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在石墨相氮化碳催化剂上聚苯乙烯催化氧化制芳香族含氧化合物

Catalytic oxidation of polystyrene to aromatic oxygenates over a graphitic carbon nitride catalyst.

作者信息

Cao Ruochen, Zhang Mei-Qi, Hu Chaoquan, Xiao Dequan, Wang Meng, Ma Ding

机构信息

Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, People's Republic of China.

State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing, 100190, People's Republic of China.

出版信息

Nat Commun. 2022 Aug 16;13(1):4809. doi: 10.1038/s41467-022-32510-x.

Abstract

The continuous increase in manufacturing coupled with the difficulty of recycling of plastic products has generated huge amounts of waste plastics. Most of the existing chemical recycling and upcycling methods suffer from harsh conditions and poor product selectivity. Here we demonstrate a photocatalytic method to oxidize polystyrene to aromatic oxygenates under visible light irradiation using heterogeneous graphitic carbon nitride catalysts. Benzoic acid, acetophenone, and benzaldehyde are the dominant products in the liquid phase when the conversion of polystyrene reaches >90% at 150 °C. For the transformation of 0.5 g polystyrene plastic waste, 0.36 g of the aromatic oxygenates is obtained. The reaction mechanism is also investigated with various characterization methods and procedes via polystyrene activation to form hydroxyl and carbonyl groups over its backbone via C-H bond oxidation which is followed by oxidative bond breakage via C-C activation and further oxidation processes to aromatic oxygenates.

摘要

制造业的持续增长以及塑料制品回收的困难产生了大量的废塑料。现有的大多数化学回收和升级回收方法都存在条件苛刻和产品选择性差的问题。在此,我们展示了一种光催化方法,使用非均相石墨相氮化碳催化剂在可见光照射下将聚苯乙烯氧化为芳族含氧化合物。当聚苯乙烯在150°C下的转化率达到>90%时,苯甲酸、苯乙酮和苯甲醛是液相中的主要产物。对于0.5g聚苯乙烯塑料废料的转化,可获得0.36g芳族含氧化合物。还通过各种表征方法研究了反应机理,该反应通过聚苯乙烯活化在其主链上通过C-H键氧化形成羟基和羰基,随后通过C-C活化进行氧化键断裂,并进一步氧化为芳族含氧化合物。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/06e3/9381527/4898720d4d40/41467_2022_32510_Fig1_HTML.jpg

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