Zhang Yang, Xing Yan-Yan, Wang Chao, Pang Rui, Ren Wei-Wei, Wang Shan, Li Zhi-Min, Yang Li, Tong Wen-Chao, Wang Qian-You, Zang Shuang-Quan
Henan Key Laboratory of Crystalline Molecular Functional Materials, Green Catalysis Center and College of Chemistry, Zhengzhou University, Zhengzhou 450001, China.
International Laboratory for Quantum Functional Materials of Henan, School of Physics and Microelectronics, Zhengzhou University, Zhengzhou 450001, China.
ACS Appl Mater Interfaces. 2022 May 16. doi: 10.1021/acsami.2c05252.
Exploring novel hypergolic fuels for modern space propulsion is highly desired. However, the analysis and understanding of the structure and hypergolic performance at the molecular level are still insufficient. To understand the factors that dictate hypergolicity, we conducted a comparative study on a series of metal-organic frameworks (MOFs) characterized by the same topology but with varied ligand structures. The ignition delay (ID) time trend was found to be imidazole < triazole < tetrazole, and the rapid ID time was 8 ms. By combining experimental studies and density functional theory (DFT) calculations, we found that propargyl and cyanoborohydride groups that functioned as dual hypergolic triggers contributed to the hypergolicity, and a distinct electronic structure was detrimental to ID time. The structure-performance relationships presented herein can potentially provide some fundamental insights into the field of developing high-performance hypergolic fuels.
探索用于现代太空推进的新型自燃燃料是非常必要的。然而，在分子水平上对其结构和自燃性能的分析与理解仍不充分。为了了解决定自燃性的因素，我们对一系列具有相同拓扑结构但配体结构不同的金属有机框架（MOF）进行了对比研究。发现点火延迟（ID）时间趋势为咪唑＜三唑＜四唑，快速ID时间为8毫秒。通过结合实验研究和密度泛函理论（DFT）计算，我们发现作为双重自燃触发剂的炔丙基和氰基硼氢化物基团促成了自燃性，而独特的电子结构对ID时间不利。本文提出的结构-性能关系可能为高性能自燃燃料的开发领域提供一些基本见解。
