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The composite solid electrolyte, which combines the advantages of inorganic conductors and organic polymer electrolytes, has become a crucial strategy for the construction of solid‐state batteries. However, the physical deposition and agglomeration of traditional composite fillers seriously affect their structural uniformity and ion transport performance, and the construction of uniform and stable composite electrolytes is still an insurmountable challenge. Herein, a strategy of in situ hybrid crosslinking polymerization of TiO2 nanoparticles is proposed for highly stable polymer composite electrolytes (NHCPE) with an ultrahigh ionic conductivity of 1.74 × 10−3 S cm−1 at 25 °C, and a high lithium‐ion transference number of 0.725. These properties enable the composed lithium symmetric battery to be stably deposited/plating off at 0.5 mA cm−2 for more than 1000 h. Moreover, the assembled LFP|PDOL@nanoTiO2|Li battery exhibits a superior specific discharge capacity of 142.6 mAh g−1 at 1 C and 25 °C, and an ultrahigh capacity retention rate of 90% after 1000 cycles. The proposed PDOL@nanoTiO2 NHCPE greatly inhibits the defects of easy agglomeration of composite electrolytes, solves the problems of easy decomposition, low thermal stability, and poor safety of polyether electrolytes, and opens up a new way for the design and industrial application of high‐stability composite polymer electrolytes. [ABSTRACT FROM AUTHOR]

Cellulose‐based solid electrolyte possesses the characteristics of low cost, high strength, and sustainability, and has great potential in the field of solid‐state lithium metal batteries. However, the large hydrogen bonds between cellulose molecules make the molecular chains tightly arranged, and hinder the ion conduction, seriously limiting its further development. Herein, an ion‐conducting molecular grafting strategy is proposed for the fabrication of cellulose acetate quasi‐solid composite electrolyte (CLA‐CN‐LATP QCE) with a superior ionic conductivity of 1.25 × 10−3 S cm−1 at room temperature. Benefited from grafted functional molecules, the assembled symmetrical battery exhibits low polarization voltage and highly stable lithium stripping/plating cycling of more than 1200 h at 0.1 mA cm−2 current density. Moreover, it endows LFP|CLA‐CN‐LATP QCE|Li battery with excellent long‐cycle stability of 1500 cycles at 0.5 C and 25 °C and superior capacity retention of 92.1%. Importantly, this work provides an effective strategy for further opening the ion transport channel between cellulose molecular chains and improving the interface properties of electrolytes and electrodes. [ABSTRACT FROM AUTHOR]

Raising the charging voltage and employing high‐capacity cathodes like lithium cobalt oxide (LCO) are efficient strategies to expand battery capacity. High voltage, however, will reveal major issues such as the electrolyte's low interface stability and weak electrochemical stability. Designing high‐performance solid electrolytes from the standpoint of substance genetic engineering design is consequently vital. In this instance, stable SEI and CEI interface layers are constructed, and a 4.7 V high‐voltage solid copolymer electrolyte (PAFP) with a fluoro‐cyanogen group is generated by polymer molecular engineering. As a result, PAFP has an exceptionally broad electrochemical window (5.5 V), a high Li+ transference number (0.71), and an ultrahigh ionic conductivity (1.2 mS cm−2) at 25 °C. Furthermore, the Li||Li symmetric cell possesses excellent interface stability and 2000 stable cycles at 1 mA cm−2. The LCO|PAFP|Li batteries have a 73.7% retention capacity after 1200 cycles. Moreover, it still has excellent cycling stability at a high charging voltage of 4.7 V. These characteristics above also allow PAFP to run stably at high loading, showing excellent electrochemical stability. Furthermore, the proposed PAFP provides new insights into high‐voltage resistant solid polymer electrolytes. [ABSTRACT FROM AUTHOR]

The development of green, controllable, and simplified pathways for rapid dopamine polymerization holds significant importance in the field of polydopamine (PDA) surface chemistry. In this study, a green strategy is successfully devised to accelerate and control the polymerization of dopamine through the introduction of ozone (O3). The findings reveal that ozone serves as an eco‐friendly trigger, significantly accelerating the dopamine polymerization process across a broad pH range, spanning from 4.0 to 10.0. Notably, the deposition rate of PDA coatings on a silicon wafer reaches an impressive value of ≈64.8 nm h−1 (pH 8.5), which is 30 times higher than that of traditional air‐assisted PDA and comparable to the fastest reported method. Furthermore, ozone exhibits the ability to accelerate dopamine polymerization even under low temperatures. It also enables control over the inhibition–initiation of the polymerization process by regulating the "ON/OFF" mode of the ozone gas. Moreover, the ozone‐induced PDA coatings demonstrate exceptional characteristics, including high homogeneity, good hydrophilicity, and remarkable chemical and mechanical stability. Additionally, the ozone‐induced PDA coatings can be rapidly and effectively deposited onto a wide range of substrates, particularly those that are adhesion‐resistant, such as polytetrafluoroethylene (PTFE). [ABSTRACT FROM AUTHOR]