Pyrene-Containing Polymer-Supported Cu/TEMPO Catalytic Systems: Aromatic Stacking-Enhanced Cooperative Catalysis

Pyrene-Containing Polymer-Supported Cu/TEMPO Catalytic Systems: Aromatic Stacking-Enhanced Cooperative Catalysis
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含芘聚合物负载的 Cu/TEMPO 催化体系:芳烃堆积增强协同催化

DOI:
10.1021/acs.jpcc.1c09972
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发表时间:
2021-12
期刊:
The Journal of Physical Chemistry C
影响因子:
--
通讯作者:
Zushun Xu
Zushun Xu
中科院分区:
其他
文献类型:
--
作者:
Tianyou Chen;Wei Xiao;Zihao Wang;Pengfei Gan;Changfeng Yi;Zushun Xu

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非共价键固载分子物种在聚合物载体上是一种独特的方法,工程多功能合作催化剂。在这里,我们设计了一个模块化的策略,通过使用疏水相互作用和芳香堆积相互作用的聚合物支撑的Cu/2,2,6,6-四甲基-1-哌啶-N-氧基(克里思)催化体系的建设。采用纳米沉淀法制备的聚合物负载Cu/克里思催化剂对苯甲醇的有氧氧化反应表现出优异的催化活性,催化活性可通过芳香基团的类型、有效组分比和聚合物组成进行调节。我们发现,强的芳香堆积相互作用和使用含芘的聚合物是至关重要的,以提高协同性。这种模块化的策略是有前途的多功能合作催化剂的固定化具有优异的催化活性,并具有潜在的工程其他非均相多功能催化剂。
Noncovalent immobilization of discrete molecular species on polymer supports is a unique approach to engineer multifunctional cooperative catalysts. Here we devise a modular strategy for the construction of polymer-supported Cu/2,2,6,6-tetramethyl-1-piperidine-N-oxyl (TEMPO) catalytic systems by using hydrophobic interactions and aromatic stacking interactions. Polymer-supported Cu/TEMPO catalysts prepared by nanoprecipitation exhibit excellent catalytic activities for aerobic oxidation of benzyl alcohol, which can be tailored by the type of aromatic moieties, effective constituent ratios, and polymer compositions. We found that strong aromatic stacking interactions and the use of pyrene-containing polymers are crucial to enhance cooperativity. This modular strategy is promising for the immobilization of multifunctional cooperative catalysts with excellent catalytic activities and has potential for the engineering of other heterogeneous multifunctional catalysts.
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