CN115448428A - Electrochemical efficient dehalogenation electrode for organic halogenated pollutants as well as preparation method and application of electrochemical efficient dehalogenation electrode - Google Patents
Electrochemical efficient dehalogenation electrode for organic halogenated pollutants as well as preparation method and application of electrochemical efficient dehalogenation electrode Download PDFInfo
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Abstract
The invention relates to an electrochemical high-efficiency dehalogenation electrode for organic halogenated pollutants, and a preparation method and application thereof. Compared with the prior art, the titanium foam-based cobalt monatomic material can effectively avoid competitive adsorption of water molecules and halides on the catalytic site in the dehalogenation process by separating the H source supply center and the dehalogenation active site in the reduction process, thereby showing excellent electrochemical selective dehalogenation performance.
Description
Technical Field
The invention relates to the technical field of electrochemistry, in particular to an organic halogenated pollutant electrochemical efficient dehalogenation electrode and a preparation method and application thereof.
Background
With the development of biomedical and environmental monitoring technologies, halogenated organic pollutants represented by perfluorinated compounds and polychlorinated biphenyls are receiving more and more attention. The electrochemical reduction technology is a high-efficiency and high-selectivity halogenated organic matter treatment means, and the biotoxicity and the environmental persistence of the halogenated organic matter can be greatly weakened through reduction, hydrogenation and dehalogenation, so that the halogenated organic pollution is treated from the source. At present, the research of electrochemical reduction dehalogenation mainly focuses on noble metal materials such as palladium, platinum, silver and the like. In the reduction dehalogenation process, the traditional noble metal-based catalyst is not only an adsorption site of halogen-containing pollutants, but also plays a role in activating water molecules to generate atoms H, and limits the dehalogenation performance of single-active-site materials.
Disclosure of Invention
The invention aims to provide an electrochemical high-efficiency dehalogenation electrode for organic halogenated pollutants, a preparation method and application thereof, and improve dehalogenation performance.
The purpose of the invention can be realized by the following technical scheme: an electrochemical high-efficiency dehalogenation electrode for organic halogenated pollutants is a foamed titanium-based cobalt monoatomic electrode (Co for short) 1 -Ti) supported on a titanium foam support, on which a monoatomic cobalt load is supported.
The 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 competitive adsorption of water molecules and halides on the catalytic sites in the dehalogenation process, thereby showing excellent electrochemical selective dehalogenation performance and providing an efficient green approach for treating 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 titanium foam is 4-16 cm 2 The thickness is 0.5-2 mm.
A preparation method of the electrochemical high-efficiency dehalogenation electrode for the organic halogenated pollutants comprises the steps of uniformly spraying a cobalt nitrate solution on the surface of a foamed titanium carrier, naturally drying in the air, placing the sprayed foamed titanium in a tube furnace, and carrying out high-temperature treatment (calcination) in a hydrogen/argon mixed atmosphere to obtain the foamed titanium-based cobalt monoatomic electrode.
Preferably, the high-temperature treatment temperature is 250-350 ℃.
Further preferably, the high-temperature treatment temperature is 300 ℃.
The application of the electrode for the electrochemical efficient dehalogenation of the organic halogenated pollutants is to use the electrode for electrochemical reduction dehalogenation reaction.
Preferably, an H-type electrolytic cell is adopted, and the electrode is used as a working electrode to perform electrochemical reduction dehalogenation on the organic halide.
Further preferably, the working electrode and the reference electrode are arranged in a cathode chamber, the counter electrode is arranged 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.
Further preferably, 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.
