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Tytuł artykułu

Radiacyjnie i sonochemicznie indukowane reakcje rodników polimerowych w roztworach wodnych

Autorzy
Ulański P. , Ulański P.
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Warianty tytułu
Języki publikacji
PL
Abstrakty
PL
Reakcje rodnikowe w wodnych roztworach polimerów mogą być inicjowane różnymi metodami, na przykład poprzez termiczny rozkład inicjatora, ale również poprzez poddanie układu reakcyjnego działaniu promieniowania jonizującego lub ultradźwięków. Takie metody inicjowania stwarzają ciekawe możliwości badawcze i syntetyczne. W pracy opisano oryginalną metodę otrzymywania nanożeli polimerowych w układach zawierających jedynie polimer i wodę na drodze wewnątrz-cząsteczkowego sieciowania wielu rodników generowanych jednocześnie na łańcuchu polimerowym w wyniku krótkiego pulsu promieniowania jonizującego. Metodę tę, jak również jej zmodyfikowaną dwuetapową wersję, przetestowano na wielu polimerach hydrofilowych. W oparciu o badania doświadczalne i symulacje opisano kinetykę i mechanizm sieciowania wenątrzcząsteczkowego, ze szczególnym uwzględnieniem przyczyn niekla-sycznego, dyspersyjnego charakteru kinetyki tej reakcji. Opracowano też nową metodę badania równowagi propagacja-depropagacja w polimeryzacji rodnikowej, którą zastosowano do wykazania istnienia takiej równowagi dla modelowego polielektrolitu w temperaturze pokojowej i wyznaczenia stałych szybkości odpowiednich reakcji elementarnych. Wykazano, na przykładzie poli(kwasu metakrylowego) i chitozanu, że metody badawcze związane z wykorzystaniem promieniowania jonizującego do generowania rodników w wodnych roztworach polimerów mogą być przydatne do badania kinetyki i mechanizmu elementarnych reakcji rodnikowych w makrocząsteczkach polimerów syntetycznych i naturalnych. Dalsza część pracy dotyczyła sonochemii polimerów w roztworach wodnych. Wykazano, że istotną rolę w inicjowaniu reakcji sonochemicznych w takich układach pełnią rodniki OH. Zbadano i podjęto próby interpretacji wpływu wybranych parametrów prowadzenia reakcji sonochemiczych na ich wydajność w modelowym układzie polimerowym. Stwierdzono, że rozkład przestrzenny makrocząsteczek w wodnych roztworach poddanych działaniu ultradźwięków może być niehomogeniczny. Cząsteczki polimerów o częściowo hydrofobowym charakterze wykazują tendencję do skupiania się przy powierzchni oscylujących pęcherzyków kawitacyjnych, przez co ich lokalne stężenie w tej strefie, będącej równocześnie strefą reakcji z generowanymi w pęcherzykach rodnikami OH, może być o dwa rzędy wielkości wyższe niż ich średnie stężenie w roztworze. Ponadto wykazano, że polimery poddawane działaniu ultradźwięków mogą ulegać nie tylko degradacji, ale i sieciowaniu, a odpowiedni dobór substratów i warunków reakcji może prowadzić do sytuacji, w których sieciowanie jest procesem dominującym i obserwuje się wzrost średniego ciężaru cząsteczkowego polimeru. Udowodniono również, że jest możliwe otrzymywanie makroskopowych, trwałych hydrożeli poprzez poddawanie działaniu ultradźwięków wodnych roztworów monomerów dwu-funkcyjnych. Metoda ta jest bardzo prosta, a czas trwania reakcji w optymalnych warunkach jest nie dłuższy od jednej minuty.
EN
Free-radical reactions in aqueous solutions of polymers can be initiated in various ways, for instance by thermal decomposition of an initiator, but also by subjecting the substrate system to the action of ionizing radiation or ultrasound. The two latter methods are of considerable interest both for basic studies on reaction mechanisms and for synthetic applications. In this work an original method of synthesizing polymeric nanogels has been described, where a system consisting only of a polymer and water is treated with a short pulse of ionizing radiation, causing instantaneous formation of many radicals at each chain and their subsequent intramolecular recombination. This one-step method, along with its two-step version, has been successfully tested on a number of hydrophilic polymers. Based on experimental evidence and Monte Carlo simulations, kinetics and mechanism of intermolecular cross-linking have been described in some detail, with particular focus on explaining the reasons for non-classical, dispersive character of the kinetics. A new method for studying the propagation-depropagation equilibrium in free radical polymerization has been proposed and applied for detecting such an equilibrium in an exemplary polyelectrolyte at room temperature and for determining rate constants of the elementary reactions involved. It has been demonstrated, on the examples of poly(methacrylic acid) and chitosan, that the research methods related to radiation-induced generation of free radicals can be useful for studying kinetics and mechanism of elementary radical reactions in both synthetic and natural polymers in aqueous solutions. Second part of this work concerned sonochemistry of polymers in aqueous solutions. It has been shown that OH radicals may play an important role in initializing polymer reactions in such systems. An attempt has been made to assess and explain the influence of selected process parameters on the efficiency of sonochemical reactions in a model polymer system. It has been found that the spatial distribution of partially hydrophobic macromolecules in aqueous solutions subjected to the action of ultrasound is non-homogeneous. Such molecules tend to accumulate at the surface of oscillating cavitation bubbles, and therefore their local concentration at the immediate vicinity of the bubbles, i.e., in the reaction zone with OH radicals generated inside the bubbles, can be higher than their average solution concentration even by two orders of magnitude. It has been demonstrated that polymers can be not only degraded, but also cross-linked by the action of ultrasound. By appropriate selection of polymeric substrate and reaction conditions one can reach a situation where cross-linking dominates over degradation and an increase in the average molecular weight of the polymer is observed. It has been proved as well that one can synthesize permanent, macroscopic hydrogels by sonication of bifunctional monomers in aqueous solutions. The method is very simple, and the reaction time under optimum conditions is less than one minute.
Słowa kluczowe
PL
EN
Wydawca
Wydawnictwo Politechniki Łódzkiej
Czasopismo
Zeszyty Naukowe. Rozprawy Naukowe / Politechnika Łódzka
Rocznik
2008
Tom
Z. 368
Strony
3--166
Opis fizyczny
Bibliogr. 447 poz., tab., wykr.
Twórcy
autor
Ulański P.
autor
Ulański P.
  • Politechnika Łódzka. Międzyresortowy Instytut techniki Radiacyjnej
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