Electrocatalyst high-throughput screening platform for electrocatalytic reaction systems and methods thereof

Abstract

The application discloses an electrocatalyst high-throughput screening platform for an electrocatalytic reaction system and a method thereof. The platform takes a flow electrolytic cell and a high-throughput pipetting workstation as cores, and integrates gas chromatography (GC) and nuclear magnetic resonance (NMR) rapid product analysis. The platform adopts an aluminum alloy gantry four-axis (XYZ1Z2) moving mechanism to realize spatial positioning of clamping and pipetting. The high-throughput pipetting workstation provides a gun head storage module, a reagent bottle storage module, a rotating bottle cap module and an electrocatalyst preparation module to realize accurate liquid proportioning and electrocatalyst preparation. The electrochemical test workstation is internally provided with a flow electrolytic cell and the like to realize continuous flow electrolysis, automatic sampling and electrolyte circulation. The GC / NMR module realizes online rapid detection of products. The platform realizes unattended, repeatable catalyst preparation and high-throughput screening of the whole process through unified control of a circuit and an upper computer. The electrocatalytic reaction system is a carbon dioxide reduction reaction system.

Description

Technical Field

[0001] This invention belongs to the field of laboratory automation technology, specifically relating to a high-throughput screening platform and method for electrocatalysts in electrocatalytic reaction systems. The platform, centered on a flow electrolyzer and a high-throughput pipetting workstation, integrates rapid product analysis using gas chromatography (GC) and nuclear magnetic resonance (NMR). Background Technology

[0002] Electrocatalytic reaction systems can achieve catalytic conversion of reactants under electrochemical conditions such as applied potential or current, and have wide applications in energy conversion, chemical synthesis, and environmental remediation. Represented by the electroreduction of carbon dioxide (CO2), the widespread use of fossil fuels has led to a continuous increase in atmospheric CO2 emissions, causing problems such as global warming and environmental pollution. Electrically driven CO2 reduction (CO2RR) has become an important electrocatalytic conversion pathway due to its mild, clean, and controllable characteristics. Thermodynamic analysis shows that CO2RR can produce various products such as CO, CH4, C2H4, HCOOH, and C2H5OH, among which ethylene (C2H4) and ethanol (C2H5OH) have attracted attention due to their industrial demand and market value.

[0003] Achieving efficient CO2RR requires high-throughput screening of a large number of electrocatalysts. Mixing techniques (such as solution preparation, emulsification, and dispersion) are used in the laboratory to mix and prepare catalyst precursors, while electrolytic cells provide the electrochemical reaction environment. To achieve rapid and accurate product detection, gas chromatography (GC) and nuclear magnetic resonance (NMR) have become core methods for online, real-time qualitative and quantitative analysis.

[0004] In modern laboratories, automation has become a key means to improve experimental reliability and reduce human error. With the rapid development of electronic information technology and computers, thin-film handling technology and mechanical positioning and clamping mechanisms are widely used to realize high-throughput pipetting workstations and robotic gripping / handling, enabling rapid sample loading, application, and retrieval, ensuring high precision, stability, and efficiency in experimental processes. Laboratory automation not only significantly improves data reproducibility and reduces random errors, but also frees researchers from tedious, low-skill operations, allowing them to focus on data analysis, mechanistic interpretation, and the exploration of new chemical systems.

[0005] In summary, combining mixing technology, electrochemical methods, flow electrolysis devices, and online analysis techniques, and achieving high-throughput, fully automated electrocatalyst screening through transport methods, is the optimal solution for constructing a reliable, large-scale electrocatalyst database. In a preferred embodiment, using a carbon dioxide reduction reaction system as the target system, this platform can rapidly screen catalyst systems exhibiting high target product Faradaic efficiencies at industrial-grade current densities. Summary of the Invention

[0006] The purpose of this invention is to overcome the shortcomings of the prior art and provide a high-throughput screening platform and method for electrocatalysts in electrocatalytic reaction systems, so as to realize the automated preparation, automated sample loading and testing and online product analysis of electrocatalysts, and improve the consistency, repeatability and data output efficiency of experiments.

[0007] The "electrocatalytic reaction system" described in this invention refers to a reaction system in which reactants undergo electrocatalytic transformation in an electrolytic cell under electrochemical conditions such as applied potential or current; the reactants and products can be in the gas phase and / or liquid phase, and the electrolyte can be an aqueous or non-aqueous electrolyte. In a preferred embodiment, the electrocatalytic reaction system is a carbon dioxide reduction reaction system.

[0008] The technical solution adopted by the present invention to solve its technical problem is: to provide a high-throughput screening platform for electrocatalysts in electrocatalytic reaction systems, including a four-axis moving mechanism, a high-throughput liquid transfer workstation, an electrochemical testing workstation, control circuits and host computer software;

[0009] The four-axis moving mechanism adopts a gantry structure, where the x-axis and y-axis are used for planar positioning, the Z1 axis is connected to a clamping mechanism, and the Z2 axis is connected to a pipetting mechanism. The high-throughput pipetting workstation is equipped with a catalyst preparation module and an electrolyte addition mechanism. The electrochemical testing workstation includes a flow electrolytic cell and a product detection module. The high-throughput pipetting workstation supplies catalyst samples and electrolyte to the flow electrolytic cell through the four-axis moving mechanism. The host computer software communicates with the four-axis moving mechanism, the high-throughput pipetting workstation, and the electrochemical testing workstation through the control circuit to achieve automatic linkage control of electrocatalyst preparation, sample loading and testing, and product detection.

[0010] In a preferred embodiment of the present invention, the platform includes an aluminum alloy panel, and the four-axis moving mechanism is disposed on the aluminum alloy panel; the working stroke of the four-axis moving mechanism includes the high-throughput liquid transfer workstation, and at least includes the interface required for the electrocatalyst pick-up, drop-off and liquid addition operations in the electrochemical testing workstation.

[0011] In a preferred embodiment of the present invention, the clamping mechanism includes a rotating jaw, a rotating jaw connector, and a rotating jaw fixture, which can accommodate all solid samples inside the platform.

[0012] In a preferred embodiment of the present invention, the pipetting mechanism includes a universal pipette tip connector, a pipette tip, and an electric push rod. The electric push rod pushes the universal pipette tip connector to retract the pipette tip (1mL pipette tip).

