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yexuqing木蟲之王 (文學(xué)泰斗)
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Photocatalytic low-temperature defluorination of PFASs
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Photocatalytic low-temperature defluorination of PFASs 全氟磺酸的光催化低溫除氟 ▲ 作者：Hao Zhang, Jin-Xiang Chen, Jian-Ping Qu & Yan-Biao Kang ▲鏈接： https://www.nature.com/articles/s41586-024-08179-1 ▲摘要： 多氟烷基和全氟烷基物質(zhì)（PFASs）存在于許多日常消費(fèi)品中，通常是因?yàn)樗鼈兙哂懈邿岱�(wěn)定性和化學(xué)穩(wěn)定性，以及疏水和疏油特性。然而，賦予全氟辛烷磺酸特性的惰性碳氟（C-F）鍵也提供了通過除氟分解的抵抗力，導(dǎo)致其長期存在于環(huán)境和人體中，引起了重大的安全和健康問題。盡管最近在銷毀功能化全氟辛烷的非焚燒方法方面取得了進(jìn)展，但回收全氟碳化合物以及聚四氟乙烯等聚合全氟辛烷的工藝僅限于使用高溫或強(qiáng)還原試劑的方法。 研究者報(bào)道了一種高度扭曲的咔唑核超光還原劑KQGZ對(duì)全氟烷的脫氟。在40℃ ~ 60℃的光催化條件下，一系列PFASs可被脫氟。聚四氟乙烯的主要產(chǎn)品是無定形碳和氟鹽。全氟化合物、全氟辛烷磺酸、多氟辛酸等低聚全氟磺酸及其衍生物的脫氟產(chǎn)品為碳酸鹽、甲酸鹽、草酸鹽和三氟乙酸鹽。這樣就可以將全氟磺酸中的氟作為無機(jī)氟化鹽進(jìn)行再循環(huán)。機(jī)理研究揭示了聚四氟乙烯和低聚全氟乙烯在反應(yīng)行為和產(chǎn)物組分上的差異。 這項(xiàng)研究為“永久化學(xué)物質(zhì)”全氟化合物的低溫光還原除氟，特別是聚四氟乙烯，以及新的超光還原劑的發(fā)現(xiàn)打開了一扇窗。 ▲ Abstract： Polyfluoroalkyl and perfluoroalkyl substances (PFASs) are found in many everyday consumer products, often because of their high thermal and chemical stabilities, as well as their hydrophobic and oleophobic properties1. However, the inert carbon–fluorine (C–F) bonds that give PFASs their properties also provide resistance to decomposition through defluorination, leading to long-term persistence in the environment, as well as in the human body, raising substantial safety and health concerns. Despite recent advances in non-incineration approaches for the destruction of functionalized PFASs, processes for the recycling of perfluorocarbons (PFCs) as well as polymeric PFASs such as polytetrafluoroethylene (PTFE) are limited to methods that use either elevated temperatures or strong reducing reagents. Here we report the defluorination of PFASs with a highly twisted carbazole-cored super-photoreductant KQGZ. A series of PFASs could be defluorinated photocatalytically at 40–60?°C. PTFE gave amorphous carbon and fluoride salts as the major products. Oligomeric PFASs such as PFCs, perfluorooctane sulfonic acid (PFOS), polyfluorooctanoic acid (PFOA) and derivatives give carbonate, formate, oxalate and trifluoroacetate as the defluorinated products. This allows for the recycling of fluorine in PFASs as inorganic fluoride salt. The mechanistic investigation reveals the difference in reaction behaviour and product components for PTFE and oligomeric PFASs. This work opens a window for the low-temperature photoreductive defluorination of the ‘forever chemicals’ PFASs, especially for PTFE, as well as the discovery of new super-photoreductants. |
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