Direct upcycling of polyethylene terephthalate (PET) waste bottles into α-Fe2O3 incorporated MIL-53(Al) for the synthesis of Al2O3/Fe3O4-encapsulated magnetic carbon composite and efficient removal of non-steroidal anti-inflammatory drugs

Eun Cho; Seon Yong Lee; Jae Woo Choi; Sang Hyoun Kim; Kyung Won Jung

doi:10.1016/j.seppur.2021.119719

Direct upcycling of polyethylene terephthalate (PET) waste bottles into α-Fe₂O₃ incorporated MIL-53(Al) for the synthesis of Al₂O₃/Fe₃O₄-encapsulated magnetic carbon composite and efficient removal of non-steroidal anti-inflammatory drugs

Eun Cho, Seon Yong Lee, Jae Woo Choi, Sang Hyoun Kim, Kyung Won Jung

Department of Civil and Environmental Engineering

Research output: Contribution to journal › Article › peer-review

5 Citations (Scopus)

Abstract

The upcycling of polyethylene terephthalate (PET) waste into high-value-added materials can have a significant contribution to global environmental protection. In this study, considering the unique thermal behaviors of PET and metal salts (i.e., Al and Fe) under similar hydrothermal conditions, we proposed a novel solvent-free one-pot approach for the upcycling of PET. In a one-pot hydrothermal reaction at 220 ℃ under self-generated pressure, PET waste was depolymerized into starting monomers (terephthalic acid and ethylene glycol), Al-based metal–organic frameworks (MIL-53(Al)) were fabricated, and iron oxides (α-Fe₂O₃) were formed simultaneously. X-ray diffraction measurements clearly demonstrated that α-Fe₂O₃ incorporated MIL-53(Al) (α-Fe₂O₃/MIL-53(Al)) was successfully synthesized directly from PET waste bottles via a novel green approach. After the annealing process, the α-Fe₂O₃/MIL-53(Al) precursor was successfully converted to an Al₂O₃/Fe₃O₄-encapsulated magnetic carbon composite (Al/Fe@MCC). The feasibility test proved that the Al/Fe@MCC prepared at an annealing temperature of 600 ℃ (Al/Fe@MCC₆₀₀) effectively removed four common non-steroidal anti-inflammatory drugs, i.e., ibuprofen (96.31%), diclofenac (66.84%), naproxen (87.83%), and ketoprofen (90.07%). Owing to its low removal rate, diclofenac was selected as the target pollutant, and the adsorption parameters were optimized using response surface methodology. Under the optimized conditions (solution pH = 5.0, adsorbent dosage = 1.21 g/L, and contact time = 15 h), the maximum actual diclofenac removal (92.94%) was obtained, which agreed with the maximum theoretical value (93.15%). In addition, Al/Fe@MCC₆₀₀ exhibited excellent reusability (removal rate > 85%) after five repetitive adsorption-regeneration cycles. This study demonstrates the promising opportunities for the upcycling PET waste bottles as efficient adsorbents for the removal of emerging environmental contaminants.

Original language	English
Article number	119719
Journal	Separation and Purification Technology
Volume	279
DOIs	https://doi.org/10.1016/j.seppur.2021.119719
Publication status	Published - 2021 Dec 15

Bibliographical note

Funding Information:
This study was financially supported by the National R&D Program through the National Research Foundation of Korea (NRF) funded by Ministry of Science and ICT ( 2020M3H4A3106366 ) and by an institutional program grant (2E31261) from the Korea Institute of Science and Technology. We would like to thank Editage for English language editing.

Publisher Copyright:
© 2021 Elsevier B.V.

All Science Journal Classification (ASJC) codes

Analytical Chemistry
Filtration and Separation

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Cho, E., Yong Lee, S., Choi, J. W., Kim, S. H., & Jung, K. W. (2021). Direct upcycling of polyethylene terephthalate (PET) waste bottles into α-Fe₂O₃ incorporated MIL-53(Al) for the synthesis of Al₂O₃/Fe₃O₄-encapsulated magnetic carbon composite and efficient removal of non-steroidal anti-inflammatory drugs. Separation and Purification Technology, 279, [119719]. https://doi.org/10.1016/j.seppur.2021.119719

