吸附法碳捕集固体胺吸附剂成型技术研究进展

doi:10.16085/j.issn.1000-6613.2021-2238

摘要/Abstract

摘要：

吸附法碳捕集技术是实现工业过程或大气中CO₂分离与脱除的重要途径之一，高性能吸附剂的开发是该技术的关键。固体胺吸附剂由于其优异的CO₂吸附量、选择性以及较低的再生能耗，近年来受到了广泛的关注，但用于工业的成型吸附剂仍面临机械强度低、稳定性差和胺流失严重等关键难题，难以在工业中大范围的推广应用。本文分析了固体胺成型吸附剂制备面临的主要难题，重点总结了近年来国内外吸附剂成型技术的研发进展，并对固体胺工业吸附剂的发展方向进行了展望。未来固体胺吸附法碳捕集技术的研发重点在于立足吸附反应机理和工业烟气的特性，创新成型固体胺吸附剂制备技术，提升吸附剂的CO₂吸附量、胺效率、机械与循环稳定性，研发低能耗的配套吸附工艺和核心装置。

关键词: 二氧化碳捕集, 吸附法, 固体胺吸附剂, 多孔载体, 成型技术

Abstract:

Adsorption method for CO₂ capture is an important approach to achieve CO₂ separation and removal from industrial process or atmosphere, and the development of high-performance adsorbents is the key for CO₂ capture technology. In recent years, solid amine adsorbents (SAAs) have attracted much attention due to their excellent CO₂ capture ability, high selectivity and low energy consumption. However, the shaped SAAs for industrial applications still face key problems, such as low mechanical strength, poor stability and serious amine loss, which hinder the large-scale applications in industry. In this paper, the key issues in the preparation of shaped SAAs are first analyzed. Emphatically, the research progress of shaping technologies at home and abroad is presented in recent years. The development direction of integral industrial CO₂ adsorbents is also prospected. Based on the adsorption reaction mechanism and the characteristics of industrial flue gas, the innovation of the shaping technology for industrial SAAs preparation, improvement of the CO₂ adsorption capacity, amine efficiency, mechanical and cyclic stability, and development of processes and related devices with low energy consumption are the future research directions of SAAs adsorption method for CO₂ capture technology.

Key words: CO₂ capture, adsorption method, solid amine adsorbents, porous supports, shaping technology

中图分类号:

X701

雷婷, 喻树楠, 周昶安, 宋磊, 马奎, 李子鹏, 岳海荣. 吸附法碳捕集固体胺吸附剂成型技术研究进展[J]. 化工进展, 2022, 41(12): 6213-6225.

LEI Ting, YU Shunan, ZHOU Chang’an, SONG Lei, MA Kui, LI Zipeng, YUE Hairong. Research progress on the shaping technology of solid amine adsorbents for CO₂ capture by adsorption method[J]. Chemical Industry and Engineering Progress, 2022, 41(12): 6213-6225.

图/表 12

参考文献 75

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捕集技术	吸收/吸附剂			文献
溶剂吸收法	MEA	3900	62.8	［2，23］
固体吸附法	PEI/silica	—	48.1～75.2	［23］
固体吸附法	TEPA/MCM-41	1800	29.68	［24］
固体吸附法	EB-PEI/SiO₂	22300	—	［25］
固体吸附法	amine polymers	2440～2650	—	［26］

捕集技术	吸收/吸附剂			文献
溶剂吸收法	MEA	3900	62.8	［2，23］
固体吸附法	PEI/silica	—	48.1～75.2	［23］
固体吸附法	TEPA/MCM-41	1800	29.68	［24］
固体吸附法	EB-PEI/SiO₂	22300	—	［25］
固体吸附法	amine polymers	2440～2650	—	［26］

