CN109470725B - Synchrotron radiation in-situ testing device for catalyst in catalyst layer of fuel cell - Google Patents
Synchrotron radiation in-situ testing device for catalyst in catalyst layer of fuel cell Download PDFInfo
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- CN109470725B CN109470725B CN201811051414.1A CN201811051414A CN109470725B CN 109470725 B CN109470725 B CN 109470725B CN 201811051414 A CN201811051414 A CN 201811051414A CN 109470725 B CN109470725 B CN 109470725B
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- G01N23/083—Investigating or analysing materials by the use of wave or particle radiation, e.g. X-rays or neutrons, not covered by groups G01N3/00 – G01N17/00, G01N21/00 or G01N22/00 by transmitting the radiation through the material and measuring the absorption the radiation being X-rays
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Abstract
The invention provides a synchrotron radiation in-situ test device for a catalyst in a catalyst layer of a fuel cell, which comprises a synchrotron radiation light source (1), a front ionization chamber, an in-situ cell and a rear ionization chamber or a fluorescence detector (7); x-rays are emitted from the synchrotron radiation light source (1) and are emitted to a rear ionization chamber or a fluorescence detector (7) through the front ionization chamber and the in-situ cell. The in-situ cell comprises a working electrode side part and an auxiliary electrode side part; the side part of the working electrode is connected with the side part of the auxiliary electrode through a through hole mechanism and a connecting piece (15). The invention provides a synchronous radiation in-situ test device for a catalyst in a catalyst layer of a fuel cell, which is suitable for an electrocatalytic reaction in-situ pool for in-situ synchronous radiation XAFS detection, thereby realizing a key technical problem of detecting the structure evolution of the catalyst in real time.
Description
Technical Field
The invention relates to a synchrotron radiation in-situ test device for a catalyst in a catalyst layer of a fuel cell, in particular to a synchrotron radiation in-situ test device for the catalyst in the catalyst layer of the fuel cell under the action of a certain electric potential.
Background
The proton exchange membrane fuel cell consists of a cathode catalyst layer, a proton exchange membrane and an anode catalyst layer, wherein the catalyst layer is a core component in electrocatalysis reaction, and the component composition and microstructure of the catalyst layer directly influence the activity and the energy conversion efficiency of the electrocatalysis reaction. In the process of electrocatalysis reaction, researchers usually adopt a rotating disk electrode cyclic voltammetry method, a linear voltammetry scanning method and an alternating current impedance method to characterize the catalytic activity and stability of the catalyst, and then combine off-line methods such as a transmission electron microscope, X-ray diffraction, X-ray photoelectron spectroscopy, element analysis and the like to characterize the composition and microstructure of the catalyst, so as to establish the structure-effect relationship between the macroscopic catalytic activity and the microstructure of the catalyst. In practical application, the surface composition and microstructure of the catalyst can change in real time with changes in the surrounding environment (e.g., reaction atmosphere, temperature, humidity, electric potential, etc.). The offline analysis method is difficult to capture the real-time structural change rule of the catalyst in the catalytic reaction process, so that the action mechanism of the catalyst cannot be reflected really, and reliable theoretical support cannot be provided for designing the catalyst with both activity and stability. The X-ray Absorption fine structure spectroscopy (XAFS) utilizes the characteristics of wide-range energy adjustability and high signal-to-noise ratio of the X-ray Absorption fine structure spectroscopy (XAFS) to study the change rule of the linear Absorption coefficient of a substance with energy, so as to obtain the information of the structure of the neighbors around the Absorption atoms. The method is mainly characterized by having element selectivity, and analyzing real-time structure information such as the type, coordination number, coordination distance with a coordination atom, oxidation state, electronic structure and the like of a neighboring coordination atom of a specific element in a catalyst layer of a fuel cell through an additional in-situ device (such as atmosphere, temperature and potential), thereby providing extremely favorable conditions for obtaining real-time structure information of substances which are difficult to obtain or can not be obtained by a plurality of conventional methods.
Based on the real-time structural information of the catalyst in the electrocatalysis reaction process of the synchrotron radiation in-situ detection, high-energy and high-brightness X rays generated by a synchrotron radiation light source are required to be irradiated on a membrane electrode in a working state, and then X ray absorption signals of detected elements in the membrane electrode catalyst are collected.
Disclosure of Invention
Aiming at the defects in the prior art, the invention aims to provide a synchrotron radiation in-situ test device for a catalyst in a catalyst layer of a fuel cell.
The invention provides a synchrotron radiation in-situ test device for a catalyst in a catalyst layer of a fuel cell, which comprises a synchrotron radiation light source, a front ionization chamber, an in-situ pool and a rear ionization chamber or a fluorescence detector;
the X-ray is emitted from the synchrotron radiation light source, and then is emitted to the back ionization chamber or the fluorescence detector through the front ionization chamber and the in-situ cell.
