CN115340193A - Device and method for degrading bisphenol A by laccase in cooperation with photoelectrocatalysis - Google Patents
Device and method for degrading bisphenol A by laccase in cooperation with photoelectrocatalysis Download PDFInfo
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- IISBACLAFKSPIT-UHFFFAOYSA-N bisphenol A Chemical compound C=1C=C(O)C=CC=1C(C)(C)C1=CC=C(O)C=C1 IISBACLAFKSPIT-UHFFFAOYSA-N 0.000 title claims abstract description 179
- 108010029541 Laccase Proteins 0.000 title claims abstract description 73
- 238000000034 method Methods 0.000 title claims abstract description 27
- 230000000593 degrading effect Effects 0.000 title claims abstract description 22
- 238000006731 degradation reaction Methods 0.000 claims abstract description 48
- 230000015556 catabolic process Effects 0.000 claims abstract description 42
- 239000003792 electrolyte Substances 0.000 claims abstract description 33
- 108090000790 Enzymes Proteins 0.000 claims abstract description 17
- 102000004190 Enzymes Human genes 0.000 claims abstract description 17
- 238000005286 illumination Methods 0.000 claims abstract description 13
- 230000001590 oxidative effect Effects 0.000 claims abstract description 6
- 230000002195 synergetic effect Effects 0.000 claims abstract description 6
- 229910052797 bismuth Inorganic materials 0.000 claims description 18
- JCXGWMGPZLAOME-UHFFFAOYSA-N bismuth atom Chemical compound [Bi] JCXGWMGPZLAOME-UHFFFAOYSA-N 0.000 claims description 18
- LSGOVYNHVSXFFJ-UHFFFAOYSA-N vanadate(3-) Chemical compound [O-][V]([O-])([O-])=O LSGOVYNHVSXFFJ-UHFFFAOYSA-N 0.000 claims description 18
- 239000000243 solution Substances 0.000 claims description 14
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 13
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 11
- 239000004744 fabric Substances 0.000 claims description 10
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- UQSXHKLRYXJYBZ-UHFFFAOYSA-N iron oxide Inorganic materials [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 claims description 3
- NDLPOXTZKUMGOV-UHFFFAOYSA-N oxo(oxoferriooxy)iron hydrate Chemical compound O.O=[Fe]O[Fe]=O NDLPOXTZKUMGOV-UHFFFAOYSA-N 0.000 claims description 3
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- 229910052760 oxygen Inorganic materials 0.000 description 5
- 239000001301 oxygen Substances 0.000 description 5
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- CBACFHTXHGHTMH-UHFFFAOYSA-N 2-piperidin-1-ylethyl 2-phenyl-2-piperidin-1-ylacetate;dihydrochloride Chemical compound Cl.Cl.C1CCCCN1C(C=1C=CC=CC=1)C(=O)OCCN1CCCCC1 CBACFHTXHGHTMH-UHFFFAOYSA-N 0.000 description 3
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- 241000222355 Trametes versicolor Species 0.000 description 3
- 239000000356 contaminant Substances 0.000 description 3
- ZOMNIUBKTOKEHS-UHFFFAOYSA-L dimercury dichloride Chemical class Cl[Hg][Hg]Cl ZOMNIUBKTOKEHS-UHFFFAOYSA-L 0.000 description 3
- 239000000446 fuel Substances 0.000 description 3
- NLKNQRATVPKPDG-UHFFFAOYSA-M potassium iodide Chemical compound [K+].[I-] NLKNQRATVPKPDG-UHFFFAOYSA-M 0.000 description 3
- AZQWKYJCGOJGHM-UHFFFAOYSA-N 1,4-benzoquinone Chemical compound O=C1C=CC(=O)C=C1 AZQWKYJCGOJGHM-UHFFFAOYSA-N 0.000 description 2
- ISPYQTSUDJAMAB-UHFFFAOYSA-N 2-chlorophenol Chemical compound OC1=CC=CC=C1Cl ISPYQTSUDJAMAB-UHFFFAOYSA-N 0.000 description 2
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- IAZDPXIOMUYVGZ-UHFFFAOYSA-N Dimethylsulphoxide Chemical compound CS(C)=O IAZDPXIOMUYVGZ-UHFFFAOYSA-N 0.000 description 2
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 2
- PMZURENOXWZQFD-UHFFFAOYSA-L Sodium Sulfate Chemical compound [Na+].[Na+].[O-]S([O-])(=O)=O PMZURENOXWZQFD-UHFFFAOYSA-L 0.000 description 2
- OUUQCZGPVNCOIJ-UHFFFAOYSA-M Superoxide Chemical compound [O-][O] OUUQCZGPVNCOIJ-UHFFFAOYSA-M 0.000 description 2
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- 244000044283 Toxicodendron succedaneum Species 0.000 description 2
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- GNTDGMZSJNCJKK-UHFFFAOYSA-N divanadium pentaoxide Chemical compound O=[V](=O)O[V](=O)=O GNTDGMZSJNCJKK-UHFFFAOYSA-N 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000004070 electrodeposition Methods 0.000 description 2
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 2
- 239000005416 organic matter Substances 0.000 description 2
