Rui Xu

Lithium‐metal batteries (LMBs) have long been considered the “holy grail” of next‐generation energy storage systems due to the unique advantages of Li metal, such as having a high specific capacity and the lowest potential. Unfortunately, the practical application of LMBs is seriously hindered by the uncontrollable growth of dendritic Li. To address this issue, a positively charged layer (PCL) with freely moving multication sidechains is successfully polymerized on a commercial polypropylene (PP) separator. The cationic groups on the sidechains of the polymer realize dendrite‐free Li deposition based on the “dynamic tip‐occupying electrostatic shield” effect. LMBs with improved cycling stability and rate performance can be achieved by using a PP‐N,N,N,N”,N”‐pentamethyldiethylenetriamine (PP‐PMDT) separator. All the results demonstrate that this strategy for constructing a flexible “electrostatic shield layer” can successfully eliminate the formation of Li dendrites while retaining the desired performance.

Lithium (Li) metal has been considered a promising anode for next‐generation high‐energy‐density batteries. However, the low reversibility and intricate Li loss hinder the widespread implementation of Li metal batteries. Herein, we quantitatively differentiate the dynamic evolution of inactive Li, and decipher the fundamental interplay among dynamic Li loss, electrolyte chemistry, and the structure of the solid electrolyte interphase (SEI). The actual dominant form in inactive Li loss is practically determined by the relative growth rates of dead Li⁰ and SEI Li⁺ because of the persistent evolution of the Li metal interface during cycling. Distinct inactive Li evolution scenarios are disclosed by ingeniously tuning the inorganic anion‐derived SEI chemistry with a low amount of film‐forming additive. An optimal polymeric film enabler of 1,3‐dioxolane is demonstrated to derive a highly uniform multilayer SEI and decreased SEI Li⁺/dead Li⁰ growth rates, thus achieving enhanced Li cycling reversibility.

Lithium (Li) metal has been considered a promising anode for next‐generation high‐energy‐density batteries. However, the low reversibility and intricate Li loss hinder the widespread implementation of Li metal batteries. Herein, we quantitatively differentiate the dynamic evolution of inactive Li, and decipher the fundamental interplay among dynamic Li loss, electrolyte chemistry, and the structure of the solid electrolyte interphase (SEI). The actual dominant form in inactive Li loss is practically determined by the relative growth rates of dead Li⁰ and SEI Li⁺ because of the persistent evolution of the Li metal interface during cycling. Distinct inactive Li evolution scenarios are disclosed by ingeniously tuning the inorganic anion‐derived SEI chemistry with a low amount of film‐forming additive. An optimal polymeric film enabler of 1,3‐dioxolane is demonstrated to derive a highly uniform multilayer SEI and decreased SEI Li⁺/dead Li⁰ growth rates, thus achieving enhanced Li cycling reversibility.

Lithium (Li) metal anodes hold great promise for next‐generation high‐energy‐density batteries, while the insufficient fundamental understanding of the complex solid electrolyte interphase (SEI) is the major obstacle for the full demonstration of their potential in working batteries. The characteristics of SEI highly depend on the inner solvation structure of lithium ions (Li⁺). Herein, we clarify the critical significance of cosolvent properties on both Li⁺ solvation structure and the SEI formation on working Li metal anodes. Non‐solvating and low‐dielectricity (NL) cosolvents intrinsically enhance the interaction between anion and Li⁺ by affording a low dielectric environment. The abundant positively charged anion–cation aggregates generated as the introduction of NL cosolvents are preferentially brought to the negatively charged Li anode surface, inducing an anion‐derived inorganic‐rich SEI. A solvent diagram is further built to illustrate that a solvent with both proper relative binding energy toward Li⁺ and dielectric constant is suitable as NL cosolvent.

Lithium (Li) metal anodes hold great promise for next‐generation high‐energy‐density batteries, while the insufficient fundamental understanding of the complex solid electrolyte interphase (SEI) is the major obstacle for the full demonstration of their potential in working batteries. The characteristics of SEI highly depend on the inner solvation structure of lithium ions (Li⁺). Herein, we clarify the critical significance of cosolvent properties on both Li⁺ solvation structure and the SEI formation on working Li metal anodes. Non‐solvating and low‐dielectricity (NL) cosolvents intrinsically enhance the interaction between anion and Li⁺ by affording a low dielectric environment. The abundant positively charged anion–cation aggregates generated as the introduction of NL cosolvents are preferentially brought to the negatively charged Li anode surface, inducing an anion‐derived inorganic‐rich SEI. A solvent diagram is further built to illustrate that a solvent with both proper relative binding energy toward Li⁺ and dielectric constant is suitable as NL cosolvent.

2D materials, their features and possible approaches to mitigating the challenges in Li–S batteries are discussed.

Lithium metal is used to achieve high‐energy‐density batteries due to its large theoretical capacity and low negative electrochemical potential. The introduction of quasi‐solid electrolytes simultaneously overcomes the safety problems induced by the liquid electrolytes and the high interfacial resistance issues confronted by all solid‐state electrolytes. In‐depth investigations involving interfacial behaviors in quasi‐solid lithium metal batteries are inadequate. Herein an ultrathin Li₃OCl quasi‐solid‐state electrolyte layer (500 nm thickness) is used to cover a lithium anode. The polarization of the anode is remarkably reduced by introducing the Li₃OCl quasi‐solid‐state electrolyte. In contrast to the decomposition of solvents in a standard electrolyte (EC‐DEC,1.0 m LiPF₆), the established quasi‐solid‐state electrolyte interfaces can significantly inhibit the decomposition of solvents when the cut‐off voltage is 4.5 V.

Lithium metal is used to achieve high‐energy‐density batteries due to its large theoretical capacity and low negative electrochemical potential. The introduction of quasi‐solid electrolytes simultaneously overcomes the safety problems induced by the liquid electrolytes and the high interfacial resistance issues confronted by all solid‐state electrolytes. In‐depth investigations involving interfacial behaviors in quasi‐solid lithium metal batteries are inadequate. Herein an ultrathin Li₃OCl quasi‐solid‐state electrolyte layer (500 nm thickness) is used to cover a lithium anode. The polarization of the anode is remarkably reduced by introducing the Li₃OCl quasi‐solid‐state electrolyte. In contrast to the decomposition of solvents in a standard electrolyte (EC‐DEC,1.0 m LiPF₆), the established quasi‐solid‐state electrolyte interfaces can significantly inhibit the decomposition of solvents when the cut‐off voltage is 4.5 V.