CN101642695B - Device for studying compound reaction of photocatalysis and enzyme catalysis - Google Patents
Device for studying compound reaction of photocatalysis and enzyme catalysis Download PDFInfo
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- CN101642695B CN101642695B CN2009101702034A CN200910170203A CN101642695B CN 101642695 B CN101642695 B CN 101642695B CN 2009101702034 A CN2009101702034 A CN 2009101702034A CN 200910170203 A CN200910170203 A CN 200910170203A CN 101642695 B CN101642695 B CN 101642695B
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Abstract
The invention discloses a device for studying compound reaction of photocatalysis and enzyme catalysis, comprising a catalytic reactor, a magnetic stirrer, an ultraviolet light source, a lucifugal external hood, a film compressing ring suite and a porous lucifugal hood. The invention is mainly used in compound activity evaluation on photocatalysis and enzyme catalysis and dynamic study for degrading organic pollutants.
Description
Technical field
Apparatus of the present invention relate to a kind of device that is used for photocatalysis and enzymatic studying compound reaction, are mainly used in photocatalysis and the evaluation of enzymatic composite reactive, the degradation of contaminant dynamics research.
Background technology
The chlorophenols material is a class difficult degradation compound, is widely used in for a long time in the production of wood preservation, Insecticides (tech) ﹠ Herbicides (tech), agricultural chemicals, fuel and plasticizer etc.Its factory effluent is poisoned very big, and biological tissue is had stronger denaturation, intense stimulus skin, mucous membrane, and have corrosivity.The toxicity of chlorophenol increases with the increase of its chlorination degree, and difficult degradation.In in the water harmful substance or priority pollutant " blacklist " are listed it by country such as the U.S., China.Therefore, how eliminating the pollution of chlorophenols compound in the environment becomes and is subjected to the problem extensively paid attention to.The method that at present common control chlorophenol pollutes has ultrafiltration, chemical deposition method, activated sludge process, aerobic/anaerobic process etc.In recent years, increasingly mature along with photocatalysis technology and enzyme technology, the two is occupying leading position aspect the chlorophenol pollutant gradually removing.But all there are certain technological deficiency in photocatalysis and enzyme technology, at present still can not large-scale application.
Laccase (Laccase) is a kind of one-electron oxidation reductase, can carry out oxidisability polymerization and depolymerization to the multiple aromatic compound that comprises chlorophenols compound, directly parachlorphenol dechlorination, thus reach the purpose of chlorophenol detoxification.Laccase is removed chlorophenol pollutant and is shown certain advantage than conventional method, as decomposition efficiency height, simple to operate, applied widely, is one of research focus of present chlorophenol pollutant process field.But use free laccase or immobilization laccase also to have the cost height, be subject to weak point such as extraneous factor interference.Particularly laccase is low to the degradation capability of high chloro chlorophenol is enzymatic inherent shortcoming, is difficult to overcome; The photocatalytic applications technical matters is simple, with low cost, but non-selectivity ground catalytic decomposition bacterium and pollutant have characteristics such as high catalytic activity, good chemical stability and heat endurance, non-secondary pollution, nonirritant, safety non-toxic.But photocatalysis is subject to the dependence to light source, particularly ultraviolet source.Therefore energy consumption and the economy problems that can't avoid its degradation process.
The two combination is expected to overcome above-mentioned defective, as realize that water treatment procedure has light not have continuity under the optical condition, raising is to the degradation rate of high chloro chlorophenol (as pentachlorophenol), and the defensive ability/resistance ability that disturbs of the factor to external world of can strengthening, and improves the detoxification efficient to multiple chlorophenol.But the necessary ultraviolet light of light-catalyzed reaction has considerable influence to enzymatic activity, can cause brokenly ring and damage to the protein structure of enzyme; The restriction that catalytic effect also can be subjected to the differential responses form is carried out in enzymatic and photocatalysis in same reaction system.This reacts in same system the two and has constituted obstacle, needs the design novel reactor to avoid the problems referred to above.Catalytic reactor has directly determined the efficient of catalytic reaction as the main equipment of reaction, because the several factors such as geometric position of the material of reactor, structure, shape, light source have determined the performance of catalyst activity and to the situations such as utilization of the energy.So how improving catalyst utilization and making catalyst activity, stability obtain maximum performance has become the center that reactor is developed and developed, also has been one of emphasis of ambient water processing research.
