CN114318383A - Gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank - Google Patents
Gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank Download PDFInfo
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- CN114318383A CN114318383A CN202210088069.9A CN202210088069A CN114318383A CN 114318383 A CN114318383 A CN 114318383A CN 202210088069 A CN202210088069 A CN 202210088069A CN 114318383 A CN114318383 A CN 114318383A
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Abstract
The invention discloses a gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank, which comprises: the device comprises a body with an inner cavity, wherein a first proton exchange membrane is arranged in the body and divides the inner cavity into a cavity A filled with reaction gas and a cavity B filled with electrolyte;the cathode electrode is arranged in the cavity A; the anode electrode is arranged in the cavity B; the conductive carbon paper is arranged between the cathode electrode and the first proton exchange membrane, and two sides of the conductive carbon paper are respectively attached to the cathode electrode and the first proton exchange membrane. The protons in the anode chamber can infiltrate into the catalyst of the conductive carbon paper through a proton exchange membrane; meanwhile, the high-purity reaction gas in the cathode chamber can be directly contacted with the surface of the catalyst; thus, a gas-solid-liquid three-phase interface catalytic active center can be formed on the surface of the catalyst, the activity of the photoelectrocatalysis reaction is greatly improved, and particularly, the photoelectrocatalysis CO is2The reduction reaction is best applied.
Description
Technical Field
The invention relates to the technical field of photoelectrocatalysis, in particular to a gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank.
Background
The photoelectrochemical reduction technology is to utilize electric energy to convert CO2、N2、H2O、CH3The reactants such as OH and the like are reduced into various chemicals with high added values, and the technology for converting solar energy and electric energy into chemical energy is realized. The technical bottleneck existing in the current reaction system with the reactant of gas is that the gas reactant used in the solution phase reaction system is saturated gas dissolved in a solvent, and the improvement of the reaction activity is limited due to the very small dissolved amount. And commercial photo-electrocatalytic CO is currently available2The problems of liquid leakage and air leakage of the reduction reaction tank are difficult to solve.
Disclosure of Invention
Therefore, the invention provides a gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank, which is used for solving one or more technical problems.
In order to achieve the above purpose, the invention provides the following technical scheme:
a gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank comprises:
the device comprises a body with an inner cavity, wherein a first proton exchange membrane is arranged in the body and divides the inner cavity into a cavity A filled with reaction gas or liquid and a cavity B filled with electrolyte;
a cathode electrode disposed within the chamber A;
the anode electrode is arranged in the cavity B;
and the conductive carbon paper is arranged between the cathode electrode and the first proton exchange membrane, and two sides of the conductive carbon paper are respectively attached to the cathode electrode and the first proton exchange membrane.
The quartz optical window is fixed at the position of the channel outside the body, and light can irradiate the conductive carbon paper after penetrating through the quartz optical window and the channel.
Furthermore, the quartz optical window comprises a sight glass pressing sheet and a quartz lens, the sight glass pressing sheet is fixed to the body and provided with a light transmitting opening, the quartz lens is clamped and fixed between the sight glass pressing sheet and the body, and the quartz lens is located between the channel and the light transmitting opening.
Further, the body comprises a titanium cathode chamber tank body, an insulation tank body and a titanium anode chamber tank body which are sequentially arranged from front to back, wherein the cathode chamber tank body is fixed with the quartz optical window through screws, and the insulation tank body, the anode electrode and the anode chamber tank body are fixed through screws.
Further, the first proton exchange membrane is fixed on one side, close to the cathode chamber tank body, of the insulation tank body, the cathode electrode is fixed with the conductive carbon paper, and the cathode electrode is detachably arranged between the cathode chamber tank body and the insulation tank body.
Furthermore, a reference electrode is arranged in the chamber A and is fixed with the cathode chamber body.
Further, a second proton exchange membrane is arranged in the body, the second proton exchange membrane divides the cavity B into a cavity B1 filled with catholyte and a cavity B2 filled with anolyte, the anode electrode is arranged in the cavity B2, and the reference electrode is arranged in the cavity B1.
