Ordered Assembly of Fluorinated Graphene with Nano Fuels for Coupling Reaction and Application in Microenergetic Devices

Ordered Assembly of Fluorinated Graphene with Nano Fuels for Coupling Reaction and Application in Microenergetic Devices | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Research Article Ordered Assembly of Fluorinated Graphene with Nano Fuels for Coupling Reaction and Application in Microenergetic Devices Jun Wang, Li Ren, Xinquan Zhang, Yao-feng Mao, Haifu Wang This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-6869022/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 24 Apr, 2026 Read the published version in Advanced Composites and Hybrid Materials → Version 1 posted 10 You are reading this latest preprint version Abstract High toughness, superior reactivity with high energy and pressure output at micro-size are the basic requirements for energy materials applied in microenergetic devices such as micro-thruster, micro-ignitor and micro-power sources. Herein, fluorinated graphene as multifunctional additive is employed to ordered assembly flexible Al-FG/B-FG film based on “brick & mortar” structured concept prepared by vacuum self-assembly. Graphene fluoride (FG), as the “brick”, integrates with fluorine rubber loading Al (aluminum) or B (boron) nanoparticles as two types "mortar" that are stacked alternately to assembly ordered structure and obtain strong toughness. The layered ordered Al-FG/B-FG could efficiently combine the high reaction kinetics of Al-FG and the ultra-high calorific value of B-FG to realize coupling reaction and achieve superior self-sustaining combustion at micro-size, release high-energy and pressure. Subsequently, Al-FG/B-FG film has been integrated in micro-ignitor and self-destructive devices to achieve ignition and damage functions. More importantly, Al-FG/B-FG film still maintains stable energy output characteristics in harsh environments and could achieve damage effects in only 20 microseconds applied in self-destructive devices. This work establishes an innovative configuration to design novel energy materials and apply in micro-devices. Al-FG/B-FG interfacial structure self-sustaining combustion pressure microenergetic device Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 1. introduction Microenergetic devices integrated with energy materials from nano- to micrometers could achieve specific functions through precise control of reaction and energy release. Micro-thruster, micro-ignitor, micro-detonators, micro-power sources, minimally invasive surgical instruments (such as intravascular blasting), precision machining (micro explosive drilling) and self-destruction have been widespread concern and great potential in aerospace, medical and industrial fields [ 1 – 5 ] . Energy materials as the key component integrated in micro-devices are required to have two basic characteristics [ 6 – 8 ] . One is excellent mechanical properties, especially high toughness to integrate on the microchip [ 9 ] . More importantly, superior reactivity with high energy and pressure output at micro-size to realize specially function [ 10 ] . However, traditional energetic materials such as explosive and thermite could not able to meet the integration and functional requirements. They are generally powder and almost brittle. Moreover, it is hard to self-sustaining combustion and release high energy and pressure at micro-size [ 11 – 13 ] . For applications and future microenergetic devices remains an elusive goal because of the lack of versatile energy materials. Lots of effort have been devoted to design and prepare versatile energy materials for microenergetic devices. At present, the construction of energetic film is the main strategy to satisfy the requirements of easy integration and high energy output [ 14 – 16 ] . Assembling the typical metal oxides (such as CuO, Bi 2 O 3 , Fe 2 O 3 ) and Al fuel could realize the ignition function [ 17 – 19 ] . However, such film is still brittle and easy to fall off from the substrate after integration resulted from brittleness of metal oxides and poor interface interaction. Additionally, the energy density and pressure are extremely hard to meet the ignition and damage requirements at micro-size. To increase energy, reaction of Al and fluorine resulted from the higher reaction heat than that of oxidation reaction become hot topic in the field of energy materials and applied in microenergetic devices [ 20 ] . A novel superlattice PTFE/Al has been designed to integrate the micro-ignitor that achieved the ignition function [ 9 ] . However, PTFE/Al has insufficient pressure output resulted from solid reaction products applied in self-destruction and airbag. It is worth to note that superlattice PTFE/Al has high mechanical properties to integrate micro-devices resulted from PTFE and laminated structure. Based on above research, to further increase energy and pressure output, boron (B) as typical high-energy fuel, may be an excellent candidate [ 21 – 23 ] because of reaction calorific value is 2 times that of Al powder. The calorific values of Al-O (oxygen) reaction and Al-F (fluorine) reaction are 31 kJ/g and 56 kJ/g, while the calorific values of B-O reaction and B-F reaction have 58 kJ/g and 105 kJ/g [ 24 – 26 ] . More importantly, the product is gaseous BF 3 , which is a unique advantage for obtaining high pressure [ 27 , 28 ] . Unfortunately, low ignition and combustion reaction is big obstacle for B because of the surface oxide layer (B 2 O 3 ) with a low melting point (450°C) and a high boiling point (1860°C) [ 29 – 31 ] . Draw support from the high combustion reaction kinetics of Al, the B-F reaction induced by the Al-F reaction and then achieving the Al-F-B coupling effect may be a potential strategy [ 32 ] . Moreover, the high calorific value and gaseous products from the B-F reaction are expected to further promote the Al-F reaction, making it possible to obtain self-sustaining combustion with high energy and pressure output at micro-size [ 33 ] . Since the Al and B reactions are both solid phase reactions, it becomes daunting challenge how to assembly structure that could maintain the high toughness for integration while has high combustion reaction to release energy and pressure. Firstly, it is necessary to construct the orderly distribution and super-large interface for the heat transfer and mass diffusion [ 34 ] to support the continuous coupling reaction between Al-F and B-F. More importantly, assembly structure can ensure a strong interaction among fluorine, Al and B to obtain excellent mechanical properties and toughness. Inspired by coupling reaction and layered ordered structure [ 32 , 35 ] greatly expanded interface for the solid phase reaction and excellent mechanical properties, it is natural to consider using B and Al as fuel and fluorine as oxidizer ordered stacked to form specially structure. To fulfill the above demands, graphene fluoride (FG) is selected as the fluorine source [ 36 – 38 ] because two-dimensional planar could realize the orderly arrangement of Al and B on the molecular scale to promote the coupling reaction. Moreover, this two-dimensional structure is easy to assembly the layered ordered structure. Based on concept from “brick & mortar” structure [ 39 , 40 ] , FG as the “brick” could ensures ordered structure and high mechanical properties [ 41 , 42 ] . Fluorine rubber loading the Al or B is introduced as the “mortar” to further enhance the film toughness while providing more fuel sources to promote the combustion reaction with high energy and pressure. Consequently, layered ordered Al-FG/B-FG film has been successfully prepared through vacuum self-assembly (Fig. 1 ), which exhibits excellent mechanical toughness and can satisfy the integrated application on the microenergetic devices. Additionally, Al-FG/B-FG could achieve coupling reaction to produce high energy and pressure output. The self-sustaining combustion reaction, energy and pressure output performance are systematically studied to provide the theoretical basis and data support for the application. Finally, Al-FG/B-FG has been integrated in microenergetic devices to achieve ignition and self-destruction function. 2. Methods 2.1 Design and Fabrication Al-FG/B-FG First, two samples of 0.05 g FG are added to beakers containing 10 mL of NMP solution, respectively, and perform ultrasonic dispersion until there is no obvious precipitation to obtain FG dispersion. Then, 0.075g Al and 0.5 g fluorine rubber (FR) solution (5 wt.%) are added to FG dispersion, ultrasonic dispersion for 2 h, magnetic stirring for 30 min, to form a suspension of the Al-FG system. Similarly, 0.025g B and 0.5 g fluorine rubber (FR) solution (5 wt.