CN115448428B - Electrochemical dehalogenation electrode for organic halogenated pollutants and preparation method and application thereof - Google Patents
Electrochemical dehalogenation electrode for organic halogenated pollutants and preparation method and application thereof Download PDFInfo
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- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
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- C02F1/467—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction
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Abstract
The invention relates to an electrochemical high-efficiency dehalogenation electrode for organic halogenated pollutants, a preparation method and application thereof. Compared with the prior art, the foam titanium-based cobalt monoatomic material can effectively avoid competitive adsorption of water molecules and halides on catalytic sites in the dehalogenation process by separating an H source supply center and dehalogenation active sites in the reduction process, so that excellent electrochemical selective dehalogenation performance is shown.
Description
Technical Field
The invention relates to the technical field of electrochemistry, in particular to an electrochemical dehalogenation electrode for organic halogenated pollutants, and a preparation method and application thereof.
Background
With the development of biomedical and environmental monitoring technologies, halogenated organic pollution represented by perfluoro compounds and polychlorinated biphenyls has received more and more attention. Electrochemical reduction technology is a high-efficiency and high-selectivity halogenated organic matter treatment means, which can greatly weaken the biotoxicity and environmental durability of halogenated organic matters through reduction hydrodehalogenation, thereby treating halogenated organic pollution from the source. Current research on electrochemical reduction dehalogenation has been mainly conducted around noble metal materials such as palladium, platinum, silver, and the like. In the reductive dehalogenation process, the traditional noble metal-based catalyst is not only an adsorption site for halogen-containing pollutants, but also takes charge of activating water molecules to generate atoms H, so that the dehalogenation performance of the single-active-site material is limited.
Disclosure of Invention
The invention aims to provide an electrochemical dehalogenation electrode for organic halogenated pollutants, a preparation method and application thereof, and the dehalogenation performance is improved.
The invention can be aimed at by the following technical proposalTo realize: an electrochemical dehalogenation electrode of organic halogenated pollutant is a foamed titanium-based cobalt monoatomic electrode (Co for short) 1 -Ti), titanium foam is used as a carrier, on which monoatomic cobalt is supported.
Competitive adsorption of halogen-containing contaminants and water molecules at the active site greatly limits the dehalogenation performance of single-active site materials. The electrode of the invention spatially separates the foam titanium carrier of the H source supply center and the monoatomic cobalt of the dehalogenation center, and the design of the double active sites avoids the competitive adsorption of water molecules and halogenated matters on the catalytic sites in the dehalogenation process, thereby showing excellent electrochemical selective dehalogenation performance and providing a high-efficiency green approach for the treatment of halogenated organic wastewater.
Preferably, the mass of the monoatomic cobalt accounts for 0.05 to 0.5 percent of the total mass of the electrode.
Preferably, the area of the foam titanium is 4-16 cm 2 The thickness is 0.5-2 mm.
The preparation method of the electrochemical efficient dehalogenation electrode for the organic halogenated pollutants comprises the steps of uniformly spraying a cobalt nitrate solution on the surface of a foam titanium carrier, naturally airing, placing the sprayed foam titanium in a tubular furnace, and carrying out high-temperature treatment (calcination) under a hydrogen/argon mixed atmosphere to obtain the foam titanium-based cobalt monoatomic electrode.
Preferably, the high temperature treatment temperature is 250-350 ℃.
Further preferably, the high temperature treatment temperature is 300 ℃.
The electrochemical efficient dehalogenation electrode for organic halogenated pollutant is used in electrochemical reduction dehalogenation reaction.
Preferably, an H-type electrolytic cell is used, and the electrode is used as a working electrode to carry out electrochemical reduction dehalogenation on the organic halogenide.
Further preferably, the working electrode and the reference electrode are arranged in the cathode chamber, the counter electrode is arranged in the anode chamber, the reference electrode is any one of a mercury-mercury oxide electrode, a silver-silver chloride electrode, a saturated calomel electrode and a mercury-mercurous sulfate electrode, and the counter electrode is any one of a platinum sheet electrode and a ruthenium iridium titanium electrode.
Further preferably, in the electrolytic cell, the electrolyte solution is a buffer solution prepared from sodium dihydrogen phosphate and potassium dihydrogen phosphate, and the ph=5 to 9.
Still more preferably, the pH of the electrolyte solution is=7.
Preferably, in the electrochemical reduction dehalogenation reaction, the reaction voltage is-1.2 to-0.5V, and the reaction time is 2 to 4 hours.
