文献类型：期刊文献

英文题名：Insight into thermal dissociation of tri-n-octylamine hydrochloride: The key to realizing CO2 mineralization with waste calcium/magnesium chloride liquids

作者：Dong, Chunhua[1,2];Song, Xingfu[1];Zhang, Jie[1];Meijer, Evert Jan[2];Chen, Hang[1];Yu, Jianguo[1]

机构：[1]East China Univ Sci & Technol, Natl Engn Res Ctr Integrated Utilizat Salt Lake R, Shanghai 200237, Peoples R China;[2]Univ Amsterdam, Van Hoff Inst Mol Sci, Amsterdam, Netherlands

年份：2018

卷号：6

期号：5

起止页码：437

外文期刊名：ENERGY SCIENCE & ENGINEERING

收录：;EI(收录号：20183105648872);WOS:【SCI-EXPANDED(收录号:WOS:000447757600008)】；

基金：National Key R&D Program of China, Grant/Award Number: 2018YFB0605703; National Natural Science Foundation of China, Grant/Award Number: U1607115; China Postdoctoral Science Foundation, Grant/Award Number: 2017M621387

语种：英文

外文关键词：amine regeneration; decalin; entropically driven; kinetics; solvent effects; thermal dissociation

摘要：A thermal dissociation process (ideally, 100% atom utilization) to regenerate the amine extractant and to produce gaseous HCl which is the key to realizing the CO2 mineralization with metal chloride waste liquids was investigated. Solvent effects on the thermal dissociation of tri-n-octylamine hydrochloride (TOAHCl) were predicted to be prominent via analyzing structure parameters, charge distribution, solvation free energy, apparent basicity, and N-H frequency with the help of molecular simulation and experiments. Inert solvents with low polarity such as decalin, dodecane were favorable in thermal dissociation experiments. In particular, decalin enhanced the dissociation most effectively which is in agreement with the prediction. In dilute solutions, the thermal dissociation kinetics was shown to be first order. The apparent reaction rate (3.0 x 10(-4) -1.5 x 10(-2) min(-1)) and activation energy (58.219-121.827 kJ/mol) differ a lot at 180-190 degrees C in various solvents, confirming a strong solvent effect. A two-stage reaction scheme in dilute solutions has been proposed from the experimental study. The overall process is entropically driven, with the removal of HCl into gas phase from the solvated state. The work could offer a fundamental direction for the further actual process.