%) are added to FG dispersion, ultrasonic dispersion for 2 h, magnetic stirring for 30 min, to form a suspension of the B-FG system. The Al-FG/B-FG film with layered stacking structure is then prepared by vacuum self-assembly. Taking the M4 film as an example, the suspensions of the Al-FG and B-FG are divided into two parts of equal quality. Use a glue head dropper to add the suspension of the Al-FG system to the vacuum-activated membrane within 1 min, until all the solvent is removed, so that Al, FG and FR are self-assembled to form the first layer of Al-FG. Subsequently, the suspension of the B-FG system is added to the Al-FG layer that has no solvent, and wait for the solvent to be completely removed to form a second layer of B-FG. Repeat the above steps to consume all prepared suspensions to form the energetic film with Al-FG/B-FG layered structure. Finally, the Al-FG/B-FG layered ordered film is dried in an oven at 40 ℃ for 12 h, and peeled off from the membrane to obtain the M4 film. 2.2 Morphology and Structure Characterization The morphology and crystal structure of the Al-FG/B-FG film is characterized by field emission scanning electron microscope (FE-SEM, ULTRA 55, ZEISS, Germany) and powder X-ray diffraction (XRD, X’Pert PRO) with a monochromatized Cu Kα radiation (λ = 1.5418Å). Surface elemental analysis of the bionic films is characterized by energy dispersive X-ray spectroscopy (EDS). 2.3 Thermal and combustion testing The thermal properties of the Al-FG/B-FG film are measured by the simultaneous thermal analyzer (TG-DSC, STA449F5, NETZSCH, Germany) from 50 to 900 ℃ under a heating rate of 10 ℃/min at N 2 atmosphere. Meanwhile, time-resolved mass spectrometry (MS) (PFEIFFER, 2 OMNI star, Germany) for on-line analysis of the fugitive gaseous products are collected via a series data collection scheme. Materials burning experiments are to test the reaction kinetics of Al-FG/B-FG film, including the maximum flame area and burning rate. The splines used in the combustion experiment have the lengths of 35 mm and widths of 4, 5 and 6 mm, respectively. A nickel-chromium wire with a diameter of 0.2 mm is used to heat one end of the spline, and then a high-speed camera (UX50, Photron FASTCAM, Japan) with 2000 fps records the entire process of flame propagation. Materials pressure experiments are to test the dynamic pressure curve in a closed chamber when the energetic sample undergoes combustion or explosion reaction. The experimental tests are carried out in a variety of atmospheres (1 atm N 2 , Air, and O 2 , respectively) using small block of Al-FG/B-FG film. Typically, 100 mg sample is placed in the confined cell with a fixed volume of 330 mL and ignited by a nichrome wire (0.2 mm in diameter, 40 mm in length). And, the dynamic pressure during the reaction process is measured by a pressure sensor (PC290, 1 kHz) attached to the confined cell and the pressure signal is converted into a voltage signal by software, and then recorded in a computer. 2.3 Self-destruction devices Excellent transient damage ability is a prerequisite for device damage application. Therefore, the transient damage performance of Al-FG/B-FG film is tested, as shown in Fig. 7 a. The Al-FG/B-FG film with a specification of 12 mm×12 mm (10 mg) was integrated on the CD through a glass substrate. A nickel-chromium wire with a diameter of 0.2 mm is used to ignite the films smoothly. The high-speed camera (X213, Qianyanlang, China) sets the frame rate to 2000 fps to capture and record the entire process of ignition and destruction of the silicon wafer by the film. 3. Results and discussions 3.1 Morphology and composition of Al-FG/B-FG To assembly layered ordered structure of Al-FG/B-FG, Al and B nano-particles are deposited on FG to form Al-FG and B-FG layers, respectively. Two-dimensional FG provides sufficient strength as a skeleton and “mortar” to impart high toughness by creating the strong adhesion between Al (or B) and FG. They are stacked alternately to assembly Al-FG/B-FG structure, which not only achieves the orderly arrangement of Al and B at the molecular level, but also fully possesses the integrated function on the microdevices. Additionally, the supporting effect of fluorine rubber and the FG skeleton endows Al-FG/B-FG with good flexibility. A circular sheet with radius of ~ 35 mm and thickness of ~ 70 µm has well uniformity and mechanical toughness that can be rolled into a cylinder with diameter of only 6 mm (Fig. 2 a). The layered ordered structure of Al-FG/B-FG consisted of Al-FG (Fig. 2 b 1 ) and B-FG layer (Fig. 2 b 2 ) is observed from SEM images (Fig. 2 b). To more clearly display the “brick & mortar” structure of Al-FG/B-FG, the element mapping of the cross section is further characterized EDS. A layered-like texture can be observed in Fig. 2 c intuitively shows the staggered arrangement of Al and B elements, further indicating that the Al-FG/B-FG stacking structure. The F elements from FG and FR are evenly distributed over the entire cross-section, providing a significant support effect for the film and the adequate fluorine source during the reaction. The layered stacking structures are also observed in Al-FG/B-FG with different layers (Fig. S1 ). The compositions of Al-FG/B-FG was further characterized via XRD and XPS spectra exhibits the presence of Al and FG, which indicates that the prepared sample have high stability during long-term storage (Fig. 2 d and S2). No peak of B be detected in XRD due to its semi-crystalline nature. Besides, the TEM image of the Al-FG/B-FG indicates that the Al and FG layers are interspersed with each other, and a small amount of irregular B nanoparticles are randomly distributed on the FG layer (Fig. 2 e). The element distribution mapping also supports this result. Because the B element is relatively light, it cannot show the element distribution state well. Based on above the results, it can be confirmed that the Al-FG/B-FG with layered stacking structure has been successfully prepared through vacuum self-assembly. Layered stacking structure of Al-FG/B-FG would offer super-large interface for mass diffusion and heat transfer, and exhibits intuitive high flexibility free-standing for integration in microenergetic devices. 3.2 Combustion reaction behavior of Al-FG/B-FG Combustion reaction and energy output of Al-FG/B-FG is key to apply in microenergetic devices. The thermal reaction of Al-FG/B-FG films with different layers was studied on TG-DSC under the heating rate of 10 ℃/min to evaluate the energy output. Two stages of mass loss from 300 to 560 ℃ have been observed in TG curves (Fig. 3 a). The decomposition of fluorine rubber and FG causes the appearance of the first declining region. The mass loss in the second stage is due to the reaction of B and FG to produce gaseous BF 3 , however, since the Al-F reaction produces solid AlF 3 , the decline rate is slightly slowed down. The largest mass loss is observed for M4 indicating that the B-F reaction is the most complete due to appropriate ratio among FG, Al and B. For all samples, a mass increasing is observed resulted from Al reacted with N 2 to form the solid product Al 4 N 3 . The reaction temperature and energy output of Al-FG/B-FG with different layers are obtained from DSC curves. The exothermic values are 1001.23 J/g, 1236.32 J/g, 1393.45 J/g, 1162.25 J/g, and 1116.74 J/g (Fig. 3 b) occurred the coupling reaction between B-F and Al-F reaction [ 32 , 43 ] . The highest value is obtained in M4 film that reaches up to 1.4 times higher than that of M0 film (Al/FG mixtures). The high energy output further illustrates that alternating stacking of Al-FG and B-FG layers could increase interface for the mass diffusion and heat transfer, and realize the chain reaction of Al-F and B-F. The real-time mass spectrometry analysis is carried out to explore the intermediates of FG decomposition and reaction processes of Al-FG/B-FG. The m/z values of 19, 31, 50 and 69 are obtained and assigned to F, CF, CF 2 and CF 3 radials, respectively (Fig. S4). Figure 3 c-d show F and CF radical peaks from FG and fluorine rubber at different temperature. Compared to Al-F and B-F, high content of F and CF radials are observed for layered ordered Al-FG/B-FG further illustrate coupling effect between Al-F and B-F, thereby generating a large number of F and CF radicals resulted in significantly increased reaction heat. The self-sustain combustion of Al-FG/B-FG at micro-size is the basic requirements for their application in microenergetic devices to achieve ignition and damage function. The combustion behavior is influenced on chemical reaction and physical process. Therefore, the effect of typical factors (mass ratios, layer number and size) of Al-FG/B-FG on the combustion reaction and flame propagation characteristics are systematically studied for the applications. Figure 4 a gives the schematic diagram of combustion test. The prepared Al-FG/B-FG are cut into splines with length of 35 mm and width of 4 mm, 5 mm, and 6 mm, respectively. The film spline is adhered to the test platform, and the nickel-chromium wire was employed to ignite at the one end, flame propagation was recorded through high-speed camera. Figure 4 b shows the combustion speed of Al-FG/B-FG with different Al/B mass ratios ranging from 1:3 to 4:0, the combustion and flame propagation speed increases from 122.81 to 259.26 mm/s. Notably, B-FG film without Al (0:4) cannot be ignited and sufficient Al particles must be added into Al-FG/B-FG. The highest combustion speed is obtained