Still further preferably, the pH of the electrolyte solution =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 monoatomic electrode material has a simple preparation process and low cost, shows excellent reduction and dehalogenation capabilities for various halogen-containing pollutants, shows good cycle dehalogenation stability, and can efficiently reduce halogenated organic pollutants in a wide pH range and various interference ion environments, so that the foamed titanium-based cobalt monoatomic electrode has a good practical application prospect;
2. the invention adopts a simple synthesis method, takes the titanium foam as a metal substrate, and utilizes the oxygen vacancy of the amorphous layer on the surface of the metal substrate to anchor the cobalt atom, wherein, the cobalt monoatomic layer is uniformly distributed and has good dispersibility;
3. the foam titanium carrier has excellent water dissociation capability, provides sufficient hydrogen source for reduction dehalogenation of halogenated substances, takes the monatomic cobalt as the dehalogenation active center to realize rapid dehalogenation of the halogenated substances, and based on the advantages, co has high activity, high efficiency and high efficiency 1 The degradation of 99.9 percent of chloramphenicol and the dechlorination of 99.9 percent can be realized within 3 hours by a Ti electrode; at the same time, co 1 Ti electrodes have a wide pH working range (pH = 5-9), dehalogenation performance not affected by PO in solution 4 3- 、NH 4 + 、SO 4 2- 、NO 3 - The influence of plasma interference ions; general aspect of utility, co 1 Ti electrodes exhibit excellent dechlorination effects on other typical halogen-containing contaminants such as florfenicol, thiamphenicol, 4-chlorophenol, etc.; in addition, co 1 Ti electrodes show little decay in dechlorination activity in a cycling test lasting 48 hours, exhibiting excellent catalytic stability;
4. the foam titanium carrier is used as a supply center of a hydrogen source and participates in a reduction dehalogenation process, and in the reduction dehalogenation reaction, a foam titanium substrate transmits H to a cobalt monoatomic atom in a hydrogen overflow mode, so that the dehalogenation reaction is promoted to be carried out;
5. the preparation method of the electrode is simple, only two steps of spraying and calcining are needed, the time consumption is short, the preparation of the electrode can be completed in only 6 hours, and the large-scale production of the electrode is facilitated;
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 is dispersed on the surface of the foamed titanium substrate in a monatomic mode, and compared with a nano catalyst, the monatomic catalyst has higher atom utilization efficiency and reaction selectivity, and can avoid side reactions while having high activity and high stability.
Drawings
FIG. 1 shows Co obtained in example 1 of the present invention 1 -transmission electron microscopy images of spherical aberration corrected Ti electrodes. The circled bright spots are Co monoatomic.
FIG. 2 shows Co obtained in example 1 of the present invention 1 Two-dimensional elemental mapping (EDS mapping) of the Ti electrode cobalt element, demonstrating that the cobalt monoatomic species are uniformly distributed on the titanium foam substrate.
FIG. 3 is an electrochemical EPR spectrum, co, of the electrode obtained in example 2 of the present invention 1 Ti and Ti have similar hydrogen radical signals, which proves that the foamed titanium substrate has good water dissociation capability; when the CAP concentration reaches 500ppm, the hydrogen radical signal disappears, which proves that the hydrogen radical participates in the electrochemical reduction reaction of CAP.
FIG. 4 is a graph showing the degradation performance of the electrode material obtained in example 3 of the present invention on Chloramphenicol (CAP): reaction for 3 hours, co 1 Ti electrodes are able to degrade 99.9% of CAP, whereas titanium foam electrodes are only able to degrade 63.8% of CAP.
FIG. 5 is a graph showing the reductive dehalogenation activity of the electrode material against CAP obtained in example 3 of the present invention: reaction for 3 hours, co 1 The dechlorination ratio of the Ti electrode to the CAP reaches 99 percent, while the foam titanium electrode does not have dechlorination capability.
FIG. 6 shows Co obtained in example 4 of the present invention 1 Degradation performance of Ti electrodes at different pH conditions for CAP: co 1 The degradation rate of CAP in 2 hours can reach 99% in the range of pH = 5-9.
FIG. 7 shows Co obtained in example 4 of the present invention 1 -reductive dehalogenation performance of Ti electrodes at different pH for CAP: reaction for 3 hours, co 1 The CAP dechlorination proportion of the Ti electrode can reach more than 95% under the condition of pH =5,7, and the CAP dechlorination proportion can reach more than 80% under the condition of pH = 9. The results show that Co 1 Ti electrodes have a wide pH working range.
FIG. 8 shows Co obtained in example 5 of the present invention 1 A graph of degradation performance of Ti electrode on halogenated organic pollutants such as Florfenicol (FLO), thiamphenicol (TAP), 4-chlorophenol (4-CP) and the like: the degradation rate of 4-CP after 1 hour of reaction reaches 99 percent; the FLO and TAP degradation rate reaches 99% after reacting for 3 hours.
