____________________Dataset for Thermal Stability of Valuable Metals in Lithium-Ion Battery Cathode Materials: Temperature Range 500-800 °C____________________

Last updated: 2024-03-08

______Contact______
* Kristýna Jílková
* ORCID: 0000-0003-4902-6482
* Department of Glass and Ceramics, Faculty of Chemical Technology, University of chemistry and Technology, Prague
* Technická 5, 166 28, Prague 6, Czech Republic

______Principal Investigator______
* Karel Bouzek
* ORCID: 0000-0002-0394-0634
* Dept. of Inorganic Technology, Faculty of Chemical Technology, University of chemistry and Technology, Prague
* Technicka 5, 166 28, Prague 6, Czech Republic

______Data manager or custodian______
* Šárka Paušová
* ORCID: 0000-0003-2494-1510
* Dept. of Inorganic Technology, Faculty of Chemical Technology, University of chemistry and Technology, Prague
* Technicka 5, 166 28, Prague 6, Czech Republic

______Licence______
* Dataset for Thermal Stability of Valuable Metals in Lithium-Ion Battery Cathode Materials: Temperature Range 500-800 °C © 2024 by Kristýna Jílková is licensed under CC BY
* licence information: https://creativecommons.org/licenses/by/4.0/

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______About the dataset______
The development of electric vehicles (EVs) is one of the fastest-growing segments in the automotive industry, closely linked to the advancement of lithium-ion batteries (LIBs). With the increasing number of EVs, the question of recycling used LIBs has emerged as a crucial issue. There are several methods for recycling the materials used in batteries, and two of the most promising ones are hydrometallurgy and pyrometallurgy. These methods involve subjecting materials to high temperatures. This article examines the cathode part of a lithium-ion battery, which is composed of NMC spinel 622 (LiNi0.6Mn0.2Co0.2O2), and investigates its stability during annealing at temperatures ranging from 500-800 °C. The quantity of remaining valuable metals lithium, nickel, manganese, and cobalt (Li, Ni, Mn, and Co) after exposure to these high temperatures was determined using inductively coupled plasma emission spectroscopy (ICP-OES) analysis. The correlation between element stability and the temperature of PVDF release, a binder in cathodes, was demonstrated by Differential thermal analysis (DTA). Confocal microscopy analysed material changes pre- and post-firing at 800 °C. Scanning electron microscopy with energy dispersive spectroscopy (SEM-EDS) performed local chemical analysis. X-ray diffraction characterised the crystalline structures of the original material and changes after annealing at 800 °C. This work builds on Part I, which focusses on the thermal stability of the material in lower temperature ranges. This research aimed to gain a deeper understanding of the pyrometallurgical aspect of the recycling process and identify the ideal annealing temperature for maximising the recovery of valuable metals. Additionally, the study sought to explore the potential use of a more environmentally friendly and economically viable solvent, demineralized water.

______Methods of data collection______
* Sample preparation
To prepare individual samples of the cathode composed of NMC spinel and aluminium foil, the battery module had to be disassembled. 
After the battery cells were opened, individual cathode layers composed of NMC spinel and aluminium foil were extracted from them. From these layers, squares measuring 25 x 25 mm were prepared. These samples were subjected to firing in a furnace from 500-800 °C for one hour. The fired samples were then cut into strips approximately 2 mm wide. Two parallel sets of processed material were prepared. In one set, the material was leached with constant stirring at laboratory temperature in demineralized water and in the second set, it was leached in 20% nitric acid. Each time, 0.1 g of each sample was leached in 25 mL of the respective solution. The time intervals at which the samples were leached in the solutions were determined based on our previous experiments (1.5 hours, 2 hours, and 4 hours). Subsequently, the 25 mL of the resulting solution was diluted in a 250 mL volumetric flask. The prepared solution was then filtered, and the 0.8 mL of the resulting filtrate was diluted 50 times and stored at laboratory temperature. 

* Scanning electron microscopy
TESCAN VEGA 3 LMU (SEM) in secondary electron (SE) and backscattered electron (BSE) modes was used for determination with VEGA3 software. The OXFORD Instruments INCA 350 EDS analyser enables chemical microanalysis of the observed sample, which is then evaluated in the AZtec software version 4.4. The composition was repeatedly measured on an area of 0.005 mm2.

* X-ray diffraction analysis: 
At room temperature using a PANanalytical X’Pert PRO θ-θ powder diffractometer featuring parafocusing Bragg-Brentano geometry, and CoKα radiation (λ = 1.79028 Å) at a 35 kV X-ray tube voltage and a current of 40 mA. Data acquisition utilised a high-speed detector X‘Celerator. Subsequent data analysis and interpretation were carried out using the software package HighScore Plus 4.0.

* DTA:
 Measured from 100 to 800 °C using Netzsch 404 EP system, with calibration made on phase transformation of α-SiO_2→β-SiO_2 at 576 °C. DTA analysis was conducted on the powder sample, weighing approximately 100 mg, in a corundum crucible in the air atmosphere. The sample was subjected to a constant heating/cooling rate of 10 °C/min, the temperature was controlled with temperature digital regulator from Clasic.

