Direct Photoreforming of Real-World Polylactic Acid Plastics into Highly Selective Value-Added Pyruvic Acid under Visible Light

化学 聚乳酸 丙酮酸 选择性 脱羧 乳酸 产量(工程) 光催化 组合化学 有机化学 化学工程 光化学 催化作用 细菌 聚合物 复合材料 材料科学 工程类 生物 遗传学
作者
Yingxuan Miao,Yunxuan Zhao,Junyu Gao,Jinhu Wang,Tierui Zhang
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:146 (7): 4842-4850 被引量:165
标识
DOI:10.1021/jacs.3c13000
摘要

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 2 at a rate of 49.8 μmol g cat. –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 H 2 but also suppress competitive side reactions (e.g., lactic acid coupling or decarboxylation), consequently augmenting the yield and selectivity of pyruvic acid and H 2 . 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.
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