[0013] In a preferred embodiment of the present invention, the high-throughput pipetting workstation includes a pipette tip storage module (accommodating 60 1mL pipette tips and corresponding gripping structures), a waste container (for recycling used pipette tips), a reagent bottle storage module (containing 48 cathode electrolyte bottle positions, 8 anolyte bottle positions, and 24 functional molecule solution bottle positions), a bottle cap storage module (accommodating 12 bottle caps for temporary storage of opened bottle caps), an electrolyte dispensing mechanism, a catalyst preparation module, and a bottle cap rotating module.

[0014] In a preferred embodiment of the present invention, the electrolyte adding mechanism is mounted on the platform via a adding mechanism base, and the adding mechanism base is provided with a liquid channel connected to the electrolyte storage tank (which can add 16.5 mL of liquid to the reagent bottle at one time).

[0015] In a preferred embodiment of the present invention, the catalyst preparation module includes a first cap storage area, a second cap storage area, a solution suction mechanism, a hot stage, a metal layer on the hot stage (used to expand the heating area and achieve uniform heating of the prepared monomer), an upper layer of the catalyst preparation module, a lower layer of the catalyst preparation module, and a cover for the preparation area. A detachable covered preparation area monomer is installed in the upper layer of the catalyst preparation module, and the metal layer on the hot stage is fixed to the surface of the hot stage.

[0016] In a preferred embodiment of the present invention, the rotating bottle cap module includes an elastic platform base, a linear guide rail is vertically arranged on the elastic platform base, a parallel gripper plate is mounted on the linear guide rail, a connecting spring is provided between the bottom of the parallel gripper plate and the elastic platform base, and the parallel gripper plate is equipped with parallel grippers to realize the three-turn rotation opening and automatic reset of the bottle cap.

[0017] In a preferred embodiment of the present invention, the electrochemical testing workstation includes a suction cup mechanism, a catalyst loading mechanism, a catalyst transport mechanism, an electrolyte transport mechanism, a flow electrolytic cell, and a hydraulic control mechanism; the product detection module includes a gas chromatography detection module and a nuclear magnetic resonance detection module.

[0018] In a preferred embodiment of the present invention, the flowing electrolytic cell realizes continuous flowing electrolysis and can be closed / opened, including an electrolytic cell bottom plate, a closure device back plate and a closure device for achieving sealing, and a gas chamber, a cathode chamber and an anode chamber are provided in the sealed cavity for electrocatalytic reaction; the cathode chamber and the anode chamber are connected to a pumping system for circulating pumping liquid.

[0019] In a preferred embodiment of the present invention, the pumping system includes a first and a second peristaltic pump and a connecting plate respectively connected to the cathode chamber and the anode chamber, and the flow rates of the first and second peristaltic pumps of the pumping system can be adjusted independently.

[0020] In a preferred embodiment of the present invention, the suction cup mechanism includes a first suction cup for moving the catalyst to be tested, a second suction cup for moving the catalyst already tested, and a suction cup storage mechanism.

[0021] In a preferred embodiment of the present invention, the catalyst loading mechanism includes a rotating disk, the rotating disk having at least four catalyst placement mechanisms at equal angles, the surface of the catalyst placement mechanism being provided with grooved silicone pads, and the outer periphery of the rotating disk being provided with a disk enclosure.

[0022] In a preferred embodiment of the present invention, the catalyst transport mechanism transfers the catalyst from a rotating disk to a flowing electrolytic cell, and includes a catalyst transport motor module, a second motor base, a third motor base, a catalyst transport platform, and a grooved limiting fence; the catalyst transport motor module is fixed on the second motor base and the third motor base, and connects the catalyst loading mechanism and the flowing electrolytic cell; the catalyst transport platform and the grooved limiting fence together form a grooved guide rail, and a catalyst placement mechanism is placed on the surface of the catalyst transport platform.

[0023] In a preferred embodiment of the present invention, the electrolyte transport mechanism includes an electrolyte transport motor module, a first motor base, a accommodating mechanism limiting device (restricting its vertical movement), and a reagent bottle accommodating mechanism; the reagent bottle accommodating mechanism accommodates at least two reagent bottles.

[0024] In a preferred embodiment of the present invention, the hydraulic control mechanism is used to realize the vertical lifting and lowering of the electrolyte inlet and outlet pipes, and to complete the rapid switching of the pipeline with the help of the small gripper; the hydraulic control mechanism includes a fourth motor, a hydraulic control motor module, a small gripper connecting plate, a small gripper, a small gripper fixture, a fifth motor base, a hydraulic lifting motor module, a hydraulic lifting connector and a hollow glass tube.

[0025] This invention also provides a fully automated method for preparing electrocatalysts based on the above-mentioned platform. In a preferred embodiment, the target electrocatalytic reaction system is a carbon dioxide reduction reaction system, comprising the following steps:

[0026] 1) The rotating gripper picks up the reagent bottle and completes a preset number of rotations (e.g., three rotations) in the rotating cap module to separate the cap from the bottle body, and the cap is transferred to the cap storage module.

[0027] 2) After the pipette tip is removed from the tip storage module, the pipette can draw a pre-set volume of molecular solution (e.g., 1 mL) into the opened reagent bottle and repeat the drawing process a preset number of times (e.g., repeat once for a total of 2 mL).

[0028] 3) Inject the absorbed solution into the preparation monomer containing the carrier (preferably carbon paper) and cap it;

[0029] 4) After completing all monomer preparation cycles of steps 1)-3), allow the mixture to stand for a predetermined time to complete the electrocatalyst modification (e.g., stand for 2 days).

[0030] 5) Transfer the entire monomer to the metal layer on the hot plate and heat and dry it according to the preset temperature and holding time (e.g., constant temperature heating at 70°C) until the carbon paper is dry and then replace the top cover.

[0031] The parameters such as liquid volume, heating temperature, and settling time in the preparation process are all preset and precisely controlled by the host computer on the platform.

