Olefin Metathesis for Effective Polymer Healing via Dynamic Exchange of Strong Carbon-Carbon Double Bonds
Olefin Metathesis for Effective Polymer Healing via Dynamic Exchange of Strong Carbon-Carbon Double Bonds
复制标题
DOI：
10.1021/ja306287s
复制
发表时间：
2012-08-29
影响因子：
15
通讯作者：
Guan, Zhibin
中科院分区：
文献类型：
--
作者：
Lu, Yi-Xuan;Guan, Zhibin
在这篇文章中，我们证明了过渡金属催化的烯烃复分解是一种简单，有效的方法，通过强碳-碳双键的动态交换来修复聚合物。在将极低水平的Grubbs第二代Ru复分解催化剂引入到交联聚丁二烯（PBD）网络中后，该材料在中等压力下的各种条件下有效地自愈合。与此形成鲜明对比的是，具有相同网络拓扑结构和交联密度的无催化剂对照样品显示出最小的愈合。在不同浓度的Ru催化剂、压缩压力和温度下仔细研究了材料的愈合效率。这是第一次证明，本体聚合物可以有效地愈合通过动态共价键形成在低于环境温度。Ru负载的PBD样品不仅与自身愈合良好，而且与没有任何催化剂的对照样品愈合良好。此外，完全不含Ru的PBD网络可以在仅在断裂表面处简单地施加非常少量的Ru催化剂时有效地愈合。这种自修复方法的简单性和有效性使其可能适用于广泛的含烯烃聚合物。
In this article, we demonstrate transition-metal-catalyzed olefin metathesis as a simple, effective method for healing polymers via dynamic exchange of strong carbon-carbon double bonds. Upon introducing a very low level of the Grubbs' second-generation Ru metathesis catalyst into cross-linked polybutadiene (PBD) network, the material self-heals effectively at various conditions under moderate pressures. In sharp contrast, catalyst-free control samples with identical network topology and cross-linking density show minimal healing. The healing efficiency of the materials was carefully investigated under different concentrations of the Ru catalyst, compression pressures, and temperatures. It is demonstrated for the first time that a bulk polymer could effectively heal via dynamic covalent bond formation at sub-ambient temperature. The Ru-loaded PBD samples not only heal well with themselves but also with control samples without any catalyst. Furthermore, a completely Ru-free PBD network can heal effectively upon simply applying a very small amount of Ru catalyst only at the fracture surface. The simplicity and effectiveness of this self-healing approach make it potentially applicable to a wide range of olefin-containing polymers.