Preferably, the in situ cell comprises a working electrode side and an auxiliary electrode side;
the side part of the working electrode is connected with the side part of the auxiliary electrode through a through hole mechanism and a connecting piece.
Preferably, the working electrode side part comprises a working electrode side fastening end plate and a working electrode side insulating support plate;
the through hole mechanism comprises a working electrode side through hole;
a working electrode side sealing gasket is arranged between one side of the working electrode side fastening end plate and one side of the working electrode side insulating support plate;
working electrode side through holes corresponding in position are formed in one side of the working electrode side fastening end plate and one side of the working electrode side insulating support plate;
the through hole on the working electrode side forms a mounting hole of the connecting piece.
Preferably, the auxiliary electrode side part comprises an auxiliary electrode side fastening end plate, an auxiliary electrode side insulating support plate;
the through hole mechanism comprises an auxiliary electrode side through hole;
auxiliary electrode side through holes corresponding in position are formed in one side of the auxiliary electrode side fastening end plate and one side of the auxiliary electrode side insulating support plate;
the position of the auxiliary electrode side through hole corresponds to the position of the working electrode side through hole of the through hole mechanism;
the side part of the working electrode penetrates through the mounting hole through a connecting piece to be connected with the side part of the auxiliary electrode.
Preferably, the middle part of the working electrode side fastening end plate and the middle part of one side of the working electrode side insulating support plate are both provided with a working electrode side insulating support plate groove;
the number of the working electrode side parts is multiple;
the working electrode side insulation support plate grooves between the middle parts of the two adjacent working electrode side fastening end plates are oppositely arranged;
the plurality of working electrode side insulating support plate grooves constitute a working electrode side optical component accommodation space.
Preferably, the middle part of the auxiliary electrode side fastening end plate is provided with an auxiliary electrode side insulating support plate groove;
an auxiliary electrode side insulating support plate groove is formed in the middle of the other side of the auxiliary electrode side insulating support plate;
the number of the auxiliary electrode side parts is multiple;
the auxiliary electrode side insulating support plate grooves between the middle parts of the other sides of the two adjacent auxiliary electrode side insulating support plates are oppositely arranged;
auxiliary electrode side insulating support plate grooves are oppositely arranged in the middle of two adjacent auxiliary electrode side fastening end plates;
the auxiliary electrode side insulation support plate grooves form an auxiliary electrode side optical component accommodating space;
the position of the optical component accommodation space on the auxiliary electrode side is set opposite to the position of the optical component accommodation space on the working electrode side.
Preferably, the working electrode side optical component includes an X-ray transparent film, a working electrode side gasket;
the optical component at the working electrode side also comprises a metal collector plate at the working electrode side;
and one sides of the working electrode side sealing gasket, the X-ray transmitting film, the working electrode side metal current collecting plate and the membrane electrode are sequentially arranged in the optical component accommodating space on the working electrode side.
Preferably, the auxiliary electrode-side optical component includes an auxiliary electrode-side metal current collecting plate, an auxiliary electrode-side gasket;
the other side of the membrane electrode, the auxiliary electrode side metal collector plate and the auxiliary electrode side sealing gasket are sequentially arranged in the optical component accommodating space on the auxiliary electrode side;
and the auxiliary electrode side metal collector plate and the working electrode side metal collector plate are provided with external through holes.
Preferably, the middle part of the optical component on the auxiliary electrode side and the middle part of the optical component on the working electrode side are both provided with through hole parts; wherein the central part of the X-ray transparent film in the central part of the optical component on the working electrode side is not provided with a through hole part;
the middle part of one side of the working electrode side fastening end plate, the middle part of one side of the working electrode side insulating support plate and the middle part of one side of the auxiliary electrode side fastening end plate are respectively provided with a through hole part;
x-rays are emitted from the synchrotron radiation light source to the rear ionization chamber or the fluorescence detector through the through hole part emitted by the front ionization chamber and the in-situ cell.
Preferably, the working electrode side fastening end plate and the auxiliary electrode side fastening end plate are both provided with fastening end plate X-ray transmission windows;
a working electrode side insulating support plate groove and an auxiliary electrode side insulating support plate groove are respectively formed in one side of the working electrode side insulating support plate and one side of the auxiliary electrode side insulating support plate;
the other side of the working electrode side fastening end plate and the other side of the auxiliary electrode side fastening end plate are respectively provided with a working electrode side insulating support plate X-ray transmission window and an auxiliary electrode side insulating support plate X-ray transmission window;
the position of the groove of the working electrode side insulating support plate, the position of the groove of the auxiliary electrode side insulating support plate, the position of the X-ray transmission window of the working electrode side insulating support plate and the position of the X-ray transmission window of the auxiliary electrode side insulating support plate are all on the same horizontal line or are superposed, and an optical part is formed;
the position of the center of the optical part and the position of the through hole part are on the same horizontal line or coincide;
the working electrode insulation supporting plate is provided with an electrolyte through hole at the working electrode side;
the opening position of the through hole is positioned at the top end of the groove of the insulating support plate at the working electrode side.
