Correlating the Solvating Power of Solvents with the Strength of Ion‐Dipole Interaction in Electrolytes of Lithium‐ion Batteries

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(47)

Опубликована: Окт. 9, 2023

The solvation structure of Li+ plays a significant role in determining the physicochemical properties electrolytes. However, to date, there is still no clear definition solvating power different electrolyte solvents, and even solvents that preferentially participate remain controversial. In this study, we comprehensively discuss process ions using both experimental characterizations theoretical calculations. Our findings reveal dependent on strength -solvent (ion-dipole) interaction. Additionally, uncover anions tend enter sheath most systems through -anion (ion-ion) interaction, which weakened by shielding effect solvents. competition between interactions ultimately determines final structures. This insight into fundamental understanding provides inspiration for design multifunctional mixed-solvent electrolytes advanced batteries.

Язык: Английский

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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

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Graphic, Quantitation, Visualization, Standardization, Digitization, and Intelligence of Electrolyte and Electrolyte‐Electrode Interface

Advanced Energy Materials, Год журнала: 2024, Номер 14(25)

Опубликована: Апрель 22, 2024

Abstract Electrolytes have recently regained significant attention in rechargeable batteries due to the discovery that electrolyte microstructures play a determinant role battery performance. By adjusting compositions of electrolytes cater various functionalities, such as high‐voltage, fast‐charging, wide‐temperature operation, and non‐flammable features, diverse range can be developed adapt different environmental working conditions. Nevertheless, elucidating understanding associated electrode interfacial behaviors remain challenging. These challenges arise from interdisciplinary nature research, encompassing subjects solution chemistry, interface electrochemistry, organic chemistry. This topic holds particular significance because chemistry solution‐solid are ubiquitous daily lives, yet their unclear inherent complexity, dynamic nature, rapid variability. In this context, electrolyte‐electrode research used an illustrative example summarize progress six key perspectives graphic, quantitation, visualization, standardization, digitization, intelligence. It is aimed provide multi‐faceted on interface. comprehensive approach enables effective design enhances accuracy predicting performance, servicing development

Язык: Английский

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Zincophilic Anionic Hydrogel Electrolyte with Interfacial Specific Adsorption of Solvation Structures for Durable Zinc Ion Hybrid Supercapacitors

Advanced Functional Materials, Год журнала: 2023, Номер 34(2)

Опубликована: Сен. 27, 2023

Abstract The rechargeable zinc ion hybrid supercapacitors (ZHSCs) are critically hindered by the low Coulombic efficiency and poor lifespan due to continuous water‐induced side reactions uncontrolled dendrite growth of Zn anode. Herein, a zincophilic anionic hydrogel electrolyte (PSCA/Zn(OTf) 2 ) is constructed incorporating dodecyl sulfate anions ((OSO 3 R) − micelles manipulate solvation structures 2+ cations via moderate ion–ion coordination interactions for manipulating deposition behavior interfacial chemistry on electrode. Joint experimental theoretical results show that solvated with ionized (OSO electron donor significantly restrict occurrence adverse (hydrogen evolution reactions). Concomitantly, newly involved influence adsorption configurations ions, which alter electrocrystallization patterns dendrite‐free induce oriented rapid reaction kinetics electrodes. As proof concept, Zn||Zn symmetric cells PSCA/Zn(OTf) exhibit high reversibility deposition/stripping an extended long cycle span. Significantly, benefiting from synergy modulatory environment regulated configurations, quasi‐solid‐state Zn||PSCA/Zn(OTf) ||N‐doped porous carbon material (NPC) ZHSC exhibits exceptional cycling stability over 40 000 cycles capacity decay (0.00027% per cycle).

Язык: Английский

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Designing Temperature-Insensitive Solvated Electrolytes for Low-Temperature Lithium Metal Batteries

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(27), С. 18281 - 18291

Опубликована: Май 30, 2024

Lithium metal batteries face problems from sluggish charge transfer at interfaces, as well parasitic reactions between lithium anodes and electrolytes, due to the strong electronegativity of oxygen donor solvents. These factors constrain reversibility kinetics low temperatures. Here, a nonsolvating cosolvent is applied weaken in ether solvents, enabling participation anionic donors solvation structure Li+. This strategy significantly accelerates desolvation process Li+ reduces side effects solvents on interfacial transport stability. The designed anion-aggregated electrolyte has unique temperature-insensitive enables achieve high average Coulombic efficiency room temperature −20 °C. A high-loading LiFePO4||Li cell exhibited with 100% capacity retention after 150 cycles temperature, −20, −40 practical 1 Ah-level pouch-cell delivered 81% 61% when charged discharged °C, respectively. constructing by regulation offers novel approach for developing electrolytes low-temperature batteries.

