CN107324452A - A kind of method that titanium net for preparing graphene nafion modifications based on Best-Effort request electrodeposition process carries palladium electrode - Google Patents
A kind of method that titanium net for preparing graphene nafion modifications based on Best-Effort request electrodeposition process carries palladium electrode Download PDFInfo
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- CN107324452A CN107324452A CN201710487239.XA CN201710487239A CN107324452A CN 107324452 A CN107324452 A CN 107324452A CN 201710487239 A CN201710487239 A CN 201710487239A CN 107324452 A CN107324452 A CN 107324452A
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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
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
- C02F1/46104—Devices therefor; Their operating or servicing
- C02F1/46109—Electrodes
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- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
- C02F1/467—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction
- C02F1/4676—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction by electroreduction
- C02F1/4678—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction by electroreduction of metals
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- C02F2101/30—Organic compounds
- C02F2101/34—Organic compounds containing oxygen
- C02F2101/345—Phenols
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- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
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Abstract
A kind of method that titanium net for preparing graphene nafion modifications based on Best-Effort request electrodeposition process carries palladium electrode, belongs to electro-catalysis field.Graphene (rGO) is scattered in nafion methanol solutions by the present invention, and ultrasonic disperse obtains uniform graphene dispersing solution.RGO is carried on by titanium net surface using dip-coating method, rGO nafion/Ti electrodes are obtained；Again using rGO nafion/Ti as negative electrode, platinized platinum is anode, using palladium chloride solution as electroplating solution, using constant current anodizing process in rGO nafion/Ti electrode surface electrodeposit metals Pd, prepares Pd/rGO nafion/Ti electrodes.The rGO nafion decorative layers loaded by dip-coating method have higher stability and controllability, improve the resistance to overturning and catalytic capability of Pd/rGO nafion/Ti electrodes.
Description
Technical field
The invention belongs to electro-catalysis field, more particularly to graphene-nafion is prepared based on Best-Effort request-electro-deposition techniques
The method that the titanium net of modification carries palladium electrode, the electrode can be used for the electro-catalysis reduction drop of chloro phenol organic matter in environment water
Solution.
Background technology
Electro-catalysis is a kind of efficient, non-secondary pollution, easily operated method, when handling waste water not by bio-toxicity
Influence, can handle high concentration, highly toxic waste water；Electrochemical techniques can be carried out at normal temperatures and pressures, additional by changing
Electric field and reach effectively control the Direction of Reaction and reaction rate purpose.It is mainly in the electrochemistry hydrogenolysis reduction process of negative electrode logical
Catholyte hydrone or the effect of hydrionic liberation of hydrogen are crossed, the atomic hydrogen (H) with strong reducing property is produced, atomic hydrogen is in electrode table
Face activation turns into reactive hydrogen (Hads), reactive hydrogen attack organic pollution realizes the fracture of C-R keys and hydrogen atom in organic molecule
Addition, realize degraded to pollutant.
Graphene (rGO) is a kind of excellent electricity material, and its electric conductivity can be carried out by the method for chemical modification
Control, the characteristics of graphene has low noise has good application in electronics.Graphene also has good mechanics and heat
Performance is learned, there is potential application value in field of compound material.By graphene-supported in matrix surface, electrode can be increased
Specific surface area, increases the attachment site of catalyst, improves electrode catalyst performance.Nafion has good electric conductivity, antipollution
Property and chemical stability, are widely used in electrode modification.
Graphene uniform is scattered in nafion- methanol solutions by the present invention, using Ti nets as matrix material, is carried using dipping
The method of drawing, graphene is loaded in Ti net surfaces.Metal Pd is carried on by graphite by electric plating method at constant current again
Alkene surface, carries palladium electrode with the titanium net for preparing graphene-nafion modifications, improves the stability of catalytic capability and electrode.
The content of the invention
The invention provides the titanium net that a kind of graphene/nafion for having higher electro-catalysis reducing power and stability is modified
Palladium electrode is carried, and there is provided the preparation method of above-mentioned electrode.