The auxiliary electrode side insulation support plate is provided with an auxiliary electrode side electrolyte injection hole and a reference electrode placing through hole;
the opening positions of the electrolyte injection hole on the auxiliary electrode side and the reference electrode placing through hole are positioned at the top end of the auxiliary electrode side insulating support plate;
and the electrolyte injection hole on the auxiliary electrode side and the tail outlet position of the reference electrode placing through hole are both positioned in the groove of the auxiliary electrode side insulating support plate.
Compared with the prior art, the invention has the following beneficial effects:
1. the invention provides a synchronous radiation in-situ test device for a catalyst in a catalyst layer of a fuel cell, which is suitable for an electrocatalytic reaction in-situ pool for in-situ synchronous radiation XAFS detection, thereby realizing a key technical problem of detecting the structure evolution of the catalyst in real time.
2. The synchrotron radiation in-situ test device for the catalyst in the catalyst layer of the fuel cell is used for an in-situ cell for electrocatalysis reaction research, and the detection window is required to meet the test requirements in a transmission mode and a fluorescence mode at the same time, and the thickness and the material of the detection window are required to avoid absorbing X rays as much as possible, so that the integrity, the accuracy and the reliability of a collected XAFS data signal are ensured.
3. Meanwhile, the synchrotron radiation in-situ test device for the catalyst in the catalyst layer of the fuel cell is suitable for in-situ XAFS test of different types of catalysts, the sample cell is simple and convenient for replacing and assembling samples, and transmission or fluorescence reflection signals of a certain element to be tested in the catalyst can be conveniently obtained.
Drawings
Other features, objects and advantages of the invention will become more apparent upon reading of the detailed description of non-limiting embodiments with reference to the following drawings:
fig. 1 is a schematic flow diagram of a synchrotron radiation XAFS in-situ detection device for electrocatalytic reaction provided by the invention.
Fig. 2 is a schematic cross-sectional view of a sample cell for in-situ detection of synchrotron radiation XAFS for electrocatalytic reaction provided by the invention.
Fig. 3 is a front-back side structural view of the working electrode side fastening end plate and the auxiliary electrode side fastening end plate provided by the present invention.
Fig. 4 is a structural view of one surface of the working electrode side insulating support plate according to the present invention.
FIG. 5 is a structural view of the other surface of the working electrode side insulating support plate according to the present invention.
Fig. 6 is a structural view of one surface of the auxiliary electrode side insulation support plate provided by the present invention.
Fig. 7 is a structural view of the other surface of the auxiliary electrode side insulating support plate according to the present invention.
FIG. 8 shows the results of the experiment in example 1 of the present invention.
The following table indicates the meanings of the respective reference numerals in the drawings attached to the specification:
Detailed Description
The present invention will be described in detail with reference to specific examples. The following examples will assist those skilled in the art in further understanding the invention, but are not intended to limit the invention in any way. It should be noted that it would be obvious to those skilled in the art that various changes and modifications can be made without departing from the spirit of the invention. All falling within the scope of the present invention.
The invention provides a synchrotron radiation in-situ test device for a catalyst in a catalyst layer of a fuel cell, which is characterized by comprising a synchrotron radiation light source 1, a front ionization chamber, an in-situ cell and a rear ionization chamber or a fluorescence detector 7; the X-ray is emitted from the synchrotron radiation light source 1 and is emitted to a rear ionization chamber or a fluorescence detector 7 through a front ionization chamber and an in-situ cell.
The in-situ cell comprises a working electrode side part and an auxiliary electrode side part; the side part of the working electrode is connected with the side part of the auxiliary electrode through a through hole mechanism and a connecting piece 15.
The side part of the working electrode comprises a working electrode side fastening end plate 11 and a working electrode side insulating support plate 12; the via mechanism includes a working electrode side via 36; a working electrode sealing gasket 17 is arranged between one side of the working electrode side fastening end plate 11 and one side of the working electrode side insulating support plate 12; working electrode side through holes 36 with corresponding positions are arranged on one side of the working electrode side fastening end plate 11 and one side of the working electrode side insulating support plate 12; the working electrode side through hole 36 constitutes a mounting hole of the connecting member 15.