for Al-FG/B-FG with Al/B mass ratio of 3:1. Figure 4 c and 4 d shows the maximum combustion flame image and flame area of Al-FG/B-FG films with layers of 1, 2, 4, 6 and widths of 4, 5 and 6 mm. The plenty of gaseous products in the intense combustion reaction leads to the diversity of the combustion flame shape. For Al-FG/B-FG, as the layer number from 1 to 6 increases, the maximum flame area increases. The Al-FG/B-FG with two layers (M2) has a relatively small flame area resulted from only one contact interface between the Al-FG and B-FG components. The Al-FG/B-FG with four layers (M4) has largest flame area resulted from layered ordered structure for mass diffusion and heat transfer, and coupling reaction between Al-F and B-F. In addition, the combustion flame area also increases with the increase of the spline width of 4, 5 and 6 mm, respectively. Figure 4 e and S5 shows the flame propagation process of the Al-FG/B-FG spline with 4 layers and widths of 4, 5 and 6 mm. The results show that the Al-FG/B-FG spline burns with a wider flame area and faster propagation rate. As the number of layer increases, the flame propagation speed increases (Fig. 4 f). The reaction interface increases with the layers increase under the same size, enhancing the mass diffusion and heat transfer process, thereby increases the combustion speed. Additionally, Al-FG/B-FG with appropriate layers would promote coupling reaction between Al-F and B-F. Therefore, the combustion reaction increases firstly and then decreases with the layer increase and the highest speed is obtained for Al-FG/B-FG with four layers (M4). Considering the complexity in the practical applications for microenergetic devices, the pressure output as an important property, especially for thruster and destruction. Therefore, pressure of Al-FG/B-FG under different atmospheres was further studied to verify its excellent environmental adaptability. Figure 5 a gives the pressure-time curves of Al-FG/B-FG with 4 layers (M4) show high-pressure output (~ 200 kPa) even in an oxygen-free environment. This proves that Al-FG/B-FG has stable ability to react and release energy and pressure in harsh environments, which is benefit for practical applications in aerospace and deep sea. In oxygen atmosphere, the much higher-pressure output is obtained because of carbon derived from FG reacted with oxygen to form CO 2 . Al-FG/B-FG with different layers also exhibit excellent pressure output performance in N 2 atmospheres (Fig. 5 b). The maximum pressure value and the average pressurization rate of Al-FG/B-FG with different layers under different atmospheres (Fig. 5 c and d) are basically same resulted from the total thickness and the total amount of reactants are same. Therefore, the gaseous product of the combustion is mainly BF 3 . A significant difference is higher pressure and pressurization rate are observed in oxygen due to oxidation reaction of carbon derived from FG to produce CO 2 . Al-FG/B-FG with 6 layers have high pressure value may be a complete oxidation reaction carbon. The high and fast pressure output is benefit for the practical applications. The above experimental results clearly confirm Al-FG/B-FG with “brick & mortar” structure that has excellent mechanical properties and combustion performance. The self-sustain combustion reaction with high energy and pressure output at micro-size has been successfully realized. The self-sustain combustion reaction, high energy and pressure output at micro-size are attributed to three main aspects. Firstly, coupling effect of high reaction kinetics of Al-FG and high reaction heat of B-FG. Secondly, layered ordered structure of Al-FG/B-FG provides super-large interface for mass diffusion and heat transfer to enhance combustion reaction. Additionally, gaseous products of BF 3 would be benefit to mass diffusion and heat transfer, and pressure output. Figure 6 shows the coupling mechanism of Al-FG/B-FG to obtain high combustion reaction and pressure output. Al would react with F and CF radials from FG decomposition [ 44 , 45 ] to release energy, which could transmit to stimulate reaction of B-FG layer due to large interface. High energy and gaseous BF 3 from the reaction of B-FG will further promote the reaction Al-FG, thereby realizing the coupling effect of Al-FG and B-FG reaction during combustion process. Al-FG/B-FG with “brick & mortar” structure offers a platform to obtain superior combustion reaction at micro-size and release high energy and pressure for the applications in microenergetic devices. 3.3 Applications of Al-FG/B-FG in microenergetic devices Stable combustion reaction, energy and pressure output performance at microscale is key for the applications, such as micro-thruster, micro-ignitor and micro-power sources. Information as cornerstone of rapid development of society has played the more important role. The vigorous development of big data and artificial intelligence has greatly challenged information security, and the consequences are always devastating [ 46 , 47 ] . Self-destruction devices, as the last defender to protect information security, have played a decisive role in maintaining national, social and technological security [ 48 ] . Therefore, designing high-performance energy materials and developing self-destructive devices is of great significance for preventing the information leakage and maintaining national stability. Herein, to verify application of the Al-FG/B-FG in self-destruction device on the information storage medium, it is integrated on the microchip to test the deflagration damage process. Figure 7 a and Fig. S6 shows a schematic of experimental apparatus for transience destruction performance test, and the deflagration process images are given in Fig. 7 b. Based on experimental results, silicon wafer crack or split due to high pressure and heat from Al-FG/B-FG reaction. Figure 7 c shows that the CD has been damaged and lost the function of storing information. Moreover, the amount of Al-FG/B-FG is only 10 mg, which is benefit to integrate nano-energetic devices. This experiment confirms that the Al-FG/B-FG has high-performance energy output while ensuring the flexibility and integrated function, which can achieve damage to the microchip at micro-size. The above results fully confirm the rationality of the “brick & mortar” strategy and the layered stacking structure. In order to further illustrate the applications of Al-FG/B-FG in microenergetic devices, an ignitor has been integrated that could realize ignition function (Fig. S7). The results further reveal that Al-FG/B-FG has excellent combustion reaction and energetic performance that can be applied to integrate kinds of devices such as micro-thruster, micro-ignitor and micro-power sources. Conclusion To develop high-performance energy materials and applied in microenergetic devices, layered ordered Al-FG/B-FG has been designed based the concept of “brick & mortar” structure and successfully prepared by vacuum self-assembly. Under the coupling effect of the “brick” FG and the “mortar” fluorine rubber loaded with Al or B atoms, Al-FG/B-FG has strong mechanical toughness to integrate in micro-devices. Self-sustaining combustion reaction, high energy and pressure output has been obtained resulted from coupling effect between Al-FG and B-FG reaction through “brick & mortar” structure. Al-FG/B-FG has been integrated in self-destruction devices and micro-ignitor. Silicon wafer and CD damaged to crack and loss of function only 20 microseconds. Furthermore, micro-ignitor with Al-FG/B-FG can realize ignition, which further prove Al-FG/B-FG with high combustion reaction and energetic performance that could be applied to integrate kinds of micro-energetic devices. Declarations The authors declare no competing financial interest. Funding This work receives financial support from the National Natural Science Foundation of China (T2222027). 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Prog Energy Combust Sci 93:101038. https://doi.org/10.1016/j.pecs.2022.101038 Qin Y, Yu H, Wang D, Song Y (2023) Preparation and characterization of energetic composite films with mutual reactions based on B-PVDF mosaic structure. Chem Eng J 451:138792. https://doi.org/10.1016/j.cej.2022.138792 Zhou W, Yetter RA, Dryer FL, Rabitz H, Brown RC, Kolb CE (1998) Effect of fluorine on the combustion of clean surface boron particles. Combust Flame 112:507–521. https://doi.org/10.1016/S0010-2180(97)00129-6 Yan L, Zhu B, Chen J, Sun Y (2023) Study on nano-boron particles modified by PVDF to enhance the combustion characteristics. Combust Flame 248:112556. https://doi.org/10.1016/j.combustflame.2022.112556 Young G, Stoltz CA, Mayo DH, Roberts CW, Milby CL (2013) Combustion behavior of solid fuels based on PTFE-boron mixtures. 