Usuwanie zanieczyszczeń z roztworów wodnych w kolumnie wypełnionej - zagadnienia modelowania dynamiki adsorpcji

• Autorzy: Tomczak E. T.
• Języki publikacji: PL

Abstrakty

PL

Woda do celów przemysłowych i potrzeb ludności musi odpowiadać ściśle określonym wymogom. W celu pochłaniania zanieczyszczeń z roztworów stosuje się proces adsorpcji z wykorzystaniem adsorbentów stałych o silnie rozwiniętej powierzchni. W ostatnim dziesięcioleciu zauważa się zainteresowanie tanimi i nowymi adsorbentami do usuwania jonów metali ciężkich. Do badań wytypowano adsorbenty z różnych grup: - węgiel aktywny: najczęściej omawiany w literaturze tematu oraz jako materiał referencyjny do sprawdzenia poprawności obliczeń modelowych, - chitozan liofilizowany; stosunkowo nowy sorbent, polecany do usuwania jonów metali ciężkich, - klinoptylolit: tani sorbent mineralny pozyskiwany na terenie Polski, również wykorzystywany do usuwania jonów metali z roztworów rozcieńczonych, - łuskę gryki: nowy materiał należący do tzw. tanich sorbentów (Iow cost), szeroko dostępny w kraju ze względu na specyfikę naszego rolnictwa. W każdym z przypadków przedstawiono prawdopodobny mechanizm wiązania jonów metali ciężkich z danym adsorbentem. W opracowaniu przedstawiono aktualny stan wiedzy na temat określania i opisu matematycznego izoterm sorpcji z roztworów ciekłych, zjawisk zachodzących w roztworze, na powierzchni i wewnątrz ziarna adsorbentu, aby w dalszej kolejności przejść do mechanizmów adsorpcji w kolumnie wypełnionej. Przedstawiono najszerzej stosowany, klasyczny bilans masy oraz możliwości obliczania wielkości charakteryzujących pracę kolumny (współczynniki dyfuzji, wysokość strefy wymiany masy etc.). W dalszej części pracy skupiono się na prowadzeniu eksperymentów. Po wykonaniu pomiarów równowagi adsorpcyjnej, w drugim etapie pracy przeprowadzono badania w kolumnie laboratoryjnej. W obu przypadkach stosowano roztwory wieloskładnikowe jonów metali ciężkich: Cu(II), Zn(II) i Ni(II). Dodatkowo w pracy przedstawiono możliwość zastosowania sztucznych sieci neuronowych do opisu równowagi sorpcji w układach wieloskładnikowych. W dalszej kolejności (w rozważaniach inżynierskich), po wyborze odpowiedniego adsorbentu i badaniach wstępnych w małej skali, należy opracować model opisujący proces. W ramach pracy zaproponowano model matematyczny pozwalający na obliczenia stężenia roztworu na wylocie z kolumny i stężenia substancji adsorbowanej w adsorbencie, jak również krzywych przebicia dla różnych warunków prowadzenia procesu i wymiarów samej kolumny. Obliczenia prowadzono w środowisku obliczeniowym Matlaba z zastosowaniem własnych algorytmów obliczeniowych. Model dynamiki procesu w kolumnie uwzględniał specyfikę sorpcji opisanej równaniami kinetyki: pseudopierwszego rzędu (dla sorpcji fizycznej), pseudo-drugiego rzędu (dla chemisorpcji), Elovicha (dla sorpcji chemicznej i wymiany jonowej). Forma modelu zależała od tego, które z równań kinetycznych zostało w nim uwzględnione. Otrzymano więc trzy zestawy równań służących do wyznaczania parametrów pracy kolumny. W modelu uwzględniono, że czas procesu i analizowana wysokość kolumny są ze sobą powiązane. Wybierając dwa dowolne miejsca (przekroje) wzdłuż kolumny można obliczyć odpowiadające im wartości stężeń w cieczy i ilości substancji zaadsorbowanej. Wartości te wynikają z opóźnienia czasowego dopłynięcia adsorbatu do wyższego miejsca w kolumnie (przy zasilaniu od dołu), co uwzględniono przez wprowadzenie zmiennej ξ. Identyfikacja dynamiki w kolumnie polegała na znalezieniu współczynników modelu q*. K, Deff lub β, K, Deff (w przypadku wykorzystania równania Elovicha) i porównaniu wartości obliczonych z danymi eksperymentalnymi. Wprowadzenie wartości q* wyznaczonej w oparciu o równowagę urealniło wyniki i pozwoliło na obliczenie dwóch pozostałych parametrów modelu K i De(f. Poszukiwanie współczynników identyfikujących pracę kolumny może odbywać się z wykorzystaniem metod optymalizacyjnych przeszukujących dziedzinę dopuszczalnych rozwiązań w celu znalezienia ekstremum globalnego. W pracy do tego zadania wykorzystano algorytm genetyczny. Kolejnym etapem sprawdzenia poprawności działania modelu było wykonanie obliczeń w oparciu o dane literaturowe. Wybrano układy: modyfikowane barwnikiem (Reactive Orange 13) i Na2CO3 włókno kokosowe jako biosorbent oraz roztwór wodny jonów Pb(II) jako adsorbat; trociny - Cr(VI); węgiel aktywny - Cu(II). Porównano własne obliczenia modelowe z prezentowanymi w literaturze, uzyskując wyższą jakość przybliżenia danych eksperymentalnych niż w cytowanych pracach (przy dużo mniejszym nakładzie obliczeniowym). Dla każdego z badanych układów adsorbent-adsorbat przedstawiono wartości obliczonych parametrów modelu i ocenę statystyczną na podstawie: sumy kwadratów odchyleń wartości obliczonych i eksperymentalnych, kwadratu współczynnika determinacji i średniego błędu kwadratowego. Pomyślna weryfikacja opracowanego modelu opisującego proces dynamiki w kolumnie laboratoryjnej pozwala, aby w dalszym etapie rozważań przejść do problematyki powiększania skali i sterowania/kontrolowania on-line procesem przemysłowym.

