Insights into the solvation chemistry in liquid electrolytes for lithium-based rechargeable batteries

Chemical Society Reviews, Год журнала: 2023, Номер 52(15), С. 5255 - 5316

Опубликована: Янв. 1, 2023

Lithium-based rechargeable batteries have dominated the energy storage field and attracted considerable research interest due to their excellent electrochemical performance. As indispensable ubiquitous components, electrolytes play a pivotal role in not only transporting lithium ions, but also expanding stable potential window, suppressing side reactions, manipulating redox mechanism, all of which are closely associated with behavior solvation chemistry electrolytes. Thus, comprehensively understanding is significant importance. Here we critically reviewed development various lithium-based including lithium-metal (LMBs), nonaqueous lithium-ion (LIBs), lithium-sulfur (LSBs), lithium-oxygen (LOBs), aqueous (ALIBs), emphasized effects interactions between cations, anions, solvents on chemistry, functions different types (strong solvating electrolytes, moderate weak electrolytes) performance mechanism abovementioned batteries. Specifically, stability electrode-electrolyte interphases, suppression dendrites LMBs, inhibition co-intercalation LIBs, improvement anodic at high cut-off voltages LIBs ALIBs, regulation pathways LSBs LOBs, hydrogen/oxygen evolution reactions LOBs thoroughly summarized. Finally, review concludes prospective outlook, where practical issues advanced situ/operando techniques illustrate theoretical calculation simulation such as "material knowledge informed machine learning" "artificial intelligence (AI) + big data" driven strategies for high-performance been proposed.

Язык: Английский

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Electrolyte solvation chemistry to construct an anion-tuned interphase for stable high-temperature lithium metal batteries

eScience, Год журнала: 2023, Номер 3(4), С. 100135 - 100135

Опубликована: Апрель 22, 2023

Lithium metal batteries are regarded as promising alternative next-generation energy storage systems. However, the unstable anode interphase results in dendrite growth and irreversible lithium consumption with low Coulombic efficiency (CE). Herein, we rationally design a Li+ coordination structure via electrolyte solvation chemistry. Nitrate anions aggregated sheath, even at concentration solvent moderate ability, which promotes desolvation constructs nitrate anion-tuned interphase. Meanwhile, high-donor-number is introduced an additive to strongly coordinate Li+, accelerates ion-transfer kinetics rate performance. This not only micro-sized deposition high CE of 99.5% over 3500 h, but also enables superior stability under 50% depth plating/stripping lean 3 g Ah–1 50 °C. A lithium–sulfur battery exhibits prolonged lifespan 2000 cycles average 100%. full using 1x excess capacity near 1600 mAh gS–1 for 100 without loss. Moreover, 0.55 Ah pouch cell delivers reversible density 423 Wh kg–1 based on these electrodes electrolyte.

Язык: Английский

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Ion–Dipole-Interaction-Induced Encapsulation of Free Residual Solvent for Long-Cycle Solid-State Lithium Metal Batteries

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(47), С. 25632 - 25642

Опубликована: Ноя. 9, 2023

Owing to high ionic conductivity and mechanical strength, poly(vinylidene fluoride) (PVDF) electrolytes have attracted increasing attention for solid-state lithium batteries, but highly reactive residual solvents severely plague cycling stability. Herein, we report a free-solvent-capturing strategy triggered by reinforced ion-dipole interactions between Li+ solvent molecules. Lithium difluoro(oxalato)borate (LiDFOB) salt additive with electron-withdrawing capability serves as redistributor of the electropositive state, which offers more binding sites solvents. Benefiting from modified coordination environment, kinetically stable anion-derived interphases are preferentially formed, effectively mitigating interfacial side reactions electrodes electrolytes. As result, assembled battery shows lifetime over 2000 cycles an average Coulombic efficiency 99.9% capacity retention 80%. Our discovery sheds fresh light on targeted regulation extend cycle life batteries.

Язык: Английский

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Multivalent Design of Low-Entropy-Penalty Ion–Dipole Interactions for Dynamic Yet Thermostable Supramolecular Networks

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(6), С. 3526 - 3534

Опубликована: Янв. 31, 2023

Dynamic supramolecular networks are constantly accompanied by thermal instability. The fundamental reason is most reversible noncovalent bonds quickly decay at elevated temperatures and dissociate below 100 °C. Here, in this paper, we realize a ion-dipole interaction with high-temperature stability exceeding 150 resultant network can simultaneously possess mechanical strength of 1.32 MPa (14.8 times that pristine material), dynamic self-healing capability, stable working temperature up to 200 From the prolonged characteristic relaxation time 600 s even °C, our material represents one thermally polymers. These remarkable performances achieved using new multivalent yet low-entropy-penalty molecular design. In way, bond reach high enthalpy while minimizing entropy-dominated dissociations.

