CN115959648A - Simple preparation method of high-defect carbon film and application of high-defect carbon film in CO2 reduction flow cell - Google Patents
Simple preparation method of high-defect carbon film and application of high-defect carbon film in CO2 reduction flow cell Download PDFInfo
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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- Y02E60/30—Hydrogen technology
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Abstract
The invention provides a simple preparation method of a high-defect carbon film and application thereof in CO 2 Application in reduction flow cell, belongs to electrocatalysis CO 2 The technical field of reduction, wherein the preparation method comprises the steps of carrying out low-temperature pre-carbonization and high-temperature carbonization on wood veneer to obtain an integral carbon film material, and then adopting CO 2 The gas etches the carbon material, causing it to produce carbon defects that can be used directly as effective catalytically active sites. The prepared high-defect carbon film has stronger mechanical stability and abundant carbon defect active sites, can be directly used as a working electrode, and is convenient for large-scale production of catalyst electrodes. Meanwhile, the high-defect carbon film material can be applied to a flow cell reaction system for electrocatalysis of CO 2 Reduction, relying only on carbon defect sitesThe high Faraday efficiency and current density of the CO product can be obtained, and after 9h stability test, the retention rate of the Faraday efficiency of CO is still 84.5%, and the product has long-time operation capability and good stability.
Description
Technical Field
The invention belongs to electrocatalysis of CO 2 The technical field of reduction, in particular to a simple preparation method of a high-defect carbon film and application thereof in CO 2 Reduction of the use in flow cells.
Background
The defect sites in the structure of the defect carbon-based material greatly influence the physicochemical characteristics of the defect carbon-based material, and due to the change of the surface charge state, the change of the adsorption free energy of the intermediate and the reduction of the band gap, the carbon defect sites not only can anchor the catalyst sites, but also can be directly used as active sites for catalytic reaction, so that the defect carbon-based material electrocatalyst attracts the wide attention of people.
Most of the existing defect carbon-based catalysts mostly use carbon black, graphene or other biomass derived carbon materials as carbon sources, and the defect production mode in the preparation process mainly comprises K + Removing N element and CO by high-temperature roasting after etching and nitriding 2 The modes of gas high-temperature etching and the like are mainly adopted, and the prepared defect carbon-based catalyst is mainly made of powdery materials. The powdery defective carbon-based catalyst cannot be directly used as an electrode, and needs to be ultrasonically dispersed in an ethanol solution together with a binder to prepare slurry, and then the slurry is coated on the surface of carbon paper to prepare a working electrode, so that the process is complex, the production cost is increased, and the loss of active sites can be caused by the falling of the catalyst in the long-time catalytic reaction process, and the large-scale popularization and application are difficult.
In addition, the defective carbon-based materials are currently used to electrocatalyze CO 2 The reduction was essentially tested in a type H reactor, where mass transfer would severely limit CO 2 The rate of the reduction reaction. The flow cell breaks through the mass transfer limit of the H-shaped reaction cell, so that CO is generated 2 The reduction current density is effectively improved, but at present, the defect carbon-based catalyst is not applied to a flow cell for electrocatalysis of CO 2 Precedent of reduction.
Disclosure of Invention
In view of the above, the present invention provides a simple method for preparing a high defect carbon film by combining two carbonization steps with CO 2 The high-defect carbon film is obtained by high-temperature gas etching, has stronger mechanical stability and abundant carbon defect active sites, can be directly used as a working electrode, and is convenient for large-scale production of a catalyst electrode.
The invention also provides the application of the high-defect carbon film in electrocatalysis of CO 2 Reduction of the use in flow cells.
The technical scheme adopted by the invention for solving the technical problems is as follows:
a simple preparation method of a high-defect carbon film comprises the following steps:
(1) Cutting raw basswood into slices with a preset size along the direction vertical to the growth direction, putting the cut thin wood slices into a muffle furnace, firstly carrying out low-temperature pre-carbonization in the air atmosphere, then carrying out high-temperature carbonization in the Ar atmosphere, and carrying out post-treatment on the carbonized product to obtain a carbon film CW;
(2) Placing CW in a corundum boat, placing the corundum boat in the center of an atmosphere tube furnace, roasting by adopting high-purity Ar, and switching gas into CO in the heat preservation process 2 And (4) gas, wherein the rest process is Ar atmosphere, so as to obtain the high-defect carbon film CW-HD.
Preferably, in the step (1), the pre-carbonization temperature is 250-270 ℃, the time is 5.5-6.5h, the carbonization temperature is 950-1050 ℃, the time is 5.5-6.5h, the gas flow rate is 40mL/min, and the heating rates of the two carbonization steps are both 4-5 ℃/min.
