An ultra-high loading copper monatomic catalyst, a preparation method thereof and an ethyne semi-hydrogenation application
By preparing a high-load supported copper single-atom catalyst, the problem of insufficient loading of copper-based catalysts was solved, achieving efficient acetylene reduction to ethylene and reducing by-product generation and cost.
Patent Information
- Application Number
- CN202411461827.2
- Authority / Receiving Office
- CN · China
- Patent Type
- Patents(China)
- Current Assignee / Owner
- Filing Date
- 2024-10-18
- Publication Date
- 2025-11-21
- Estimated Expiration
- 2044-10-18
AI Technical Summary
Existing copper-based single-atom catalysts are difficult to achieve high loading rates, which cannot meet the application requirements of acetylene reduction reactions. Furthermore, traditional thermocatalytic processes are energy-intensive and costly.
A polymeric carbon nitride support was prepared by calcining a nitrogen-containing precursor. After mixing with a copper precursor, the mixture was ultrasonicated, evaporated, and calcined to prepare a high-load supported copper single-atom catalyst. The support structure and metal distribution were optimized through multi-step calcination.
This method achieves highly selective catalytic conversion of acetylene to ethylene, reduces the formation of butadiene as a byproduct, improves the purity and atom utilization of ethylene, reduces costs, and meets the practical requirements of acetylene reduction reactions.
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Figure CN119186622B_ABST
Abstract
Description
TECHNICAL FIELD
[0001] The application belongs to the technical field of catalyst preparation, and more particularly relates to a super-high-loading copper monatomic catalyst, a preparation method thereof and an ethyne semi-hydrogenation application. BACKGROUND
[0002] Ethylene is a very important chemical raw material and an important commodity raw material for producing polymers such as polyethylene. However, about 0.5-3 % of ethyne is inevitably produced in the process of industrial production of ethylene, and these small amounts of ethyne can rapidly poison the Ziegler-Natta polymerization catalyst in the olefin polymerization process, greatly reducing the yield of the target polymer. Therefore, it is particularly important to purify industrial ethylene and remove ethyne impurities. At present, this goal is mainly achieved by the thermal catalytic hydrogenation of ethyne, but this reaction usually needs to be carried out at a relatively high temperature and pressure (~ 200℃, ~ 5bar); in addition, the large consumption of hydrogen and the high cost of palladium-based catalytic materials also increase the application cost of the reaction
[0003] The electrochemical ethyne reduction process based on clean and renewable energy driving has the characteristics of greenness and low energy consumption, and can avoid the participation of excess hydrogen by using water as a proton source, and is expected to replace the traditional thermal catalytic process. Copper monatomic catalysts have been widely used due to their low cost and high atomic utilization, but existing copper-based monatomic catalysts are difficult to achieve high loading, which cannot meet the application requirements. SUMMARY
[0004] To solve the problem that copper-based monatomic catalysts are difficult to achieve high loading in the prior art, the purpose of the present application is to provide a super-high-loading copper monatomic catalyst, a preparation method thereof and an ethyne semi-hydrogenation application. The monatomic catalyst has high loading and excellent catalytic performance in the electrocatalytic reduction of ethyne.
[0005] To achieve the above-mentioned purpose, the technical scheme adopted by the present application is as follows:
[0006] A preparation method of a super-high-loading supported copper monatomic catalyst, comprising the following steps:
[0007] The nitrogen-containing precursor is calcined to obtain a polymer carbon nitride;
[0008] The polymer carbon nitride is added to an ethanol dispersion solution of a copper precursor, ultrasonicated to obtain a mixed liquid, and evaporated to obtain a powder;
[0009] The powder is calcined under vacuum to obtain a high-loading supported copper monatomic catalyst.
[0010] A further improvement of the present application is that the nitrogen-containing precursor is dicyandiamide or melamine.
[0011] The further improvement of the present application is that the nitrogen-containing precursor is calcined under the following conditions: first calcined at 550-560 DEG C for 1-3h, then calcined at 500-510 DEG C for 5-7h, and repeated 3-4 times of calcination at 500-510 DEG C for 5-7h.
[0012] The further improvement of the present application is that the temperature is raised to 550-560 DEG C at a temperature raising rate of 1-3 DEG C per minute, and the temperature is raised to 500-510 DEG C at a temperature raising rate of 4-6 DEG C per minute. -1 -1
[0013] The further improvement of the present application is that the mass ratio of the polymer carbon nitride and the copper precursor is 0.05:0.0082-0.0571.
