New Organic Electrode Materials As Cathode and Anode for All Organic Li-Ion Greener Batteries
Authors: Lakraychi Alae Eddine , Bonnet Jean-Pierre , Poizot Philippe , Becuwe Matthieu , Dolhem Franck 
Published: February 2020

Li-ion batteries (LIBs) meet nowadays some development bottlenecks because of the world high energy needs prompting the necessity of technology improvements particularly in terms of energy density of the inorganic cathode materials traditionally used. In addition to the environmental and safety concerns which become of primal importance.1,2

Because of their interesting electrochemical performance, their large structural diversity, their natural environmental friendliness, the flexibility they offer and their potential low cost, organic electrode materials become more-and-more promising candidates (for both positive and negative electrodes) for the next generation of sustainable LIBs.2,3,4

Conjugated carbonyl compounds have been early recognized as interesting electroactive materials characterized by high energy/power density and high cycling stability, but their implementation is still limited to Li cells with the serious safety issue caused by Li dendrite.3 To be successful the Li-ion organic battery technology needs first, the implementation of a lithiated positive electrode able of competing with LiCoO2 or LiFePO4and second, a negative electrode material operating at the target potentials just above 0.5 V (0.5-1.0 V) providing high output voltage as well as safety.

Seeking for such efficient organic materials, our research group has reported recently, for positive electrode application, two organic salts able to reversibly deintercalate Li ions with promising electrochemical performance.5,6 However their operating redox potential were still too low which makes them unstable in ambient environment (difficult to store) and reduce the final output voltage. Concerning the negative electrode application, we proposed π-extended carboxylate core unit thus improving the cycling rate capability.7,8

Herein we would like to report on the design, the preparation and the electrochemical performance of an efficient lithiated organic structure able of being reversibly delithiated at high redox potential (>3.0 V vs. Li+/Li0) as a lithiated organic positive electrode stable to air. We will also present a new approach with the aim to decrease the redox potential of carboxylate-based systems leading to a low operating redox potential (<0.8 V vs. Li+/Li0) allowing in addition to substitute copper-based current collector by aluminum. Both materials will pave the way toward a novel n-type all-organic Li-ion cell with a working voltage greater than 2 Volts.

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(3) Song, Z.; Zhou, H. Energy Environ. Sci. 2013, 6, 2280−2301

(4) Liang, Y.; Tao, Z.; Chen, J. Adv. Energy Mater. 2012, 2, 742−769

(5) Renault, S.; Gottis, S.; Courty, M.; Chauvet, O.; Dolhem, F.;Poizot, P. Energy Environ. Sci. 2013, 6, 2124−2133.

(6) Gottis, S.; Barrès A-L.; Dolhem, F.;Poizot, P. ACS Appl. Mater. Interfaces. 2014, 6, 10870−10876.

(7) Fédèle, L.; Sauvage, F.; Bois, J.; Tarascon, J.-M.; Bécuwe, M. Electrochem. Soc. 2014, 161, A46−A52

(8) Fédèle, L.; Sauvage, F.; Bécuwe, M. J. Mater. Chem. 2014, 6, 18225−18228.

Figure 1