Gemischte polyanionische Verbindungen als positive Elektroden für die kostengünstige elektrochemische Energiespeicherung

Dual‐ion batteries (DIBs) inherently suffer from limited energy density. Proposed here is a strategy to effectively tackle this issue by employing locally ordered graphitized carbon (LOGC) cathodes. Quantum mechanical modeling suggests that strong anion–anion repulsions and severe expansion at the deep‐charging stage raise the anion intercalation voltage, therefore only part of the theoretical anion storage sites in graphite is accessible. The LOGC interconnected with disordered carbon is predicted to weaken the interlaminar van der Waals interactions, while disordered carbons not only interconnect the dispersed nanographite but also partially buffer severe anion–anion repulsion and offer extra capacitive anion storage sites. As a proof‐of‐concept, ketjen black (KB) with LOGC was used as a model cathode for a potassium‐based DIB (KDIB). The KDIB delivers an unprecedentedly high specific capacity of 232 mAh g−1 at 50 mA g−1, a good rate capability of 110 mAh g−1 at 2000 mA g−1, and excellent cycling stability of 1000 cycles without obvious capacity fading.

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Locally Ordered Graphitized Carbon Cathodes for High‐Capacity Dual‐Ion Batteries

Yang

Liu

Zheng

et al. 2021

Angewandte Chemie

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Novel Lamellar Tetrapotassium Pyromellitic Organic for Robust High‐Capacity Potassium Storage

et al. 2021

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Redox‐active organics are investigation hotspots for metal ion storage due to their structural diversity and redox reversibility. However, they are plagued by limited storage capacity, sluggish ion diffusion kinetics, and weak structural stability, especially for K+ ion storage. Herein, we firstly reported the lamellar tetrapotassium pyromellitic (K4PM) with four active sites and large interlayer distance for K+ ion storage based on a design strategy, where organics are constructed with the small molecular mass, multiple active sites, fast ion diffusion channels, and rigid conjugated π bonds. The K4PM electrode delivers a high capacity up to 292 mAh g−1 at 50 mA g−1, among the best reported organics for K+ ion storage. Especially, it achieves an excellent rate capacity and long‐term cycling stability with a capacity retention of ≈83 % after 1000 cycles. Incorporating in situ and ex‐situ techniques, the K+ ion storage mechanism is revealed, where conjugated carboxyls are reversibly rearranged into enolates to stably store K+ ions. This work sheds light on the rational design and optimization of organic electrodes for efficient metal ion storage.

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Ether‐Based Electrolyte Chemistry Towards High‐Voltage and Long‐Life Na‐Ion Full Batteries

Liang

Zhao

et al. 2021

Angewandte Chemie

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Although ether‐based electrolytes have been extensively applied in anode evaluation of batteries, anodic instability arising from solvent oxidability is always a tremendous obstacle to matching with high‐voltage cathodes. Herein, by rational design for solvation configuration, the fully coordinated ether‐based electrolyte with strong resistance against oxidation is reported, which remains anodically stable with high‐voltage Na3V2(PO4)2O2F (NVPF) cathode under 4.5 V (versus Na+/Na) protected by an effective interphase. The assembled graphite//NVPF full cells display superior rate performance and unprecedented cycling stability. Beyond that, the constructed full cells coupling the high‐voltage NVPF cathode with hard carbon anode exhibit outstanding electrochemical performances in terms of high average output voltage up to 3.72 V, long‐term cycle life (such as 95 % capacity retention after 700 cycles) and high energy density (247 Wh kg−1). In short, the optimized ether‐based electrolyte enriches systematic options, the ability to maintain oxidative stability and compatibility with various anodes, exhibiting attractive prospects for application.

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Gemischte polyanionische Verbindungen als positive Elektroden für die kostengünstige elektrochemische Energiespeicherung

Cited by 10 publications

References 82 publications

Locally Ordered Graphitized Carbon Cathodes for High‐Capacity Dual‐Ion Batteries

Locally Ordered Graphitized Carbon Cathodes for High‐Capacity Dual‐Ion Batteries

Novel Lamellar Tetrapotassium Pyromellitic Organic for Robust High‐Capacity Potassium Storage

Ether‐Based Electrolyte Chemistry Towards High‐Voltage and Long‐Life Na‐Ion Full Batteries

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