Ruixuan Xu, Zhihua Xue, Danfeng Yang, Xin Li, Hongqi Nie, Yongqiang Guo, Hua Guo, Qi-Long Yan* and Junwei Gu*. Highly Energy Release of Aluminum@Ammonium Perchlorate Composites Incorporated with Graphene Oxide-based Energetic Coordination Polymer. Advanced Functional Materials, 2024, DOI: 10.1002/adfm.202423205. 2023IF=18.5.（1區(qū)材料科學(xué)Top期刊）
http://doi.org/10.1002/adfm.202423205
Abstract
Achieving high energy release of aluminum (Al) and ammonium perchlorate (AP) is of significant importance in the realm of energy materials. In this work, integrated Al@AP/GO-CHZ-M (M = Co2+ or Ni2+) composites have been successfully synthesized through an integrated design and precise catalysis approach. The integrated Al@AP/Co composites exhibit fast decomposition, with a 76.6℃ reduction in decomposition temperature and a 66.0% increase in heat release compared to Al+AP mixture counterpart. From a kinetic perspective, the decomposition activation energy for Al@AP/Co is largely decreased by 215.5 kJ mol-1 (-67.4%) and its kinetics shifted to an autocatalytic model. Transition metals in GO-CHZ-M facilitate the proton transfer during the decomposition of AP, significantly increasing the yield of low-valence nitrogen oxides. The ignition of the Al@AP/M composites was enhanced, with a 37.2 ms (-40.2%) reduction in ignition delay and a 6.6-fold increase in radiation intensity over Al+AP. The change from deflagration for the physical mixture to detonation for integrated Al@AP/M composites further suggests highly energy release. Furthermore, the mechanism of the integrated design and precise catalysis on the energy release enhancement of Al@AP composites was elucidated. This approach holds broad application prospects in the fields of solid propellants, aluminized explosives, micro-thrusters and pyrotechnics.
實(shí)現(xiàn)鋁粉（Al）和高氯酸銨（AP）的高釋能效率在含能材料領(lǐng)域具有重要意義。本文基于鋁/氧化劑一體化和精準(zhǔn)催化設(shè)計(jì)，成制備了Al@AP/GO-CHZ-M (M = Co2+ or Ni2+)復(fù)合材料。Al@AP/Co擁有更快的分解速率，其分解峰溫較物理混合物Al+AP降低了76.6℃，反應(yīng)放熱量提高了66.0%。動(dòng)力學(xué)計(jì)算表明Al@AP/Co分解活化能減少了215.5 kJ mol-1 (-67.4%)，其分解動(dòng)力學(xué)過(guò)程轉(zhuǎn)為自催化模型。GO-CHZ-M催化劑中的過(guò)渡金屬有助于促進(jìn)AP分解的質(zhì)子轉(zhuǎn)移過(guò)程，顯著提高了產(chǎn)物中低價(jià)態(tài)氮氧化物的含量。一體化Al@AP/M復(fù)合物的點(diǎn)火性能得到改善，點(diǎn)火延遲時(shí)間較物理混合物Al+AP縮短了37.2 ms (-40.2%)，火焰輻射強(qiáng)度提高了6.6倍。與物理混合物的爆燃行為相比，一體化Al@AP/M復(fù)合物點(diǎn)火后迅速發(fā)生爆炸，表明釋能效率得到顯著增強(qiáng)。此外，本文提出了一體化設(shè)計(jì)和精準(zhǔn)催化對(duì)Al@AP復(fù)合物的釋能增強(qiáng)機(jī)制。該設(shè)計(jì)策略在固體推進(jìn)劑、含鋁炸藥、微推進(jìn)系統(tǒng)及火工品等領(lǐng)域具有廣闊的應(yīng)用前景。
論文亮點(diǎn)
1. 優(yōu)化制備了Al@AP/GO-CHZ-M (M = Co2+ or Ni2+）復(fù)合材料，實(shí)現(xiàn)了組分的致密接觸及對(duì)AP的精準(zhǔn)催化。
2. 一體化Al@AP/M復(fù)合材料的反應(yīng)放熱量較物理混合物提高了289.2 J g-1 (+66.0%)，分解活化能降低了215.5 kJ mol-1 (-67.4%)。
3. 一體化Al@AP/M復(fù)合材料較物理混合物擁有更快的能量釋放速率，點(diǎn)火延遲縮短了40.2%，火焰輻射強(qiáng)度提高了6.6倍，呈現(xiàn)出劇烈的爆炸特性。
第一作者：許睿軒郵件地址：xrxpd@nwpu.edu.cn
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