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Adv Mater 29:1603169. https://doi.org/10.1002/adma.201603169 Yang H, Qiao Z, Wang W, Tan P (2023) Self-destructive microchip: support-free energetic film of BiOBr/Al/Bi2O3 nanothermites and its destructive performance. Chem Eng J 459:141506. https://doi.org/10.1016/j.cej.2023.141506 Additional Declarations No competing interests reported. Supplementary Files SupportingInformation.docx Cite Share Download PDF Status: Published Journal Publication published 24 Apr, 2026 Read the published version in Advanced Composites and Hybrid Materials → Version 1 posted Editorial decision: Revision requested 18 Jan, 2026 Reviews received at journal 12 Jan, 2026 Reviewers agreed at journal 26 Oct, 2025 Reviews received at journal 09 Oct, 2025 Reviewers agreed at journal 01 Sep, 2025 Reviewers agreed at journal 29 Aug, 2025 Reviewers invited by journal 27 Aug, 2025 Editor assigned by journal 18 Aug, 2025 Submission checks completed at journal 07 Jul, 2025 First submitted to journal 11 Jun, 2025 You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. 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Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-6869022","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":508468270,"identity":"aaece4dd-ce43-4d1d-858d-a62f4a205a67","order_by":0,"name":"Jun Wang","email":"","orcid":"","institution":"Beijing Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Jun","middleName":"","lastName":"Wang","suffix":""},{"id":508468271,"identity":"ab0ecec0-9fd4-4817-885c-18c084174a29","order_by":1,"name":"Li Ren","email":"","orcid":"","institution":"Southwest University of Science and Technology","correspondingAuthor":false,"prefix":"","firstName":"Li","middleName":"","lastName":"Ren","suffix":""},{"id":508468272,"identity":"91583a1d-21ef-4c76-a9aa-b7c39d408830","order_by":2,"name":"Xinquan Zhang","email":"","orcid":"","institution":"Southwest University of Science and Technology","correspondingAuthor":false,"prefix":"","firstName":"Xinquan","middleName":"","lastName":"Zhang","suffix":""},{"id":508468273,"identity":"f114e310-c4db-4c3d-838d-a1552b18158d","order_by":3,"name":"Yao-feng Mao","email":"","orcid":"","institution":"Beijing Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Yao-feng","middleName":"","lastName":"Mao","suffix":""},{"id":508468275,"identity":"68435ec3-0a50-495a-9883-97a428a57221","order_by":4,"name":"Haifu Wang","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAyUlEQVRIiWNgGAWjYJACZgYbmwQ2EIuHeC1paQlsbCRqOZzAQLQWg+NnD78uSDifxyffwPjgbRuDvDlBLWfy0qxnJNwuBjqM2XBuG4PhzgYCWswO5JgZ8/64ndjGxsAmzdvGkGBwgJCW82/MjHkSzoG0sP8mTsuNHOPHPAkHwLYwE6XF/sYbM2aehGSgXxKbJeeckzDcQEiLZH+O8WeeBLs8+ebDBz+8KbORJ2gLELBJQGjGBiAhQVg9EDB/IErZKBgFo2AUjFwAAGhcOse8vQKAAAAAAElFTkSuQmCC","orcid":"","institution":"Beijing Institute of Technology","correspondingAuthor":true,"prefix":"","firstName":"Haifu","middleName":"","lastName":"Wang","suffix":""}],"badges":[],"createdAt":"2025-06-11 07:38:27","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-6869022/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-6869022/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1007/s42114-026-01775-x","type":"published","date":"2026-04-24T16:00:01+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":90535599,"identity":"a3b403d7-6525-4546-b1b6-c5fbc7f2b153","added_by":"auto","created_at":"2025-09-03 20:02:23","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":7843136,"visible":true,"origin":"","legend":"\u003cp\u003eSchematic illustration of layered ordered Al-FG/B-FG based on concept of “brick \u0026amp; mortar” structure prepared through the vacuum self-assembly.\u003c/p\u003e","description":"","filename":"floatimage1.png","url":"https://assets-eu.researchsquare.com/files/rs-6869022/v1/f7833de1f2bebe3cadeca7ba.png"},{"id":90535600,"identity":"c876442c-3a99-4be0-a66e-8d34b76282e6","added_by":"auto","created_at":"2025-09-03 20:02:23","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":3103430,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003ea\u003c/strong\u003e The layered ordered Al-FG/B-FG with four layers (M4) is obtained through vacuum filtration and drying. \u003cstrong\u003eb\u003c/strong\u003e The cross-view SEM images of film, in which b\u003csub\u003e1\u003c/sub\u003e and b\u003csub\u003e2\u003c/sub\u003e are the upper surface and lower surface of film, respectively. \u003cstrong\u003ec\u003c/strong\u003e The cross-view EDS images with F, B, and Al elements. \u003cstrong\u003ed\u003c/strong\u003e XRD patterns of Al-FG/B-FG with different layers. \u003cstrong\u003ee\u003c/strong\u003e TEM and the element distribution mapping images of Al-FG/B-FG.\u003c/p\u003e","description":"","filename":"floatimage2.png","url":"https://assets-eu.researchsquare.com/files/rs-6869022/v1/f7abf905bc2c2747e7e632b0.png"},{"id":90535597,"identity":"9624b290-eaa9-44b4-b892-8cd66a3074ab","added_by":"auto","created_at":"2025-09-03 20:02:23","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":284680,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003ea \u003c/strong\u003eThe TG curves. \u003cstrong\u003eb \u003c/strong\u003eDSC curves. \u003cstrong\u003ec and d\u003c/strong\u003e real-time MS curves under the heating rate of 10 ℃/min (c is m/z of 19, d is m/z of 31 corresponding to F and CF radicals).\u003c/p\u003e","description":"","filename":"floatimage3.png","url":"https://assets-eu.researchsquare.com/files/rs-6869022/v1/a49ffd80cdc0770bcc63b679.png"},{"id":90535603,"identity":"69120c77-f379-4b7d-b26b-4bd576dbc02e","added_by":"auto","created_at":"2025-09-03 20:02:23","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":4591907,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003ea\u003c/strong\u003eSchematic diagram of combustion experiment. \u003cstrong\u003eb\u003c/strong\u003e The combustion speed of Al-FG/B-FG with Al/B mass ratio from 1:3 to 4:0. \u003cstrong\u003ec\u003c/strong\u003e The images of combustion flame and \u0026nbsp;\u003cstrong\u003ed\u003c/strong\u003e \u0026nbsp;the flame area of Al-FG/B-FG with different layers and width. \u003cstrong\u003ee\u003c/strong\u003e The evolution process images and\u003cstrong\u003e f \u003c/strong\u003ecombustion speed of M4 film with width of 4, 5 and 6 mm.\u003c/p\u003e","description":"","filename":"floatimage4.png","url":"https://assets-eu.researchsquare.com/files/rs-6869022/v1/087655189f514135a306245d.png"},{"id":90536042,"identity":"3bb5a418-5b97-4cdd-b6f5-49f1e6afbc70","added_by":"auto","created_at":"2025-09-03 20:10:23","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":232128,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003ea\u003c/strong\u003e The pressure output curves of M4 film at different atmosphere. \u003cstrong\u003eb\u003c/strong\u003e The pressure of Al-FG/B-FG with different layers in N\u003csub\u003e2\u003c/sub\u003e atmosphere. \u003cstrong\u003ec\u003c/strong\u003e The maximum pressure output value and \u003cstrong\u003ed\u003c/strong\u003e average pressurization rate of Al-FG/B-FG with different layers in N\u003csub\u003e2\u003c/sub\u003e, O\u003csub\u003e2\u003c/sub\u003e and air atmospheres.\u003c/p\u003e","description":"","filename":"floatimage5.png","url":"https://assets-eu.researchsquare.com/files/rs-6869022/v1/04983f7e6bf4959a017f0acd.png"},{"id":90536041,"identity":"9d6898ba-e739-4dd8-a911-00db7e98c798","added_by":"auto","created_at":"2025-09-03 20:10:23","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":6249097,"visible":true,"origin":"","legend":"\u003cp\u003eSchematic diagram of the coupling reaction mechanism of layered ordered Al-FG/B-FG during combustion process.\u003c/p\u003e","description":"","filename":"floatimage6.png","url":"https://assets-eu.researchsquare.com/files/rs-6869022/v1/e60183c2835a7b543e1a197e.png"},{"id":90536149,"identity":"c74b958e-46b2-4cfe-a858-dc0e331cd3e4","added_by":"auto","created_at":"2025-09-03 20:18:23","extension":"png","order_by":7,"title":"Figure 7","display":"","copyAsset":false,"role":"figure","size":5307472,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003ea\u003c/strong\u003eSchematic of micro-energetic devices to destruct silicon and CD. \u003cstrong\u003eb\u003c/strong\u003e The pictures of deflagration process and fragmented silicon. \u003cstrong\u003ec\u003c/strong\u003e Pictures of CD, transience destruction and loss of function.