Fluorination in advanced battery design

Single-phase local-high-concentration solid polymer electrolytes for lithium-metal batteries

Solid polymer electrolytes with large-scale processability and interfacial compatibility are promising candidates for solid-state lithium metal batteries. Among various systems, poly(vinylidene fluoride)-based polymer electrolytes with residual solvent are appealing for room-temperature battery operations. However, their porous structure and limited ionic conductivity hinder practical application. Herein, we propose a phase regulation strategy to disrupt the symmetry of poly(vinylidene fluoride) chains and obtain the dense composite electrolyte through the incorporation of MoSe2 sheets. The electrolyte with high dielectric constant can optimize the solvation structures to achieve high ionic conductivity and low activation energy. The in-situ reactions between MoSe2 and Li metal generate Li2Se fast conductor in solid electrolyte interphase, which improves the Coulombic efficiency and interfacial kinetics. The solid-state Li||Li cells achieve robust cycling at 1 mA cm-2, and the Li||LiNi0.8Co0.1Mn0.1O2 full cells show practical performance at high rate (3C), high loading (2.6 mAh cm-2) and in pouch cell. 

Phase regulation enabling dense polymer-based composite electrolytes for solid-state lithium metal batteries

The practical application of polymer electrolytes is hindered due to the low ionic conductivity and the interfacial instability between the electrodes. Herein, a strategy for designing solid polymer electrolytes is developed that facilitates the rapid lithium‐ion migration through weak coordination with polymer chain segments, as well as the fast ion channel transport of oligomers. Moreover, the in situ‐produced solid polymer electrolyte (PFVS) can form stable LiF‐rich interfaces with both the lithium metal anode and different cathodes. When the PFVS is applied in Li‐metal batteries, excellent properties are achieved at room temperature. A Li||Li symmetric cell can be stably cycled for 4000 h at a current density of 0.1 mA cm−1, a Li||LiFePO4 full cell can maintain capacity retention as high as still 94.4% after 600 cycles at 1 C, and a Li||NCM811 full cell can retain 80% capacity after 180 cycles at 1 C. A 2.6 Ah Graphite|PFVS|NCM90 pouch cell is made for demonstrating the practical application potential, and it can be also stably cycled. The developed strategy provides a promising path for designing solid polymer electrolytes that can effectively extend the lifespan of Li metal batteries.

Molecular Design for In‐Situ Polymerized Solid Polymer Electrolytes Enabling Stable Cycling of Lithium Metal Batteries

Introducing fluorine (F) groups into a passivator plays an important role in enhancing the defect passivation effect for the perovskite film, which is usually attributed to the direct interaction of F and defect states. However, the interaction between electronegative F and electron-rich passivation groups in the same molecule, which may influence the passivation effect, is ignored. We herein report that such interactions can vary the electron cloud distribution around the passivation groups and thus changing their coordination with defect sites. By comparing two fluorinated molecules, heptafluorobutylamine (HFBM) and heptafluorobutyric acid (HFBA), we find that the F/-NH2 interaction in HFBM is stronger than the F/-COOH one in HFBA, inducing weaker passivation ability of HFBM than HFBA. Accordingly, HFBA-based perovskite solar cells (PSCs) provide an efficiency of 24.70% with excellent long-term stability. Moreover, the efficiency of a large-area perovskite module (14.0 cm2) based on HFBA reaches 21.13%. Our work offers an insight into understanding an unaware role of the F group in impacting the passivation effect for the perovskite film. ​.

Understanding the Role of Fluorine Groups in Passivating Defects for Perovskite Solar Cells ​.

Solid polymer electrolytes (SPEs), which are favorable to form intimate interfacial contacts with electrodes, are promising electrolyte of choice for long-cycling lithium metal batteries (LMBs). However, typical SPEs with easily oxidized oxygen-bearing polar groups exhibit narrow electrochemical stability window (ESW), making it impractical to increase specific capacity and energy density of SPE based LMBs with charging cut-off voltage of 4.5 V or higher. Here, we apply a polyfluorinated crosslinker to enhance oxidation resistance of SPEs. The crosslinked network facilitates transmission of the inductive electron-withdrawing effect of polyfluorinated segments. As a result, polyfluorinated crosslinked SPE exhibits a wide ESW, and the Li|SPE|LiNi0.5Co0.2Mn0.3O2 cell with a cutoff voltage of 4.5 V delivers a high discharge specific capacity of ~164.19 mAh g-1 at 0.5 C and capacity retention of ~90% after 200 cycles. This work opens a direction in developing SPEs for long-cycling high-voltage LMBs by using polyfluorinated crosslinking strategy. 

https://www.nature.com/articles/s41467-023-37997-6.pdf

Polyfluorinated crosslinker-based solid polymer electrolytes for long-cycling 4.5 V lithium metal batteries

Recovery of chlorogenic acid from the DES-based extract of Eucommia ulmoides leaves by molecularly imprinted solid-phase extraction

Deep eutectic solvents in the extraction of active compounds from Eucommia Ulmoides Oliv. leaves

Aiming to provide a new way that preserves more active components in Eucommia ulmoides (EU) leaves, this paper utilizes 4 methods, i.e., microwave, steam, air heating, and frying, to process EU leaves before drying, and their respective effects on the leaves were evaluated. The antioxidant activity of EU leaves in vitro was measured by the DPPH free radical method; the contents of total flavonoids (TFC) and total phenols (TPC) were analyzed by spectrophotometry; and the contents of main active components were determined by high-performance liquid chromatography (HPLC). The results showed the pre-process improved the quality of the EU leaves. As a simple and fast process, the microwave process is the most effective technique in the retention of flavonoids and four active ingredients except aucubin. High power (800 W) and short time (2.5 min) are more conducive to the retention of active ingredients, with high antioxidant activity. Appropriate steam and frying processes also exhibited benefits for the active components. In particular, the samples treated with steam for 10 minutes showed great potential for industrial application with the highest antioxidant activity and polyphenol content. Therefore, proper pre-processing before drying should be conducted to effectively protect the active components of EU leaves. 

Effects of pre-processing on the active compounds before drying Eucommia ulmoides leaves

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Papers

Polyfluorinated crosslinker-based solid polymer electrolytes for long-cycling 4.5 V lithium metal batteries

Recovery of chlorogenic acid from the DES-based extract of Eucommia ulmoides leaves by molecularly imprinted solid-phase extraction

Deep eutectic solvents in the extraction of active compounds from Eucommia Ulmoides Oliv. leaves

Effects of pre-processing on the active compounds before drying Eucommia ulmoides leaves