- 238000002360 preparation method Methods 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 229910052938 sodium sulfate Inorganic materials 0.000 description 2
- 235000011152 sodium sulphate Nutrition 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 229910021642 ultra pure water Inorganic materials 0.000 description 2
- 239000012498 ultrapure water Substances 0.000 description 2
- 238000005406 washing Methods 0.000 description 2
- FSJSYDFBTIVUFD-SUKNRPLKSA-N (z)-4-hydroxypent-3-en-2-one;oxovanadium Chemical compound [V]=O.C\C(O)=C\C(C)=O.C\C(O)=C\C(C)=O FSJSYDFBTIVUFD-SUKNRPLKSA-N 0.000 description 1
- 229930185605 Bisphenol Natural products 0.000 description 1
- 108010031396 Catechol oxidase Proteins 0.000 description 1
- 102000030523 Catechol oxidase Human genes 0.000 description 1
- JPVYNHNXODAKFH-UHFFFAOYSA-N Cu2+ Chemical compound [Cu+2] JPVYNHNXODAKFH-UHFFFAOYSA-N 0.000 description 1
- 102000043368 Multicopper oxidase Human genes 0.000 description 1
- 102000003992 Peroxidases Human genes 0.000 description 1
- 239000012327 Ruthenium complex Substances 0.000 description 1
- 229910021607 Silver chloride Inorganic materials 0.000 description 1
- 239000005708 Sodium hypochlorite Substances 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- FBXVOTBTGXARNA-UHFFFAOYSA-N bismuth;trinitrate;pentahydrate Chemical compound O.O.O.O.O.[Bi+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O FBXVOTBTGXARNA-UHFFFAOYSA-N 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
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- 229910001431 copper ion Inorganic materials 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 239000007857 degradation product Substances 0.000 description 1
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- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical compound [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 description 1
- 108040007629 peroxidase activity proteins Proteins 0.000 description 1
- 239000002957 persistent organic pollutant Substances 0.000 description 1
- 238000007146 photocatalysis Methods 0.000 description 1
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- 230000005622 photoelectricity Effects 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- 210000004994 reproductive system Anatomy 0.000 description 1
- HKZLPVFGJNLROG-UHFFFAOYSA-M silver monochloride Chemical compound [Cl-].[Ag+] HKZLPVFGJNLROG-UHFFFAOYSA-M 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 239000003115 supporting electrolyte Substances 0.000 description 1
- OJNFDOAQUXJWED-XCSFTKGKSA-N tatp Chemical compound NC(=S)C1=CC=C[N+]([C@H]2[C@@H]([C@@H](O)[C@H](COP([O-])(=O)O[P@@](O)(=O)OC[C@H]3[C@@H]([C@@H](OP(O)(O)=O)[C@@H](O3)N3C4=NC=NC(N)=C4N=C3)O)O2)O)=C1 OJNFDOAQUXJWED-XCSFTKGKSA-N 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/34—Biological treatment of water, waste water, or sewage characterised by the microorganisms used
- C02F3/342—Biological treatment of water, waste water, or sewage characterised by the microorganisms used characterised by the enzymes used
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/005—Combined electrochemical biological processes
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/34—Organic compounds containing oxygen
- C02F2101/345—Phenols
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2203/00—Apparatus and plants for the biological treatment of water, waste water or sewage
- C02F2203/006—Apparatus and plants for the biological treatment of water, waste water or sewage details of construction, e.g. specially adapted seals, modules, connections
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2303/00—Specific treatment goals
- C02F2303/14—Maintenance of water treatment installations
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- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/02—Specific form of oxidant
- C02F2305/023—Reactive oxygen species, singlet oxygen, OH radical
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- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W10/00—Technologies for wastewater treatment
- Y02W10/30—Wastewater or sewage treatment systems using renewable energies
- Y02W10/37—Wastewater or sewage treatment systems using renewable energies using solar energy
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Abstract
