As an alternative to conventional inorganic intercalation electrode materials, organic electrode materials are promising candidates for the next generation of sustainable and versatile energy storage devices. In this paper we provide an overview of organic electrode materials, including their fundamental knowledge, development history and perspective applications. Based on different organics including n-type, p-type and bipolar, we firstly analyzed their working principles, reaction mechanisms, electrochemical performances, advantages and challenges. To understand the development history and trends in organic electrode materials, we elaborate in detail various organics with different structures, including conducting polymers, organodisulfides, thioethers, nitroxyl radical polymers and conjugated carbonyl compounds. The high electrochemical performance, in addition with the unique features of organics such as flexibility, processability and structure diversity, provide them great perspective in various energy storage devices, including rechargeable Li/Na batteries, supercapacitors, thin film batteries, aqueous rechargeable batteries, redox flow batteries and even all-organic batteries. It is expected that organic electrode materials will show their talents in the “post Li-ion battery” era, towards cheap, green, sustainable and versatile energy storage devices.

Towards sustainable and versatile energy storage devices: an overview of organic electrode materials

Sodium-ion batteries (SIBs) receive significant attention for electrochemical energy storage and conversion owing to their wide availability and the low cost of Na resources. However, SIBs face challenges of low specific energy, short cycling life, and insufficient specific power, owing to the heavy mass and large radius of Na(+) ions. As an important component of SIBs, cathode materials have a significant effect on the SIB electrochemical performance. The most recent advances and prospects of inorganic and organic cathode materials are summarized here. Among current cathode materials, layered transition-metal oxides achieve high specific energies around 600 mW h g(-1) owing to their high specific capacities of 180-220 mA h g(-1) and their moderate operating potentials of 2.7-3.2 V (vs Na(+) /Na). Porous Na3 V2 (PO4 )3 /C nanomaterials exhibit excellent cycling performance with almost 100% retention over 1000 cycles owing to their robust structural framework. Recent emerging cathode materials, such as amorphous NaFePO4 and pteridine derivatives show interesting electrochemical properties and attractive prospects for application in SIBs. Future work should focus on strategies to enhance the overall performance of cathode materials in terms of specific energy, cycling life, and rate capability with cationic doping, anionic substitution, morphology fabrication, and electrolyte matching.

Recent Advances and Prospects of Cathode Materials for Sodium‐Ion Batteries

The storage of electric energy is of ever growing importance for our modern, technology-based society, and novel battery systems are in the focus of research. The substitution of conventional metals as redox-active material by organic materials offers a promising alternative for the next generation of rechargeable batteries since these organic batteries are excelling in charging speed and cycling stability. This review provides a comprehensive overview of these systems and discusses the numerous classes of organic, polymer-based active materials as well as auxiliary components of the battery, like additives or electrolytes. Moreover, a definition of important cell characteristics and an introduction to selected characterization techniques is provided, completed by the discussion of potential socio-economic impacts.

Polymer-Based Organic Batteries

Covalent organic frameworks (COFs) have attracted growing interest by virtue of their structural diversity and tunability. Herein, we present a novel approach for the development of organic rechargeable battery cathodes in which three distinct redox-active COFs were successfully prepared and delaminated into 2D few-layer nanosheets. Compared with the pristine COFs, the exfoliated COFs with shorter Li+ diffusion pathways allow a significant higher utilization efficiency of redox sites and faster kinetics for lithium storage. Unlike diffusion-controlled manners in the bulk COFs, the redox reactions in ECOFs are mainly dominated by charge transfer process. The capacity and potential are further engineered by reticular design of COFs without altering the underlying topology. Specifically, DAAQ-ECOF exhibits excellent rechargeability (98% capacity retention after 1800 cycles) and fast charge–discharge ability (74% retention at 500 mA g–1 as compared to at 20 mA g–1). DABQ-ECOF shows a specific capacity of 210 ...

Exfoliation of Covalent Organic Frameworks into Few-Layer Redox-Active Nanosheets as Cathode Materials for Lithium-Ion Batteries

The application of organic carbonyl compounds as high performance electrode materials in secondary batteries enables access to metal-free, low-cost, environmental friendly, flexible, and functional rechargeable energy storage systems. Organic compounds have so far not received much attention as potential active materials in batteries, mainly because of the success of inorganic materials in both research and commercial applications. However, new requirements in secondary batteries such as flexibility accompanied with low production costs and environmental friendliness, in particular for portable devices, reach the limit of inorganic electrode materials. Organic carbonyl compounds represent the most promising materials to satisfy these needs. Here, recent efforts of the research in the field of organic carbonyl materials for secondary batteries are summarized, and the working principle and the structural design of different groups of carbonyl material is presented. Finally, the influence of conductive additives and binders on the cell performance is closely evaluated for each class of materials.

Carbonyls: Powerful Organic Materials for Secondary Batteries

Organic rechargeable batteries have received significant research interest from the viewpoints of structural diversity and sustainability of electrode materials. We designed core structures of organic cathode materials for lithium-ion (Li-ion) batteries based on density functional theory (DFT) calculations, which indicated that six-membered cyclic 1,2-diketones serve as excellent core structures because of the high redox energy change resulting from favorable coordination of the oxygen atoms to Li and the aromaticity of the reduced form. Here, we show that the Li-ion battery composed of pyrene-4,5,9,10-tetraone (PYT), which has two six-membered cyclic 1,2-diketone units, bound to polymethacrylate exhibits remarkable charge–discharge properties with a high specific capacity of 231 mAh/g, excellent rechargeability (83% of the capacity retained after 500 cycles), and charge–discharge ability (90% of the capacity at 30 C as compared to 1 C) in the LiNTf2/tetraglyme ionic-liquid system.

Takahiro Matsuo

Papers

Polymer-bound pyrene-4,5,9,10-tetraone for fast-charge and -discharge lithium-ion batteries with high capacity.