Yingxuan Miao, Yunxuan Zhao*, Junyu Gao, Jinhu Wang and Tierui Zhang*,
{"title":"在可见光下将现实世界中的聚乳酸塑料直接光转化为高选择性增值丙酮酸","authors":"Yingxuan Miao, Yunxuan Zhao*, Junyu Gao, Jinhu Wang and Tierui Zhang*, ","doi":"10.1021/jacs.3c13000","DOIUrl":null,"url":null,"abstract":"<p >Although polylactic acid (PLA) represents a pivotal biodegradable polymer, its biodegradability has inadvertently overshadowed the development of effective recycling techniques, leading to the potential wastage of carbon resources. The photoreforming–recycling approach for PLA exhibits significant potential in terms of concepts and methods. However, the reaction faces enormous challenges due to the limited selectivity of organic oxidation products as well as the increased costs and challenging separation of organic products associated with alkali-solution-assisted prehydrolysis. Herein, we report an alkali-free direct-photoreforming pathway for real-world PLA plastics utilizing the Pd-CdS photocatalyst under visible-light illumination, obviating the need for chemical pretreatment of PLA. The devised pathway successfully produces H<sub>2</sub> at a rate of 49.8 μmol g<sub>cat.</sub><sup>–1</sup> h<sup>–1</sup>, sustained over 100 h, and exhibits remarkable selectivity toward pyruvic acid (95.9% in liquid products). Additionally, experimental findings elucidate that Pd sites not only function as a typical cocatalyst for enhancing the photocatalytic evolution of H<sub>2</sub> but also suppress competitive side reactions (e.g., lactic acid coupling or decarboxylation), consequently augmenting the yield and selectivity of pyruvic acid and H<sub>2</sub>. This investigation provides a straightforward and sustainable direct-photoreforming route capable of simultaneously mitigating and repurposing plastic waste into valuable chemicals, thus offering a promising solution to the current environmental challenges.</p>","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":null,"pages":null},"PeriodicalIF":14.4000,"publicationDate":"2024-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Direct Photoreforming of Real-World Polylactic Acid Plastics into Highly Selective Value-Added Pyruvic Acid under Visible Light\",\"authors\":\"Yingxuan Miao, Yunxuan Zhao*, Junyu Gao, Jinhu Wang and Tierui Zhang*, \",\"doi\":\"10.1021/jacs.3c13000\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Although polylactic acid (PLA) represents a pivotal biodegradable polymer, its biodegradability has inadvertently overshadowed the development of effective recycling techniques, leading to the potential wastage of carbon resources. The photoreforming–recycling approach for PLA exhibits significant potential in terms of concepts and methods. However, the reaction faces enormous challenges due to the limited selectivity of organic oxidation products as well as the increased costs and challenging separation of organic products associated with alkali-solution-assisted prehydrolysis. Herein, we report an alkali-free direct-photoreforming pathway for real-world PLA plastics utilizing the Pd-CdS photocatalyst under visible-light illumination, obviating the need for chemical pretreatment of PLA. The devised pathway successfully produces H<sub>2</sub> at a rate of 49.8 μmol g<sub>cat.</sub><sup>–1</sup> h<sup>–1</sup>, sustained over 100 h, and exhibits remarkable selectivity toward pyruvic acid (95.9% in liquid products). Additionally, experimental findings elucidate that Pd sites not only function as a typical cocatalyst for enhancing the photocatalytic evolution of H<sub>2</sub> but also suppress competitive side reactions (e.g., lactic acid coupling or decarboxylation), consequently augmenting the yield and selectivity of pyruvic acid and H<sub>2</sub>. This investigation provides a straightforward and sustainable direct-photoreforming route capable of simultaneously mitigating and repurposing plastic waste into valuable chemicals, thus offering a promising solution to the current environmental challenges.</p>\",\"PeriodicalId\":49,\"journal\":{\"name\":\"Journal of the American Chemical Society\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":14.4000,\"publicationDate\":\"2024-01-31\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of the American Chemical Society\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/jacs.3c13000\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/jacs.3c13000","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Direct Photoreforming of Real-World Polylactic Acid Plastics into Highly Selective Value-Added Pyruvic Acid under Visible Light
Although polylactic acid (PLA) represents a pivotal biodegradable polymer, its biodegradability has inadvertently overshadowed the development of effective recycling techniques, leading to the potential wastage of carbon resources. The photoreforming–recycling approach for PLA exhibits significant potential in terms of concepts and methods. However, the reaction faces enormous challenges due to the limited selectivity of organic oxidation products as well as the increased costs and challenging separation of organic products associated with alkali-solution-assisted prehydrolysis. Herein, we report an alkali-free direct-photoreforming pathway for real-world PLA plastics utilizing the Pd-CdS photocatalyst under visible-light illumination, obviating the need for chemical pretreatment of PLA. The devised pathway successfully produces H2 at a rate of 49.8 μmol gcat.–1 h–1, sustained over 100 h, and exhibits remarkable selectivity toward pyruvic acid (95.9% in liquid products). Additionally, experimental findings elucidate that Pd sites not only function as a typical cocatalyst for enhancing the photocatalytic evolution of H2 but also suppress competitive side reactions (e.g., lactic acid coupling or decarboxylation), consequently augmenting the yield and selectivity of pyruvic acid and H2. This investigation provides a straightforward and sustainable direct-photoreforming route capable of simultaneously mitigating and repurposing plastic waste into valuable chemicals, thus offering a promising solution to the current environmental challenges.
期刊介绍:
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