The invention belongs to the field of environmental protection, and discloses a device and a method for degrading bisphenol A by laccase synergistic photoelectrocatalysis, wherein the method specifically comprises the following steps: (1) Preparing a to-be-treated contaminated solution containing bisphenol A into an electrolyte; preparing a photoelectrode and a counter electrode, wherein the electrolyte and/or the counter electrode also contain a laccase component; (2) The photoelectrode and the counter electrode are inserted into the electrolyte, bias voltage and illumination are applied, laccase in the system can induce bisphenol A to be oxidized and polymerized, and meanwhile, the photoelectrode can generate active free radicals with strong oxidizing property under illumination conditions and bias voltage, so that enzyme-linked photoelectrochemical degradation of bisphenol A is realized. According to the invention, by improving key reaction participants and corresponding reaction mechanisms, compared with the prior art, the degradation efficiency of bisphenol A can be improved, and rapid conversion and removal of pollutants can be realized by coupling laccase catalytic degradation reaction with semiconductor photoelectrocatalysis to construct an enzyme-linked photoelectrocatalysis sewage treatment device.
Description
Technical Field
The invention belongs to the field of environmental protection, and particularly relates to a device and a method for degrading bisphenol A by laccase synergistic photoelectrocatalysis.
Background
Bisphenol a is a typical environmental endocrine disrupter, can enter the organism through polluted water sources and the like, and damages the endocrine system, the reproductive system and the like of the organism under low exposure level, so that the environmental pollution problem caused by the damage is widely concerned. Because bisphenol A has the characteristics of durability, difficult biodegradability and the like, the traditional physical adsorption method and biological treatment method cannot realize the rapid conversion and degradation of the pollutants. As a novel advanced oxidation technology, the photoelectrocatalysis combines the synergistic advantages of semiconductor photocatalysis and an electrochemical method, has the characteristics of mild reaction conditions, low energy consumption, no secondary pollution and the like, and is widely used in the research fields of environmental management, green energy utilization and the like. In the bisphenol A degradation aspect, the photoelectric catalysis efficiency is still low at present, and a certain gap is still formed between the photoelectric catalysis efficiency and the actual industrial application.
CN107946607B discloses an application of an electro-catalyst nickel oxide constructed photo-assisted fuel cell in degradation of pollutant bisphenol A, and CdS/TiO 2 NiO prepared by electrodeposition method with ITO electrode as anode x the/ITO electrode is used as a cathode, and the bisphenol A-sodium hypochlorite double-chamber light-assisted fuel cell is constructed and used for degradation research of bisphenol A in aqueous solution. The technical scheme can degrade bisphenol A into CO under the condition of no external voltage 2 And H 2 And O, the conversion of light energy and chemical energy to electric energy is realized simultaneously, the maximum degradation efficiency of visible light to the bisphenol A after continuous irradiation for 2 hours is 48%, and an improvement space also exists.
CN110921939A discloses an experimental method for degrading bisphenol A by polypyridine ruthenium complex photoelectrocatalysis [ Ru (bpy) 2 (tatp)] 2+ Sensitized TiO 2 The electrode is used as a photoanode, the Ag/AgCl electrode is used as a cathode, and the degradation effect of the electrode is monitored according to the change of the direct oxidation peak or mediated oxidation peak current of the bisphenol A solution on the ITO electrode before and after degradation along with the illumination time. According to the technical scheme, the bisphenol A in the electrolyte solution is used as a fuel, and the bisphenol A can be subjected to photoelectric induced oxidative degradation according to differential pulse voltammetry of the bisphenol A solution before and after ultraviolet illumination, wherein the degradation rate of the bisphenol A is 24.2% after 20min, and an improvement space exists.
In view of the above, the prior art still lacks a treatment method for realizing rapid conversion and degradation of organic pollutant bisphenol A.
