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环化聚丙烯腈作为具有协同活性位点的单原子金属催化剂的一种有前景的载体

Cyclized Polyacrylonitrile as a Promising Support for Single Atom Metal Catalyst with Synergistic Active Site.

作者信息

Liu Lulu, Duan Yandong, Liang Yu, Kan Amin, Wang Lin, Luo Qingzhi, Zhang Yaqiang, Zhang Bingkai, Li Zhen, Liu Jing, Wang Desong

机构信息

Hebei Key Laboratory of Photoelectric Control on Surface and Interface, School of Sciences, Hebei University of Science and Technology, Shijiazhuang, 050018, P. R. China.

School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou, 510006, P. R. China.

出版信息

Small. 2022 Feb;18(8):e2104142. doi: 10.1002/smll.202104142. Epub 2021 Dec 8.

Abstract

Metal single atom catalysts (SAC) have been successfully used in heterogeneous catalysis but developing a scalable and economic support for SAC is still a great challenge. Here, cyclized polyacrylonitrile (CPAN) is proposed as a promising support for single atom metal catalysts. CPAN can be easily prepared from cheap industrial product polyacrylonitrile (PAN), which has excellent processability. A series of SAC on CPAN (M/CPAN, M = Ag, Cu, Ru) are designed and the catalytic activities of the as synthesized M/CPAN are investigated by the model reduction reaction of p-nitrophenol (4-NP). M/CPAN presents excellent catalytic performance with high stability and theoretical calculations elucidate that Ag/CPAN synergistically catalyze 4-NP reduction following the Langmuir-Hinshelwood (L-H) mechanism with 4-NP preferentially adsorbing at the Ag sites and H adsorbing at the bridge C sites. These results, for the first time, reveal that the single atom on CPAN can catalyze 4-NP reduction efficiently. This methodology provides a convenient route for the preparation of a variety of SAC, and this strategy is readily scalable and holds great potential in catalytic applications.

摘要

金属单原子催化剂(SAC)已成功应用于多相催化,但开发一种可扩展且经济的SAC载体仍然是一个巨大的挑战。在此,环化聚丙烯腈(CPAN)被提议作为单原子金属催化剂的一种有前景的载体。CPAN可以很容易地由廉价的工业产品聚丙烯腈(PAN)制备而成,PAN具有优异的加工性能。设计了一系列负载于CPAN上的SAC(M/CPAN,M = Ag、Cu、Ru),并通过对硝基苯酚(4-NP)的模型还原反应研究了所合成的M/CPAN的催化活性。M/CPAN表现出优异的催化性能和高稳定性,理论计算表明,Ag/CPAN按照朗缪尔-欣谢尔伍德(L-H)机理协同催化4-NP还原,4-NP优先吸附在Ag位点,H吸附在桥连C位点。这些结果首次揭示了CPAN上的单原子能够高效催化4-NP还原。该方法为制备各种SAC提供了一条便捷途径,并且这种策略易于扩展,在催化应用中具有巨大潜力。

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