EN

Water for the needs of industry and people must satisfy strictly determined requirements. To absorb pollutants from solutions, the process of adsorption with the use of solid adsorbents with strongly developed surface is applied. In the last decade a growing interest is observed in inexpensive and very cheap adsorbents to remove heavy metal ions. For our investigations adsorbents from various groups were selected: - activated carbon: most frequently discussed in the literature and used as a reference material to verify model calculations. - freeze-dried chitosan: a relatively new sorbent recommended to remove heavy metal ions, - clinoptilolite: a cheap mineral sorbent extracted in Poland used also to remove heavy metal ions from diluted solutions, - buckwheat hulls: an innovative material belonging to the so-called low-cost sorbents, readily available in Poland due to the specificity of our agriculture. In each case, a probable mechanism of binding heavy metal ions with the adsorbent is shown. The present state of knowledge on the determination and mathematical description of sorption isotherms from liquid solutions and phenomena occurring in the solution, on the surface and inside adsorbent particles are discussed in the study. Next, the mechanisms of adsorption in a packed column are presented. The most widely used, classical mass balance and the possibilities of calculating values which characterize column operation, such as diffusion coefficients, the height of mass transfer zone, etc. are considered. Experimental procedures are presented further in the study. Once adsorption equilibrium had been measured, experiments were carried out in a laboratory column. In both cases multicomponent solutions of heavy metal ions, i.e. Cu(II), Zn(II) and Ni(II), were used. Additionally, a possibility of applying artificial neural networks to describe sorption equilibrium in multicomponent systems is considered in the study. Further on, in engineering considerations, after choosing a promising adsorbent and carrying out preliminary investigations in a small scale, a model describing the process should be developed. A mathematical model to calculate the concentration of solution at the column outlet and the concentration of adsorbed substance in the adsorbent, as well as breakthrough curves for different process conditions and column dimensions was proposed in the study. Calculations were carried out in the Matlab computing environment. The model of process dynamics in the column took into account the specificity of sorption described by the kinetic equations of pseudo-first order (for physical sorption), pseudo-second order (for chemisorption) and Elovich equation (for chemical sorption and ion exchange). The model equations assumed forms which depended on which kinetic equation had been considered. Hence, three sets of equations were obtained to determine the column operation parameters. It was taken into account in the model that the process time and analyzed column height were interrelated. Two analyzed places in the column, both for the liquid and adsorbent, were delayed in time in relation to each other which was reflected by introducing variable ξ. Identification of the column dynamics consisted in finding model coefficients q*, K and Deff, or β , K and Deff when the Elovich equation was used, and comparing the calculated values with experimental data. Introduction of the value of q* determined on the basis of equilibrium made the results realistic and allowed us to calculate two other model parameters, i.e. K and Deff. Searching for the coefficients which identify the column operation can involve the use of optimization methods to find the area of feasible solutions in order to obtain a global extremum. To fulfill this task a genetic algorithm is applied in the study. A subsequent stage in the model verification were calculations based on literature data. The following systems were selected: modified with Reactive Orange 13 dye and Na2CO3 coconut fiber as a biosorbent and water solution of Pb(II) ions as an adsorbate; sawdust-Cr(VI); activated carbon-Cu(II). The model calculations were compared with those presented in the literature and the obtained approximation of experimental data appeared to be better than in the quoted studies (at a much lower computational effort). For each tested adsorbent-adsorbate system the calculated model parameters and statistical evaluation were presented on the basis of the sum of squared deviations of calculated and experimental values, the square of the determination coefficient and mean square error. A successful verification of the proposed model which describes process dynamics in the column is an encouragement for scaling-up and on-line control of an industrial process in the future.

Słowa kluczowe

PL

adsorpcja; roztwór wodny; kolumna z wypełnieniem; kolumna wypełniona; metale ciężkie; adsorbent; proces adsorpcji; adsorbenty stałe; woda; zanieczyszczenia

EN

adsorption; aqueous solution; packed column; heavy metals; adsorbents; adsorption process; solid adsorbents; water; pollutants

• Wydawca: Wydawnictwo Politechniki Łódzkiej
• Czasopismo: Zeszyty Naukowe. Rozprawy Naukowe / Politechnika Łódzka
• Rocznik: 2011
• Tom: Z. 412
• Strony: 5--172
• Opis fizyczny: Bibliogr. 225 poz.

Twórcy

autor

Tomczak E. T.

• Katedra Termodynamiki Procesowej, Politechnika Łódzka

Bibliografia

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