Ultra-Fast and Economical Pre-Breakdown Electrochemical Synthesis of Intrinsically Conductive Polymer Suspension for Production of Safe Lithium-Ion Batteries

Evgenii Beletskii , Valentin Romanovski , Mikhail Pinchuk , Vadim Snetov , Alexey Volkov , Peixia Yang , Yurii K. Gun'ko

Energy & Environmental Materials ›› 2026, Vol. 9 ›› Issue (3) : e70179

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Energy & Environmental Materials ›› 2026, Vol. 9 ›› Issue (3) :e70179 DOI: 10.1002/eem2.70179
Research Article
Ultra-Fast and Economical Pre-Breakdown Electrochemical Synthesis of Intrinsically Conductive Polymer Suspension for Production of Safe Lithium-Ion Batteries
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Abstract

We report a novel pre-breakdown electrochemical synthesis method for producing polyNiMeOSalen suspensions with exceptional scalability and economic viability. Operating at ultra-high current density (1 A cm−2), this method achieves 83% yield and produces nanoscale particles (~30 nm) with superior electrochemical performance. The resulting P-polyNiMeOSalen demonstrates 1.7 times higher rate capability than conventional electrochemically synthesized materials, attributed to increased surface area and enhanced non-Faradaic contributions. Techno-economic analysis reveals remarkable commercial potential with production costs of circa $1500/kg (significantly lower than competing materials), rapid payback period (1.17 years), and high internal rate of return (49.5%). Despite the presence of impurities, P-polyNiMeOSalen, when employed as a protective layer in composite cathodes with NMC532, demonstrates negligible impact on the Coulombic efficiency of NMC532, achieving 99.3% by the fifth cycle. Furthermore, P-polyNiMeOSalen exhibits comparable protective properties to E-polyNiMeOSalen upon overcharge of NMC532 to 8 V. This scalable synthesis represents a paradigm shift toward the economically viable production of protective coatings for next-generation lithium-ion battery safety systems.

Keywords

electrode protective coatings / intrinsically conductive polymer / lithium-ion battery safety / overcharge protection / pre-breakdown electrochemical synthesis

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Evgenii Beletskii, Valentin Romanovski, Mikhail Pinchuk, Vadim Snetov, Alexey Volkov, Peixia Yang, Yurii K. Gun'ko. Ultra-Fast and Economical Pre-Breakdown Electrochemical Synthesis of Intrinsically Conductive Polymer Suspension for Production of Safe Lithium-Ion Batteries. Energy & Environmental Materials, 2026, 9 (3) : e70179 DOI:10.1002/eem2.70179

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References

[1]

L. Lu, X. Han, J. Li, J. Hua, M. Ouyang, J. Power Sources 2013, 226, 272.

[2]

Z. B. Omariba, L. Zhang, D. Sun, Des. Electron. 2018, 7, 72.

[3]

M. S. H. Lipu, M. A. Hannan, A. Hussain, M. M. Hoque, P. J. Ker, M. H. M. Saad, A. Ayob, J. Clean. Prod. 2018, 205, 115.

[4]

J. Zhu, T. Wierzbicki, W. Li, J. Power Sources 2018, 378, 153.

[5]

E. V. Beletskii, E. V. Alekseeva, O. V. Levin, Russ. Chem. Rev. 2022, 91, RCR5030.

[6]

Y. Matsuo, K. Fumita, T. Fukutsuka, Y. Sugie, H. Koyama, K. Inoue, J. Power Sources 2003, 119, 373.

[7]

D. Aurbach, K. Gamolsky, B. Markovsky, Y. Gofer, M. Schmidt, U. Heider, Electrochim. Acta 2002, 47, 1423.

[8]

S. Komaba, B. Kaplan, T. Ohtsuka, Y. Kataoka, N. Kumagai, H. Groult, J. Power Sources 2003, 119, 378.

[9]

K. Abraham, D. M. Pasquariello, E. B. Willstaedt, J. Electrochem. Soc. 1990, 137, 1856.

[10]

G. Halpert, S. Surampudi, D. Shen, C.-K. Huang, S. Narayanan, E. Vamos, D. Perrone, J. Power Sources 1993, 47, 287.

[11]

L. M. Moshurchak, C. Buhrmester, J. R. Dahn, J. Electrochem. Soc. 2008, 155, A129.

[12]

L. M. Moshurchak, W. M. Lamanna, M. Bulinski, R. L. Wang, R. R. Garsuch, J. Jiang, D. Magnuson, M. Triemert, J. R. Dahn, J. Electrochem. Soc. 2009, 156, A309.

