洁净煤技术2024,Vol.30Issue(10) :77-87.DOI:10.13226/j.issn.1006-6772.CCUS24043002

用于高效稳定吸附CO2的胺基功能化MOF-808开发及机理

Development and mechanism of amine-functionalized MOF-808 for efficient and stable CO2 adsorption

沈遥 鲁恒霞 潘幸迪 叶杰旭 赵景开 张士汉
洁净煤技术2024,Vol.30Issue(10) :77-87.DOI:10.13226/j.issn.1006-6772.CCUS24043002

用于高效稳定吸附CO2的胺基功能化MOF-808开发及机理

Development and mechanism of amine-functionalized MOF-808 for efficient and stable CO2 adsorption

沈遥 1鲁恒霞 2潘幸迪 2叶杰旭 1赵景开 1张士汉1
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作者信息

  • 1. 浙江工业大学能源与碳中和科教融合学院,浙江 杭州 310014;浙江工业大学环境学院,浙江 杭州 310014
  • 2. 浙江工业大学环境学院,浙江 杭州 310014
  • 折叠

摘要

胺基功能化金属有机骨架具有孔隙率高、CO2吸附容量大、抗水性好的优点,被认为是适用于燃煤烟气CO2捕集的吸附材料,但其表面胺基分子在高温脱附过程易发生团聚,导致吸附速率和吸附容量下降.采用物理浸渍将四乙烯五胺分子(TEPA)封装入MOF-808的孔道内,开发了一种胺基分子高度分散的胺基功能化吸附材料TEPA@MOF-808.TEPA@MOF-808的吸附容量相比MOF-808提高了 2.15倍,吸附速率常数、吸附选择性分别提高了 13%和498%,10次吸脱附循环后吸附容量仅下降10.9%,说明基于TEPA的胺基功能化策略可显著提高CO2吸附性能和稳定性.热力学结果显示TEPA@MOF-808的等量吸附热仅为40 kJ/mol,小于普遍认为的化学吸附门槛,13C固体核磁和原位红外表征结果进一步揭示了其以物理吸附为主的吸附机理.

Abstract

The amine-functionalized metal-organic frameworks are regarded as promising adsorbents for capturing CO2 from coal-fired flue gas due to their high porosity,large CO2 adsorption capacity,and good water resistance.However,the aggregation of surface amine molecules during high-temperature desorption processes leads to a drop in both adsorption rate and uptake.In this study,a novel amine-functionalized adsorbent was developed by physically encapsulating tetraethylenepentamine molecules into the pores of MOF-808(TEPA@MOF-808)through a simple impregnation method.Compared to pristine MOF-808,TEPA@MOF-808 exhibited a 2.15-fold increase in CO2 adsorption uptake,along with enhancements of 13%in adsorption rate constant and 498%in adsorption selectivity.After 10 cycles,its adsorption uptake only decreased by 10.9%.Thermodynamic analysis revealed a low heat of adsorption of 40 kJ/mol,suggesting a physical adsorption mechanism.13C SSNMR and in situ DRIFTS characterization further elucidated the CO2 physisorption mechanism of TEPA@MOF-808.

关键词

碳捕集/CO2吸附/胺基功能化金属有机骨架/吸附动力学

Key words

carbon capture/CO2 adsorption/amine-functionalization/adsorption kinetic

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基金项目

浙江省科技计划资助项目(2023C03156)

国家自然科学基金资助项目(U23A20677)

国家自然科学基金资助项目(22022610)

国家自然科学基金资助项目(52400137)

中国博士后科学基金资助项目(2024T170805)

中国博士后科学基金资助项目(GZC20232363)

出版年

2024
洁净煤技术
煤炭科学研究总院 煤炭工业洁净煤工程技术研究中心

洁净煤技术

CSTPCDCSCD北大核心
影响因子:0.893
ISSN:1006-6772
参考文献量40
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