[0014] The further improvement of the present application is that the copper precursor is 1,5-cyclooctadiene copper chloride dimer or copper chloride.
[0015] The further improvement of the present application is that the powder is calcined under vacuum at a temperature of 450-460 DEG C for 1-2h.
[0016] The further improvement of the present application is that the temperature is raised to 450-460 DEG C at a temperature raising rate of 5 DEG C per minute. -1
[0017] A super-high-loading supported copper monatomic catalyst.
[0018] Application of a super-high-loading supported copper monatomic catalyst in electrocatalytic acetylene reduction reaction.
[0019] The present application provides application of the supported copper monatomic catalyst in electrocatalytic acetylene reduction reaction.
[0020] Compared with the prior art, the present application has the following beneficial effects:
[0021] This invention involves calcining a nitrogen-containing precursor to obtain polymeric carbon nitride, which is then mixed with a copper precursor, ultrasonicated, dried, and calcined to obtain a powder, yielding a high-load supported copper single-atom catalyst. The raw materials are widely available and easy to implement. The copper single-atom catalyst prepared by this invention is used for the electrocatalytic reduction of acetylene. The catalyst with the optimal material loading composition can highly selectively catalyze the C2H2→C2H4 reaction (achieving a C2H4 Faradaic efficiency >98%). Furthermore, the atomically dispersed metal sites suppress carbon-carbon coupling in the reaction. The Faradaic efficiency of butadiene can be reduced to below 0.5% across the entire tested current range. Compared to current nanoscale copper-based catalysts (butadiene Faradaic efficiency is generally 3%-10%), this significantly reduces butadiene formation during ethylene preparation and crude ethylene impurity removal, improves the purity of the target product ethylene, facilitates subsequent ethylene processing, greatly improves atom utilization, and saves costs. Attached Figure Description
[0022] Figure 1 X-ray powder diffraction (XRD) patterns of the catalysts prepared in Examples 1-5.
[0023] Figure 2 The image shows an aberration-corrected scanning transmission electron microscope (AC-STEM) image of the catalyst prepared in Example 3.
[0024] Figure 3 The X-ray absorption fine structure (EXAFS) spectra of the catalysts prepared in Examples 1-5 are shown below.
[0025] Figure 4 The catalysts prepared in Examples 1-5 were subjected to an amplitude of 100 mA cm⁻¹. -2 Faraday efficiency distribution under constant current test;
[0026] Figure 5 The image shows the Faraday efficiency distribution of the catalyst prepared in Example 3 using a flow cell as an electrolytic cell at different current densities.
[0027] Figure 6 The image shows data on the removal of impurities from a crude ethylene gas stream containing acetylene impurities using a membrane electrode as an electrolytic cell, as shown in Example 3. Detailed Implementation
[0028] To facilitate understanding of the present invention, a more complete description will be given below with reference to the accompanying drawings. Preferred embodiments of the invention are shown in the drawings. However, the invention can be implemented in many different forms and is not limited to the embodiments described herein. Rather, these embodiments are provided to provide a thorough and complete understanding of the disclosure of the invention.
[0029] The application discloses a preparation method of a super-high-loading supported copper monatomic catalyst.
[0030] S1: roasting a nitrogen-containing precursor to obtain a carrier polymeric carbon nitride; wherein the nitrogen-containing precursor includes but is not limited to dicyandiamide or melamine. The roasting is divided into multiple steps, the first step is roasting at a temperature of 550-560℃ for 1-3h, and the heating rate is 1-3℃·min -1 , the second step is roasting at a temperature of 500-510℃ for 5-7h, and the heating rate is 4-6℃·min -1 , and the second step is repeated for 3-4 times until the polymeric carbon nitride becomes white. After multiple calcinations, the polymeric carbon nitride carrier can be converted from a block to a nanosheet by simple thermal stripping, thereby increasing the specific surface area of the catalyst and providing more sites for loading metal.
[0031] S2: dispersing a copper precursor into anhydrous ethanol and ultrasonically treating for 10-30min to obtain a dispersion A; wherein the copper precursor includes but is not limited to 1,5-cyclooctadiene copper chloride dimer or copper chloride.