The inventor of the invention has studied earlier in the subject group to obtain a device for treating chlorophenol pollutants by using photoelectric synergistic hydrogen peroxide and application thereof (see China patent application CN114162956A for details), which can effectively degrade chlorophenol pollutants, but if the device is directly transferred to treatment of bisphenol A, the degradation efficiency is only 60% after 90min for 20ppm of bisphenol A under the optimal conditions (electrolyte pH 7.4 and voltage 2.0V) because bisphenol A has a more stable chemical structure; meanwhile, the dependence on hydrogen peroxide in the catalytic reaction process of peroxidase also limits the application of the system.
Laccase is a kind of multi-copper oxidase, which can catalyze the oxidation coupling reaction of low molecular organic matter and degrade high molecular organic matter to form small molecular compound in the presence of molecular oxygen. However, when laccase was directly applied to the catalytic degradation of 20ppm bisphenol A, the degradation efficiency after 90min was only 49% (see comparative example 2 below).
Disclosure of Invention
Aiming at the defects or improvement requirements of the prior art, the invention aims to provide a device and a method for degrading bisphenol A by laccase in cooperation with photoelectrocatalysis, wherein key reaction participants and corresponding reaction mechanisms are improved, the degradation efficiency of bisphenol A can be improved compared with the prior art, and rapid conversion and removal of pollutants can be realized by constructing an enzyme-linked photoelectrocatalysis sewage treatment device by coupling laccase catalytic degradation reaction with semiconductor photoelectrocatalysis.
To achieve the above object, according to one aspect of the present invention, there is provided a method for degrading bisphenol a by laccase in cooperation with photoelectrocatalysis, comprising the steps of:
(1) Preparing a to-be-treated polluted solution containing bisphenol A into an electrolyte, wherein the obtained electrolyte correspondingly contains the bisphenol A; simultaneously, preparing a photoelectrode and a counter electrode; wherein the electrolyte and/or the counter electrode further comprise a laccase component;
(2) Inserting the photoelectrode and the counter electrode into the electrolyte, and then applying bias voltage to the photoelectrode and the counter electrode to enable the voltage of the photoelectrode to be higher than that of the counter electrode; simultaneously applying light to the photoelectrode; laccase in the system can induce bisphenol A to be oxidized and polymerized, and meanwhile, the photoelectrode can generate active free radicals with strong oxidizing property under the illumination condition and bias voltage, so that enzyme-linked photoelectrochemical degradation of bisphenol A is realized.
In a further preferred embodiment of the present invention, in the step (2), the bias voltage is 0.8V to 1.4V.
In a more preferred aspect of the present invention, the electrolyte solution obtained in the step (1) has a pH of 3 to 6.
According to another aspect of the invention, the invention provides a device for degrading bisphenol A by laccase in cooperation with photoelectrocatalysis, which is characterized by comprising an electrolyte, a photoelectrode and a counter electrode, wherein the photoelectrode and the counter electrode are positioned in the electrolyte,
the electrolyte is an electrolyte solution containing bisphenol A;
the photoelectrode is used for generating active free radicals under the action of illumination;
the photoelectrode and the counter electrode are used for being connected with a power supply to form a current loop, so that the effective separation of the hole-electron pairs generated by the photoelectrode is promoted;
and the electrolyte and/or the counter electrode further comprise a laccase component.
As a further preference of the invention, the laccase is supported on the surface of the counter electrode.
As a further preference of the invention, the laccase is free in the electrolyte.
As a further preferable aspect of the present invention, the photoelectrode includes a photoelectric active material layer and a conductive substrate supporting the photoelectric active material layer, and the photoelectric active material layer contains at least one of bismuth vanadate, tungsten trioxide, ferric oxide, titanium dioxide, and zinc oxide;
preferably, the conductive substrate is one of a conductive glass electrode, a platinum sheet electrode, a glassy carbon electrode, a graphite electrode and a carbon cloth electrode.
As a further preferred aspect of the present invention, the counter electrode is a conductive substrate, specifically, one of a conductive glass electrode, a platinum sheet electrode, a glassy carbon electrode, a graphite electrode, and a carbon cloth electrode.
As a further preferred aspect of the present invention, the power supply is a potentiostat or a regulated dc power supply.
As a further preference of the present invention, the illumination is provided by a light source having a light intensity of 20-1000mW/cm 2 The light source is one of a xenon lamp, a tungsten lamp and an LED lamp.
