CN113130952A - PdNPs/NiNPs/ITO electrode and method for constructing ethanol fuel cell by electrocatalytic oxidation of ethanol solution - Google Patents
PdNPs/NiNPs/ITO electrode and method for constructing ethanol fuel cell by electrocatalytic oxidation of ethanol solution Download PDFInfo
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Abstract
The invention relates to a PdNPs/NiNPs/ITO electrode and a method for constructing an ethanol fuel cell by electrocatalytic oxidation of an ethanol solution. The method comprises the steps of taking a PdNPs/NiNPs/ITO electrode as a working electrode, an Ag/AgCl electrode as a reference electrode and a platinum wire as an auxiliary electrode to form a three-electrode system, placing the three-electrode system in an ethanol solution and a supporting electrolyte, setting the initial potential to be-0.2V, the termination potential to be 1.3V, recording cyclic voltammetry curves of ethanol with the concentrations of 20mmol/L, 40mmol/L, 60mmol/L, 80mmol/L and 100mmol/L, and analyzing the control process of the electrode in the electrocatalytic oxidation of the ethanol solution by using a standard curve method. The invention aims to develop a non-enzymatic fuel cell anode, which combines the advantages of nano materials to obtain a fuel cell anode with higher catalytic activity and stability, improve the conversion rate of chemical energy and promote the development of fuel cells.
Description
Technical Field
The invention relates to the field of fuel cells, in particular to application of a nano nickel-palladium particle composite electrode based on ITO in constructing an ethanol fuel cell by ethanol solution electrocatalytic oxidation.
Background
In the 21 st century, people are confronted with ever-increasing environmental pollution problems and energy crisis. In one aspect, a large amount of harmful gases, including NO, released by burning fossil fuelsX、SOXAnd various inhalable particles, which cause great damage to the environment and cause concern to the survival condition of people. On the other hand, the development of human economy and society is hindered by the problems of the sharp increase of the production amount of fossil fuels, the reduction of reserves, the increase of the production difficulty and the like. This has led to a schedule for efficient, clean alternative energy research. In order to reduce the dependence on fossil energy and improve the quality of life, people need to develop and utilize renewable energy sources such as solar energy, wind energy, hydraulic energy, geothermal energy, biological energy and the like according to local conditions. On the other hand, the utilization efficiency of the existing energy sources is improved, and the efficiency is improved. Therefore, the demand for energy can be reduced under the condition of not reducing the quality of life, and the emission of pollutants is reduced.
A fuel cell is a power generation device that directly converts chemical energy of a fuel and an oxidant into electrical energy through an electrochemical reaction. It generally uses hydrogen as fuel, oxygen as oxidant and water as product, so that it has less environmental pollution. Because different types of fuel cells are applied to different occasions, the fuel cells have wide application. Therefore, the preparation of fuel cell anodes with higher catalytic activity and stronger stability is the key to accelerate the industrialization of fuel cells.
At the present stage, biological enzymes are commonly used for the oxidation of glucose to produce fuel cell anodes with better oxidation activity. However, the enzyme cannot survive in a strongly acidic or strongly alkaline environment due to insufficient tolerance, and also cannot provide a stable current, thereby limiting its application to fuel cells.
Disclosure of Invention
The invention aims to develop a non-enzymatic fuel cell anode, which combines the advantages of nano materials to obtain a fuel cell anode with higher catalytic activity and stability, improve the conversion rate of chemical energy and promote the development of fuel cells. The invention takes Indium Tin Oxide (ITO) glass as a substrate and a conducting layer at the same time, and nano nickel-palladium particles as an electrochemical deposition layer; and depositing nano nickel-palladium particles on the substrate by using an electrochemical deposition method by taking the ITO as a conductive layer to prepare the nano nickel-palladium electrode.
The three-electrode system constructed by the invention is as follows: the PdNPs/NiNPs/ITO electrode is used as a working electrode, the Ag/AgCl electrode is used as a reference electrode, a platinum wire is used as an auxiliary electrode to form a three-electrode system, and the three-electrode system is placed in ethanol solution which takes potassium hydroxide solution as electrolyte to be used as fuel to form the fuel cell.
The invention adopts ethanol as fuel and has the following functions and advantages: among fuel cells, alcohol fuel cells use cheap and readily available alcohols as fuel, and the fuel is liquid at normal temperature and pressure, and compared with other fuel cells, the alcohol fuel cells have the advantages of safety, reliability, high energy density, low operating temperature, no electrolyte corrosion, and the like. The ethanol has wide sources and is renewable energy, and the manufactured fuel cell has small volume, convenient fuel utilization, cleanness and environmental protection. Therefore, the research of the alcohol fuel cell has great application potential.
