CN116657173A - Fe-Te urea oxidation electrode with high catalytic activity and preparation method thereof - Google Patents
Fe-Te urea oxidation electrode with high catalytic activity and preparation method thereof Download PDFInfo
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- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 title claims abstract description 75
- 239000004202 carbamide Substances 0.000 title claims abstract description 75
- 238000007254 oxidation reaction Methods 0.000 title claims abstract description 61
- 230000003647 oxidation Effects 0.000 title claims abstract description 58
- 230000003197 catalytic effect Effects 0.000 title claims abstract description 26
- 238000002360 preparation method Methods 0.000 title abstract description 18
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims abstract description 40
- 238000000034 method Methods 0.000 claims abstract description 33
- 238000004070 electrodeposition Methods 0.000 claims abstract description 26
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 23
- 239000006260 foam Substances 0.000 claims abstract description 20
- 229910052759 nickel Inorganic materials 0.000 claims abstract description 20
- 239000011248 coating agent Substances 0.000 claims abstract description 16
- 238000000576 coating method Methods 0.000 claims abstract description 16
- 239000000758 substrate Substances 0.000 claims abstract description 13
- 238000009713 electroplating Methods 0.000 claims description 32
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 20
- 239000007864 aqueous solution Substances 0.000 claims description 17
- 239000007788 liquid Substances 0.000 claims description 16
- 239000000243 solution Substances 0.000 claims description 12
- 238000005406 washing Methods 0.000 claims description 12
- 239000008367 deionised water Substances 0.000 claims description 11
- 229910021641 deionized water Inorganic materials 0.000 claims description 11
- 229910052742 iron Inorganic materials 0.000 claims description 11
- 230000001590 oxidative effect Effects 0.000 claims description 11
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 8
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims description 8
- ZOMNIUBKTOKEHS-UHFFFAOYSA-L dimercury dichloride Chemical class Cl[Hg][Hg]Cl ZOMNIUBKTOKEHS-UHFFFAOYSA-L 0.000 claims description 8
- 230000007935 neutral effect Effects 0.000 claims description 8
- 229910052714 tellurium Inorganic materials 0.000 claims description 7
- PORWMNRCUJJQNO-UHFFFAOYSA-N tellurium atom Chemical compound [Te] PORWMNRCUJJQNO-UHFFFAOYSA-N 0.000 claims description 7
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 6
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 claims description 6
- 239000006258 conductive agent Substances 0.000 claims description 6
- 229910002804 graphite Inorganic materials 0.000 claims description 6
- 239000010439 graphite Substances 0.000 claims description 6
- 239000011159 matrix material Substances 0.000 claims description 6
- 238000000151 deposition Methods 0.000 claims description 5
- 238000007747 plating Methods 0.000 claims description 5
- 238000001291 vacuum drying Methods 0.000 claims description 5
- NLXLAEXVIDQMFP-UHFFFAOYSA-N Ammonia chloride Chemical compound [NH4+].[Cl-] NLXLAEXVIDQMFP-UHFFFAOYSA-N 0.000 claims description 4
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 claims description 4
- 239000006172 buffering agent Substances 0.000 claims description 4
- 239000000203 mixture Substances 0.000 claims description 4
- VOADVZVYWFSHSM-UHFFFAOYSA-L sodium tellurite Chemical compound [Na+].[Na+].[O-][Te]([O-])=O VOADVZVYWFSHSM-UHFFFAOYSA-L 0.000 claims description 4
- 235000019270 ammonium chloride Nutrition 0.000 claims description 2
- KGBXLFKZBHKPEV-UHFFFAOYSA-N boric acid Chemical compound OB(O)O KGBXLFKZBHKPEV-UHFFFAOYSA-N 0.000 claims description 2
- 239000004327 boric acid Substances 0.000 claims description 2
- 239000000872 buffer Substances 0.000 claims description 2
- 238000005520 cutting process Methods 0.000 claims description 2
- 230000010355 oscillation Effects 0.000 claims description 2
- 238000004321 preservation Methods 0.000 claims description 2
- 150000003839 salts Chemical class 0.000 claims description 2
- 239000011780 sodium chloride Substances 0.000 claims description 2
- LAJZODKXOMJMPK-UHFFFAOYSA-N tellurium dioxide Chemical compound O=[Te]=O LAJZODKXOMJMPK-UHFFFAOYSA-N 0.000 claims description 2
- 239000000463 material Substances 0.000 abstract description 17
- 238000006243 chemical reaction Methods 0.000 abstract description 5
- 239000007772 electrode material Substances 0.000 abstract description 5
- 238000011010 flushing procedure Methods 0.000 description 12
- 230000000052 comparative effect Effects 0.000 description 10
- 239000003054 catalyst Substances 0.000 description 6
- KWGKDLIKAYFUFQ-UHFFFAOYSA-M lithium chloride Chemical compound [Li+].[Cl-] KWGKDLIKAYFUFQ-UHFFFAOYSA-M 0.000 description 6
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 4
