Toward Maximizing the Gravimetric Capacity of Carbonyl-Based Electrode Materials for K-Ion Batteries

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Despite the current breakthroughs in the progress of lithium-ion batteries (LIBs), the ever-growing market demand/expenses and the incorporation of environmentally hazardous materials in LIBs will not relieve corresponding challenges by 2030.1 Therefore, implementing practical strategies to address these challenges is imperative by either recycling precious elements from used batteries or introducing alternative technologies such as post-lithium batteries.2 To address these issues, novel electrode materials must be produced from light and earth-abundant elements such as alkaline Na, K, and non-metallic N, H, S, O P, and F. Potassium-ion batteries (KIBs) have been considered a proper replacement due to the vast abundance of K and a number of its fundamental advantages over Li such as higher electropositivity in carbonate electrolytes resulting in higher electrode potentials, faster diffusion in liquids owing to smaller Stoke’s radius and in solids due to larger ionicity of K-O bonds, non-alloying with aluminum, etc.3. In addition, a substantial amount of research has been focused on introducing non-toxic and environmentally benign electrode materials for metal-ion batteries. Redox-active polymers represent a promising solution. Organic redox-active materials could enable record-high capacities and energy densities since they are composed of common lightweight chemical elements. Another important feature of organic redox-active materials is that they usually have a soft amorphous structure, which makes them non-specific to the inserting ions. Therefore, the same material can operate equally well in Li, Na, and K-ion batteries. Among all explored organic materials, carbonyl-containing organic redox-active materials have attracted tremendous attention. However, this class of materials has some challenges such as solubility, capacity fading, low conductivity, and tap density.4 Herein, this talk focuses on circumventing the predominant obstacles in the further developments of carbonyl-containing organic materials, which are the stabilization and optimization of specific capacity, electrode composition, and gravimetric capacity while using 11 types of organic redox-active materials (OHTAP, OHTAPQ, and P1-P9).5–8 Our investigation revealed that applying the super-concentrated electrolyte (2.2 M KPF6 in diglyme) optimized the cyclability and discharge capacity of P1-P9, e.g. P1 delivers the specific capacity of 420 mAh g-1 after 400 cycles @ current density (0.5 A g-1) with no faded capacity. Finally, the gravimetric capacity of P7-P9 was improved, e.g. P7 delivers >140 mAh g-1 at 70 mAh g-1 while consuming 10 Wt.% of MWCNT and 85 Wt.% of P7. References 1 C. Friebe, A. Lex-Balducci and U. S. Schubert, ChemSusChem, 2019, 12, 4093–4115. 2 J. Neumann, M. Petranikova, M. Meeus, J. D. Gamarra, R. Younesi, M. Winter and S. Nowak, John Wiley and Sons Inc, Adv. Energy Mater.2022, 12, 2102917. 3 T. Hosaka, K. Kubota, A. S. Hameed and S. Komaba, Chem Rev, 2020, 120, 6358–6466. 4 Y. Lu, Q. Zhang, L. Li, Z. Niu and J. Chen, Chem, 2018, 4, 2786–2813. 5 V. Ramezankhani, I. K. Yakuschenko, A. V. Mumyatov, S. G. Vasil’ev, I. S. Zhidkov, E. Z. Kurmaev, A. F. Shestakov and P. A. Troshin, J Power Sources, 2022, 517, 230711 6 V. Ramezankhani, A. Kozlov, E. V. Shchurik, S. Pluczyk-Małek, S. Vasil’ev, A. V. Mumyatov, M. Lapkowski, A. F. Shestakov and P. A. Troshin, J Power Sources, 2023, 562, 232744. 7 A. Slesarenko, I. K. Yakuschenko, V. Ramezankhani, V. Sivasankaran, O. Romanyuk, A. V. Mumyatov, I. Zhidkov, S. Tsarev, E. Z. Kurmaev, A. F. Shestakov, O. V. Yarmolenko, K. J. Stevenson and P. A. Troshin, J Power Sources, 2019, 435, 226724. 8 V. Ramezankhani, I. K. Yakuschenko, S. Vasilyev, T. A. Savinykh, A. V Mumyatov, I. S. Zhidkov, E. V Shchurik, E. Z. Kurmaev, A. F. Shestakov and P. A. Troshin, J. Mater. Chem. A, 2022, 10, 3044-3050

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