[13]

X. M. Feng, X. P. Ai, H. X. Yang, J. Appl. Electrochem. 2004, 34, 1199.

[14]

S. Tobishima, Y. Ogino, Y. Watanabe, J. Appl. Electrochem. 2003, 33, 143.

[15]

L. Xia, D. Wang, H. Yang, Y. Cao, X. Ai, Electrochem. Commun. 2012, 25, 98.

[16]

M. Baginska, B. J. Blaiszik, S. A. Odom, A. E. Esser-Kahn, M. M. Caruso, J. S. Moore, N. R. Sottos, S. R. White, in Experimental Mechanics on Emerging Energy Systems and Materials, Volume 5 (Ed: T. Proulx), Springer, New York, NY 2011,

[17]

A. A. Fedorova, D. V. Anishchenko, E. V. Beletskii, A. Y. Kalnin, O. V. Levin, J. Power Sources 2021, 510, 230392.

[18]

E. V. Beletskii, A. A. Fedorova, D. A. Lukyanov, A. Y. Kalnin, V. A. Ershov, S. E. Danilov, D. V. Spiridonova, E. V. Alekseeva, O. V. Levin, J. Power Sources 2021, 490, 229548.

[19]

E. V. Beletskii, A. Y. Kal'nin, D. A. Luk'yanov, M. A. Kamenskii, D. V. Anishchenko, O. V. Levin, Russ. J. Electrochem. 2021, 57, 1028.

[20]

E. V. Beletskii, E. V. Alekseeva, D. V. Anishchenko, O. V. Levin, Batteries 2022, 8, 171.

[21]

E. V. Beletskii, A. I. Volkov, E. V. Alekseeva, D. V. Anishchenko, A. S. Konev, O. V. Levin, ACS Appl Energy Mater 2023, 6, 11242.

[22]

E. V. Beletskii, V. Romanovski, J. Power Sources 2024, 624, 235576.

[23]

Y. Lan, X. Li, G. Zhou, W. Yao, H. Cheng, Y. Tang, Adv. Sci. 2024, 11, 2304425.

[24]

J. Wang, J. Ma, Z. Zhuang, Z. Liang, K. Jia, G. Ji, G. Zhou, H.-M. Cheng, Chem. Rev. 2024, 124, 2839.

[25]

J. Song, H. Song, J. Song, G. Noh, H. Kim, J. Ma, J. Woo, Adv. Energy Mater. 2025, 15, 2402106.

[26]

E. Beletskii, A. Volkov, E. Evshchik, V. Kolmakov, A. Shikhovtseva, V. Romanovski, Energy Environ. Mater. 2024, 8, e12850.

[27]

S. K. Sen Gupta, Plasma Chem. Plasma Process. 2017, 37, 897.

[28]

G. B. Alteri, M. Bonomo, F. Decker, D. Dini, Catalysts 2020, 10, 1104.

[29]

A. L. Yerokhin, X. Nie, A. Leyland, A. Matthews, S. J. Dowey, Surf. Coat. Technol. 1999, 122, 73.

[30]

S. P. Davis, J. G. Phillips, Eds The Red System (A 2 Π-X 2~) of the CN Molecule, University of California Press, Berkeley, CA 1963.

[31]

Pyrolysis and combustion of acetonitrile (CH3CN), https://info.ornl.gov/sites/publications/Files/Pub57226.pdf (accessed: July 2025).