FIG. 9 shows Co obtained in example 5 of the present invention 1 Plot of reductive dehalogenation Performance of the Ti electrode pairs FLO, TAP, 4-CP: dechlorination ratio of 4-CP after 1 hour of reactionThe example reaches 99 percent; FLO dechlorination ratio reaches 98% after reacting for 2 hours; the TAP dechlorination proportion reached 99% after the reaction for 3 hours. End description of Co 1 Ti electrodes have general applicability to the reductive dehalogenation of halogen-containing contaminants.
FIG. 10 shows Co obtained in example 6 of the present invention 1 Degradation performance of Ti electrodes on CAP under different electrolyte conditions: after reacting for 3 hours, the CAP degradation rate in various electrolyte solutions reaches 99 percent.
FIG. 11 shows Co obtained in example 6 of the present invention 1 Graphs of reductive dehalogenation performance of Ti electrodes on CAP under different electrolyte conditions: after 3 hours of reaction, the dechlorination proportion of CAP in various electrolyte solutions reaches more than 95 percent. This proves that Co 1 Ti electrode 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.
FIG. 12 shows Co obtained in example 7 of the present invention 1 -reduction dehalogenation stability of Ti electrode to CAP test. The activity of the material is not obviously reduced in the reaction process of 48 hours (16 rounds), the CAP degradation rate is kept above 99.9%, and the dechlorination ratio is kept above 90%. The results demonstrate that the foamed titanium based cobalt monatomic electrode (Co) 1 Ti) has good stability in reductive dehalogenation.
Detailed Description
The invention is described in detail below with reference to the figures and specific embodiments. The following examples are carried out on the premise of the technical scheme of the invention, and detailed embodiments and specific operation procedures are given, but the scope of the invention is not limited to the following examples.
Example 1
(1) Foamed titanium based cobalt monoatomic electrode (Co) 1 -Ti) preparation method:
first, a 6.25mg/mL ethanolic cobalt nitrate solution was prepared. 1125. Mu.L of an ethanol solution of cobalt nitrate was uniformly sprayed on a titanium foam (area 9 cm) 2 0.68mm thick). Then, the sprayed titanium foam is placed in a porcelain boat, placed in a tube furnace, and introduced with hydrogen/argon mixed gas to remove air, and then the titanium foam is placed in a hydrogen/argon mixtureTreating at 300 deg.C for 3 hr under mixed gas atmosphere to obtain foamed titanium-base cobalt monoatomic electrode (Co) 1 -Ti)。
(2) Material characterization:
foamed titanium-based cobalt monoatomic electrode (Co) prepared in example 1 1 Ti) performing transmission electron microscopy characterization for spherical aberration correction and two-dimensional elemental image (EDS mapping) characterization for cobalt elements. The characterization result shows that the method successfully synthesizes the monatomic material, and the cobalt monatomic is uniformly dispersed on the surface of the foam titanium.
Example 2
(1) Foamed titanium based cobalt monatomic electrode (Co) 1 -Ti) preparation method:
the same as in example 1.
(2) The electrode prepared in example 1 was subjected to an electrochemical EPR test:
DMPO was used as a scavenger to test the hydrogen radicals generated during the reaction. Reaction conditions are as follows: initial concentration of CAP was 0 or 500mg/L, with foamed titanium based cobalt monatomic electrode (Co) 1 -Ti) or a titanium foam electrode (Ti) as a cathode, a platinum sheet electrode as a counter electrode and a mercury oxide electrode as a reference electrode, and reacting for 5 minutes. In a solution with initial CAP concentration of 0, co 1 Significant H.signal was detected around both Ti and Ti electrodes, demonstrating Co 1 Ti and Ti electrodes have similar H.generating capacity. When the CAP concentration increased to 500ppm, the H.signal disappeared, demonstrating that H.was involved in the reduction reaction of CAP.
Example 3:
(1) Foamed titanium based cobalt monatomic electrode (Co) 1 -Ti) preparation method:
the same as in example 1.
