Sorption Mechanisms and Enhancement of Selected Organochlorine Pollutants in Water on Zeolites

This study investigates the adsorption capacities of selected organochlorines on zeolites, focusing on hexachlorobenzene (HCB), hexachlorotetradecane (HCTD), hexachlorodecane (HCD), hexachlorocyclohexane (HCH), heptachlorodecane (HPCD), octachlorodecane (OCD), dichlorodiphenyltrichloroethane (DDT),...

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Main Authors: Timothy Manda, Solomon Omwoma, Godfrey Okumu Barasa, Anthony M. Pembere, Douglas Sifuna, Livingstone Ochilo, Silas Lagat, Emily Ngeno, Patrick Ssebugere, Christine Betty Nagawa, Christine Kyarimpa
Format: Article
Language:English
Published: Wiley 2024-01-01
Series:Journal of Chemistry
Online Access:http://dx.doi.org/10.1155/2024/4008315
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author Timothy Manda
Solomon Omwoma
Godfrey Okumu Barasa
Anthony M. Pembere
Douglas Sifuna
Livingstone Ochilo
Silas Lagat
Emily Ngeno
Patrick Ssebugere
Christine Betty Nagawa
Christine Kyarimpa
author_facet Timothy Manda
Solomon Omwoma
Godfrey Okumu Barasa
Anthony M. Pembere
Douglas Sifuna
Livingstone Ochilo
Silas Lagat
Emily Ngeno
Patrick Ssebugere
Christine Betty Nagawa
Christine Kyarimpa
author_sort Timothy Manda
collection DOAJ
description This study investigates the adsorption capacities of selected organochlorines on zeolites, focusing on hexachlorobenzene (HCB), hexachlorotetradecane (HCTD), hexachlorodecane (HCD), hexachlorocyclohexane (HCH), heptachlorodecane (HPCD), octachlorodecane (OCD), dichlorodiphenyltrichloroethane (DDT), and octachlorotetradecane (OCTD). The structures of the organochlorines were optimized and their Frontier molecular orbitals were calculated. The analysis of HOMO (highest occupied molecular orbital) and LUMO (lowest unoccupied molecular orbital) energies provided insights into the molecules’ electron-donating and -accepting capabilities. The present research identified the universal force field as suitable for the investigation and used it to evaluate the adsorption capacities of the pollutants on various zeolites. It was found that CLO (a cubic microporous gallophosphate) demonstrated the highest adsorption capacity for HCB among 245 zeolites, with a loading capacity of 65.84 wt%. In terms of molecules adsorbed per cell, CLO remained the highest with 120 molecules per cell for HCB, 113 molecules per cell for HCH, 43 molecules per cell for DDT, 21 molecules per cell for HCTD, 19 molecules per cell for OCTD, 47 molecules per cell for HCD, 30 molecules per cell for HPCD, and 22 molecules per cell for OCD. The analysis revealed correlations between the structural parameters of zeolites (mass, density, HVF, APV, VSA, GSA, DPS, and Di) and their adsorption capacities. The investigation delved into cluster models to understand the interaction of organochlorines with the zeolite framework. The study explored the impact of doping CLO zeolite with different atoms (Al, Si, and Na) on adsorption capacity. The results showed that doping with aluminum improved both loading capacity and adsorption energy and dissociate the chlorinated compounds during adsorption. Quantum chemical calculations show that hydrogen-based bonding of the organochlorides on the CLO is thermodynamically favorable compared to dissociative adsorption. In addition, oxygen atoms in the zeolites provide active adsorption sites. In the present work, laboratory adsorption experiments were performed, treating zeolites with heat at 400°C. Surprisingly, untreated zeolites outperformed treated ones, adsorbing up to 91% of HCB, while treated zeolites reached saturation after the third run. The study attributed the better performance of untreated zeolites to the presence of interstitial water and hydrogen atoms, which are critical for electrostatic interactions with organic compounds. In general, this research provides a comprehensive analysis of the adsorption capacities of organochlorines on zeolites, combining computational simulations and laboratory experiments. This work’s distinctive quality is its methodology that combines molecular simulations, experimental verification, doping, and interstitial water effects. The findings emphasize the importance of zeolite (a high-porosity nanostructured material) structure, composition, and treatment methods in determining their effectiveness as adsorbents for environmental pollutants.