Further, still be equipped with the reference cell body between cathode chamber cell body and the insulating cell body, second proton exchange membrane presss from both sides and locates the reference cell body with between the insulating cell body, cathode electrode and conductive carbon paper are fixed mutually, cathode electrode detachably set up in between cathode chamber cell body and the reference cell body.
Further, the body is provided with a gas inlet and a gas outlet (which can also be used as liquid inlets and outlets) communicated with the A cavity and used for introducing gases such as CO2, N2 and the like, a first liquid inlet and a first liquid outlet communicated with the B2 cavity, and a second liquid inlet and a second liquid outlet communicated with the B1 cavity.
Further, the terminal post of each electrode is located outside the body.
The invention has the following advantages:
a proton exchange membrane is adopted to separate a cathode chamber (A chamber) from an anode chamber (B chamber), the cathode chamber is used for filling high-purity reaction gas, and the anode chamber is used for filling anolyte; the conductive carbon paper loaded with the catalyst is placed between the proton exchange membrane and the cathode gold-plated copper conductive plate, so that protons in the anode chamber can infiltrate into the catalyst of the conductive carbon paper through the proton exchange membrane; meanwhile, the high-purity reaction gas in the cathode chamber can be directly contacted with the surface of the catalyst; thus, a gas-solid-liquid three-phase interface catalytic active center can be formed on the surface of the catalyst, and the activity of the photoelectrocatalysis reaction is greatly improved.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings used in the description of the embodiments or the prior art will be briefly described below. It should be apparent that the drawings in the following description are merely exemplary, and that other embodiments can be derived from the drawings provided by those of ordinary skill in the art without inventive effort.
The structures, ratios, sizes, and the like shown in the present specification are only used for matching with the contents disclosed in the specification, so that those skilled in the art can understand and read the present invention, and do not limit the conditions for implementing the present invention, so that the present invention has no technical significance, and any structural modifications, changes in the ratio relationship, or adjustments of the sizes, without affecting the functions and purposes of the present invention, should still fall within the scope covered by the contents disclosed in the present invention.
Fig. 1 is a perspective view (two-chamber structure) of a gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank provided in embodiment 1 of the present invention;
FIG. 2 is an exploded view of a gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank provided in example 1 of the present invention;
fig. 3 is a perspective view (three-chamber structure) of another gas-liquid-solid three-phase interface photoelectrocatalysis reaction tank provided in embodiment 2 of the present invention;
fig. 4 is an exploded view of a gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank provided in embodiment 2 of the invention.
In the figure: 1-body, 11-cathode chamber tank body, 12-insulating tank body, 13-anode chamber tank body, 14-reference tank body, 21-first proton exchange membrane, 22-second proton exchange membrane, 3-cathode electrode, 4-anode electrode, 5-conductive carbon paper, 6-quartz optical window, 61-sight glass pressing sheet, 62-quartz lens and 7-reference electrode.
Detailed Description
The present invention is described in terms of particular embodiments, other advantages and features of the invention will become apparent to those skilled in the art from the following disclosure, and it is to be understood that the described embodiments are merely exemplary of the invention and that it is not intended to limit the invention to the particular embodiments disclosed. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
In the present specification, the terms "upper", "lower", "left", "right", "middle", and the like are used for clarity of description, and are not intended to limit the scope of the present invention, and changes or modifications in the relative relationship may be made without substantial changes in the technical content.
Example 1
As shown in fig. 1 and 2, example 1 provides a gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank, which comprises a body 1, a first proton exchange membrane 21, a cathode electrode 3, an anode electrode 4, conductive carbon paper 5, a quartz optical window 6 and a reference electrode 7.
