Organic pH Buffer for Dendrite‐Free and Shuttle‐Free Zn‐I₂ Batteries

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(21)

Опубликована: Март 23, 2023

Aqueous Zn-Iodine (I2 ) batteries are attractive for large-scale energy storage. However, drawbacks include, Zn dendrites, hydrogen evolution reaction (HER), corrosion and, cathode "shuttle" of polyiodines. Here we report a class N-containing heterocyclic compounds as organic pH buffers to obviate these. We evidence that addition pyridine /imidazole regulates electrolyte pH, and inhibits HER anode corrosion. In addition, imidazole preferentially absorb on metal, regulating non-dendritic plating /stripping, achieving high Coulombic efficiency 99.6 % long-term cycling stability 3200 h at 2 mA cm-2 , mAh . It is also confirmed polyiodines shuttling boosts conversion kinetics I- /I2 As result, the Zn-I2 full battery exhibits long cycle >25 000 cycles specific capacity 105.5 g-1 10 A conclude buffer engineering practical dendrite-free shuttle-free batteries.

Язык: Английский

---

Non‐Flammable Ester Electrolyte with Boosted Stability Against Li for High‐Performance Li Metal Batteries

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(41)

Опубликована: Авг. 19, 2022

Abstract In traditional non‐flammable electrolytes a trade‐off always exists between non‐flammability and battery performance. Previous research focused on reducing free solvents forming anion‐derived solid‐electrolyte interphase. However, the contribution of solvated anions in boosting stability electrolyte has been overlooked. Here, we resolve this via introducing into Li + solvation sheaths using with similar Gutmann donor number (DN) to that solvents. Taking trimethyl phosphate fire‐retardant (DN=23.0 kcal mol −1 ) NO 3 − (DN=22.2 as an example, is readily involved sheath reduces polarity solvent. This results boosted against Li. The developed low viscosity, high ionic conductivity cost. reversibility Li‐Cu cell was improved 99.49 % lifespan practical LMBs extended by >100 %.

Язык: Английский

---

Engineering an electrostatic field layer for high-rate and dendrite-free Zn metal anodes

Energy & Environmental Science, Год журнала: 2023, Номер 16(8), С. 3612 - 3622

Опубликована: Янв. 1, 2023

The Co(TAPC) additive can be preferentially adsorbed on the Zn anode surface to create a dense zincophilic molecular layer. layer could promote desolvation of 2+ and redistribute flux, resulting in smooth stable deposition.

Язык: Английский

---

Covalent triazine frameworks for advanced energy storage: challenges and new opportunities

Energy & Environmental Science, Год журнала: 2023, Номер 16(8), С. 3181 - 3213

Опубликована: Янв. 1, 2023

This Review provides a comprehensive overview of recent advancements in CTF materials and CTF-based batteries. The aims to make batteries viable for next-generation high-energy battery systems.

Язык: Английский

---

Inorganic Filler Enhanced Formation of Stable Inorganic‐Rich Solid Electrolyte Interphase for High Performance Lithium Metal Batteries

Advanced Functional Materials, Год журнала: 2023, Номер 33(29)

Опубликована: Апрель 2, 2023

Abstract Lithium metal (LM) is a promising anode material for next generation lithium ion based electrochemical energy storage devices. Critical issues of unstable solid electrolyte interphases (SEIs) and dendrite growth however still impede its practical applications. Herein, composite gel polymer (GPE), formed through in situ polymerization pentaerythritol tetraacrylate with fumed silica fillers, developed to achieve high performance batteries (LMBs). As evidenced theoretically experimentally, the presence SiO 2 not only accelerates Li + transport but also regulates solvation sheath structures, thus facilitating fast kinetics formation stable LiF‐rich interphase achieving uniform depositions suppress growth. The GPE‐based Li||Cu half‐cells Li||Li symmetrical cells display Coulombic efficiency (CE) 90.3% after 450 cycles maintain stability over 960 h at 3 mA cm −2 mAh , respectively. In addition, Li||LiFePO 4 full‐cells LM limited supply capacity retention 68.5% 700 0.5 C (1 = 170 g −1 ). Especially, when further applied anode‐free LMBs, carbon cloth||LiFePO full‐cell exhibits excellent cycling an average CE 99.94% 160th cycle C.

Язык: Английский

---

Weakly solvating electrolytes for next-generation lithium batteries: design principles and recent advances

Energy Materials and Devices, Год журнала: 2023, Номер 1(1), С. 9370003 - 9370003

Опубликована: Сен. 1, 2023

Lithium batteries play a dominant role in the power source market of electric vehicles and portable electronic devices. The electrolyte is critical to determining performance lithium batteries. Conventional electrolytes cannot meet ever-growing demands fast-charging, wide-temperature operation, safety properties Despite great success (localized) high-concentration electrolytes, they still suffer from disadvantages like low ionic conductivity high cost. emerging weakly solvating also known as low-solvating offer another solution these challenges have attracted intensive research interests recent years. This contribution reviews working mechanisms, design principles, advances developing electrolytes. A summary perspective about future directions this field provided. insights will benefit both academic industrial communities designing safe high-performance next-generation Li