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 4
- 238000001035 drying Methods 0.000 description 4
- 239000001257 hydrogen Substances 0.000 description 4
- 229910052739 hydrogen Inorganic materials 0.000 description 4
- 238000001228 spectrum Methods 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- 230000008021 deposition Effects 0.000 description 3
- 239000012153 distilled water Substances 0.000 description 3
- 238000005265 energy consumption Methods 0.000 description 3
- 238000004299 exfoliation Methods 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 239000002105 nanoparticle Substances 0.000 description 3
- 238000003860 storage Methods 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 238000005868 electrolysis reaction Methods 0.000 description 2
- 239000011521 glass Substances 0.000 description 2
- 238000003760 magnetic stirring Methods 0.000 description 2
- 229910000510 noble metal Inorganic materials 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 238000011056 performance test Methods 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- 239000002243 precursor Substances 0.000 description 2
- 238000003786 synthesis reaction Methods 0.000 description 2
- 229910052723 transition metal Inorganic materials 0.000 description 2
- -1 transition metal tellurides Chemical class 0.000 description 2
- 238000004832 voltammetry Methods 0.000 description 2
- 238000001075 voltammogram Methods 0.000 description 2
- 238000004458 analytical method Methods 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 238000005234 chemical deposition Methods 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000012937 correction Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 239000010411 electrocatalyst Substances 0.000 description 1
- 235000019441 ethanol Nutrition 0.000 description 1
- IDGUHHHQCWSQLU-UHFFFAOYSA-N ethanol;hydrate Chemical compound O.CCO IDGUHHHQCWSQLU-UHFFFAOYSA-N 0.000 description 1
- JEGUKCSWCFPDGT-UHFFFAOYSA-N h2o hydrate Chemical compound O.O JEGUKCSWCFPDGT-UHFFFAOYSA-N 0.000 description 1
- 238000001000 micrograph Methods 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 230000000877 morphologic effect Effects 0.000 description 1
- 239000005486 organic electrolyte Substances 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- OMEPJWROJCQMMU-UHFFFAOYSA-N selanylidenebismuth;selenium Chemical compound [Se].[Bi]=[Se].[Bi]=[Se] OMEPJWROJCQMMU-UHFFFAOYSA-N 0.000 description 1
- 230000002194 synthesizing effect Effects 0.000 description 1
- XSOKHXFFCGXDJZ-UHFFFAOYSA-N telluride(2-) Chemical compound [Te-2] XSOKHXFFCGXDJZ-UHFFFAOYSA-N 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- 238000004506 ultrasonic cleaning Methods 0.000 description 1
- 239000012808 vapor phase Substances 0.000 description 1
- 239000002351 wastewater Substances 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
- C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
- C25B11/052—Electrodes comprising one or more electrocatalytic coatings on a substrate
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/01—Products
- C25B1/02—Hydrogen or oxygen
- C25B1/04—Hydrogen or oxygen by electrolysis of water
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
- C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
- C25B11/073—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material
- C25B11/091—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of at least one catalytic element and at least one catalytic compound; consisting of two or more catalytic elements or catalytic compounds
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- Materials Engineering (AREA)
- Metallurgy (AREA)
- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Electrodes For Compound Or Non-Metal Manufacture (AREA)
Abstract
The invention discloses a high catalytic activity Fe-Te urea oxidation electrode, which comprises a conductive substrate and a Fe-Te coating deposited on the surface of the conductive substrate by an electrodeposition method. The invention also discloses a preparation method of the Fe-Te urea oxidation electrode with high catalytic activity. The Fe-Te urea oxidation electrode has low urea oxidation overpotential and can be used as an alkaline electrolyzed water urea oxidation electrode material; the invention selects the three-dimensional structure foam nickel with good conductivity and stable structure as the base material, adopts the electrodeposition method to synthesize the Fe-Te urea oxidation electrode in one step, has the advantages of short preparation time, mild reaction condition and simple steps in a constant current electrodeposition method, and the obtained Fe-Te coating has uniform components, small grain size and uniform thickness, and simultaneously the electrodeposition method ensures that the Fe-Te coating is firmly combined with the base material, reduces the falling-off phenomenon of the electrode material in the urea oxidation reaction process, and greatly improves the electrochemical stability of the electrode.
