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

IF 14.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Journal of the American Chemical Society Pub Date : 2024-01-31 DOI:10.1021/jacs.3c13000
Yingxuan Miao, Yunxuan Zhao*, Junyu Gao, Jinhu Wang and Tierui Zhang*, 
{"title":"Direct Photoreforming of Real-World Polylactic Acid Plastics into Highly Selective Value-Added Pyruvic Acid under Visible Light","authors":"Yingxuan Miao,&nbsp;Yunxuan Zhao*,&nbsp;Junyu Gao,&nbsp;Jinhu Wang and Tierui Zhang*,&nbsp;","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}
引用次数: 0

Abstract

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.

Abstract Image

Abstract Image

查看原文
分享 分享
微信好友 朋友圈 QQ好友 复制链接
本刊更多论文
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
尽管聚乳酸(PLA)是一种重要的可生物降解聚合物,但其可生物降解性无意中掩盖了有效回收技术的发展,导致碳资源的潜在浪费。聚乳酸的光转化-回收方法在概念和方法上都显示出巨大的潜力。然而,由于有机氧化产物的选择性有限,以及碱溶液辅助预水解所带来的成本增加和有机产物分离的挑战,该反应面临着巨大的挑战。在此,我们报告了一种利用 Pd-CdS 光催化剂在可见光照明下直接光转化聚乳酸塑料的无碱途径,从而避免了对聚乳酸的化学预处理。所设计的途径能以 49.8 μmol gcat.-1 h-1 的速率成功产生 H2,持续时间超过 100 小时,并对丙酮酸具有显著的选择性(液态产物中的选择性为 95.9%)。此外,实验结果还阐明,钯位点不仅是一种典型的协同催化剂,可增强 H2 的光催化进化,还能抑制竞争性副反应(如乳酸偶联或脱羧),从而提高丙酮酸和 H2 的产量和选择性。这项研究提供了一条直接、可持续的直接光转化路线,能够同时将塑料废物转化为有价值的化学品,从而为解决目前的环境挑战提供了一个前景广阔的解决方案。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 去求助
来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
期刊最新文献
Annulated 1,4-Disilabenzene-1,4-diide and Dihydrogen Splitting cis-Dihydroxylation by Synthetic Iron(III)-Peroxo Intermediates and Rieske Dioxygenases: Experimental and Theoretical Approaches Reveal the Key O-O Bond Activation Step. Retraction of "Solvent Polarity under Vibrational Strong Coupling". Ultra-Narrowband Circularly Polarized Luminescence from Multiple 1,4-Azaborine-Embedded Helical Nanographenes. Long-Lived Charge Carrier Photogeneration in a Cooperative Supramolecular Double-Cable Polymer
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
已复制链接
已复制链接
快去分享给好友吧!
我知道了
×
扫码分享
扫码分享
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1