Through the technical scheme, compared with the prior art, photoelectrochemistry and laccase catalytic degradation reaction are coupled, and active free radicals generated by cooperation of photoelectrocatalysis and enzyme catalysis processes are utilized to degrade the environmental pollutant bisphenol A. The laccase fixed on the surface of the counter electrode or the laccase dissociated in the electrolyte solution can catalyze the oxidative degradation of the oxygen to the bisphenol A (no oxidant such as hydrogen peroxide is additionally added into the system, and the reaction condition is mild); meanwhile, photo-generated electrons and holes generated by the photoelectrode under illumination can be effectively separated under the action of an external electric field, and the holes and the electrons react with water molecules, dissolved oxygen and the like in electrolyte to generate active species with strong oxidizing property, such as hydroxyl free radicals, superoxide free radicals and the like, so that bisphenol A and enzyme catalysis products thereof are further converted and degraded.
As is well known, laccase is polyphenol oxidase containing four copper ions, and can catalyze the oxidative coupling reaction of low-molecular organic matters and degrade high-molecular organic matters to form small-molecular compounds in the presence of molecular oxygen. The source of the extract can be at least one of Coriolus versicolor, rhus verniciflua and Agaricus bisporus. The invention preferably controls the pH value of the electrolyte to be 3-6, and can provide a more suitable reaction environment for the catalytic degradation of laccase.
Specifically, the invention can achieve the following beneficial effects:
(1) The invention couples the semiconductor photoelectrocatalysis and the biological laccase catalytic degradation process to form an enzyme-linked photoelectricity system for degrading the bisphenol A, wherein, the photoelectrode can generate active oxygen species such as hydroxyl free radicals, superoxide free radicals and the like with strong oxidizing property under illumination (such as visible light irradiation) to oxidize and degrade the pollutant bisphenol A; meanwhile, laccase can also catalyze the oxidative degradation of bisphenol A in the presence of dissolved oxygen.
(2) According to the invention, the laccase is combined with the photoelectrocatalysis to degrade the pollutant bisphenol A, and the advantages of thorough degradation reaction, high oxidation activity, mild biological laccase catalysis reaction condition, high efficiency and the like of the photoelectrocatalysis reaction can be synergistically utilized, so that the degradation efficiency of the bisphenol A is effectively improved. Taking the following embodiment as an example, the highest removal rate of 20ppm of bisphenol A in the water body within 90min can reach 93% based on the method disclosed by the invention, so that the bisphenol A can be rapidly removed, and the effect of degrading the pollutant bisphenol A by single photoelectrocatalysis or laccase catalysis is obviously better.
(3) In addition, the invention can effectively reduce the operation cost of a pollutant degradation system. The photo-anode loaded with the photoactive material or the cathode loaded with the laccase can realize the recycling of a photo-electrode and a bio-enzyme electrode when being used for pollutant degradation, and is beneficial to reducing the running cost of an enzyme-linked photo-catalytic degradation system.
In conclusion, the invention can comprehensively utilize the synergistic advantages of photoelectrocatalysis and enzyme catalysis, and can realize the rapid conversion and removal of bisphenol A.
Drawings
FIG. 1 is a schematic structural diagram of a device for treating pollutant bisphenol A by laccase in cooperation with photoelectrocatalysis.
Fig. 2 is a structure diagram of a micro-area of a bismuth vanadate photo-anode prepared in application example 1.
FIG. 3 is a graph showing the concentration change of the process for degrading contaminant bisphenol A in application example 1, comparative example 1 and comparative example 2; in this case, the application example 1 corresponds to the legend "1 free laccase coupled to photoelectrocatalysis", the comparative example 1 corresponds to the legend "2 photoelectrocatalysis", and the comparative example 2 corresponds to the legend "3 free laccase".
FIG. 4 is a graph showing the change in concentration of bisphenol A as a contaminant in application example 2 and comparative example 3; in this case, the application example 2 corresponds to the legend "1 immobilized laccase coupled with photoelectrocatalysis" and the comparative example 3 corresponds to the legend "2 immobilized laccase".
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is described in further detail below with reference to the accompanying drawings and embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention. In addition, the technical features involved in the embodiments of the present invention described below may be combined with each other as long as they do not conflict with each other.
