Chemical Recycling of Polystyrene to Valuable Chemicals via Selective Acid-Catalyzed Aerobic Oxidation under Visible Light.
Chemical Recycling of Polystyrene to Valuable Chemicals via Selective Acid-Catalyzed Aerobic Oxidation under Visible Light.
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DOI：
10.1021/jacs.2c01410
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发表时间：
2022-04-13
影响因子：
15
通讯作者：
Xiao, Jianliang
中科院分区：
文献类型：
--
作者：
Huang, Zhiliang;Shanmugam, Muralidharan;Liu, Zhao;Brookfield, Adam;Bennett, Elliot L.;Guan, Renpeng;Herrera, David E. Vega;Lopez-Sanchez, Jose A.;Slater, Anna G.;McInnes, Eric J. L.;Qi, Xiaotian;Xiao, Jianliang
化学回收是最有前途的技术之一，可以通过提供塑料废物的解决方案来促进循环经济目标；然而，它仍处于开发的早期阶段。在这项工作中，我们描述了第一个光驱动、酸催化的方案，用于在1bar O2下将聚苯乙烯废料化学回收为有价值的化学品。该方案不需要光敏剂，反应条件温和，操作简单，也已在流动系统中得到验证。电子顺磁共振(EPR)研究和密度泛函理论(DFT)计算表明，在这个降解过程中，单线态氧作为活性氧物种，从三级C-H键中抽出一个氢原子，通过自由基过程导致氢过氧化和随后的C-C键断裂。值得注意的是，我们的研究表明，聚苯乙烯和酸性催化剂的加合物可能在原位形成，它可以作为光敏剂启动单线态氧的形成。此外，氧化后的聚苯乙烯聚合物可能在光下产生单线态氧中起作用。
Chemical recycling is one of the most promising technologies that could contribute to circular economy targets by providing solutions to plastic waste; however, it is still at an early stage of development. In this work, we describe the first light-driven, acid-catalyzed protocol for chemical recycling of polystyrene waste to valuable chemicals under 1 bar of O2. Requiring no photosensitizers and only mild reaction conditions, the protocol is operationally simple and has also been demonstrated in a flow system. Electron paramagnetic resonance (EPR) investigations and density functional theory (DFT) calculations indicate that singlet oxygen is involved as the reactive oxygen species in this degradation process, which abstracts a hydrogen atom from a tertiary C–H bond, leading to hydroperoxidation and subsequent C–C bond cracking events via a radical process. Notably, our study indicates that an adduct of polystyrene and an acid catalyst might be formed in situ, which could act as a photosensitizer to initiate the formation of singlet oxygen. In addition, the oxidized polystyrene polymer may play a role in the production of singlet oxygen under light.
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影响因子：
13.6
作者：
Geyer R;Jambeck JR;Law KL
通讯作者：
Law KL
影响因子：
15
作者：
Huang Z;Guan R;Shanmugam M;Bennett EL;Robertson CM;Brookfield A;McInnes EJL;Xiao J
通讯作者：
Xiao J
影响因子：
8.4
作者：
Chamas, Ali;Moon, Hyunjin;Suh, Sangwon
通讯作者：
Suh, Sangwon
DOI：
10.1098/rstb.2008.0205
发表时间：
2009-07-27
影响因子：
6.3
作者：
Barnes, David K. A.;Galgani, Francois;Barlaz, Morton
通讯作者：
Barlaz, Morton
影响因子：
2.9
作者：
Bancirova, Martina
通讯作者：
Bancirova, Martina