Zhou Yuting, Rodríguez-López Joaquín, Moore Jeffrey S
Beckman Institute for Advanced Science and Technology, University of Illinois at Urbana-Champaign, Urbana, IL, USA.
Joint Center for Energy Storage Research, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, IL, 60439, USA.
Nat Commun. 2023 Aug 10;14(1):4847. doi: 10.1038/s41467-023-39362-z.
Post-consumer plastic waste in the environment has driven the scientific community to develop deconstruction methods that yield valued substances from these synthetic macromolecules. Electrocatalysis is a well-established method for achieving challenging transformations in small molecule synthesis. Here we present the first electro-chemical depolymerization of polyoxymethylene-a highly crystalline engineering thermoplastic (Delrin®)-into its repolymerizable monomer, formaldehyde/1,3,5-trioxane, under ambient conditions. We investigate this electrochemical deconstruction by employing solvent screening, cyclic voltammetry, divided cell studies, electrolysis with redox mediators, small molecule model studies, and control experiments. Our findings determine that the reaction proceeds via a heterogeneous electro-mediated acid depolymerization mechanism. The bifunctional role of the co-solvent 1,1,1,3,3,3-hexafluoro-2-propanol (HFIP) is also revealed. This study demonstrates the potential of electromediated depolymerization serving as an important role in sustainable chemistry by merging the concepts of renewable energy and circular plastic economy.
环境中消费后的塑料垃圾促使科学界开发解构方法,以便从这些合成大分子中获得有价值的物质。电催化是在小分子合成中实现具有挑战性转化的成熟方法。在此,我们展示了在环境条件下,聚甲醛(一种高度结晶的工程热塑性塑料,即赛钢®)首次电化学解聚为其可再聚合单体甲醛/1,3,5-三恶烷。我们通过溶剂筛选、循环伏安法、分隔式电解池研究、使用氧化还原介质的电解、小分子模型研究和对照实验来研究这种电化学解构过程。我们的研究结果确定该反应通过非均相电介导酸解聚机制进行。还揭示了共溶剂1,1,1,3,3,3-六氟-2-丙醇(HFIP)的双重功能。本研究通过融合可再生能源和循环塑料经济的概念,证明了电介导解聚在可持续化学中发挥重要作用的潜力。