BatCAT deliverable 1.1: Experimental campaign plan and taxonomy

101137725/BatCAT/WP1/D1.1 D1.1 Experimental campaign plan and taxonomy Grant agreement number: 101137725 Project acronym: BatCAT Project title: Battery Cell Assembly Twin Project website: http://batcat.info/ Project start date: 01.01.2024 Project duration: 42 months Call topic: HORIZON-CL5-2023-D2-01-03 Deliverable type1: Report (R) Related work package: WP1 Due date: 30.06.2025 Actual submission date: 29.06.2025 Responsible beneficiary: IFPEN Dissemination level2: PU Abstract: The experimental campaign plan for BatCAT is described jointly with the methods and nomenclature used to store the respective data. Author list Beneficiary Name Contact e-mail IFPEN Martin Petit martin.p[email protected] NIC Sara Drvaric Talian [email protected] CPI Nicole Fleck [email protected] VANEVO Thorben Sieling thorben.s[email protected] 1 Deliverable type: R = Report, P = Prototype, D = Demonstrator, O = Other. 2 Dissemination level: PU = Public, SEN = Sensitive. Public Version v1 Page 2 of 14 Reviewer list Beneficiary Name Contact e-mail NMBU Martin Thomas Horsch martin.tho[email protected] Document history Version Date Reason/comment Revised by 1.0 29.06.2025 Delivery date See author list for all who contributed Disclaimer Funded by the European Union. Views and opinions expressed are however those of the author(s) only and do not necessarily reflect those of the European Union or the European Climate, Infrastructure and Environment Executive Agency (CINEA). Neither the EU nor the CINEA can be held responsible for them. Abbreviations and acronyms EIS Electrochemical impedance spectroscopy LIB Lithium ion battery NIB Sodium ion battery RFB Redox flow battery BatCAT has received funding from the European Union’s Horizon Europe research and innovation programme under grant agreement no. 101137725. Contents 1. Executive summary ___________________________________________________________________ 3 Description of the deliverable content and objectives __________________________________________ 3 Deviation from objectives, corrective action (if applicable) ______________________________________ 3 2. Progress report (main activities) _________________________________________________________ 3 Experimental campaign description ________________________________________________________ 4 LIB/NIB use case _____________________________________________________________________ 4 RFB use case ________________________________________________________________________ 6 Characterization methods ________________________________________________________________ 7 LIB/NIB use case _____________________________________________________________________ 7 Data storage and sharing ________________________________________________________________ 8 Characterization master file. ____________________________________________________________ 8 Recipe files_________________________________________________________________________ 10 Shared protocols ____________________________________________________________________ 12 Experimental campaign plan _____________________________________________________________ 12 LIB/NIB use case ____________________________________________________________________ 12 RFB use case _______________________________________________________________________ 13 3. Conclusion _________________________________________________________________________ 13 Public Version v1 Page 3 of 14 1. Executive summary Description of the deliverable content and objectives In this deliverable, the experimental campaign plan necessary for BatCAT is described as well as the methods and nomenclature used to store its data. It is the initial step of the experimental work done since the beginning of the BatCAT project. The BatCAT project is focusing on the manufacturing of batteries regarding 2 use-cases : Li-ion/Sodium-ion batteries (LIB/NIB) and redox-flow batteries (RFB) and the impact of manufacturing parameters on the operation of the batteries. As a consequence, the experimental campaign accounts for both cell manufacturing but also battery performance during operation. In this deliverable the manufacturing steps considered experimentally in both LIB/NIB and RFB use cases along with the tunable parameters considered in each step are presented. Then the experimental characterization planned for the manufacturing steps as well as the battery operation are described. Then the data storage system is described by explaining the different files and storage locations used up until now to store the data and metadata of the experiments performed so far. The experimental files are completed by experimental partners of WP1 so that other beneficiaries are able to recover the data as well as the history of samples tested through “recipe” files. This work was performed in collaboration with WP4 to ensure that all necessary data and metadata required in WP4 are available in the information collected in WP1 and at the same time that all data types encountered in WP1 experiments fits within the taxonomy described in WP4. The information in this deliverable will be used to plan the next steps of the experimental campaign in agreement with requirements of other beneficiaries in the BatCAT project. Deviation from objectives, corrective action (if applicable) Final ELN and data storage tools are not running completely up until now as a consequence a provisional solution was adopted using BatCAT SharePoint to ensure a reliable and easy sharing of data among partners. 