In general, the device for degrading bisphenol A by laccase in cooperation with photoelectrocatalysis based on the invention can be shown in FIG. 1 and comprises:
photoelectrode (such as semiconductor photoelectrode) for generating active free radical to degrade bisphenol A under the action of illumination;
the counter electrode is connected with the semiconductor photoelectrode through a power supply and is used for forming an electrode loop;
the electrolyte solution contains bisphenol A and is used for providing a reaction environment suitable for laccase catalytic degradation; the electrolyte is prepared by adopting bisphenol A pollutants, and if a solution system obtained by direct preparation cannot meet the conductivity requirement of the electrolyte, a supporting electrolyte can be additionally added to improve the conductivity;
an electrochemical cell for loading a semiconductor photoelectrode, a counter electrode and an electrolyte;
the power supply is used for driving the carriers generated by the semiconductor photoelectrode to flow to the counter electrode;
a light source for providing illumination.
Taking the example of using a semiconductor photoelectrode as the photoelectrode, correspondingly, the actual operation process may include the following steps:
(1) Preparing a semiconductor photoelectrode and a counter electrode, connecting the semiconductor photoelectrode with the positive pole of a power supply, connecting the counter electrode with the negative pole of the power supply, and placing the counter electrode in an electrolytic cell;
(2) And adding an electrolyte containing bisphenol A into the electrolytic cell, turning on a light source and a power supply to enable the semiconductor photoelectrode to be irradiated by the light source, and applying bias voltage between the semiconductor photoelectrode and the counter electrode to realize enzyme-linked photoelectrochemical degradation of the bisphenol A.
The application example is as follows:
application example 1
The application embodiment mainly relates to application of degrading 20ppm of bisphenol A by adopting an enzyme-linked photoelectrocatalysis system constructed by free laccase and a bismuth vanadate photoanode.
(1) Preparing a bismuth vanadate photoelectrode: adding 20mmol of pentahydrate bismuth nitrate into 50mL of solution (pH is adjusted to 1.7-1.8) containing 0.2mol of potassium iodide, then adding 20mL of ethanol solution containing 46mmol of p-benzoquinone, and uniformly mixing to obtain the electrolyte. Electrodeposition was carried out under a three-electrode system: the working electrode is an FTO electrode (20mm-20mm), the reference electrode is a saturated calomel electrode, the counter electrode is a platinum sheet, and the deposition is carried out for 300s at a constant potential of-0.1V to obtain a bismuth oxyiodide electrode; 0.15mL of 0.2M dimethylsulfoxide solution of vanadyl acetylacetonate is dripped on the surface of the bismuth oxyiodide electrode, and the bismuth oxyiodide electrode is heated to 450 ℃ (the heating rate is 2 ℃/min) in a high-temperature resistance furnace and maintained for 2 hours. After cooling to room temperature, the obtained electrode was immersed in 1M sodium hydroxide solution and slowly shaken to remove excess vanadium pentoxide. Then washing with pure water and drying in the air to obtain the bismuth vanadate photo-anode. The structure of the micro-area is shown in figure 2.
(2) Free laccase is combined with photoelectrocatalysis and is used for degrading pollutant bisphenol A: a bismuth vanadate photoanode is used as a working electrode, a saturated calomel electrode is used as a reference electrode, a platinum wire electrode is used as a counter electrode, a three-electrode system is formed and placed in an electrolytic cell, and 50mL of 0.1mol/L sodium sulfate solution containing 20ppm of bisphenol A is used as electrolyte (the pH value is adjusted to be 5.0). The light source is a xenon lamp light source provided with an artificial sunlight (AM1.5G) filter, and the light intensity is 200mW/cm 2 . Turning on a light source, adding laccase with a concentration of 10 μ g/mL into the electrolyte, applying a bias voltage of 1.2V by using an electrochemical workstation, and recording the degradation efficiency of bisphenol A at different times (the change of the concentration of bisphenol A is monitored by high performance liquid chromatography, the same below).
Analysis of the curve corresponding to legend "1 free laccase coupled with photoelectrocatalysis" in FIG. 3 shows that for 20ppm bisphenol A, the degradation efficiency after 90min can reach 93%.
Application example 2
The application embodiment mainly relates to application of degrading 20ppm of bisphenol A by adopting an enzyme-linked photoelectrocatalysis system constructed by adopting a bismuth vanadate photoanode and a laccase modified carbon cloth cathode.
(1) The preparation process of the bismuth vanadate photo-anode is the same as that of application example 1.
