Angew Chem Int Ed Engl
May 2025
Developing sacrificial cathode prelithiation technology to compensate for irreversible lithium loss is crucial for enhancing the energy density of lithium-ion batteries. Antifluorite Li-rich LiFeO (LFO) is a promising prelithiation agent due to its high theoretical capacity (867 mAh g) and superior decomposition dynamic (<4.0 V vs.
View Article and Find Full Text PDFJ Am Chem Soc
November 2024
Extending the depth-of-charge (DoC) of the layered oxide cathode presents an essential route to improve the competitiveness of the Na-ion battery versus the commercialized LiFePO-based Li-ion battery (0.8 CNY/Wh). However, the DoC-dependent boundary between detrimental/irreversible structural distortion and neutral/reversible structure interconversion cannot be clearly distinguished, which is attributed to the ambiguous recognition of correlation among the complex phase transition, local covalent environment evolution, and charge compensation.
View Article and Find Full Text PDFAfter charging to a high state-of-charge (SoC), layered oxide cathodes exhibit high capacities but suffer from gliding-induced structural distortions caused by deep Li depletion within alkali metal (AM) layers, especially for high-nickel candidates. In this study, we identify the essential structure of the detrimental H3 phase formed at high SoC to be an intergrowth structure characterized by random sequences of the O3 and O1 slabs, where the O3 slabs represent Li-rich layers and the O1 slabs denote Li-depleted (or empty) layers that glide from the O3 slabs. Moreover, we adopt two doping strategies targeting different doping sites to eliminate the formation of Li-vacant O1 slabs.
View Article and Find Full Text PDFDeveloping sacrificial cathode prelithiation technology to compensate for active lithium loss is vital for improving the energy density of lithium-ion battery full-cells. LiCO owns high theoretical specific capacity, superior air stability, but poor conductivity as an insulator, acting as a promising but challenging prelithiation agent candidate. Herein, extracting a trace amount of Co from LiCoO (LCO), a lattice engineering is developed through substituting Li sites with Co and inducing Li defects to obtain a composite structure consisting of (LiCo▫)CO and ball milled LiCoO (Co-LiCO@LCO).
View Article and Find Full Text PDFBoth LiFePO (LFP) and NaFePO (NFP) are phosphate polyanion-type cathode materials, which have received much attention due to their low cost and high theoretical capacity. Substitution of manganese (Mn) elements for LFP/NFP materials can improve the electrochemical properties, but the connection between local structural changes and electrochemical behaviors after Mn substitution is still not clear. This study not only achieves improvements in energy density of LFP and cyclic stability of NFP through Mn substitution, but also provides an in-depth analysis of the structural evolutions induced by the substitution.
View Article and Find Full Text PDFJ Am Chem Soc
April 2023
Element doping/substitution has been recognized as an effective strategy to enhance the structural stability of layered cathodes. However, abundant substitution studies not only lack a clear identification of the substitution sites in the material lattice, but the rigid interpretation of the transition metal (TM)-O covalent theory is also not sufficiently convincing, resulting in the doping/substitution proposals being dragged into design blindness. In this work, taking LiNiMnO as a prototype, the intense correlation between the "disordered degree" (Li/Ni mixing) and interface-structure stability (e.
View Article and Find Full Text PDFThe prominent problem with graphite anodes in practical applications is the detrimental Li plating, resulting in rapid capacity fade and safety hazards. Herein, secondary gas evolution behavior during the Li-plating process was monitored by online electrochemical mass spectrometry (OEMS), and the onset of local microscale Li plating on the graphite anode was precisely/explicitly detected in situ/operando for early safety warnings. The distribution of irreversible capacity loss (e.
View Article and Find Full Text PDFAnode-free lithium metal batteries (AF-LMBs) can deliver the maximum energy density. However, achieving AF-LMBs with a long lifespan remains challenging because of the poor reversibility of Li plating/stripping on the anode. Here, coupled with a fluorine-containing electrolyte, we introduce a cathode pre-lithiation strategy to extend the lifespan of AF-LMBs.
View Article and Find Full Text PDF