{"title":"Dual Single Atoms Boosting Photocatalytic Upcycling of Raw Polyvinylidene Fluoride Plastic","authors":"Amin Talebian‐Kiakalaieh, Shiying Ren, Wenzhong Ji, Yun Liu, Bingquan Xia, Jingrun Ran, Shi‐Zhang Qiao","doi":"10.1002/adma.75436","DOIUrl":null,"url":null,"abstract":"Polyvinylidene fluoride (PVDF) is a highly recalcitrant fluorinated polymer that is highly resistant to chemical degradation, making its sustainable recycling and upcycling challenging. Despite its widespread use as a binder in the lithium‐ion battery industry, effective strategies for converting PVDF waste into value‐added chemicals remain limited. To resolve this, Fe and Cu dual single atoms incorporated on a new two‐dimensional material nanosheets (In <jats:sub>2</jats:sub> P <jats:sub>3</jats:sub> S <jats:sub>9</jats:sub> NSs/Fe‐Cu DSAs) were prepared as photocatalysts for direct raw PVDF plastic conversion to high‐value chemicals. The best‐performing photocatalyst (Fe <jats:sub>1.0</jats:sub> Cu <jats:sub>0.5</jats:sub> ) achieves a total acetic/formic acid generation of ∼1351.8 µmol g <jats:sup>−1</jats:sup> . Various in situ characterizations such as atomic force microscopy‐kelvin probe force microscopy, x‐ray photoelectron spectroscopy, and electron paramagnetic resonance (EPR) demonstrate superior electron extraction from In <jats:sub>2</jats:sub> P <jats:sub>3</jats:sub> S <jats:sub>9</jats:sub> NSs to Fe and Cu DSAs, after which the electrons are subsequently scavenged by O <jats:sub>2</jats:sub> under ambient conditions. Moreover, quenching experiments as well as in situ infrared spectroscopy, and in situ EPR reveal the vital impact of photoexcited electrons and hydroxyl radicals in PVDF upcycling into high‐value products. These findings highlight the significant potential of photocatalysis in transforming one of the most resistant plastic wastes (PVDF) into value‐added products, providing a sustainable remedy for plastic pollution crisis.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"16 1","pages":""},"PeriodicalIF":29.1000,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/adma.75436","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Polyvinylidene fluoride (PVDF) is a highly recalcitrant fluorinated polymer that is highly resistant to chemical degradation, making its sustainable recycling and upcycling challenging. Despite its widespread use as a binder in the lithium‐ion battery industry, effective strategies for converting PVDF waste into value‐added chemicals remain limited. To resolve this, Fe and Cu dual single atoms incorporated on a new two‐dimensional material nanosheets (In 2 P 3 S 9 NSs/Fe‐Cu DSAs) were prepared as photocatalysts for direct raw PVDF plastic conversion to high‐value chemicals. The best‐performing photocatalyst (Fe 1.0 Cu 0.5 ) achieves a total acetic/formic acid generation of ∼1351.8 µmol g −1 . Various in situ characterizations such as atomic force microscopy‐kelvin probe force microscopy, x‐ray photoelectron spectroscopy, and electron paramagnetic resonance (EPR) demonstrate superior electron extraction from In 2 P 3 S 9 NSs to Fe and Cu DSAs, after which the electrons are subsequently scavenged by O 2 under ambient conditions. Moreover, quenching experiments as well as in situ infrared spectroscopy, and in situ EPR reveal the vital impact of photoexcited electrons and hydroxyl radicals in PVDF upcycling into high‐value products. These findings highlight the significant potential of photocatalysis in transforming one of the most resistant plastic wastes (PVDF) into value‐added products, providing a sustainable remedy for plastic pollution crisis.
聚偏氟乙烯(PVDF)是一种高度顽固的氟化聚合物,具有很强的抗化学降解性,这使得其可持续回收和升级利用具有挑战性。尽管PVDF在锂离子电池工业中广泛用作粘合剂,但将PVDF废物转化为增值化学品的有效策略仍然有限。为了解决这一问题,制备了一种新的二维材料纳米片(In 2 P 3 S 9 NSs/Fe - Cu dsa)上的Fe和Cu双单原子作为光催化剂,直接将原料PVDF塑料转化为高价值化学品。性能最好的光催化剂(Fe 1.0 Cu 0.5)的乙酸/甲酸总生成量为~ 1351.8µmol g−1。各种原位表征,如原子力显微镜-开尔文探针力显微镜,x射线光电子能谱和电子顺磁共振(EPR)证明了从in2p3s9nss到Fe和Cu dsa的优越电子萃取,之后电子随后在环境条件下被o2清除。此外,淬火实验、原位红外光谱和原位EPR揭示了光激发电子和羟基自由基对PVDF升级回收成高价值产品的重要影响。这些发现突出了光催化在将最具抗性的塑料废物(PVDF)转化为增值产品方面的巨大潜力,为塑料污染危机提供了可持续的补救措施。
期刊介绍:
Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.