Atmospheric Oxidation of Piperazine by OH has a Low Potential To Form Carcinogenic Compounds
Atmospheric Oxidation of Piperazine by OH has a Low Potential To Form Carcinogenic Compounds
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DOI：
10.1021/ez5002159
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发表时间：
2014-08
影响因子：
10.9
通讯作者：
L. Onel;M. Dryden;M. Blitz;P. Seakins
中科院分区：
文献类型：
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作者：
L. Onel;M. Dryden;M. Blitz;P. Seakins
哌嗪[HN(CH2CH2)2NH，PZ]是公认的碳捕获(CC)的有效溶剂。本文首次用脉冲激光光解-激光诱导荧光检测技术测定了PZ与OH在气相中反应的速率系数k和分支比，得到K298K为(2.38±0.28)×10~(-10)cm~3分子~(-1)S~(-1)。该反应具有负的温度依赖性，参数为KOH+Pz=(2.37±0.03)×10~(-10)(T/298)−(1.76±0.08)。高速率系数表明，大气中的气相处理将与气溶胶的吸收竞争。通过对O2/NO存在下的OH时间分布的分析，确定了从C-H和N-H中提取的分支比。结果(Rn-H=0.09±0.06)表明，PZ氧化生成致癌亚硝胺或硝胺的可能性小于基准CC溶剂一乙醇胺(MEA)的氧化。
Piperazine [HN(CH2CH2)2NH, PZ] is widely recognized as an efficient solvent for carbon capture (CC). We present the first determination of the rate coefficient, k, and the branching ratios for the reaction of OH with PZ in the gas phase using the technique of pulsed laser photolysis with detection of OH by laser-induced fluorescence giving k298 K of (2.38 ± 0.28) × 10–10 cm3 molecule–1 s–1. The reaction has a negative temperature dependence parametrized as kOH+PZ = (2.37 ± 0.03) × 10–10(T/298)−(1.76±0.08). The high rate coefficient suggests that gas phase processing in the atmosphere will compete with uptake onto aerosols. The branching ratios, abstraction from C–H versus N–H, have been determined by analysis of OH temporal profiles obtained in the presence of O2/NO. The result (rN–H = 0.09 ± 0.06) shows that the potential for forming the carcinogenic nitrosamines or nitramines from PZ oxidation is smaller than for the oxidation of the benchmark CC solvent monoethanolamine (MEA).