[0032] This invention also provides a fully automated testing method for electrocatalysts based on the above-mentioned platform. In a preferred embodiment, the target electrocatalytic reaction system is a carbon dioxide reduction reaction system, comprising the following steps:

[0033] 1) The rotating gripper picks up the electrolyte bottles from the cathode and anode chambers of the reagent bottle storage module and places them in the reagent bottle receiving mechanism of the electrolyte transport mechanism;

[0034] 2) The motor module of the electrolyte delivery mechanism inserts the hollow glass tube into the corresponding reagent bottle to connect the electrolyte;

[0035] 3) The first suction cup removes the prepared catalyst from the monomer and places it in the groove of the silicone pad on the rotating disk;

[0036] 4) The rotating disk rotates 180°, and the catalyst delivery platform sends the catalyst into the flow electrolyzer and closes the electrolyzer;

[0037] 5) The peristaltic pump circulates the electrolyte at a preset flow rate (e.g., 10 mL / min) and starts the electrochemical workstation to carry out the target electrocatalytic reaction according to the preset electrochemical reaction conditions; in a preferred embodiment, the target electrocatalytic reaction is a CO2 reduction reaction and the reaction time is, for example, 15 min.

[0038] 6) Subsequently, gas chromatography was started to detect the product in real time;

[0039] 7) After the reaction is complete (cumulative 15 min), turn off the electrochemical workstation, raise and lower the hollow glass tube to extract the electrolyte and discharge it at a reverse flow rate of 20 mL / min, and collect the liquid phase product;

[0040] 8) Open the flow electrolyzer, and the electrolyte delivery mechanism and catalyst delivery mechanism return to their initial positions;

[0041] 9) Rotate the rotating disk another 180°, and the second suction cup will transfer the tested catalyst to the waste container to complete one cycle.

[0042] The gas chromatography detection module is linked in real time with the platform's control circuit to achieve online quantification and rapid feedback of the product. The fully automated testing process can operate continuously for 24 hours to improve data output speed.

[0043] This technical solution achieves high-precision, low-error, rapid, and repeatable fully automated screening of electrocatalysts, providing technical support for the rapid discovery of electrocatalysts in different electrocatalytic reaction systems. Compared with the background technology, it has the following advantages:

[0044] 1. This invention achieves full-process automation through a four-axis (XY-Z1-Z2) gantry motion system, clamping / pipetting mechanism, and unified control circuit, enabling unmanned operation from sample preparation, sample loading, flow electrolysis to product detection, completely eliminating human intervention;

[0045] 2. The present invention employs a closed-loop flow electrolysis cell and a hydraulic control mechanism to achieve safe transfer of gas and liquid and rapid shutdown. By pre-setting parameters and monitoring in real time, it avoids volume deviation, time error and inconsistency caused by human operation, effectively reducing errors.

[0046] 3. This invention uses a high-throughput pipetting workstation in hybrid technology to achieve liquid distribution from milliliters to microliters. Combined with the continuous and adjustable flow rate electrolysis environment provided by the flow electrolyzer, each electrocatalytic experiment can be repeated within the same process window, significantly improving the accuracy and reproducibility of the experimental results, and exhibiting high precision and consistency.

[0047] 4. The platform of this invention can complete the preparation, loading, continuous electrolysis and online product analysis of catalyst (gas chromatography and nuclear magnetic resonance) in a single cycle, reducing the experimental cycle from several hours to several minutes, and realizing efficient catalyst preparation and high-throughput screening.

[0048] Other features and beneficial effects of the present invention will be set forth in the following description, and some of these features and beneficial effects may be learned by practicing the invention. The objectives and other beneficial effects of the invention can be achieved and obtained through the structures specifically pointed out in the description and other contents. Attached Figure Description

[0049] To more clearly illustrate the technical solutions in the embodiments of the present invention or the prior art, the drawings used in the description of the embodiments or the prior art will be briefly introduced below. Obviously, the drawings described below are some embodiments of the present invention. For those skilled in the art, other drawings can be obtained based on these drawings without creative effort. Unless otherwise specified, the positional relationships in the drawings described below are based on the direction shown by the components in the figures.

[0050] Figure 1 This is a schematic diagram of the automated electrocatalyst screening platform provided in Example 1;

[0051] Figure 2 This is a schematic diagram of the four-axis moving mechanism provided in Embodiment 1;

[0052] Figure 3 This is a schematic diagram of the clamping mechanism provided in Embodiment 1;

[0053] Figure 4 This is a schematic diagram of the pipetting mechanism provided in Example 1;

[0054] Figure 5 This is a partial schematic diagram of the high-throughput pipetting workstation provided in Example 1;

[0055] Figure 6 This is a schematic diagram of the rotating bottle cap module provided in Embodiment 1;

[0056] Figure 7 This is a schematic diagram of the catalyst preparation module provided in Example 1;

[0057] Figure 8 This is a schematic diagram of the electrochemical testing workstation provided in Example 1;

[0058] Figure 9 This is a schematic diagram of the suction cup mechanism provided in Embodiment 1;

[0059] Figure 10 This is a schematic diagram of the catalyst loading mechanism, catalyst transport mechanism, electrolytic cell and its closing mechanism provided in Example 1;

[0060] Figure 11 This is a schematic diagram of the electrolyte delivery mechanism and hydraulic control mechanism provided in Example 1;

[0061] Figure 12 This is a schematic diagram of the pump system provided in Example 1.

[0062] Figure label:

[0063] 1. Aluminum alloy panel; 2. Four-axis moving mechanism; 3. Clamping mechanism; 4. Pipetting mechanism; 5. Control circuit; 6. High-throughput pipetting workstation; 7. Electrochemical testing workstation;

[0064] 31. Clamping jaw connector; 32. Rotating clamp; 33. Rotating clamp fixture; 41. Pipette connector; 42. Pipette; 43. Electric push rod; 44. Fixed flange; 45. Universal pipette tip connector; 46. Pipette tip assembly; 47. Pipette tip; 61. Reagent bottle storage module; 62. Universal base; 63. Waste container; 64. Pipette tip storage module; 65. Bottle cap storage module; 66. Electrolyte dispensing mechanism; 67. Dispensing mechanism base; 68. Rotating bottle cap module; 69. Catalyst preparation module; 71. Suction cup mechanism; 72. Catalyst sample loading mechanism; 73. Electrolyte transport mechanism; 74. Catalyst transport mechanism; 75. Flow electrolyzer; 76. Pump system; 77. Hydraulic control mechanism;

