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Keywords = artificial interphase film

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34 pages, 3599 KB  
Review
Challenges and Issues in Using Coated and Uncoated Graphitic Anodes in Lithium-Ion Batteries
by Keerthan Nagendra, Koorosh Nikgoftar, Anil Kumar Madikere Raghunatha Reddy, Jitendrasingh Rajpurohit, Jeremy I. G. Dawkins, Thiago M. Guimaraes Selva and Karim Zaghib
Batteries 2026, 12(5), 154; https://doi.org/10.3390/batteries12050154 - 25 Apr 2026
Viewed by 1439
Abstract
Graphite remains the predominant negative electrode material in commercial lithium-ion batteries (LIBs); however, its practical performance is increasingly limited by interface-driven degradation rather than bulk intercalation. This review examines the interconnected electrochemical, mechanical, and safety challenges associated with uncoated and coated graphite, with [...] Read more.
Graphite remains the predominant negative electrode material in commercial lithium-ion batteries (LIBs); however, its practical performance is increasingly limited by interface-driven degradation rather than bulk intercalation. This review examines the interconnected electrochemical, mechanical, and safety challenges associated with uncoated and coated graphite, with particular focus on how solid electrolyte interphase (SEI) formation and evolution deplete cyclable lithium, increase interfacial resistance, and induce polarization that leads to lithium plating and dendritic growth during rapid charging and low-temperature operation. Electrolyte and solvation engineering are highlighted as coating-free strategies to mitigate these issues by reducing Li+ desolvation barriers and directing interphase chemistry toward thinner, more ion-conductive, fluorinated SEI films that inhibit plating while maintaining high-rate capability. Coated graphite approaches are compared, including carbon, inorganic, and polymer coatings that function as artificial SEI layers to minimize direct electrolyte contact, stabilize interphase composition, and enhance mechanical durability. Key trade-offs are discussed, including decreased first-cycle coulombic efficiency (FCCE) due to increased surface area, transport limitations arising from excessively thick coatings, nonuniform coverage leading to local current hotspots, and side reactions induced by the coatings. The discussion is further extended to sodium and potassium systems, explaining how larger ion sizes, unfavorable thermodynamics, and significant lattice expansion hinder their insertion into graphite, and summarizing strategies such as interlayer expansion and alternative carbon architectures that improve reversibility for larger ions. This review concludes that achieving durable, safe, and fast-charging graphite electrodes requires an integrated interfacial design that combines optimized graphite morphology, electrode architecture, and electrolyte chemistry. Full article
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47 pages, 7412 KB  
Review
Fluoride-Free MXene–Polymer Composites for Li-Metal and Li–S Batteries: Comparative Synthesis Methods, Integration Rules, Challenges, and Future Directions
by Truong Le Khang and Joonho Bae
Polymers 2025, 17(23), 3109; https://doi.org/10.3390/polym17233109 - 23 Nov 2025
Cited by 6 | Viewed by 2679
Abstract
MXene–polymer hybrids combine the high in-plane conductivity and rich surface chemistry of MXenes with the processability and mechanical tunability of polymers for lithium-metal and lithium–sulfur batteries. Most reported systems still rely on HF-etched MXenes, introducing F-rich terminations, safety and waste issues, and poorly [...] Read more.
MXene–polymer hybrids combine the high in-plane conductivity and rich surface chemistry of MXenes with the processability and mechanical tunability of polymers for lithium-metal and lithium–sulfur batteries. Most reported systems still rely on HF-etched MXenes, introducing F-rich terminations, safety and waste issues, and poorly controlled surfaces. This review instead centers on fluoride-free synthesis routes, benchmarks them against HF methods, and translates route–termination relationships into practical rules for choosing polymer backbones. We track the evolution from early linear hosts such as PEO- and PVDF-type polymers to polar nitrile or carbonyl matrices, crosslinked and ionogel networks, and emerging biopolymers and COF-type porous frameworks that are co-designed with MXene terminations to regulate ion transport, interfacial chemistry, and mechanical robustness. These chemistry–backbone pairings are linked to five scalable fabrication modes, including solution blending and film casting, in situ polymerization, surface grafting, layer-by-layer assembly, and electrospinning, and to roles as solid or quasi-solid electrolytes, artificial interphases, separator-like coatings, and electrode-facing architectures. Finally, we highlight key evidence gaps and reporting standards needed to de-risk scale-up of green MXene–polymer batteries. Full article
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21 pages, 4601 KB  
Article
Artificial Interfacial Layers with Zwitterionic Ion Structure Improves Lithium Symmetric Battery Life and Inhibits Dendrite Growth
by Haihua Wang, Wei Yuan, Chaoxian Chen, Rui Cao, Huizhu Niu, Ling Song, Jie Wang and Xinyu Shang
Symmetry 2025, 17(5), 652; https://doi.org/10.3390/sym17050652 - 25 Apr 2025
Viewed by 2231
Abstract
Lithium (Li) metal’s exceptional low electrode potential and high specific capacity for next-gen energy storage devices make it a top contender. However, the unregulated and unpredictable proliferation of Li dendrites and the instability of interfaces during repeated Li plating and stripping cycles pose [...] Read more.
Lithium (Li) metal’s exceptional low electrode potential and high specific capacity for next-gen energy storage devices make it a top contender. However, the unregulated and unpredictable proliferation of Li dendrites and the instability of interfaces during repeated Li plating and stripping cycles pose significant challenges to the widespread commercialization of Li metal anodes. We introduce the creation of a hydrogen bond network solid electrolyte interphase (SEI) film that integrates zwitterionic groups, designed to facilitate the stability and longevity of lithium metal batteries (LMBs). Here, we design a PVA/P(SBMA-MBA) hydrogen bond network film (PSM) as an artificial SEI, integrating zwitterions and polyvinyl alcohol (PVA) to synergistically regulate Li⁺ flux. The distinctive zwitterionic effect in the network amplifies the SEI film’s ionic conductivity to 1.14 × 10−4 S cm−1 and attains an impressive Li+ ion transfer number of 0.84. In situ Raman spectroscopy reveals dynamic hydrogen bond reconfiguration under strain, endowing the SEI with self-adaptive mechanical robustness. These properties facilitate a homogeneous Li flux and exceptionally suppress dendritic growth. The advanced Li metal anode may endure over 1200 h at 1 mA cm−2 current density and 1 mAh cm−2 area capacity in a Li|Li symmetric battery. And in full cells paired with LiFePO4 cathodes, 93.8% capacity retention is reached after 300 cycles at 1C. Consequently, this work provides a universal strategy for designing dynamic interphases through molecular dipole engineering, paving the way for safe and durable lithium metal batteries. Full article
(This article belongs to the Section Engineering and Materials)
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