The auxiliary electrode side part comprises an auxiliary electrode side fastening end plate 14 and an auxiliary electrode side insulating support plate 13; the via mechanism includes an auxiliary electrode-side via 37; auxiliary electrode side through holes 37 with corresponding positions are arranged on one side of the auxiliary electrode side fastening end plate 14 and one side of the auxiliary electrode side insulating support plate 13; the position of the auxiliary electrode side through hole 37 corresponds to the position of the working electrode side through hole 36 of the through hole mechanism; the side of the working electrode is connected with the side of the auxiliary electrode by a connecting piece 15 passing through the mounting hole.
Working electrode side insulating support plate grooves 24 are formed in the middle of the working electrode side fastening end plate 11 and the middle of one side of the working electrode side insulating support plate 12; the number of the working electrode side parts is multiple; the working electrode side insulation support plate grooves 24 between the middle parts of two adjacent working electrode side fastening end plates 11 are oppositely arranged; a plurality of the working electrode side insulating support plate grooves 24 constitute an optical component accommodation space on the working electrode side.
An auxiliary electrode side insulating support plate groove 28 is formed in the middle of the auxiliary electrode side fastening end plate 14; an auxiliary electrode side insulating support plate groove 28 is formed in the middle of the other side of the auxiliary electrode side insulating support plate 13; the number of the auxiliary electrode side parts is multiple; auxiliary electrode side insulating support plate grooves 28 between the other side middle parts of two adjacent auxiliary electrode side insulating support plates 13 are oppositely arranged; auxiliary electrode side insulation support plate grooves 28 are oppositely arranged at the middle parts of two adjacent auxiliary electrode side fastening end plates 14; a plurality of the auxiliary electrode side insulating support plate grooves 28 constitute an auxiliary electrode side optical component accommodation space; the position of the optical component accommodation space on the auxiliary electrode side is set opposite to the position of the optical component accommodation space on the working electrode side.
The optical component on the working electrode side includes an X-ray transmitting film 16, a working electrode side gasket 17; one side of the working electrode side seal gasket 17, the X-ray transmitting film 16, the working electrode side metal current collecting plate 21, and the membrane electrode 20 is disposed in the optical module accommodating space on the working electrode side in this order.
The auxiliary electrode side optical component includes an auxiliary electrode side metal current collecting plate 19, an auxiliary electrode side gasket 18; the optical component on the working electrode side further includes a working electrode side metal current collecting plate 21; the other side of the membrane electrode 20, the auxiliary electrode side metal current collecting plate 19 and the auxiliary electrode side sealing gasket 18 are sequentially arranged in the optical component accommodating space on the auxiliary electrode side; and the auxiliary electrode side metal current collecting plate 19 and the working electrode side metal current collecting plate 21 are provided with external through holes.
The middle part of the optical component on the auxiliary electrode side and the middle part of the optical component (except the X-ray transmission film) on the working electrode side are both provided with through hole parts 34; more specifically; the central portion of the X-ray transmitting film 16 in the optical assembly on the working electrode side is not provided with the through hole portion 34; and no X-ray transparent film in the optical component at the auxiliary electrode side; the middle part of one side of the working electrode side fastening end plate 11, the middle part of one side of the working electrode side insulating support plate 12 and the middle part of one side of the auxiliary electrode side fastening end plate 14 are all provided with through hole parts 34; x-rays are emitted from the synchrotron radiation source 1 through the through-hole 34 of the front ionization chamber, the in-situ cell, and onto the back ionization chamber or the fluorescence detector 7. The through hole portion 34 is not provided in the middle of one side of the auxiliary electrode side insulating support plate 13.
The working electrode side fastening end plate 11 and the auxiliary electrode side fastening end plate 14 are both provided with fastening end plate X-ray transmission windows 22; a working electrode side insulating support plate groove 24 and an auxiliary electrode side insulating support plate groove 28 are respectively formed in one side of the working electrode side insulating support plate 12 and one side of the auxiliary electrode side insulating support plate 13; the other side of the working electrode side fastening end plate 11 and the other side of the auxiliary electrode side fastening end plate 14 are respectively provided with a working electrode side insulating support plate X-ray transmission window 25 and an auxiliary electrode side insulating support plate X-ray transmission window 29; the positions of the electrode side insulating support plate groove 24, the auxiliary electrode side insulating support plate groove 28, the working electrode side insulating support plate X-ray transmission window 25 and the auxiliary electrode side insulating support plate X-ray transmission window 29 are all on the same horizontal line or are superposed to form an optical part; the position of the center of the optical part is on the same horizontal line or coincided with the position of the through hole part 34; the working electrode insulation support plate 12 is provided with an electrolyte through hole 26 on the working electrode side; the opening position of the through hole 26 is located at the top end of the working electrode side insulating support plate 12.