This example uses CO2The gas raw material is taken as an example. The body 1 is provided with an inner cavity, and a first proton exchange membrane 21 is arranged in the body 1 to divide the inner cavity into a part filled with CO2A gas chamber A and a gas chamber B filled with electrolyte; wherein the chamber A is called as cathode chamber, and the chamber B is called as anode chamber; the chamber A is provided with an air inlet and an air outlet, and the chamber B is provided with a liquid inlet and an liquid outlet, and can adopt a mobile phase to continuously provide reaction raw materials for the reaction tank. The cathode electrode 3 is arranged in the cavity A, and a binding post of the cathode electrode is positioned outside the body 1. The anode electrode 4 is arranged in the cavity B, and a binding post of the anode electrode is positioned outside the body 1. The surface of the conductive carbon paper 5 is loaded with a catalyst, the conductive carbon paper 5 is arranged between the cathode electrode 3 and the first proton exchange membrane 21, and two sides of the conductive carbon paper 5 are respectively attached to the cathode electrode 3 and the first proton exchange membrane 21; thus, the conductive carbon paper 5 can realize good conductive function, can also accept protons infiltrated by the proton exchange membrane to participate in reaction, and improves the catalytic effect of a gas-solid-liquid three-phase interface. The quartz optical window 6 is fixed outside the body 1, a channel is arranged at the position where the quartz optical window 6 is fixed on the body 1, the channel is communicated with the chamber A, and the joint of the quartz optical window 6 and the body 1 is provided with a sealing design. A reference electrode 7 is arranged in the chamber A, the reference electrode 7 is fixed with a cathode chamber body 11, and a binding post of the reference electrode is positioned outside the body 1. It should be noted that the chamber a can also be used for expanding the experiment to introduce the reaction liquid.
In this embodiment, the quartz optical window 6 includes a mirror pressing sheet 61 and a quartz lens 62, the mirror pressing sheet 61 is fixed to the body 1, the mirror pressing sheet 61 has a light-transmitting opening, the quartz lens 62 is sandwiched and fixed between the mirror pressing sheet 61 and the body 1, and the quartz lens 62 is located between the channel and the light-transmitting opening. The quartz light window 6 has a size of 30mm in diameter, and light can irradiate the surface of the catalyst on the conductive carbon paper 5 after passing through the light-transmitting opening, the quartz lens 62 and the channel.
In this embodiment, the main body 1 includes a titanium cathode chamber tank 11, a teflon insulating tank 12 and a titanium anode chamber tank 13, which are sequentially arranged from front to back, the joints of the tanks are sealed, and the three tanks are combined together to form the main body 1 with an inner cavity, so that the three tanks have cavities required for forming the inner cavity, which should be appreciated by those skilled in the art, and therefore, the shape of each cavity is not described again. The cell body 11 of the cathode chamber and the quartz light window 6 are fixed through screws (regarded as a first integral part), and are not disassembled in the subsequent use process after being fastened; the insulating tank body 12, the anode electrode 4 and the anode chamber tank body 13 are fixed by screws (regarded as a second integral component), and are not disassembled in the subsequent use process after being fastened; the first integral component and the second integral component are connected through screws; the first proton exchange membrane 21 is fixed on one side of the insulation tank body 12 close to the cathode chamber tank body 11; the cathode electrode 3 is fixed with the conductive carbon paper 5, the cathode electrode 3 is detachably arranged between the cathode chamber body 11 and the insulating chamber body 12, and the cathode electrode 3 is clamped through a first integral component and a second integral component; when the catalyst needs to be replaced in the subsequent use process, the screw between the first integral component and the second integral component is removed, the cathode electrode 3 is taken out, and the conductive carbon paper 5 or the catalyst on the conductive carbon paper 5 is replaced.