[0032] S3: adding the carrier prepared in S1 into the dispersion A and ultrasonically treating, and then performing rotary evaporation on the obtained mixture liquid to obtain a powder; wherein the rotary evaporation temperature is preferably 50℃, the rotation speed is 130rpm, and the application does not have special requirements on the rotary evaporation time, and the liquid in the mixture liquid can be evaporated to dryness.
[0033] S4: placing the powder obtained in S3 into a single-end opening quartz tube at a raw material end of the bottom, using a vacuum sealing machine to draw air, so that the air pressure in the tube is reduced to 10 -4 Pa, and then using a hydrogen oxygen machine to seal the tube.
[0034] S5: roasting to obtain a high-loading supported copper monatomic catalyst, wherein the roasting temperature is 450-460℃, the time is 1-2h, and the heating rate is 5℃·min -1 .
[0035] The super-high-loading supported copper monatomic catalyst prepared in the application includes a carrier and copper monatomic loaded on the carrier, and the mass of the copper monatomic is 5-35% of the mass of the catalyst.
[0036] The super-high-loading supported copper monatomic catalyst prepared in the application can be used for electrocatalytic acetylene reduction reaction.
[0037] The following are specific embodiments.
[0038] Embodiment 1
[0039] Burning the nitrogen-containing precursor to obtain a carrier polymer carbon nitride; wherein the nitrogen-containing precursor is dicyandiamide. The burning is divided into multiple steps, the first step is to burn at a temperature of 550 DEG C for 2 h, and the heating rate is 2.3 DEG C·min -1 , the second step is to burn at a temperature of 500 DEG C for 5 h, and the heating rate is 5 DEG C·min -1 , and the second step is repeated for 3 times until the polymer carbon nitride becomes white.
[0040] Put 0.0082 g of 1,5-cyclooctadiene copper chloride dimer and 30 mL of anhydrous ethanol in a 150 mL tomato bottle, mix thoroughly under ultrasonic for 10 min, then add 0.0500 g of polymer carbon nitride carrier, and ultrasonic for 20 min to obtain a mixed liquid; the mixed liquid is rotary evaporated at a rotary evaporation temperature of 50 DEG C and a rotation speed of 130 rpm to obtain a powder; the obtained powder is placed in the bottom of a single-end opening quartz tube, the gas pressure in the quartz tube is reduced to 10 -4 Pa by using a vacuum sealing machine, and then the quartz tube is sealed by using a hydrogen oxygen machine; the quartz tube is placed in a tube furnace, and calcined at 450 DEG C for 1 h with a heating rate of 5 DEG C·min -1 to obtain a copper monatomic catalyst with a mass content of 5 wt% loaded on the polymer carbon nitride substrate.
[0041] Example 2
[0042] Burning the nitrogen-containing precursor to obtain a carrier polymer carbon nitride; wherein the nitrogen-containing precursor is dicyandiamide. The burning is divided into multiple steps, the first step is to burn at a temperature of 550 DEG C for 2 h, and the heating rate is 2.3 DEG C·min -1 , the second step is to burn at a temperature of 500 DEG C for 5 h, and the heating rate is 5 DEG C·min -1 , and the second step is repeated for 3 times until the polymer carbon nitride becomes white.
[0043] Put 0.0082 g of 1,5-cyclooctadiene copper chloride dimer and 30 mL of anhydrous ethanol in a 150 mL tomato bottle, mix thoroughly under ultrasonic for 10 min, then add 0.0500 g of polymer carbon nitride carrier, and ultrasonic for 20 min to obtain a mixed liquid; the mixed liquid is rotary evaporated at a rotary evaporation temperature of 50 DEG C and a rotation speed of 130 rpm to obtain a powder; the obtained powder is placed in the bottom of a single-end opening quartz tube, the gas pressure in the quartz tube is reduced to 10 -4 Pa by using a vacuum sealing machine, and then the quartz tube is sealed by using a hydrogen oxygen machine; the quartz tube is placed in a tube furnace, and calcined at 450 DEG C for 1 h with a heating rate of 5 DEG C·min -1 to obtain a copper monatomic catalyst with a mass content of 5 wt% loaded on the polymer carbon nitride substrate.
[0044] Example 3
[0045] The nitrogen-containing precursor is dicyandiamide. The calcination is divided into multiple steps, the first step is 550℃ for 2h, the heating rate is 2.3℃·min -1 , the second step is 500℃ for 5h, the heating rate is 5℃·min -1 , and the second step is repeated for 3 times until the polymer carbon nitride becomes white.