A kind of preparation method of Pd/rGO-nafion/Ti electrodes provided by the present invention, comprises the following steps：
(1) titanium (Ti) net is used into Na successively2CO3And oxalic acid treatment, the oil and oxide of Ti net surfaces are removed, is then spent
Ionized water is rinsed well, and nitrogen drying is standby；
(2) the nafion- methanol solutions that nafion mass fractions are 0.1~0.5wt% are prepared, it is molten to nafion- methanol
A certain amount of graphene (rGO) is added in liquid, ultrasonic wave is uniformly dispersed, be made uniform point that rGO concentration is preferably 0.2~1g/L
Dispersion liquid；
(3) dip-coating method is used, the Ti nets after being handled in step (1) are impregnated in the graphene prepared in step (2)
Certain time in dispersion liquid, preferably 10~20s, at the uniform velocity to lift out Ti nets from graphene dispersing solution, room temperature is dried, repeatedly
Best-Effort request repeatedly, such as 1~10 time, Ti net surfaces is carried on by rGO-nafion layers, rGO-nafion/ is made after drying in room temperature
Ti electrodes；
(4) compound concentration is 2~15mmol/L palladium bichloride (PdCl2) solution, with hydrochloric acid (HCl) by pH value of solution adjust to
0.1~0.9, as electroplate liquid；
(5) the rGO-nafion/Ti electrodes using step (3) preparation is negative electrodes, using platinized platinum as anode, are prepared with step (4)
PdCl2Solution is electroplate liquid, using constant current anodizing process in rGO-nafion/Ti electrode surface electro-deposition Pd, and Pd/rGO- is made
Nafion/Ti electrodes, wherein current density are 2.5~7.5mA/cm2, electrodeposition time is 15~75min.
The method that a kind of titanium net for preparing rGO-nafion modifications of the present invention carries palladium electrode has following characteristics：
(1) nafion solution has good filming performance, and rGO is scattered in nafion solution, can after Best-Effort request
To obtain uniform and stable rGO-nafion decorative layers on titanium net surface, be conducive to further electro-deposition Pd.
(2) rGO is loaded using dip-coating method, by changing rGO concentration and Best-Effort request number of times, in that context it may be convenient to control
Contents of the rGO on titanium net surface.
(3) using electro-deposition method carried metal Pd, can enable Pd stablize be deposited on rGO-nafion/Ti
Electrode surface, improves the resistance to overturning and catalytic activity of Pd/rGO-nafion/Ti electrodes.
The chloro phenols that Pd/rGO-nafion/Ti electrodes prepared by the present invention can be used in processing environment water body is organic
Thing, the chlorine on chlorophenol by applying constant current, can be removed, reduce its toxicity.
Brief description of the drawings
Fig. 1 is the CV of the Pd/rGO-nafion/Ti electrodes prepared by embodiment 1, embodiment 2, embodiment 3 and embodiment 4
Curve map.Wherein：(1) embodiment 1 prepares the photocurrent response curve map of electrode；(2) embodiment 2 prepares the photoelectric current sound of electrode
Answer curve map；(3) embodiment 3 prepares the photocurrent response curve map of electrode；(4) embodiment 4 prepares the photocurrent response of electrode
Curve map.
Fig. 2 is the surface SEM figures of the Pd/rGO-nafion/Ti electrodes prepared by embodiment 3.
Fig. 3 is the surface SEM figures of the rGO-nafion/Ti electrodes prepared by embodiment 3.
Embodiment
Example below and comparative example will the present invention is further illustrated with reference to accompanying drawing, but the present invention be not limited to
Lower embodiment.