Preferably, in the step (1), the post-treatment step comprises sequentially sanding the carbonized product with sand paper, ultrasonically cleaning the product with water and ethanol, and then drying the product in a vacuum oven overnight.
Preferably, in the step (2), the temperature of the tubular furnace is set to be 700-800 ℃, the temperature is kept for 2.5-3.5h, the gas flow rate is 40mL/min, and the temperature rise rate is 4-5 ℃/min.
The high-defect carbon film prepared by the method is used for electrocatalysis of CO 2 Reduction of the use in flow cells.
Preferably, when in application, the high-defect carbon film CW-HD is placed on a 65-75 ℃ heating plate, a PTFE emulsion with the concentration of 14-16mg/mL is sprayed on one side of a whole electrode, 50 mu L of PTFE emulsion is sprayed each time, the next spraying is carried out after drying, 0.5mL of PTFE emulsion is sprayed in a cumulative mode, a hydrophobic layer is formed after drying, then a piece of hydrophobic carbon paper is added on the airflow side to be used as a gas diffusion layer to be directly assembled into a flow cell for testing, 1MKOH is used as an electrolyte in the flow cell testing process, nifoam and Ag/AgCl electrodes are respectively used as a counter electrode and a reference electrode, and an anode and a cathode are separated by an anion exchange membrane.
According to the technical scheme, the invention provides a simple preparation method of a high-defect carbon film and application of the high-defect carbon film in CO 2 The application in the reduction flow cell has the advantages that: firstly, the veneer is pre-carbonized at low temperature and carbonized at high temperature to obtain an integral carbon film material, the two carbonization processes improve the crystallization degree and the electrical conductivity of the carbon material on the one hand and form a developed pore channel structure in the carbon material on the other hand, the hierarchical porous structure is favorable for rapid mass transfer and can provide larger specific surface area for catalytic reaction, and further more carbon defect catalytic active sites for electrocatalysis of CO 2 Reduction and then by using CO 2 The gas etches the carbon material, causing it to produce carbon defects that can be used directly as effective catalytically active sites. The high-defect carbon film prepared by the invention is of a blocky integral structure and has strong mechanical stability, so that when the high-defect carbon film is used as an electrode, a binder and a conductive additive are not needed, and slurry preparation for coating is not needed, so that the high-defect carbon film can be directly tested, the preparation process is simple, and the large-scale production, popularization and application of the working electrode are facilitated.
Meanwhile, the invention applies the high-defect carbon film material to the flow cell reaction system for electrocatalysis of CO for the first time 2 And (4) reducing. The high-defect carbon film is subjected to hydrophobic treatment to obtain a high-defect carbon film gas diffusion electrode, a flowing pool system is further assembled for testing, test results show that the high-defect carbon film can obtain high Faraday efficiency and current density of CO products only by virtue of carbon defect sites, and after 9h stability test, the retention rate of the Faraday efficiency of CO is still 84.5%, which shows that the high-defect carbon film has long-time operation capability and good stability. In addition, since the electrodes of the monolithic structure are catalysts, the CO is electrocatalyzed 2 After the reduction reaction for a long time, can be directly recycled.
Drawings
FIG. 1 is a topographical analysis of a high defect carbon film.
Fig. 2 is a result of composition analysis of the high-defect carbon film.
Fig. 3 is a contact angle test result after a hydrophobic treatment of a high defect carbon film.
FIG. 4 is a high defect carbon film on CO 2 And (4) reducing the catalytic performance test result of the flow cell.
FIG. 5 shows the formation of a high defect carbon film in CO 2 Results of catalytic stability testing of the reduction flow cell.
Detailed Description
The technical solutions and effects of the embodiments of the present invention will be further described in detail below with reference to the accompanying drawings of the present invention.
The invention provides a simple preparation method of a high-defect carbon film, which comprises the following steps:
(1) Cutting raw basswood into slices with a preset size along the direction vertical to the growth direction, putting the cut thin wood slices into a muffle furnace, firstly carrying out low-temperature pre-carbonization in the air atmosphere, then carrying out high-temperature carbonization in the Ar atmosphere, and carrying out post-treatment on the carbonized product to obtain a carbon film CW;
in a specific embodiment, native basswood is cut into slices with the size of 3.5cm multiplied by 2.2cm multiplied by 2.0mm along the direction vertical to the growth direction, the cut slices are placed in a muffle furnace, the temperature is set to be 260 ℃, the pre-carbonization is carried out for 6h under the air atmosphere, then the carbonization is carried out for 6h under the Ar atmosphere in a tube furnace, the gas flow rate is 40mL/min, the temperature is set to be 1000 ℃, and the heating rate of the two-step operation is set to be 5 ℃/min; and the post-treatment step comprises the steps of sequentially polishing the carbonized product by using sand paper, ultrasonically cleaning the carbonized product by using water and ethanol, and then drying the product in a vacuum oven overnight, wherein the temperature of the oven is set to be 60 ℃. The wood veneer is carbonized into a carbon material with hierarchical porosity by controlling the temperature and the carbonization time of the two carbonization processes, the degree of crystallization is high, and the conductivity of the material is improved.