(2) Preparing a laccase-modified carbon cloth cathode: the area is 4cm 2 The carbon cloth is respectively cleaned by ultrasonic in acetone, ethanol and ultrapure water to remove organic matters and inorganic matters attached to the surface, and is dried in the air for later use. And dripping 200 mu L of a mixed solution of 20-percent PVP and 500 mu L of 1mg/mL laccase on the cleaned carbon cloth, shaking and incubating for 24h in an incubator at 4 ℃, then washing with ultrapure water to remove tightly bound laccase molecules, and placing in a dark place at 4 ℃ for later use.
(3) Immobilized laccase in combination with photoelectrocatalysis is used for degrading pollutant bisphenol A: a bismuth vanadate photoanode is used as a working electrode, a saturated calomel electrode is used as a reference electrode, a carbon cloth electrode fixed with laccase is used as a counter electrode to form a three-electrode system, the three-electrode system is placed in an electrolytic cell, and 50mL of 0.1mol/L sodium sulfate solution containing 20ppm of bisphenol A (the pH value is adjusted to be 5.0). The light source is a xenon lamp light source provided with an artificial sunlight (AM1.5G) filter, and the light intensity is 200mW/cm 2 . The light source was turned on and a 1.2V bias was applied using the electrochemical workstation and the efficiency of degradation of bisphenol A was recorded at different times.
Analysis of the curve corresponding to the legend "immobilized laccase in combination with photoelectrocatalysis" in FIG. 4 shows that for 20ppm bisphenol A, the degradation efficiency after 90min can reach 83%.
Application example 3
The application embodiment mainly relates to application of an enzyme-linked photoelectrocatalysis system constructed by adopting free laccase and a bismuth vanadate photoanode to degrade 20ppm bisphenol A under different external bias voltages.
The procedure was similar to application example 1, except that a different potential was applied to the bismuth vanadate electrode. The results showed that for 20ppm of bisphenol A, the degradation efficiencies reached 65%,75% and 74% after 90min at applied potentials of 0.8V,1.0V and 1.4V, respectively.
Application example 4
The application embodiment mainly relates to application of an enzyme-linked photoelectrocatalysis system constructed by adopting free laccase and a bismuth vanadate photoanode to degradation of bisphenol A with the concentration of 20ppm under different initial pH values.
The procedure was similar to application example 1, except that the bisphenol A-containing solution was adjusted to a different pH before degradation. The results show that for 20ppm bisphenol A, the degradation efficiency after 90min can reach 51%,75% and 76%, respectively, at an initial pH of 3,4 and 6.
Comparative example 1
The comparative example mainly relates to the application of an enzyme-free photoelectrocatalysis system constructed by adopting a bismuth vanadate photoanode to degrade 20ppm of bisphenol A.
The process is the same as that of application example 1, and is different from application example 1 in that: the electrolyte used for the degradation test does not contain laccase. The method has the degradation efficiency of 48 percent after 90min for 20ppm of bisphenol A.
Comparative example 2
This comparative example relates generally to the use of a free enzyme catalyzed system to degrade 20ppm bisphenol A.
The process is the same as that of application example 1, and is different from application example 1 in that: no light and three-electrode system. Because the device only depends on the catalytic oxidation activity of free laccase, the degradation efficiency of the method is 49% after 90min for 20ppm of bisphenol A.
Comparative example 3
This comparative example mainly relates to the use of an immobilized laccase catalytic system for the degradation of 20ppm of bisphenol A.
The process is the same as that of application example 2, and is different from application example 2 in that: no light and no voltage are applied. Since this device relies only on the catalytic oxidation activity of laccase immobilized on the electrodes, the method has a degradation efficiency of 62% after 90min for 20ppm bisphenol A.
The results show that for solutions containing 20ppm of bisphenol A, 93% and 83% degradation efficiency can be achieved by combining photoelectrocatalysis with free laccase (application example 1) or immobilized laccase (application example 2), respectively, and the degradation efficiency is obviously superior to that of photoelectrocatalysis (comparative example 1), free laccase catalysis (comparative example 2) or immobilized laccase catalysis (comparative example 3) alone. This is mainly benefited by the fact that laccase can catalyze the oxidative degradation of the contaminant bisphenol A by oxygen, and bisphenol A and its degradation products can be further oxidized by active free radicals generated by the photoelectrode. Therefore, the rapid conversion and removal of the pollutant bisphenol A can be realized by synergistically utilizing the advantages of mild enzyme catalysis reaction conditions, high efficiency, high oxidation activity of the photoelectrocatalysis reaction, thorough degradation reaction and the like.
