As the world moves toward electromobility and a concomitant decarbonization of its electrical supply, modern society is also entering a so-called fourth industrial revolution marked by a boom of electronic devices and digital technologies. Consequently, battery demand has exploded along with the need for ores and metals to fabricate them. Starting from such a critical analysis and integrating robust structural data, this review aims at pointing out there is room to promote organic-based electrochemical energy storage. Combined with recycling solutions, redox-active organic species could decrease the pressure on inorganic compounds and offer valid options in terms of environmental footprint and possible disruptive chemistries to meet the energy storage needs of both today and tomorrow. We review state-of-the-art developments in organic batteries, current challenges, and prospects, and we discuss the fundamental principles that govern the reversible chemistry of organic structures. We provide a comprehensive overview of all reported cell configurations that involve electroactive organic compounds working either in the solid state or in solution for aqueous or nonaqueous electrolytes. These configurations include alkali (Li/Na/K) and multivalent (Mg, Zn)-based electrolytes for conventional "sealed" batteries and redox-flow systems. We also highlight the most promising systems based on such various chemistries relying on appropriate metrics such as operation voltage, specific capacity, specific energy, or cycle life to assess the performances of electrodes.

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Opportunities and Challenges for Organic Electrodes in Electrochemical Energy Storage.

Sodium‐ion batteries (SIBs) are considered as promising candidates for large‐scale energy storage systems due to the wide availability and low cost of raw sodium resources. However, the heavier mass and larger radius of Na+ inevitably result in lower electrochemical kinetics and larger volume expansion of active materials than that of lighter and smaller Li+. To solve these problems, rational electrode design by integrating nanomaterials with graphene is an effective approach. In this review, the authors mainly focus on recent progress of graphene‐based nanomaterials for SIBs, including their design principle, preparation, characterization, and electrochemical performance. The important roles of graphene in graphene‐based inorganic and organic electrode materials are discussed in depth. In such composites, graphene can effectively enhance the electrical conductivity and mitigate volume change due to the robust and highly conductive networks formed by graphene. Moreover, the nanosized materials can enhance the reaction kinetics. Future research should focus on revealing the interaction mechanism between graphene and active materials, and improving the whole energy/power density, cycling stability, and the initial Coulombic efficiency of graphene‐based nanomaterials via elaborate design.

Graphene-Based Nanomaterials for Sodium-Ion Batteries

The limited availability of lithium is hindering the high demand of lithium-ion batteries (LIBs) resulting from rapid development in electric vehicle technology. Sodium-ion batteries (SIBs) are considered potential alternatives for LIBs owing to the large availability of sodium resources, low cost, and their similar electrochemical properties to LIBs. SIBs are also considered promising options for large-scale next-generation energy storage systems. In the last few decades, extensive research has been conducted to identify suitable anode materials for the high performance of SIBs. Among the carbonaceous materials, graphene exhibited excellent physical and chemical properties for utilization as the anode material, such as high specific surface area, energy storage density, and electric conductivity. The construction of composite anode materials through the incorporation of graphene with metal oxides and metal sulfides shows promising overall performance in SIBs. This paper critically reviews the recent advancements in graphene-based composite anode materials for SIBs, focusing on synthesis and energy storage techniques. The characteristics of various compositions and their energy storage behaviors are elaborately discussed and summarized. In addition, certain major challenges and advantages in graphene-based composite as a future anode materials for SIBs are discussed. This critical review illuminates a path to achieve economic, safe, and energy-efficient graphene composites as anode materials for SIBs.

Advancement in graphene-based nanocomposites as high capacity anode materials for sodium-ion batteries

High-performance graphene/disodium terephthalate electrodes with ether electrolyte for exceptional cooperative sodiation/desodiation

As a promising candidate for large-scale energy storage systems, sodium-ion batteries (SIBs) are experiencing a rapid development. Organic conjugated carboxylic acid anodes not only have tailorable electrochemical properties but also are easily accessible. However, the low stability and electrical conductivity hamper their practical applications. In this study, disodium terephthalate (Na2 TP), the most favorable organic conjugated carboxylic acid anode material for SIBs, was proposed to integrate with graphene oxide (GO) by an anti-solvent precipitation process, which ensures the uniform and tight coating of GO on the Na2 TP surface. GO is electrochemically reduced during the first several cycles of the electrochemical measurement, which buffers the volume change and improves the electrical conductivity of Na2 TP, resulting in a better cyclic and rate performance. The incorporation of only 5 wt % GO onto Na2 TP leads to a reversible capability of 235 mA h g-1 after 100 cycles at a current rate of 0.1 C, which is the best among the state of the art organic anodes for SIBs. The one-step synthesis together with the low costs of the raw materials show a promise for the scalable preparation of anode materials for practical SIBs.

A Reduced Graphene Oxide/Disodium Terephthalate Hybrid as a High‐Performance Anode for Sodium‐Ion Batteries

A reduced graphene oxide/disodium terephthalate (RGO/DST) composite was prepared via ultrasonic-assisted co-precipitation. The ultrasonication of an azeotropic H2O/acetonitrile solution at elevated temperature induced simultaneous precipitations of RGO and DST with solvent evaporation. RGO/DST, collected before complete evaporation, showed that the DST was in a well-dispersed state between the graphene layers of the RGO, giving the RGO/DST a more densely stacked microstructure. When applied as an anode for sodium ion batteries (SIBs), the RGO/DST revealed an enhancement in Na+-storage capability, relative to composites prepared via simple evaporation (E-RGO/DST) and mechanical mixing (M-RGO/DST). The RGO/DST delivered a reversible capacity of 422 mAh/g at a charge/discharge (C/D) rate of 50 mA/g, in contrast to 368 and 303 mAh/g for E-RGO/DST and M-RGO/DST, respectively. The superiority of the RGO/DST was maintained during repeated cycles. With an increase in the current densities, however, the reversible capability of the RGO/DST was decreased more substantially than that of the M-RGO/DST. Since Na+ diffusivity was greater in the RGO/DST than in the M-RGO/DST, this glitch in the high-rate performance of RGO/DST was considered because of a high level of charge-transfer impedance, in which a dense microstructure hampered the structural change of DST during reduction and oxidation.

Reduced Graphene Oxide/Disodium Terephthalate Composites via Ultrasonic‐assisted Co‐Precipitation for Sodium Ion Battery Anodes

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Reduced Graphene Oxide/Disodium Terephthalate Composites via Ultrasonic‐assisted Co‐Precipitation for Sodium Ion Battery Anodes