(2) Placing CW in a corundum boat, placing the corundum boat in the center of an atmosphere tube furnace, roasting by adopting high-purity Ar, and switching gas into CO in the heat preservation process 2 And (4) gas, wherein the rest process is Ar atmosphere, so as to obtain the high-defect carbon film CW-HD.
In a specific embodiment, the CW is put in a tube furnace, the temperature of Ar atmosphere is raised to 750 ℃, the roasting is carried out for 3 hours, the gas flow rate is 40mL/min, and the gas is switched into CO in the heat preservation process 2 And the rest process is Ar atmosphere, thus obtaining the high-defect carbon film CW-HD. By CO 2 And etching the carbon material CW by the gas to generate carbon defects, and adjusting the defect density of the carbon material by controlling the temperature rise temperature at 750 ℃, the roasting time for 3h and the gas flow rate at 40mL/min in the etching process to obtain the carbon material with the surface rich in defect sites.
Referring to fig. 1, the morphology of the high-defect carbon film is analyzed by SEM and TEM, and fig. 1a is a SEM picture of a three-dimensional structure of CW-HD, which shows that CW-HD has a three-dimensional porous structure; FIG. 1b is a top view of SE M showing that CW-HD has many open microchannels with pore size of 2-50 μ M; FIG. 1c is a side view of SEM showing CW-HD with a through, developed tunnel structure; FIG. 1d is a TEM image showing the presence of significant defects on the CW-HD surface, wherein the inserted SAED image shows diffuse diffraction rings with low crystallinity, further corroborating the presence of defects; fig. 1e is an HRTEM picture, which shows that the lattice fringes are arranged in a short-range, ordered manner, which may assist in the presence of defects. The morphology analysis result shows that the surface of the carbon film has defects.
Referring to fig. 2, the structure of the sample was analyzed by X-ray diffraction (XRD). Fig. 2a is an XRD result, which shows that CW-HD has only diffraction peaks of carbon, and no diffraction peaks of metal or other heteroatoms appear, indicating that the active sites for subsequent catalysis are carbon materials, and excluding the interference of other heteroatoms. FIG. 2b shows the results of Raman spectroscopy, in which D-peak and G-peak are both Raman characteristic peaks of a C atom crystal, D-peak represents a defect of a C atom lattice, G-peak represents in-plane stretching vibration of sp2 hybridization of a C atom, and I D /I G Is the ratio of the intensities of the D-peak and the G-peak, and the larger this ratio, the more defects are represented inside the carbon material. It can be seen that in the present invention, I D /I G The increase from 1.05 for CW to 1.24 for CW-HD indicates that CW-HD has a larger number of carbon defects than CW. Fig. 2c shows an EPR mode, and a strong signal of CW-HD around g =2.0 can be observed, further demonstrating that there are a large number of carbon defects on CW-HD. FIG. 2d is a fine XPSN1s spectrum picture, which shows that no N element exists in the interior of the CW-HD material, and the influence of the N element on the catalytic activity of the CW-HD electrode can be eliminated. From the above characterization, it can be demonstrated that the CW-HD material has a large sizeCarbon deficiency, absence of other heteroatoms, indicating electrocatalytic CO 2 The catalytically active sites in the reduction process are defect carbons.
The invention also provides a high-defect carbon film prepared by the method in CO 2 Reducing the application in the flow cell, during specific application, placing CW-HD with the specification of 2.5cm multiplied by 1.0mm on a heating plate at 70 ℃, spraying 15mg/mL PTFE emulsion on one side of an integral electrode, spraying 50 mu L each time, carrying out next spraying after drying, forming a hydrophobic layer after accumulative spraying of 0.5mL and drying, then attaching a piece of hydrophobic carbon paper to the gas side to be used as a gas diffusion layer, and then directly assembling the flow cell for testing; in the flow cell test process, 1MKOH is used as electrolyte, nifoam and Ag/AgCl electrodes are respectively used as a counter electrode and a reference electrode, and an anode and a cathode are separated by an anion exchange membrane.