The auxiliary electrode side insulating support plate 13 is provided with an auxiliary electrode side electrolyte injection hole 30 and a reference electrode placing through hole 31; the opening positions of the electrolyte injection hole 30 and the reference electrode placing through hole 31 on the auxiliary electrode side are positioned at the top end of the auxiliary electrode side insulating support plate 13; the electrolyte injection hole 30 on the auxiliary electrode side and the tail outlet position 32 of the reference electrode placing through hole are both positioned in the auxiliary electrode side insulating support plate groove 28. The electrolyte injection hole 30 on the auxiliary electrode side and the reference electrode placing through hole 31 are both bent.
The synchrotron radiation in-situ test device for the catalyst in the catalyst layer of the fuel cell provided by the invention is further explained as follows:
the invention provides a synchrotron radiation in-situ test device for a catalyst in a catalyst layer of a fuel cell under the action of a certain potential, which comprises a working electrode side fastening end plate 11, a working electrode side insulating support plate 12, a working electrode side metal collector plate 21, an auxiliary electrode side metal collector plate 19 and an auxiliary electrode side insulating support plate 13, wherein the auxiliary electrode side fastening end plate 14 is sequentially overlapped and fastened together;
the middle part of the working electrode side fastening end plate 11 is provided with a through hole part 34 for facilitating the transmission of X-rays; the middle parts of the working electrode side metal current collecting plate 21 and the auxiliary electrode side metal current collecting plate 19 are provided with a through hole, the working electrode side current collecting plate, namely the working electrode side metal current collecting plate 21 and the auxiliary electrode side current collecting plate 19 are externally connected with an electrochemical workstation, and potential is applied to a catalytic layer of one electrode to be researched by utilizing the electrochemical workstation.
The middle part of the surface of the working electrode side insulating support plate 12 close to the membrane electrode 20 is provided with a through hole part 34, and the middle part of the surface far away from the membrane electrode 20 is provided with a working electrode side insulating support plate groove 24; the size of the through hole part 34 on the working electrode side insulating support plate 12 on the side close to the membrane electrode 20 is smaller than the size of the groove 24 on the working electrode side insulating support plate on the side far from the membrane electrode 20; the top of the working electrode side insulating support plate 12 is provided with a working electrode side electrolyte through hole 26, and the opening position of the through hole 26 is located at the top end of the working electrode side insulating support plate 12. The sealing gasket with a through hole in the middle and the X-ray transmitting film are sequentially placed in the groove of the insulating support plate on the working electrode side; the gasket is referred to as a working electrode-side gasket 17.
An auxiliary electrode side insulating support plate groove 28 is formed in the middle of the surface of the auxiliary electrode side insulating support plate 13 close to the membrane electrode 20, an auxiliary electrode side insulating support plate groove 28 is formed in the middle of the surface of the auxiliary electrode side insulating support plate 13 far away from the membrane electrode 20, and an auxiliary electrode side sealing gasket 18 is arranged in the middle of the auxiliary electrode side insulating support plate groove 28 in the middle of the surface of the auxiliary electrode side insulating support plate 13 close to the membrane electrode 20; the auxiliary electrode side insulating support plate 13 is provided with a bent electrolyte injection hole on the auxiliary electrode side, i.e., an auxiliary electrode side electrolyte injection hole 30 and a bent reference electrode placing through hole, i.e., a reference electrode placing through hole 31, the opening positions of the bent electrolyte injection hole on the auxiliary electrode side (hereinafter referred to as bent electrolyte injection hole) and the bent reference electrode placing through hole are located at the top end of the auxiliary electrode side insulating support plate 13, and the tail outlet position 32 of the bent electrolyte injection hole and the reference electrode placing through hole is located in the auxiliary electrode side insulating support plate groove 28.
The center of the working electrode side insulating support plate groove 24 and the center of the auxiliary electrode side insulating support plate groove 28 correspond to each other; the size of the through hole part 34 at the side of the working electrode side insulating support plate far away from the membrane electrode 20 is larger than the size of the groove 24 of the working electrode side insulating support plate at the side close to the membrane electrode 20; the size of the auxiliary electrode side insulating support plate groove 28 on the side of the auxiliary electrode side insulating support plate close to the membrane electrode 20 is larger than the size of the auxiliary electrode side insulating support plate groove 28 on the side of the auxiliary electrode side insulating support plate away from the membrane electrode 20.
A working electrode gasket 17 is provided between the working electrode side fastening end plate 11 and the working electrode side insulating support plate 12, and an auxiliary electrode side gasket 18 is provided between the auxiliary electrode side insulating support plate 13 and an auxiliary electrode side current collecting plate, i.e., an auxiliary electrode side metal current collecting plate 19. The through-hole portion 34 is provided in the middle of the auxiliary electrode-side metal current collecting plate 19, and the size of the through-hole portion 34 of the auxiliary electrode-side gasket 18 is larger than the size of the through-hole portion 34 of the working electrode-side gasket 17.