* ICP-OES:
Determined by the inductively coupled plasma emission spectrometer 5900 ICP-OES (Agilent, USA). The plasma was generated from the Ar flow using a water-cooled semiconductor radiofrequency generator with a frequency of 27 Hz and a power of 1.2 kW. The measurements were performed in the so-called synchronous vertical dual view (SVDV) mode, which allows measurements in axial and radial views simultaneously. Quantitative analysis was based on a five-point calibration series for each measured element, ranging from 0.2 to 1.0 mg/L. The results are based on three measurements of each sample.

______Methods of data processing______
The dataset contains raw data and tables including modified recalculated data for EDS analysis (Table 1), where only elements with a content above 1 wt.% were counted; from ICP-OES were calculated theoretical yields of valuable metals (Table 2a) and in Table 2b is shown the comparison of the efficiency [%] of the hydrometallurgical method and with the results of our work. 

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______File name structure_____
* VZx_000_111_XXXXX_Y_0000_v1
     VZx – research proposal (3 characters)
     000 – order of the publication in the research proposal (3 char.)
     111 – last 3 numerals of the superior indicator (3 char.)
     XXXXX – institution abbreviation (max. 5 char.)
          VSCHT - University of chemistry and technology, Prague
          CVUT - Czech Technical University
          UFCH - Institute of Physical Chemistry, Czech Academy of Sciences
          UK - Charles University
          VUT - Brno University of Technology
     Y – file type (1 char.):
          M – manuscript
          D – data
          S – supplementary information
          P – published version of the arctile
     0000 – order of the files in the dataset (4 char.)
     v1 – versioning (v + version number)

* example: VZ1_001_023_VSCHT_D_0001_v1.csv

______File formats______
* EDS reports - converted from DOCX to PDF/A
* XRD reports - converted from DOC to PDF/A
* DTA - original CSV
* ICP-OES - converted from XLSX to PDF/A (analytes calibrations) and CSV (measured data)
* Tabular data - converted from DOCX to TXT

______Date formats______
* DD-MM-YYYY (XRD), MM-DD-YYYY (EDS, ICP-OES)
* HH-MM-SS 24hr format (XRD), HH:MM:SS 12hr format (ICP-OES)


______Units and abbreviations______
* EDS reports raw data of chemical composition in wt.%, and map spectrum
* XRD reports raw data of phases compositions Counts (a.u.) vs Position (2Θ)
* DTA dta signal (mV) vs temperature (°C)
* ICP-OES concentration (mg/L) vs dissolution time (h)
* modified recalculated data Table 1 chemical composition in wt.%, recalculated data from ICP-OES measurements (Table 2a) theoretical yields and data of efficiency from literature compared with our data (Table 2b)


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______List of files______
* In this file can be found content of raw data from DTA report for NMC sample, for the article Thermal Stability of Valuable Metals in Lithium-Ion Battery Cathode Materials: Part II - Temperature Range 500-800 °C.
VZ1_001_021_VSCHT_D_0001.csv

* In these files can be found content of raw data from EDS reports for NMC samples for temperature range from 500-800°C, for the article Thermal Stability of Valuable Metals in Lithium-Ion Battery Cathode Materials: Part II - Temperature Range 500-800 °C.
VZ1_001_021_VSCHT_D_0002.pdf
VZ1_001_021_VSCHT_D_0003.pdf
VZ1_001_021_VSCHT_D_0004.pdf
VZ1_001_021_VSCHT_D_0005.pdf
VZ1_001_021_VSCHT_D_0006.pdf
VZ1_001_021_VSCHT_D_0007.pdf
VZ1_001_021_VSCHT_D_0008.pdf
VZ1_001_021_VSCHT_D_0009.pdf

* In these files can be found content of raw data from ICP-OES measurements for NMC samples for temperature range from 500-800°C, for the article Thermal Stability of Valuable Metals in Lithium-Ion Battery Cathode Materials: Part II - Temperature Range 500-800 °C.
VZ1_001_021_VSCHT_D_0010.pdf
VZ1_001_021_VSCHT_D_0011.csv
VZ1_001_021_VSCHT_D_0012.pdf
VZ1_001_021_VSCHT_D_0013.csv
VZ1_001_021_VSCHT_D_0014.pdf
VZ1_001_021_VSCHT_D_0015.csv
VZ1_001_021_VSCHT_D_0016.pdf
VZ1_001_021_VSCHT_D_0017.csv

* In these files can be found content of modified raw data for tables with content from EDS, and calculated theoretical yields and comparison of efficiency with our study for NMC samples for temperature range from 500-800°C, for the article Thermal Stability of Valuable Metals in Lithium-Ion Battery Cathode Materials: Part II - Temperature Range 500-800 °C.
VZ1_001_021_VSCHT_D_0018.txt
VZ1_001_021_VSCHT_D_0019.txt
VZ1_001_021_VSCHT_D_0020.txt

* In these files can be found content of raw data from XRD reports for NMC samples for temperatures 0 and 800°C, for the article Thermal Stability of Valuable Metals in Lithium-Ion Battery Cathode Materials: Part II - Temperature Range 500-800 °C.
VZ1_001_021_VSCHT_D_0021.pdf
VZ1_001_021_VSCHT_D_0022.pdf