Fig 1

Fundamentals, challenges and AI-centered strategies for green cathode slurry systems."

Fig 2

(a) Schematic of polymer dissolution process in solvents [39]; (b) Effect of mixing speed on material interaction in cathode slurry [40]; (c) Three common thermodynamic calculations to predict polymer solubility [41]; (d) Rheology using shear rheometers for measurement of motion resistance in a shear flow [42]."

Fig 3

(a) Schematic illustration of the drying of a particulate film for the production of a battery electrode [61]; (b) Geometries employed in peel tests of electrodes [71]; (c) Reconstructed volume of NMC cathode with different phases based on X-ray CT data [72]; (d) Cross-sectional SEM image and fluorine elemental map for electrodes dried at different temperatures [73]."

Fig 4

(a) Schematic of large-scale manufacturing of next-generation batteries [84]; (b, c) Surface (left) and cross-section (right) SEM images of DMSO-coated electrodes before calendering; (d, e) SEM images of NMP-coated electrodes; (f) Viscosity vs. shear rate of slurries using DMSO and NMP solvents (inset is photos of DMSO-based slurry after casting and drying); (g) Cycling performances of electrodes using DMSO and NMP slurries; (h) C-rate performances of cathodes from 0.1C to 5C [90]."

Fig 5

(a) Surface morphology characterization of NMC88 cathode prepared from (a) NMP (left) and DMF (right) slurries; (b) TGA analysis of formulated slurries; (c) Elemental distribution for DMF-coated NMC88 cathode; (d) Influence solvent on the specific capacity of NMC88 cathodes [95]; (e, f) Cross-section images of cathode using NMP (upper) and MDMPA (lower) slurries; (g) Cycling performances of cathodes; (h) EIS spectra at 1st, 150th, 700th and 1000th cycles [96]."

Fig 6

(a) Hansen solubility map of various solvents; (b) Rheology of NMP and GVL slurries as a function of shear rate; (c) Rate capability of electrodes higher with mass loading [49]; (d) Snapshots of PVDF chain conformation in NMP (left) and TEP (right) solvents via molecular dynamics simulations; (e) MSD for the PVDF polymer chains in NMP and TEP solvents [103]; (f) Charge-discharge voltage profile of the initial cycle; (g) Cycle stability over 100 cycles at C/3; (h) DRT from 106 to 0.1 Hz for TEP- and NMP-based NMC622 coin-cells [104]."

Fig 7

(a) Surface electrostatic potentials of Cyrene and solute molecules [109]; (b) Cyrene-slurry-prepared NCM 811 cathode with high mass loading [110]; (c) Graphical representation of HSPs (δd, δp, δh) of typical polymers with DMI and the most used solvents [111]; (d) Cycling performances of the electrodes made using PolarClean slurry processed at room temperature [85]. "

Table 1

Physical and nickel-rich cathode electrochemical characteristics of various green solvents discussed in this review."

Fig 8

(a) Physical aspects of dissolution process of solid and corresponding descriptors; (b) Descriptor correlation analysis [125]; (c) Comparison between model predictions and experimental results for NMC-111 simulations in the test dataset [126]; (d) Simulation acceleration of slurry drying stage enabled by DL-DEM modeling workflow [127]; (e) Matrix representation of data partitioning strategy for training multiple ANN prediction models [128]."