Description
Technical Field
The invention relates to a Fe-Te urea oxidation electrode with high catalytic activity and a preparation method of the Fe-Te urea oxidation electrode.
Background
The electrolysis of water is one of the hydrogen production means with great development prospect at present. The electrolyzed water consists of a Hydrogen Evolution Reaction (HER) of a cathode and an Oxygen Evolution Reaction (OER) of an anode, and the theoretical potential of the OER of the anode is too high, the dynamics are slow, so that the efficiency of the whole electrolyzed water is influenced. In recent years, the hydrogen production by utilizing urea oxidation to assist electrolysis of water is favored by the electrocatalytic world, and the theoretical potential of the Urea Oxidation Reaction (UOR) of the anode is only 0.37V, so that the catalyst can be used for replacing OER (1.23V) with high energy consumption, thereby achieving the purpose of reducing the energy consumption. In addition, urea can be degraded by adopting urea oxidation to assist hydrogen production, and the pollution of urea wastewater to the environment is relieved.
In recent years, a great deal of research effort has been devoted to developing low cost non-noble metal electrocatalysts to increase the efficiency of the urea oxidation reaction. Among the numerous catalyst materials, transition metal telluride materials have excellent electrical conductivity and become good non-noble metal urea oxidation catalysts. Patent CN109985642A discloses a Ni-Te-S composite carbon material, a preparation method and application thereof, and the material synthesized by the method has good catalytic activity, stability and acid-base adaptability, however, the method has complicated synthesis steps.
Currently, the main methods of synthesizing transition metal tellurides are exfoliation methods (including physical exfoliation methods and chemical exfoliation methods) and vapor phase chemical deposition methods. Patent CN115274883a discloses a bismuth selenide (Bi 2 Se 3 ) An electrode, a preparation method and application thereof. The catalyst synthesized by the method has long time consumption and high energy consumption, the preparation steps are complicated, the synthesized catalyst material is a powder material, and the catalyst material can be loaded on a substrate material only by using an organic binder, so that the charge transfer speed in the reaction process is reduced.
Disclosure of Invention
The invention aims to: the invention aims to provide an Fe-Te urea oxidation electrode with high catalytic activity, and another aim of the invention is to provide a method for preparing the Fe-Te urea oxidation electrode by using an electrodeposition method.
The technical scheme is as follows: the Fe-Te urea oxidation electrode with high catalytic activity comprises a conductive substrate and a Fe-Te coating deposited on the surface of the conductive substrate by an electrodeposition method.
Wherein, in the Fe-Te coating, the mass percentage of Fe is 20-70%, and the balance is Te.
Wherein the thickness of the Fe-Te coating is 1-2 micrometers. If the Fe-Te coating is too thin, the coating is insufficient; if the Fe-Te coating is too thick, the resistance is relatively high and the coating is liable to crack.
Wherein the conductive matrix is foam nickel.
