胺功能化介孔二氧化硅捕集CO2的研究进展

doi:10.16085/j.issn.1000-6613.2022-0890

摘要/Abstract

摘要：

胺功能化介孔二氧化硅因其高选择性、高吸附容量、快速的吸附动力学、良好的再生性能和循环稳定性受到广泛关注，在二氧化碳捕集技术中具有优良的应用前景。本文比较了胺改性的M41S、SBA-n、KIT-n、介孔二氧化硅泡沫、介孔二氧化硅纳米球和六方介孔二氧化硅的吸附性能，总结了MCM-41和SBA-15的结构特点。介绍了胺化合物的负载方式——湿法浸渍、化学接枝和原位聚合的胺负载原理。分析了硅源、载体内部性质、气体选择性和不同添加剂对胺功能化介孔二氧化硅材料吸附二氧化碳能力的影响。最后，点明了吸附剂未来的发展目标，对胺功能化介孔二氧化硅材料的研究方向进行了展望。指出未来可关注介孔二氧化硅微观结构和温度对胺与二氧化碳相互作用的影响，增强胺功能化介孔二氧化硅的稳定性，推进其在实际环境下的应用。

关键词: 二氧化碳捕集, 二氧化硅, 吸附（作用）, 脱附, 吸附剂

Abstract:

As to its high selectivity, high adsorption capacity, fast adsorption kinetics, good regeneration performance and cycling stability, amine-functionalized mesoporous has received much attention and has excellent prospects for application in CO₂ capture technology. In this paper, the adsorption capacity of mesoporous silica M41S, SBA-n, FDU-n, KIT-n, MCF, MSN and HMS was compared, and the structural characteristics of MCM-41 and SBA-15 are summarized. The principles of physical impregnation, covalent tethering via silane linkage and direct covalent tethering via in-situ polymerization for amine loading are presented. The effects of differences in silica source, internal material properties, other gases and additives on the adsorption capacity are analyzed. In conclusion, the future development goals of adsorbents were clarified and an outlook on the research direction of amine-functionalized mesoporous silica materials is provided. It is noted that future attention can be paid to the effect of mesoporous silica microstructure and temperature on the interaction between amine and CO₂ to enhance the stability of amine-functionalized mesoporous silica to promote its application in practical environments.

Key words: CO₂capture, silica, adsorption, desorption, adsorbents

中图分类号:

TQ028

王一茹, 宋小三, 水博阳, 王三反. 胺功能化介孔二氧化硅捕集CO₂的研究进展[J]. 化工进展, 2022, 41(S1): 536-544.

WANG Yiru, SONG Xiaosan, SHUI Boyang, WANG Sanfan. Progress in amine-functionalized mesoporous silica for CO₂ capture[J]. Chemical Industry and Engineering Progress, 2022, 41(S1): 536-544.

图/表 7

参考文献 68

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介孔 SiO₂	胺功能化（胺类别，与载体重量比）	吸附条件	吸附容量 /mmol·(gCO₂)^-1	解吸条件	循环能力（吸附容量的损失率，总循环次数）	参考文献
MCM-41	—	10%CO₂/N₂，75℃	0.66	—	—	［15］
MCM-41	TEPA，60%	12%CO₂/N₂，75℃	2.80	N₂，100℃	7.8%，5	［15］
MCM-41	PEI，50%	100%CO₂，25℃	3.53	真空，100℃	14.22%，5	［19］
MCM-48	—	100%CO₂，25℃	0.64	—	—	［20］
MCM-48	AEEA，30%	100%CO₂，25℃	3.33	—	—	［20］
SBA-15	PEI，70%	20%CO₂/N₂，75℃	3.71	—	—	［21］
SBA-15	PEI，30%+DEA，40%	20%CO₂/N₂，75℃	4.64	N₂，105℃	13.36%，15	［21］
SBA-15	TEPA，50%	400ppmCO₂/N₂，35℃	2.30	N₂，110℃	—，10	［18］
SBA-16	PEHA，30%	15%CO₂/He，70℃	2.1	He，120℃	6.2%，20	［22］
SBA-16	TEPA，30%	10%CO₂/N₂，60℃	0.97	N₂，110℃	—	［23］
KIT-6	3N +TETA，30%	15%CO₂/N₂，60℃	2.06	N₂，110℃	2.5%，20	［24］
KIT-6	APTES	100%CO₂，30℃	1.56	He，120℃	0，10	［25］
MCF	DAEAPTS，35%	15%CO₂/N₂，25℃	2.07	N₂，110℃	0，50	［26］
MSN	PEI，65%	15%CO₂/N₂，80℃	4.07	N₂，100℃	19%，5	［27］
HMS	PEI，50%	100%CO₂，45℃	2.40	—，110℃	0，4	［28］