In addition, the laccase used in the above application examples and comparative examples is derived from Coriolus versicolor. In the invention, besides the carbon cloth electrode can be used as a conductive substrate for fixing the laccase, a graphite electrode, a metal electrode and the like can be used as the conductive substrate; the laccase used in the invention can be derived from coriolus versicolor, lacquer tree, agaricus bisporus and the like; besides the bismuth vanadate photoelectrode, the photoanode in the invention can also adopt photoanodes such as bismuth vanadate/ferric oxide, bismuth vanadate/tungsten trioxide, titanium dioxide/bismuth vanadate and the like.
It will be understood by those skilled in the art that the foregoing is only a preferred embodiment of the present invention, and is not intended to limit the invention, and that any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the scope of the present invention.
Claims (10)
1. A method for degrading bisphenol A by laccase in cooperation with photoelectrocatalysis is characterized by comprising the following steps:
(1) Preparing a to-be-treated polluted solution containing bisphenol A into an electrolyte, wherein the obtained electrolyte correspondingly contains the bisphenol A; simultaneously, preparing a photoelectrode and a counter electrode; wherein the electrolyte and/or the counter electrode further comprise a laccase component;
(2) Inserting a photoelectrode and a counter electrode into the electrolyte, and then applying bias voltage to the photoelectrode and the counter electrode to enable the voltage of the photoelectrode to be higher than that of the counter electrode; simultaneously applying light to the photoelectrode; laccase in the system can induce bisphenol A to be oxidized and polymerized, and meanwhile, the photoelectrode can generate active free radicals with strong oxidizing property under the illumination condition and bias voltage, so that enzyme-linked photoelectrochemical degradation of bisphenol A is realized.
2. The method for the concerted photoelectrocatalytic degradation of bisphenol A of claim 1, wherein in step (2), the bias voltage is 0.8V-1.4V.
3. The method for the synergistic photoelectrocatalytic degradation of bisphenol A with laccase as claimed in claim 1, wherein the pH value of the electrolyte obtained in step (1) is 3-6.
4. The device for degrading bisphenol A by laccase collaborative photoelectrocatalysis is characterized by comprising electrolyte, a photoelectrode and a counter electrode, wherein the photoelectrode and the counter electrode are positioned in the electrolyte,
the electrolyte is an electrolyte solution containing bisphenol A;
the photoelectrode is used for generating active free radicals under the action of illumination;
the photoelectrode and the counter electrode are used for being connected with a power supply to form a current loop, so that the effective separation of the hole-electron pairs generated by the photoelectrode is promoted;
and the electrolyte and/or the counter electrode further comprise a laccase component.
5. The device for the concerted photoelectrocatalytic degradation of bisphenol A of claim 4, wherein the laccase is supported on the surface of the counter electrode.
6. The device for the photoelectrocatalytic degradation of bisphenol a in cooperation with the laccase of claim 4, wherein the laccase is free in the electrolyte.
7. The device for degrading bisphenol A with the laccase collaborative photoelectrocatalysis as claimed in claim 4, wherein the photoelectrode comprises a photoelectric active material layer and a conductive substrate for supporting the photoelectric active material layer, and the photoelectric active material layer contains at least one of bismuth vanadate, tungsten trioxide, ferric oxide, titanium dioxide and zinc oxide;
preferably, the conductive substrate is one of a conductive glass electrode, a platinum sheet electrode, a glassy carbon electrode, a graphite electrode and a carbon cloth electrode.
8. The device for degrading bisphenol A through laccase collaborative photoelectrocatalysis as claimed in claim 4, wherein the counter electrode is a conductive substrate, and is specifically one of a conductive glass electrode, a platinum sheet electrode, a glassy carbon electrode, a graphite electrode and a carbon cloth electrode.
9. The device for degrading bisphenol A by laccase collaborative photoelectrocatalysis according to claim 4, wherein the power supply is a potentiostat or a regulated DC power supply.
10. The laccase device for degrading bisphenol A with photoelectrocatalysis as claimed in claim 4, wherein the light is provided by a light source with intensity of 20-1000mW/cm 2 The light source is one of a xenon lamp, a tungsten lamp and an LED lamp.
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