The preparation method of the Fe-Te urea oxidation electrode with high catalytic activity comprises the following steps:
(1) Preparing an electroplating aqueous solution: dissolving an iron source, a tellurium source, a buffering agent and a conductive agent in water to obtain an electroplating aqueous solution;
(2) Electrodepositing to prepare Fe-Te electrode: and electroplating and depositing the electroplating aqueous solution by taking the pretreated conductive matrix as a working electrode, taking a graphite sheet as an auxiliary electrode and a saturated calomel electrode as a reference electrode to obtain the Fe-Te urea oxidation electrode.
Wherein in the step (1), the iron source is one or a mixture of a plurality of water-soluble ferric salts; the tellurium source is one or a mixture of more of tellurium dioxide, sodium tellurite or sodium tellurite.
Wherein in the step (1), the buffer is one of boric acid, citric acid or ammonium chloride; the conductive agent is one of NaCl, liCl or KCl.
Wherein, in the step (1), in the electroplating aqueous solution, the mass concentration of the iron source is 20-40 g/L; the mass concentration of the tellurium source is 1-3 g/L; the mass concentration of the buffering agent is 20-30 g/L; the mass concentration of the conductive agent is 2-5 g/L.
In the step (2), the pretreatment of the conductive substrate means: cutting the conductive substrate into rectangular pieces, placing the cut conductive substrate into absolute ethyl alcohol for ultrasonic oscillation, and then washing with deionized water; then ultrasonic oscillating is carried out in dilute hydrochloric acid, deionized water is used for washing until the pH value of the washing liquid is neutral, and the washing liquid is put into a vacuum drying oven for preservation, thus obtaining the conductive matrix.
Wherein in the step (2), the electrodeposition mode is constant current electrodeposition, and the current in the constant current electrodeposition process is 20-30 mA.cm -2 The plating solution temperature in the constant current electrodeposition process is 20-60 ℃, and the electroplating time in the constant current electrodeposition process is 30-60 min.
The beneficial effects are that: compared with the prior art, the invention has the following remarkable advantages: (1) The Fe-Te urea oxidation electrode has low urea oxidation overpotential and can be used as an alkaline electrolyzed water urea oxidation electrode material; (2) The invention selects the three-dimensional structure foam nickel with good conductivity and stable structure as the base material, adopts the electrodeposition method to synthesize the Fe-Te urea oxidation electrode in one step, has the advantages of short preparation time and simple steps, and the obtained Fe-Te coating has uniform components, small grain size and uniform thickness.
Drawings
FIG. 1 is a scanning electron microscope image of the Fe-Te urea oxidizing electrode of example 1;
FIG. 2 is a linear voltammetry (LSV) plot of Fe-Te urea oxidation electrodes in examples 1-3;
FIG. 3 is a linear voltammogram (LSV) of the urea oxidation electrode of example 1 and comparative examples 1-3.
Detailed Description
Example 1
The preparation method of the Fe-Te urea oxidation electrode with high catalytic activity comprises the following steps:
(1) Pretreatment of foam nickel: ultrasonically oscillating the cut foam nickel material in absolute ethyl alcohol for 20min to chemically remove oil, and then washing with deionized water; then ultrasonic oscillating is carried out in hydrochloric acid with the mass fraction of 10% for 20min to remove oxide on the surface of the material, deionized water is used for flushing until the pH value of flushing liquid is neutral, and finally the flushing liquid is put into a vacuum drying oven for storage for standby;
(2) Preparation of Fe-Te electrode by electrodeposition
Preparing an Fe-Te urea oxidation electrode by adopting a two-electrode system on a direct-current power supply through electrodeposition, wherein the foam nickel treated in the step (1) is used as a working electrode, a graphite sheet is used as an auxiliary electrode, and a saturated calomel electrode (Saturated calomel electrode, abbreviated as SCE) is used as a reference electrode; the mass concentration of each substance in the electroplating aqueous solution is as follows: 30 g/LFASO 4 、1g/L TeO 2 、26g/L NH 4 Cl and 4g/L LiCl, the pH value of the electroplating aqueous solution is 2.4; in the constant current electrodeposition process, the temperature of the electroplating aqueous solution is 40 ℃ and the current density is 30mA cm -2 The electroplating temperature is 40 ℃ and the electroplating time is 30min;
(3) And taking out the foam nickel after the electroplating deposition is finished, flushing the foam nickel with distilled water until the pH value of residual liquid is neutral, and drying the residual liquid for 12 hours at 70 ℃ in a vacuum environment to obtain the Fe-Te urea oxidation electrode.
