Cherniuk O. Synthesis, modification and application of multiwall carbon nanotubes for molecular reinforcement of fiberglass based on epoxy resins

Українська версія

Thesis for the degree of Doctor of Philosophy (PhD)

State registration number

0824U003075

Thesis Registration Form

0824U003075.pdf

Applicant for

Specialization

  • 102 - Хімія

24-10-2024

Specialized Academic Board

ДФ 26.210.6871

Chuiko Institute of Surface Chemistry of NAS of Ukraine

Essay

The dissertation is devoted to the development of methods for modifying carbon nanotubes (CNTs) with oxygen by anodic oxidation, nitrogen in the process of CCVD synthesis of CNTs, to obtain effective reinforcing fillers of epoxy binder fiberglass with an amine hardener, their optimization in terms of composition and content, and the catalysis of redox reactions. It was optimized method of aerosol synthesis of the complex oxide catalyst (1…3)Al : Fe : (0,04…0,21), which includes the use of an aqueous solution of the compound of aluminum with formic acid and the compound of ferrum (III) citrate and the citrate complex of molybdenum (IV), feeding into an electric furnace or propane-butane burner's flame using an ultrasonic mixer-sprayer, and the catalyst powder is collected on an electrostatic precipitator. A method for the synthesis of N–CNTs by the CCVD method on a complex catalyst Al–Fe–Mo–O was developed using as a precursor acetonitrile, ethylenediamine and their mixtures with propylene — the main source of сarbon, at temperatures of 750—780 °C, which makes it possible to regulate nitrogen content in the range of 0.6—4.6 at.% and the ratio of its various states. It was established that the specific surface area of CNTs and the oxygen content during their anodic oxidation are a non-monotonic function of the amount of electricity passed and are correlated with each other. The CVD method of direct synthesis allows to obtain N–CNTs with a higher nitrogen content, mainly of pyrrole and quaternary type, and high catalytic activity in redox reactions. Regardless of the method of synthesis of N–CNTs, the maximum catalytic activity in the decomposition of hydrogen peroxide is observed at pH 7. It was established that the specific surface area of CNTs and the oxygen content during their anodic oxidation are a non-monotonic function of the amount of electricity passed through. For the first time, the synergistic effect of increasing the strength of fiberglass model samples by almost two times under the condition of introducing the initial (hydrophobic) CNTs into the hardener, and oxidized CNTs (O–CNTs) into the epoxy binder, compared to samples with the same content of CNTs in the same state (initial or oxidized). Using quantum chemical calculations, a scheme of chemical processes is proposed that explains the effect of the chemical state of the surface of CNTs on the polymerization of epoxy resin: equally charged O–CNTs have no tendency to reverse agglomeration, they catalyze the polymerization of epoxy resin, and the amine hardener performs the function of a surfactant in relation to initial hydrophobic CNTs, which also prevents the reverse agglomeration of CNTs, and together these phenomena lead to a synergistic effect of increasing the strength of the composite. Keywords: aerosol synthesis, catalytic vapors deposition, carbon nanotubes,anodic oxidation, N–CNT, O–CNT, fiberglass, synergistic effect, catalytic activity, quantum chemical modeling.

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Research papers

M.I. Terets, E.M. Demianenko, S.V. Zhuravsky, О.А. Сhernyuk, V.S. Kuts, A.G. Grebenyuk, Yu.I. Sementsov, L.M. Kokhtych, M.T. Kartel. Quantum chemical study on the interaction of carbon nanotube with polyethylene and polypropylene oligomers. Himia, Fizika ta Tehnologia Poverhni 10, p. 75—86 (2019). https://doi.org/10.15407/hftp10.01.075

M. Kartel, E. Demianenko, О. Сherniuk, M. Terets, Yu. Sementsov, B. Wang. Quantum-Chemical Estimating Interaction of sp2-Carbon Nanoclusters with PE and PP Oligomers. Journal of Materials Science and Chemical Engineering 7, p. 1—11 (2019). https://doi.org/10.4236/msce.2019.77001

Yu. Sementsov, O. Cherniuk, G. Dovbeshko, S. Zhuravskyi, S. Makhno, B. Wang, M. Kartel. Glass-Reinforced Plastic Filled by Multiwall Carbon Nanotubes and Their Modified Forms. Journal of Materials Science and Chemical Engineering 7, p. 26—35 (2019). https://doi.org/10.4236/msce.2019.77004

О.A. Cherniuk, E.M. Demianenko, M.I. Terets, S.V. Zhuravskyi, S.M. Makhno, V.V. Lobanov, M.T. Kartel, Yu.I. Sementsov. Study of the mechanism of influence of carbon nanotubes surface chemistry on the mechanical properties of fiberglass. Applied Nanoscience 10, p. 4797—4807 (2020). https://doi.org/10.1007/s13204-020-01448-1.

