首页|TEPA改性Cu-BTC@SiO2复合气凝胶制备及其捕集CO2特性研究

TEPA改性Cu-BTC@SiO2复合气凝胶制备及其捕集CO2特性研究

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在"碳达峰、碳中和"这一国家重大战略背景下,CO2 捕集已经成为当前重大科技发展方向.固体吸附剂吸附法在CO2 的捕集过程中应用广泛,其中SiO2 气凝胶具有成本低、合成方法灵活、分离效率高、表面易修饰等优点.然而,SiO2 气凝胶材料也存在CO2/N2 吸附选择性低,CO2 吸附容量有待继续提高等缺陷.为解决上述问题,制备了一种Cu-BTC@SiO2 复合气凝胶CO2 吸附材料.首先,利用扫描电子显微镜(SEM)、傅里叶红外光谱(FTIR)和氮气吸脱附测试对材料表面化学和孔隙结构进行了系统表征.然后,通过二氧化碳吸附测试对其CO2 吸附量、选择性吸附、循环吸附进行了研究.最后,采用理论与试验研究结合的方法,对吸附剂的CO2 吸附动力学进行了研究.结果表明:Cu-BTC与SiO2 气凝胶具有结构协同作用,与Cu-BTC复合后的SiO2 气凝胶不会改变材料的Si-O-Si骨架结构,同时可以保持Cu-BTC的晶体结构不受到损坏.复合材料具有 726.431 m2/g的高比表面积,570.781 m2/g的微孔比表面积和 0.184 cm3/g的高微孔体积.负载四乙烯五胺(TEPA)后CO2吸附量高达 3.20 mmol/g,CO2/N2 选择性吸附系数为 40.8,循环 10次CO2 吸附循环,吸附容量仅下降 14%,提高了SiO2 气凝胶材料的CO2 吸附容量和吸附选择性.Avrami分数动力学模型对吸附试验结果拟合相关系数为 0.99,且Avrami指数nA为 1.9表明吸附剂对CO2 的吸附是非均质的多层吸附,既有物理吸附又有化学吸附,且以物理吸附为主.利用具有丰富微孔结构的金属有机骨架材料Cu-BTC与SiO2 气凝胶进行复合,使复合材料具有分级微/介孔结构,通过增强分子间作用力(范德华力)来增强材料对CO2 的物理吸附;使用TEPA对材料进行浸渍改性,利用有机胺和酸性气体之间的酸碱相互作用来增强材料对CO2 的化学吸附.
TEPA modification Cu-BTC@SiO2 preparation of composite aerogel and its CO2 capture characteristics
Under the dual strategic background of"carbon peaking and carbon neutrality",CO2 capture has become an important task at present.Solid adsorbent adsorption is widely used in CO2 capture process,among which SiO2 aerogel has the advantages of low cost,flex-ible synthesis method,high separation efficiency,easy surface modification,etc.However,SiO2 aerogel materials also have some defects,such as low CO2/N2 adsorption selectivity and CO2 adsorption capacity to be further improved.To address the above issues,this article has prepared a Cu-BTC@SiO2 Composite aerogel CO2 adsorption material.Firstly,the surface chemistry and pore structure were systematic-ally characterized by scanning electron microscopy(SEM),Fourier transform infrared spectroscopy(FTIR),and nitrogen adsorption and desorption tests.Then,the CO2 adsorption capacity,selective adsorption,and cyclic adsorption were studied through carbon dioxide ad-sorption testing.Finally,a combination of theoretical and experimental research was used to study the CO2 adsorption kinetics of the ad-sorbent.The results show that the SiO2 aerogel compounded with Cu BTC has a high specific surface area of 726.431 m2/g,a specific sur-face area of 570.781 m2/g,and a high microporous volume of 0.184 cm3/g.After loading tetraethylenepentamine(TEPA),the adsorption capacity of CO2 is up to 2.95 mmol/g,and the selective adsorption is 40.8,after 10 cycles of CO2 adsorption,the adsorption capacity de-creased slightly.Therefore,TEPA-modified Cu-BTC@SiO2 composite aerogels can significantly improve the CO2 adsorption perform-ance of SiO2 aerogels.The metal organic framework material Cu BTC with rich micropore structure is compounded with SiO2 aerogel,and is prepared by the sol gel method Cu-BTC@SiO2 Composite aerogel to make the composite have hierarchical micro/mesoporous structure and enhance the physical adsorption of CO2 by enhancing the intermolecular force(van der Waals force);The material is impregnated with TEPA,and the chemical adsorption of CO2 is enhanced by acid-base interaction between organic amine and acid gas.

SiO2 aerogelCu-BTCCO2 adsorptionadsorption kineticscarbon neutralization

周刚、杨思奥、王凯丽、董晓素、柳茹林、孙彪、徐翠翠

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山东科技大学安全与环境工程学院,山东青岛 266590

山东科技大学矿山灾害预防控制省部共建国家重点实验室培育基地,山东青岛 266590

SiO2气凝胶 Cu-BTC CO2吸附 吸附动力学 碳中和

国家自然科学基金面上资助项目山东省自然科学基金资助项目

52274215ZR2021QE237

2024

煤炭科学技术
煤炭科学研究总院

煤炭科学技术

CSTPCD北大核心
影响因子:2.095
ISSN:0253-2336
年,卷(期):2024.52(7)
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