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title = "Direct upcycling of polyethylene terephthalate (PET) waste bottles into α-Fe2O3 incorporated MIL-53(Al) for the synthesis of Al2O3/Fe3O4-encapsulated magnetic carbon composite and efficient removal of non-steroidal anti-inflammatory drugs",

abstract = "The upcycling of polyethylene terephthalate (PET) waste into high-value-added materials can have a significant contribution to global environmental protection. In this study, considering the unique thermal behaviors of PET and metal salts (i.e., Al and Fe) under similar hydrothermal conditions, we proposed a novel solvent-free one-pot approach for the upcycling of PET. In a one-pot hydrothermal reaction at 220 ℃ under self-generated pressure, PET waste was depolymerized into starting monomers (terephthalic acid and ethylene glycol), Al-based metal–organic frameworks (MIL-53(Al)) were fabricated, and iron oxides (α-Fe2O3) were formed simultaneously. X-ray diffraction measurements clearly demonstrated that α-Fe2O3 incorporated MIL-53(Al) (α-Fe2O3/MIL-53(Al)) was successfully synthesized directly from PET waste bottles via a novel green approach. After the annealing process, the α-Fe2O3/MIL-53(Al) precursor was successfully converted to an Al2O3/Fe3O4-encapsulated magnetic carbon composite (Al/Fe@MCC). The feasibility test proved that the Al/Fe@MCC prepared at an annealing temperature of 600 ℃ (Al/Fe@MCC600) effectively removed four common non-steroidal anti-inflammatory drugs, i.e., ibuprofen (96.31%), diclofenac (66.84%), naproxen (87.83%), and ketoprofen (90.07%). Owing to its low removal rate, diclofenac was selected as the target pollutant, and the adsorption parameters were optimized using response surface methodology. Under the optimized conditions (solution pH = 5.0, adsorbent dosage = 1.21 g/L, and contact time = 15 h), the maximum actual diclofenac removal (92.94%) was obtained, which agreed with the maximum theoretical value (93.15%). In addition, Al/Fe@MCC600 exhibited excellent reusability (removal rate > 85%) after five repetitive adsorption-regeneration cycles. This study demonstrates the promising opportunities for the upcycling PET waste bottles as efficient adsorbents for the removal of emerging environmental contaminants.",

author = "Eun Cho and {Yong Lee}, Seon and Choi, {Jae Woo} and Kim, {Sang Hyoun} and Jung, {Kyung Won}",

note = "Funding Information: This study was financially supported by the National R&D Program through the National Research Foundation of Korea (NRF) funded by Ministry of Science and ICT ( 2020M3H4A3106366 ) and by an institutional program grant (2E31261) from the Korea Institute of Science and Technology. We would like to thank Editage for English language editing. Publisher Copyright: {\textcopyright} 2021 Elsevier B.V.",

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Cho, E, Yong Lee, S, Choi, JW, Kim, SH & Jung, KW 2021, 'Direct upcycling of polyethylene terephthalate (PET) waste bottles into α-Fe₂O₃ incorporated MIL-53(Al) for the synthesis of Al₂O₃/Fe₃O₄-encapsulated magnetic carbon composite and efficient removal of non-steroidal anti-inflammatory drugs', Separation and Purification Technology, vol. 279, 119719. https://doi.org/10.1016/j.seppur.2021.119719

Direct upcycling of polyethylene terephthalate (PET) waste bottles into α-Fe₂O₃ incorporated MIL-53(Al) for the synthesis of Al₂O₃/Fe₃O₄-encapsulated magnetic carbon composite and efficient removal of non-steroidal anti-inflammatory drugs. / Cho, Eun; Yong Lee, Seon; Choi, Jae Woo et al.

In: Separation and Purification Technology, Vol. 279, 119719, 15.12.2021.

Research output: Contribution to journal › Article › peer-review

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T1 - Direct upcycling of polyethylene terephthalate (PET) waste bottles into α-Fe2O3 incorporated MIL-53(Al) for the synthesis of Al2O3/Fe3O4-encapsulated magnetic carbon composite and efficient removal of non-steroidal anti-inflammatory drugs

AU - Cho, Eun

AU - Yong Lee, Seon

AU - Choi, Jae Woo

AU - Kim, Sang Hyoun

AU - Jung, Kyung Won

N1 - Funding Information: This study was financially supported by the National R&D Program through the National Research Foundation of Korea (NRF) funded by Ministry of Science and ICT ( 2020M3H4A3106366 ) and by an institutional program grant (2E31261) from the Korea Institute of Science and Technology. We would like to thank Editage for English language editing. Publisher Copyright: © 2021 Elsevier B.V.