Язык: Английский

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Electrolyte Chemistry toward Ultrawide-Temperature (−25 to 75 °C) Sodium-Ion Batteries Achieved by Phosphorus/Silicon-Synergistic Interphase Manipulation

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(11), С. 7295 - 7304

Опубликована: Фев. 16, 2024

All-weather operation is considered an ultimate pursuit of the practical development sodium-ion batteries (SIBs), however, blocked by a lack suitable electrolytes at present. Herein, introducing synergistic manipulation mechanisms driven phosphorus/silicon involvement, compact electrode/electrolyte interphases are endowed with improved interfacial Na-ion transport kinetics and desirable structural/thermal stability. Therefore, modified carbonate-based electrolyte successfully enables all-weather adaptability for long-term over wide temperature range. As verification, half-cells using designed operate stably range −25 to 75 °C, accompanied capacity retention rate exceeding 70% even after 1700 cycles 60 °C. More importantly, full cells assembled Na3V2(PO4)2O2F cathode hard carbon anode also have excellent cycling stability, 500 1000 50 °C superb during dynamic testing continuous change. In short, this work proposes advanced regulation strategy targeted all-climate SIB operation, which good practicability reference significance.

Язык: Английский

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Deshielding Anions Enable Solvation Chemistry Control of LiPF₆‐Based Electrolyte toward Low‐Temperature Lithium‐Ion Batteries

Advanced Materials, Год журнала: 2024, Номер 36(16)

Опубликована: Янв. 15, 2024

Abstract Severe capacity decay under subzero temperatures remains a significant challenge for lithium‐ion batteries (LIBs) due to the sluggish interfacial kinetics. Current efforts mitigate this deteriorating behavior rely on high‐solubility lithium salts (e.g., Lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), bis(fluorosulfonyl)imide (LiFSI))‐based electrolytes construct anion participated solvation structures. However, such bring issues of corrosion current collector and increased costs. Herein, most commonly used hexafluorophosphate (LiPF 6 ) instead, establish peculiar structure with high ratio ion pairs aggregates by introducing deshielding NO 3 − additive low‐temperature LIBs is utilized. The significantly reduces energy barrier at low temperatures. Benefiting from this, graphite (Gr) anode retains ≈72.3% −20 °C, which far superior 32.3% 19.4% retention counterpart electrolytes. Moreover, LiCoO 2 /Gr full cell exhibits stable cycling performance 100 cycles °C inhibited plating. This work heralds new paradigm in LiPF ‐based electrolyte design operating

Язык: Английский

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Self-purification and silicon-rich interphase achieves high-temperature (70°C) sodium-ion batteries with nonflammable electrolyte

Energy storage materials, Год журнала: 2024, Номер 66, С. 103230 - 103230

Опубликована: Янв. 26, 2024

Язык: Английский

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Transparent, stretchable, self-healing, and self-adhesive ionogels for flexible multifunctional sensors and encryption systems

Chemical Engineering Journal, Год журнала: 2024, Номер 484, С. 149632 - 149632

Опубликована: Фев. 13, 2024

Язык: Английский

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Strong Lewis-acid coordinated PEO electrolyte achieves 4.8 V-class all-solid-state batteries over 580 Wh kg−1

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Окт. 23, 2024

Polyethylene oxide (PEO) based electrolytes critically govern the security and energy density of solid-state batteries, but typically suffer from poor oxidation resistance at high voltages, which limits batteries. Here, we report a Lewis-acid coordinated strategy to significantly improve cyclic stability 4.8 V-class PEO-based battery. The introduced Mg

Язык: Английский

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Unraveling the temperature-responsive solvation structure and interfacial chemistry for graphite anodes

Energy & Environmental Science, Год журнала: 2023, Номер 17(1), С. 227 - 237

Опубликована: Ноя. 14, 2023

Correlations between the temperature-responsive solvation structure, interfacial chemistry and performance of graphite anodes are revealed to understand structure–property relationships, providing insights into designing temperature-adaptative batteries.

Язык: Английский

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