胺改性微介孔分子筛的制备及其CO_2吸附性能
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摘要
采用微孔沸石硅源法合成出具有微介孔复合结构的分子筛,用浸渍法将四乙烯五胺(TEPA)负载到复合分子筛上,得到一系列微/介孔复合固态胺吸附剂。采用X射线衍射(XRD)、N_2吸脱附、傅里叶变换红外光谱(FT-IR)、热重分析(TGA)等手段对吸附剂进行表征,并在固定床反应器中考察了NaOH溶液浓度、TEPA负载量、吸附温度等因素对吸附剂吸附CO_2性能的影响以及吸附剂的循环吸脱附性能。结果表明:硅铝比为50的HZSM-5经2.5mol·L~(-1)的NaOH溶液处理后水热合成的微介孔分子筛,负载40%TEPA,控制吸附温度为70℃,饱和吸附量可达到4.45mmol·g~(-1),经过10次吸脱附循环,吸附量仅下降7.6%。
The micro/mesoporous composite were obtained from micro-mesoporous zeolitic source method.Tetraethylenepentamine(TEPA)modified the composite sorbents were prepared by the impregnation method.The sorbents were characterized by XRD,nitrogen adsorption/desorption,Fourier transform infrared spectroscopy(FT-IR)and thermogravimetric analysis(TGA)techniques.The effects of the NaOH concentration,TEPA loading,adsorption temperatures on adsorption capacity of CO_2 were investigated in a fixed bed reactor.It showed that the maximum amounts of CO_2 adsorption capacity was 4.45 mmol·g~(-1) of ZSM-5/MCM-41-40%TEPA at the adsorption temperature of 70 ℃.After a ten-cycle,the CO_2 adsorption capacity decreased by 7.6%.
The micro/mesoporous composite were obtained from micro-mesoporous zeolitic source method.Tetraethylenepentamine(TEPA)modified the composite sorbents were prepared by the impregnation method.The sorbents were characterized by XRD,nitrogen adsorption/desorption,Fourier transform infrared spectroscopy(FT-IR)and thermogravimetric analysis(TGA)techniques.The effects of the NaOH concentration,TEPA loading,adsorption temperatures on adsorption capacity of CO_2 were investigated in a fixed bed reactor.It showed that the maximum amounts of CO_2 adsorption capacity was 4.45 mmol·g~(-1) of ZSM-5/MCM-41-40%TEPA at the adsorption temperature of 70 ℃.After a ten-cycle,the CO_2 adsorption capacity decreased by 7.6%.
引文
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[2]陈琳琳,王霞,郭庆杰.四乙烯五胺修饰介孔硅胶吸附CO2性能的研究[J].燃料化学学报,2015,43(1):108-115.CHEN Linlin,WANG Xia,GUO Qingjie.Study on CO2 adsorption properties of tetraethylenepentamine modified mesoporous silica gel[J].Journal of Fuel Chemistry and Technology,2015,43(1):108-115.
[3]SAMANTA A,BANDYOPADHYAY S.Absorption of carbon dioxide into aqueous solutions of piperazine activated 2-amino-2-methyl-propanol[J].Chemical Engineering Science,2009,64(6):1185-1194.
[4]YAN X L,ZHANG L,ZHANG Y,et al.Amine-modified mesocellular silica foams for CO2capture[J].Chemical Engineering Journal,2011,168(2):918-924.
[5]WANG X,GUO Q J,KONG T T.Tetraethylenepentaminemodified MCM-41/silica gel with hierarchical mesoporous structure for CO2capture[J].Chemical Engineering Journal,2015,273:472-480.
[6]孔童童,王霞,郭庆杰.新型多级微/介孔固态胺吸附剂的制备及其CO2吸附性能研究[J].燃料化学学报,2015,43(12):1489-1497.KONG Tongtong,WANG Xia,GUO Qingjie.Preparation and CO2adsorption performance of a novel hierarchical micro/mesoporous solid amine sorbent[J].Journal of Fuel Chemistry and Technology,2015,43(12):1489-1497.
[7]LIU Z L,TENG Y,ZHANG K,et al.CO2adsorption properties and thermal stability of different amine-impregnated MCM-41materials[J].Journal of Fuel Chemistry and Technology,2013,41(4):469-476.
[8]马燕辉,赵会玲,唐圣杰,等.微孔/介孔复合分子筛的合成及其对CO2的吸附性能[J].物理化学学报,2011,27(3):689-696.MA Yanhui,ZHAO Huiling,TANG Shengjie,et al.Synthesis of micro/mesoporous composites and their application as CO2 adsorbents[J].Acta Physico-Chimica Sinica,2011,27(3):689-696.
[9]WANG W,YANG X,FANG Y,et al.Preparation and performance of form-stable polyethylene glycol/silicon dioxide composites as solid-liquid phase change materials[J].Applied Energy,2009,86(2):170-174.
[10]WANG J T,CHEN H C,ZHOU H H,et al.Carbon capture using polyethylemine-loaded mesoporous carbon[J].Journal of Environmental Sciences,2013,25(1):124-132.
[11]刘新民,张学诗.MCM-41与5A分子筛二氧化碳吸附特性对比[J].青岛科技大学学报(自然科学版),2016,37(4):392-398.LIU Xinmin,ZHANG Xueshi.CO2adsorption characteristics of MCM-41and 5A molecular sieve[J].Journal of Qingdao University of Science and Technology(Natural Science Edition),2016,37(4):392-398.
[12]WANG X,CHEN L L,GUO Q J.Development of hybrid amine-functionalized MCM-41 sorbents for CO2 capture[J].Chemical Engineering Journal,2015,260:573-581.
[13]YUE M B,CHUN Y,CAO Y,et al.Novel CO2-capturer derived from the as-prepared SBA-15occluded by template[J].Advancecl Functional Materials,2006,16(13):1717-1722.
[14]史晶金,刘亚敏,陈杰,等.氨基功能化SBA-16对CO2的动态吸附特性[J].物理化学学报,2010,26(11):3023-3029.SHI Jingjin,LIU Yamin,CHEN Jie,et al.Dynamic performance of CO2adsorption with amine-modified SBA-16[J].Acta Physico-Chimica Sinica,2010,26(11):3023-3029.
[15]SU F,LU C,KUO S,et al.Adsorption of CO2 on aminefunctionalized Y-type zeolites[J].Energy Fuels,2010,24(2):1441-1448.