[0065] 211. Aluminum alloy connecting plate; 212. Aluminum profile support column; 221. Y-axis (left); 222. Y-axis slider (left); 223. Y-axis (right); 224. Y-axis slider (right); 225. Y-axis drive motor; 231. X-axis support beam; 232. X-axis; 233. X-axis slider; 234. X-axis drive motor; 241. Z1 axis (left); 242. Z2 axis (right); 243. Z1 axis drive motor (left); 244. Z2 axis drive motor (right); 681. Flexible platform base; 682. Connecting spring; 683. Parallel gripper plate; 684. Parallel gripper; 685. Parallel gripper fixture; 686. Linear guide rail; 687. Slider; 688. Slider connector; 691. First cover temporary storage area; 692. Second cover temporary storage area; 693. Solution suction mechanism; 694. Heating stage; 695. Metal layer on the heating stage; 696. Upper layer of catalyst preparation module; 697. Lower layer of catalyst preparation module; 698. Monomer in preparation area; 699. Upper cover of preparation area; 711. First suction cup; 712. Second suction cup; 713. Suction cup storage mechanism; 721. Rotating disk; 722. Catalyst placement mechanism; 723. Silicone gasket; 724. Disk enclosure; 731. Electrolyte transport motor module; 732. First motor base; 733. Receptacle mechanism limiting device; 734. Reagent bottle receiving mechanism; 741. Catalyst transport motor module; 742. Second motor base; 743. Third motor base; 744. Catalyst transport platform; 745. Grooved limiting enclosure; 751. Electrolytic cell closing device back plate 752. Electrolytic cell bottom plate; 753. Electrolytic cell closing device; 754. Gas chamber; 755. Cathode chamber; 756. Anode chamber; 761. First peristaltic pump; 762. Second peristaltic pump; 763. Peristaltic pump connecting plate; 771. Fourth motor base; 772. Hydraulic control motor module; 773. Small gripper connecting plate; 774. Small gripper; 775. Small gripper fixture; 776. Fifth motor base; 777. Hydraulic lifting motor module; 778. Hydraulic lifting connector; 779. Hollow glass tube. Detailed Implementation

[0066] To make the objectives, technical solutions, and advantages of the embodiments of the present invention clearer, the technical solutions of the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings. Obviously, the described embodiments are only some embodiments of the present invention, not all embodiments. The technical features designed in the different embodiments of the present invention described below can be combined with each other as long as they do not conflict with each other. All other embodiments obtained by those skilled in the art based on the embodiments of the present invention without creative effort are within the scope of protection of the present invention.

[0067] In the description of this invention, it should be understood that the terms "center," "upper," "lower," "left," "right," "vertical," "top," "bottom," "inner," and "outer," etc., indicating orientation or positional relationships based on the orientation or positional relationships shown in the accompanying drawings, are only for the convenience of describing the invention and simplifying the description, and do not indicate or imply that the device or component referred to must have a specific orientation, or be constructed and operated in a specific orientation, and therefore should not be construed as a limitation of the invention. Furthermore, the terms "first," "second," "third," "fourth," and "fifth" are used for descriptive purposes only and should not be construed as indicating or implying relative importance or implicitly specifying the number of indicated technical features. Thus, a feature defined as "first" or "second" may explicitly or implicitly include one or more of that feature. In the description of this invention, unless otherwise stated, "a plurality of" means two or more. Additionally, the term "comprising" and any variations thereof mean "at least comprising."

[0068] Example 1

[0069] Please see Figures 1 to 12 , Figure 1 This is a schematic diagram of the automated electrocatalyst screening platform provided in this embodiment. Figure 1 As shown, the automated electrocatalyst screening platform includes an aluminum alloy panel 1, a four-axis moving mechanism 2, a clamping mechanism 3, a pipetting mechanism 4, a control circuit 5, a high-throughput pipetting workstation 6, and an electrochemical testing workstation 7.

[0070] The four-axis moving mechanism 2 is fixed to the aluminum alloy panel 1 via an aluminum alloy connecting plate 211 and an aluminum profile support column 212. Based on its travel range, the entire device is divided into two parts: a high-throughput pipetting workstation 6 and an electrochemical testing workstation 7. The high-throughput pipetting workstation 6 is entirely within its travel range, while the vast majority of the electrochemical testing workstation 7 is outside its travel range, with only a small portion within it. Both workstations can operate independently. In addition, the aluminum alloy panel 1 includes a control circuit 5, which is also located outside the travel range of the moving mechanism. The four-axis moving mechanism 2 presents a gantry structure with four axes XYZ1Z2. Specifically, the Y-axis (left) 221 and Y-axis (right) 223 are fixed on the aluminum profile support columns 212 on both sides. The Y-axis (left) 221 is connected to the Y-axis drive motor 225 and serves as the active axis. The Y-axis (right) 223 does not have a drive motor and serves as the driven axis. Above the two Y-axis are Y-axis sliders (left) 222 and Y-axis sliders (right) 224, respectively. The X-axis support beam 231 is fixed above the two sliders. The X-axis 232, which includes the X-axis slider 233 and the X-axis drive motor 234, is fixed on the beam. The Z1 axis (left) 241, which has the Z1 axis drive motor (left) 243, and the Z2 axis (right) 242, which has the Z2 axis drive motor (right) 244, are fixed on the sliders.

[0071] The clamping mechanism 3 is installed at the end of the Z1 axis and includes a jaw connector 31, a rotating jaw 32, and a rotating jaw clamp 33. The rotating jaw 32 is fixed to the jaw connector 31 by screws and positioning pins. Preferably, a pair of rotating jaw clamps 33 are installed at the end of the jaw to accommodate the clamping of all solid materials inside the device.