[32]

A. Lifshitz, A. Moran, S. Bidani, Int. J. Chem. Kinet. 1987, 19, 61.

[33]

I. E. Gordon, L. S. Rothman, R. J. Hargreaves, J. Quant. Spectrosc. Radiat. Transf. 2022, 277, 107949.

[34]

U. Fink, D. C. Benner, K. A. Dick, J. Quant. Spectrosc. Radiat. Transf. 1977, 18, 447.

[35]

A. E. Douglas, D. Sharma, J. Chem. Phys. 1953, 21, 448.

[36]

O. M. Lyulin, V. I. Perevalov, Journal of Quantitative Spectroscopy and Radiative Transfer 2016, 177, 59.

[37]

O. Kylian, A. Shelemin, P. Solar, A. Choukourov, J. Hanus, M. Vaidulych, A. Kuzminova, H. Biederman, Thin Solid Films 2017, 630, 86.

[38]

H. Y. Sohn, A. Murali, Molecules 2021, 26, 1456.

[39]

H. J. Jang, E. Y. Jung, T. Parsons, H.-S. Tae, C.-S. Park, Polymers (Basel) 2021, 13, 2267.

[40]

H. Jang, B. Shin, E. Jung, G. Bae, J. Kim, T. heung-sik, Appl. Surf. Sci. 2022, 608, 155129.

[41]

J.-G. Shin, C.-S. Park, E. Y. Jung, B. J. Shin, H.-S. Tae, Polymers 2019, 11, 105.

[42]

J. S. Danilova, S. M. Avdoshenko, M. P. Karushev, A. M. Timonov, E. Dmitrieva, J. Mol. Struct. 2021, 1241, 130668.

[43]

A. B. D. Nandiyanto, R. Ragadhita, M. Fiandini, Ind. J. Sci. Technol. 2023, 8, 113.

[44]

J. Polozhentseva, M. Novozhilova, M. Karushev, Int. J. Mol. Sci. 2022, 23, 1795.

[45]

N. Kuznetsov, P. Yang, G. Gorislov, Y. Zhukov, V. Bocharov, V. Malev, O. Levin, Electrochim. Acta 2018, 271, 190.

[46]

L. Chiang, A. Kochem, O. Jarjayes, T. J. Dunn, H. Vezin, M. Sakaguchi, T. Ogura, M. Orio, Y. Shimazaki, F. Thomas, Chem. Eur. J. 2012, 18, 14117.

[47]

L. Chiang, R. M. Clarke, K. Herasymchuk, M. Sutherland, K. E. Prosser, Y. Shimazaki, T. Storr, Eur. J. Inorg. Chem. 2016, 2016, 49.

[48]

R. Schnepf, A. Sokolowski, J. Müller, V. Bachler, K. Wieghardt, P. Hildebrandt, J. Am. Chem. Soc. 1998, 120, 2352.

[49]

M. Cochet, G. Louarn, S. Quillard, M. I. Boyer, J. P. Buisson, S. Lefrant, J. Raman Spectrosc. 2000, 31, 1029.

[50]

B. A. Kolesov, Int. J. Mol. Sci. 2021, 22, 5380.

[51]

P. M. Korusenko, O. V. Petrova, A. A. Vereshchagin, K. P. Katin, O. V. Levin, S. V. Nekipelov, D. V. Sivkov, V. N. Sivkov, A. S. Vinogradov, Int. J. Mol. Sci. 2023, 24, 9868.

[52]

T. Semenistaya, Russ. J. Inorg. Chem. 2004, 50, 912.

[53]

E. Beletskii, V. Ershov, S. Danilov, D. Lukyanov, E. Alekseeva, O. Levin, Polymers 2020, 12, 1.

[54]

X. Li, J. Li, F. Kang, Ionics (Kiel) 2019, 25, 1045.

[55]

E. V. Beletskii, Y. A. Volosatova, S. N. Eliseeva, O. V. Levin, Russ. J. Electrochem. 2019, 55, 339.

[56]

M. Karushev, E. Smirnova, I. Chepurnaya, Molecules 2021, 26, 2646.

[57]

J. Heinze, B. A. Frontana-Uribe, S. Ludwigs, Chem. Rev. 2010, 110, 4724.

[58]

B. Löchel, H. Strehblow, J. Electrochem. Soc. 1984, 131, 713.

[59]

G. I. Svirskiy, A. V. Generalov, N. A. Vinogradov, X. O. Brykalova, A. V. Vereshchagin, O. V. Levin, A. G. Lyalin, A. B. Preobrajenski, A. S. Vinogradov, Phys. Chem. Chem. Phys. 2021, 23, 11015.