The proton exchange membrane is used to separate a cathode chamber (A chamber) filled with high-purity reaction gas (such as CO) from an anode chamber (B chamber)2) The anode chamber is used for charging anode electrolyte; the conductive carbon paper 5 loaded with the catalyst is placed between the proton exchange membrane and the cathode gold-plated copper conductive plate, so that protons in the anode chamber can infiltrate into the catalyst of the conductive carbon paper 5 through the proton exchange membrane; meanwhile, the high-purity reaction gas in the cathode chamber can be directly contacted with the surface of the catalyst; thus, a gas-solid-liquid three-phase interface catalytic active center can be formed on the surface of the catalyst, and reactants are greatly improvedIs the catalytic activity of the gas. The device is provided with a quartz optical window 6, light can be irradiated on the catalyst through the quartz optical window 6, and the light is added at the same time of electrocatalysis, so that a photoelectrocatalysis reaction system is formed.
In the present embodiment, the cathode electrode 3 is a gold-plated copper conductive plate, and the anode electrode 4 is in the form of a platinum sheet fixed on the surface of the gold-plated copper conductive plate (which may be referred to as a platinum electrode); wherein the connection of each electrode and the body 1 has an insulation design.
In this example, a silver/silver chloride electrode was used as the reference electrode 7, and a three-electrode system was used.
By using CO2The reduction reaction system is an example, and the photocatalytic activity, the electrocatalytic activity and the photoelectrocatalytic activity are respectively tested. The test conditions were: catalyst loading 2mg/cm2，CO2High purity gas flow rate of 2ml/min, 0.1M KOH aqueous solution as anolyte, light source T3 lamp, full spectrum 15A, 500mW/cm2The voltage is-1V. The results are shown in the table below, which proves that the structure and the function of the photoelectrocatalysis reaction tank are very complete, the activity of the test reaction system is improved by orders of magnitude compared with the activity in the same field, and the photoelectrocatalysis reaction tank is breakthrough progress in the field.
Example 2
As shown in fig. 3 and 4, example 2 provides another gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank, the structure of which is substantially the same as that of example 1, and only the difference is described below.
This example still uses CO2The gas raw material is taken as an example. In this embodiment, the body 1 is further provided with a second proton exchange membrane 22, the second proton exchange membrane 22 divides the chamber B into a chamber B1 filled with catholyte and a chamber B2 filled with anolyte, wherein the chamber a is called a first cathode chamber, the chamber B1 is called a second cathode chamber, and the chamber B2 is called an anode chamber. An anode electrode 4 is arranged in the B2 chamber, and a reference electrode 7 is arranged in the B1 chamber. A reference cell body 14 is also arranged between the cathode chamber cell body 11 and the insulation cell body 12, and the joints of the cell bodies are sealedAnd (5) designing. Second proton exchange membrane 22 is sandwiched between reference cell 14 and insulated cell 12. In this embodiment, the cathode electrode 3 is still fixed to the conductive carbon paper 5, but the cathode electrode 3 is detachably disposed between the cathode chamber body 11 and the reference chamber body 14. The body 1 is provided with an air inlet and an air outlet which are communicated with the cavity A, a first liquid inlet and a first liquid outlet which are communicated with the cavity B2, and a second liquid inlet and a second liquid outlet which are communicated with the cavity B1.
When three chambers are adopted, two proton exchange membranes are adopted to divide the inner cavity into a first cathode chamber, a second cathode chamber and an anode chamber, wherein the first cathode chamber is used for filling high-purity reaction gas (such as CO)2) The second cathode chamber is used for charging catholyte, and the third cathode chamber is used for charging anolyte. The first cathode chamber and the second cathode chamber can be separately activated, thereby forming an experimental comparison.
Although the invention has been described in detail above with reference to a general description and specific examples, it will be apparent to one skilled in the art that modifications or improvements may be made thereto based on the invention. Accordingly, such modifications and improvements are intended to be within the scope of the invention as claimed.
Claims (10)
1. The utility model provides a gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank which characterized in that includes:
the device comprises a body with an inner cavity, wherein a first proton exchange membrane is arranged in the body and divides the inner cavity into a cavity A filled with reaction gas and a cavity B filled with electrolyte;
a cathode electrode disposed within the chamber A;
the anode electrode is arranged in the cavity B;
and the conductive carbon paper is arranged between the cathode electrode and the first proton exchange membrane, and two sides of the conductive carbon paper are respectively attached to the cathode electrode and the first proton exchange membrane.
