Direct recycling of lithium-ion batteries (LIBs) focuses on the development of environmentally friendly methods for recycling and upcycling spent electrode materials, thereby facilitating the creation of a circular economy for LIB materials [1]. A key emphasis of our work lies in evaluating the economic benefits and diminished carbon footprint associated with direct recycling compared to prevalent commercialized methods. We also acknowledge the challenges inherent in realizing the full industrial-scale potential of this methodology [2]. A noteworthy advancement within our laboratory involves the integration of pretreatment and relithiation processes, showcasing both scalability and the universality of chemical processes [3, 4, 5].

Representative publications:
[1] Xu, Panpan, et al. A Materials Perspective on Direct Recycling of Lithium‐Ion Batteries: Principles, Challenges and Opportunities, Advanced Functional Materials, 2023, 33, 2213168. Found here.
[2] Xu, Panpan, et al. Efficient Direct Recycling of Lithium-Ion Battery Cathodes by Targeted Healing, Joule, 2020, 4(12), 2609-2626. Found here.
[3] Gupta, Varun, et al. Scalable Direct Recycling of Cathode Black Mass from Spent Lithium‐Ion Batteries, Advanced Energy Materials, 2023, 113, 2203093. Found here.
[4] Gao, Hongpeng, et al. Efficient Direct Recycling of Degraded LiMn2O4 Cathodes by One-Step Hydrothermal Relithiation, 2020, ACS Applied Materials and Interfaces, 2020, 12, 46, 51546–51554. Found here.
[5] Gao, Hongpeng, et al. Upcycling of Spent LiNi0.33Co0.33Mn0.33O2 to Single-Crystal Ni-Rich Cathodes Using Lean Precursors, ACS Energy Letters, 2023, 8, 10, 4136–4144. Found here.

Our research on energy storage materials focuses on improving both safety and performance. Strategies involve integrating thermo-responsive polymer switching materials (TRPS) into battery electrodes through solvent-based processes and conductive fillers such as Tungsten carbide [1-4]. We explore TRPS because they show promise in rapid resistance switching for effective battery thermal regulation.

Representative publications:
[1] Li, Mingqian, et al. Thermo-responsive Polymers for Thermal Regulation in Electrochemical Energy Devices, Journal of Polymer Science, 2021, 59(20), 2230. Found here.
[2] Li, Mingqian, et al. Scalable Solvent-Based Fabrication of Thermo-Responsive Polymer Nanocomposites for Battery Safety Regulation,  Journal of The Electrochemical Society, 2021,168(8), 080507. Found here.
[3] Li, Mingqian, et al. Hierarchically Structured Metal Carbides as Conductive Fillers in Thermo-Responsive Polymer Nanocomposites for Battery Safety, Nano Energy, 2022, 103, 107726. Found here.
[4] Li, Mingqian, et al. Bio-Inspired Nanospiky Metal Particles Enable Thin, Flexible and Thermo-Responsive Polymer Nanocomposites for Thermal Regulation, Advanced Functional Materials, 2020, 30(23), 1910328. Found here.

"All-solid-state batteries (ASSBs) offer superior safety and higher energy density compared to traditional lithium-ion batteries [1]. Our lab is focused on addressing both the scientific and technical obstacles that hinder the practical implementation of ASSBs at the lab and industrial scales. One area of study involves the use of machine learning to optimize the production of high-quality solid-state electrolyte (SSE) films [2]. Additionally, we also explore the dry process as a promising fabrication method for ASSBs to reduce energy consumption. Controlling binder fibrillation in this process enables the creation of physio-electrochemically durable SSE films, improving cycling stability and charge storage capability in ASSBs [3]

Representative publications:
[1] Tan, D. H. S., et al. Sustainable Design of Fully Recyclable All Solid-State Batteries, MRS Bulletin, 2020, December 10, 990-991. (MRS Energy Quarterly Invited Article). Found here.
[2] Chen, Y.-T., et al. Fabrication of High-Quality Thin Solid-State Electrolyte Films Assisted by Machine Learning, ACS Energy Letters, 2021, 6, 1639-1648. Found here.
[3] Lee, D. J., et al. Physio‐Electrochemically Durable Dry‐Processed Solid‐State Electrolyte Films for All‐Solid‐State Batteries, Advanced Functional Materials, 2023, 33, 2301341. Found here.

We design electrolyte systems to enhance electrochemical performance of cells operating at ultra-low temperature conditions. Our group have discovered that by confining liquefied gas electrolytes in nanoscale pores and introducing ion-pairing for advanced Li metal full-cell batteries, stable operations at the cell level can be achieved at -40 °C [1]. Further advancements in our group have enabled stable cycling, even under conditions as extreme as -60°C for different battery systems [2, 3, 4].

Representative publications:
[1] Holoubek, John, et al. Tailoring electrolyte solvation for Li metal batteries cycled at ultra-low temperature, Nature Energy, 2021, 6, 303-313. Found here.
[2] Holoubek, John, et al. Exploiting Mechanistic Solvation Kinetics for Dual-Graphite Batteries with High Power Output at Extremely Low Temperature, Angewandte Chemie International Edition, 2019, 58(52), 18892-18897. Found here.
[3] Yin, Yijie, et al. Ultra-Low Temperature Li/CFx Batteries Enabled by Fast-transport and Anion-pairing Liquefied Gas Electrolytes, Advanced Materials, 2022, 2200099, DOI: 10.1002/adma.202207932. Found here.
[4] Holoubek, John, et al., Toward a quantitative interfacial description of solvation for Li metal battery operation under extreme conditions, Proceedings of the National Academy of Sciences, 2023, 120, 41, e2310714120. Found here.

Metal-organic frameworks (MOFs) are a class of porous crystalline materials comprised of metal nodes coordinated to organic ligands, leading to high porosity, tunable compositions, and well-ordered networks. Our research focuses on exploiting the distinct properties of MOFs to confine and facilitate ion transport, host active materials, and selectively screen ions for next-generation battery materials.

Representative publications:
[1] Cai, Guorui, et al. Sub-nanometer confinement enables facile condensation of gas electrolyte for low-temperature batteries, Nature Communications, 2021, 12, 3395. Found here.
[2] Cai, Guorui, et al. Unravelling Ultrafast Li Ion Transport in Functionalized Metal–Organic Framework-Based Battery Electrolytes, Nano Letters, 2023, 23, 15, 7062–7069. Found here.

Sodium-ion batteries (SIBs) emerge as one of the most promising candidates in application of large-scale energy storage and cheaper replacement for LIBs. However, SIBs usually suffer from lower capacity and energy density. We are focusing on developing advanced SIB electrodes to enhance energy density by two different methods. First, we develop novel and advanced electrode materials with higher specific capacity and energy density. Second, we optimize the electrode manufacturing process to reduce inactive components in electrodes and further promote energy density.

Representative publications:
[1] Yabuuchi, Naoaki, et al. Research Development on Sodium-Ion Batteries, Chemical Reviews, 2014, 114, 11636-11682.

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