Detection of the Elusive Triazane Molecule (N3 H5 ) in the Gas Phase.
Detection of the Elusive Triazane Molecule (N3 H5 ) in the Gas Phase.
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DOI：
10.1002/cphc.201500560
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发表时间：
2015-10
期刊：
影响因子：
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通讯作者：
M. Förstel;Pavlo Maksyutenko;B. Jones;B. Sun;S. Chen;A. Chang;R. Kaiser
中科院分区：
文献类型：
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作者：
M. Förstel;Pavlo Maksyutenko;B. Jones;B. Sun;S. Chen;A. Chang;R. Kaiser
我们报告了气相中三氮烷 (N3 H5 ) 的检测。三氮烷是氨 (NH3 ) 和肼 (N2 H4 ) 的高阶氮氢化物，对于理解氮原子单键链的稳定性至关重要，也是氢氮化学中潜在的关键中间体。实验结果和电子结构计算表明，三氮烷是一种稳定的分子，其氮-氮键长度比肼短几皮米，在170 K的升华温度下寿命超过6±2 μs。三氮烷是通过用高能电子照射氨冰合成的，并在升华时在气相中被检测到。 通过软真空紫外 (VUV) 光电离结合反射飞行时间质谱仪对冰进行分析。利用[D3]-氨冰的同位素替代实验通过检测其完全氘化的对应物[D5]-三氮烷(N3 D5)证实了这一鉴定。
We report the detection of triazane (N3 H5 ) in the gas phase. Triazane is a higher order nitrogen hydride of ammonia (NH3 ) and hydrazine (N2 H4 ) of fundamental importance for the understanding of the stability of single-bonded chains of nitrogen atoms and a potential key intermediate in hydrogen-nitrogen chemistry. The experimental results along with electronic-structure calculations reveal that triazane presents a stable molecule with a nitrogen-nitrogen bond length that is a few picometers shorter than that of hydrazine and has a lifetime exceeding 6±2 μs at a sublimation temperature of 170 K. Triazane was synthesized through irradiation of ammonia ice with energetic electrons and was detected in the gas phase upon sublimation of the ice through soft vacuum ultraviolet (VUV) photoionization coupled with a reflectron-time-of-flight mass spectrometer. Isotopic substitution experiments exploiting [D3 ]-ammonia ice confirmed the identification through the detection of its fully deuterated counterpart [D5 ]-triazane (N3 D5 ).