Effect of metal-carbonitride layered composites with different Ni/Fe molar ratios on the thermal decomposition and combustion performance of energetic components

IF 5.9 2区工程技术 Q2 ENERGY & FUELS

Combustion and Flame Pub Date : 2026-05-01 Epub Date: 2026-03-09 DOI:10.1016/j.combustflame.2026.114928

Tengyue Song , Yuhuai Shi , Shuhan Guo , Ying Kang , Peijia Li , Yuhao Wu , Xiong Cao

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Abstract

The development of highly efficient catalysts for regulating thermal decomposition and combustion behavior of energetic components is of great significance. This study successfully designed, synthesized and characterized a series of nickel-iron layered double oxide doped graphitic carbon nitride (NFL@CN-X, X = 1, 3, 5) composite combustion catalysts with varying Ni/Fe molar ratios through electrostatic self-assembly followed by thermal treatment. These catalysts exhibit well-developed porous structures and highly active metal centers. The effects of these catalysts on the thermal decomposition behavior of Ammonium perchlorate (AP), Cyclotrimethylene trinitramine (RDX), Cyclotetramethylene tetranitramine (HMX) and Hexanitrohexaazaisowurtzitane (CL-20) were systematically investigated using differential scanning calorimetry (DSC) and thermogravimetric (TG) analyses, and relevant kinetic and thermodynamic parameters were calculated. In addition, the optimal catalyst was employed for ignition experiments, and high-speed camera technology was employed to evaluate their impact on the combustion performance of various energetic composite systems. Furthermore, a potential catalytic mechanism was proposed using HMX as a representative energetic compound, based on thermogravimetric-mass spectrometry (TG-MS) analysis. The DSC and TG results revealed that the incorporation of NFL@CN-X (X = 1, 3, 5) significantly lowered the peak decomposition temperatures (T_p) of AP, RDX, HMX and CL-20 by 73.6∼81.0 °C, 1.3∼2.4 °C, 1.1∼1.5 °C, and 5.1∼7.7 °C, respectively. Correspondingly, the apparent activation energies (E_a) of the energetic composite systems markedly reduced by 113.41∼140.86 kJ·mol⁻¹, 3.44∼29.85 kJ·mol⁻¹, 32.73∼134.58 kJ·mol⁻¹, and 49.77∼66.74 kJ·mol⁻¹ compared with those of the raw samples, respectively. Among these, NFL@CN-5 exhibited the most pronounced catalytic thermal decomposition effect and also significantly enhanced combustion characteristics and energy release efficiency of energetic composite systems. Ignition experiments further demonstrate that energetic systems incorporating NFL@CN-5 exhibit increased flame heights, prolonged combustion durations, and more complete combustion behavior. The NFL@CN series catalysts show great potential as superior alternatives to conventional combustion catalysts.

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不同Ni/Fe摩尔比金属-碳氮层状复合材料对含能组分热分解和燃烧性能的影响

开发高效的催化剂来调节含能组分的热分解和燃烧行为具有重要意义。本研究通过静电自组装和热处理，成功设计、合成并表征了一系列不同Ni/Fe摩尔比的镍铁层状双氧化物掺杂石墨氮化碳（NFL@CN-X, X = 1,3,5）复合燃烧催化剂。这些催化剂具有发育良好的多孔结构和高活性的金属中心。采用差示扫描量热法（DSC）和热重法（TG）研究了这些催化剂对高氯酸铵（AP）、环三亚甲基三硝胺（RDX）、环四亚甲基四硝胺（HMX）和六硝基六氮杂二磺齐坦（CL-20）热分解行为的影响，并计算了相关的动力学和热力学参数。此外，采用最优催化剂进行了点火实验，并采用高速摄像技术评价了其对各种含能复合材料体系燃烧性能的影响。此外，基于热重质谱（TG-MS）分析，提出了以HMX为代表的含能化合物的潜在催化机理。DSC和TG结果表明，NFL@CN-X （X = 1,3,5）的掺入显著降低了AP、RDX、HMX和CL-20的峰值分解温度（Tp），分别降低了73.6 ~ 81.0℃、1.3 ~ 2.4℃、1.1 ~ 1.5℃和5.1 ~ 7.7℃。与原始样品相比，复合体系的表观活化能（Ea）分别显著降低了113.41 ~ 140.86 kJ·mol−1、3.44 ~ 29.85 kJ·mol−1、32.73 ~ 134.58 kJ·mol−1和49.77 ~ 66.74 kJ·mol−1。其中NFL@CN-5表现出最显著的催化热分解效果，也显著提高了含能复合体系的燃烧特性和能量释放效率。点火实验进一步证明，含有NFL@CN-5的高能系统表现出更高的火焰高度，延长的燃烧持续时间和更完全的燃烧行为。NFL@CN系列催化剂作为传统燃烧催化剂的优良替代品显示出巨大的潜力。

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来源期刊

Combustion and Flame 工程技术-工程：化工

CiteScore

9.50

自引率

20.50%

发文量

631

审稿时长

3.8 months

期刊介绍： The mission of the journal is to publish high quality work from experimental, theoretical, and computational investigations on the fundamentals of combustion phenomena and closely allied matters. While submissions in all pertinent areas are welcomed, past and recent focus of the journal has been on: Development and validation of reaction kinetics, reduction of reaction mechanisms and modeling of combustion systems, including: Conventional, alternative and surrogate fuels; Pollutants; Particulate and aerosol formation and abatement; Heterogeneous processes. Experimental, theoretical, and computational studies of laminar and turbulent combustion phenomena, including: Premixed and non-premixed flames; Ignition and extinction phenomena; Flame propagation; Flame structure; Instabilities and swirl; Flame spread; Multi-phase reactants. Advances in diagnostic and computational methods in combustion, including: Measurement and simulation of scalar and vector properties; Novel techniques; State-of-the art applications. Fundamental investigations of combustion technologies and systems, including: Internal combustion engines; Gas turbines; Small- and large-scale stationary combustion and power generation; Catalytic combustion; Combustion synthesis; Combustion under extreme conditions; New concepts.