[0072] The pipetting mechanism 4 is mounted at the end of the Z2 axis and includes a pipette connector 41, a pipette 42, an electric actuator 43, a fixing flange 44, a universal pipette tip connector 45, a pipette tip pusher 46, and a pipette tip 47. The pipette 42 is fixed to the pipette connector 41 by screws and locating pins. To achieve rapid solution transfer and reduce the time spent cleaning the internal container of the pipette, this mechanism is designed with a quick-change pipette tip structure, inspired by the use of laboratory pipettes. This structure is mainly functionalized by the electric actuator 43. In use, the pipette tip is fixed to the universal pipette tip connector 45, which is installed at the end of the pipette 42 via the fixing flange 44 and is tightly connected to its solution outlet. When the pipette tip needs to be removed, the electric actuator 43 drives the pipette tip pusher 46 fitted on the connector, enabling quick tip replacement. Furthermore, the universal pipette tip connector 45 can accommodate pipette tips of different sizes; preferably, the pipette tips used in this device are all 1 mL in size.

[0073] The high-throughput pipetting workstation 6 can be divided into three parts according to its function: a storage area, a functional area, and a waste area. The storage area includes a reagent bottle storage module 61, a pipette tip storage module 64, and a bottle cap storage module 65. The functional area includes an electrolyte dispensing mechanism 66, a rotating bottle cap module 68, and a catalyst preparation module 69. The waste area only contains a waste container 63.

[0074] The reagent bottle storage module 61 has a total of 80 holes. Based on the type of solution placed inside, these 80 holes can be divided into three parts: a cathode electrolyte storage area, an anolyte storage area, and a modification molecular solution storage area. These three parts occupy 48, 8, and 24 holes, respectively.

[0075] The nozzle storage module 64 can hold a total of 60 1mL nozzles to meet the needs of continuous operation of the device, and has a gripping structure designed in the center of its surface for easy and quick replacement.

[0076] The bottle cap storage module 65 is used to store the bottle caps of reagent bottles that need to be opened for a long time during the operation of the device. Preferably, a total of 12 corresponding placement areas are designed to meet the needs of continuous and uninterrupted operation of the device.

[0077] The electrolyte addition mechanism 66 is housed in the addition mechanism base 67 and is connected to a large quantity of pre-prepared electrolyte via a dedicated liquid circuit, enabling rapid addition of the electrolyte for the reaction. In this embodiment, the top of the electrolyte addition mechanism 66 is clamped by the clamping mechanism 3, and moved above an open empty reagent bottle by the four-axis moving mechanism 2, thus achieving rapid addition of the electrolyte. Preferably, the electrolyte volume is set to 16.5 mL.

[0078] The rotating cap module 68 is fixed to the aluminum alloy panel 1 via the elastic platform base 681, and the platform moves up and down via the connecting spring 682, linear guide rail 686, and slider 687. The parallel gripper plate 683 is placed above the connecting spring 682, and a parallel gripper 684 with a parallel gripper fixture 685 is fixed on the plate. The entire platform is fixed to the slider 687 via the slider connector 688. In this embodiment, the clamping mechanism 3 picks up a capped reagent bottle from the reagent bottle storage module 61 and transfers it to the middle of the parallel gripper fixture 685 in the parallel gripper plate 683 via the four-axis moving mechanism 2, closing the parallel gripper 684. Then, the rotating gripper 32 rotates a certain number of times. At the same time, the parallel gripper plate 683 automatically adapts to the change in bottle height caused by the cap being loosened. Preferably, the number of rotations is set to 3 rotations. After the bottle cap is unscrewed, the four-axis moving mechanism 2 transfers the bottle cap to the bottle cap storage module 65. At the same time, the parallel gripper plate 683 returns to its initial height under the action of the connecting spring 682.

[0079] The catalyst preparation module 69 includes a first cover storage area 691, a second cover storage area 692, a solution suction mechanism 693, a heating stage 694, a metal layer 695 on the heating stage, an upper layer 696 of the catalyst preparation module, a lower layer 697 of the catalyst preparation module, a monomer in the preparation area 698, and a top cover 699 for the preparation area. The first cover storage area 691 is located to the left of the heating stage 694, and the second cover storage area 692 is located to the right of the lower layer 697 of the catalyst preparation module, used for temporarily storing the top cover 699 of the preparation area during device operation. The solution suction mechanism 693 is located directly behind the second cover storage area 692, used to drain the solution inside the monomer 698 in the preparation area after catalyst preparation is completed. The metal layer 695 on the heating stage is installed above the heating stage 694 to extend the heating area of ​​the heating stage. This area is equipped with an upper catalyst preparation module 696 capable of accommodating 24 preparation zone monomers 698 and a lower catalyst preparation module 697 capable of accommodating a corresponding number of preparation zone covers 699. The preparation zone monomers 698 are designed to be quickly detachable. Most of the time, the preparation zone covers 699 are fastened above the preparation zone monomers 698, and the upper catalyst preparation module 696 rests on top of the lower catalyst preparation module 697 via a raised structure on its surface.

[0080] Waste container 63 is used to collect the nozzle 47 that is replaced during the operation of the device. Similar to the nozzle storage module 64, the surface of waste container 63 is also designed with a gripping structure for easy and quick replacement. Both waste container 63 and nozzle storage module 64 are placed on universal base 62, and their number and position can be adjusted according to actual needs and the stroke range of the four-axis moving mechanism 2. Preferably, this device is equipped with one nozzle storage module and one waste container.

[0081] The electrochemical testing workstation 7 includes a suction cup mechanism 71, a catalyst loading mechanism 72, an electrolyte transport mechanism 73, a catalyst transport mechanism 74, a flow electrolyzer 75, a pump system 76, and a hydraulic control mechanism 77. Except for the leftmost parts of the suction cup mechanism 71, the catalyst loading mechanism 72, and the catalyst transport mechanism 74, which are within the travel range of the four-axis moving mechanism 2, all other components are located outside the travel range.

[0082] The suction cup mechanism 71 includes a first suction cup 711, a second suction cup 712, and a suction cup storage mechanism 713. The first suction cup 711 is responsible for moving the catalyst to be tested, and the second suction cup 712 is responsible for moving the catalyst that has already been tested. Both suction cups are stored in the suction cup storage mechanism 713.

[0083] The catalyst loading mechanism 72 includes a rotating disk 721, a catalyst placement mechanism 722, a silicone gasket 723, and a disk enclosure 724. The rotating disk 721 is mounted above the second motor base 742 and rotates smoothly via a 42-stepper motor. Above the disk is a disk enclosure 724 surrounding it, with four equally spaced grooves on its surface. Each groove is used to hold the catalyst placement mechanism 722. The catalyst placement mechanism 722 contains a grooved hollow silicone gasket 723.