[0046] 0.0408g 1,5-cyclooctadiene copper chloride dimer and 30mL of anhydrous ethanol were placed in a 150mL tomato bottle, mixed by ultrasonic for 10min, then 0.0500g of polymer carbon nitride carrier was added, and mixed by ultrasonic for 20min to obtain a mixed liquid; the mixed liquid was rotary evaporated at a rotary evaporation temperature of 50℃ and a rotation speed of 130rpm to obtain a powder; the obtained powder was placed in the bottom of a single-end opening quartz tube, the gas pressure in the quartz tube was reduced to 10 -4 Pa by using a vacuum sealing machine, and then the quartz tube was sealed using a hydrogen oxygen machine; the quartz tube was placed in a tube furnace and calcined at 450℃ for 1h with a heating rate of 5℃·min -1 to prepare a copper monatomic catalyst with a mass content of 25wt% loaded on the polymer carbon nitride substrate.
[0047] Example 4
[0048] The nitrogen-containing precursor is dicyandiamide. The calcination is divided into multiple steps, the first step is 550℃ for 2h, the heating rate is 2.3℃·min -1 , the second step is 500℃ for 5h, the heating rate is 5℃·min -1 , and the second step is repeated for 3 times until the polymer carbon nitride becomes white.
[0049] 0.0408g 1,5-cyclooctadiene copper chloride dimer and 30mL of anhydrous ethanol were placed in a 150mL tomato bottle, mixed by ultrasonic for 10min, then 0.0500g of polymer carbon nitride carrier was added, and mixed by ultrasonic for 20min to obtain a mixed liquid; the mixed liquid was rotary evaporated at a rotary evaporation temperature of 50℃ and a rotation speed of 130rpm to obtain a powder; the obtained powder was placed in the bottom of a single-end opening quartz tube, the gas pressure in the quartz tube was reduced to 10 -4 Pa by using a vacuum sealing machine, and then the quartz tube was sealed using a hydrogen oxygen machine; the quartz tube was placed in a tube furnace and calcined at 450℃ for 1h with a heating rate of 5℃·min -1 to prepare a copper monatomic catalyst with a mass content of 25wt% loaded on the polymer carbon nitride substrate.
[0050] Example 5
[0051] The nitrogen-containing precursor is dicyandiamide. The calcination is divided into multiple steps, the first step is 550℃ for 2h, the heating rate is 2.3℃·min -1 , the second step is 500℃ for 5h, the heating rate is 5℃·min -1 , and the second step is repeated 3 times until the polymer carbon nitride becomes white.
[0052] 0.0571g 1,5-cyclooctadiene copper chloride dimer and 30mL anhydrous ethanol are placed in a 150mL tomato bottle, mixed by ultrasonic for 10min, then 0.0500g polymer carbon nitride carrier is added, and mixed by ultrasonic for 20min to obtain a mixed liquid; the mixed liquid is rotary evaporated at a rotary evaporation temperature of 50℃ and a rotation speed of 130rpm to obtain a powder; the obtained powder is placed in the bottom of a single-end opening quartz tube, the gas pressure in the quartz tube is reduced to 10 -4 Pa by using a vacuum sealing machine, and then the quartz tube is sealed by using a hydrogen oxygen machine; the quartz tube is placed in a tube furnace, and heated at a heating rate of 5℃·min -1 to 450℃ for 1h to prepare a copper monatomic catalyst with a mass content of 35wt% loaded on the polymer carbon nitride substrate.
[0053] Example 6
[0054] The nitrogen-containing precursor is dicyandiamide. The calcination is divided into multiple steps, the first step is 555℃ for 2h, the heating rate is 3℃·min -1 , the second step is 505℃ for 6h, the heating rate is 5℃·min -1 , and the second step is repeated 3 times until the polymer carbon nitride becomes white. After multiple calcinations, the polymer carbon nitride carrier can be converted from a block to a nanosheet by simple thermal peeling, which increases the specific surface area of the catalyst and provides more sites for loading metals.
[0055] 0.0571g 1,5-cyclooctadiene copper chloride dimer and 30mL anhydrous ethanol are placed in a 150mL tomato bottle, mixed by ultrasonic for 10min, then 0.0500g polymer carbon nitride carrier is added, and mixed by ultrasonic for 20min to obtain a mixed liquid; the mixed liquid is rotary evaporated at a rotary evaporation temperature of 50℃ and a rotation speed of 130rpm to obtain a powder; the obtained powder is placed in the bottom of a single-end opening quartz tube, the gas pressure in the quartz tube is reduced to 10 -4 Pa by using a vacuum sealing machine, and then the quartz tube is sealed by using a hydrogen oxygen machine; the quartz tube is placed in a tube furnace, and heated at a heating rate of 5℃·min-1 The temperature was raised to 450℃ at a rate of 5℃ / min and calcined for 1h to prepare the copper monatomic catalyst.