(2) The electrode obtained in example 1 was subjected to catalytic activity evaluation:
the electrochemical reductive dechlorination performance was tested with Chloramphenicol (CAP) as a model contaminant. Reaction conditions are as follows: 0.067mol/L phosphate buffer (pH = 7) was used as the electrolyte, 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-shaped electrolytic cell, and a foam titanium-based cobalt monoatomic electrode (Co) is used 1 -Ti) or foamed titanium electrode (Ti) as cathode, charged with platinum sheetThe electrode was a counter electrode, and a mercury-mercury oxide electrode was a reference electrode, and the reaction was carried out at a potential of-1.0V for 3 hours. At the end of the reaction, a foamed titanium-based cobalt monatomic electrode (Co) 1 Ti) can degrade 99.9 percent of CAP, and the dechlorination proportion can reach 99 percent; whereas the titanium foam electrode (Ti) was able to degrade only 63.8% of CAP with almost no dechlorination performance.
Example 4:
(1) Foamed titanium based cobalt monatomic electrode (Co) 1 -Ti) preparation method:
the same as in example 1.
(2) The electrodes prepared in example 1 were subjected to activity evaluation under different pH conditions:
the electrolyte pH 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. Foamed titanium based cobalt monatomic electrode (Co) 1 -Ti) material at pH =5-9, the CAP degradation rate reached 99% in 2 hours. The CAP dechlorination proportion can reach more than 95% under the condition of pH =5,7, and can reach more than 80% under the condition of pH = 9. This demonstrates a foamed titanium based cobalt monatomic electrode (Co) 1 Ti) has a wide pH working range.
Example 5:
(1) Foamed titanium based cobalt monatomic electrode (Co) 1 -Ti) preparation method:
the same 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 Florfenicol (FLO), thiamphenicol (TAP) or 4-chlorophenol (4-CP) at the same initial concentration, and the rest of the experimental conditions were the same as in example 2. The degradation rate and dechlorination proportion of the 4-CP after 1 hour of reaction reach 99 percent; the degradation rate and dechlorination ratio of FLO and TAP reach 99% after reacting for 3 hours. This demonstrates a foamed titanium based cobalt monatomic 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) Foamed titanium based cobalt monoatomic electrode (Co) 1 -Ti) preparation method:
the same as in example 1.
(2) The electrode obtained in example 1 was subjected to activity evaluation under different electrolyte conditions:
changing the phosphate to Na of 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 CAP degradation rate in various electrolyte solutions reaches 99 percent, and the dechlorination proportion reaches more than 95 percent. This demonstrates a 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) Foamed titanium based cobalt monoatomic electrode (Co) 1 -Ti) preparation method:
the same as in example 1.
(2) The stability evaluation was performed on the electrode obtained in example 1:
to the same foamed titanium based cobalt monoatomic electrode (Co) 1 Ti) cycling experiments were carried out under the experimental conditions of example 2. After each reaction cycle for 3 hours, the electrolyte solution was replaced after sampling and the next reaction cycle was started for a total of 48 hours (16 cycles). The CAP degradation rate in the circulation experiment is kept above 99.9 percent, and the dechlorination proportion is kept above 90 percent, which indicates that Co is in a high-temperature environment 1 Ti has good stability of reduction dehalogenation.
According to the invention, through separating the H source supply center and the dehalogenation active site in the reduction process, the foamed titanium-based cobalt monatomic material can effectively avoid competitive adsorption of water molecules and halides on the catalytic site in the dehalogenation process, and further shows excellent electrochemical selective dehalogenation performance. The foamed titanium-based cobalt monoatomic electrode has excellent reduction dehalogenation capability on various halogen-containing pollutants, has good cycle dehalogenation stability, and can work efficiently and stably in a wide pH range and various interference ion environments. The foamed titanium-based cobalt monoatomic electrode has the advantages of cheap raw materials and simple process, is favorable for the amplified production and the actual industrial application of the electrode, and provides an efficient green approach for the actual treatment of halogenated organic wastewater.
The embodiments described above are described to facilitate an understanding and use of the invention by those skilled in the art. It will be readily apparent to those skilled in the art that various modifications to these embodiments may be made, 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 embodiments, and those skilled in the art should make modifications and alterations without departing from the scope of the present invention.
