journal article·2026-07-12Open access

Electrochemical and Thermal Interplay in Blended Cathodes for All Solid‐State Batteries

Simon Si Ming Ji, Zhuo Li, Abhinand Ayyaswamy, Sascha Kremer, Shintaro Inaba, Ana G. Claus, Dayoung Jun, Se Hwan Park, Moonseong Kim, Bairav S. Vishnugopi, Hui Zhong, Sanjit Ghose, Michael Drakopoulos, Nghia T. Vo, Zhong Zhong, Jürgen Janek, Partha P. Mukherjee, Kelsey B. Hatzell

Abstract

ABSTRACT We investigate composite solid state blended cathodes composed of lithium iron phosphate (LFP), nickel cobalt manganese oxide (NMC), and halide solid electrolyte for application in all solid state batteries (ASSBs). Electrochemical characterization indicates that the blended cathode integrates the high rate capability of LFP with the high specific capacity of NMC. Synchrotron X‐ray diffraction (XRD) techniques, including spatially resolved operando micro‐diffraction, reveal asymmetric charge distribution, and lithiation gradients across the cathode depth during electrochemical cycling. Complementary thermal modeling demonstrates that the blended cathode generates less heat than pure NMC, thereby enhancing thermal stability. These results highlight the potential of blended cathodes to achieve an optimal balance between performance and safety in ASSBs and provide valuable insights for the design of microstructures for next‐generation solid state battery systems.
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Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Advancements in Battery Materials · Thermal Expansion and Ionic Conductivity

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Mechanical and Aerospace Engineering Princeton University Princeton New Jersey USA

Andlinger Center for Energy and Environment Princeton University Princeton New Jersey USA

School of Mechanical Engineering Purdue University West Lafayette Indiana USA

Institute of Physical Chemistry and Center for Materials Research Justus‐Liebig‐University Giessen Giessen Germany

Department of Physics Swarthmore College Swarthmore Pennsylvania USA

School of Materials Science and Engineering Kookmin University Seoul Republic of Korea

National Synchrotron Light Source II Brookhaven National Laboratory Upton New York USA

Funding

U.S. Department of Energy · Office of Naval Research

References (48)

