可商业化的金属有机框架的孔表面氟化和PDMS复合用于高湿度下C2H2/CO2高效分离
Pore surface fluorination and PDMS deposition within commercially viable metal-organic framework for efficient C2H2/CO2 separation
刘红岩 1王小康 1高飞 1王雨桐 1孙萌 1谢德禹 1陈文淼 1康子曦 1王荣明 1范卫东 1孙道峰1
作者信息
- 1. State Key Laboratory of Heavy Oil Processing,School of Materials Science and Engineering,China University of Petroleum(East China),Qingdao 266580,China
- 折叠
摘要
从C2H2/CO2混合物中去除CO2杂质是在高湿度下生产高纯度C2H2的重要过程.高稳定性和低成本的金属有机框架(MOFs)在C2H2/CO2工业分离中具有巨大的应用潜力.然而,由于H2O和CO2的竞争吸附,水蒸气会影响C2H2的吸附.因此,我们提出了一种孔表面功能化和聚二甲基硅氧烷(PDMS)沉积的协同策略,以避免水蒸气的影响,同时提高C2H2/CO2分离性能.用可商业化的金属有机骨架(ALP-MOF-1)作为模板,用CH3、Br和F对其孔表面进行官能化,最佳材料ALP-MOF-1(F)在298 K和106 Pa下表现出最高的C2H2吸附量(117.78 cm3/g)和3.1 C2H2/CO2吸附比.模拟计算表明,ALP-MOF-1(F)孔空间与C2H2匹配良好,并且氟基团显著的电负性和极化率增强了骨架与C2H2的相互作用.此外,PDMS在ALP-MOF-1上的沉积(ALP-MOF-1(F))显著提高了其在80％湿度条件下的C2H2/CO2分离稳定性.
Abstract
Removing CO2 impurities from C2H2/CO2 mixtures is an essential process for producing high-purity C2H2 under high humidity.High-stability and low-cost metal-organic frameworks(MOFs)have great potential in C2H2/CO2 industrial separation.However,due to the complementary adsorption of H2O and CO2,water vapor has a negative impact on the implementation of C2H2 purification.Herein,we pro-pose a synergistic strategy of pore surface functionalization and polydimethylsiloxane(PDMS)deposition to avoid the influence of water vapor while improving C2H2/CO2 separa-tion performance.A commercially available metal-organic framework(ALP-MOF-1)was used as a template to functio-nalize its pore surface with CH3,Br,and F.The optimized material ALP-MOF-1(F)exhibits the highest C2H2 uptake(117.78 cm3/g at 298 K and 106 Pa)and C2H2/CO2 uptake ratio(3.1)among ALP-MOF systems.Computational simulations show that the well-matched pore space and the significant electronegativity and polarizability of the fluorine groups on the pore surface jointly enhance the framework-C2H2 inter-action.Furthermore,the deposition of PDMS on ALP-MOF-1 and ALP-MOF-1(F)significantly improves their C2H2/CO2 separation stability under 80％humidity conditions.
关键词
metal-organic framework/C2H2/CO2 separation/fluorination strategy/PDMS coatingKey words
metal-organic framework/C2H2/CO2 separation/fluorination strategy/PDMS coating引用本文复制引用
出版年
2024
NETL
NSTL
万方数据