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Influence of formaldehyde on N-nitrosopiperazine formation from nitrite and piperazine in CO2 capture
International Journal of Greenhouse Gas Control ( IF 4.6 ) Pub Date : 2017-12-27 , DOI: 10.1016/j.ijggc.2017.12.013
Yan Zhou , Yiheng Rao , Tielin Wang , Klaus-J. Jens

Piperazine (PZ) based amine blends are promising solvents for post-combustion CO2 capture, but PZ can form potential carcinogenic nitrosamines from nitrite. In this work, the kinetics of the reaction between nitrite and PZ to form N-nitrosopiperazine (MNPZ) was determined in 0.1–0.5 mol L−1 PZ in the presence of 17–170 mmol L−1 formaldehyde at 60–135 °C. The nitrosation of PZ can be catalyzed by formaldehyde, a primary degradation product of PZ. And the reaction involving nitrite and PZ is first order in nitrite, formaldehyde, and hydronium ion. A kinetic model was established, and the activation energy is 33.6 ± 1.8 kJ mol−1 with a rate constant of 2.3 × 103 ± 0.4 × 103 L2 mol−2 s−1 at 100 °C. The kinetics will be helpful to develop strategies to reduce nitrosamine formation and accumulation in PZ based CO2 capture systems.



中文翻译:

甲醛对CO 2捕集中亚硝酸盐和哌嗪形成N-亚硝基哌嗪的影响

基于哌嗪(PZ)的胺混合物是燃烧后捕获CO 2的有前途的溶剂,但PZ可以从亚硝酸盐形成潜在的致癌亚硝胺。在这项工作中,在60–135°C下存在17–170 mmol L -1甲醛的条件下,在0.1–0.5 mol L -1 PZ中测定亚硝酸盐与PZ之间形成N-亚硝基哌嗪(MNPZ)的反应动力学。。PZ的亚硝基化可以通过甲醛(PZ的主要降解产物)进行催化。涉及亚硝酸盐和PZ的反应是亚硝酸盐,甲醛和水合氢离子的一级反应。建立了动力学模型,活化能为33.6±1.8 kJ mol -1,速率常数为2.3×10 3  ±0.4×10 3 L在100°C下为2  mol -2  s -1。动力学将有助于开发策略,以减少基于PZ的CO 2捕集系统中亚硝胺的形成和积累。

更新日期:2017-12-27
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