Hua Mutian, Peng Zhengxing, Guha Rishabh D, Ruan Xiaoxu, Ng Ka Chon, Demarteau Jeremy, Haber Shira, Fricke Sophia N, Reimer Jeffrey A, Salmeron Miquel B, Persson Kristin A, Wang Cheng, Helms Brett A
Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720 USA.
Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA 94720 USA.
Sci Adv. 2024 Sep 20;10(38):eadq3801. doi: 10.1126/sciadv.adq3801. Epub 2024 Sep 18.
Plastics redesign for circularity has primarily focused on monomer chemistries enabling faster deconstruction rates concomitant with high monomer yields. Yet, during deconstruction, polymer chains interact with their reaction medium, which remains underexplored in polymer reactivity. Here, we show that, when plastics are deconstructed in reaction media that promote swelling, initial rates are accelerated by over sixfold beyond those in small-molecule analogs. This unexpected acceleration is primarily tied to mechanochemical activation of strained polymer chains; however, changes in the activity of water under polymer confinement and bond activation in solvent-separated ion pairs are also important. Together, deconstruction times can be shortened by seven times by codesigning plastics and their deconstruction processes.
为实现循环利用而进行的塑料重新设计主要集中在单体化学上，以实现更快的解构速率并伴随高单体产率。然而，在解构过程中，聚合物链会与其反应介质相互作用，而这在聚合物反应性方面仍未得到充分探索。在这里，我们表明，当塑料在促进溶胀的反应介质中解构时，初始速率比小分子类似物中的速率加快了六倍以上。这种意外的加速主要与应变聚合物链的机械化学活化有关；然而，聚合物受限下水的活性变化以及溶剂分离离子对中的键活化也很重要。综合起来，通过共同设计塑料及其解构过程，解构时间可以缩短七倍。