Compared with the prior art, the invention has the following advantages:
1. the foamed titanium-based cobalt single-atom electrode material has simple preparation process and low cost, has excellent reduction dehalogenation capability on various halogen-containing pollutants, and in addition, the material has good cyclic dehalogenation stability, and can reduce halogenated organic pollutants in a wide pH range and various interference ion environments with high efficiency, so that the foamed titanium-based cobalt single-atom electrode has good practical application prospect;
2. according to the invention, a simple synthesis method is adopted, titanium foam is used as a metal substrate, oxygen vacancies of an amorphous layer on the surface of the titanium foam are utilized to anchor cobalt atoms, wherein the cobalt monoatoms are uniformly distributed, the dispersibility is good, the operation is simple, the reaction conditions are simple and controllable, the cost is low, and the mass production of the electrode is facilitated;
3. the foam titanium carrier of the invention has excellent hydrolytic capability, provides sufficient hydrogen source for the reductive dehalogenation of the halogenate, takes single-atom cobalt as dehalogenation active center, realizes the rapid dehalogenation of the halogenate, and based on the advantages, co 1 The Ti electrode can realize 99.9 percent degradation and 99.9 percent dechlorination of chloramphenicol within 3 hours; at the same time Co 1 Ti electrodes have a broad pH working range (ph=5-9), dehalogenation performance is not affected by PO in solution 4 3- 、NH 4 + 、SO 4 2- 、NO 3 - Influence of plasma; general applicability, co 1 Ti electrodes exhibit outstanding dechlorination effects against other typical halogen-containing contaminants such as florfenicol, thiamphenicol, 4-chlorophenol, etc.; in addition, co 1 The dechlorination activity of the Ti electrode is hardly attenuated in the cyclic test lasting for 48 hoursReduced, exhibiting excellent catalytic stability;
4. the foam titanium carrier is taken as a supply center of a hydrogen source, participates in a reduction dehalogenation process, and transmits H to cobalt monoatoms through a hydrogen overflow mode in a reduction dehalogenation reaction, so that dehalogenation reaction is promoted, and the invention firstly provides application of hydrogen overflow in the field of electrochemical reduction degradation of pollutants;
5. the electrode preparation method is simple, only needs two steps of spraying and calcining, consumes short time, can finish the preparation of the electrode only by 6 hours, and is beneficial to the mass production of the electrode;
6. the invention has less consumption of electric energy in the electrolysis process, and can effectively reduce the treatment cost of sewage;
7. the cobalt of the invention is dispersed on the surface of the foam titanium substrate in the form of single atoms, and compared with a nano catalyst, the single-atom catalyst has higher atom utilization efficiency and reaction selectivity, has high activity and high stability, and can avoid side reactions.
Drawings
FIG. 1 is Co obtained in example 1 of the present invention 1 Spherical aberration correcting transmission electron microscopy of Ti electrode. The circled bright spots are Co monoatoms.
FIG. 2 is Co obtained in example 1 of the present invention 1 Two-dimensional elemental image (EDS mapping) of the Ti electrode cobalt element, demonstrating that the cobalt monoatoms are uniformly distributed on the titanium foam substrate.
FIG. 3 is an electrochemical EPR spectrum of an electrode obtained in example 2 of the present invention, co 1 Ti and Ti have similar hydrogen radical signals, and the titanium foam substrate has good water dissociation capability; when the CAP concentration reached 500ppm, the hydrogen radical signal disappeared, proving that the hydrogen radical participated in the electrochemical reduction of CAP.
FIG. 4 is a graph showing the degradation performance of Chloramphenicol (CAP) by the electrode material obtained in example 3 of the present invention: reacting for 3 hours, co 1 Ti electrodes are able to degrade 99.9% of CAP, while titanium foam electrodes only degrade 63.8% of CAP.
FIG. 5 is a graph showing the effect of the electrode material obtained in example 3 of the present invention on CAPRaw dehalogenation Performance graph: reacting for 3 hours, co 1 The Ti electrode has a dechlorination rate of 99% to CAP, whereas the titanium foam electrode does not have dechlorination capability.
FIG. 6 is Co obtained in example 4 of the present invention 1 Degradation performance profile of Ti electrode for CAP at different pH conditions: co (Co) 1 The degradation rate of the Ti electrode material in the pH=5-9 can reach 99% in 2 hours.
FIG. 7 is Co obtained in example 4 of the present invention 1 -Ti electrode reductive dehalogenation performance profile for CAP at different pH conditions: reacting for 3 hours, co 1 The CAP dechlorination ratio of the Ti electrode can reach more than 95% under the conditions of pH=5 and 7, and the CAP dechlorination ratio can reach more than 80% under the conditions of pH=9. The results illustrate Co 1 Ti electrodes have a wide pH working range.