The Fe-Te urea oxidizing electrode prepared in example 1 was subjected to morphological analysis by a scanning electron microscope, and the results are shown in FIG. 1. As can be seen from FIG. 1, the electrode surface presents a cauliflower-shaped structure, is tightly combined and is structurally attached with small nano particles, so that the specific surface area of the electrode is greatly increased, active sites are increased, and the improvement of the urea oxidation performance of the electrode is facilitated. The Fe-Te section was observed by a scanning electron microscope, and the thickness of the plating layer was found to be about 1. Mu.m. By carrying out energy spectrum scanning on the Fe-Te urea oxidation electrode, the mass percent of Fe is 40%, and the balance is Te.
Example 2
The preparation method of the Fe-Te urea oxidation electrode with high catalytic activity comprises the following steps:
(1) Pretreatment of foam nickel: ultrasonically oscillating the cut foam nickel material in absolute ethyl alcohol for 20min to chemically remove oil, and then washing with deionized water; then ultrasonic oscillating is carried out in hydrochloric acid with the mass fraction of 10% for 20min to remove oxide on the surface of the material, deionized water is used for flushing until the pH value of flushing liquid is neutral, and finally the flushing liquid is put into a vacuum drying oven for storage for standby;
(2) Preparation of Fe-Te electrode by electrodeposition
Preparing an Fe-Te urea oxidation electrode by adopting a two-electrode system on a direct-current power supply through electrodeposition, wherein the foam nickel treated in the step (1) is used as a working electrode, a graphite sheet is used as an auxiliary electrode, and a saturated calomel electrode (Saturated calomel electrode, abbreviated as SCE) is used as a reference electrode; the mass concentration of each substance in the electroplating aqueous solution is as follows: 30 g/LFASO 4 、2g/L TeO 2 、26g/L NH 4 Cl and 4g/L LiCl, the pH value of the electroplating aqueous solution is 2.4; in the constant current electrodeposition process, the temperature of the electroplating aqueous solution is 40 ℃ and the current density is 30mA cm -2 The electroplating temperature is 40 ℃ and the electroplating time is 30min;
(3) And taking out the foam nickel after the electroplating deposition is finished, flushing the foam nickel with distilled water until the pH value of residual liquid is neutral, and drying the residual liquid for 12 hours at 70 ℃ in a vacuum environment to obtain the Fe-Te urea oxidation electrode.
The Fe-Te section was observed by a scanning electron microscope, and the thickness of the plating layer was found to be about 1.5. Mu.m. By carrying out energy spectrum scanning on the Fe-Te urea oxidation electrode, the mass percent of Fe is 48%, and the balance is Te.
Example 3
The preparation method of the Fe-Te urea oxidation electrode with high catalytic activity comprises the following steps:
(1) Pretreatment of foam nickel: ultrasonically oscillating the cut foam nickel material in absolute ethyl alcohol for 20min to chemically remove oil, and then washing with deionized water; then ultrasonic oscillating is carried out in hydrochloric acid with the mass fraction of 10% for 20min to remove oxide on the surface of the material, deionized water is used for flushing until the pH value of flushing liquid is neutral, and finally the flushing liquid is put into a vacuum drying oven for storage for standby;
(2) Preparation of Fe-Te electrode by electrodeposition
Electrodepositing and preparing Fe-Te urea oxidation electrode on a direct-current power supply by adopting a two-electrode system, and treating the foam nickel in the step (1)As a working electrode, a graphite sheet is used as an auxiliary electrode, and a saturated calomel electrode (Saturated calomel electrode, abbreviated as SCE) is used as a reference electrode; the mass concentration of each substance in the electroplating aqueous solution is as follows: 30 g/LFASO 4 、3g/L TeO 2 、26g/L NH 4 Cl and 4g/L LiCl, the pH value of the electroplating aqueous solution is 2.4; in the constant current electrodeposition process, the temperature of the electroplating aqueous solution is 40 ℃ and the current density is 30mA cm -2 The electroplating temperature is 40 ℃ and the electroplating time is 30min;
(3) And taking out the foam nickel after the electroplating deposition is finished, flushing the foam nickel with distilled water until the pH value of residual liquid is neutral, and drying the residual liquid for 12 hours at 70 ℃ in a vacuum environment to obtain the Fe-Te urea oxidation electrode.