[0084] The electrolyte delivery mechanism 73 includes an electrolyte delivery motor module 731, a first motor base 732, a receiving mechanism limiting device 733, and a reagent bottle receiving mechanism 734. The electrolyte delivery motor module 731 is fixed to the aluminum alloy panel 1 via two first motor bases 732. The receiving mechanism limiting device 733 is fixed to the slider of the electrolyte delivery motor module 731, and a reagent bottle receiving mechanism 734 capable of accommodating two electrolyte reagent bottles is placed at its center. Due to the limitation imposed by the receiving mechanism limiting device 733, the reagent bottle receiving mechanism 734 can only move up and down.

[0085] The catalyst delivery mechanism 74 includes a catalyst delivery motor module 741, a second motor base 742, a third motor base 743, a catalyst delivery platform 744, and a grooved limiting fence 745. The catalyst delivery motor module 741 is fixed to the aluminum alloy panel 1 via the second motor base 742 and the third motor base 743. The catalyst delivery platform 744 is fixed on the module slider. The platform moves left and right within the grooved limiting fence 745 to transfer the catalyst placement mechanism 722 from the catalyst sample loading mechanism 72 to the flow electrolysis cell 75.

[0086] The flowing electrolytic cell 75 includes an electrolytic cell closure device back plate 751, an electrolytic cell bottom plate 752, an electrolytic cell closure device 753, a gas chamber 754, a cathode chamber 755, and an anode chamber 756. The gas chamber 754, cathode chamber 755, and anode chamber 756 are components of the electrolytic cell. The gas chamber is fixed to the bottom of the electrolytic cell closure device 753. The cathode chamber 755 and anode chamber 756 are fixed to the surface of the electrolytic cell bottom plate 752. The electrolytic cell bottom plate 752 and the electrolytic cell closure device 753 are fixed to the electrolytic cell closure device back plate 751. The electrolytic cell closure device back plate 751 is fixed to the right-side aluminum profile support column 212.

[0087] The pumping system 76 includes a first peristaltic pump 761, a second peristaltic pump 762, and a peristaltic pump connecting plate 763. The first peristaltic pump 761 and the second peristaltic pump 762 are fixed on the surface of the peristaltic pump connecting plate 763 and are responsible for circulating the pumping fluid in the cathode chamber 755 and the anode chamber 756, respectively. The peristaltic pump connecting plate 763 is fixed on the aluminum profile support column 212 on the right side.

[0088] The hydraulic control mechanism 77 includes a fourth motor base 771, a hydraulic control motor module 772, a small gripper connecting plate 773, a small gripper 774, a small gripper fixture 775, a fifth motor base 776, a hydraulic lifting motor module 777, a hydraulic lifting connector 778, and a hollow glass tube 779. The fourth motor base 771 is fixed on the aluminum alloy panel 1, the hydraulic control motor module 772 is fixed inside the fourth motor base 771, the small gripper connecting plate 773 is fixed on the module slider, the connecting plate is fixed with a small gripper 774 with a small gripper clamp 775, the fifth motor base 776 is fixed above the small gripper 774, the hydraulic lifting motor module 777 is fixed on the surface of the fifth motor base 776, the hydraulic lifting connector 778 is fixed on the module slider, and the connector is divided into two areas at the end, corresponding to the reagent bottle containing the cathode chamber electrolyte and the reagent bottle containing the anode chamber electrolyte, respectively. Each area is fitted with two hollow glass tubes 779 of different lengths, which are responsible for liquid inlet and liquid outlet. Preferably, the lengths of the two glass tubes are 120mm and 100mm.

[0089] It should be noted that the operable parts of the above-mentioned device are all automatically controlled by a host computer (the control system and method are conventional technical means, and will not be described in detail here).

[0090] Therefore, the automated electrocatalyst screening platform provided by this invention can realize the full automation of the catalyst preparation and testing process without human intervention, fundamentally eliminating random errors introduced by human operation. The entire experimental process is set with precise parameters to ensure that each experiment can be carried out accurately according to the preset conditions, thereby improving the accuracy and consistency of operation, thus improving the efficiency of the experiment and enhancing the repeatability of the data.

[0091] Example 2

[0092] This embodiment describes a fully automated method for preparing electrocatalysts using the automated electrocatalyst screening platform of Example 1. The following description uses a carbon dioxide reduction reaction system as an example and includes the following steps:

[0093] The rotating gripper 32 moves to the reagent bottle storage module 61 to grab the cap of the reagent bottle containing the molecular solution and transfers it to the middle of the parallel gripper 685 of the rotating cap module 68. After the parallel gripper 684 grips the reagent bottle, the rotating gripper 32 rotates three times to separate the cap from the bottle body and places the cap into the cap storage module 65.

[0094] The pipette 42 moves to the pipette tip storage module 64 to obtain the pipette tip, and moves to the opened reagent bottle to draw 1 mL of molecular solution.

[0095] After the rotating gripper 32 grasps the preparation area cover 699, the molecular solution is injected into the preparation area monomer 698 where the carbon paper is placed using the pipette 42.

[0096] Repeat the pipetting operation once, injecting a total of 2 mL of molecular solution into the monomer 698 in the preparation area, and then cover the preparation area with the cap 699;

[0097] The rotating gripper 32 picks up the bottle cap and moves it above the opened reagent bottle. It rotates in the opposite direction for the same number of turns to close the bottle cap with the reagent bottle. The parallel gripper 684 is then released, and the reagent bottle is returned to the reagent bottle storage module 61.

[0098] The pipette 42 moves above the waste container 63, the electric push rod 43 extends, and after the pipette tip retraction operation is completed, the electric push rod 43 retracts.

[0099] After repeating the above operations on all monomer preparation regions, let it stand for two days to wait for catalyst modification.