Yu. I. Sementsov, O. A. Cherniuk, S. V. Zhuravskyi, Wang Bo, K. V. Voitko, O. M. Bakalinska, M. T. Kartel. Synthesis and catalytic properties of nitrogencontaining carbon nanotubes. Himia, Fizika ta Tehnologia Poverhni 12(2), p. 135— 143 (2021). https://doi.org/10.15407/hftp12.02.135

Yu. Sementsov, Weiyou Yang, O. Cherniuk, K. Ivanenko, M. Kartel, S. Makhno, S. Zhuravskyi1. Synergistic effect of the strength increasing of fiberglass by reinforcing epoxy binder with carbon nanotubes. Applied Nanoscience 13(7), p. 5313—5321. https://doi.org/10.1007/s13204-023-02763-z

Патент № 126624 України від 02.11.2022. Заявка на винахід № а202104609 від 10.08.2021. Бюл. 44 від 02.11.2022. Спосіб виготовлення склопластику // Семенцов Ю.І, Чернюк О. А., Махно С.М., Картель М.Т, Гождзінський С.М., Іваненко К.О., Журавський С.В., Дин Анг (CN), Ван Бо (CN), Ван Дунсин (CN), Ли Тяньцзюнь (CN).

Патент України на корисну модель № 132497 від 25.02.2019, бюл. № 4, 25.02.2019. Спосіб одержання каталізатора для синтезу вуглецевих нанотрубок // Чернюк О.А., Журавський С.В., Ігнатенко О.М., Картель М.Т., Каплуненко В.Г., Махно С.М., Семенцов Ю.І.

O.A. Cherniuk, S.V. Zhuravsky, Yu.I. Sementsov, M.T. Kartel. Characteristics of elastomers filled with carbon nanotubes. Ukrainian Conference with International Participation “Chemistry, physics and technology of surface” (Kyiv, 23—24 May 2018), p. 37.

O.A. Cherniuk, S.V. Zhuravsky, Yu.I. Sementsov, M.T. Kartel. Characteristics of elastomers filled with carbon nanotubes. International research and practice conference «Nanotechnology and nanomaterials» (Kyiv, 27—30 August 2018), p. 344.

O.A. Чернюк, С.В. Журавський, Ю.І. Семенцов, M.Т. Kaртель. Cинтез складного металоксидного каталізатора для росту вуглецевих нанотрубок пірогенним методом. ІІI Всеукраїнська наукова конференція «Актуальні задачі хімії: дослідження та перспективи» (м. Житомир, 17 квітня 2019), с. 166—167.

O.A. Cherniuk, G.I. Dovbeshko, S.V. Zhuravskyi, S. Makhno, M.T. Kartel, Yu.I. Sementsov. Study of glass-reinforced plastic, filled by surface modified multiwall carbon nanotubes. Characteristics of elastomers filled with carbon nanotubes. Ukrainian Conference with International Participation “Chemistry, physics and technology of surface” (Kyiv, 15—17 May 2019), p. 46.

O.A. Cherniuk, S.V. Zhuravskyi, Makhno S. M., Yu.I. Sementsov, M.T. Kartel. Research of structures made of polymer composite materials filled with carbon nanotubes. International research and practice conference «Nanotechnology and nanomaterials» (Lviv, 27—30 August, 2019), p 160.

O. Cherniuk, Weiyou Yang, Yu. Grebelna, K. Ivanenko, M. Kartel, Yu. Sementsov, L. Ushakova, S. Zhuravskyi. Modification of carbon nanotubes by oxygen and nitrogen. Ist International research and practice conference «Nanoobjects and nanostructuring», (Lviv, 20—23 September, 2020), p.10.

О.А. Чернюк, Е.М. Дем’яненко, М.І. Терець, С.В. Журавський, С.М. Махно, В.В. Лобанов, М.Т. Картель, Ю.І. Семенцов. Дослідження механізму впливу хімії поверхні вуглецевих нанотрубок на механічні властивості склопластиків. IV Всеукраїнська наукова конференція «Актуальні задачі хімії: дослідження та перспективи» (м. Житомир, 29 квітня 2020), с. 110—111.

O.A. Cherniuk, S.V. Zhuravskyi, S. Makhno, M.T. Kartel, Yu.I. Sementsov. Synergistic effect of increasing the strength of the composite with the simultaneous addition of carbon nanotubes and their oxidized forms. Characteristics of elastomers filled with carbon nanotubes. Ukrainian Conference with International Participation“Chemistry, physics and technology of surface” (Kyiv, 21—22 October 2020), p. 46.

O.A. Cherniuk, S.V. Zhuravskyi, Yu.I. Sementsov, M.T. Kartel, K.V. Voitko, O.M. Bakalinska. Synthesis and catalytic properties of nitrogen-containing carbon nanotubes. International research and practice conference «Nanotechnology and nanomaterials» (Lviv, 25—27 August, 2021), p. 151.

M.T Kartel., Yu.I. Sementsov, O.A. Cherniuk, E.M. Demianenko, Yu.V. Grebelna, S.M. Makhno, M.I. Terets, S.V Zhuravskyi. Synergistic effect of the strength increasing of fiberglass by reinforcing epoxy binder with carbon nanotubes. EPF European Polymer Congress 2022 (Prague, 26 June—1 July 2022), p. 316.

O. Cherniuk, V. Tolmachova, S. Zhuravskyi, M. Terets, E. Demianenko, Y. Sementsov, M. Kartel Synthesis and Properties of Layered Materials Based on Epoxy Binder Reinforced with Carbon Nanotubes and their Oxygen-modified Forms. IEEE 12th International Conference “Nanomaterials: Applications & Properties” (IEEE NAP-2022). (Kraków, Poland, 11—16 September, 2022), p. 01nssa-34.

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