FIG. 8 is Co obtained in example 5 of the present invention 1 Degradation performance profile of Ti electrode on halogenated organic pollutants such as Florfenicol (FLO), thiamphenicol (TAP), 4-chlorophenol (4-CP): the degradation rate of 4-CP reaches 99% after 1 hour of reaction; the degradation rate of FLO and TAP reaches 99% after 3 hours of reaction.
FIG. 9 is Co obtained in example 5 of the present invention 1 Reduction dehalogenation performance profile of Ti electrode versus FLO, TAP, 4-CP: the dechlorination ratio of 4-CP reaches 99% after 1 hour of reaction; the FLO dechlorination ratio reaches 98% after 2 hours of reaction; the dechlorination rate of TAP reaches 99% after 3 hours of reaction. End description Co 1 Ti electrodes are versatile for the reductive dehalogenation of halogen-containing contaminants.
FIG. 10 is Co obtained in example 6 of the present invention 1 Degradation performance profile of Ti electrode for CAP under different electrolyte conditions: after 3 hours of reaction, the degradation rate of CAP in various electrolyte solutions reaches 99 percent.
FIG. 11 is Co obtained in example 6 of the present invention 1 Reduction dehalogenation performance profile of Ti electrode for CAP under different electrolyte conditions: the reaction is carried out for 3 hours, and the dechlorination ratio of CAP in various electrolyte solutions is more than 95 percent. This demonstrates Co 1 Ti electrode in various coexisting ions (PO 4 3- 、NH 4 + 、SO 4 2- 、NO 3 - ) Can be effectively used in the environment of (1)The reduction dehalogenation of halogen-containing pollutants is realized.
FIG. 12 is Co obtained in example 7 of the present invention 1 -Ti electrode to CAP reductive dehalogenation stability test. The activity of the material is not obviously attenuated in the reaction process of 48 hours (16 rounds), the degradation rate of CAP is maintained above 99.9%, and the dechlorination ratio is maintained above 90%. The results demonstrate that the foamed titanium-based cobalt monoatomic electrode (Co 1 Ti) has good stability to reductive dehalogenation.
Detailed Description
The invention will now be described in detail with reference to the drawings and specific examples. The following examples are given by way of illustration of detailed embodiments and specific procedures based on the technical scheme of the present invention, but the scope of the present invention is not limited to the following examples.
Example 1
(1) Foam titanium-based cobalt monoatomic electrode (Co) 1 -Ti) preparation method:
first, a cobalt nitrate ethanol solution of 6.25mg/mL was prepared. 1125. Mu.L of cobalt nitrate ethanol solution was uniformly sprayed on titanium foam (9 cm in area) 2 Thickness of 0.68 mm). Then, the sprayed foam titanium is placed in a porcelain boat, the porcelain boat is placed in a tube furnace, hydrogen/argon mixed gas is introduced to remove air, and the foam titanium-based cobalt monoatomic electrode (Co) is prepared by high-temperature treatment for 3 hours at 300 ℃ under the hydrogen/argon mixed gas atmosphere 1 -Ti)。
(2) Characterization of materials:
for the foamed titanium-based cobalt monoatomic electrode (Co) obtained in example 1 1 -Ti) performing spherical aberration correcting transmission electron microscopy characterization and two-dimensional elemental image (EDS mapping) characterization of cobalt element. The characterization result shows that the monoatomic material is successfully synthesized by the method, and the cobalt monoatoms are uniformly dispersed on the surface of the foam titanium.
Example 2
(1) Foam titanium-based cobalt monoatomic electrode (Co) 1 -Ti) preparation method:
as in example 1.
(2) Electrochemical EPR test was performed on the electrode prepared in example 1:
measurement with DMPO as Capture agentThe hydrogen radicals generated during the reaction were tested. Reaction conditions: CAP was initially at a concentration of 0 or 500mg/L, and was applied to a titanium-based cobalt monoatomic electrode (Co 1 -Ti) or a titanium foam electrode (Ti) as cathode, a platinum sheet electrode as counter electrode, a mercury oxide electrode as reference electrode, for 5 minutes. Co in a solution with initial CAP concentration of 0 1 Obvious H.signal is detected around Ti and Ti electrodes, proving Co 1 Ti and Ti electrodes have similar H.generating capacity. When the CAP concentration increased to 500ppm, the H signal disappeared, proving that H involved in CAP reduction reaction.
Example 3:
(1) Foam titanium-based cobalt monoatomic electrode (Co) 1 -Ti) preparation method:
as in example 1.