The working electrode side insulating support plate 12, the auxiliary electrode side insulating support plate 13, the working electrode side fastening end plate 11 and the auxiliary electrode side fastening end plate 14 are provided with a circle of screw through holes, namely a working electrode side through hole 36 and an auxiliary electrode side through hole 37. In other words, the working electrode side insulating support plate 12 surface, the working electrode side fastening end plate 11 are each provided with a working electrode side through hole 36; the auxiliary electrode side insulating support plate 13 and the auxiliary electrode side fastening end plate 14 are provided with auxiliary electrode side through holes 37; the positions of the working electrode side through hole 36 and the auxiliary electrode side through hole 37 correspond to each other.
The working electrode side fastening end plate 11, the working electrode side insulating support plate 12 and the auxiliary electrode side insulating support plate 13 of the in-situ cell are all provided with grooves in the middle, and the center positions of the grooves are overlapped or positioned on the same horizontal line. And they have the same outer frame size and the corresponding screw through hole size; when the two are connected by the screw, the center positions of the grooves for transmitting the X-rays in the middle can be coincided or positioned on the same horizontal line, and the X-rays can be irradiated on the membrane electrode 20. The grooves are a working electrode side insulating support plate groove 24 and an auxiliary electrode side insulating support plate groove 28; and controlling the potential of the in-situ cell by using a metal current collecting plate connected with the electrochemical workstation.
The in-situ cell is arranged in an X-ray Absorption fine structure spectrum (XAFS) line station, X-rays emitted by a synchronous radiation light source enter a front ionization chamber of the XAFS line station through a monochromator, then irradiate a membrane electrode 20, and reach a rear ionization chamber or a fluorescence detector 7 in a transmission or reflection mode, and the in-situ test of a catalyst structure in the electrocatalysis reaction process is realized by collecting transmission or fluorescence XAFS signals of elements to be detected in a sample; the X-rays emitted by the synchrotron radiation pass through the front ionization chamber, then pass through the through hole part 34 of the working electrode side fastening end plate 11, the through hole part 34 of the working electrode side sealing gasket 17, the X-ray transmitting film 16, the through hole part 34 of the working electrode side insulating support plate 12 and the through hole of the working electrode side metal current collecting plate 21 and irradiate on the membrane electrode 20;
the synchrotron radiation in-situ test device for the catalyst in the catalyst layer of the fuel cell provided by the invention has two light emitting modes for X rays irradiated on the membrane electrode 20: a rear ionization chamber which is provided in a transmissive manner through the through-hole portion 34 of the auxiliary electrode-side metal current collecting plate 19, the through-hole portion 34 of the auxiliary electrode-side gasket 18, the auxiliary electrode-side insulating support plate groove 28 of the auxiliary electrode-side insulating support plate 13, the through-hole of the auxiliary electrode-side fastening end plate 14 to the synchrotron radiation XAFS line station; one is to pass through a working electrode side metal collector plate through hole, a working electrode side insulation support plate through hole, an X-ray transmitting film, a working electrode side sealing gasket through hole and a working electrode side fastening end plate through hole in a reflection mode to reach a fluorescence detector.
The synchrotron radiation in-situ testing device for the catalyst in the catalyst layer of the fuel cell provided by the invention is further described below, and the following is a preferred example of the invention:
the X-ray absorption fine structure spectrum of the cathode Pt/C catalyst Pt under operating conditions of the pem fuel cell was tested. The catalyst layers are sprayed on both sides of the membrane by an electrostatic spraying method, wherein the catalyst used by the auxiliary electrode, namely the auxiliary electrode part, is a Pd/C catalyst, the catalyst used by the working electrode, namely the working electrode part, is a Pt/C catalyst, and the proton exchange membrane is DuPont Nafion 211. The XAFS signal of the working electrode Pt/C catalyst Pt was detected using a transmission mode in situ cell. The assembly process of the in-situ tank is as follows: processing a 3cm part on one side of the working electrode insulation supporting plate 122The other side of the square groove is processed with a round groove with the diameter of 5cm, an X-ray transparent film 16 is sequentially arranged in the round groove, and the middle part of the round groove is provided with a 3cm opening2Through-hole gaskets, which refer to the working electrode-side gasket 17, the auxiliary electrode-side gasket 18; then placing the outer frame at 9cm x 9cm,the middle part is provided with a hole of 3cm2One side of the working electrode of the through hole is provided with a stainless steel fastening end plate; a circular groove with the diameter of 5cm is processed at one side of the auxiliary electrode side insulating support plate 13, and 3cm is processed at the other side2The square groove and the round groove are auxiliary electrode side insulation support plate grooves 28; the middle of the round groove is provided with 4cm2A gasket for the through hole; fastening a working electrode side fastening end plate 11, a working electrode side insulating support plate 12, a working electrode side metal current collecting plate 21, an assembled membrane electrode 20, an auxiliary electrode side metal current collecting plate 19, an auxiliary electrode side insulating support plate and an auxiliary electrode side fastening end plate 14 in sequence by using a screw, and then putting a nut to screw so as to ensure that the in-situ cell does not leak liquid; injecting 0.1M HClO to both sides of the membrane electrode 204Inserting an Ag/AgCl reference electrode into the bent through hole at the top of the insulating plate 13 close to the auxiliary electrode side; different potentials are applied to the working electrode by using the electrochemical workstation, and the XAFS signal of the Pt/C catalyst Pt of the working electrode is detected by using a groove in the middle of the in-situ cell as a detection window. It can be observed that the white line peak intensity of Pt in the Pt/C catalyst gradually increases and the oxidation state of Pt gradually increases with increasing potential, indicating that the Pt surface of the catalyst adsorbs oxygen-containing species with increasing potential. The intermediate grooves are a working electrode side insulating support plate groove 24, a working electrode side insulating support plate X-ray transmitting window 25, an auxiliary electrode side insulating support plate groove 28, and an auxiliary electrode side insulating support plate X-ray transmitting window 29.
