CHINESE JOURNAL OF ENERGETIC MATERIALS
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一种铁基单原子催化剂的制备与催化性能研究
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中北大学

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国家自然科学基金项目(面上项目,重点项目,重大项目)


Preparation and Catalytic Performance of Iron-based Single-atom Catalysts
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North University of China

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    摘要:

    为探究单原子催化剂对固体推进剂用高能炸药组分的催化效果,采用高温煅烧法制备了一种铁基单原子催化剂(Fe-NC@PC),通过X-射线粉末衍射(XRD)、X-射线光电子能谱仪(XPS)、扫描电镜(SEM)、透射电镜(TEM)、原位球差校正透射电镜(AC-TEM )、X-射线吸收精细结构谱(XAFS)和热重-差示扫描量热法(TG-DSC)研究了Fe-NC@PC的组成、结构、形貌及对催化热分解性能。实验结果表明,Fe-NC@PC中Fe单原子以Fe-N键负载于载体表面,且能有效促进固体推进剂含能组分的热分解。在Fe-NC@PC添加量为5%且催化剂中Fe单原子负载量仅为0.98%(有效成分含量约0.05%)的情况下,4种代表性推进剂用高能组分如1,1-二氨基-2,2-二硝基乙烯(FOX-7)、奥克托今(HMX)、六硝基六氮杂异伍兹烷(CL-20)和1,1"-二羟基-5,5"-联四唑二羟铵盐(TKX-50)的热分解峰温分别提前34.6,9.4,6.3和27.9 ℃,达到了传统催化剂有效成分含量>2%的效果,催化效果极其显著。在此基础上,探究了Fe-NC@PC对上述高能组分热分解特性和相关动力学参数的影响。通过发展Fe基单原子燃速催化剂,拓展了固体推进剂用燃烧催化剂的范围和催化热解作用的对象,具有较高的学术参考价值和应用价值。

    Abstract:

    To explore the catalysis in energy-containing explosives, an iron-based monoatomic catalyst (Fe-NC@PC) were successfully obtained by high-temperature calcination. The physical phase composition, morphological structure and catalytic thermal decomposition performance were studied by X-ray Powder diffractometer (XRD), X-ray Photoelectron Spectroscopy (XPS), Scanning Electron Microscope (SEM), Transmission Electron Microscope (TEM), Spherical Aberration Corrected Transmission Electron Microscope(ACTEM), X-ray Absorption Fine Structure (XAFS), and Thermogravimetric-differential Scanning Calorimetry (TG-DSC). Results show that Fe atoms were supported on the surface of the carrier by Fe-N bonds, which can effectively promote the thermal decomposition of energetic components of solid propellant. When the addition of Fe-NC@PC is 5% and the single atom loading of Fe in the catalyst is only 0.98% (the content of effective components is about 0.05%), the exothermic decomposition peak temperature of four representative high-energy components for propellants, such as 1,1-diamino-2,2-dinitroethylene (FOX-7), cyclotetramethylenetetranitramine (HMX), hexanitrohexaazaisowurtzane (CL-20) and 5,5’-bistetrazole-1,1’-diolate (TKX-50) were advanced by 34.6℃, 9.4℃, 6.3℃ and 27.9℃ respectively, which achieved the effect that the content of effective components in traditional catalyst was more than 2%, and the catalytic effect was extremely remarkable. Then, the influence of Fe-NC@PC on the thermal decomposition characteristics and kinetic parameters of the above high-energy components was investigated. By developing Fe-based monoatomic burning rate catalyst, the scope of combustion catalyst for solid propellant and the object of catalytic pyrolysis are expanded, which has high academic reference value and application value.

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要雅靖,杜熙凤,张鑫慧,等. 一种铁基单原子催化剂的制备与催化性能研究[J]. 含能材料,DOI:10.11943/CJEM2024248.

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  • 收稿日期: 2024-09-14
  • 最后修改日期: 2025-04-01
  • 录用日期: 2025-04-02
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