\u003c/p\u003e","description":"","filename":"floatimage7.png","url":"https://assets-eu.researchsquare.com/files/rs-6869022/v1/331fd8c0c4d21dfc5527b739.png"},{"id":107928548,"identity":"ff54f50b-5ffa-4c08-88d4-8a4dd9845a04","added_by":"auto","created_at":"2026-04-27 16:11:17","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":25492693,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-6869022/v1/2977d5ea-745e-46af-a67a-056dc62fb519.pdf"},{"id":90535616,"identity":"4b54ca8c-3691-4125-84e2-6a44ff59500a","added_by":"auto","created_at":"2025-09-03 20:02:24","extension":"docx","order_by":0,"title":"","display":"","copyAsset":false,"role":"supplement","size":20494159,"visible":true,"origin":"","legend":"","description":"","filename":"SupportingInformation.docx","url":"https://assets-eu.researchsquare.com/files/rs-6869022/v1/98bf4ea1ef9d8ea5065a153a.docx"}],"financialInterests":"No competing interests reported.","formattedTitle":"Ordered Assembly of Fluorinated Graphene with Nano Fuels for Coupling Reaction and Application in Microenergetic Devices","fulltext":[{"header":"1. introduction","content":"\u003cp\u003eMicroenergetic devices integrated with energy materials from nano- to micrometers could achieve specific functions through precise control of reaction and energy release. Micro-thruster, micro-ignitor, micro-detonators, micro-power sources, minimally invasive surgical instruments (such as intravascular blasting), precision machining (micro explosive drilling) and self-destruction have been widespread concern and great potential in aerospace, medical and industrial fields \u003csup\u003e[\u003cspan additionalcitationids=\"CR2 CR3 CR4\" citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e]\u003c/sup\u003e. Energy materials as the key component integrated in micro-devices are required to have two basic characteristics\u003csup\u003e[\u003cspan additionalcitationids=\"CR7\" citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e]\u003c/sup\u003e. One is excellent mechanical properties, especially high toughness to integrate on the microchip \u003csup\u003e[\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e]\u003c/sup\u003e. More importantly, superior reactivity with high energy and pressure output at micro-size to realize specially function\u003csup\u003e[\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e]\u003c/sup\u003e. However, traditional energetic materials such as explosive and thermite could not able to meet the integration and functional requirements. They are generally powder and almost brittle. Moreover, it is hard to self-sustaining combustion and release high energy and pressure at micro-size \u003csup\u003e[\u003cspan additionalcitationids=\"CR12\" citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e]\u003c/sup\u003e. For applications and future microenergetic devices remains an elusive goal because of the lack of versatile energy materials.\u003c/p\u003e\u003cp\u003eLots of effort have been devoted to design and prepare versatile energy materials for microenergetic devices. At present, the construction of energetic film is the main strategy to satisfy the requirements of easy integration and high energy output\u003csup\u003e[\u003cspan additionalcitationids=\"CR15\" citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e]\u003c/sup\u003e. Assembling the typical metal oxides (such as CuO, Bi\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e, Fe\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e) and Al fuel could realize the ignition function\u003csup\u003e[\u003cspan additionalcitationids=\"CR18\" citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e]\u003c/sup\u003e. However, such film is still brittle and easy to fall off from the substrate after integration resulted from brittleness of metal oxides and poor interface interaction. Additionally, the energy density and pressure are extremely hard to meet the ignition and damage requirements at micro-size. To increase energy, reaction of Al and fluorine resulted from the higher reaction heat than that of oxidation reaction become hot topic in the field of energy materials and applied in microenergetic devices\u003csup\u003e[\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e]\u003c/sup\u003e. A novel superlattice PTFE/Al has been designed to integrate the micro-ignitor that achieved the ignition function \u003csup\u003e[\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e]\u003c/sup\u003e. However, PTFE/Al has insufficient pressure output resulted from solid reaction products applied in self-destruction and airbag. It is worth to note that superlattice PTFE/Al has high mechanical properties to integrate micro-devices resulted from PTFE and laminated structure. Based on above research, to further increase energy and pressure output, boron (B) as typical high-energy fuel, may be an excellent candidate\u003csup\u003e[\u003cspan additionalcitationids=\"CR22\" citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e]\u003c/sup\u003e because of reaction calorific value is 2 times that of Al powder. The calorific values of Al-O (oxygen) reaction and Al-F (fluorine) reaction are 31 kJ/g and 56 kJ/g, while the calorific values of B-O reaction and B-F reaction have 58 kJ/g and 105 kJ/g\u003csup\u003e[\u003cspan additionalcitationids=\"CR25\" citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e]\u003c/sup\u003e. More importantly, the product is gaseous BF\u003csub\u003e3\u003c/sub\u003e, which is a unique advantage for obtaining high pressure \u003csup\u003e[\u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e, \u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e]\u003c/sup\u003e. Unfortunately, low ignition and combustion reaction is big obstacle for B because of the surface oxide layer (B\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e) with a low melting point (450\u0026deg;C) and a high boiling point (1860\u0026deg;C) \u003csup\u003e[\u003cspan additionalcitationids=\"CR30\" citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e]\u003c/sup\u003e. Draw support from the high combustion reaction kinetics of Al, the B-F reaction induced by the Al-F reaction and then achieving the Al-F-B coupling effect may be a potential strategy\u003csup\u003e[\u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e]\u003c/sup\u003e. Moreover, the high calorific value and gaseous products from the B-F reaction are expected to further promote the Al-F reaction, making it possible to obtain self-sustaining combustion with high energy and pressure output at micro-size \u003csup\u003e[\u003cspan citationid=\"CR33\" class=\"CitationRef\"\u003e33\u003c/span\u003e]\u003c/sup\u003e.\u003c/p\u003e\u003cp\u003eSince the Al and B reactions are both solid phase reactions, it becomes daunting challenge how to assembly structure that could maintain the high toughness for integration while has high combustion reaction to release energy and pressure. Firstly, it is necessary to construct the orderly distribution and super-large interface for the heat transfer and mass diffusion \u003csup\u003e[\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e]\u003c/sup\u003e to support the continuous coupling reaction between Al-F and B-F. More importantly, assembly structure can ensure a strong interaction among fluorine, Al and B to obtain excellent mechanical properties and toughness. Inspired by coupling reaction and layered ordered structure \u003csup\u003e[\u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e, \u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e35\u003c/span\u003e]\u003c/sup\u003e greatly expanded interface for the solid phase reaction and excellent mechanical properties, it is natural to consider using B and Al as fuel and fluorine as oxidizer ordered stacked to form specially structure. To fulfill the above demands, graphene fluoride (FG) is selected as the fluorine source\u003csup\u003e[\u003cspan additionalcitationids=\"CR37\" citationid=\"CR36\" class=\"CitationRef\"\u003e36\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR38\" class=\"CitationRef\"\u003e38\u003c/span\u003e]\u003c/sup\u003e because two-dimensional planar could realize the orderly arrangement of Al and B on the molecular scale to promote the coupling reaction. Moreover, this two-dimensional structure is easy to assembly the layered ordered structure. Based on concept from \u0026ldquo;brick \u0026amp; mortar\u0026rdquo; structure \u003csup\u003e[\u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e39\u003c/span\u003e, \u003cspan citationid=\"CR40\" class=\"CitationRef\"\u003e40\u003c/span\u003e]\u003c/sup\u003e, FG as the \u0026ldquo;brick\u0026rdquo; could ensures ordered structure and high mechanical properties\u003csup\u003e[\u003cspan citationid=\"CR41\" class=\"CitationRef\"\u003e41\u003c/span\u003e, \u003cspan citationid=\"CR42\" class=\"CitationRef\"\u003e42\u003c/span\u003e]\u003c/sup\u003e. Fluorine rubber loading the Al or B is introduced as the \u0026ldquo;mortar\u0026rdquo; to further enhance the film toughness while providing more fuel sources to promote the combustion reaction with high energy and pressure. Consequently, layered ordered Al-FG/B-FG film has been successfully prepared through vacuum self-assembly (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e), which exhibits excellent mechanical toughness and can satisfy the integrated application on the microenergetic devices. Additionally, Al-FG/B-FG could achieve coupling reaction to produce high energy and pressure output. The self-sustaining combustion reaction, energy and pressure output performance are systematically studied to provide the theoretical basis and data support for the application. Finally, Al-FG/B-FG has been integrated in microenergetic devices to achieve ignition and self-destruction function.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e"},{"header":"2. Methods","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e\u003ch2\u003e2.1 Design and Fabrication Al-FG/B-FG\u003c/h2\u003e\u003cp\u003eFirst, two samples of 0.05 g FG are added to beakers containing 10 mL of NMP solution, respectively, and perform ultrasonic dispersion until there is no obvious precipitation to obtain FG dispersion. Then, 0.075g Al and 0.5 g fluorine rubber (FR) solution (5 wt.