Embodiment 1：
1st, titanium (Ti) net is used into Na successively2CO3And oxalic acid treatment, remove Ti net surfaces oil and oxide, then spend from
Sub- water is rinsed well, and nitrogen drying is standby；
2nd, the nafion- methanol solutions that nafion mass fractions are 0.1wt% are prepared, to 0.1wt% nafion- methanol
Graphene (rGO) is added in solution, ultrasonic wave is uniformly dispersed, the uniform dispersion that rGO concentration is 0.8g/L is made；
3rd, using dip-coating method, the Ti nets after being handled in step 1 are impregnated in the graphene dispersion prepared in step (2)
15s in liquid, at the uniform velocity to lift out Ti nets from graphene dispersing solution, room temperature is dried, repeatedly Best-Effort request 5 times, by rGO-
Nafion layers are carried on Ti net surfaces, and rGO-nafion/Ti electrodes are made after drying in room temperature；
4th, compound concentration is 5mmol/L palladium bichloride (PdCl2) solution, pH value of solution is adjusted to 0.7 with hydrochloric acid (HCl),
As electroplate liquid；
5th, the rGO-nafion/Ti electrodes using step 3 preparation is negative electrodes, using platinized platinum as anode, are prepared with step 4
PdCl2Solution is electroplate liquid, using constant current anodizing process in rGO-nafion/Ti electrode surface electro-deposition Pd, and Pd/rGO- is made
Nafion/Ti electrodes, wherein current density are 6.25mA/cm2, electrodeposition time is 15min.
6th, electrochemical property test：Respectively using Pd/rGO-nafion/Ti electrodes as working electrode, platinized platinum be to electrode,
Hg/Hg2SO4Electrode is reference electrode, with 0.5mol/L H2SO4For electrolyte solution, electricity is determined using cyclic voltammetry (CV)
The chemical property of pole, sweep speed is 50mV/s.Measure the hydrogen under -650mV and adsorb peak point current for -79.1mA, in such as Fig. 1
Shown in curve (1).
Embodiment 2：
Present embodiment difference from Example 1 is the time in rGO-nafion/Ti electrode surface electro-deposition Pd
For 30min.
Electrochemical property test：Respectively using Pd/rGO-nafion/Ti electrodes as working electrode, platinized platinum be to electrode,
Hg/Hg2SO4Electrode is reference electrode, with 0.5mol/L H2SO4For electrolyte solution, electricity is determined using cyclic voltammetry (CV)
The chemical property of pole, sweep speed is 50mV/s.It is -130.6mA, such as Fig. 1 to measure the hydrogen absorption peak point current under -650mV
Shown in middle curve (2).
Embodiment 3：
Present embodiment difference from Example 1 is the time in rGO-nafion/Ti electrode surface electro-deposition Pd
For 60min.
SEM (SEM) is tested：The Pd/rGO-nafion/Ti electrode surface patterns of preparation are characterized
Test, as a result as shown in Fig. 2 surface has the film of cicada's wings shape.The rGO-nafion/Ti electrode surfaces pattern of preparation is carried out
Characterization test, as a result as shown in figure 3, Pd particles are deposited into bud shape.
Electrochemical property test：Respectively using Pd/rGO-nafion/Ti electrodes as working electrode, platinized platinum be to electrode,
Hg/Hg2SO4Electrode is reference electrode, with 0.5mol/L H2SO4For electrolyte solution, electricity is determined using cyclic voltammetry (CV)
The chemical property of pole, sweep speed is 50mV/s.It is -150.7mA, such as Fig. 1 to measure the hydrogen absorption peak point current under -650mV
Shown in middle curve (3).
Embodiment 4：
Present embodiment difference from Example 1 is the time in rGO-nafion/Ti electrode surface electro-deposition Pd
For 75min.
Electrochemical property test：Respectively using Pd/rGO-nafion/Ti electrodes as working electrode, platinized platinum be to electrode,
Hg/Hg2SO4Electrode is reference electrode, with 0.5mol/L H2SO4For electrolyte solution, electricity is determined using cyclic voltammetry (CV)
The chemical property of pole, sweep speed is 50mV/s.Measure the hydrogen under -650mV and adsorb peak point current for -96.4mA, in such as Fig. 1
Shown in curve (4).