Claims (10)
1. The electrochemical high-efficiency dehalogenation electrode for the organic halogenated pollutants is characterized by being a foamed titanium-based cobalt monoatomic electrode, taking foamed titanium as a carrier, and loading monoatomic cobalt on the foamed titanium monoatomic electrode.
2. The electrode for electrochemical high-efficiency dehalogenation of organic halogenated pollutants as claimed in claim 1, wherein the mass of the monatomic cobalt accounts for 0.05-0.5% of the total mass of the electrode.
3. The electrode for electrochemical high-efficiency dehalogenation of organic halogenated pollutants as claimed in claim 1, wherein the area of the titanium foam is 4-16 cm 2 The thickness is 0.5-2 mm.
4. The preparation method of the electrochemical high-efficiency dehalogenation electrode for organic halogenated pollutants as claimed in any one of claims 1 to 3, characterized in that a cobalt nitrate solution is uniformly sprayed on the surface of a titanium foam carrier, the titanium foam carrier is naturally dried, and the sprayed titanium foam is treated at high temperature in a hydrogen/argon mixed atmosphere to obtain the titanium foam based cobalt monatomic electrode.
5. The method for preparing the electrode for electrochemical high-efficiency dehalogenation of organic halogenated pollutants as claimed in claim 4, wherein the high-temperature treatment temperature is 250-350 ℃.
6. Use of an electrode for electrochemical high-efficiency dehalogenation of organohalogenated pollutants as defined in any one of claims 1 to 3, characterised in that said electrode is used for electrochemical reductive dehalogenation.
7. The use of the electrode for electrochemical efficient dehalogenation of organic halogenated pollutants as claimed in claim 6, characterized in that an H-type electrolytic cell is used, and the electrode is used as a working electrode to perform electrochemical reductive dehalogenation on organic halogenated matters.
8. The application of the electrode for electrochemical high-efficiency dehalogenation of organic halogenated pollutants as claimed in claim 7, wherein the working electrode and the reference electrode are arranged in a cathode chamber, the counter electrode is arranged 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.
9. The application of the electrode for electrochemical high-efficiency dehalogenation of organic halogenated pollutants as claimed in claim 7, wherein in the electrolytic cell, the electrolyte solution is a buffer solution prepared from sodium monohydrogen phosphate and potassium dihydrogen phosphate, and the pH is = 5-9.
10. The application of the electrode for electrochemical high-efficiency dehalogenation of organic halogenated pollutants as claimed in claim 6, wherein in the electrochemical reduction dehalogenation reaction, the reaction voltage is-1.2 to-0.5V, and the reaction time is 2 to 4 hours.
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Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104947142A (en) * | 2015-05-29 | 2015-09-30 | 广西大学 | Preparation method of electrocatalytic reduction halogenated organic matter cathode material |
| US20190275506A1 (en) * | 2018-03-08 | 2019-09-12 | Exxonmobil Chemical Patents Inc. | Catalyst Systems Comprising Activator, Polymerization Processes Using Same, and Products Made Therefrom |
| 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 |
| CN114921799A (en) * | 2022-05-11 | 2022-08-19 | 上海交通大学 | Method and device for simultaneously synthesizing high-purity chlorine dioxide gas by using single-atom cathode and anode |
-
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Patent Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104947142A (en) * | 2015-05-29 | 2015-09-30 | 广西大学 | Preparation method of electrocatalytic reduction halogenated organic matter cathode material |
| US20190275506A1 (en) * | 2018-03-08 | 2019-09-12 | Exxonmobil Chemical Patents Inc. | Catalyst Systems Comprising Activator, Polymerization Processes Using Same, and Products Made Therefrom |
| 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 |
| CN114921799A (en) * | 2022-05-11 | 2022-08-19 | 上海交通大学 | Method and device for simultaneously synthesizing high-purity chlorine dioxide gas by using single-atom cathode and anode |
Non-Patent Citations (1)
| Title |
|---|
| YANCAI YAO: "Single Atom Ru Monolithic Electrode for Efficient Chlorine Evolution and Nitrate Reduction", ANGEW. CHEM. INT. ED. * |
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