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Formation and fragmentation of 2-hydroxyethylhydrazinium nitrate (HEHN) cluster ions: a combined electrospray ionization mass spectrometry, molecular dynamics and reaction potential surface study
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2023-06-16 , DOI: 10.1039/d3cp02610h
Wenjing Zhou 1, 2 , Jianbo Liu 1, 2 , Steven D Chambreau 3 , Ghanshyam L Vaghjiani 4
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2023-06-16 , DOI: 10.1039/d3cp02610h
Wenjing Zhou 1, 2 , Jianbo Liu 1, 2 , Steven D Chambreau 3 , Ghanshyam L Vaghjiani 4
Affiliation
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The 2-hydroxyethylhydrazinium nitrate ([HOCH2CH2NH2NH2]+NO3−, HEHN) ionic liquid has the potential to power both electric and chemical thrusters and provide a wider range of specific impulse needs. To characterize its capabilities as an electrospray propellant, we report the formation of HEHN cluster ions in positive electrospray ionization (ESI) and their collision-induced dissociation. The experiment was carried out using ESI guided-ion beam mass spectrometry which mimics an electrospray thruster in terms of ion emission, injection into a vacuum and fragmentation in space. Measurements include compositions of primary ions in the electrospray plume and their individual dissociation product ion cross sections and threshold energies. The results were interpreted in light of theoretical modeling. To determine cluster structures that are comprised of [HE + H]+ and NO3− constituents, classical mechanics simulations were used to create initial guesses; and for clusters that are formed by reactions between ionic constituents, quasi-classical direct dynamics trajectory simulations were used to mimic covalent bond formation and structures. All candidate structures were subject to density functional theory optimization, from which global minimum structures were identified and used for construction of reaction potential energy surface. The comparison between experimental values and calculated dissociation thermodynamics was used to verify the structures for the emitted species [(HEHN)nHE + H]+, [(HEHN)n(HE)2 + H]+, [(HE)n+1 + H]+ and [(HE)nC2H4OH]+ (n = 0–2), of which [(HE)1–2 + H]+ dominates. Due to the protic nature of HEHN, cluster fragmentation can be rationalized by proton transfer-mediated elimination of HNO3, HE and HE·HNO3, and the latter two become dominant in larger clusters. [(HE)2 + H]+ and [(HE)nC2H4OH]+ contain H-bonded water and consequently are featured by water elimination in fragmentation. These findings help to evaluate ion formation and fragmentation efficiencies and their impacts on electrospray propulsion.
中文翻译：
硝酸 2-羟乙基肼 (HEHN) 簇离子的形成和裂解：电喷雾电离质谱、分子动力学和反应电位表面的组合研究
硝酸2-羟乙基肼 ([HOCH 2 CH 2 NH 2 NH 2 ] + NO 3 −，HEHN）离子液体有潜力为电动和化学推进器提供动力，并提供更广泛的比冲需求。为了表征其作为电喷雾推进剂的能力，我们报告了 HEHN 簇离子在正电喷雾电离 (ESI) 中的形成及其碰撞诱导的解离。该实验是使用 ESI 引导离子束质谱仪进行的，该质谱仪在离子发射、注入真空和空间碎片方面模拟电喷雾推进器。测量包括电喷雾羽流中初级离子的组成及其各自的解离产物离子截面和阈值能量。根据理论模型解释结果。确定由 [HE + H] +和 NO组成的簇结构3 −成分、经典力学模拟用于创建初步猜测；对于离子成分之间反应形成的簇，使用准经典直接动力学轨迹模拟来模拟共价键的形成和结构。所有候选结构均经过密度泛函理论优化，从中识别出全局最小结构并用于构建反应势能面。实验值与计算的解离热力学之间的比较用于验证发射物种的结构 [(HEHN) n HE + H] +、[(HEHN) n (HE) 2 + H] +、[(HE) n + 1+ H] +和 [(HE) n C 2 H 4 OH] + ( n = 0–2)，其中 [(HE) 1–2 + H] +占主导地位。由于HEHN的质子性质，可以通过质子转移介导的HNO 3、HE和HE·HNO 3的消除来使簇破碎合理化，并且后两者在较大的簇中占主导地位。[(HE) 2 + H] +和 [(HE) n C 2 H 4 OH] +含有氢键水，因此具有碎片消除水的特点。这些发现有助于评估离子形成和碎片效率及其对电喷雾推进的影响。
更新日期：2023-06-16
中文翻译：
硝酸 2-羟乙基肼 (HEHN) 簇离子的形成和裂解：电喷雾电离质谱、分子动力学和反应电位表面的组合研究
硝酸2-羟乙基肼 ([HOCH 2 CH 2 NH 2 NH 2 ] + NO 3 −，HEHN）离子液体有潜力为电动和化学推进器提供动力，并提供更广泛的比冲需求。为了表征其作为电喷雾推进剂的能力，我们报告了 HEHN 簇离子在正电喷雾电离 (ESI) 中的形成及其碰撞诱导的解离。该实验是使用 ESI 引导离子束质谱仪进行的，该质谱仪在离子发射、注入真空和空间碎片方面模拟电喷雾推进器。测量包括电喷雾羽流中初级离子的组成及其各自的解离产物离子截面和阈值能量。根据理论模型解释结果。确定由 [HE + H] +和 NO组成的簇结构3 −成分、经典力学模拟用于创建初步猜测；对于离子成分之间反应形成的簇，使用准经典直接动力学轨迹模拟来模拟共价键的形成和结构。所有候选结构均经过密度泛函理论优化，从中识别出全局最小结构并用于构建反应势能面。实验值与计算的解离热力学之间的比较用于验证发射物种的结构 [(HEHN) n HE + H] +、[(HEHN) n (HE) 2 + H] +、[(HE) n + 1+ H] +和 [(HE) n C 2 H 4 OH] + ( n = 0–2)，其中 [(HE) 1–2 + H] +占主导地位。由于HEHN的质子性质，可以通过质子转移介导的HNO 3、HE和HE·HNO 3的消除来使簇破碎合理化，并且后两者在较大的簇中占主导地位。[(HE) 2 + H] +和 [(HE) n C 2 H 4 OH] +含有氢键水，因此具有碎片消除水的特点。这些发现有助于评估离子形成和碎片效率及其对电喷雾推进的影响。
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