[0056] Example 7
[0057] The nitrogen-containing precursor was calcined to obtain the carrier polymeric cubic carbon nitride; wherein the nitrogen-containing precursor was melamine. The calcination was divided into multiple steps, the first step was calcined at 560℃ for 1h, the temperature was raised at a rate of 1℃ / min -1 , the second step was calcined at 510℃ for 5h, the temperature was raised at a rate of 4℃ / min -1 , and the second step was repeated 4 times until the polymeric cubic carbon nitride turned white. After multiple calcinations, the polymeric cubic carbon nitride carrier could be converted from bulk to nanosheet by simple thermal exfoliation, which increased the specific surface area of the catalyst and provided more sites for metal loading.
[0058] 0.0082g of 1,5-cyclooctadiene copper chloride dimer and 30mL of anhydrous ethanol were placed in a 150mL tomato bottle, mixed by ultrasonic for 10min, then 0.0500g of the polymeric cubic carbon nitride carrier was added, and the mixture was ultrasonically mixed for 20min; the mixture was rotary evaporated at a rotary evaporation temperature of 50℃ and a rotation speed of 130rpm to obtain a powder; the obtained powder was placed at the raw material end of the bottom of a single-end opening quartz tube, the gas pressure in the quartz tube was reduced to 10 -4 Pa by using a vacuum sealing machine, and then the quartz tube was sealed using a hydrogen machine; the quartz tube was placed in a tube furnace, and the temperature was raised at a rate of 5℃ / min -1 to 460℃ and calcined for 1h to prepare the copper monatomic catalyst.
[0059] Example 8
[0060] The nitrogen-containing precursor was calcined to obtain the carrier polymeric cubic carbon nitride; wherein the nitrogen-containing precursor was melamine. The calcination was divided into multiple steps, the first step was calcined at 560℃ for 1h, the temperature was raised at a rate of 1℃ / min -1 , the second step was calcined at 510℃ for 5h, the temperature was raised at a rate of 4℃ / min -1 , and the second step was repeated 4 times until the polymeric cubic carbon nitride turned white. After multiple calcinations, the polymeric cubic carbon nitride carrier could be converted from bulk to nanosheet by simple thermal exfoliation, which increased the specific surface area of the catalyst and provided more sites for metal loading.
[0061] Put 0.0082g copper chloride and 30mL anhydrous ethanol in a 150mL tomato bottle, mix thoroughly under ultrasonic for 10min, then add 0.0500g polymer carbon nitride carrier, mix thoroughly under ultrasonic for 20min to obtain a mixed liquid; the mixed liquid is rotary evaporated at a rotary evaporation temperature of 50℃ and a rotation speed of 130rpm to obtain a powder; the obtained powder is placed in the bottom of a single-end opening quartz tube, and a vacuum sealing machine is used to draw air to make the air pressure in the quartz tube drop to 10 -4 Pa, and then the quartz tube is sealed with hydrogen and oxygen; the quartz tube is placed in a tube furnace, and the temperature is raised at a rate of 5℃·min -1 -1 to 455℃ and calcined for 2h to prepare a copper monatomic catalyst.
[0062] Characterization of examples 1-5:
[0063] Referring to Figure 1 and Figure 2 , the XRD spectrum and the TEM diagram do not detect or observe Cu-related nanoparticles. The AC-STEM diagram further proves the formation of Cu monatomic atoms, which are uniformly dispersed in the carrier.
[0064] Referring to Figure 4 , it can be seen that example 3 has the best catalytic activity, and a high load of monatomic catalyst has practical significance.