2. The gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank according to claim 1, further comprising a quartz optical window, wherein the body is provided with a channel communicated with the chamber A, the quartz optical window is fixed at the position of the channel outside the body, and light can irradiate the conductive carbon paper after passing through the quartz optical window and the channel.
3. The gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank according to claim 2, wherein the quartz optical window comprises a sight glass pressing sheet and a quartz lens, the sight glass pressing sheet is fixed with the body, the sight glass pressing sheet is provided with a light transmission opening, the quartz lens is clamped and fixed between the sight glass pressing sheet and the body, and the quartz lens is positioned between the channel and the light transmission opening.
4. The gas-liquid-solid three-phase interface photoelectrocatalysis reaction tank of claim 2, wherein the body comprises a titanium cathode chamber tank body, an insulating tank body and a titanium anode chamber tank body which are sequentially arranged from front to back, the cathode chamber tank body is fixed with the quartz light window through screws, and the insulating tank body, the anode electrode and the anode chamber tank body are fixed through screws.
5. The gas-liquid-solid-phase interface photoelectrocatalysis reaction tank of claim 4, wherein the first proton exchange membrane is fixed on one side of the insulating tank body close to the cathode chamber tank body, the cathode electrode is fixed with conductive carbon paper, and the cathode electrode is detachably arranged between the cathode chamber tank body and the insulating tank body.
6. The gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank of claim 4, wherein a reference electrode is arranged in the chamber A, and the reference electrode is fixed with the cathode chamber tank body.
7. The gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank according to claim 4, wherein a second proton exchange membrane is further arranged in the body, the second proton exchange membrane divides the B chamber into a B1 chamber filled with catholyte and a B2 chamber filled with anolyte, the anode electrode is arranged in the B2 chamber, and the reference electrode is arranged in the B1 chamber.
8. The gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank of claim 7, wherein a reference tank body is further arranged between the cathode chamber tank body and the insulating tank body, the second proton exchange membrane is clamped between the reference tank body and the insulating tank body, the cathode electrode is fixed with conductive carbon paper, and the cathode electrode is detachably arranged between the cathode chamber tank body and the reference tank body.
9. The gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank of claim 7, wherein the body is provided with a gas inlet and a gas outlet which are communicated with the A cavity, a first liquid inlet and a first liquid outlet which are communicated with the B2 cavity, and a second liquid inlet and a second liquid outlet which are communicated with the B1 cavity.
10. The gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank according to any one of claims 1 to 9, wherein the binding post of each electrode is positioned outside the body.
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| Application Number | Priority Date | Filing Date | Title |
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| CN202210088069.9A CN114318383A (en) | 2022-01-25 | 2022-01-25 | Gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank |
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| CN202210088069.9A CN114318383A (en) | 2022-01-25 | 2022-01-25 | Gas-solid-liquid three-phase interface photoelectrocatalysis reaction tank |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115403134A (en) * | 2022-08-30 | 2022-11-29 | 南京工业大学 | Electrically driven microbial three-phase interface reactor and application thereof |
| CN115404502A (en) * | 2022-07-26 | 2022-11-29 | 电子科技大学 | Horizontal opposed double-optical-window gas diffusion electrolytic cell for photoelectrocatalysis and application thereof |
-
2022
- 2022-01-25 CN CN202210088069.9A patent/CN114318383A/en active Pending
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115404502A (en) * | 2022-07-26 | 2022-11-29 | 电子科技大学 | Horizontal opposed double-optical-window gas diffusion electrolytic cell for photoelectrocatalysis and application thereof |
| CN115403134A (en) * | 2022-08-30 | 2022-11-29 | 南京工业大学 | Electrically driven microbial three-phase interface reactor and application thereof |
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