Sarkar Shubhra, Somani Ankit, Sander Wolfram
Lehrstuhl für Organische Chemie II, Ruhr-Universität Bochum, 44801, Bochum, Germany.
Chemistry. 2025 Jun 23;31(35):e202501150. doi: 10.1002/chem.202501150. Epub 2025 May 30.
Solvated electrons, one of the strongest reducing agents, exhibit short lifetimes in the range of pico- to milliseconds when generated photochemically or by radiolysis in solution. In contrast, solvated electrons produced using sodium metal in liquid ammonia are stable for days and have long been used in synthetic chemistry. Using sodium atoms as an electron source, we were able to trap solvated electrons in low-density amorphous (LDA) water ice matrices with lifetimes of several days and use these electrons as reducing reagents. In LDA matrices doped with benzonitrile 1, these electrons react with 1 to form the benzonitrile radical anion 2. In argon matrices, in the absence of water, only small amounts of 2 were observed after deposition, and most of the sodium and 1 remained unreacted. The yield of radical anion 2 is significantly higher in amorphous water ice than in solid argon. The photoexcitation of radical anion 2 in both argon and LDA water ice matrices resulted in a reversal of the electron transfer under back formation of benzonitrile 1. Annealing of argon matrices doped with small amounts of water containing 2 resulted in the formation of 1:1 and 2:1 hydrogen-bonded complexes between water and radical anion 2.
溶剂化电子是最强的还原剂之一,当通过光化学方法或在溶液中进行辐射分解产生时,其寿命很短,在皮秒到毫秒范围内。相比之下,在液氨中使用金属钠产生的溶剂化电子能稳定存在数天,并且长期以来一直用于合成化学。以钠原子作为电子源,我们能够将溶剂化电子捕获在低密度非晶态(LDA)水冰基质中,其寿命可达数天,并将这些电子用作还原剂。在掺杂有苯甲腈1的LDA基质中,这些电子与1反应形成苯甲腈自由基阴离子2。在氩气基质中,在没有水的情况下,沉积后仅观察到少量的2,并且大部分钠和1仍未反应。自由基阴离子2在非晶态水冰中的产率明显高于在固态氩中的产率。在氩气和LDA水冰基质中,自由基阴离子2的光激发导致在苯甲腈1的反向形成过程中电子转移发生逆转。对掺杂有少量含有2的水的氩气基质进行退火处理,导致水与自由基阴离子2之间形成1:1和2:1的氢键复合物。