(2) The electrode prepared in example 1 was evaluated for catalytic activity:
the electrochemical reduction dechlorination performance was tested using Chloramphenicol (CAP) as a model contaminant. Reaction conditions: the electrolyte used was 0.067mol/L phosphate buffer solution (pH=7), and the initial concentration of CAP was 50mg/L. 40mL of electrolyte is respectively added into the cathode chamber and the anode chamber of the H-type electrolytic cell, so that a titanium-based cobalt monoatomic electrode (Co) 1 -Ti) or a foam titanium electrode (Ti) as a cathode, a platinum sheet electrode as a counter electrode, and a mercury-oxidized mercury electrode as a reference electrode, for 3 hours under the condition of a potential of-1.0V. At the end of the reaction, a titanium-based cobalt foam monoatomic electrode (Co 1 -Ti) is able to degrade 99.9% of CAP, and the dechlorination ratio can reach 99%; while titanium foam electrodes (Ti) only degrade 63.8% of CAP with little dechlorination.
Example 4:
(1) Foam titanium-based cobalt monoatomic electrode (Co) 1 -Ti) preparation method:
as in example 1.
(2) The electrode prepared in example 1 was subjected to activity evaluation under different pH conditions:
the pH of the electrolyte was adjusted to 5,7, 9 by controlling the phosphate ratio, and the rest of the experimental conditions were the same as in example 2. Foam titanium-based cobalt monoatomic electrode (Co) 1 -Ti) material in the ph=5-9 range, 2 smallThe degradation rate of CAP can reach 99 percent. The CAP dechlorination ratio can reach more than 95% under the conditions of pH=5 and 7, and can reach more than 80% under the conditions of pH=9. This demonstrates that the foamed titanium-based cobalt monoatomic electrode (Co 1 Ti) has a broad pH working range.
Example 5:
(1) Foam titanium-based cobalt monoatomic electrode (Co) 1 -Ti) preparation method:
as in example 1.
(2) The electrode prepared in example 1 was evaluated for dehalogenation activity of various halogen-containing organic contaminants:
CAP was changed to the same initial concentration of Florfenicol (FLO), thiamphenicol (TAP) or 4-chlorophenol (4-CP) and the rest of the experimental conditions were the same as in example 2. The degradation rate and the dechlorination ratio of 4-CP in 1 hour of reaction reach 99 percent; the degradation rate and dechlorination ratio of FLO and TAP reach 99% after 3 hours of reaction. This demonstrates that the foamed titanium-based cobalt monoatomic electrode (Co 1 Ti) has universality for reduction dehalogenation of halogen-containing organic pollutants, and can meet the treatment requirements of various halogen-containing organic wastewater.
Example 6:
(1) Foam titanium-based cobalt monoatomic electrode (Co) 1 -Ti) preparation method:
as in example 1.
(2) The electrode prepared in example 1 was subjected to activity evaluation under different electrolyte conditions:
conversion of phosphate to Na at the same mass concentration 2 SO 4 、(NH 4 ) 2 SO 4 、NaNO 3 The rest of the experimental conditions were the same as in example 2. After 3 hours of reaction, the degradation rate of CAP in various electrolyte solutions reaches 99 percent, and the dechlorination ratio reaches more than 95 percent. This demonstrates that the foamed titanium-based cobalt monoatomic electrode (Co 1 Ti) in various coexisting ions (PO) 4 3- 、NH 4 + 、SO 4 2- 、NO 3 - ) Can effectively realize the reduction dehalogenation of halogen-containing pollutants in the environment.
Example 7:
(1) Foam titanium-based cobalt monoatomic electrode (Co) 1 -Ti) preparation method:
as in example 1.
(2) Stability evaluation was performed on the electrode prepared in example 1:
for the same piece of foam titanium-based cobalt monoatomic electrode (Co 1 -Ti) a cyclic experiment was performed under the experimental conditions of example 2. Each reaction run was run for 3 hours, the electrolyte solution was changed after sampling and the next run was started for 48 hours (16 runs). The CAP degradation rate in the cycling experiment was maintained above 99.9% and the dechlorination rate was maintained above 90%, indicating Co 1 Ti has good reductive dehalogenation stability.
According to the invention, through separating the H source supply center and the dehalogenation active site in the reduction process, the foam titanium-based cobalt monoatomic material can effectively avoid competitive adsorption of water molecules and halogenated matters on the catalytic site in the dehalogenation process, so that excellent electrochemical selective dehalogenation performance is shown. The foam titanium-based cobalt monoatomic electrode has excellent reduction dehalogenation capability for various halogen-containing pollutants, good cyclic dehalogenation stability and high-efficiency and stable operation in a wide pH range and various interference ion environments. The preparation raw materials of the foam titanium-based cobalt monoatomic electrode are cheap, the process is simple, the enlarged production and the practical industrial application of the electrode are facilitated, and an efficient green approach is provided for the practical treatment of halogenated organic wastewater.
