生物质焦油制备多级孔碳及其二氧化碳吸附性能研究
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摘要
以生物质焦油为前驱体,ZnCl_2为活化剂,通过一步简易活化制备具有发达孔隙结构的多孔碳,幵开展在CO_2吸附方面的应用研究。结果表明,产物表面N含量可达5.22wt.%,其中吡啶氮占比高达71.68%,具有孔隙率可调节和比表面积高(达827.040 m2/g)等特点。当生物质焦油与ZnCl_2质量比为1∶4,活化温度为800℃时,吸附剂表现出最佳CO_2吸附性能,其在273 K和298 K的吸附量分别为2.52 mmol/g和1.64 mmol/g,初始等量吸附热为33.84 kJ/mol,相应的CO_2对氮气选择性分别为4.2和1.9。本研究为CO_2分离和储存提供了一种原料来源广泛且兼具可再生特点的炭基吸附材料,同时也为生物质焦油资源化利用开辟了新思路。
Highly-developed porous carbon was prepared from biomass tar by using ZnCl_2 as activator in carbonization process. The results revealed high surface nitrogen content was up to 5.22 wt.%, whilst the pyridinic nitrogen accounted for nearly 71.86%. Moreover, their porosity and specific surface area can be easily tuned by controlling mass ratio of carbon source and activation agents. When applied for CO_2 adsorption, a best performance was achieved with the product prepared at800 oC and tar/ZnCl_2 ratio of 1:4, the CO_2 adsorption capacity at 273 K and 298 K were 2.52 mmol/g and 1.64 mmol/g,respectively. Additionally, the corresponding CO_2/N2 selectivity were 4.2 and 1.9, initial isosteric heat of adsorption was as high as 33.84 kJ/mol. This research enabled such hierarchically porous carbon as promising alternative absorbent for CO_2 separation and storage, and opened up a new idea for the resource utilization of biomass tar.
Highly-developed porous carbon was prepared from biomass tar by using ZnCl_2 as activator in carbonization process. The results revealed high surface nitrogen content was up to 5.22 wt.%, whilst the pyridinic nitrogen accounted for nearly 71.86%. Moreover, their porosity and specific surface area can be easily tuned by controlling mass ratio of carbon source and activation agents. When applied for CO_2 adsorption, a best performance was achieved with the product prepared at800 oC and tar/ZnCl_2 ratio of 1:4, the CO_2 adsorption capacity at 273 K and 298 K were 2.52 mmol/g and 1.64 mmol/g,respectively. Additionally, the corresponding CO_2/N2 selectivity were 4.2 and 1.9, initial isosteric heat of adsorption was as high as 33.84 kJ/mol. This research enabled such hierarchically porous carbon as promising alternative absorbent for CO_2 separation and storage, and opened up a new idea for the resource utilization of biomass tar.
引文
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[2]ZHANG Z J,YAO Z Z,XIANG S C,et al.Perspective of microporous metal-organic frameworks for CO2 capture and separation[J].Energy&environmental science,2014,7(9):2868-2899.DOI:10.1039/C4EE00143E.
[3]FRANCKE R,SCHILLE B,ROEMELT M.Homogeneously catalyzed electroreduction of carbon dioxide-methods,mechanisms,and catalysts[J].Chemical review,2018,118(9):4631-4701.DOI:10.1021/acs.chemrev.7b00459.
[4]WANG Q,LUO J Z,ZHONG Z Y,et al.CO2 capture by solid adsorbents and their applications:current status and new trends[J].Energy&environmental science,2011,4(1):42-55.DOI:10.1039/C0EE00064G.
[5]ZOU L F,SUN Y J,CHE S,et al.Porous organic polymers for post-combustion carbon capture[J].Advanced materials,2017,29(37):1700229.DOI:10.1002/adma.201700229.
[6]LI J R,SCULLEY J,ZHOU H C.Metal-organic frameworks for separations[J].Chemical review,2012,112(2):869-932.DOI:10.1021/cr200190s.
[7]ROCHELLE G T.Amine scrubbing for CO2 capture[J].Science,2009,325(5948):1652-1654.DOI:10.1126/science.1176731.
[8]LI J R,MA Y G,MCCARTHY M C,et al.Carbon dioxide capture-related gas adsorption and separation in metal-organic frameworks[J].Coordination chemistry reviews,2011,255(15/16):1791-1823.DOI:10.1016/j.ccr.2011.02.012.
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[10]SIRCAR S.Basic research needs for design of adsorptive gas separation processes[J].Industrial&engineering chemistry research,2006,45(16):5435-5448.DOI:10.1021/ie051056a.
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[14]XUE D X,CAIRNS A J,BELMABKHOUT Y,et al.Tunable rare-earth fcu-MOFs:a platform for systematic enhancement of CO2 adsorption energetics and uptake[J].Journal of the American chemical society,2013,135(20):7660-7667.DOI:10.1021/ja401429x.
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[24]邓静倩,韩家玺,杜中杰,等.三聚氰胺改性酚醛基多孔碳材料的制备及其二氧化碳吸附性能[J].北京化工大学学报(自然科学版),2018,45(5):64-71.DOI:10.13543/j.bhxbzr.2018.05.008.
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[36]DING L G,YAO B J,JIANG W L,et al.Bifunctional imidazolium-based ionic liquid decorated UiO-67 type MOF for selective CO2 adsorption and catalytic property for CO2 cycloaddition with epoxides[J].Inorganic chemistry,2017,56(4):2337-2344.DOI:10.1021/acs.inorgchem.6b03169.
[37]徐雍捷,唐云辉,仸世杰.咔唑基有机微孔聚合物的制备及其二氧化碳吸附性能研究[J].中国科技论文,2017,12(12):1434-1438.DOI:10.3969/j.issn.2095-2783.2017.12.021.
[38]BANDYOPADHYAY S,ANIL A G,JAMES A,et al.Multifunctional porous organic polymers:tuning of porosity,CO2,and H2 storage and visible-light-driven photocatalysis[J].ACS applied materials&interfaces,2016,8(41):27669-27678.DOI:10.1021/acsami.6b08331.