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Catalytically-active porous assembly with dynamic pulsating motion for efficient exchange of products and reagents
Communications Chemistry ( IF 5.9 ) Pub Date : 2020-01-24 , DOI: 10.1038/s42004-020-0259-4
Shanshan Wu 1 , Liping Huang 1 , Yu Hou 1 , Xin Liu 2 , Jehan Kim 3 , Yongri Liang 4 , Jiong Zhao 5 , Liwei Zhang 1 , Hongbing Ji 1 , Myongsoo Lee 2 , Zhegang Huang 1
Affiliation  

Despite recent advances in the use of porous materials as efficient heterogeneous catalysts which operate through effectively trapping reagents in a well-defined space, continuously uptaking reagents to substitute products in the cavity for efficient product turnover still remains challenging. Here, a porous catalyst is endowed with ‘breathing’ characteristics by thermal stimulus, which can enable the efficient exchange of reagents and products through reversible stacking from inflated aromatic hexamers to contracted trimeric macrocycles. The contracted super-hydrophobic tubular interior with pyridine environment exhibits catalytic activity towards a nucleophilic aromatic substitution reaction by promoting interactions between concentrated reagents and active sites. Subsequent expansion facilitates the exchange of products and reagents, which ensures the next reaction. The strategy of mesoporous modification with inflatable transition may provide a new insight for construction of dynamic catalysts.



中文翻译:


具有动态脉动运动的催化活性多孔组件,可有效交换产品和试剂



尽管最近在使用多孔材料作为高效多相催化剂方面取得了进展,通过在明确的空间中有效地捕获试剂来发挥作用,但持续吸收试剂来替代腔中的产品以实现有效的产品周转仍然具有挑战性。在这里,多孔催化剂通过热刺激被赋予了“呼吸”特性,可以通过从膨胀的芳香六聚体到收缩的三聚大环的可逆堆积,实现试剂和产物的有效交换。具有吡啶环境的收缩的超疏水管状内部通过促进浓试剂和活性位点之间的相互作用而表现出对亲核芳香族取代反应的催化活性。后续的扩增有利于产物和试剂的交换,保证了下一步反应的进行。充气转变的介孔修饰策略可能为动态催化剂的构建提供新的见解。

更新日期:2020-01-24
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