The foregoing description of specific embodiments of the present invention has been presented. It is to be understood that the present invention is not limited to the specific embodiments described above, and that various changes or modifications may be made by one skilled in the art within the scope of the appended claims without departing from the spirit of the invention. The embodiments and features of the embodiments of the present application may be combined with each other arbitrarily without conflict.
Claims (3)
1. A synchrotron radiation in-situ test device for a catalyst in a catalyst layer of a fuel cell is characterized by comprising a synchrotron radiation light source (1), a front ionization chamber, an in-situ cell and a rear ionization chamber or a fluorescence detector (7);
x-rays are emitted from the synchrotron radiation light source (1) and are emitted to a rear ionization chamber or a fluorescence detector (7) through a front ionization chamber and an in-situ pool;
the in-situ cell comprises a working electrode side part and an auxiliary electrode side part;
the side part of the working electrode is connected with the side part of the auxiliary electrode through a through hole mechanism and a connecting piece (15);
the working electrode side part comprises a working electrode side fastening end plate (11) and a working electrode side insulating support plate (12);
the through hole mechanism comprises a working electrode side through hole (36);
a working electrode side sealing gasket (17) is arranged between one side of the working electrode side fastening end plate (11) and one side of the working electrode side insulating support plate (12);
working electrode side through holes (36) with corresponding positions are arranged on one side of the working electrode side fastening end plate (11) and one side of the working electrode side insulating support plate (12);
the working electrode side through hole (36) forms a mounting hole of the connecting piece (15);
the working electrode insulation support plate (12) is provided with an electrolyte through hole (26) on the working electrode side;
the opening position of the electrolyte through hole (26) on the working electrode side is positioned at the top end of the insulating support plate (12) on the working electrode side;
the auxiliary electrode side portion includes an auxiliary electrode side insulating support plate (13);
the auxiliary electrode side insulation support plate (13) is provided with an auxiliary electrode side electrolyte injection hole (30) and a reference electrode placing through hole (31);
the opening positions of the electrolyte injection hole (30) on the auxiliary electrode side and the reference electrode placing through hole (31) are positioned at the top end of the auxiliary electrode side insulating support plate (13);
the electrolyte injection hole (30) on the auxiliary electrode side and the tail outlet position (32) of the reference electrode placing through hole (31) are both positioned in the auxiliary electrode side insulating support plate groove (28) on one side of the auxiliary electrode side insulating support plate (13);
the auxiliary electrode side part further comprises an auxiliary electrode side fastening end plate (14);
the through hole mechanism comprises an auxiliary electrode side through hole (37);
auxiliary electrode side through holes (37) with corresponding positions are formed in one side of the auxiliary electrode side fastening end plate (14) and one side of the auxiliary electrode side insulating support plate (13);
the position of the auxiliary electrode side through hole (37) corresponds to the position of the working electrode side through hole (36) of the through hole mechanism;
the side part of the working electrode penetrates through the mounting hole through a connecting piece (15) and is connected with the side part of the auxiliary electrode;
working electrode side insulating support plate grooves (24) are formed in the middle of the working electrode side fastening end plate (11) and the middle of one side of the working electrode side insulating support plate (12);
the number of the working electrode side parts is multiple;
the working electrode side insulation support plate grooves (24) between the middle parts of the two adjacent working electrode side fastening end plates (11) are oppositely arranged;
a plurality of working electrode side insulating support plate grooves (24) constitute a working electrode side optical component accommodation space;
an auxiliary electrode side insulation support plate groove (28) is formed in the middle of the auxiliary electrode side fastening end plate (14);
an auxiliary electrode side insulation support plate groove (28) is formed in the middle of the other side of the auxiliary electrode side insulation support plate (13);
the number of the auxiliary electrode side parts is multiple;
auxiliary electrode side insulating support plate grooves (28) between the middle parts of the other sides of the two adjacent auxiliary electrode side insulating support plates (13) are oppositely arranged;
auxiliary electrode side insulation support plate grooves (28) are arranged in the middle of two adjacent auxiliary electrode side fastening end plates (14) and are opposite to each other;