%) are added to FG dispersion, ultrasonic dispersion for 2 h, magnetic stirring for 30 min, to form a suspension of the Al-FG system. Similarly, 0.025g B and 0.5 g fluorine rubber (FR) solution (5 wt.%) are added to FG dispersion, ultrasonic dispersion for 2 h, magnetic stirring for 30 min, to form a suspension of the B-FG system.\u003c/p\u003e\u003cp\u003eThe Al-FG/B-FG film with layered stacking structure is then prepared by vacuum self-assembly. Taking the M4 film as an example, the suspensions of the Al-FG and B-FG are divided into two parts of equal quality. Use a glue head dropper to add the suspension of the Al-FG system to the vacuum-activated membrane within 1 min, until all the solvent is removed, so that Al, FG and FR are self-assembled to form the first layer of Al-FG. Subsequently, the suspension of the B-FG system is added to the Al-FG layer that has no solvent, and wait for the solvent to be completely removed to form a second layer of B-FG. Repeat the above steps to consume all prepared suspensions to form the energetic film with Al-FG/B-FG layered structure. Finally, the Al-FG/B-FG layered ordered film is dried in an oven at 40 ℃ for 12 h, and peeled off from the membrane to obtain the M4 film.\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec4\" class=\"Section2\"\u003e\u003ch2\u003e2.2 Morphology and Structure Characterization\u003c/h2\u003e\u003cp\u003eThe morphology and crystal structure of the Al-FG/B-FG film is characterized by field emission scanning electron microscope (FE-SEM, ULTRA 55, ZEISS, Germany) and powder X-ray diffraction (XRD, X\u0026rsquo;Pert PRO) with a monochromatized Cu Kα radiation (λ\u0026thinsp;=\u0026thinsp;1.5418\u0026Aring;). Surface elemental analysis of the bionic films is characterized by energy dispersive X-ray spectroscopy (EDS).\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec5\" class=\"Section2\"\u003e\u003ch2\u003e2.3 Thermal and combustion testing\u003c/h2\u003e\u003cp\u003eThe thermal properties of the Al-FG/B-FG film are measured by the simultaneous thermal analyzer (TG-DSC, STA449F5, NETZSCH, Germany) from 50 to 900 ℃ under a heating rate of 10 ℃/min at N\u003csub\u003e2\u003c/sub\u003e atmosphere. Meanwhile, time-resolved mass spectrometry (MS) (PFEIFFER, 2 OMNI star, Germany) for on-line analysis of the fugitive gaseous products are collected via a series data collection scheme.\u003c/p\u003e\u003cp\u003eMaterials burning experiments are to test the reaction kinetics of Al-FG/B-FG film, including the maximum flame area and burning rate. The splines used in the combustion experiment have the lengths of 35 mm and widths of 4, 5 and 6 mm, respectively. A nickel-chromium wire with a diameter of 0.2 mm is used to heat one end of the spline, and then a high-speed camera (UX50, Photron FASTCAM, Japan) with 2000 fps records the entire process of flame propagation.\u003c/p\u003e\u003cp\u003eMaterials pressure experiments are to test the dynamic pressure curve in a closed chamber when the energetic sample undergoes combustion or explosion reaction. The experimental tests are carried out in a variety of atmospheres (1 atm N\u003csub\u003e2\u003c/sub\u003e, Air, and O\u003csub\u003e2\u003c/sub\u003e, respectively) using small block of Al-FG/B-FG film. Typically, 100 mg sample is placed in the confined cell with a fixed volume of 330 mL and ignited by a nichrome wire (0.2 mm in diameter, 40 mm in length). And, the dynamic pressure during the reaction process is measured by a pressure sensor (PC290, 1 kHz) attached to the confined cell and the pressure signal is converted into a voltage signal by software, and then recorded in a computer.\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec6\" class=\"Section2\"\u003e\u003ch2\u003e2.3 Self-destruction devices\u003c/h2\u003e\u003cp\u003eExcellent transient damage ability is a prerequisite for device damage application. Therefore, the transient damage performance of Al-FG/B-FG film is tested, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ea. The Al-FG/B-FG film with a specification of 12 mm\u0026times;12 mm (10 mg) was integrated on the CD through a glass substrate. A nickel-chromium wire with a diameter of 0.2 mm is used to ignite the films smoothly. The high-speed camera (X213, Qianyanlang, China) sets the frame rate to 2000 fps to capture and record the entire process of ignition and destruction of the silicon wafer by the film.\u003c/p\u003e\u003c/div\u003e"},{"header":"3. Results and discussions","content":"\u003cdiv id=\"Sec8\" class=\"Section2\"\u003e\u003ch2\u003e3.1 Morphology and composition of Al-FG/B-FG\u003c/h2\u003e\u003cp\u003eTo assembly layered ordered structure of Al-FG/B-FG, Al and B nano-particles are deposited on FG to form Al-FG and B-FG layers, respectively. Two-dimensional FG provides sufficient strength as a skeleton and \u0026ldquo;mortar\u0026rdquo; to impart high toughness by creating the strong adhesion between Al (or B) and FG. They are stacked alternately to assembly Al-FG/B-FG structure, which not only achieves the orderly arrangement of Al and B at the molecular level, but also fully possesses the integrated function on the microdevices. Additionally, the supporting effect of fluorine rubber and the FG skeleton endows Al-FG/B-FG with good flexibility. A circular sheet with radius of ~\u0026thinsp;35 mm and thickness of ~\u0026thinsp;70 \u0026micro;m has well uniformity and mechanical toughness that can be rolled into a cylinder with diameter of only 6 mm (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea). The layered ordered structure of Al-FG/B-FG consisted of Al-FG (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb\u003csub\u003e1\u003c/sub\u003e) and B-FG layer (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb\u003csub\u003e2\u003c/sub\u003e) is observed from SEM images (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb). To more clearly display the \u0026ldquo;brick \u0026amp; mortar\u0026rdquo; structure of Al-FG/B-FG, the element mapping of the cross section is further characterized EDS. A layered-like texture can be observed in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ec intuitively shows the staggered arrangement of Al and B elements, further indicating that the Al-FG/B-FG stacking structure. The F elements from FG and FR are evenly distributed over the entire cross-section, providing a significant support effect for the film and the adequate fluorine source during the reaction. The layered stacking structures are also observed in Al-FG/B-FG with different layers (Fig. \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003e).\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eThe compositions of Al-FG/B-FG was further characterized via XRD and XPS spectra exhibits the presence of Al and FG, which indicates that the prepared sample have high stability during long-term storage (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ed and S2). No peak of B be detected in XRD due to its semi-crystalline nature. Besides, the TEM image of the Al-FG/B-FG indicates that the Al and FG layers are interspersed with each other, and a small amount of irregular B nanoparticles are randomly distributed on the FG layer (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ee). The element distribution mapping also supports this result. Because the B element is relatively light, it cannot show the element distribution state well. Based on above the results, it can be confirmed that the Al-FG/B-FG with layered stacking structure has been successfully prepared through vacuum self-assembly. Layered stacking structure of Al-FG/B-FG would offer super-large interface for mass diffusion and heat transfer, and exhibits intuitive high flexibility free-standing for integration in microenergetic devices.