[60]

M. Barber, J. A. Connor, M. F. Guest, I. H. Hillier, M. Schwarz, M. Stacey, J. Chem. Soc. Faraday Trans. 2 Mol. Chem. Phys. 1973, 69, 551.

[61]

I. Chepurnaya, M. Karushev, E. Alekseeva, D. Lukyanov, O. Levin, Pure Appl. Chem. 2020, 1, 1239.

[62]

E. V. Alekseeva, J. V. Novoselova, D. V. Anischenko, V. V. Potapenkov, O. V. Levin, Polymers (Basel) 2023, 15, 1323.

[63]

X. Chen, X. Wang, D. Fang, Nanotub. Carbon Nanostructures 2020, 28, 1048.

[64]

T. R. Gengenbach, G. H. Major, M. R. Linford, C. D. Easton, J. Vac. Sci. Technol. A 2021, 39, 013204.

[65]

H. Shi, Q. Ouyang, X. Wang, Y. Yang, T. Song, J. Hao, X. Huang, Measurement 2022, 200, 111565.

[66]

H. W. Nesbitt, D. Legrand, G. M. Bancroft, Phys. Chem. Miner. 2000, 27, 357.

[67]

E. Beletskii, M. Pinchuk, V. Snetov, A. Dyachenko, A. Volkov, E. Savelev, V. Romanovski, ChemPlusChem 2024, 89, e202400427.

[68]

Y. Abe, N. Hori, S. Kumagai, Energies 2019, 12, 4507.

[69]

N. Vicente, M. Haro, G. Garcia-Belmonte, Chem. Commun. 2018, 54, 1025.

[70]

D. Pritzl, A. E. Bumberger, M. Wetjen, J. Landesfeind, S. Solchenbach, H. A. Gasteiger, J. Electrochem. Soc. 2019, 166, A582.

[71]

H. Li, X. Zhang, C. Zhang, Y. Cao, H. Yang, X. Ai, F. Zhong, Energ. Technol. 2020, 8, 2000365.

[72]

H. Maddali, A. M. Tyryshkin, D. M. O'Carroll, ACS Appl. Electron. Mater. 2021, 3, 4718.

[73]

H. Chen, S. Miao, L. Hui, Y. Cao, X. Ai, Y. Fang, ChemSusChem 2025, 18, e202500398.

[74]

C. Liu, K. Oshima, M. Shimomura, S. Miyauchi, J. Appl. Polym. Sci. 2005, 97, 1848.

[75]

A. Yankin, D. Lukyanov, E. Beletskii, O. Bakulina, P. Vlasov, O. Levin, Chemistryselect 2019, 4, 8886.

[76]

D. V. Anishchenko, O. V. Levin, V. V. Malev, Electrochim. Acta 2016, 188, 480.

[77]

S. N. Eliseeva, E. V. Alekseeva, A. A. Vereshchagin, A. I. Volkov, P. S. Vlasov, A. S. Konev, O. V. Levin, Macromol. Chem. Phys. 2017, 1, 1700361.

[78]

D. V. Horváth, J. Coelho, R. Tian, V. Nicolosi, J. N. Coleman, ACS Appl Energy Mater 2020, 3, 10154.

[79]

X. Chen, F. Meng, Z. Zhou, X. Tian, L. Shan, S. Zhu, X. Xu, M. Jiang, L. Wang, D. Hui, Nanoscale 2014, 6, 8140.

[80]

Z. Chen, Y. Qin, K. Amine, Electrochim. Acta 2009, 54, 5605.

[81]

T. Pham-Truong, Q. Wang, J. Ghilane, H. Randriamahazaka, ChemSusChem 2020, 13, 2142.

[82]

N. Mao, T. Zhang, Z. Wang, Q. Cai, J. Power Sources 2022, 518, 230767.

[83]

Y. Kang, J. Wang, L. Du, Z. Liu, X. Zou, X. Tang, Z. Cao, C. Wang, D. Xiong, Q. Shi, Y. Qian, Y. Deng, ACS Appl Energy Mater 2019, 2, 8615.