Язык: Английский

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Electrolytes Design for Extending the Temperature Adaptability of Lithium‐Ion Batteries: from Fundamentals to Strategies

Advanced Materials, Год журнала: 2024, Номер 36(21)

Опубликована: Фев. 13, 2024

Abstract With the continuously growing demand for wide‐range applications, lithium‐ion batteries (LIBs) are increasingly required to work under conditions that deviate from room temperature (RT). However, commercial electrolytes exhibit low thermal stability at high temperatures (HT) and poor dynamic properties (LT), hindering operation of LIBs extreme conditions. The bottleneck restricting practical applications has promoted researchers pay more attention developing a series innovative electrolytes. This review primarily covers design adaptability perspective. First, fundamentals concerning temperature, including donor number (DN), dielectric constant, viscosity, conductivity, ionic transport, theoretical calculations elaborated. Second, prototypical examples, such as lithium salts, solvent structures, additives, interfacial layers in both liquid solid electrolytes, presented explain how these factors can affect electrochemical behavior or temperatures. Meanwhile, principles limitations electrolyte discussed corresponding Finally, summary outlook regarding extend proposed.

Язык: Английский

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Modulating the Electrolyte Microenvironment in Electrical Double Layer for Boosting Electrocatalytic Nitrate Reduction to Ammonia

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(32)

Опубликована: Май 29, 2024

Abstract Electrochemical nitrate reduction reaction (NO 3 RR) is a promising approach to achieve remediation of nitrate‐polluted wastewater and sustainable production ammonia. However, it still restricted by the low activity, selectivity Faraday efficiency for ammonia synthesis. Herein, we propose an effective strategy modulate electrolyte microenvironment in electrical double layer (EDL) mediating alkali metal cations enhance NO RR performance. Taking bulk Cu as model catalyst, experimental study reveals that − ‐to‐NH performance different electrolytes follows trend Li + <Cs <Na <K . Theoretical studies illustrate proton transport rate activity rate‐determining step 2 ) increase order The cation effects are also general two typical nanostructured catalysts including copper/cuprous oxide nickel phosphides, achieving near‐100 % Faradaic over 99 conversion NH Furthermore, demonstrate can be converted high‐purity 4 Cl catalyst K ‐containing electrolyte.

Язык: Английский

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Lithium Bis(Trifluoromethanesulfonyl)Imide (LiTFSI): A Prominent Lithium Salt in Lithium‐Ion Battery Electrolytes – Fundamentals, Progress, and Future Perspectives

Advanced Functional Materials, Год журнала: 2024, Номер 34(48)

Опубликована: Июль 9, 2024

Abstract Lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) is a widely used lithium (Li) salt that extensively studied in the field of electrolytes for Li‐ion batteries (LIBs) to improve their performance. A thorough understanding its underlying mechanisms LIBs crucial gaining deeper insights into future development. This paper provides an extensive review role LiTFSI enhancing battery performance, including benefits negative electrode protection, facilitation fast charging capabilities, and promotion operation across wide temperature range. It also highlights specific drawbacks electrolyte domain examines potential solutions. By leveraging unique properties LiTFSI, strategies effective utilization current research are outlined. Finally, discusses lack mechanism interface particularly evolution multi‐component Li salts at positive interfaces, it reasonably anticipates applications realm non‐liquid batteries. study not only more comprehensive profound but aids exploration novel systems.

Язык: Английский

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Selection of Negative Charged Acidic Polar Additives to Regulate Electric Double Layer for Stable Zinc Ion Battery

Nano-Micro Letters, Год журнала: 2024, Номер 16(1)

Опубликована: Авг. 14, 2024

Zinc-ion batteries are promising for large-scale electrochemical energy storage systems, which still suffer from interfacial issues, e.g., hydrogen evolution side reaction (HER), self-corrosion, and uncontrollable dendritic Zn electrodeposition. Although the regulation of electric double layer (EDL) has been verified principle to select additive as regulator is misted. Here, several typical amino acids with different characteristics were examined reveal behaviors in regulated EDL on anode. Negative charged acidic polarity (NCAP) unveiled guideline selecting reconstruct an inner zincophilic H

Язык: Английский

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A weakly coordinating-intervention strategy for modulating Na+ solvation sheathes and constructing robust interphase in sodium-metal batteries

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

Опубликована: Июль 26, 2024

Constructing powerful anode/cathode interphases by modulate ion solvation structure is the principle of electrolyte design. However, methodological and theoretical design principles electrolyte/solvation their effect on electrochemical performance are still vague. Here, we propose a cationic weakly coordinating-intervention strategy for modulating Na+ sheathes constructing robust in sodium-metal batteries. Unlike local highly concentrated electrolytes, 1,2-difluorobenzene can coordinate with thus transforming into Na+-anion-incorporated structures strengthening formation combining salt decomposition. Furthermore, correlations between electrode interface properties revealed, which be tuned coordination. Ultimately, modulated achieves 97.5% Coulombic efficiency 600 cycles Na‖Cu cells at 1 mA cm−2 beneficial lifetime (2500 h) Na‖Na cells. Meanwhile, Na‖PB have achieved long-term operation 4.8 V, along wide temperatures. authors to sheath construct interphase Correlation also stated.

Язык: Английский

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