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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Picosecond Pulse Radiolysis of Highly Concentrated Sulfuric Acid Solutions: Evidence for the Oxidation Reactivity of Radical Cation H_2O?+
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Picosecond Pulse Radiolysis of Highly Concentrated Sulfuric Acid Solutions: Evidence for the Oxidation Reactivity of Radical Cation H_2O?+

机译：皮秒脉冲高浓度硫酸溶液的放射裂解：自由基阳离子H_2O？+的氧化反应性的证据

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摘要

Aqueous solution of sulfuric acid is used as a suitable system to investigate the reactivity of the short-lived radical cation H_2O~(?+) which is generated by radiation in water. Ten aqueous solutions containing sulfuric acid with concentration from 1 to 18 mol L~(?1) are studied by picosecond pulse radiolysis. The absorbance of the secondary radical SO_4~(??) (or HSO_4~?) formed within the 10 ps electron pulse is measured by a pulse?probe method in the visible range. The analysis of the kinetics show that the radicals of sulfuric acid are formed within the picosecond electron pulse via two parallel mechanisms: direct electron detachment by the electron pulse and oxidation by the radical cation of water H_2O~(?+). In highly concentrated solution when SO_4~(2?) is in contact with H_2O~(?+), the electron transfer becomes competitive against proton transfer with another water molecule. Therefore, H_2O~(?+) may act as an extremely strong oxidant. The maximum radiolytic yield of scavenged H_2O~(?+) is estimated to be 5.3 ± 0.1 × 10~(?7) mol J~(?1).
机译：硫酸水溶液用作研究在水中辐射产生的短寿命自由基阳离子H_2O〜（α+）的反应性的合适系统。通过皮秒脉冲辐射分解研究了十种浓度为1至18 mol L〜（？1）的硫酸水溶液。通过脉冲探针法在可见光范围内测量在10 ps电子脉冲内形成的次级自由基SO_4〜（??）（或HSO_4〜）的吸光度。动力学分析表明，在皮秒电子脉冲中，硫酸的自由基是通过两种平行的机制形成的：通过电子脉冲使电子直接脱离，并通过水H_2O〜（α+）的自由基阳离子进行氧化。在SO_4〜（2？）与H_2O〜（？+）接触的高浓度溶液中，电子转移变得竞争于与另一水分子的质子转移。因此，H_2O〜（α+）可以作为极强的氧化剂。清除的H_2O〜（α+）的最大放射解产率估计为5.3±0.1×10〜（？7）mol J〜（？1）。

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