吸附剂	载体材料	负载胺	负载量	测试条件	吸附量/mg·g^-1	文献
1	Silica CS-2129	PEI	32%（质量分数）	75℃、60kPa、60mL/min	85.8	［31］
2	γ-Al₂O₃（6.9MPa）	PEI	4.3mmol N/g	35℃、10kPa、90mL/min	26.4	［53］
3	γ-Al₂O₃（34.5MPa）	PEI	4.3mmol N/g	35℃、10kPa、90mL/min	22.0	［53］
4	PD-09024（6.9MPa）	PEI	4.3mmol N/g	35℃、10kPa、90mL/min	31.2	［53］
5	PD-09024（34.5MPa）	PEI	4.3mmol N/g	35℃、10kPa、90mL/min	28.2	［53］
6	SBA-15（6.9MPa）	PEI	4.2mmol N/g	35℃、10kPa、90mL/min	17.6	［53］
7	SBA-15（34.5MPa）	PEI	4.2mmol N/g	35℃、10kPa、90mL/min	10.6	［53］
8	γ-Al₂O₃（17.2~20.7MPa）	PEI	7.81mmol N/g	30℃、0.4Pa、60mL/min	75.2	［57］
9	Silica PD-09024	TEPA	11.5mmol N/g	25℃、10kPa、60mL/min	98.1	［56］
10	Silica PD-09024	PEI	13.2mmol N/g	25℃、10kPa、60mL/min	53.7	［56］
11	MIL-101	TEPA	3.5mmol N/g	25℃、3Pa、60mL/min	70.4	［55］
12	MIL-101	PEI	5.5mmol N/g	25℃、3Pa、60mL/min	61.6	［55］

吸附剂	载体材料	负载胺	负载量	测试条件	吸附量/mg·g^-1	文献
1	Silica CS-2129	PEI	32%（质量分数）	75℃、60kPa、60mL/min	85.8	［31］
2	γ-Al₂O₃（6.9MPa）	PEI	4.3mmol N/g	35℃、10kPa、90mL/min	26.4	［53］
3	γ-Al₂O₃（34.5MPa）	PEI	4.3mmol N/g	35℃、10kPa、90mL/min	22.0	［53］
4	PD-09024（6.9MPa）	PEI	4.3mmol N/g	35℃、10kPa、90mL/min	31.2	［53］
5	PD-09024（34.5MPa）	PEI	4.3mmol N/g	35℃、10kPa、90mL/min	28.2	［53］
6	SBA-15（6.9MPa）	PEI	4.2mmol N/g	35℃、10kPa、90mL/min	17.6	［53］
7	SBA-15（34.5MPa）	PEI	4.2mmol N/g	35℃、10kPa、90mL/min	10.6	［53］
8	γ-Al₂O₃（17.2~20.7MPa）	PEI	7.81mmol N/g	30℃、0.4Pa、60mL/min	75.2	［57］
9	Silica PD-09024	TEPA	11.5mmol N/g	25℃、10kPa、60mL/min	98.1	［56］
10	Silica PD-09024	PEI	13.2mmol N/g	25℃、10kPa、60mL/min	53.7	［56］
11	MIL-101	TEPA	3.5mmol N/g	25℃、3Pa、60mL/min	70.4	［55］
12	MIL-101	PEI	5.5mmol N/g	25℃、3Pa、60mL/min	61.6	［55］

吸附剂	载体	改性胺	负载质量分数/%	测试条件	吸附量/mg·g^-1	制备周期/d	文献
1	SiO₂整体柱	PEI	50	75℃、100kPa、70mL/min	70.84	5	［72］
2	SiO₂整体柱	TEPA	65	75℃、5kPa、30mL/min	260.00	6	［61］
3	SiO₂整体柱	PEI	60	75℃、100kPa、20mL/min	183.04	12	［62］
4	硅气凝胶	APS	—	25℃、100kPa、0.3mL/min	283.80	1	［63］
5	硅气凝胶	APS	—	25℃、100kPa、2mL/min	96.80	2	［64］
6	碳球	PEI	50	75℃、100kPa、100mL/min	163.40	6	［73］
7	聚合物气凝胶	APS	—	30℃、1kPa、300mL/min	157.08	3	［65］
8	SiO₂整体柱	TEPA	39	75℃、100kPa	171	3	［66］
9	SiO₂整体柱	PEI	50	80℃、100kPa、40mL/min	167	19	［67］
10	蜂窝式陶瓷纤维	PEI	—	75℃、10kPa、75mL/min	45.1	—	［68］
11	蜂窝式氧化铝	PEI	—	7℃、0.4Pa、90mL/min	30.8	—	［69］
12	聚丙烯聚烯烃聚合物泡沫	PEHA	—	50℃、10kPa、75mL/min	7.18cm³/g	—	［70］
13	分级多孔SiO₂	APS	—	28℃、100kPa	66.44	—	［71］
14	MCM-41载体	TEPA	70	75℃、100kPa、60mL/min	151	2	［56］
15	3D打印载体	TEPA	43	25℃、100kPa	98.1	—	［74］