Show source-provided references
1. High‐Rate Blended Cathode with Mixed Morphology for All‐Solid‐State Li‐Ion Batteries10.33961/jecst.2019.00661 ↗
2. A Solid Future for Battery Development10.1038/nenergy.2016.141 ↗
3. Designing Cathodes and Cathode Active Materials for Solid‐State Batteries10.1002/aenm.202201425 ↗
4. Operando Investigation on the Role of Densification and Chemo‐Mechanics on Solid‐State Cathodes10.1002/aenm.202304544 ↗
5. Chemo‐Mechanical Behavior and Stability of High‐Loading Cathodes in Solid‐State Batteries10.1021/acsnano.5c04431 ↗
6. Visualizing the Impact of the Composite Cathode Microstructure and Porosity on Solid‐State Battery Performance10.1149/1945-7111/ad510e ↗
7. Challenges and Recent Progress in Fast‐Charging Lithium‐Ion Battery Materials10.1016/j.jpowsour.2023.232965 ↗
8. Toward High Rate Performance Solid‐State Batteries10.1002/aenm.202200948 ↗
9. Challenges in Speeding Up Solid‐State Battery Development10.1038/s41560-023-01208-9 ↗
10. Morphological Heterogeneity Impact of Film Solid‐State Cathode on Utilization and Fracture Dynamics10.1021/acsnano.5c06799 ↗
11. A Cost‐Effective and Humidity‐Tolerant Chloride Solid Electrolyte for Lithium Batteries10.1038/s41467-021-24697-2 ↗
12. Designing Lithium Halide Solid Electrolytes10.1038/s41467-024-45258-3 ↗
13. Microstructural Modeling of Composite Cathodes for All‐Solid‐State Batteries10.1021/acs.jpcc.8b11043 ↗
14. Impact of the Solid Electrolyte Particle Size Distribution in Sulfide‐Based Solid‐State Battery Composites10.1002/aenm.202302309 ↗
15. Impact of Cathode Material Particle Size on the Capacity of Bulk‐Type All‐Solid‐State Batteries10.1021/acsenergylett.8b00275 ↗
16. Co‐Design of Active Material and Solid Electrolyte Particulate Phases in Solid‐State Battery Composite Electrodes10.1021/acsami.5c10908 ↗
17. 10.1021/acsenergylett.4c0074410.1021/acsenergylett.4c00744 ↗
18. Quantifying the Impact of Cathode Composite Mixing Quality on Active Mass Utilization and Reproducibility of Solid‐State Battery Cells10.1002/aenm.202405405 ↗
19. A Cost‐Effective All‐in‐One Halide Material for All‐Solid‐State Batteries10.1038/s41586-025-09153-1 ↗
20. Blended Cathode Materials for All‐Solid‐State Li‐Ion Batteries10.1016/j.jallcom.2018.12.025 ↗
21. Understanding Charge Transfer Dynamics in Blended Positive Electrodes for Lithium‐Ion Batteries
22. Recent Insights into the Electrochemical Behavior of Blended Lithium Insertion Cathodes: A Review10.1016/j.electacta.2018.02.165 ↗
23. Comparative Study on Experiments and Simulation of Blended Cathode Active Materials for Lithium Ion Batteries10.1016/j.electacta.2015.11.029 ↗
24. Chemo‐Mechanical Expansion of Lithium Electrode Materials—On the Route to Mechanically Optimized All‐Solid‐State Batteries10.1039/C8EE00907D ↗
25. A Reflection on Lithium‐Ion Battery Cathode Chemistry10.1038/s41467-020-15355-0 ↗
26. Phospho‐Olivines as Positive‐Electrode Materials for Rechargeable Lithium Batteries10.1149/1.1837571 ↗
27. Evolution of Structure and Lithium Dynamics in LiNi0.8${\rm LiNi}0.8$Mn0.1${\rm Mn}0.1$Co0.1${\rm Co}0.1$O2${\rm O}_2$ (NMC811) Cathodes During Electrochemical Cycling10.1021/acs.chemmater.9b00140 ↗
28. Li‐Ion Battery Materials: Present and Future10.1016/j.mattod.2014.10.040 ↗
29. Understanding Kinetic and Thermodynamic Properties of Blended Cathode Materials for Lithium‐Ion Batteries10.1016/j.mtener.2021.100845 ↗
30. Synergistic Effect Between LiNi0.5${\rm LiNi}0.5$Co0.2${\rm Co}0.2$Mn0.3${\rm Mn}0.3$O2${\rm O}_2$ and LiFe0.15${\rm LiFe}0.15$Mn0.85${\rm Mn}0.85$PO4${\rm PO}_4$/C on Rate and Thermal Performance for Lithium Ion Batteries
31. Reversible Heat Generation Rates of Blended Insertion Electrodes10.1007/s10008-017-3594-3 ↗
32. A Reduced Order Electrochemical and Thermal Model for a Pouch Type Lithium Ion Polymer Battery with LiNix${\rm LiNi}_x$Mny${\rm Mn}_y$Co1−x−y${\rm Co}1-x-y$O2${\rm O}_2$/LiFePO4${\rm LiFePO}_4$ Blended Cathode10.1016/j.jpowsour.2015.06.090 ↗
33. The State of Reliable Characterization and Testing of Solid‐State Batteries10.1021/acsenergylett.5c00923 ↗
34. Operando EDXRD Study of All‐Solid‐State Lithium Batteries Coupling Thioantimonate Superionic Conductors with Metal Sulfide10.1002/aenm.202002861 ↗
35. Heterogeneities Affect Solid‐State Battery Cathode Dynamics10.1016/j.ensm.2022.11.055 ↗
36. Synchrotron Operando Depth Profiling Studies of State‐of‐Charge Gradients in Thick Li(Ni0.8${\rm Ni}0.8$Mn0.1${\rm Mn}0.1$Co0.1${\rm Co}0.1$)O2${\rm O}_2$ Cathode Films10.1021/acs.chemmater.0c00983 ↗
37. Overcoming the Interfacial Challenges of LiFePO4${\rm LiFePO}_4$ in Inorganic All‐Solid‐State Batteries10.1021/acsenergylett.2c02138 ↗
38. Phytic Acid Derived LiFePO4${\rm LiFePO}_4$ Beyond Theoretical Capacity as High‐Energy Density Cathode for Lithium Ion Battery10.1016/j.nanoen.2017.03.006 ↗
39. Comparison on Thermal Runaway and Critical Characteristics of Cylindrical Lithium‐Ion Batteries: A Review10.1021/acs.chas.4c00121 ↗
40. Low‐Cost Iron Trichloride Cathode for All‐Solid‐State Lithium‐Ion Batteries10.1038/s41893-024-01431-6 ↗
41. Navigating Battery Choices: A Comparative Study of Lithium Iron Phosphate and Nickel Manganese Cobalt Battery Technologies10.1016/j.fub.2024.100007 ↗
42. Surface Reconstruction and Chemical Evolution of Stoichiometric Layered Cathode Materials for Lithium‐Ion Batteries10.1038/ncomms4529 ↗
43. Battery Materials for Ultrafast Charging and Discharging10.1038/nature07853 ↗
44. Irreversible Phase Transition Between LiFePO4${\rm LiFePO}_4$ and FePO4${\rm FePO}_4$ During High‐Rate Charge‐Discharge Reaction by Operando X‐ray Diffraction10.1016/j.jpowsour.2016.01.077 ↗
45. Lithiation Gradients and Tortuosity Factors in Thick NMC111‐Argyrodite Solid‐State Cathodes10.1021/acsenergylett.2c02699 ↗
46. HEX: A New High Energy Beamline at NSLS‐II10.1080/08940886.2024.2312071 ↗
47. GSAS‐II: The Genesis of a Modern Open‐Source All Purpose Crystallography Software Package10.1107/S0021889813003531 ↗
48. TOPAS and TOPAS‐Academic: An Optimization Program Integrating Computer Algebra and Crystallographic Objects Written in C++10.1107/S1600576718000183 ↗