低碳化学与化工2025，Vol.50Issue(9)：17-26,10.DOI:10.12434/j.issn.2097-2547.20240499
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
Spent FCC catalyst-derived mesocellular silica foam-based solid amine adsorbents for flue gas CO2 capture
摘要
Abstract
Utilizing spent fluid catalytic cracking(FCC)catalysts as a low-cost silicon source to prepare solid amine CO2 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-Nx)were synthesized as supports by extracting silicon from spent FCC catalysts via an alkaline dissolution method.Subsequently,solid amine adsorbents MCF-Nx-PEIy with high CO2 adsorption capacity and excellent cyclic stability were prepared by polyethyleneimine(PEI)impregnation.The pore structure of MCF-Nx was optimized by adjusting the mass ratio of mineralizer NH4F 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,N2 adsorption/desorption,SEM,TEM,and FT-IR.Furthermore,the effects of PEI loading amounts,adsorption temperatures and water vapor on the CO2 adsorption performance of MCF-Nx-PEIy in simulated flue gas(10%CO2/90%N2,volume fraction)were investigated.The results show that when the mass ratio of NH4F 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 CO2 adsorption capacity.Under the combined effects of adsorption thermodynamics and kinetics,the CO2 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 CO2 adsorption,increasing the CO2 adsorption capacity to 6.08 mmol/g.During 30 flue gas adsorption/desorption cycles,the CO2 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 CO2 diffusion,thereby increasing CO2 adsorption capacity while significantly improving amine efficiency.These findings highlight the promising application potential of this material for CO2 capture in flue gas.关键词
废FCC催化剂/聚乙烯亚胺/介孔二氧化硅泡沫/固态胺/烟气CO2捕集Key words
spent FCC catalysts/polyethyleneimine/mesocellular silica foam/solid amine/flue gas CO2 capture分类
化学化工引用本文复制引用
明红芳,贾晓浩,陈峰,郭鹏辉,杨培恒,秦锋,樊燕芳,刘梦溪..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):17-26,10.基金项目
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主任基金(KJQZ-2024-1105). （KJQZ-2024-1105）
