Chen Liang, Liu Renjie, Yan Qiang
State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Fudan University, Shanghai, 200433, China.
Angew Chem Int Ed Engl. 2018 Jul 20;57(30):9336-9340. doi: 10.1002/anie.201804034. Epub 2018 Jun 28.
Frustrated Lewis pairs (FLP), a couple comprising a sterically encumbered Lewis acid and Lewis base, can offer latent reactivity for activating inert gas molecules. However, their use as a platform for fabricating gas-responsive materials has not yet developed. Merging the FLP concept with polymers, we report a new generation CO -responsive system, differing from the first-generation ones based on an acid-base equilibrium mechanism. Two complementary Lewis acidic and basic block copolymers, installing bulky borane- and phosphine-containing blocks, were built as the macromolecular FLP. They can bind CO to drive micellar formation, in which CO as a cross-linker bridges the block chains. This dative bonding endows the assembly with ultrafast response (<20 s), thermal reversibility, and excellent reproducibility. Moreover, such micelles bound highly active CO can function as nanocatalysts for recyclable C catalysis, opening a new direction of sustainable CO conversion.
受阻路易斯酸碱对（FLP）由空间位阻较大的路易斯酸和路易斯碱组成，能够为活化惰性气体分子提供潜在反应活性。然而，将其用作制备气体响应材料的平台尚未得到发展。通过将FLP概念与聚合物相结合，我们报道了一种新一代的CO响应体系，它不同于基于酸碱平衡机制的第一代体系。构建了两种互补的路易斯酸性和碱性嵌段共聚物，它们含有庞大的含硼烷和膦的嵌段，作为大分子FLP。它们能够结合CO以驱动胶束形成，其中CO作为交联剂桥接嵌段链。这种配位键赋予组装体超快响应（<20秒）、热可逆性和出色的重现性。此外，这种结合了高活性CO的胶束可作为可循环C催化的纳米催化剂，为可持续的CO转化开辟了新方向。
