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Graphene Acid for Lithium-Ion Batteries—Carboxylation Boosts Storage Capacity in Graphene

  • Environmentally sustainable, low-cost, flexible, and lightweight energy storage technologies require advancement in materials design in order to obtain more efficient organic metal-ion batteries. Synthetically tailored organic molecules, which react reversibly with lithium, may address the need for cost-effective and eco-friendly anodes used for organic/lithium battery technologies. Among them, carboxylic group-bearing molecules act as high-energy content anodes. Although organic molecules offer rich chemistry, allowing a high content of carboxyl groups to be installed on aromatic rings, they suffer from low conductivity and leakage to the electrolytes, which restricts their actual capacity, the charging/discharging rate, and eventually their application potential. Here, a densely carboxylated but conducting graphene derivative (graphene acid (GA)) is designed to circumvent these critical limitations, enabling effective operation without compromising the mechanical or chemical stability of the electrode. Experiments including operando Raman measurements and theoretical calculations reveal the excellent charge transport, redox activity, and lithium intercalation properties of the GA anode at the single-layer level, outperforming all reported organic anodes, including commercial monolayer graphene and graphene nanoplatelets. The practical capacity and rate capability of 800 mAh g−1 at 0.05 A g−1 and 174 mAh g−1 at 2.0 A g−1 demonstrate the true potential of GA anodes in advanced lithium-ion batteries.

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Document Type:Article
Author:Ievgen ObraztsovORCiD, Aristides BakandritsosORCiD, Veronika SedajováORCiD, Rostislav Langer, Petr Jakubec, Giorgio ZoppellaroORCiD, Martin PykalORCiD, Volker PresserORCiD, Michael OtyepkaORCiD, Radek ZborilORCiD
Parent Title (English):Advanced energy materials
First Page:2103010
Date of Publication (online):2021/12/22
Year of first Publication:2022
Release Date:2022/05/19
Tag:lithium ion batteries
carboxylation; graphene acid; organic anodes
Impact:29.698 (2021)
Funding Information:European Regional Development Fund European Social Fund (CZ.02.1.01/0.0/0.0/16_019/0000754) Grantová Agentura České Republiky (19–27454X) Univerzita Palackého v Olomouci (IGA_PrF_2021_031) H2020 European Research Council (683024)
DDC classes:600 Technik, Medizin, angewandte Wissenschaften / 624 Ingenieurbau und Umwelttechnik
Open Access:Open Access
Signature:INM 2022/003
Licence (German):License LogoCreative Commons - CC BY - Namensnennung 4.0 International