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.

/pdf/opportunities-and-challenges-for-organic-electrodes-in-5c3qesf3qc.pdf

Opportunities and Challenges for Organic Electrodes in Electrochemical Energy Storage.

Li-ion batteries presently operate on inorganic insertion compounds. The abundance and materials life-cycle costs of such batteries may present issues in the long term with foreseeable large-scale applications. To address the issue of sustainability of electrode materials, a radically different approach from the conventional route has been adopted to develop new organic electrode materials. The oxocarbon salt Li2C6O6 is synthesized through potentially low-cost processes free of toxic solvents and by enlisting the use of natural organic sources (CO2-harvesting entities). It contains carbonyl groups as redox centres and can electrochemically react with four Li ions per formula unit. Such battery processing comes close to both sustainable and green chemistry concepts, which are not currently present in Li-ion cell technology. The consideration of renewable resources in designing electrode materials could potentially enable the realization of green and sustainable batteries within the next decade.

https://chemistry-europe.onlinelibrary.wiley.com/doi/pdf/10.1002/cssc.200990010

From biomass to a renewable LixC6O6 organic electrode for sustainable Li-ion batteries.

Aromatic Carbonyl Derivative Polymers as High-Performance Li-Ion Storage Materials†

Poly(2,5-dihydroxy-1,4-benzoquinone-3,6-methylene): a new organic polymer as positive electrode material for rechargeable lithium batteries

Pillararene/calixarene-based functional materials have garnered significant attention for their unique topological/chemical structures and physicochemical properties, and their extended applications in electrochemistry have given rise to a promising area of research. This review details current advance in developing electrochemical energy materials based on pillararene/calixarene systems from the viewpoint of both fundamental theoretical simulations and research on practical applications. First, we discuss the underlying mechanisms of applying pillararene/calixarene-based systems for electrochemical energy applications. Second, we summarize simulation studies on pillarquinone and calixquinone with intrinsic structures for applications in batteries. In addition, state-of-the-art applications of pillararene/calixarene-based systems in electrochemical energy storage devices such as lithium/sodium-ion batteries and supercapacitors are highlighted. The diverse roles they play and the various design strategies that have been investigated for high-performance pillararene/calixarene-based batteries are analyzed. Finally, we discuss the prospects for further developments in this emerging field. This review not only describes recent advances in pillararene/calixarene-based batteries and supercapacitors but also lays a firm groundwork for their further application in electrochemical energy engineering.

Pillararene/calixarene-based systems for battery and supercapacitor applications

The electrochemical reduction of the oxocarbons: squarate, croconate and especially rhodizonate lithium salts have been studied in all solid state lithium batteries. Lithium rhodizonate cells were tested on cycling in the 1.5 – 3.5 V potential range The reduction of lithium rhodizonate occurs in two waves of two electrons. The number of electrons transferred in reduction on the first cycle was around 3.5 based on a capacity of 515 mA.h.g−1 and a discharge depth of 87 %. This process is quite reversible but we observed a fast decline of the capacity on cycling. This loss of capacity may be attributed to residual water in the salt. The reduction of the lithium croconate occurs at a potential of 1.8 V in a quasi-irreversible process. We could not observe the reduction of lithium squarate which occurs in the potential range where the lithium is inserted in carbon black. We also report an investigation on rhodizonate salts of transition metals. The best results, in term of capacity, on the 1.5 – 3.5 V potential range, were obtained with copper rhodizonate which exhibits a capacity of 579 mA.h.g−1 on the first discharge.

Novel Cathode Materials Based on Organic Couples for Lithium Batteries

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Novel Cathode Materials Based on Organic Couples for Lithium Batteries