Bimolecular reactions of CH2CN2+ with Ar, N2 and CO: reactivity and dynamics.
Bimolecular reactions of CH2CN2+ with Ar, N2 and CO: reactivity and dynamics.
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CH2CN2 与 Ar、N2 和 CO 的双分子反应：反应性和动力学。
DOI：
10.1039/d2cp01523d
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发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Armenta Butt S
中科院分区：
文献类型：
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作者：
Armenta Butt S
采用位置敏感符合方法研究了ch2cn2 +与三种中性物质（Ar、n2和CO）在4.3 ~ 5.0 eV的质心碰撞能量下的反应活性、能量学和动力学。这是第一次对涉及ch2cn2 +的双分子反应进行研究，ch2cn2 +是一种与包括泰坦在内的行星和卫星的电离层有关的物质。所研究的所有碰撞体系都显示出两个碰撞诱导解离（CID）通道，导致形成c++ ch2n +和h++ h2n +。在n2和CO体系中发现了涉及CID产物h2cn +进一步解离形成H+ CCN+的通道的证据。质子从阳离子到中性的转移在这三种体系中都是通过直接机制发生的。此外，ch2cn2 +与n2和CO碰撞后的单电子转移产生了产物通道，但有趣的是，与Ar碰撞后没有电子转移。ch2cn2 +的最低能量电子态的电子结构计算揭示了6个局部几何最小值：循环、线性（ch2cn）和线性异氰化物（ch2nc）分子几何的双重态和四重自旋态。确定了最低能电子态为循环的重态。碰撞诱导解离产生的C+离子表明，[ch2cn] 2+束中存在环状或线性异氰化物的构型。
The reactivity, energetics and dynamics of bimolecular reactions between CH 2 CN 2+ and three neutral species (Ar, N 2 and CO) have been studied using a position sensitive coincidence methodology at centre-of-mass collision energies of 4.3-5.0 eV. This is the first study of bimolecular reactions involving CH 2 CN 2+, a species relevant to the ionospheres of planets and satellites, including Titan. All of the collision systems investigated display two collision-induced dissociation (CID) channels, resulting in the formation of C++ CH 2 N+ and H++ HC 2 N+. Evidence for channels involving further dissociation of the CID product HC 2 N+, forming H+ CCN+, were detected in the N 2 and CO systems. Proton-transfer from the dication to the neutral species occurs in all three of the systems via a direct mechanism. Additionally, there are product channels resulting from single electron transfer following collisions of CH 2 CN 2+ with both N 2 and CO, but interestingly no electron transfer following collisions with Ar. Electronic structure calculations of the lowest energy electronic states of CH 2 CN 2+ reveal six local geometric minima: both doublet and quartet spin states for cyclic, linear (CH 2 CN), and linear isocyanide (CH 2 NC) molecular geometries. The lowest energy electronic state was determined to be the doublet state of the cyclic dication. The ready generation of C+ ions by collision-induced dissociation suggests that the cyclic or linear isocyanide dication geometries are present in the [CH 2 CN] 2+ beam.