Recently developed elastomers with an adaptable covalent network, e.g., elastic vitrimers, have great potential as sustainable materials, although most of them suffer from limited recyclability and unsatisfied mechanical properties. Here, we report a polydimethylsiloxane (PDMS)-based recyclable elastic network, combining permanent chemical and high-density dynamic physical crosslinks utilizing side-chain reactions, which provides energy dissipation for superb toughness and enables efficient chain rearrangement for excellent recyclability. The optimal elastic network achieves an unprecedented recyclability of 70 cycles, one order of magnitude higher than existing elastic vitrimers, extraordinary toughness of 66 MJ/m³, significantly higher than previously reported PDMS elastomers, excellent chemical resistance, and vitrimer-like rheological behavior. Physical analysis is also performed to provide the accurate estimation of bond-exchange dynamics excluding the often-neglected chain dynamics and to offer insight into the superb performance. We anticipate that such a design principle enables an alternative approach for developing superior recyclable polymer networks.

Recently developed elastomers with an adaptable covalent network, e.g., elastic vitrimers, have great potential as sustainable materials, although most of them suffer from limited recyclability and unsatisfied mechanical properties. Here, we report a polydimethylsiloxane (PDMS)-based recyclable elastic network, combining permanent chemical and high-density dynamic physical crosslinks utilizing side-chain reactions, which provides energy dissipation for superb toughness and enables efficient chain rearrangement for excellent recyclability. The optimal elastic network achieves an unprecedented recyclability of 70 cycles, one order of magnitude higher than existing elastic vitrimers, extraordinary toughness of 66 MJ/m³，显着高于先前报道的 PDMS 弹性体，具有优异的耐化学性和类似 vitrimer 的流变行为。还进行物理分析，以提供键交换动态的准确估计，排除经常被忽视的链动态，并提供对卓越性能的洞察。我们预计这样的设计原则可以为开发优质的可回收聚合物网络提供一种替代方法。