The Fe-Te section was observed by a scanning electron microscope, and the thickness of the plating layer was found to be about 2. Mu.m. By carrying out energy spectrum scanning on the Fe-Te urea oxidation electrode, the mass percent of Fe is 53%, and the balance is Te.
Comparative example 1
The urea oxidation electrode of comparative example 1 was prepared in substantially the same manner as in example 1, with the only difference that: no iron source was added to the aqueous electroplating solution.
Comparative example 2
The urea oxidation electrode of comparative example 2 was prepared in substantially the same manner as in example 1, with the only difference that: no tellurium source was added to the aqueous electroplating solution.
Comparative example 3
The preparation method of the Fe-Te urea oxidation electrode with high catalytic activity comprises the following steps:
(1) Pretreatment of foam nickel: NF of size 1cm×1cm was first washed and sonicated in acetone, ethanol and deionized water, respectively, for 5 minutes. After ultrasonic cleaning, the sample is dried in an eye-NDO-420 constant temperature dryer at 70 ℃;
(2) Microwave-assisted preparation of Fe-Te electrode
Under continuous magnetic stirring, 0.25g of TeCl 4 And 15g FeSO 4 The powder was dissolved in 10mL of 1-butyl-3-methylimidazole-tetrafluoroborate (C) at 65 ℃ 8 H 15 BF 4 N 2 ) Organic electrolyte; after magnetic stirring for 3 hours, the color of the solution turned yellow, argon was introduced into the reaction flask for 10 minutes in order to eliminate dissolved oxygen in the solution, the yellow solution was an fe—te precursor solution in which NF was immersed prior to synthesis, a glass vial containing NF and precursor solution was positioned at the center of a 700W microwave oven with adjustable power options, and then heated under three different power conditions of 90W, 130W and 180W, respectively, and the glass vial and the solution therein were naturally cooled;
(3) And after the completion, taking out the sample, respectively washing the sample with acetone, water and ethanol water solutions for 2 to 3 minutes, and drying the sample to obtain the Fe-Te urea oxidation electrode.
The Fe-Te section was observed by a scanning electron microscope to give a catalytic layer having a thickness of about 15. Mu.m. By carrying out energy spectrum scanning on the Fe-Te urea oxidation electrode, the mass percent of Fe is 46%, and the balance is Te.
Test of oxidation performance of Fe-Te electrode urea
The Fe-Te urea oxidation electrode materials prepared in examples 1 to 3 were subjected to electrochemical performance testing in a three-electrode system using an electrochemical workstation (CHI 600E, beijing Dewar far eastern scientific instruments Co., ltd.), the Fe-Te urea oxidation electrode material was a working electrode, a graphite sheet was an auxiliary electrode, and the SCE was a reference electrode, and the urea oxidation linear scan curve was tested in a mixed solution of 1mol/L KOH and 0.33mol/L urea at a temperature of 25℃and a scan speed of 5 mV/s. And carrying out impedance compensation correction on the electrode potential. All potentials were obtained according to the following Nernst equation: e (E) RHE ＝E SCE +0.242+0.059pH-iR (where i is the current tested and R is the solution impedance). Comparative examples 1 to 3 the urea oxidation performance test was substantially the same as the above method.
FIG. 2 is a linear voltammetry (LSV) plot of Fe-Te urea oxidation electrodes in examples 1-3; FIG. 3 is a linear voltammogram (LSV) of the urea oxidation electrode of example 1 and comparative examples 1-3.