\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec9\" class=\"Section2\"\u003e\u003ch2\u003e3.2 Combustion reaction behavior of Al-FG/B-FG\u003c/h2\u003e\u003cp\u003eCombustion reaction and energy output of Al-FG/B-FG is key to apply in microenergetic devices. The thermal reaction of Al-FG/B-FG films with different layers was studied on TG-DSC under the heating rate of 10 ℃/min to evaluate the energy output. Two stages of mass loss from 300 to 560 ℃ have been observed in TG curves (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ea). The decomposition of fluorine rubber and FG causes the appearance of the first declining region. The mass loss in the second stage is due to the reaction of B and FG to produce gaseous BF\u003csub\u003e3\u003c/sub\u003e, however, since the Al-F reaction produces solid AlF\u003csub\u003e3\u003c/sub\u003e, the decline rate is slightly slowed down. The largest mass loss is observed for M4 indicating that the B-F reaction is the most complete due to appropriate ratio among FG, Al and B. For all samples, a mass increasing is observed resulted from Al reacted with N\u003csub\u003e2\u003c/sub\u003e to form the solid product Al\u003csub\u003e4\u003c/sub\u003eN\u003csub\u003e3\u003c/sub\u003e. The reaction temperature and energy output of Al-FG/B-FG with different layers are obtained from DSC curves. The exothermic values are 1001.23 J/g, 1236.32 J/g, 1393.45 J/g, 1162.25 J/g, and 1116.74 J/g (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eb) occurred the coupling reaction between B-F and Al-F reaction\u003csup\u003e[\u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e, \u003cspan citationid=\"CR43\" class=\"CitationRef\"\u003e43\u003c/span\u003e]\u003c/sup\u003e. The highest value is obtained in M4 film that reaches up to 1.4 times higher than that of M0 film (Al/FG mixtures). The high energy output further illustrates that alternating stacking of Al-FG and B-FG layers could increase interface for the mass diffusion and heat transfer, and realize the chain reaction of Al-F and B-F. The real-time mass spectrometry analysis is carried out to explore the intermediates of FG decomposition and reaction processes of Al-FG/B-FG. The m/z values of 19, 31, 50 and 69 are obtained and assigned to F, CF, CF\u003csub\u003e2\u003c/sub\u003e and CF\u003csub\u003e3\u003c/sub\u003e radials, respectively (Fig. S4). Figure\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ec-d show F and CF radical peaks from FG and fluorine rubber at different temperature. Compared to Al-F and B-F, high content of F and CF radials are observed for layered ordered Al-FG/B-FG further illustrate coupling effect between Al-F and B-F, thereby generating a large number of F and CF radicals resulted in significantly increased reaction heat.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eThe self-sustain combustion of Al-FG/B-FG at micro-size is the basic requirements for their application in microenergetic devices to achieve ignition and damage function. The combustion behavior is influenced on chemical reaction and physical process. Therefore, the effect of typical factors (mass ratios, layer number and size) of Al-FG/B-FG on the combustion reaction and flame propagation characteristics are systematically studied for the applications. Figure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea gives the schematic diagram of combustion test. The prepared Al-FG/B-FG are cut into splines with length of 35 mm and width of 4 mm, 5 mm, and 6 mm, respectively. The film spline is adhered to the test platform, and the nickel-chromium wire was employed to ignite at the one end, flame propagation was recorded through high-speed camera. Figure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eb shows the combustion speed of Al-FG/B-FG with different Al/B mass ratios ranging from 1:3 to 4:0, the combustion and flame propagation speed increases from 122.81 to 259.26 mm/s. Notably, B-FG film without Al (0:4) cannot be ignited and sufficient Al particles must be added into Al-FG/B-FG. The highest combustion speed is obtained for Al-FG/B-FG with Al/B mass ratio of 3:1.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eFigure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ec and \u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ed shows the maximum combustion flame image and flame area of Al-FG/B-FG films with layers of 1, 2, 4, 6 and widths of 4, 5 and 6 mm. The plenty of gaseous products in the intense combustion reaction leads to the diversity of the combustion flame shape. For Al-FG/B-FG, as the layer number from 1 to 6 increases, the maximum flame area increases. The Al-FG/B-FG with two layers (M2) has a relatively small flame area resulted from only one contact interface between the Al-FG and B-FG components. The Al-FG/B-FG with four layers (M4) has largest flame area resulted from layered ordered structure for mass diffusion and heat transfer, and coupling reaction between Al-F and B-F. In addition, the combustion flame area also increases with the increase of the spline width of 4, 5 and 6 mm, respectively. Figure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ee and S5 shows the flame propagation process of the Al-FG/B-FG spline with 4 layers and widths of 4, 5 and 6 mm. The results show that the Al-FG/B-FG spline burns with a wider flame area and faster propagation rate. As the number of layer increases, the flame propagation speed increases (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ef). The reaction interface increases with the layers increase under the same size, enhancing the mass diffusion and heat transfer process, thereby increases the combustion speed. Additionally, Al-FG/B-FG with appropriate layers would promote coupling reaction between Al-F and B-F. Therefore, the combustion reaction increases firstly and then decreases with the layer increase and the highest speed is obtained for Al-FG/B-FG with four layers (M4).\u003c/p\u003e\u003cp\u003eConsidering the complexity in the practical applications for microenergetic devices, the pressure output as an important property, especially for thruster and destruction. Therefore, pressure of Al-FG/B-FG under different atmospheres was further studied to verify its excellent environmental adaptability. Figure\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ea gives the pressure-time curves of Al-FG/B-FG with 4 layers (M4) show high-pressure output (~\u0026thinsp;200 kPa) even in an oxygen-free environment. This proves that Al-FG/B-FG has stable ability to react and release energy and pressure in harsh environments, which is benefit for practical applications in aerospace and deep sea. In oxygen atmosphere, the much higher-pressure output is obtained because of carbon derived from FG reacted with oxygen to form CO\u003csub\u003e2\u003c/sub\u003e. Al-FG/B-FG with different layers also exhibit excellent pressure output performance in N\u003csub\u003e2\u003c/sub\u003e atmospheres (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eb). The maximum pressure value and the average pressurization rate of Al-FG/B-FG with different layers under different atmospheres (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ec and d) are basically same resulted from the total thickness and the total amount of reactants are same. Therefore, the gaseous product of the combustion is mainly BF\u003csub\u003e3\u003c/sub\u003e. A significant difference is higher pressure and pressurization rate are observed in oxygen due to oxidation reaction of carbon derived from FG to produce CO\u003csub\u003e2\u003c/sub\u003e. Al-FG/B-FG with 6 layers have high pressure value may be a complete oxidation reaction carbon. The high and fast pressure output is benefit for the practical applications.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eThe above experimental results clearly confirm Al-FG/B-FG with \u0026ldquo;brick \u0026amp; mortar\u0026rdquo; structure that has excellent mechanical properties and combustion performance. The self-sustain combustion reaction with high energy and pressure output at micro-size has been successfully realized. The self-sustain combustion reaction, high energy and pressure output at micro-size are attributed to three main aspects. Firstly, coupling effect of high reaction kinetics of Al-FG and high reaction heat of B-FG. Secondly, layered ordered structure of Al-FG/B-FG provides super-large interface for mass diffusion and heat transfer to enhance combustion reaction. Additionally, gaseous products of BF\u003csub\u003e3\u003c/sub\u003e would be benefit to mass diffusion and heat transfer, and pressure output. Figure\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003e shows the coupling mechanism of Al-FG/B-FG to obtain high combustion reaction and pressure output. Al would react with F and CF radials from FG decomposition \u003csup\u003e[\u003cspan citationid=\"CR44\" class=\"CitationRef\"\u003e44\u003c/span\u003e, \u003cspan citationid=\"CR45\" class=\"CitationRef\"\u003e45\u003c/span\u003e]\u003c/sup\u003e to release energy, which could transmit to stimulate reaction of B-FG layer due to large interface. High energy and gaseous BF\u003csub\u003e3\u003c/sub\u003e from the reaction of B-FG will further promote the reaction Al-FG, thereby realizing the coupling effect of Al-FG and B-FG reaction during combustion process. Al-FG/B-FG with \u0026ldquo;brick \u0026amp; mortar\u0026rdquo; structure offers a platform to obtain superior combustion reaction at micro-size and release high energy and pressure for the applications in microenergetic devices.