Язык: Английский

---

Engineering the Structural Uniformity of Gel Polymer Electrolytes via Pattern‐Guided Alignment for Durable, Safe Solid‐State Lithium Metal Batteries

Advanced Materials, Год журнала: 2023, Номер 35(38)

Опубликована: Июнь 3, 2023

Ultrathin and super-toughness gel polymer electrolytes (GPEs) are the key enabling technology for durable, safe, high-energy density solid-state lithium metal batteries (SSLMBs) but extremely challenging. However, GPEs with limited uniformity continuity exhibit an uneven Li+ flux distribution, leading to nonuniform deposition. Herein, a fiber patterning strategy developing engineering ultrathin (16 µm) fibrous high ionic conductivity (≈0.4 mS cm-1 ) superior mechanical toughness (≈613%) durable safe SSLMBs is proposed. The special patterned structure provides fast transport channels tailoring solvation of traditional LiPF6 -based carbonate electrolyte, rapid transfer kinetics uniform flux, boosting stability against Li anodes, thus realizing ultralong plating/stripping in symmetrical cell over 3000 h at 1.0 mA cm-2 , mAh . Moreover, LiFePO4 loading 10.58 mg deliver stable cycling life 1570 cycles C 92.5% capacity retention excellent rate 129.8 g-1 5.0 cut-off voltage 4.2 V (100% depth-of-discharge). Patterned systems powerful strategies producing SSLMBs.

Язык: Английский

---

Stabilizing Interfaces in High‐Temperature NCM811‐Li Batteries via Tuning Terminal Alkyl Chains of Ether Solvents

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(28)

Опубликована: Май 11, 2023

Ether electrolytes are promising for lithium metal batteries. Despite the intensive research in recent years, most state-of-the-art ether still cannot form reliable electrode-electrolyte interfaces NCM811-Li batteries at diluted concentrations, especially those operating elevated temperatures. We report a simple but effective strategy to break this bottleneck and stabilize high-temperature electrolytes. propose that by gradually extending terminal groups of glycol diethers from methyl n-butyl groups, comprehensive stability is improved. An anion-dominated solvation structure realized concentration 1 M. Accordingly, interactions suppressed, thinner, denser, more inorganic-rich solid- /cathode-electrolyte interface achieved. Additionally, surface phase transition structural degradation NCM811 cathode alleviated. Consequently, ethylene dibutyl ether-based electrolyte, Coulombic efficiency Li-Cu cells working 60 °C boosted 99.41 % with cycling life over 200 cycles. The lifespan prolonged than 400 stable average 99.77 quasi-practical conditions 50 μm Li, lean electrolyte 10 μL mAh-1 , medium-high loading >2.2 mAh cm-2 .

Язык: Английский

---

Work‐Function‐Induced Interfacial Electron/Ion Transport in Carbon Hosts toward Dendrite‐Free Lithium Metal Anodes

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(44)

Опубликована: Сен. 15, 2023

Coupled electron/ion transport is a decisive feature of Li plating/stripping, wherein the compatibility rates determines morphology deposited Li. Local Li+ hotspots form due to inhomogeneous interfacial charge transfer and lead uncontrolled deposition, which decreases utilization rate safety metal anodes. Herein, we report method obtain dendrite-free anodes by driving electron pumping accumulating boosting ion diffusion tuning work function carbon host using cobalt-containing catalysts. The results reveal that increasing provides an deviation from C Co, electron-rich Co shows favorable binding . catalysts boost on fiber scaffolds without local aggregation reducing migration barrier. as-obtained anode exhibits Coulombic efficiency 99.0 %, cycle life over 2000 h, 50 capacity retention 83.4 % after 130 cycles in pouch cells at negative/positive ratio 2.5. These findings provide novel strategy stabilize regulating materials electrocatalysts.

Язык: Английский

---

Hydrofluoric Acid‐Removable Additive Optimizing Electrode Electrolyte Interphases with Li⁺ Conductive Moieties for 4.5 V Lithium Metal Batteries

Advanced Functional Materials, Год журнала: 2023, Номер 33(12)

Опубликована: Янв. 10, 2023

Abstract High‐voltage lithium metal batteries (LMBs) are capable to achieve the increasing energy density. However, their cycling life is seriously affected by unstable electrolyte/electrode interfaces and capacity instability at high voltage. Herein, a hydrofluoric acid (HF)‐removable additive proposed optimize electrode electrolyte interphases for addressing above issues. N, N‐dimethyl‐4‐(4,4,5,5‐tetramethyl‐1,3,2‐dioxaborolan‐2‐yl) aniline (DMPATMB) used as induce PF 6 − decomposition form dense robust LiF‐rich solid interphase (SEI) suppressing Li dendrite growth. Moreover, DMPATMB can help highly + conductive 3 N LiBO 2 , which boost transport across SEI cathode (CEI). In addition, scavenge traced HF in protect both CEI from corrosion. As expected, 4.5 V Li|| LiNi 0.6 Co 0.2 Mn O with such deliver 145 mAh g −1 after 140 cycles 200 mA . This work provides novel insight into high‐voltage additives LMBs.

Язык: Английский

---