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Spent FCC catalyst-derived mesocellular silica foam-based solid amine adsorbents for flue gas CO2 capture
- Low-Carbon Chemistry and Chemical Engineering Vol. 50, Issue 9, Pages: 17-26(2025)
- 作者机构：
1.中国海洋石油集团有限公司 液化天然气及低碳技术重点实验室，北京 100028
2.中国石油大学（北京） 化学工程与环境学院，北京 102249
3.中国石油大学（北京） 碳中和未来技术学院，北京 102249
4.山东石油化工学院 化学工程学院，山东 东营 257061
- 作者简介：
- 基金信息：
DOI：10.12434/j.issn.2097-2547.20240499
CLC： TQ424;TE65Received：23 December 2024，
Revised：2025-01-19，
Published：25 September 2025
- 稿件说明：
移动端阅览
明红芳,贾晓浩,陈峰等.废FCC催化剂源二氧化硅泡沫基固态胺吸附剂的烟气CO2吸附性能研究[J].低碳化学与化工,2025,50(9):17-26.
MING Hongfang,JIA Xiaohao,CHEN Feng,et al.Spent FCC catalyst-derived mesocellular silica foam-based solid amine adsorbents for flue gas CO2 capture[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(9):17-26.
明红芳,贾晓浩,陈峰等.废FCC催化剂源二氧化硅泡沫基固态胺吸附剂的烟气CO2吸附性能研究[J].低碳化学与化工,2025,50(9):17-26. DOI： 10.12434/j.issn.2097-2547.20240499.
MING Hongfang,JIA Xiaohao,CHEN Feng,et al.Spent FCC catalyst-derived mesocellular silica foam-based solid amine adsorbents for flue gas CO2 capture[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(9):17-26. DOI： 10.12434/j.issn.2097-2547.20240499.
摘要
将流化催化裂化（FCC）废催化剂作为廉价硅源，制备固态胺CO
2
吸附剂，能够实现废催化剂的高值化利用，并同时达到碳减排的双重目标，从而实现“以废治废”。首先采用碱溶法从FCC废催化剂中提取硅，制备了一系列介孔二氧化硅泡沫材料（MCF-N
x
）作为载体；随后通过聚乙烯亚胺（PEI）负载改性，制备了具有高CO
2
吸附量和优异循环稳定性的固态胺吸附剂MCF-N
x
-PEI
y
。通过调节矿化剂NH
4
F与模板剂三嵌段共聚物（P123）的质量比（
x
= 0.0113、0.0226或0.0339），优化了MCF-N
x
的孔结构。通过XRD、N
2
吸/脱附、SEM、TEM和FT-IR等表征手段分析了泡沫载体和吸附剂的结构与形貌，并考察了PEI负载量、吸附温度以及水汽对MCF-N
x
-PEI
y
在模拟烟气（10%CO
2
/90%N
2
，体积分数）中CO
2
吸附性能的影响。结果表明，当NH
4
F与P123的质量比为0.0226时，获得了最优结构的载体MCF-N0.0226，其平均孔径为10.7 nm，有利于PEI的负载。在该载体上负载质量分数50%的PEI所制备的MCF-N0.0226-PEI50表现出最佳的CO
2
吸附量。在吸附热力学与动力学的共同作用下，MCF-N0.0226-PEI50的CO
2
吸附量随着吸附温度的升高先增大后减小，在75 ℃时，达到烟气条件下的最大值3.13 mmol/g；此外，在烟气中加入水汽可显著促进CO
2
的吸附，使得CO
2
吸附量增大至6.08 mmol/g。在30次烟气吸附-解吸循环中，吸附剂的CO
2
吸附量保持稳定，展现出优异的循环稳定性。废FCC催化剂源的介孔二氧化硅泡沫载体具有三维孔道结构和高孔容，这有利于PEI的分散，同时促进了CO
2
的扩散，从而在增大CO
2
吸附量的同时显著提高了胺效率，显示出在烟气CO
2
捕集中的应用潜力。
Abstract
Utilizing spent fluid catalytic cracking (FCC) catalysts as a low-cost silicon source to prepare solid amine CO
2
adsorbents enables the high-value utilization of waste catalysts while simultaneously achieving carbon emission reduction
thereby realizing “waste against waste treatment”. First
a series of mesocellular silica foam materials (MCF-N
x
) were synthesized as supports by extracting silicon from spent FCC catalysts via an alkaline dissolution method. Subsequently
solid amine adsorbents MCF-N
x
-PEI
y
with high CO
2
adsorption capacity and excellent cyclic stability were prepared by polyethyleneimine (PEI) impregnation. The pore structure of MCF-N
x
was optimized by adjusting the mass ratio of mineralizer NH
4
F to template agent triblock copolymer (P123) (
x
= 0.0113
0.0226 or 0.0339). The structure and morphology of the foam supports and adsorbents were characterized by XRD
N
2
adsorption/desorption
SEM
TEM
and FT-IR. Furthermore
the effects of PEI loading amounts
adsorption temperatures and water vapor on the CO
2
adsorption performance of MCF-N
x
-PEI
y
in simulated flue gas (10%CO
2
/90%N
2
volume fraction) were investigated. The results show that when the mass ratio of NH
4
F and P123 is 0.0226
the optimal structural support MCF-N0.0226 is obtained
with a average pore diameter of 10.7 nm
which facilitates PEI loading. The MCF-N0.0226-PEI50
prepared by impregnating the optimal support with 50% (mass fraction) PEI
exhibits the highest CO
2
adsorption capacity. Under the combined effects of adsorption thermodynamics and kinetics
the CO
2
adsorption capacity of MCF-N0.0226-PEI50 first increases and then decreases with increasing adsorption temperature
reaching a maximum of 3.13 mmol/g at 75 ℃ under simulated flue gas conditions. Moreover
the presence of water vapor in the flue gas significantly enhances CO
2
adsorption
increasing the CO
2
adsorption capacity to 6.08 mmol/g. During 30 flue gas adsorption/desorption cycles
the CO
2
adsorption capacity of MCF-N0.0226-PEI50 remains stable
demonstrating excellent cyclic stability. The mesocellular silica foam support derived from spent FCC catalysts features a three-dimensional pore structure and high pore volume
which promote PEI dispersion and facilitate CO
2
diffusion
thereby increasing CO
2
adsorption capacity while significantly improving amine efficiency. These findings highlight the promising application potential of this material for CO
2
capture in flue gas.
关键词
Keywords
references
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