Construction of Multistep Charge Transfer Pathways in Bi0@Bi3+-KNbO3 for Significantly Accelerated Photoconversion of Waste Plastics

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2025-03-22 DOI:10.1002/anie.202502874
Xulong Fan, Lidan Lan, Yuanyu Chang, Long Yang, Yun Huang, Yi Dan, Long Jiang
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Abstract

Photoconversion of waste plastics into valuable CO and CH3COOH represents a ground-breaking strategy for addressing plastic pollution issues. However, this process currently encounters significant challenges, primarily due to the limitation of catalyst activity and the difficulty in breaking C─C bonds. Herein, we present a novel approach that integrates multistep charge transfer pathways with photothermal-driven reactions to improve photoconversion efficiency. By incorporating Bi0/Bi3+ metal as an electron transport mediator for multistep charge transfer, we markedly enhanced the separation and transport of photoelectrons, thereby accelerating the generation of active species. Meanwhile, the heat generated by the localized surface plasmon resonance effect of Bi0 drove the reactions related to the photoconversion of polypropylene. Subsequently, the photoconversion rates of PP into CO by Bi0@Bi3+-KNbO3 reached 209.41 µmol gcat−1 h−1, which is 27.55 times higher than that achieved with KNbO3. Furthermore, the dual Bi–Nb sites effectively stabilize the key intermediate *COOH, thereby promoting the production of CH3COOH at a rate of 213.00 µmol gcat−1 h−1. This strategy of boosting photoconversion activity of PP into CO and CH3COOH offers an effective green solution to the serious issue of plastic pollution.

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在Bi0@Bi3+-KNbO3中构建多步电荷转移途径以显著加速废塑料的光转化
废塑料光转化为有价值的CO和CH3COOH代表了解决塑料污染问题的突破性战略。然而,该工艺目前面临着重大挑战,主要是由于催化剂活性的限制和C-C键断裂的困难。在此,我们提出了一种将多步电荷转移途径与光热驱动反应相结合的新方法,以提高光转换效率。通过加入Bi0/Bi3+金属作为多步电荷转移的电子传递介质,我们显著增强了光电子的分离和传递,从而加速了活性物质的产生。同时,Bi0的局部表面等离子体共振效应产生的热量驱动了聚丙烯的光转化相关反应。随后,Bi0@Bi3+-KNbO3将PP转化为CO的光转化率达到209.41 μmol gcat-1 h-1,是使用KNbO3的光转化率的27.55倍。此外,双Bi-Nb位点有效地稳定了关键中间体*COOH,从而以213.00 μmol gcat-1 h-1的速率促进了CH3COOH的生成。这种提高PP向CO和CH3COOH的光转化活性的策略为严重的塑料污染问题提供了有效的绿色解决方案。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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