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The advanced lithium-ion batteries that can tolerate zero-volt storage (ZVS) are in high demand for implantable medical devices and spacecraft. However, ZVS can raise the anode potential, leading to Cu current collector dissolution and solid-electrolyte interphase (SEI) degradation, especially at 37 °C. In this contribution, by quantitatively regulating the dosage of LiCoO cathode additives, controllable potential of the working anode under abusive-discharge conditions is demonstrated. The addition of LiCoO keeps zero-crossing potential (ZCP) and the potential of ZVS below 2.0 V (vs Li/Li) for LiCoO|mesocarbon microbead cells at 37 °C. The capacity retention ratio (CRR) increases from 69.1% and 35.9% to 98.6% and 90.8% after 10 and 20 days of ZVS, respectively. The Cu dissolution and SEI degradation are effectively suppressed, while the over-lithiated cathode exhibits high reversible capacity after ZVS. The limiting conditions of long-term ZVS are further explored and a corresponding guide map is designed. When quantitatively regulating ZCP and the potential in ZVS, Cu dissolution, SEI degradation, and irreversible conversion of the cathode constitute the limiting conditions. This contribution designs the most reasonable potential range for ZVS protection at 37 °C, and realizes the best CRR record through precise potential regulation for the first time.
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http://dx.doi.org/10.1002/adma.202400656 | DOI Listing |
J Vis Exp
August 2025
Tencent Quantum Laboratory;
Electrolytes are important components in lithium-ion batteries. However, battery degradation due to irreversible electrochemical reactions in the electrolyte can consume electrolyte molecules and severely reduce its effective operation lifetime. It is hence important to study the electrochemical reaction pathways in the battery electrolyte to further improve lithium-ion battery reliability.
View Article and Find Full Text PDFAdv Mater
September 2025
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, China.
The detrimental effects of Fe-ion crosstalk on LiFePO||Graphite battery performance, coupled with limited mechanistic insights into solid electrolyte interphase (SEI) evolution under such interference, warrant systematic investigation. Herein, advanced characterization techniques-including X-ray photoelectron spectroscopy, time-of-flight secondary ion mass spectrometry, and cryogenic transmission electron microscopy-are employed to reveal SEI evolution on graphite anodes under Fe/Fe influence. Results demonstrate that Fe exerts more severe adverse effects than Fe.
View Article and Find Full Text PDFSci Data
August 2025
Department of Energy Science & Engineering, Stanford University, 367 Panama St., Stanford, 94305, CA, USA.
High-power lithium-ion battery (LIB) applications, such as electric racing cars and electric vertical take-off and landing (eVTOL) aircrafts, are growing rapidly. Degradation in LIBs such as lithium plating, particle cracking, and SEI breakdown is accelerated at high C-rate at different temperatures and depth-of-discharges (DOD); however, high-power cells are designed to better withstand these operating conditions as compared to high-energy cells. Despite this, publicly available datasets of high-power batteries are limited.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
August 2025
Guangdong Provincial Key Laboratory of Advanced Energy Storage Materials, School of Materials Science and Engineering, South China University of Technology, Guangzhou, 510641, China.
The development of solid electrolyte interfaces (SEI) using lithium and nitrate salts represents a promising approach to enhancing the performance of lithium metal batteries (LMBs). However, the inherent stability of lithium and nitrate salts often results in incomplete decomposition, leading to the formation of inhomogeneous SEI that degrade battery performance. In this study, a strong dipole moment and increased charge transfer strategy are used, which can effectively catalyze the decomposition of NO and TFSI and accelerate the migration of Li, as well as the formation of LiN-LiF-rich SEI.
View Article and Find Full Text PDFJ Phys Chem C Nanomater Interfaces
August 2025
Department of Chemical Engineering, Department of Chemistry, Department of Materials Science and Engineering, Texas A&M University, College Station, Texas 77843, United States.
In this work, we report the results of a theoretical-computational analysis of the solid electrolyte interphase (SEI) growth and degradation dynamics occurring in lithium metal batteries during cycling. We use ab initio-kinetic Monte Carlo simulations to generate a synthetic data set, which is analyzed by machine learning methods. We aim to determine: (i) how modifications in interfacial interaction energies between solid electrolyte interphase (SEI) blocks and between Li ions and SEI facets impact the Coulombic efficiency (CE) of the battery and (ii) what factors, including reactions, microscopic transport, and other interfacial events, may lead to cell performance "failure" during prolonged charge and discharge cycles, signaled as a sharp decay in the CE over cycling.
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