The previous description of the embodiments is provided to facilitate a person of ordinary skill in the art in order to make and use the present invention. It will be apparent to those skilled in the art that various modifications can be readily made to these embodiments and the generic principles described herein may be applied to other embodiments without the use of the inventive faculty. Therefore, the present invention is not limited to the above-described embodiments, and those skilled in the art, based on the present disclosure, should make improvements and modifications without departing from the scope of the present invention.
Claims (8)
1. The application of the electrochemical dehalogenation electrode of the organic halogenated pollutant is characterized in that the electrode is a foam titanium-based cobalt monoatomic electrode, and the foam titanium is used as a carrier to load monoatomic cobalt thereon;
the preparation method of the electrochemical dehalogenation electrode for the organic halogenated pollutants comprises the following steps: uniformly spraying a cobalt nitrate solution on the surface of a foam titanium carrier, naturally airing, and carrying out high-temperature treatment on the sprayed foam titanium in a hydrogen/argon mixed atmosphere to obtain a foam titanium-based cobalt monoatomic electrode;
the electrode is used for electrochemical reduction dehalogenation reaction.
2. The use of an electrochemical dehalogenation electrode of an organic halogenated contaminant according to claim 1, wherein the mass of monoatomic cobalt is between 0.05 and 0.5% of the total mass of the electrode.
3. The use of an electrochemical dehalogenation electrode of an organohalogenated contaminant according to claim 1, wherein the area of the titanium foam is from 4 to 16cm 2 The thickness is 0.5-2 mm.
4. The use of an electrochemical dehalogenation electrode for organic halogenated contaminants according to claim 1, wherein said high temperature treatment temperature is between 250 and 350 ℃.
5. The use of an electrochemical dehalogenation electrode for organic halogenated pollutants according to claim 1, characterized in that it uses an H-type electrolytic cell, said electrode being used as a working electrode for electrochemical reductive dehalogenation of organic halogenated compounds.
6. The electrochemical dehalogenation electrode for organic halogenated pollutants according to claim 5, wherein the working electrode and the reference electrode are placed in a cathode chamber, the counter electrode is placed in an anode chamber, the reference electrode is any one of a mercury-mercury oxide electrode, a silver-silver chloride electrode, a saturated calomel electrode and a mercury-mercurous sulfate electrode, and the counter electrode is any one of a platinum sheet electrode and a ruthenium iridium titanium electrode.
7. The electrochemical dehalogenation electrode for organic halogenated pollutants according to claim 5, characterized in that in the electrolytic cell, the electrolyte solution is a buffer solution prepared from sodium monohydrogen phosphate and potassium dihydrogen phosphate, and the ph=5-9.
8. The use of an electrochemical dehalogenation electrode for organic halogenated pollutants according to claim 1, wherein the electrochemical reduction dehalogenation reaction has a reaction voltage of-1.2 to-0.5V and a reaction time of 2 to 4 hours.
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| CN104947142A (en) * | 2015-05-29 | 2015-09-30 | 广西大学 | Preparation method of electrocatalytic reduction halogenated organic matter cathode material |
| CN110252347A (en) * | 2019-06-14 | 2019-09-20 | 清华-伯克利深圳学院筹备办公室 | A kind of monatomic material, and its preparation method and application |
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| US11103860B2 (en) * | 2018-03-08 | 2021-08-31 | Exxonmobil Chemical Patents Inc. | Catalyst systems comprising activator, polymerization processes using same, and products made therefrom |
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| CN104947142A (en) * | 2015-05-29 | 2015-09-30 | 广西大学 | Preparation method of electrocatalytic reduction halogenated organic matter cathode material |
| CN110252347A (en) * | 2019-06-14 | 2019-09-20 | 清华-伯克利深圳学院筹备办公室 | A kind of monatomic material, and its preparation method and application |
| CN110694690A (en) * | 2019-11-01 | 2020-01-17 | 苏州大学 | Method for preparing metal monatomic catalyst |
| CN114318403A (en) * | 2021-12-31 | 2022-04-12 | 上海大学 | Method for preparing platinum monoatomic material by adopting alkyl imidazole ionic liquid |
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| Single Atom Ru Monolithic Electrode for Efficient Chlorine Evolution and Nitrate Reduction;Yancai Yao;Angew. Chem. Int. Ed. * |
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