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Enthalpy–entropy compensation and isoequilibrium relationship in thermo-chemical conversion of cigarette butt filters (CBFs) based on cellulose acetate (CA): causes and effects

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Abstract

The aim of this study is to explain the consequences of the occurrence of enthalpy–entropy compensation (EEC) and isoequilibrium relationship during slow pyrolysis of cigarette butt filters (CBFs), consisting cellulose acetate (AC) as the main component. By using model-free and model-based kinetic methods and thermodynamic calculations, the complete reaction mechanism and extrathermodynamic issues about investigated process are completely resolved. It was established that compensation phenomenon where isoequilibrium temperature occurs is a consequence of formation of low-entropy molecular structure (cellulose II) and breaking of hydrogen bonds. Consequently, it was concluded that mechanisms which include a formation of low-entropy molecular structure and H-bonds breakage enter the changes in both enthalpy and entropy, which compensate each other. For the cellulose II generation, it was necessary to invest energy which represents use up energy. This “wasted” energy turns into work for creation of cellulose II molecular structures, whereby additional energy was provided from “local” decomposition reactions (which were identified in the established process mechanism) that arise from pyrolysis of starting material. Therefore, it was concluded that for “local reactions”, a negative ΔS° value was identified, but for the global process, the entropy change retained a positive value. Considering thermodynamic effects manifested through compensation temperature found below glass transition temperature (Tg) in the undercooling conditions, it was concluded that small amounts of plasticizers affect reduction of free volume in the glassy state. Obtained results indicated a decrease in β-relaxation mode of cellulose acetate by an abatement of the polymer free volume.

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The datasets generated during and/or analyzed during the current study are available from the corresponding author on reasonable request.

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Funding

Authors would like to acknowledge financial support of Ministry of Science, Technological Development and Innovation of the Republic of Serbia, under Contract numbers 451-03-47/2023-01/200017 (“Vinča” Institute of Nuclear Sciences—National Institute of the Republic of Serbia), 451-03-47/2023-01/200105 (Faculty of Mechanical Engineering), and 451-03-47/2023-01/200051 (Institute of General and Physical Chemistry).

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Authors and Affiliations

  1. Department of Physical Chemistry, “Vinča” Institute of Nuclear Sciences – National Institute of the Republic of Serbia, University of Belgrade, Mike Petrovića Alasa 12-14, P.O. Box 522, 11001, Belgrade, Serbia

    Bojan Janković

  2. Department of Radiation Chemistry and Physics, “Vinča” Institute of Nuclear Sciences – National Institute of the Republic of Serbia, University of Belgrade, Mike Petrovića Alasa 12-14, P.O. Box 522, 11001, Belgrade, Serbia

    Milena Marinović-Cincović

  3. Fuel and Combustion Laboratory, Faculty of Mechanical Engineering, University of Belgrade, Kraljice Marije 16, P.O. Box 35, 11120, Belgrade, Serbia

    Nebojša Manić

  4. Radiation and Environmental Protection Department, “Vinča” Institute of Nuclear Sciences – National Institute of the Republic of Serbia, University of Belgrade, Mike Petrovića Alasa 12-14, P.O. Box 522, 11001, Belgrade, Serbia

    Marija Janković

  5. Institute of General and Physical Chemistry, University of Belgrade, Studentski trg 12/V, P.O. Box 45, 11158, Belgrade, Serbia

    Hadi Waisi

  6. Faculty of Ecology and Environmental Protection, University UNION-Nikola Tesla, Cara Dušana 62-64, Belgrade, Serbia

    Hadi Waisi

  7. Department of Materials Science, “Vinča” Institute of Nuclear Sciences – National Institute of the Republic of Serbia, University of Belgrade, Mike Petrovića Alasa 12-14, P.O. Box 522, 11001, Belgrade, Serbia

    Vladimir Dodevski

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  1. Bojan Janković
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Contributions

BJ was contributed to conceptualization, methodology, software, validation, formal analysis, data curation, writing—original draft, writing—review and editing, visualization, supervision, and project administration. MM-C was contributed to validation, investigation, data curation, writing—review and editing, and supervision. NM was contributed to methodology, software, validation, investigation, data curation, and supervision. MJ was contributed to methodology, validation, formal analysis, investigation, data curation, and supervision. HW was contributed to validation, formal analysis, investigation, resources, data curation, and supervision. VD was contributed to validation, investigation, resources, data curation, writing—review and editing, and supervision. All authors read and approved the final manuscript.

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Correspondence to Bojan Janković.

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Janković, B., Marinović-Cincović, M., Manić, N. et al. Enthalpy–entropy compensation and isoequilibrium relationship in thermo-chemical conversion of cigarette butt filters (CBFs) based on cellulose acetate (CA): causes and effects. Polym. Bull. (2024). https://doi.org/10.1007/s00289-024-05343-5

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