摘要
比较了9种不同配方醇胺溶液对CO_(2)的吸收解吸性能。其中,N-乙基乙醇胺(EMEA)+二乙氨基乙醇(DEEA)+哌嗪(PZ)和2-氨基-2-甲基-1,3丙二醇(AMPD)+哌嗪(PZ)+水(H_(2)O)两种溶液的吸收解吸的稳定性最佳,平均解吸率高于94.00%。本文对这两种溶液进行了144h热降解和96h氧化降解实验,结果表明热降解后的EMEA+DEEA+PZ溶液的吸收解吸性能稳定性较高,每千克溶液对CO_(2)的平均吸收量、平均解吸量略有升高,分别升高1.58L、0.35L,平均解吸率下降2.04%;而氧化降解造成每千克EMEA+DEEA+PZ溶液对CO_(2)的平均吸收量、平均解吸量分别下降0.45L、1.75L,平均解吸率下降2.25%;热降解对于AMPD+PZ+H_(2)O溶液吸收解吸性能影响较大,造成每千克该溶液对CO_(2)的平均吸收量、平均解吸量分别下降5.63L、4.03L,平均解吸率升高2.32%;在经过氧化降解之后,每千克AMPD+PZ+H_(2)O溶液对CO_(2)的平均吸收量、平均解吸量分别下降1.05L、0.70L,平均解吸率升高0.59%。液质联用分析结果表明,热降解导致EMEA浓度减小了19.67%,AMPD浓度减小了71.89%;氧化降解导致EMEA浓度减小了18.18%,AMPD浓度减小了74.53%。由此说明,EMEA+DEEA+PZ比AMPD+PZ+H_(2)O具有更佳的抗降解性能。同时,根据电喷雾质谱结果对两种溶液的热降解、氧化降解的机理进行推测,热降解中生成恶唑烷酮类物质,氧化降解则是生成酸类物质。其中,氧化降解对两种溶液都造成了负面影响,而热降解则不然。
The CO_(2)absorption and desorption performances of nine alcohol amines were compared.Among them,there were two kinds of solutions that showed the better stability of absorption-desorption performance,which contained N-ethylethanolamine(EMEA)+diethylaminoethanol(DEEA)+piperazine(PZ)and 2-amino-2-methyl-1,3-propanediol(AMPD)+piperazine(PZ)+H_(2)O.The average desorption rate of the solvents were above 94.0%after two cyclic tests.The solutions were subjected to thermal degradation for 144h and oxidative degradation for 96h.It was found that the absorption-desorption performance of EMEA+DEEA+PZ solution after thermal degradation was stable.The average absorption amount and desorption amount of the solution increased slightly by 1.58L CO_(2)/kg solution and 0.35L CO_(2)/kg solution,respectively,and the average desorption rate decreased by 2.0%.While oxidative degradation caused the average absorption amount and desorption amount of the solution to decrease by 0.45L CO_(2)/kg solution and 1.75L CO_(2)/kg solution,respectively,and the average desorption rate decreased by 2.3%.The thermal degradation had a distinct impact on the absorption-desorption performance of AMPD+PZ+H_(2)O solution,which caused a decrease in the average absorption amount and desorption amount of the solution by 5.63L CO_(2)/kg solution and 4.03L CO_(2)/kg solution,respectively,and the average desorption rate increased by 2.3%.After oxidative degradation,the average absorption amount and desorption amount of the solution decreased by 1.05L CO_(2)/kg solution and 0.70L CO_(2)/kg solution,respectively,and the average desorption rate increased by 0.6%.The liquid mass spectrometry analysis showed that the concentrations of EMEA and AMPD decreased by 19.7%and 71.8%due to thermal degradation,18.2%and 74.5%due to oxidative degradation,respectively.The thermal and oxidative degradation experiments demonstrated that EMEA+DEEA+PZ had the better anti-degradation performance than AMPD+PZ+H_(2)O.The mechanisms of thermal and oxidative degradation of the two kinds of alcohol amines were speculated based on the results of electrospray mass spectrometry,in which oxazolidinones were generated in thermal degradation and acids were generated in oxidative degradation.In both cases,oxidative degradation had negative effects on both solutions,while thermal degradation did not.
作者
李红
吉轲
齐天勤机
李晓静
万慧慧
张永春
陈绍云
LI Hong;JI Ke;QI Tianqinji;LI Xiaojing;WAN Huihui;ZHANG Yongchun;CHEN Shaoyun(State Key Laboratory of Fine Chemistry,School of Chemical Engineering,Dalian University of Technology,Dalian 116024,Liaoning,China;Luoyang Research Institute of Dalian University of Technology,Luoyang 471000,Henan,China)
出处
《化工进展》
EI
CAS
CSCD
北大核心
2022年第2期1025-1035,共11页
Chemical Industry and Engineering Progress
基金
国家重点研发计划(2017YFB0603301)。
关键词
醇胺
二氧化碳捕集
吸收
解吸
降解
alcohol amines
CO_(2)capture
absorption
desorption
degradation
作者简介
第一作者:李红(1997—),女,硕士研究生,研究方向为二氧化碳捕集。E-mail:lh970715@hotmail.com。;通信作者:陈绍云,高级工程师,研究方向为二氧化碳捕集与提纯。E-mail:chensy@dlut.edu.cn。