a plurality of auxiliary electrode side insulating support plate grooves (28) constitute an auxiliary electrode side optical component accommodation space;
the position of the optical component accommodation space on the auxiliary electrode side is set opposite to the position of the optical component accommodation space on the working electrode side;
the auxiliary electrode side optical component comprises an auxiliary electrode side metal current collecting plate (19) and an auxiliary electrode side sealing gasket (18);
the other side of the membrane electrode (20), the auxiliary electrode side metal collector plate (19) and the auxiliary electrode side sealing gasket (18) are sequentially arranged in the optical component accommodating space on the auxiliary electrode side;
the auxiliary electrode side metal current collecting plate (19) and the working electrode side metal current collecting plate (21) are provided with external through holes;
the middle part of the optical component on the auxiliary electrode side and the middle part of the optical component on the working electrode side are both provided with through hole parts (34); wherein, the middle part of the X-ray transmitting film (16) in the middle part of the optical component on the working electrode side is not provided with a through hole part (34), the auxiliary electrode side is not provided with the X-ray transmitting film, and only the auxiliary electrode side insulating support plate is not provided with the through hole part (34);
the middle part of one side of the working electrode side fastening end plate (11), the middle part of one side of the working electrode side insulating support plate (12) and the middle part of one side of the auxiliary electrode side fastening end plate (14) are respectively provided with a through hole part (34);
x-rays are emitted from the synchrotron radiation light source (1) and pass through the through hole part (34) emitted by the front ionization chamber and the in-situ cell to the rear ionization chamber or the fluorescence detector (7);
detecting XAFS signals of a working electrode Pt/C catalyst Pt by using a groove in the middle of an in-situ pool as a detection window, wherein the detection window simultaneously meets the requirements of testing in a transmission mode and a fluorescence mode, and the thickness and the material of the detection window need to avoid absorbing X rays, so that the integrity, the accuracy and the reliability of collected XAFS data signals are ensured;
the middle grooves are a working electrode side insulation support plate groove (24), a working electrode side insulation support plate X-ray transmission window (25), an auxiliary electrode side insulation support plate groove (28) and an auxiliary electrode side insulation support plate X-ray transmission window (29).
2. The synchrotron radiation in-situ test apparatus for catalysts in catalytic layers of fuel cells of claim 1, wherein the working electrode side optical assembly comprises an X-ray transparent membrane (16), a working electrode side gasket (17);
the optical component on the working electrode side further comprises a working electrode side metal current collecting plate (21);
one side of the working electrode side sealing gasket (17), the X-ray transmitting film (16), the working electrode side metal current collecting plate (21) and the membrane electrode (20) is arranged in the optical component accommodating space on the working electrode side in sequence.
3. The synchrotron radiation in-situ test device for catalysts in catalyst layers of fuel cells according to claim 1, wherein the working electrode side fastening end plate (11) and the auxiliary electrode side fastening end plate (14) are provided with fastening end plate X-ray transmission windows (22);
a working electrode side insulation support plate groove (24) and an auxiliary electrode side insulation support plate groove (28) are respectively formed on one side of the working electrode side insulation support plate (12) and one side of the auxiliary electrode side insulation support plate (13);
the other side of the working electrode side fastening end plate (11) and the other side of the auxiliary electrode side fastening end plate (14) are respectively provided with a working electrode side insulating support plate X-ray transmission window (25) and an auxiliary electrode side insulating support plate X-ray transmission window (29);
the position of the groove (24) of the working electrode side insulating support plate, the position of the groove (28) of the auxiliary electrode side insulating support plate, the position of the X-ray transmission window (25) of the working electrode side insulating support plate and the position of the X-ray transmission window (29) of the auxiliary electrode side insulating support plate are all on the same horizontal line or are superposed, and an optical part is formed;
the position of the center of the optical part is on the same horizontal line or coincident with the position of the through hole part (34).
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| KR102538085B1 (en) * | 2021-04-30 | 2023-05-30 | 강원대학교산학협력단 | Electrochemical cells capable of x-ray analysis under practical operating conditions, including fuel cells |
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