In order to realize the purpose of the invention, the adopted specific technical scheme is as follows:
the method comprises the following steps of taking a PdNPs/NiNPs/ITO electrode as a working electrode, an Ag/AgCl electrode as a reference electrode and a platinum wire as an auxiliary electrode to form a three-electrode system, placing the three-electrode system in an ethanol solution and a supporting electrolyte, setting the potential to be-0.2-1.3V, recording a cyclic voltammetry curve of ethanol with the concentration of 20 mmol/L-100 mmol/L, and analyzing the control process of the electrode in the electrocatalytic oxidation of the ethanol solution by using a standard curve method.
Further, the supporting electrolyte is 1mol/LKOH, and the pH is 14.
The invention utilizes the good conductivity of ITO to prepare the electrode with high sensitivity to ethanol, and the electrode has the advantages of good catalytic effect, high sensitivity, good selectivity, stable structure and the like when ethanol is used as a base liquid.
Drawings
FIG. 1 is a surface topography of a nano nickel-palladium composite electrode based on ITO.
FIG. 2 is a comparison of cyclic voltammograms of an ethanol solution and a blank solution.
FIG. 3 is a cyclic voltammogram of ethanol solutions of different concentrations.
FIG. 4 is a standard curve of ethanol at various concentrations.
FIG. 5 is the PdNPs/NiNPs/ITO electrode anti-poisoning curve.
Detailed Description
The technical solutions of the present invention are further described below with reference to the drawings and the specific embodiments, but the present invention is not limited to the embodiments in any way. In the examples, unless otherwise specified, the experimental methods are all conventional methods; unless otherwise indicated, the experimental reagents and materials were commercially available.
The preparation method of the PdNPs/NiNPs/ITO electrode in the following embodiment comprises the following steps:
(1) and taking a piece of ITO glass to be used, testing the conductive surface of the ITO glass by using a universal meter, ensuring that the conductive surface faces downwards, and cutting the ITO glass with the size of 10 x 20mm for later use by using a glass cutter. And ultrasonically cleaning the ITO glass with deionized water for 30 minutes, taking out, washing with the deionized water, and drying with nitrogen. And ultrasonically cleaning the mixture for 30 minutes by using acetone and ethanol in sequence, and repeating the steps.
(2) A three-electrode system is adopted, a cleaned ITO electrode is used as a working electrode, an Ag/AgCl electrode and a platinum wire electrode are used as reference electrodes and a counter electrode, and the working electrode, the Ag/AgCl electrode and the platinum wire electrode are placed in an electrolytic cell filled with 0.02M nickel sulfate and 0.1M sodium sulfate solution. Setting electrodeposition parameters of an electrochemical workstation by adopting square wave voltammetry: initial voltage is-1.0V, end point potential is-0.75V, potential increment is 0.05V, amplitude is 0.025V, frequency is 15HZ, and standing time is 10 s. After deposition, the electrode is taken out and washed by ultrapure water, dried by nitrogen and placed for one day.
(3) Adopting a three-electrode system, putting a NiNPs/ITO electrode with a nano structure in acetic acid-sodium acetate with pH of 4 as a buffer solution, and PdCl with the concentration of 5mmol/L2In solution. A platinum electrode was used as the counter electrode and Ag/AgCl as the reference electrode. Setting electrodeposition parameters of an electrochemical workstation by adopting an alternating current voltammetry method: initial potential-0.5V, end potential-0.15V, potential increment 0.009V, frequency 60HZ, sampling period 10S.
Taking a PdNPs/NiNPs/ITO electrode as an anode and a Pt electrode as a cathode; adding potassium hydroxide solution with the concentration of 1mol/L into an anode pool as electrolyte solution, adding ethanol with the concentration of 0.01mol/L into the anode pool as fuel, adding potassium hydroxide with the pH value of 14 into a cathode pool as solvent, adding 0.01mol/L ethanol solution and introducing oxygen into the cathode pool, and connecting the two pools by an anion exchange membrane to construct the electrocatalytic oxidation ethanol fuel cell.
In the PdNPs/NiNPs/ITO electrode, the particle size of NiNPs is between 50 and 100nm, and the particle size of PdNPs is between 5 and 10 nm. If the size of PdNPs is larger than that of NiNPs, the palladium nanoparticles cover nickel, the synergistic catalysis effect cannot be achieved, meanwhile, the pore diameter of the palladium nanoparticles is also large, fuel enters a large amount, and the reaction is not facilitated to be further carried out. The product is not easy to diffuse out, and if the palladium nano particles are too small, the pore diameter is small. The fuel is difficult to diffuse to the active sites of the catalyst for activation, resulting in a decrease in current and thus in a decrease in power, and poor cell performance.
The surface topography based on the ITO/nano nickel-palladium composite electrode is shown in figure 1: the nano-particle size and distribution on the electrode are uniform, and the electrocatalysis performance is particularly outstanding.