Claims (4)
1. a kind of method that titanium net for preparing graphene-nafion modifications based on Best-Effort request-electrodeposition process carries palladium electrode, it is special
Levy and be, carry out as steps described below：
(1) titanium (Ti) net is used into Na successively2CO3And oxalic acid treatment, the oxide and oil of Ti net surfaces are removed, deionization is then used
Water is rinsed well, and nitrogen drying is standby；
(2) the nafion- methanol solutions that nafion mass fractions are 0.1~0.5wt% are prepared, into nafion- methanol solutions
A certain amount of graphene (rGO) is added, ultrasonic wave is uniformly dispersed, and graphene dispersing solution is made；
(3) dip-coating method is used, the Ti nets after being handled in step (1) are impregnated in the graphene dispersion prepared in step (2)
Certain time in liquid, then at the uniform velocity Ti nets are lifted out from graphene dispersing solution, room temperature is dried, Best-Effort request repeatedly, will
RGO-nafion layers are carried on Ti net surfaces, and rGO-nafion/Ti electrodes are made；
(4) compound concentration is 2~15mmol/L palladium bichloride (PdCl2) solution, adjusted pH value of solution to 0.1 with hydrochloric acid (HCl)~
0.9；
(5) the rGO-nafion/Ti electrodes using step (3) preparation is negative electrodes, using platinized platinum as anode, are prepared with step (4)
PdCl2Solution is electroplate liquid, and Pd/rGO-nafion/Ti electrodes are made using constant current anodizing process electro-deposition, and wherein current density is
2.5~7.5mA/cm2, electrodeposition time is 15~75min.
2. a kind of titanium net that graphene-nafion modifications are prepared based on Best-Effort request-electrodeposition process according to claim 1
The method for carrying palladium electrode, it is characterised in that in graphene dispersing solution prepared by step (2), graphene concentration is 0.2~1g/L.
3. a kind of titanium net that graphene-nafion modifications are prepared based on Best-Effort request-electrodeposition process according to claim 1
The method for carrying palladium electrode, it is characterised in that Ti nets are impregnated in 10 in the graphene dispersing solution prepared in step (2) in step (3)
~20s.
4. a kind of titanium net that graphene-nafion modifications are prepared based on Best-Effort request-electrodeposition process according to claim 1
The method for carrying palladium electrode, it is characterised in that Best-Effort request number of times is 1~10 time in step (3).
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| TWI761858B (en) * | 2019-07-26 | 2022-04-21 | 大陸商四川茵地樂材料科技集團常州有限公司 | Method of making electrode with protection layers |
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| CN103343342A (en) * | 2013-07-09 | 2013-10-09 | 北京工业大学 | Preparation method and application of polypyrrole-multiwalled carbon nanotube collaboratively-modified palladium-carried composite electrode |
| KR20150135116A (en) * | 2014-05-22 | 2015-12-02 | 단국대학교 천안캠퍼스 산학협력단 | Composite electrolyte membranes, Preparation Method thereof and Uses thereof |
| CN105905993A (en) * | 2016-06-14 | 2016-08-31 | 北京工业大学 | Method for preparing supported palladium catalyst electrode on basis of graphene-doped Nafion film modification |
| CN106876727A (en) * | 2015-12-13 | 2017-06-20 | 中国科学院大连化学物理研究所 | A kind of graphene oxide modifies zinc-bromine flow battery carbon felt electrode and its application |
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- 2017-06-23 CN CN201710487239.XA patent/CN107324452A/en active Pending
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103343342A (en) * | 2013-07-09 | 2013-10-09 | 北京工业大学 | Preparation method and application of polypyrrole-multiwalled carbon nanotube collaboratively-modified palladium-carried composite electrode |
| KR20150135116A (en) * | 2014-05-22 | 2015-12-02 | 단국대학교 천안캠퍼스 산학협력단 | Composite electrolyte membranes, Preparation Method thereof and Uses thereof |
| CN106876727A (en) * | 2015-12-13 | 2017-06-20 | 中国科学院大连化学物理研究所 | A kind of graphene oxide modifies zinc-bromine flow battery carbon felt electrode and its application |
| CN105905993A (en) * | 2016-06-14 | 2016-08-31 | 北京工业大学 | Method for preparing supported palladium catalyst electrode on basis of graphene-doped Nafion film modification |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| TWI761858B (en) * | 2019-07-26 | 2022-04-21 | 大陸商四川茵地樂材料科技集團常州有限公司 | Method of making electrode with protection layers |
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Application publication date: 20171107 |