Secondly, catalytic activity to the composite catalyzing reaction does not have unified evaluation criterion and standard, the designed device of different researchers differs greatly, the evaluation method difference, the experimental result of different experiments chamber does not have comparativity to make Many researchers be compelled to do much to repeat work, thereby influenced the development of water technology, therefore, the composite catalyzing reactor of demanding development of new urgently is to realize the purpose of accurate control, highly effective reaction and instant evaluation to reaction.
Summary of the invention
The purpose of apparatus of the present invention is to overcome above-mentioned deficiency, provides a kind of simple in structure, easy to operate, can estimate the device of the composite catalyzing activity of all kinds photochemical catalyst and immobilized enzyme catalysis.
Apparatus of the present invention realize by following scheme:
A kind of device that is used for photocatalysis and enzymatic studying compound reaction comprises the porous lucifuge cover 6 of lucifuge outer cover 4, mould ring set spare 5 and tubular of ultraviolet source 3, the tubular of catalytic reactor 1 cylindraceous, magnetic stirring apparatus 2, tubulose.Catalytic reactor 1 is flat upper shed cylinder, is placed on the magnetic stirring apparatus 2, to realize the even dispersion to the reactor Dissolve things inside.The a plurality of ultraviolet lamp tubes of vertical distribution are as ultraviolet source 3 on every side 1 of catalytic reactor, and ultraviolet source 3 adds tubular lucifuge outer cover 4 outward, to prevent the injury of short wave ultraviolet light to the people.At catalytic reactor 1 inner mould ring set spare 5 and the porous lucifuge cover 6 that connects that insert.Mould ring set spare 5 vertically is inserted in the inside of tubular porous lucifuge cover 6, to avoid the injury of ultraviolet light to enzyme.
Described catalytic reactor 1 is quartzy material;
Described magnetic stirring apparatus 2 is commercially available plain edition, adjustable rotating speed, maximum speed 1200rpm;
Described ultraviolet source 3 is commercially available Ultraluminescence lamp, tubulose, and dominant wavelength is 365nm;
Described mould ring set spare 5 is a stainless steel, be made up of a plurality of stainless steel rings, the stainless steel ring side has a plurality of circular holes equably, during use enzyme membrane is clipped between two annulus, compress layer by layer and be combined into a long tube and place in the porous lucifuge cover, circular hole is used to provide the passage of water body exchange;
Described lucifuge outer cover and porous lucifuge cover are stainless steel, and lucifuge outer cover top and porous lucifuge cover top are welded together by annulus.Evenly open a plurality of holes on the annulus, to place ultraviolet lamp tube.Evenly have a plurality of circular holes on the porous lucifuge cover barrel, can guarantee that the inside and outside water body fully exchanges, again can ultraviolet shielding to prevent its infringement to enzyme.
This device adopts the enzyme catalyst of graininess photochemical catalyst and film immobilization; During reaction, reactant liquor places quartzy catalytic reactor, is blended in mutually with powder photocatalyst to be the suspended state reaction under the UV-irradiation; After the immobilized enzyme catalysis film is fixed by the pressure ring external member, at lucifuge protective cover internal reaction.
Advantage of the present invention is to separate photocatalysis and enzymic catalytic reaction district by porous lucifuge cover, preventing the destruction of ultraviolet light to enzyme, simultaneously again can guarantee system between the abundant exchange of water body, can work in coordination with light enzymatic system, Each performs its own functions to make the two, do not interfere with each other, and plays a role jointly.
The light-catalyzed reaction part can place quartz reactor with powder photocatalyst, and ultraviolet lamp tube places the reactor outside; The immobilised enzymes film catalyst utilizes the pressure ring external member to compress layer by layer, and can settle 1～10 layer of diameter is 20 millimeters enzyme catalyst film.After sample enters reactor, open the power supply of ultraviolet lamp tube, according to the curve of timing sampling concentration, carry out dynamics research to the time, can obtain apparent complete degradation reaction speed constant, be used to estimate photocatalysis and enzymatic composite catalyzing activity.
This device also can be estimated separately photocatalysis or enzymatic.When carrying out the photocatalysis evaluation, do not use metal crimp ring set spare and enzyme membrane catalyst; When carrying out the enzymatic activity evaluation, do not open uviol lamp, do not use powder photocatalyst.Use separately, do not influence the evaluation effect of this device.
