Fricke Sophia N, Haber Shira, Hua Mutian, Salgado Mia, Helms Brett A, Reimer Jeffrey A
Department of Chemical and Biomolecular Engineering, University of California, Berkeley, Berkeley, CA 94720, USA.
Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
Sci Adv. 2024 Apr 5;10(14):eadl0568. doi: 10.1126/sciadv.adl0568. Epub 2024 Apr 3.
Moving toward a circular plastics economy is a vital aspect of global resource management. Chemical recycling of plastics ensures that high-value monomers can be recovered from depolymerized plastic waste, thus enabling circular manufacturing. However, to increase chemical recycling throughput in materials recovery facilities, the present understanding of polymer transport, diffusion, swelling, and heterogeneous deconstruction kinetics must be systematized to allow industrial-scale process design, spanning molecular to macroscopic regimes. To develop a framework for designing depolymerization processes, we examined acidolysis of circular polydiketoenamine elastomers. We used magnetic resonance to monitor spatially resolved observables in situ and then evaluated these data with a fractal method that treats nonlinear depolymerization kinetics. This approach delineated the roles played by network architecture and reaction medium on depolymerization outcomes, yielding parameters that facilitate comparisons between bulk processes. These streamlined methods to investigate polymer hydrolysis kinetics portend a general strategy for implementing chemical recycling on an industrial scale.
迈向循环塑料经济是全球资源管理的一个重要方面。塑料的化学回收可确保从解聚的塑料废料中回收高价值单体，从而实现循环制造。然而，为了提高材料回收设施中的化学回收通量，必须对目前关于聚合物传输、扩散、溶胀和非均相解构动力学的理解进行系统化，以实现跨越分子到宏观尺度的工业规模工艺设计。为了开发一种设计解聚工艺的框架，我们研究了环状聚二酮烯胺弹性体的酸解过程。我们使用磁共振原位监测空间分辨的可观测物，然后用一种处理非线性解聚动力学的分形方法评估这些数据。这种方法阐明了网络结构和反应介质在解聚结果中所起的作用，得出了有助于批量工艺之间比较的参数。这些简化的研究聚合物水解动力学的方法预示着一种在工业规模上实施化学回收的通用策略。