The electrodes prepared in examples 1 to 3 and comparative examples 1 to 3 were each subjected to a urea oxidation performance test, and the resulting urea oxidation overpotential (V) was measured as shown in table 1.
Table 1 overpotential test meter for electrocatalytic urea oxidation materials
As can be seen from Table 1, the urea oxidation overpotential of the Fe-Te urea oxidation electrode prepared by the invention is far lower than that of comparative examples 1-3, which indicates that the Fe-Te urea oxidation electrode of the invention has excellent urea oxidation performance.
As can be seen from FIG. 2, example 1 performs best, and this phenomenon occurs due to the fact that with TeO 2 The mass is increased, the small nano particles on the surface of the coating are gradually increased, the specific surface area is increased, and the catalytic performance is improved, but after the specific surface area exceeds a certain amount, the Fe-Te compound grows rapidly, the number of the small nano particles on the surface of the coating is reduced, so that the specific surface area is reduced, and the catalytic performance is reduced.
Claims (10)
1. A Fe-Te urea oxidation electrode with high catalytic activity is characterized in that: comprises a conductive substrate and a Fe-Te coating deposited on the surface of the conductive substrate by an electrodeposition method.
2. The high catalytic activity Fe-Te urea oxidizing electrode according to claim 1, characterized in that: in the Fe-Te coating, the mass percentage of Fe is 20-70%, and the balance is Te.
3. The high catalytic activity Fe-Te urea oxidizing electrode according to claim 1, characterized in that: the thickness of the Fe-Te coating is 1-2 microns.
4. The high catalytic activity Fe-Te urea oxidizing electrode according to claim 1, characterized in that: the conductive matrix is foam nickel.
5. The method for preparing a high catalytic activity Fe-Te urea oxidizing electrode as set forth in claim 1, comprising the steps of:
(1) Preparing an electroplating aqueous solution: dissolving an iron source, a tellurium source, a buffering agent and a conductive agent in water to obtain an electroplating aqueous solution;
(2) Electrodepositing to prepare Fe-Te electrode: and electroplating and depositing the electroplating aqueous solution by taking the pretreated conductive matrix as a working electrode, taking a graphite sheet as an auxiliary electrode and a saturated calomel electrode as a reference electrode to obtain the Fe-Te urea oxidation electrode.
6. The method for preparing a high catalytic activity Fe-Te urea oxidizing electrode according to claim 5, characterized in that: in the step (1), the iron source is one or a mixture of a plurality of water-soluble ferric salts; the tellurium source is one or a mixture of more of tellurium dioxide, sodium tellurite or sodium tellurite.
7. The method for preparing a high catalytic activity Fe-Te urea oxidizing electrode according to claim 5, characterized in that: in the step (1), the buffer is one of boric acid, citric acid or ammonium chloride; the conductive agent is one of NaCl, liCl or KCl.
8. The method for preparing a high catalytic activity Fe-Te urea oxidizing electrode according to claim 5, characterized in that: in the step (1), in the electroplating aqueous solution, the mass concentration of the iron source is 20-40 g/L; the mass concentration of the tellurium source is 1-3 g/L; the mass concentration of the buffering agent is 20-30 g/L; the mass concentration of the conductive agent is 2-5 g/L.
9. The method for preparing a high catalytic activity Fe-Te urea oxidizing electrode according to claim 5, characterized in that: in the step (2), the pretreatment of the conductive substrate means: cutting the conductive substrate into rectangular pieces, placing the cut conductive substrate into absolute ethyl alcohol for ultrasonic oscillation, and then washing with deionized water; then ultrasonic oscillating is carried out in dilute hydrochloric acid, deionized water is used for washing until the pH value of the washing liquid is neutral, and the washing liquid is put into a vacuum drying oven for preservation, thus obtaining the conductive matrix.
10. The method for preparing a high catalytic activity Fe-Te urea oxidizing electrode according to claim 5, characterized in that: in the step (2), the electrodeposition mode is constant current electrodeposition, and the current in the constant current electrodeposition process is 20-30 mA.cm -2 The plating solution temperature in the constant current electrodeposition process is 20-60 ℃, and the electroplating time in the constant current electrodeposition process is 30-60 min.
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