Description of drawings
Fig. 1 is used for the device schematic diagram of composite catalyzing repercussion study for the present invention;
Wherein: catalytic reactor (1), magnetic stirring apparatus (2), ultraviolet source (3), lucifuge outer cover (4), mould ring set spare (5), porous lucifuge cover (6);
Fig. 2 is lucifuge outer cover and porous lucifuge cover design drawing;
Fig. 3 a be single mould ring design drawing, Fig. 3 b be used for combined films pressure ring external member be fixed in stainless steel sleeve design drawing in the porous lucifuge cover, the two is collectively referred to as mould ring set spare; Fig. 3 c is the quartz reactor design drawing;
Fig. 4 is this reactor when loading the immobilization laccase catalyst separately to 2, and the clearance of 4-two chlorophenols and pentachlorophenol mixed liquor changes;
Fig. 5 for this reactor when adding carried photocatalyst separately to 2, the clearance of 4-two chlorophenols and pentachlorophenol mixed liquor changes;
To 2, the clearance of 4-two chlorophenols and pentachlorophenol mixed liquor changed when Fig. 6 loaded immobilization laccase catalyst and photochemical catalyst at the same time for this reactor.
The specific embodiment
The present invention is the new device that is used for photocatalysis and the repercussion study of enzymatic composite catalyzing, comprises the porous lucifuge cover 6 of lucifuge outer cover 4, mould ring set spare 5 and tubular of ultraviolet source 3, the tubular of catalytic reactor 1 cylindraceous, magnetic stirring apparatus 2, tubulose.Catalytic reactor 1 is flat upper shed cylinder, is placed on the magnetic stirring apparatus 2, to realize the even dispersion to the reactor Dissolve things inside.Eight ultraviolet lamp tubes of vertical distribution are as ultraviolet source 3 on every side 1 of catalytic reactor, and ultraviolet source 3 adds tubular lucifuge outer cover 4 outward, to prevent the injury of short wave ultraviolet light to the people.At catalytic reactor 1 inner mould ring set spare 5 and the porous lucifuge cover 6 that connects that insert.Mould ring set spare 5 vertically is inserted in the inside of tubular porous lucifuge cover, to avoid the injury of ultraviolet light to enzyme.
Described catalytic reactor is quartzy material, tube diameter of phi 64mm, and high 300mm can contain solution 800mL;
Described magnetic stirring apparatus adopts Jintan City's gold to divide the magnetic stirring apparatus of the 85-2 model of instrument Co., Ltd production, adjustable rotating speed, maximum speed 1200rpm;
Described ultraviolet source adopts the Ultraluminescence lamp of the ADJT15365 model of U.S. nature gene Co., Ltd production, tubulose, and long 250mm, diameter of phi 20mm, dominant wavelength is 365nm;
Described lucifuge outer cover and porous lucifuge cover are stainless steel, highly are respectively 250mm and 240mm, and radius is respectively Φ 124mm and Φ 41mm.The lucifuge outer cover is apart from catalytic reactor barrel 30mm, and top and porous lucifuge cover top are welded together by annulus.Evenly open the hole of eight Φ 24mm on the annulus, to place ultraviolet lamp tube, close up and be Φ 64mm in the bottom.Evenly open the circular hole of 500～1000 Φ 3mm on the porous lucifuge cover barrel, can guarantee that the inside and outside water body fully exchanges, can prevent its infringement by ultraviolet shielding again enzyme.Closing up and be Φ 23mm in porous lucifuge cover bottom, is positioned over porous lucifuge cover inside to guarantee that mould ring set spare can be stablized.
Described mould ring set spare 5 is a stainless steel, by a plurality of external diameters is Φ 24mm, stainless steel ring and the fixed muffle of height 14mm are formed, each 2mm place, stainless steel ring bottom reducing is Φ 21mm, the stainless steel ring side is opened the circular hole of 4 Φ 9mm equably, during use enzyme membrane is clipped between two annulus, compresses layer by layer to be combined into a long tube, be fixed in the porous lucifuge cover under the stainless steel sleeve is assisted, its side circular hole can provide the passage of water body exchange.
Photochemical catalyst is taked powder type, opens ultraviolet source 3 add target substance to be measured in photo catalysis reactor after, under UV-irradiation, and organic pollutions such as catalytic oxidation chlorophenols, its product is carbon dioxide, water and chlorion; Immobilized enzyme catalysis agent film is cut into the thin slice of 20 millimeters of diameters, is fixed in porous lucifuge cover 6 inside layer by layer with the pressure ring external member, carries out simultaneously with light-catalyzed reaction, and its product is chlorophenol dimer, oligomer and high polymer.Timing sampling according to the curve of chlorophenol concentration to the time, carries out dynamics research and calculates.Estimate the composite catalyzing activity of photochemical catalyst and enzyme catalyst.
