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嵌入钯纳米颗粒的金属有机框架衍生的分级多孔碳纳米片作为不同电解质中一氧化碳氧化的高效电催化剂。

Pd-Nanoparticles Embedded Metal-Organic Framework-Derived Hierarchical Porous Carbon Nanosheets as Efficient Electrocatalysts for Carbon Monoxide Oxidation in Different Electrolytes.

作者信息

Ipadeola Adewale K, Eid Kamel, Abdullah Aboubakr M, Ozoemena Kenneth I

机构信息

Center for Advanced Materials, Qatar University, Doha 2713, Qatar.

Gas Processing Center (GPC), College of Engineering, Qatar University, Doha 2713, Qatar.

出版信息

Langmuir. 2022 Sep 13;38(36):11109-11120. doi: 10.1021/acs.langmuir.2c01841. Epub 2022 Aug 30.

DOI:10.1021/acs.langmuir.2c01841
PMID:36040806
Abstract

Rational synthesis of Co-ZIF-67 metal-organic framework (MOF)-derived carbon-supported metal nanoparticles is essential for various energy and environmental applications; however, their catalytic activity toward carbon monoxide (CO) oxidation in various electrolytes is not yet emphasized. Co-ZIF-67-derived hierarchical porous carbon nanosheet-supported Pd nanocrystals (Pd/ZIF-67/C) were prepared using a simple microwave-irradiation approach followed by carbonization and etching. Mechanistically, during microwave irradiation, triethyleneamine provides abundant reducing gases that promote the formation of Pd nanoparticles/Co-N in porous carbon nanosheets with the assistance of ethylene glycol and also form a multimodal pore size. The electrocatalytic CO oxidation activity and stability of Pd/ZIF-67/C outperformed those of commercial Pd/C and Pt/C catalysts by (4.2 and 4.4, 4.0 and 2.7, 3.59 and 2.7) times in 0.1 M HClO, 0.1 M KOH, and 0.1 M NaHCO, respectively, due to the catalytic properties of Pd besides the conductivity of Co-N active sites and delicate porous structures of ZIF-67. Notably, using Pd/ZIF-67/C results in a higher CO oxidation activity than Pd/C and Pt/C. This study may pave the way for using MOF-supported multi-metallic nanoparticles for CO oxidation electrocatalysis.

摘要

合理合成钴基金属有机框架(MOF)衍生的碳负载金属纳米颗粒对于各种能源和环境应用至关重要;然而,它们在各种电解质中对一氧化碳(CO)氧化的催化活性尚未得到强调。采用简单的微波辐射方法,随后进行碳化和蚀刻,制备了钴基金属有机框架衍生的分级多孔碳纳米片负载的钯纳米晶体(Pd/ZIF-67/C)。从机理上讲,在微波辐射过程中,三乙胺提供了丰富的还原气体,在乙二醇的辅助下促进了多孔碳纳米片中钯纳米颗粒/Co-N的形成,并且还形成了多峰孔径。由于除了Co-N活性位点的导电性和ZIF-67精细的多孔结构外,Pd还具有催化性能,因此在0.1 M HClO、0.1 M KOH和0.1 M NaHCO中,Pd/ZIF-67/C的电催化CO氧化活性和稳定性分别比商业Pd/C和Pt/C催化剂高出(4.2和4.4、4.0和2.7、3.59和2.7)倍。值得注意的是,使用Pd/ZIF-67/C比Pd/C和Pt/C具有更高的CO氧化活性。这项研究可能为使用MOF负载的多金属纳米颗粒进行CO氧化电催化铺平道路。

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