2. Progress report (main activities) The work described in this deliverable is focused on 3 main activities: - Performing specific steps of the manufacturing process to get representative samples which can be further analysed to get their properties and calibrate and validate models - Analyse these samples - Store the data in a sensible way so that other BatCAT partners are able to recover and use them in their activities. In the following section, the experimental campaign, available characterization methods and data storage processes will be described. They cover both use case from the BatCAT project Li-ion and Sodium-ion batteries (LIB/NIB) as well as the redox-flow batteries (RFB). Public Version v1 Page 4 of 14 Experimental campaign description LIB/NIB use case The LIB/NIB process is a sequence of several steps from the raw active materials to the final battery cells (Figure 1). Figure 1: LIB/NIB cell production process The following parameters must be optimised in the LIB/NIB use cases to ensure optimal device performance. These hold for a single formulation or combination of materials and any changes to the chemistry requires additional optimisation. Formulation of the coating slurry Formulations consist of an active material (e.g. NMC, LFP, graphite), a binder (e.g. PVDF) and a conductive additive (e.g. carbon black) to enhance electron conduction. Sometimes, additional additives are included to further enhance device performance (e.g. carbon nanotubes). These “dry” ingredients are mixed stepwise with a solvent to form a slurry which can be coated onto current collectors to form battery electrode anodes and cathodes. The tuneable control parameters for the slurry formulation are as follows at CPI: 1. Material choices (limited by market availability) a. Active material particle size and distribution b. Conductive additive (carbon black) particle size c. Binder type (informs solvent) d. Additive type (if any) 2. Active material: binder : conductive additive ratio 3. Solids/liquid ratio (solids content) 4. Additive content (e.g. carbon nanotubes) 5. Mixing order 6. Mixing speed Coating of the slurry onto current collector Formulation slurries are coated onto current collector foils by a doctor blade-style process. Wet electrodes are dried in an oven to remove the solvent. Public Version v1 Page 5 of 14 The tuneable control parameters for the coating process are as follows at CPI: 1. Wet coating thickness 2. Drying temperature 3. Drying time Calendaring the coated electrodes Coated and dried electrodes are calendared for numerous reasons. These include the improvement of the electronic conductivity between the current collector and the film and increasing the energy density by decreasing the porosity of the films. Calendaring involves pressing the electrode between two rollers at a set distance apart. While reducing the porosity increases the density, some porosity is necessary to allow diffusion of electrolyte into the electrode. The tuneable control parameters for calendaring are as follows at CPI: 1. Calendaring thickness/density 2. Calendaring speed 3. Calendaring temperature (heating only, no cooling) Cell assembly Cells are assembled in either a half or full cell configuration. Half cells incorporate lithium or sodium as a counter electrode for LIB and NIB use case respectively to test the performance of individual anodes or cathodes. Full cells allow the testing of the full battery performance. The electrodes cut to size and stacked with electrolyte and sealed to complete the cells ready for electrical testing. These can be in coin or pouch cell configuration at CPI. The tuneable control parameters for cell assembly are as follows at CPI: 1. N/P ratio (anode to cathode capacity ratio) 2. N/P area ratio (anode to cathode electrode area ratio) 3. Electrolyte salt (e.g lithium hexafluorophosphate) 4. Electrolyte solvent and solvent mixes (e.g. ethylene carbonate, dimethyl carbonate) 5. Electrolyte volume Cell testing Cells are cycled to investigate cell performance. Several cycles at the beginning of the cell cycling lead to the formation of the solid electrolyte interphase (SEI) layer. There is large flexibility in the tunable parameters for