Adopting the immobilization laccase amount is 10 enzyme membranes (always being equivalent to the free laccase of 5mg than vigor), the photochemical catalyst consumption is under the situation of 0.5g/L, in reactor of the present invention, be pentachlorophenol (PCP) 10mg/L to concentration, 2, the 500mL simulated wastewater of 4-two chlorophenols (DCP) 10mg/L is handled.
Use immobilization laccase reaction 5 hours separately, reactor is to 2, and the clearance of 4-two chlorophenols and pentachlorophenol is respectively 45% and 35.1%; Use photochemical catalyst reaction 3 hours separately, reactor is to 2, and the clearance of 4-two chlorophenols and pentachlorophenol is respectively 55.4% and 82.7%; As seen laccase is to pentachlorophenol, and photochemical catalyst is to 2, and the degradation effect of 4-two chlorophenols is relatively poor.
The two is compound, in reactor of the present invention, carry out water treatment experiment, the degradation rate of 4-two chlorophenols and pentachlorophenol can reach 66.1% and 79.9%, 7 hour respectively and more can reach 82.5% and 84.3% to 2 in 5 hours.This shows that the two compound object selectivity defective that can effectively remedy two kinds of water technologies reaches the removal effect of better parachlorphenol pollutant.
Claims (5)
1. device that is used for photocatalysis and enzymatic studying compound reaction is characterized in that: described device comprises the porous lucifuge cover (6) of lucifuge outer cover (4), mould ring set spare (5) and tubular of ultraviolet source (3), the tubular of catalytic reactor cylindraceous (1), magnetic stirring apparatus (2), tubulose; Catalytic reactor (1) is flat upper shed cylinder, is placed on the magnetic stirring apparatus (2), to realize the even dispersion to solution in the reactor; The a plurality of ultraviolet lamp tubes of vertical distribution are as ultraviolet source (3) around catalytic reactor (1) tube, and ultraviolet source (3) is outer to add tubular lucifuge outer cover (4), to prevent the injury of short wave ultraviolet light to the people; At inner mould ring set spare (5) and the porous lucifuge cover (6) that connects that insert of catalytic reactor (1); Mould ring set spare (5) vertically is inserted in the inside of tubular porous lucifuge cover, to avoid the injury of ultraviolet light to enzyme;
Mould ring set spare (5) is a stainless steel, by a plurality of external diameters is Φ 24mm, stainless steel ring and the fixed muffle of height 14mm are formed, each 2mm place, stainless steel ring bottom reducing is Φ 21mm, the stainless steel ring side is opened the circular hole of 4 Φ 9mm equably, during use enzyme membrane is clipped between two annulus, compresses layer by layer to be combined into a long tube, be fixed in the porous lucifuge cover under the stainless steel sleeve is assisted, its side circular hole can provide the passage of water body exchange.
2. device as claimed in claim 1 is characterized in that: the material of described catalytic reactor (1) is for quartzy; The material of lucifuge outer cover (4), mould ring set spare (5) and porous lucifuge cover (6) is a stainless steel.
3. device as claimed in claim 1 is characterized in that: this device adopts the enzyme catalyst of graininess photochemical catalyst and film immobilization.
4. device as claimed in claim 1 is characterized in that: it is the Ultraluminescence lamp of 365 nanometers that ultraviolet source (3) adopts dominant wavelength.
5. device as claimed in claim 1 is characterized in that: described device can also be estimated separately photocatalysis or enzymatic.
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| CN101785985B (en) * | 2010-03-29 | 2011-04-20 | 北京师范大学 | Device used for combination reaction study of photo catalysis and enzyme catalysis |
| CN102179029B (en) * | 2011-03-21 | 2012-08-08 | 北京交通大学 | Experimental apparatus of photocatalytic degradation antibiotic and other emerging contaminants |
| CN102701544B (en) * | 2012-06-29 | 2013-10-30 | 河海大学 | External-mounting photocatalytic - biological fluidized bed reactor |
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| CN101407803A (en) * | 2008-07-01 | 2009-04-15 | 北京师范大学 | Polylactic acid electrospinning fibre immobilized laccase and preparation thereof |
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