Catalytic oxidation upcycling of polyethylene terephthalate to commodity carboxylic acids
Abstract Catalytic upcycling of polyethylene terephthalate (PET) into high-value oxygenated products is a fascinating process, yet it remains challenging. Here, we present a one-step tandem strategy to realize the thermal catalytic oxidation upcycling of PET to terephthalic acid (TPA) and high-value...
Saved in:
| Main Authors: | , , , , , , , , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2024-12-01
|
| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-54822-w |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1841559280657891328 |
|---|---|
| author | Qinghai Chen Hao Yan Kai Zhao Shuai Wang Dongrui Zhang Yaqian Li Rong Fan Jie Li Xiaobo Chen Xin Zhou Yibin Liu Xiang Feng De Chen Chaohe Yang |
| author_facet | Qinghai Chen Hao Yan Kai Zhao Shuai Wang Dongrui Zhang Yaqian Li Rong Fan Jie Li Xiaobo Chen Xin Zhou Yibin Liu Xiang Feng De Chen Chaohe Yang |
| author_sort | Qinghai Chen |
| collection | DOAJ |
| description | Abstract Catalytic upcycling of polyethylene terephthalate (PET) into high-value oxygenated products is a fascinating process, yet it remains challenging. Here, we present a one-step tandem strategy to realize the thermal catalytic oxidation upcycling of PET to terephthalic acid (TPA) and high-value glycolic acid (GA) instead of ethylene glycol (EG). By using the Au/NiO with rich oxygen vacancies as catalyst, we successfully accelerate the hydrolysis of PET, accompanied by obtaining 99% TPA yield and 87.6% GA yield. The results reveal that the oxygen vacancies in NiO (NiO-Ov) support tend to adsorb hydrolysis product TPA, preferentially ensuring the strong adsorption of EG at the Au-NiO interface. Moreover, during the EG oxidation process, the Au-NiO interface, composed of two types of structures, quasi “AuNi alloy” and NiO-Ov, simultaneously promote the C-H bond activation, where Ni in “AuNi alloy” exhibits an oxytropism effect to anchor the C = O bond of the intermediate, while the residual O in NiO-Ov pillages the H in the C-H bond. Such Au/NiO catalyst is further extended to promote the thermal catalytic oxidation upcycling of other polyethylene glycol esters to GA with excellent catalytic performance. |
| format | Article |
| id | doaj-art-548e7a19563e4c89b5f552414ffe7ff8 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2024-12-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-548e7a19563e4c89b5f552414ffe7ff82025-01-05T12:35:35ZengNature PortfolioNature Communications2041-17232024-12-0115111110.1038/s41467-024-54822-wCatalytic oxidation upcycling of polyethylene terephthalate to commodity carboxylic acidsQinghai Chen0Hao Yan1Kai Zhao2Shuai Wang3Dongrui Zhang4Yaqian Li5Rong Fan6Jie Li7Xiaobo Chen8Xin Zhou9Yibin Liu10Xiang Feng11De Chen12Chaohe Yang13State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China)State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China)State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China)State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China)State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China)State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China)State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China)State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China)State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China)College of Chemistry and Chemical Engineering, Ocean University of ChinaState Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China)State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China)Department of Chemical Engineering, Norwegian University of Science and TechnologyState Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China)Abstract Catalytic upcycling of polyethylene terephthalate (PET) into high-value oxygenated products is a fascinating process, yet it remains challenging. Here, we present a one-step tandem strategy to realize the thermal catalytic oxidation upcycling of PET to terephthalic acid (TPA) and high-value glycolic acid (GA) instead of ethylene glycol (EG). By using the Au/NiO with rich oxygen vacancies as catalyst, we successfully accelerate the hydrolysis of PET, accompanied by obtaining 99% TPA yield and 87.6% GA yield. The results reveal that the oxygen vacancies in NiO (NiO-Ov) support tend to adsorb hydrolysis product TPA, preferentially ensuring the strong adsorption of EG at the Au-NiO interface. Moreover, during the EG oxidation process, the Au-NiO interface, composed of two types of structures, quasi “AuNi alloy” and NiO-Ov, simultaneously promote the C-H bond activation, where Ni in “AuNi alloy” exhibits an oxytropism effect to anchor the C = O bond of the intermediate, while the residual O in NiO-Ov pillages the H in the C-H bond. Such Au/NiO catalyst is further extended to promote the thermal catalytic oxidation upcycling of other polyethylene glycol esters to GA with excellent catalytic performance.https://doi.org/10.1038/s41467-024-54822-w |
| spellingShingle | Qinghai Chen Hao Yan Kai Zhao Shuai Wang Dongrui Zhang Yaqian Li Rong Fan Jie Li Xiaobo Chen Xin Zhou Yibin Liu Xiang Feng De Chen Chaohe Yang Catalytic oxidation upcycling of polyethylene terephthalate to commodity carboxylic acids Nature Communications |
| title | Catalytic oxidation upcycling of polyethylene terephthalate to commodity carboxylic acids |
| title_full | Catalytic oxidation upcycling of polyethylene terephthalate to commodity carboxylic acids |
| title_fullStr | Catalytic oxidation upcycling of polyethylene terephthalate to commodity carboxylic acids |
| title_full_unstemmed | Catalytic oxidation upcycling of polyethylene terephthalate to commodity carboxylic acids |
| title_short | Catalytic oxidation upcycling of polyethylene terephthalate to commodity carboxylic acids |
| title_sort | catalytic oxidation upcycling of polyethylene terephthalate to commodity carboxylic acids |
| url | https://doi.org/10.1038/s41467-024-54822-w |
| work_keys_str_mv | AT qinghaichen catalyticoxidationupcyclingofpolyethyleneterephthalatetocommoditycarboxylicacids AT haoyan catalyticoxidationupcyclingofpolyethyleneterephthalatetocommoditycarboxylicacids AT kaizhao catalyticoxidationupcyclingofpolyethyleneterephthalatetocommoditycarboxylicacids AT shuaiwang catalyticoxidationupcyclingofpolyethyleneterephthalatetocommoditycarboxylicacids AT dongruizhang catalyticoxidationupcyclingofpolyethyleneterephthalatetocommoditycarboxylicacids AT yaqianli catalyticoxidationupcyclingofpolyethyleneterephthalatetocommoditycarboxylicacids AT rongfan catalyticoxidationupcyclingofpolyethyleneterephthalatetocommoditycarboxylicacids AT jieli catalyticoxidationupcyclingofpolyethyleneterephthalatetocommoditycarboxylicacids AT xiaobochen catalyticoxidationupcyclingofpolyethyleneterephthalatetocommoditycarboxylicacids AT xinzhou catalyticoxidationupcyclingofpolyethyleneterephthalatetocommoditycarboxylicacids AT yibinliu catalyticoxidationupcyclingofpolyethyleneterephthalatetocommoditycarboxylicacids AT xiangfeng catalyticoxidationupcyclingofpolyethyleneterephthalatetocommoditycarboxylicacids AT dechen catalyticoxidationupcyclingofpolyethyleneterephthalatetocommoditycarboxylicacids AT chaoheyang catalyticoxidationupcyclingofpolyethyleneterephthalatetocommoditycarboxylicacids |