the cycling stage, their order and analysis metrics. Comparison of cells cycled under identical protocols is standard. The tuneable control parameters for cell cycling protocols are as follows at CPI: 1. Resting time 2. Voltage limits (high and low) 3. Current limits for each step 4. Time limits for each step 5. Temperature Public Version v1 Page 6 of 14 6. Cycle C-rate (fast or slow charge/discharge) 7. Cycle number RFB use case Redox flow batteries (RFBs) work by storing energy in liquid electrolytes, which flow through the electrochemical cell. Two separate tanks store these electrolytes, which contain dissolved electroactive species. With the use of pumps and pipes, these species circulate between the tanks and the cell. In the cell, electrochemical reactions occur – oxidation (loss of electrons) on the anode and reduction (gain of electrons) on the cathode. The two electrolytes are separated with an ion exchange membrane, which allows maintenance of charge balance. Figure 2: RFB manufacturing process description RFBs typically use porous carbon-based electrodes as anodes and cathodes. Carbon felts originating from Polyacrylonitrile (PAN) are commonly used. These electrodes provide a high surface area for electrochemical reactions and enable electrolyte flow through its pores. Advanced design of RFBs includes surface treatments to modify the carbon electrodes to enhance electrode reaction kinetics and electrolyte wettability. Heat or chemical treatments, plasma or electrochemical modifications are commonly used, but the full understanding of why and how these activations work is still missing in the scientific field. Figure 3: Felt preparation process The focus of BatCAT project will therefore be on understanding how the surface modification manufacturing step influences the performance of RFBs (Figure 2). In close cooperation of NIC and VANEVO, the number and type of samples, number of process parameter variation steps, process parameter ranges and refinement iterations were discussed and specified. An activation procedure with three steps was designed (Figure 3). In an iterative procedure, the activation of the electrode felt samples are activated and subsequently characterized with various methods by NIC and then sent to VANEVO to be further electrochemically and hydraulically characterized. Based on the results, a new iteration with varied process parameters is planned and performed, aiming at both extending the investigated process parameter domain as well as finding well performing parameter sets and activation procedures. Public Version v1 Page 7 of 14 Characterization methods Several characterization methods are implemented to assess the samples properties all along the manufacturing processes and also on the final products. LIB/NIB use case For LIB and NIB use cases the following characterization methods are in use at CPI in the manufacturing process: 1. Rheology measurement – slurries 2. Photographs – electrode 3. Mass measurements – weight of coated and cut electrodes 4. Resistance measurements – electrode before and after calendaring 5. Thickness measurements – electrode before and after calendaring Cell cycling – to determine performance For LIB/NIB use cases, the following characterization will be performed in IFPEN: Electrode level characterization: - Novel NMR tests to evaluate microstructure properties - Symmetric cell measurements: o Electrochemical Impedance Spectroscopy (EIS) to assess the tortuosity of manufactured electrodes - Half-cell manufacturing and testing o Electrode rate capability o GITT tests to measure active material diffusion properties o Aging test in 1C/1D cycles Full cell characterization - Coin cell measurements o Slow charge and discharge tests to evaluate electrode balancing o EIS test to assess cell internal impedance o Charge and discharge rate capability tests o HPPC test to assess cell power capability o Aging tests in calendar - Pouch cell measurements o Slow charge and discharge tests to evaluate electrode balancing o EIS test to assess cell internal impedance o Charge and discharge rate capability tests o HPPC test to assess cell power capability o Aging tests in calendar and cycling aging For RFB use case, the following characterisation techniques will be used to determine the effect of carbon felt activation: - Scanning electron microscopy (visualisation of the felt morphology) - X-ray photoelectron spectroscopy (determination of surface specific chemical composition, C1s and O1s spectra will be measured) - Wetting angle measurement using water and 2 M H2SO4 to determine the improvement in wettability - Raman spectroscopy (information of carbon structure) - Thickness measurement - Weight determination Public Version v1 Page 8 of 14 - Electrochemical performance testing including o Energy, voltaic, and coulombic efficiency o Specific capacity and energy