Jin Xie

Super-resolution microscopy reveals the impact of adsorbent clustering on adsorption heterogeneity and cooperativity in pollutant removal.

The lifespan of practical lithium (Li)‐metal batteries is severely hindered by the instability of Li‐metal anodes. Fluorinated solid electrolyte interphase (SEI) emerges as a promising strategy to improve the stability of Li‐metal anodes. The rational design of fluorinated molecules is pivotal to construct fluorinated SEI. Herein, design principles of fluorinated molecules are proposed. Fluoroalkyl (−CF₂CF₂−) is selected as an enriched F reservoir and the defluorination of the C−F bond is driven by leaving groups on β‐sites. An activated fluoroalkyl molecule (AFA), 2,2,3,3‐tetrafluorobutane‐1,4‐diol dinitrate is unprecedentedly proposed to render fast and complete defluorination and generate uniform fluorinated SEI on Li‐metal anodes. In Li–sulfur (Li−S) batteries under practical conditions, the fluorinated SEI constructed by AFA undergoes 183 cycles, which is three times the SEI formed by LiNO₃. Furthermore, a Li−S pouch cell of 360 Wh kg⁻¹ delivers 25 cycles with AFA. This work demonstrates rational molecular design principles of fluorinated molecules to construct fluorinated SEI for practical Li‐metal batteries.

The lifespan of practical lithium (Li)‐metal batteries is severely hindered by the instability of Li‐metal anodes. Fluorinated solid electrolyte interphase (SEI) emerges as a promising strategy to improve the stability of Li‐metal anodes. The rational design of fluorinated molecules is pivotal to construct fluorinated SEI. Herein, design principles of fluorinated molecules are proposed. Fluoroalkyl (−CF₂CF₂−) is selected as an enriched F reservoir and the defluorination of the C−F bond is driven by leaving groups on β‐sites. An activated fluoroalkyl molecule (AFA), 2,2,3,3‐tetrafluorobutane‐1,4‐diol dinitrate is unprecedentedly proposed to render fast and complete defluorination and generate uniform fluorinated SEI on Li‐metal anodes. In Li–sulfur (Li−S) batteries under practical conditions, the fluorinated SEI constructed by AFA undergoes 183 cycles, which is three times the SEI formed by LiNO₃. Furthermore, a Li−S pouch cell of 360 Wh kg⁻¹ delivers 25 cycles with AFA. This work demonstrates rational molecular design principles of fluorinated molecules to construct fluorinated SEI for practical Li‐metal batteries.

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.

Polysulfide intermediates (PSs), the liquid‐phase species of active materials in lithium–sulfur (Li‐S) batteries, connect the electrochemical reactions between insulative solid sulfur and lithium sulfide and are key to full exertion of the high‐energy‐density Li‐S system. Herein, the concept of sulfur container additives is proposed for the direct modification on the PSs species. By reversible storage and release of the sulfur species, the container molecule converts small PSs into large organosulfur species. The prototype di(tri)sulfide‐polyethylene glycol sulfur container is highly efficient in the reversible PS transformation to multiply affect electrochemical behaviors of sulfur cathodes in terms of liquid‐species clustering, reaction kinetics, and solid deposition. The stability and capacity of Li‐S cells was thereby enhanced. The sulfur container is a strategy to directly modify PSs, enlightening the precise regulation on Li‐S batteries and multi‐phase electrochemical systems.

Polysulfide intermediates (PSs), the liquid‐phase species of active materials in lithium–sulfur (Li‐S) batteries, connect the electrochemical reactions between insulative solid sulfur and lithium sulfide and are key to full exertion of the high‐energy‐density Li‐S system. Herein, the concept of sulfur container additives is proposed for the direct modification on the PSs species. By reversible storage and release of the sulfur species, the container molecule converts small PSs into large organosulfur species. The prototype di(tri)sulfide‐polyethylene glycol sulfur container is highly efficient in the reversible PS transformation to multiply affect electrochemical behaviors of sulfur cathodes in terms of liquid‐species clustering, reaction kinetics, and solid deposition. The stability and capacity of Li‐S cells was thereby enhanced. The sulfur container is a strategy to directly modify PSs, enlightening the precise regulation on Li‐S batteries and multi‐phase electrochemical systems.