[0100] Using the rotating gripper 32, the entire upper layer 696 of the catalyst preparation module is moved from the surface of the lower layer 697 of the catalyst preparation module to the surface of the metal layer 695 on the hot stage. Then, the upper cover 699 of the preparation area is sequentially transferred to the corresponding position on the lower layer 697 of the catalyst preparation module. The solution suction mechanism 693 is then engaged and inserted sequentially into the monomer 698 of the preparation area to drain the remaining solution. The hot stage 694 is then activated and heated at a constant temperature of 70°C. After the carbon paper is dried, the upper cover is replaced to prevent dust from affecting the experiment. This completes the fully automated preparation of the carbon dioxide electroreduction catalyst.

[0101] The fully automated method for preparing electrocatalysts provided by this invention (taking a carbon dioxide reduction reaction system as an example) simplifies the catalyst preparation steps and standardizes the solution transfer volume compared to existing technologies. The fully automated device ensures high consistency in the preparation process of different batches of electrocatalysts, reducing random and systematic errors.

[0102] Example 3

[0103] This embodiment describes a fully automated method for testing electrocatalysts using the automated electrocatalyst screening platform of Example 1. The following description uses a carbon dioxide reduction reaction system as an example and includes the following steps:

[0104] The rotating gripper 32 sequentially picks up reagent bottles containing cathode chamber electrolyte and anode chamber electrolyte from the reagent bottle storage module 61, and places them into the reagent bottle receiving mechanism 734 after opening the caps;

[0105] The electrolyte transport motor module 731 moves from left to right, aligning the reagent bottle opening with the bottom of the hollow glass tube 779. Then, the liquid path lifting motor module 777 moves from top to bottom, inserting the glass tube into the reagent bottle.

[0106] The rotating gripper 32 grasps the preparation area cover 699 and places it in the first cover storage area 691; then it grasps the first suction cup 711, picks up the prepared catalyst from the corresponding preparation area monomer 698, and transfers it to the groove of the silicone pad 723 of the catalyst placement mechanism 722 on the far left of the rotating disk 721; then the first suction cup 711 is put back into the suction cup storage mechanism 713; finally, the preparation area cover 699 is placed back from the first cover storage area 691 above the corresponding preparation area monomer 698.

[0107] The rotating disk 721 rotates 180°, transferring the catalyst placement mechanism 722, which contains the untested catalyst, to the catalyst transport platform 744, and then sending it into the electrolytic cell via the catalyst transport motor module 741.

[0108] The electrolytic cell is closed by the electrolytic cell closing device 753;

[0109] The first peristaltic pump 761 and the second peristaltic pump 762 circulate the solution at a rate of 10 mL / min;

[0110] After waiting for 1 minute, start the electrochemical workstation to begin the electrocatalytic reaction;

[0111] After the reaction has been complete for 5 minutes, run the chromatogram to detect the gaseous products.

[0112] After the reaction has been going on for 15 minutes, the electrocatalytic reaction is stopped. The liquid path lifting motor module 777 moves from bottom to top to pull the glass tube out of the reagent bottle. The first peristaltic pump 761 and the second peristaltic pump 762 are reversed to pump out the solution at a rate of 20 mL / min.

[0113] After waiting for 1 minute, the first peristaltic pump 761 and the second peristaltic pump 762 stopped rotating;

[0114] The electrolytic cell is opened by the electrolytic cell closing device 753;

[0115] The electrolyte delivery motor module 731 and the catalyst delivery motor module 741 move from right to left, returning them to their initial positions;

[0116] The rotating gripper 32 sequentially picks up reagent bottles from the reagent bottle receiving mechanism 734 and puts them back into the reagent bottle storage module 61 after the cap is closed.

[0117] Rotating disk 721 rotates 180°, and the catalyst placement mechanism 722, which contains the tested catalyst, is moved to the far right of the disk;

[0118] The rotating gripper 32 picks up the second suction cup 712 and transfers the tested catalyst from the far right of the disc into the waste container 63. Finally, the second suction cup 712 is returned to the suction cup storage mechanism 713. This completes the fully automated testing of the carbon dioxide electroreduction catalyst.

[0119] The fully automated operation method for electrocatalyst testing provided by this invention (taking a carbon dioxide reduction reaction system as an example) achieves fully automated operation from catalyst sample change to testing, compared with existing technologies. Through the fully automated device, experiments can be conducted 24 hours a day without interruption, greatly increasing the data output speed.

[0120] The above embodiments are only used to illustrate the technical solutions of the present invention, and are not intended to limit it. Although the present invention has been described in detail with reference to the foregoing embodiments, those skilled in the art should understand that modifications can still be made to the technical solutions described in the foregoing embodiments, or equivalent substitutions can be made to some or all of the technical features therein. Such modifications or substitutions do not cause the essence of the corresponding technical solutions to deviate from the scope of the technical solutions of the embodiments of the present invention.

Claims

1. A high-throughput screening platform for electrocatalysts in electrocatalytic reaction systems, characterized in that: Includes a four-axis moving mechanism, a high-throughput pipetting workstation, an electrochemical testing workstation, control circuitry, and host computer software; The four-axis moving mechanism adopts a gantry structure, where the x-axis and y-axis are used for planar positioning, the Z1 axis is connected to a clamping mechanism, and the Z2 axis is connected to a pipetting mechanism. The high-throughput pipetting workstation is equipped with a catalyst preparation module and an electrolyte addition mechanism. The electrochemical testing workstation includes a flow electrolytic cell and a product detection module. The high-throughput pipetting workstation supplies catalyst samples and electrolyte to the flow electrolytic cell through the four-axis moving mechanism. The host computer software communicates with the four-axis moving mechanism, the high-throughput pipetting workstation, and the electrochemical testing workstation through the control circuit to achieve automatic linkage control of electrocatalyst preparation, sample loading and testing, and product detection. The high-throughput pipetting workstation includes a pipette tip storage module, a waste container, a reagent bottle storage module, a bottle cap storage module, an electrolyte dispensing mechanism, a catalyst preparation module, and a rotating bottle cap module. The electrolyte filling mechanism is mounted on the platform via a filling mechanism base, and the filling mechanism base is provided with a liquid passage connecting to the electrolyte storage tank. The catalyst preparation module includes a first cover storage area, a second cover storage area, a solution suction mechanism, a hot stage, a metal layer on the hot stage, an upper layer of the catalyst preparation module, a lower layer of the catalyst preparation module, and a cover for the preparation area. A detachable preparation area unit with a cover is installed in the upper layer of the catalyst preparation module, and the metal layer on the hot stage is fixed to the surface of the hot stage. The rotating bottle cap module includes an elastic platform base, on which a linear guide rail is vertically mounted. A parallel gripper plate is mounted on the linear guide rail. A connecting spring is provided between the bottom of the parallel gripper plate and the elastic platform base. The parallel gripper plate is equipped with parallel grippers.