o Pressure drop across the felt o Electrochemical impedance spectroscopy All this characterization techniques will provide the project with various data in terms of type and quantity. This data need to be collected, organised, stored and shared to allow further use along the project. Data storage and sharing To ensure a smooth collaboration of partners and WP within the projects, data are made available using the BatCAT SharePoint before the final KB is available to all. This sharing comprises information of the experiments performed on each sample chronologically as well as the manufacturing process of each sample studied in BatCAT. The global file organization detailed for the LIB use case can be seen in Figure 4. Figure 4: File storage organization in the BatCAT SharePoint Characterization master file. The characterization Masterfile is stored in the T1.1 folder to follow the progress of the experimental campaign. Public Version v1 Page 9 of 14 Figure 5: Characterization Masterfile for LIB/NIB usecase It is an Excel file composed of 3 sheets. The first one is a general explanation of the expected inputs. The second one is dedicated to LIB/NIB use case and the last one is for the RFB use case. In the first part of the spreadsheet, sample information is given with the sample name, its type (active material, slurry, electrode, half-cell, full cell…). Then the positive sample used is given for half and full cell to link the sample to the manufactured objects described in the recipe files. The manufacturing time is then asked as well as internal IFPEN and CPI references. Finally, the general protocol when available is given. In the nex part of the spreadsheet, each test is given through its name from the protocol, a link to the raw data and finally when available a simple result (for instance the available capacity during 1C/1D cycles). An example is shown in Figure 5. Sample LIB-2024-001 LIB-2024-002 LIB-2024-003 LIB-2024-004 LIB-2024-005 LIB-2024-006 Type Half-cell Half-cell Half-cell Half-cell Half-cell Half-cell Positive sample NMC_series4_NC.xlsx NMC_series4_NC.xlsx NMC_series4_NC.xlsx NMC_series4_cal1.xlsx NMC_series4_cal1.xlsx NMC_series4_cal1.xlsx Negative sample Li M Li M Li M Li M Li M Li M Cell recipe Coin cell preparation.xlsx Coin cell preparation.xlsx Coin cell preparation.xlsx Coin cell preparation.xlsx Coin cell preparation.xlsx Coin cell preparation.xlsx Manufacturing time 12/04/2024 12/04/2024 12/04/2024 12/04/2024 12/04/2024 12/04/2024 CPI internal reference Batcat S4-Uncal Batcat S4-Uncal Batcat S4-Uncal Batcat S4-Cal1 Batcat S4-Cal1 Batcat S4-Cal1 IFPEN internal reference NMC_serie4_NC_prot1 NMC_serie4_NC_prot2 NMC_serie4_NC_prot3 NMC_series4_cal1_prot1 NMC_series4_cal1_prot2 NMC_series4_cal1_prot3 Overall protocol Prot 1.xlsx Prot 2.xlsx Prot 3.xlsx Prot 1.xlsx Prot 2.xlsx Prot 3.xlsx Test 1 name Cell formation Cell formation Cell formation Cell formation Cell formation Cell formation Test 1 raw data D051224-01_01_MB_CB1.mpt D051224-02_01_MB_CB2.mpt D051224-03_01_MB_CC4.mpt D051224-04_01_MB_CB3.mpt D171224-01_01_MB_CA4.mpt D051224-06_01_MB_CC5.mpt Test 1 result Test 2 name Check up Check up Check up Check up Check up Check up Test 2 raw data D051224-01_02_MB_CB1.mpt D051224-02_02_MB_CB2.mpt D051224-03_02_MB_CC4.mpt D051224-04_02_MB_CB3.mpt D171224-01_02_MB_CA4.mpt D051224-06_02_MB_CC5.mpt Test 2 result Test 3 name Performance test GITT test GITT test Performance test GITT test GITT test Test 3 raw data D051224-01_03_MB_CB1.mpt D051224-02_03_MB_CB2.mpt D051224-03_03_MB_CC4.mpt D051224-04_03_MB_CB3.mpt D171224-01_03_MB_CA4.mpt D051224-06_03_MB_CC5.mpt Test 3 result Test 4 name Check up Check up Check up Check up Check up Check up Test 4 raw data D051224-01_04_MB_CB1.mpt D051224-02_04_MB_CB2.mpt D051224-03_04_MB_CC4.mpt D051224-04_04_MB_CB3.mpt D171224-01_04_MB_CA4.mpt D051224-06_04_MB_CC5.mpt Test 4 result Test 5 name Aging Discharge capability test Discharge capability test Aging Discharge capability test Discharge capability test Test 5 raw data D051224-01_05_MB_CB1.mpt D051224-02_05_MB_CB2.mpt D051224-03_05_MB_CC4.mpt D051224-04_05_MB_CB3.mpt D171224-01_05_MB_CA4.mpt D051224-06_05_MB_CC5.mpt Test 5 result Test 6 name Check up Charge capability test Charge capability test Check up Charge capability test Charge capability test Test 6 raw data D051224-01_06_MB_CB1.mpt D051224-02_06_MB_CB2.mpt D051224-03_06_MB_CC4.mpt D051224-04_06_MB_CB3.mpt D171224-01_06_MB_CA4.mpt D051224-06_06_MB_CC5.mpt Test 6 result Test 7 name Check up Check up Check up Check up Test 7 raw data D051224-02_07_MB_CB2.mpt D051224-03_07_MB_CC4.mpt D171224-01_07_MB_CA4.mpt D051224-06_07_MB_CC5.mpt Test 7 result Test 8 name Aging Aging Test 8 raw data D051224-02_08_MB_CB2.mpt D171224-01_08_MB_CA4.mpt Test 8 result Test 9 name Check up Check up Test 9 raw data D051224-02_09_MB_CB2.mpt D100125-01_09_MB_CA4.mpt Test 9 result