[84]

Z. Wu, S. Ji, J. Zheng, Z. Hu, S. Xiao, Y. Wei, Z. Zhuo, Y. Lin, W. Yang, K. Xu, K. Amine, F. Pan, Nano Lett. 2015, 15, 5590.

[85]

H. Cui, L. Wang, Y. Song, T. Lai, Z. Liu, D. Ren, H. Zhang, X. He, Energy Storage Mater 2025, 75, 104094.

[86]

A. Shodiev, F. M. Zanotto, J. Yu, M. Chouchane, J. Li, A. A. Franco, Energy Storage Mater 2022, 49, 268.

[87]

H. Yoshida, N. Imamura, T. Inoue, K. Komada, Electrochemistry 2003, 71, 1018.

[88]

W. Ji, F. Wang, D. Liu, J. Qian, Y. Cao, Z. Chen, H. Yang, X. Ai, J Mater Chem A 2016, 4, 11239.

[89]

H. Zhang, J. Pang, X. Ai, Y. Cao, H. Yang, S. Lu, Electrochim. Acta 2016, 187, 173.

[90]

H. Zuo, K. Yuan, W. Zhou, N. Chen, A. Wang, D. Zhao, X. Liang, L. Li, Electrochim. Acta 2024, 504, 144950.

[91]

T. Li, J. Li, C. Lu, L. Wang, J. Luo, Chem. Eng. J. 2023, 452, 139620.

[92]

D. Tomczyk, W. Bukowski, K. Bester, P. Urbaniak, P. Seliger, G. Andrijewski, S. Skrzypek, New J. Chem. 2017, 41, 2112.

[93]

D. Tomczyk, W. Bukowski, K. Bester, J. Electrochem. Soc. 2019, 166, H194.

[94]

D. Tomczyk, W. Bukowski, K. Bester, Electrochim. Acta 2018, 267, 181.

[95]

M. Novozhilova, J. Polozhentseva, M. Karushev, Polymers (Basel) 2023, 15, 1127.

[96]

K. Łępicka, P. Pieta, A. Shkurenko, P. Borowicz, M. Majewska, M. Rosenkranz, S. Avdoshenko, A. A. Popov, W. Kutner, J. Phys. Chem. C 2017, 121, 16710.

[97]

E. V. Antipov, A. M. Abakumov, O. A. Drozhzhin, D. V. Pogozhev, Therm. Eng. 2019, 66, 219.

[98]

V. Nilsson, R. Younesi, D. Brandell, K. Edström, P. Johansson, J. Power Sources 2018, 384, 334.

[99]

L. Yu, Y. Tian, Y. Xing, C. Hou, Y. Si, H. Lu, Y. Zhao, Ionics (Kiel) 2021, 27, 5021.

[100]

S. Zhang, K. Xu, R. Jow, J. Electrochem. Soc. 2002, 149, A586.

[101]

D. Zhao, D. Lei, P. Wang, S. Li, H. Zhang, X. Cui, ChemistrySelect 2019, 4, 5853.

[102]

E.-S. Hong, S. Okada, T. Sonoda, S. Gopukumar, J. Yamaki, J. Electrochem. Soc. 2004, 151, A1836.

[103]

X. Zhou, X. Gao, M. Liu, Z. Gao, X. Qin, W. Xu, S. Ye, W. Zhou, H. Fan, J. Li, Nat. Commun. 2022, 13, 4379.

[104]

Polypyrrole, doped, 5 wt % dispersion in H2O, conductivity >0.005 S/cm (dried cast film), https://www.scientificlabs.co.uk/product/organic-and-printed-electronics/482552-100ML#specification (accessed: July 2025).

[105]

Made-in-China, https://epochmaterial.en.made-in-china.com/ (accessed: July 2025).

[106]

E. V. Alekseeva, I. A. Chepurnaya, V. V. Malev, A. M. Timonov, O. V. Levin, Electrochim. Acta 2017, 225, 378.

[107]

R. Tian, S.-H. Park, P. J. King, G. Cunningham, J. Coelho, V. Nicolosi, J. N. Coleman, Nat. Commun. 2019, 10, 1933.

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