2. The high-throughput screening platform for electrocatalysts in electrocatalytic reaction systems according to claim 1, characterized in that: It includes an aluminum alloy panel, and the four-axis moving mechanism is disposed on the aluminum alloy panel; the working stroke of the four-axis moving mechanism includes the high-throughput liquid transfer workstation, and at least includes the interface required for the electrocatalyst picking, placing and adding liquid in the electrochemical testing workstation.

3. The high-throughput screening platform for electrocatalysts in electrocatalytic reaction systems according to claim 1, characterized in that: The clamping mechanism includes a rotating jaw, a rotating jaw connector, and a rotating jaw clamp.

4. The high-throughput screening platform for electrocatalysts in electrocatalytic reaction systems according to claim 1, characterized in that: The pipetting mechanism includes a universal pipette tip connector, a pipette tip, and an electric push rod. The electric push rod pushes the universal pipette tip connector to retract the pipette tip.

5. The high-throughput screening platform for electrocatalysts in electrocatalytic reaction systems according to claim 1, characterized in that: The electrochemical testing workstation includes a suction cup mechanism, a catalyst loading mechanism, a catalyst delivery mechanism, an electrolyte delivery mechanism, a flow electrolytic cell, and a hydraulic control mechanism. The product detection module includes a gas chromatography detection module and a nuclear magnetic resonance detection module. The suction cup mechanism includes a first suction cup for moving the catalyst to be tested, a second suction cup for moving the tested catalyst, and a suction cup storage mechanism. The catalyst loading mechanism includes a rotating disk, at least four catalyst placement mechanisms are provided at equal angles on the rotating disk, the surface of the catalyst placement mechanism is provided with a grooved silicone pad, and a disk fence is provided on the outer periphery of the rotating disk. The catalyst delivery mechanism includes a catalyst delivery motor module, a second motor base, a third motor base, a catalyst delivery platform, and a grooved limiting fence; the catalyst delivery motor module is fixed on the second motor base and the third motor base, and connects to the catalyst loading mechanism and the flow electrolysis cell; the catalyst delivery platform and the grooved limiting fence together form a groove-shaped guide rail, and a catalyst placement mechanism is placed on the surface of the catalyst delivery platform; The electrolyte delivery mechanism includes an electrolyte delivery motor module, a first motor base, a limiting device for the receiving mechanism, and a reagent bottle receiving mechanism; the reagent bottle receiving mechanism can accommodate at least two reagent bottles. The hydraulic control mechanism includes a fourth motor, a hydraulic control motor module, a small gripper connecting plate, a small gripper, a small gripper fixture, a fifth motor base, a hydraulic lifting motor module, a hydraulic lifting connector, and a hollow glass tube. The flowing electrolytic cell includes an electrolytic cell bottom plate, an electrolytic cell closure device back plate, and an electrolytic cell closure device for achieving sealing. The sealed cavity formed is provided with a gas chamber, a cathode chamber, and an anode chamber for electrocatalytic reaction. The cathode chamber and the anode chamber are connected to a pumping system for circulating pumping liquid.

6. The high-throughput screening platform for electrocatalysts in electrocatalytic reaction systems according to claim 1, characterized in that: Used in carbon dioxide reduction reaction systems.

7. A fully automated method for preparing an electrocatalyst based on the platform described in any one of claims 1 to 6, characterized in that, Includes the following steps: S1. The reagent bottle is gripped by the clamping mechanism, and the cap and bottle body are rotated relative to each other at the cap rotation module to separate the cap from the bottle body, and the separated cap is transferred to the cap storage module. S2. Install the pipette tip using the pipetting mechanism and draw a predetermined volume of molecular solution from the opened reagent bottle; S3. Inject the molecular solution into the monomer in the preparation region containing the carrier and cover it; S4. Repeat steps S1 to S3 for monomers in multiple preparation regions, and allow monomers in the preparation regions that have been added to stand for a predetermined time to complete the electrocatalyst modification. S5. Transfer the monomer in the preparation area to the hot plate and heat and dry it according to the preset temperature and holding time. After drying, reset the monomer in the preparation area and close the top cover. The volume, settling time, heating temperature, and holding time are preset by the host computer software and controlled by the control circuit.

8. A fully automated testing method for electrocatalysts based on the platform described in any one of claims 1 to 6, characterized in that, Includes the following steps: T1. The electrolyte bottle is transferred to the reagent bottle receiving mechanism of the electrolyte transport mechanism via the clamping mechanism; T2. The hollow tube is driven by the electrolyte delivery mechanism to insert into the corresponding reagent bottle to achieve electrolyte pipeline connection, and the lifting and switching of the inlet and outlet pipes is completed by the hydraulic control mechanism. T3. The prepared electrocatalyst is removed from the monomer in the preparation area by the first suction cup and placed on the grooved silicone pad of the rotating disk. T4. After the rotating disk is rotated, the electrocatalyst is fed into the flow electrolysis cell through the conveying mechanism, and the closing device is driven to close the flow electrolysis cell. T5. Start the pump system to circulate the electrolyte at a preset flow rate, and the electrochemical testing workstation will carry out the target electrocatalytic reaction according to the preset electrochemical reaction conditions. T6. The product detection module performs online detection of the reaction products and feeds the detection data back to the host computer software for recording. T7. After the reaction is complete, control the pump system and pipeline to perform drainage and reset, and collect the liquid phase product; T8. Open the flow electrolysis cell; the electrolyte delivery mechanism and catalyst delivery mechanism return to their initial positions. T9. After the rotating disk is rotated, the tested electrocatalyst is transferred to the waste container through the second suction cup to enter the next cycle. The flow rate and electrochemical reaction conditions are preset by the host computer software and controlled by the control circuit.

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