一种通过表面引发的原子转移自由基聚合构建 MOF@polymer 功能复合材料的通用方法†,Chemical Science

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一种通过表面引发的原子转移自由基聚合构建 MOF@polymer 功能复合材料的通用方法†
Chemical Science ( IF 7.6 ) Pub Date : 2018-12-12 00:00:00 , DOI: 10.1039/c8sc03520b
Sanfeng He ₁ , Hongliang Wang ₁ , Cuizheng Zhang ₁ , Songwei Zhang ₁ , Yi Yu ₁ , Yongjin Lee ₁ , Tao Li ₁

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我们报告了一种通过表面引发的原子转移自由基聚合 (SI-ATRP) 构建 MOF@polymer 功能复合材料的通用方法。与需要将引发基团共价预锚定在基材表面上的传统 SI-ATRP 不同，在我们的方法中，合理设计的无规共聚物 (RCP) 宏观引发剂首先通过链间氢键交联在 MOF 表面上自组装。在交联单体存在下的后续聚合将这些聚合物链共价连接到一个坚固的网络中，将 MOF 颗粒物理地限制在聚合物壳内。我们通过在五种不同金属（Zr、Zn、Co、Al 和 Cr）的 MOF 上生长各种聚合物来完全控制壳厚度，证明了这种方法的普遍性，功能和层顺序，同时仍保留 MOF 的固有孔隙率。此外，只需通过明智的单体选择，即可将 UiO-66 的润湿性从超亲水连续调整为超疏水。我们还证明了 7 nm 聚苯乙烯壳可以有效地屏蔽 UiO-66 粒子免受 1 MH₂ SO₄和 1 M NaOH 在高温下，使其在苛刻的化学环境中具有潜在应用。

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A generalizable method for the construction of MOF@polymer functional composites through surface-initiated atom transfer radical polymerization†

We report a generalizable approach to construct MOF@polymer functional composites through surface-initiated atom transfer radical polymerization (SI-ATRP). Unlike conventional SI-ATRP that requires covalent pre-anchoring of the initiating group on substrate surfaces, in our approach, a rationally designed random copolymer (RCP) macroinitiator first self-assembles on MOF surfaces through inter-chain hydrogen bond crosslinking. Subsequent polymerization in the presence of a crosslinking monomer covalently threads these polymer chains into a robust network, physically confining the MOF particle inside the polymer shell. We demonstrated the universality of this approach by growing various polymers on five MOFs of different metals (Zr, Zn, Co, Al, and Cr) with complete control over shell thickness, functionality and layer sequence while still retaining the inherent porosity of the MOFs. Moreover, the wettability of UiO-66 can be continuously tuned from superhydrophilic to superhydrophobic simply through judicious monomer(s) selection. We also demonstrated that a 7 nm polystyrene shell can effectively shield UiO-66 particles against 1 M H₂SO₄ and 1 M NaOH at elevated temperature, enabling their potential application in demanding chemical environments.

更新日期：2018-12-12

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