Referring to fig. 3, contact angle measurements were made on CW-HD after hydrophobic treatment. Placing the CW-HD sample on a horizontal glass plate, dripping a drop of 1MKOH vertically by a needle cylinder, standing for 30s, and calculating a contact angle (included angle at a solid-liquid-gas three-phase interface) after the state of the drop is completely stable. As shown in fig. 3a, the included angle of the liquid drop on the gas-repellent side of the sample is 137 °, which indicates that the gas-repellent requirement on the gas-side of the gas diffusion electrode can be satisfied; FIG. 3b shows the side without hydrophobic treatment and the included angle is 9 degrees, which shows that the hydrophilic electrolyte has good hydrophilicity and can well transfer mass with the electrolyte. The CW-HD gas diffusion electrode can fully satisfy the conditions of the gas diffusion electrode.
With reference to FIG. 4, a CW-HD gas diffusion electrode was successfully assembled into a flow cell system for testing, in which FE is shown co Is the Faraday efficiency of CO, j co Is the CO current density. It can be seen that CW-HD at-0.35Vvs. RHE, CO Faraday efficiency as high as 79.2%, with increasing potential, CO current density increasing with increasing CO current density at-0.72Vvs. RHE, with CO current density as high as 45.92mA cm -2 At this time, the CO Faraday efficiency still reaches 59.3%.
Referring to FIG. 5, a stability test was performed for a CW-HD gas diffusion electrode at-0.79Vvs. RHE current density for a duration of 9h, j Total As total current density, FE co For CO Faraday efficiency, FE H2 Is H 2 Faraday effectAnd (4) rate. The total current density increased from 71.52mA cm with the increase of the polarization time -2 Reduced to 66.46mA cm -2 And the retention rate of the Faraday efficiency of CO is still 84.5%, so that the capability of long-time operation and good stability can be proved.
While the invention has been described in connection with what is presently considered to be the most practical and preferred embodiment, it is to be understood that the invention is not to be limited to the disclosed embodiment, but on the contrary, is intended to cover various modifications and equivalent arrangements included within the spirit and scope of the appended claims.
Claims (6)
1. A simple preparation method of a high-defect carbon film is characterized by comprising the following steps: the method comprises the following steps:
(1) Cutting raw basswood into slices with a preset size along the direction vertical to the growth direction, putting the cut thin wood slices into a muffle furnace, firstly carrying out low-temperature pre-carbonization in the air atmosphere, then carrying out high-temperature carbonization in the Ar atmosphere, and carrying out post-treatment on the carbonized product to obtain a carbon film CW;
(2) Placing CW in a corundum boat, placing the corundum boat in the center of an atmosphere tube furnace, roasting by adopting high-purity Ar, and switching gas into CO in the heat preservation process 2 And (4) gas, wherein the rest process is Ar atmosphere, so as to obtain the high-defect carbon film CW-HD.
2. The simple method for producing a high-defect carbon film according to claim 1, wherein: in the step (1), the pre-carbonization temperature is 250-270 ℃, the time is 5.5-6.5h, the carbonization temperature is 950-1050 ℃, the time is 5.5-6.5h, the gas flow rate is 40mL/min, and the heating rates of the two-time carbonization are both 4-5 ℃/min.
3. The simple method for producing a high-defect carbon film according to claim 1, wherein: in the step (1), the post-treatment step comprises the steps of sequentially polishing the carbonized product by using sand paper, ultrasonically cleaning the carbonized product by using water and ethanol, and then drying the product in a vacuum oven overnight.
4. The simple method for producing a high-defect carbon film according to claim 1, wherein: in the step (2), the temperature of the tubular furnace is set to be 700-800 ℃, the temperature is kept for 2.5-3.5h, the gas flow rate is 40mL/min, and the heating rate is 4-5 ℃/min.
5. The method for preparing the high-defect carbon film according to claim 1 by the simple method for preparing the high-defect carbon film, wherein the high-defect carbon film is used for electrocatalysis of CO 2 Reduction of the use in flow cells.
6. The high defect carbon film of claim 5 in CO 2 Use in a reduction flow cell, characterized in that: when in application, the high-defect carbon film CW-HD is placed on a heating plate at 65-75 ℃, PTFE emulsion of 14-16mg/mL is sprayed on one side of an integral electrode, 50 mu L of PTFE emulsion is sprayed each time, the next spraying is carried out after drying, 0.5mL of PTFE emulsion is sprayed in an accumulated mode, a hydrophobic layer is formed after drying, then a piece of hydrophobic carbon paper is added on the airflow side and is used as a gas diffusion layer to be directly assembled into a flow cell for testing, 1M KOH is used as electrolyte in the flow cell testing process, ni foam and Ag/AgCl electrodes are respectively used as a counter electrode and a reference electrode, and an anode and a cathode are separated by an anion exchange membrane.
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