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spelling doaj-art-e15987013cb74bc9b47c771d3027d3732025-08-20T03:21:06ZengWileyJournal of Chemistry2090-90712024-01-01202410.1155/2024/4008315Sorption Mechanisms and Enhancement of Selected Organochlorine Pollutants in Water on ZeolitesTimothy Manda0Solomon Omwoma1Godfrey Okumu Barasa2Anthony M. Pembere3Douglas Sifuna4Livingstone Ochilo5Silas Lagat6Emily Ngeno7Patrick Ssebugere8Christine Betty Nagawa9Christine Kyarimpa10Department of Physical SciencesDepartment of Physical SciencesDepartment of Physical SciencesDepartment of Physical SciencesDepartment of Physical SciencesDepartment of Physical SciencesDepartment of Physical SciencesDepartment of Physical SciencesDepartment of ChemistryDepartment of Forestry, Bio-Diversity and TourismDepartment of ChemistryThis study investigates the adsorption capacities of selected organochlorines on zeolites, focusing on hexachlorobenzene (HCB), hexachlorotetradecane (HCTD), hexachlorodecane (HCD), hexachlorocyclohexane (HCH), heptachlorodecane (HPCD), octachlorodecane (OCD), dichlorodiphenyltrichloroethane (DDT), and octachlorotetradecane (OCTD). The structures of the organochlorines were optimized and their Frontier molecular orbitals were calculated. The analysis of HOMO (highest occupied molecular orbital) and LUMO (lowest unoccupied molecular orbital) energies provided insights into the molecules’ electron-donating and -accepting capabilities. The present research identified the universal force field as suitable for the investigation and used it to evaluate the adsorption capacities of the pollutants on various zeolites. It was found that CLO (a cubic microporous gallophosphate) demonstrated the highest adsorption capacity for HCB among 245 zeolites, with a loading capacity of 65.84 wt%. In terms of molecules adsorbed per cell, CLO remained the highest with 120 molecules per cell for HCB, 113 molecules per cell for HCH, 43 molecules per cell for DDT, 21 molecules per cell for HCTD, 19 molecules per cell for OCTD, 47 molecules per cell for HCD, 30 molecules per cell for HPCD, and 22 molecules per cell for OCD. The analysis revealed correlations between the structural parameters of zeolites (mass, density, HVF, APV, VSA, GSA, DPS, and Di) and their adsorption capacities. The investigation delved into cluster models to understand the interaction of organochlorines with the zeolite framework. The study explored the impact of doping CLO zeolite with different atoms (Al, Si, and Na) on adsorption capacity. The results showed that doping with aluminum improved both loading capacity and adsorption energy and dissociate the chlorinated compounds during adsorption. Quantum chemical calculations show that hydrogen-based bonding of the organochlorides on the CLO is thermodynamically favorable compared to dissociative adsorption. In addition, oxygen atoms in the zeolites provide active adsorption sites. In the present work, laboratory adsorption experiments were performed, treating zeolites with heat at 400°C. Surprisingly, untreated zeolites outperformed treated ones, adsorbing up to 91% of HCB, while treated zeolites reached saturation after the third run. The study attributed the better performance of untreated zeolites to the presence of interstitial water and hydrogen atoms, which are critical for electrostatic interactions with organic compounds. In general, this research provides a comprehensive analysis of the adsorption capacities of organochlorines on zeolites, combining computational simulations and laboratory experiments. This work’s distinctive quality is its methodology that combines molecular simulations, experimental verification, doping, and interstitial water effects. The findings emphasize the importance of zeolite (a high-porosity nanostructured material) structure, composition, and treatment methods in determining their effectiveness as adsorbents for environmental pollutants.http://dx.doi.org/10.1155/2024/4008315
spellingShingle Timothy Manda
Solomon Omwoma
Godfrey Okumu Barasa
Anthony M. Pembere
Douglas Sifuna
Livingstone Ochilo
Silas Lagat
Emily Ngeno
Patrick Ssebugere
Christine Betty Nagawa
Christine Kyarimpa
Sorption Mechanisms and Enhancement of Selected Organochlorine Pollutants in Water on Zeolites
Journal of Chemistry
title Sorption Mechanisms and Enhancement of Selected Organochlorine Pollutants in Water on Zeolites
title_full Sorption Mechanisms and Enhancement of Selected Organochlorine Pollutants in Water on Zeolites
title_fullStr Sorption Mechanisms and Enhancement of Selected Organochlorine Pollutants in Water on Zeolites
title_full_unstemmed Sorption Mechanisms and Enhancement of Selected Organochlorine Pollutants in Water on Zeolites
title_short Sorption Mechanisms and Enhancement of Selected Organochlorine Pollutants in Water on Zeolites
title_sort sorption mechanisms and enhancement of selected organochlorine pollutants in water on zeolites
url http://dx.doi.org/10.1155/2024/4008315
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