O 3(N)catalyst as the

oper-

Fig.10.Conversions of TCE by ZnO/Al 2O 3(N)catalysts at different operation temperatures.

ation temperature was higher than 250?C,which demonstrated that TCE is signi?cantly decomposed by the ZnO/Al 2O 3(N)catalyst at such temperature.Moreover,the BET surface area of ZnO/Al 2O 3(N)catalyst is reduced to 170–185m 2g ?1as the reaction temperatures were higher than 150?C (Table 2).The decreases of BET surface areas at high temperatures are attributed to the sintering of catalyst materials and the aggrega-tions of reaction residues on the surface of catalysts.The surface morphologies of fresh and reacted catalysts are quite different.As shown in Fig.3,the surface and porosity of fresh catalyst are smooth and uniform,while the reacted catalysts are sintered,melted,or blocked with reaction residues.These phenomena are especially evident for the reacted catalysts which operation temperature was 450?C.

3.3.2.Different oxygen concentrations

For studying the effects of different oxygen concentrations on the performances of ZnO/Al 2O 3(N),the concentrations of oxygen in the feed gas were controlled at 21,15,10and 5%,respectively.As shown in Fig.11,the conversions of TCE by ZnO/Al 2O 3(N)catalyst are all higher than 95%at these four O 2concentrations.This result indicates that the decomposition of TCE gas by ZnO/Al 2O 3(N)catalyst is not sensitive to these four O 2concentrations,because these O 2concentrations in the feed gas are much greater than the stoichiometric O 2concentration (1913ppm)required for the complete decomposition of TCE.This good performance of ZnO/Al 2O 3(N)catalyst at low O 2concentration also provides a outstanding advantage in future application.

J.-C.Chen,C.-T.Tang /Journal of Hazardous Materials 142(2007)88–96

95

Fig.11.Conversions of TCE by ZnO/Al 2O 3(N)catalyst at different oxygen

concentrations.

Fig.12.Conversions of TCE by ZnO/Al 2O 3(N)catalysts at different space velocities.

3.3.3.Different space velocities

The conversions of TCE at different space velocities (72,000,36,000,18,000and 12,000h ?1)are shown in Fig.12.The best conversion of TCE (98%)is occurred at space velocity 18,000h ?1,the next is 72,000h ?1(97%),36,000h ?1(96%),and the last is 12,000h ?1(85%).Decreasing space velocity increases the retention time of TCE gas in the catalyst bed and the conversion of TCE increases,but our results show that the conversion of TCE at space velocity 12,000h ?1is the least.This phenomenon can be interpreted from the FT-IR spectra of reac-tion products.As shown in Fig.13,the peak intensities of CO and HCl become higher and lower,respectively,as the

space

Fig.13.FT-IR spectra for the ef?uent reaction products at different space veloc-ities.

velocities are decreased from 72,000to 12,000h ?1.The higher concentrations of CO in the ef?uent gas indicate that the cat-alytic decomposition of TCE is not complete.Some residues are accumulated on the surface of catalyst and the performance of catalyst decreases.4.Conclusion

This study tries to prepare granular ZnO/Al 2O 3catalysts for the catalytic incineration of hazardous TCE gas.The effects of different preparation and operation conditions on the perfor-mances of catalysts are also investigated.Experimental results show that the granular ZnO/Al 2O 3catalyst has good catalytic activities on TCE decomposition and the conversion of TCE is 98%.ZnO/Al 2O 3(N)catalyst has better performance than ZnO/Al 2O 3(O)at high operation temperature.Five percent of active metal concentration and 550?C calcination temperature are the better and economic preparation conditions,and the opti-mum operation temperature and space velocity are 450?C and 18,000h ?1,respectively.The conversions of TCE are similar and all higher than 90%at these four O 2concentrations in the feed gas.By FT-IR measurement,the major reaction products during catalytic decomposition of TCE are HCl and CO 2.The BET surface areas of catalysts are signi?cantly decreased as the calcinations temperature is higher than 550?C due to the sintering of catalyst materials and as the reaction temperature is higher than 150?C due to the accumulations of reaction residues on the surfaces of catalysts.These results are also demonstrated by SEM micrographs and EDS spectra.References

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expand/enlarge one’s scope of knowledge knowledge reserve/base/storage theoretical knowledge practical skills social experience broaden one’s knowledge base promote one’s overall/ comprehensive competence accumulate experiences learn lessons from past experiences Work and experience the scarcity of employment o p p o r t u n i t i lay the foundations for career p r o s p e r i t y

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