[0065] Application experiment:
[0066] The electrochemical performance detection of the application is carried out on a CHI 760e (Shanghai Chenhua Instrument Co., Ltd.) electrochemical workstation, the pure acetylene activity test uses a flow cell as an electrolytic cell, C2H2 (99.999%) gas as a reaction gas, 1mol·L -1 -1 KOH as an electrolyte, and an anion membrane is used to separate the cathode chamber and the anode chamber, and Hg / HgO and foamed nickel are used as the reference electrode and the counter electrode respectively; the impurity removal test of the crude ethylene gas stream containing acetylene uses a membrane electrode (MEA) as an electrolytic cell, a crude ethylene mixed gas (0.5% C2H2, 20% C2H4, Ar filling) as a reaction gas, 1mol·L -1 -1 KOH as an electrolyte, and an anion membrane is used to separate the cathode chamber and the anode chamber, and foamed nickel is used as the counter electrode. The working electrode is prepared as follows:
[0067] 3mg of the catalyst prepared in example 3 is uniformly dispersed in a mixture of isopropanol (600μL) and 5% nafion solution (4μL), and ultrasonic is used for 30min; then 200μL of the catalyst ink is sprayed on a gas diffusion layer YLS30T carbon paper (1×1cm) using a gas brush, and a copper monatomic atom catalyst working electrode is obtained after natural drying.
[0068] The gas flow rate was controlled by a mass flow meter in the specific test. The product content was detected by a gas chromatograph in a continuous constant current mode, and a FID detector was used to detect C2H2, C2H4, C2H6 and butadiene, and a TCD detector was used to detect H2.
[0069] Referring to Figure 5 It can be seen that the catalyst can inhibit the generation of C4 products while efficiently generating ethylene (Faraday efficiency < 0.5%).
[0070] Table 1 is the copper monatomic ICP test data of the catalyst prepared in Examples 1-5
[0071]
[0072] The present application details the preparation method of the catalyst and its practical effect in the application of acetylene hydrogenation to prepare ethylene and acetylene removal in acetylene-ethylene mixed gas. The present application can obtain a super-high load supported copper monatomic catalyst, which can better meet the actual application requirements, and the raw materials are widely available and easy to implement.
[0073] The above only describes the best embodiments of the present application, but cannot be understood as a limitation on the claims. The present application is not limited to the above embodiments, and the specific structure allows changes. Any changes made within the protection scope of the independent claims of the present application are within the protection scope of the present application.
[0074] Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which the present application belongs. The terms used in the specification of the present application are only for the purpose of describing the specific embodiments and are not intended to limit the present application. The term "and / or" used herein includes any and all combinations of one or more related listed items.
Claims
1. The application of an ultra-high loading copper single-atom catalyst in the electrocatalytic reduction of acetylene, characterized in that, The preparation method of the ultra-high loading supported copper single-atom catalyst includes the following steps: The nitrogen-containing precursor is calcined to obtain polymer carbon nitride; wherein the nitrogen-containing precursor is dicyandiamide or melamine, and the calcination conditions of the nitrogen-containing precursor are: first calcining at 550-560℃ for 1-3h, then calcining at 500-510℃ for 5-7h, and repeating the step of calcining at 500-510℃ for 5-7h 3-4 times. The polymer carbon nitride was added to the ethanol dispersion of the copper precursor, ultrasonicated to obtain a mixed liquid, and then evaporated to obtain a powder. The powder was calcined under vacuum to obtain a high-loading supported copper single-atom catalyst.
2. The application of the ultra-high loading supported copper single-atom catalyst according to claim 1 in the electrocatalytic reduction of acetylene, characterized in that, In the calcination step of the nitrogen-containing precursor, the temperature is 1-3℃·min. -1 The temperature was increased to 550-560℃ at a heating rate of 4-6℃·min. -1 The heating rate is increased to 500-510℃.
3. The application of the ultra-high loading supported copper single-atom catalyst according to claim 1 in the electrocatalytic acetylene reduction reaction, characterized in that, The mass ratio of polymeric carbon nitride to copper precursor is 0.05:0.0082-0.0571.
4. The application of the ultra-high loading supported copper single-atom catalyst according to claim 1 in the electrocatalytic acetylene reduction reaction, characterized in that, The copper precursor is a 1,5-cyclooctadiene copper chloride dimer or copper chloride.
5. The application of the ultra-high loading supported copper single-atom catalyst according to claim 1 in the electrocatalytic reduction of acetylene, characterized in that, The powder is calcined under vacuum at a temperature of 450-460℃ for 1-2 hours.
6. The application of the ultra-high loading supported copper single-atom catalyst according to claim 5 in the electrocatalytic reduction of acetylene, characterized in that, In the calcination step of the powder, at 5℃·min -1 The heating rate is increased to 450-460℃.
Citation Information
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