PY - 2021/12/15

Y1 - 2021/12/15

N2 - The upcycling of polyethylene terephthalate (PET) waste into high-value-added materials can have a significant contribution to global environmental protection. In this study, considering the unique thermal behaviors of PET and metal salts (i.e., Al and Fe) under similar hydrothermal conditions, we proposed a novel solvent-free one-pot approach for the upcycling of PET. In a one-pot hydrothermal reaction at 220 ℃ under self-generated pressure, PET waste was depolymerized into starting monomers (terephthalic acid and ethylene glycol), Al-based metal–organic frameworks (MIL-53(Al)) were fabricated, and iron oxides (α-Fe2O3) were formed simultaneously. X-ray diffraction measurements clearly demonstrated that α-Fe2O3 incorporated MIL-53(Al) (α-Fe2O3/MIL-53(Al)) was successfully synthesized directly from PET waste bottles via a novel green approach. After the annealing process, the α-Fe2O3/MIL-53(Al) precursor was successfully converted to an Al2O3/Fe3O4-encapsulated magnetic carbon composite (Al/Fe@MCC). The feasibility test proved that the Al/Fe@MCC prepared at an annealing temperature of 600 ℃ (Al/Fe@MCC600) effectively removed four common non-steroidal anti-inflammatory drugs, i.e., ibuprofen (96.31%), diclofenac (66.84%), naproxen (87.83%), and ketoprofen (90.07%). Owing to its low removal rate, diclofenac was selected as the target pollutant, and the adsorption parameters were optimized using response surface methodology. Under the optimized conditions (solution pH = 5.0, adsorbent dosage = 1.21 g/L, and contact time = 15 h), the maximum actual diclofenac removal (92.94%) was obtained, which agreed with the maximum theoretical value (93.15%). In addition, Al/Fe@MCC600 exhibited excellent reusability (removal rate > 85%) after five repetitive adsorption-regeneration cycles. This study demonstrates the promising opportunities for the upcycling PET waste bottles as efficient adsorbents for the removal of emerging environmental contaminants.

AB - The upcycling of polyethylene terephthalate (PET) waste into high-value-added materials can have a significant contribution to global environmental protection. In this study, considering the unique thermal behaviors of PET and metal salts (i.e., Al and Fe) under similar hydrothermal conditions, we proposed a novel solvent-free one-pot approach for the upcycling of PET. In a one-pot hydrothermal reaction at 220 ℃ under self-generated pressure, PET waste was depolymerized into starting monomers (terephthalic acid and ethylene glycol), Al-based metal–organic frameworks (MIL-53(Al)) were fabricated, and iron oxides (α-Fe2O3) were formed simultaneously. X-ray diffraction measurements clearly demonstrated that α-Fe2O3 incorporated MIL-53(Al) (α-Fe2O3/MIL-53(Al)) was successfully synthesized directly from PET waste bottles via a novel green approach. After the annealing process, the α-Fe2O3/MIL-53(Al) precursor was successfully converted to an Al2O3/Fe3O4-encapsulated magnetic carbon composite (Al/Fe@MCC). The feasibility test proved that the Al/Fe@MCC prepared at an annealing temperature of 600 ℃ (Al/Fe@MCC600) effectively removed four common non-steroidal anti-inflammatory drugs, i.e., ibuprofen (96.31%), diclofenac (66.84%), naproxen (87.83%), and ketoprofen (90.07%). Owing to its low removal rate, diclofenac was selected as the target pollutant, and the adsorption parameters were optimized using response surface methodology. Under the optimized conditions (solution pH = 5.0, adsorbent dosage = 1.21 g/L, and contact time = 15 h), the maximum actual diclofenac removal (92.94%) was obtained, which agreed with the maximum theoretical value (93.15%). In addition, Al/Fe@MCC600 exhibited excellent reusability (removal rate > 85%) after five repetitive adsorption-regeneration cycles. This study demonstrates the promising opportunities for the upcycling PET waste bottles as efficient adsorbents for the removal of emerging environmental contaminants.

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Cho E, Yong Lee S, Choi JW, Kim SH, Jung KW. Direct upcycling of polyethylene terephthalate (PET) waste bottles into α-Fe₂O₃ incorporated MIL-53(Al) for the synthesis of Al₂O₃/Fe₃O₄-encapsulated magnetic carbon composite and efficient removal of non-steroidal anti-inflammatory drugs. Separation and Purification Technology. 2021 Dec 15;279:119719. doi: 10.1016/j.seppur.2021.119719