介孔 SiO₂	胺功能化（胺类别，与载体重量比）	吸附条件	吸附容量 /mmol·(gCO₂)^-1	解吸条件	循环能力（吸附容量的损失率，总循环次数）	参考文献
MCM-41	—	10%CO₂/N₂，75℃	0.66	—	—	［15］
MCM-41	TEPA，60%	12%CO₂/N₂，75℃	2.80	N₂，100℃	7.8%，5	［15］
MCM-41	PEI，50%	100%CO₂，25℃	3.53	真空，100℃	14.22%，5	［19］
MCM-48	—	100%CO₂，25℃	0.64	—	—	［20］
MCM-48	AEEA，30%	100%CO₂，25℃	3.33	—	—	［20］
SBA-15	PEI，70%	20%CO₂/N₂，75℃	3.71	—	—	［21］
SBA-15	PEI，30%+DEA，40%	20%CO₂/N₂，75℃	4.64	N₂，105℃	13.36%，15	［21］
SBA-15	TEPA，50%	400ppmCO₂/N₂，35℃	2.30	N₂，110℃	—，10	［18］
SBA-16	PEHA，30%	15%CO₂/He，70℃	2.1	He，120℃	6.2%，20	［22］
SBA-16	TEPA，30%	10%CO₂/N₂，60℃	0.97	N₂，110℃	—	［23］
KIT-6	3N +TETA，30%	15%CO₂/N₂，60℃	2.06	N₂，110℃	2.5%，20	［24］
KIT-6	APTES	100%CO₂，30℃	1.56	He，120℃	0，10	［25］
MCF	DAEAPTS，35%	15%CO₂/N₂，25℃	2.07	N₂，110℃	0，50	［26］
MSN	PEI，65%	15%CO₂/N₂，80℃	4.07	N₂，100℃	19%，5	［27］
HMS	PEI，50%	100%CO₂，45℃	2.40	—，110℃	0，4	［28］

名称	化学式	分子量
聚乙烯亚胺（PEI）	（C₂H₅N） _n NH₃	600~5000
二乙烯三胺（DETA）	C₄H₁₃N₃	103.17
三乙烯四胺（TETA）	C₆H₁₈N₄	146.23
四乙烯五胺（TEPA）	C₈H₂₃N₅	189.30
五乙烯六胺（PEHA）	C₁₀H₂₈N₆	232.37
单乙醇胺（MEA）	C₂H₇NO	61.08
二乙醇胺（DEA）	C₄H₁₁NO₂	105.14
乙二胺（EDA）	C₂H₈N₂	60.10

名称	化学式	分子量
聚乙烯亚胺（PEI）	（C₂H₅N） _n NH₃	600~5000
二乙烯三胺（DETA）	C₄H₁₃N₃	103.17
三乙烯四胺（TETA）	C₆H₁₈N₄	146.23
四乙烯五胺（TEPA）	C₈H₂₃N₅	189.30
五乙烯六胺（PEHA）	C₁₀H₂₈N₆	232.37
单乙醇胺（MEA）	C₂H₇NO	61.08
二乙醇胺（DEA）	C₄H₁₁NO₂	105.14
乙二胺（EDA）	C₂H₈N₂	60.10

硅源	提取方法	SiO₂含量/%	结构特征			参考文献
硅源	提取方法	SiO₂含量/%	表面积/m²·g^-1	孔体积/cm³·g^-1	孔径/nm	参考文献
石英砂	NaOH提取法	99.99	1028	0.907	3.04	［44］
粉煤灰	NaOH提取法	44.41	115	0.13	3	［45］
稻壳灰	碳化法	81.72	—	—	40~50	［46］
电子废物	酸浸法	—	1033	0.887	2.73	［47］
小麦秸秆灰	NaOH提取法	90.00	1312	1.053	3.656	［48］
甘蔗渣	NaOH提取法	81.60	265	0.425	6.25	［49］
竹叶灰	NaOH提取法	83.30	1096	0.51	2.14	［50］
高岭土	NaOH提取法	60.00~61.00	637	0.682	4.3	［51］
铜尾矿	碱熔法	68.23~96.82	946.68	0.76	3.24	［52］

胺功能化介孔二氧化硅捕集CO₂的研究进展

Progress in amine-functionalized mesoporous silica for CO₂ capture

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