Example 1 comparison of Cyclic voltammograms of an ethanol solution and a blank solution
Firstly, placing a three-electrode system in a KOH solution with the pH of 14 and the concentration of 1mol/L, scanning within a potential range of-0.2-1.3V by using a cyclic voltammetry method, and recording a cyclic voltammetry curve of a blank solution; then, the three-electrode system is placed in 100mmol/L ethanol solution to be detected containing 1mol/L KOH solution with the pH value of 14 as supporting electrolyte, and scanning is carried out within the potential range of-0.2-1.3V by using cyclic voltammetry, and the cyclic voltammetry curve of ethanol is recorded. As shown in fig. 2: the catalytic effect of PdNPs/NiNPs/ITO electrodes at 100mmol/L ethanol was tested at a scan rate of 100 mV/s. It can be seen from the figure that the catalytic current of the PdNPs/NiNPs/ITO electrode to ethanol reaches one hundred thirty million microamperes per square centimeter per mole. The fuel composed of the PdNPs/NiNPs/ITO electrode can efficiently convert the biological energy into the electric energy.
Example 2 Cyclic voltammetric response of PdNPs/NiNPs/ITO electrode to ethanol of different concentrations at the same sweep Rate
And sequentially placing the three-electrode system in ethanol solutions to be detected with different concentrations and containing 1mol/L KOH solution with the pH value of 14 as supporting electrolyte, and scanning within a potential range of-0.2-1.3V by using a cyclic voltammetry method. Recording cyclic voltammograms of 20mmol/L, 40mmol/L, 60mmol/L, 80mmol/L, 100mmol/L ethanol as shown in FIGS. 3 and 4: as can be seen from the figure, with the increasing concentration, the oxidation current of the nano electrode in the ethanol solution is also increased continuously, the oxidation peak is also increased continuously, and good linear response for catalyzing ethanol is presented, so that the oxidation-reduction reaction of the ethanol is proved to be controlled by diffusion. A good linear relation also exists between the two in the range of 10-100 mmol/L, and the linear regression equation of the ethanol oxidation peak current and the concentration is as follows: I-0.0426C + 7.8409 with a correlation coefficient of 0.9826.
EXAMPLE 3 determination of the antitoxic Capacity of the electrode
Firstly, the three-electrode system is placed in 10mm ethanol solution to be tested containing 1mol/L KOH solution with pH of 14 as supporting electrolyte, and the time current curve of the ethanol is recorded under the potential of 0.7V by using a time current method. However, as shown in fig. 5, the current density drops sharply at the beginning. At the beginning of the reaction, it is a fast kinetic reaction, so the active site does not contain adsorbed ethanol molecules. The adsorption of new ethanol molecules then depends on the release of electrocatalytic sites by ethanol oxidation, or on the occupation of electrode catalytically active sites by intermediate species such as CO, CHx, etc. formed in the first few minutes (rate determining step). Therefore, the slight decrease in current density is mainly due to the poisoning of the catalyst. Furthermore, the specific current experienced a rapid drop during the first 300 seconds throughout the test and was still a smooth and gentle change after the end of the test, with a decay of about 15%. Therefore, the electrode has strong anti-poisoning capacity and stable structure.
The above description is only for the purpose of creating a preferred embodiment of the present invention, but the scope of the present invention is not limited thereto, and any person skilled in the art can substitute or change the technical solution and the inventive concept of the present invention within the technical scope of the present invention.
Claims (4)
- The method for constructing the ethanol fuel cell by electrocatalytic oxidation of ethanol solution by the PdNPs/NiNPs/ITO electrode is characterized in that the PdNPs/NiNPs/ITO electrode is used as a working electrode, the Ag/AgCl electrode is used as a reference electrode, a platinum wire is used as an auxiliary electrode to form a three-electrode system, and the three-electrode system is placed in ethanol solution which takes potassium hydroxide solution as electrolyte to form the fuel cell.
- 2. The method according to claim 1, wherein the constructed three-electrode system is placed in an ethanol solution and a supporting electrolyte, the potential is set to be-0.2-1.3V, a cyclic voltammetry curve of ethanol with the concentration of 20 mmol/L-100 mmol/L is recorded, and the control process of the electrode electrocatalytic oxidation of the ethanol solution is analyzed by using a standard curve method.
- 3. The method of claim 1, wherein the supporting electrolyte is 1mol/LKOH and the pH is 14.
- 4. The method as claimed in claim 1, wherein the PdNPs/NiNPs/ITO electrode uses ITO as a substrate and a conductive layer at the same time, and nano nickel-palladium particles are electrochemically deposited layers; and depositing nano nickel-palladium particles on the ITO substrate by using an electrochemical deposition method to prepare the nano nickel-palladium electrode.
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