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec10\" class=\"Section2\"\u003e\u003ch2\u003e3.3 Applications of Al-FG/B-FG in microenergetic devices\u003c/h2\u003e\u003cp\u003eStable combustion reaction, energy and pressure output performance at microscale is key for the applications, such as micro-thruster, micro-ignitor and micro-power sources. Information as cornerstone of rapid development of society has played the more important role. The vigorous development of big data and artificial intelligence has greatly challenged information security, and the consequences are always devastating\u003csup\u003e[\u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e46\u003c/span\u003e, \u003cspan citationid=\"CR47\" class=\"CitationRef\"\u003e47\u003c/span\u003e]\u003c/sup\u003e. Self-destruction devices, as the last defender to protect information security, have played a decisive role in maintaining national, social and technological security\u003csup\u003e[\u003cspan citationid=\"CR48\" class=\"CitationRef\"\u003e48\u003c/span\u003e]\u003c/sup\u003e. Therefore, designing high-performance energy materials and developing self-destructive devices is of great significance for preventing the information leakage and maintaining national stability. Herein, to verify application of the Al-FG/B-FG in self-destruction device on the information storage medium, it is integrated on the microchip to test the deflagration damage process. Figure\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ea and Fig. S6 shows a schematic of experimental apparatus for transience destruction performance test, and the deflagration process images are given in Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003eb. Based on experimental results, silicon wafer crack or split due to high pressure and heat from Al-FG/B-FG reaction. Figure\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ec shows that the CD has been damaged and lost the function of storing information. Moreover, the amount of Al-FG/B-FG is only 10 mg, which is benefit to integrate nano-energetic devices. This experiment confirms that the Al-FG/B-FG has high-performance energy output while ensuring the flexibility and integrated function, which can achieve damage to the microchip at micro-size. The above results fully confirm the rationality of the \u0026ldquo;brick \u0026amp; mortar\u0026rdquo; strategy and the layered stacking structure. In order to further illustrate the applications of Al-FG/B-FG in microenergetic devices, an ignitor has been integrated that could realize ignition function (Fig. S7). The results further reveal that Al-FG/B-FG has excellent combustion reaction and energetic performance that can be applied to integrate kinds of devices such as micro-thruster, micro-ignitor and micro-power sources.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003c/div\u003e"},{"header":"Conclusion","content":"\u003cp\u003eTo develop high-performance energy materials and applied in microenergetic devices, layered ordered Al-FG/B-FG has been designed based the concept of \u0026ldquo;brick \u0026amp; mortar\u0026rdquo; structure and successfully prepared by vacuum self-assembly. Under the coupling effect of the \u0026ldquo;brick\u0026rdquo; FG and the \u0026ldquo;mortar\u0026rdquo; fluorine rubber loaded with Al or B atoms, Al-FG/B-FG has strong mechanical toughness to integrate in micro-devices. Self-sustaining combustion reaction, high energy and pressure output has been obtained resulted from coupling effect between Al-FG and B-FG reaction through \u0026ldquo;brick \u0026amp; mortar\u0026rdquo; structure. Al-FG/B-FG has been integrated in self-destruction devices and micro-ignitor. Silicon wafer and CD damaged to crack and loss of function only 20 microseconds. Furthermore, micro-ignitor with Al-FG/B-FG can realize ignition, which further prove Al-FG/B-FG with high combustion reaction and energetic performance that could be applied to integrate kinds of micro-energetic devices.\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003eThe authors declare no competing financial interest.\u003c/p\u003e\u003ch2\u003eFunding\u003c/h2\u003e\u003cp\u003eThis work receives financial support from the National Natural Science Foundation of China (T2222027).\u003c/p\u003e\u003ch2\u003eAuthor Contribution\u003c/h2\u003e\u003cp\u003eJun Wang done formal analysis and wrote \u0026amp; edited manuscript, provided methodology and supervision.Li Ren done experiment, data curation.Xingquan Zhang done formal analysis.Yaofeng Mao prepared figures 1-6.Haifu Wang provided resources and edited manuscript.All authors reviewed the manuscript.\"\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\u003cli\u003e\u003cspan\u003eWang Z, Guan C, Wang X, Zheng W, Su L (2024) Study on characteristics of a high-precision cold gas micro thruster. 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Chem Eng J 459:141506. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.cej.2023.141506\u003c/span\u003e\u003cspan address=\"10.1016/j.cej.2023.141506\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"advanced-composites-and-hybrid-materials","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"achm","sideBox":"Learn more about [Advanced Composites and Hybrid Materials](https://link.springer.com/journal/42114)","snPcode":"42114","submissionUrl":"https://submission.nature.com/new-submission/42114/3","title":"Advanced Composites and Hybrid Materials","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"em","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"Al-FG/B-FG, interfacial structure, self-sustaining combustion, pressure, microenergetic device","lastPublishedDoi":"10.21203/rs.3.rs-6869022/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-6869022/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eHigh toughness, superior reactivity with high energy and pressure output at micro-size are the basic requirements for energy materials applied in microenergetic devices such as micro-thruster, micro-ignitor and micro-power sources. Herein, fluorinated graphene as multifunctional additive is employed to ordered assembly flexible Al-FG/B-FG film based on \u0026ldquo;brick \u0026amp; mortar\u0026rdquo; structured concept prepared by vacuum self-assembly. Graphene fluoride (FG), as the \u0026ldquo;brick\u0026rdquo;, integrates with fluorine rubber loading Al (aluminum) or B (boron) nanoparticles as two types \"mortar\" that are stacked alternately to assembly ordered structure and obtain strong toughness. The layered ordered Al-FG/B-FG could efficiently combine the high reaction kinetics of Al-FG and the ultra-high calorific value of B-FG to realize coupling reaction and achieve superior self-sustaining combustion at micro-size, release high-energy and pressure. Subsequently, Al-FG/B-FG film has been integrated in micro-ignitor and self-destructive devices to achieve ignition and damage functions. More importantly, Al-FG/B-FG film still maintains stable energy output characteristics in harsh environments and could achieve damage effects in only 20 microseconds applied in self-destructive devices. This work establishes an innovative configuration to design novel energy materials and apply in micro-devices.\u003c/p\u003e","manuscriptTitle":"Ordered Assembly of Fluorinated Graphene with Nano Fuels for Coupling Reaction and Application in Microenergetic Devices","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-09-03 20:02:18","doi":"10.21203/rs.3.rs-6869022/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"decision","content":"Revision requested","date":"2026-01-19T00:31:13+00:00","index":"","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2026-01-13T01:52:19+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"156469118571514330220412522848858784345","date":"2025-10-26T16:07:06+00:00","index":"hide","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2025-10-09T08:51:28+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"57753359704301197594555408943517661037","date":"2025-09-01T10:23:51+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"108688622509418422756263883758393946073","date":"2025-08-29T09:48:50+00:00","index":"hide","fulltext":""},{"type":"reviewersInvited","content":"","date":"2025-08-27T04:59:50+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2025-08-18T11:09:41+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2025-07-08T01:27:13+00:00","index":"","fulltext":""},{"type":"submitted","content":"Advanced Composites and Hybrid Materials","date":"2025-06-11T07:31:29+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"advanced-composites-and-hybrid-materials","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"achm","sideBox":"Learn more about [Advanced Composites and Hybrid Materials](https://link.springer.com/journal/42114)","snPcode":"42114","submissionUrl":"https://submission.nature.com/new-submission/42114/3","title":"Advanced Composites and Hybrid Materials","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"em","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"a6866a3d-df89-4a2b-a3be-bec8d783f561","owner":[],"postedDate":"September 3rd, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[],"tags":[],"updatedAt":"2026-04-27T16:08:50+00:00","versionOfRecord":{"articleIdentity":"rs-6869022","link":"https://doi.org/10.1007/s42114-026-01775-x","journal":{"identity":"advanced-composites-and-hybrid-materials","isVorOnly":false,"title":"Advanced Composites and Hybrid Materials"},"publishedOn":"2026-04-24 16:00:01","publishedOnDateReadable":"April 24th, 2026"},"versionCreatedAt":"2025-09-03 20:02:18","video":"","vorDoi":"10.1007/s42114-026-01775-x","vorDoiUrl":"https://doi.org/10.1007/s42114-026-01775-x","workflowStages":[]},"version":"v1","identity":"rs-6869022","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-6869022","identity":"rs-6869022","version":["v1"]},"buildId":"XKTyCvWXoU3ODBz1xrDgd","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}