近红外光利用供体-受体共晶触发高温,The Journal of Physical Chemistry Letters

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近红外光利用供体-受体共晶触发高温
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2022-07-14 , DOI: 10.1021/acs.jpclett.2c01037
Wenbin Chen ₁ , Li Dang ₁ , Zicong Situ ₁ , Shaofei Ni ₁ , Yetao Chen ₁ , Sheng Zhu ₁ , Hailin Li ₁ , Shun-Li Chen ₁ , David Lee Phillips ₂ , Ming-De Li _{1,

3}

Affiliation

为响应低功率近红外激光的高能材料开发合适的引发可以帮助取代当前昂贵且笨重的激光引发系统。在这里，我们报告了一种分子定制的 1:1 供体 - 受体 (DA) 电荷转移 (CT) 共晶体系统，该系统表现出超宽吸收（200-2500 nm）特性以及值得注意的非常快速的自组装行为。非常窄的最高占据分子轨道-最低未占据分子轨道间隙使N , N , N ', N '-四甲基- p-苯二胺和四卤代-1,4-苯醌 (TMPD-TXBQ) 共晶体在近红外范围内具有出色的光捕获能力。^{当用输入能量仅为 40 mJ 或功率密度为 260 mW·cm –2}的低功率手持式 808 nm 激光照射时，这些 TMPD-TXBQ 共晶体立即进行有效的光热转换，随后发生剧烈的放热热转换。由于这些cocystals中面对面的DADA堆叠导致聚合反应达到高达318.9°C的温度。该温度足以热引发最常见的含能材料，因此这种 TMPD-TXBQ 共晶体可以作为一种紧凑、轻便且具有成本效益的近红外激光引发剂。

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Near-Infrared Light Triggered a High Temperature Utilizing Donor–Acceptor Cocrystals

Developing a suitable initiation for the energetic materials that respond to a low-power near-infrared laser can aid in replacing the current expensive and bulky laser-initiation systems. Here, we report on a system of molecularly tailored 1:1 donor–acceptor (D-A) charge-transfer (CT) cocrystals that manifest ultrabroad absorption (200–2500 nm) characteristics as well as noteworthy very fast self-assembly behaviors. The very narrow highest occupied molecular orbital–lowest unoccupied molecular orbital gap enables N,N,N′,N′-tetramethyl-p-phenylenediamine and tetrahalo-1,4-benzoquinones (TMPD-TXBQ) cocrystals to have a great light-harvesting ability in the near-infrared range. When irradiated with a low-power hand-held 808 nm laser with an input energy of only 40 mJ or a power density of 260 mW·cm^–2, these TMPD-TXBQ cocrystals immediately undergo an efficient photothermal conversion followed by a dramatic exothermic thermal polymerization reaction due to the face-to-face D-A-D-A stacking in these cocystals to achieve a temperature as high as 318.9 °C. This temperature is high enough for a thermal initiation of most common energetic materials, and thus this TMPD-TXBQ cocrystal can potentially act as a near-infrared laser initiator that is compact, lightweight, and cost-effective.

更新日期：2022-07-14

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