单重态氧的气固化学反应发生体系的热力学分析
Thermodynamic analysis on gas-solid reaction systems for singlet oxygen generation
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摘要: 采用Gaussian程序软件包，在RHF/Lanl2dz计算水平上，计算了由4类无机固体反应物(包括碱金属的过氧化物或超氧化物、碱土金属的过氧化物或超氧化物)与3类气体反应物(包括卤素气体、卤化氢气体和卤化氘气体)所组合的12种可产生单重态氧(O2(1Δg))的气固化学反应体系的热力学参数(如反应焓变、Gibbs反应自由能变化值以及化学反应平衡常数)。计算结果结合O2(1Δg)在氧碘化学激光器(COIL)中的实际应用，分析比较了不同固体反应物和不同气体反应物对气固化学反应体系产生O2(1Δg)的影响。分析结果表明：大部分的上述气固化学反应体系的Gibbs反应自由能变化值为负值，反应可自发进行；但在所有的气固化学反应体系组合中，由碱金属超氧化物与F2或Cl2组成的气固化学反应体系的反应生成热是比较少的，这有利于气固化学反应体系产生的O2(1Δg)用于COIL中。分析同时表明由碱金属超氧化物(如LiO2，NaO2或KO2)与卤素气体(如F2或Cl2)所组成的气固化学反应体系能更高效地产生O2(1Δg)，较适合用于COIL中。Abstract: The thermodynamic quantities (such as the enthalpies of reaction, ΔHr, the Gibbs free energies of reaction, ΔGr and the constant of chemical reaction equilibrium, K) of the gas-solid reaction systems for singlet oxygen generation were calculated through the Gaussian 03 program in the level of RHF/Lanl2dz. The gas-solid reaction systems were made up of four possible solid reactants (alkali metal or alkaline earth metal peroxides or superoxides) with three possible gas reactants (the possible halogen gas or hydrogen (deuterium) halide gas). The effects of different solid reactants and gas reactants on the thermodynamic quantities of the gas-solid reaction system for singlet oxygen generation were compared and analyzed. The calculations showed that most of the gas-solid reaction systems hav
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Key words:
- coil /
- singlet oxygen /
- peroxides /
- superoxides /
- gas-solid reaction /
- thermodynamics
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