Abstract
Recycling of spent lithium-ion batteries (LIBs) is an urgent need to address their environmental and global sustainability issues. Here, we report an efficient and environmentally benign LIB regeneration method based on defect-targeted healing, which represents a paradigm-shift LIB recycling strategy. Specifically, by combining low-temperature aqueous solution relithiation and rapid post-annealing, we demonstrate successful direct regeneration of spent LiFePO4 (LFP) cathodes, one of the most important materials for EVs and grid storage applications. We show revitalization of composition, structure, and electrochemical performance of LFP with various degradation conditions to the same levels as the pristine LFP. Life-cycle analysis of different LIB recycling processes shows that this defect-targeted direct reycling approach can significantly reduce energy usage and greenhouse gas (GHG) emissions, leading to more economic and environmental benefits compared with today's hydrometallurgical and pyrometallurgical methods. The consumption of lithium-ion batteries is experiencing booming growth in the modern industry due to their widespread applications. With billions of batteries reaching their lifetime soon, significant concerns on the economic and environmental issues have been raised about how to treat these spent batteries so that our society will not face similar crisis incurred in the case of plastic wastes. However, traditional technologies used in today's recycling industry are limited to recovering expensive metals through energy-intensive processes, which cause significant greenhouse gas emissions and secondary wastes, posing additional environmental concerns. To tackle this challenge, we developed a safe, low-cost, and efficient direct recycling approach that is based on targeted healing. This paradigm-shift method leverages our understanding on phase and structure evaluations of the LIB cathode and produces ready-to-use recycled cathode materials that match the electrochemical performance of pristine materials. A paradigm-shift lithium-ion battery recycling method based on defect-targeted healing can fully recover the composition, structure, and electrochemical performance of spent LiFePO4 cathodes with various degradation conditions to the same levels as that of the pristine materials. Such a direct recycling approach can significantly reduce energy usage and greenhouse gas emissions, leading to significant economic and environmental benefits compared with today's hydrometallurgical and pyrometallurgic methods. This work may pave the way for industrial adoption of directly recycled lithium-ion battery materials.
| Original language | English |
|---|---|
| Pages (from-to) | 2609-2626 |
| Number of pages | 18 |
| Journal | Joule |
| Volume | 4 |
| Issue number | 12 |
| DOIs | |
| State | Published - Dec 16 2020 |
Funding
This work was supported by US National Science Foundation via award CBET-1805570 (for experimental work), US Department of Energy via ReCell Center (for EverBatt modeling work), and the start-up fund support from the Jacob School of Engineering at UC San Diego to Z.C.; M.Z. and Y.S.M. acknowledge the funding support from Zable Endowed Chair Fund . We acknowledge the UC Irvine Materials Research Institute for the use of the (S)TEM facilities, funded, in part, by the NSF Major Research Instrumentation Program under grant CHE-1338173 . The part of the work at Argonne National Laboratory was supported from the U. S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy , Vehicle Technologies Office . Argonne National Laboratory is operated for DOE Office of Science by UChicago Argonne, LLC, under contract number DE-AC02-06CH11357. A portion of the work used the UCSD-MTI Battery Fabrication Facility and the UCSD-Arbin Battery Testing Facility. The neutron diffraction work used resources at the Spallation Neutron Source, a US Department of Energy (DOE) Office of Science User Facility operated by the Oak Ridge National Laboratory . We thank Ms. S.B. for assistance on TEM characterization. The authors also thank Prof. Jeff Dahn at Dalhousie University for comments and suggestions on the experiment and the revision of the manuscript. This work was supported by US National Science Foundation via award CBET-1805570 (for experimental work), US Department of Energy via ReCell Center (for EverBatt modeling work), and the start-up fund support from the Jacob School of Engineering at UC San Diego to Z.C.; M.Z. and Y.S.M. acknowledge the funding support from Zable Endowed Chair Fund. We acknowledge the UC Irvine Materials Research Institute for the use of the (S)TEM facilities, funded, in part, by the NSF Major Research Instrumentation Program under grant CHE-1338173. The part of the work at Argonne National Laboratory was supported from the U. S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office. Argonne National Laboratory is operated for DOE Office of Science by UChicago Argonne, LLC, under contract number DE-AC02-06CH11357. A portion of the work used the UCSD-MTI Battery Fabrication Facility and the UCSD-Arbin Battery Testing Facility. The neutron diffraction work used resources at the Spallation Neutron Source, a US Department of Energy (DOE) Office of Science User Facility operated by the Oak Ridge National Laboratory. We thank Ms. S.B. for assistance on TEM characterization. The authors also thank Prof. Jeff Dahn at Dalhousie University for comments and suggestions on the experiment and the revision of the manuscript. Z.C. conceived the idea, designed the experiment, and directed the project. P.X. carried out the synthesis, processing and electrochemical evaluations and analyzed the data. P.X. and Q.D. performed the economic and environmental modeling. H.G. assisted the experiment design and studied the relithiation kinetics. H.L. Y.C. and K.A. assisted with neutron diffraction characterization. M.Z. collected and analyzed the (S)TEM and EELS data. M.L. made the pouch cells. P.X. and Z.C. wrote the manuscript. Y.S.M. P.L. Y.L. J.S.S. L.G. and J.L. revised the manuscript and interacted with other authors regarding experiment design and data analysis. All the authors discussed the results and commented on the manuscript. A patent was filed for this work through the UCSD Office of Innovation and Commercialization.
| Funders | Funder number |
|---|---|
| Jacob School of Engineering at UC San Diego | |
| Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office | |
| U. S. Department of Energy | |
| UCSD-Arbin Battery Testing Facility | |
| UCSD-MTI Battery Fabrication Facility | |
| US Department of Energy | |
| US National Science Foundation | |
| National Science Foundation | CHE-1338173, CBET-1805570 |
| U.S. Department of Energy | |
| Office of Science | |
| Office of Energy Efficiency and Renewable Energy | DE-AC02-06CH11357 |
| Oak Ridge National Laboratory | |
| UC Irvine Materials Research Institute |
Keywords
- cathode
- life cycle analysis
- lithium-ion batteries
- recycling
- relithiation
- structure defects
- sustainability
