Stable cellulose-based carbon molecular sieve membranes with very high selectivities

被引:29
作者
Araujo, Tiago [1 ]
Andrade, Marcia [1 ]
Bernardo, Gabriel [1 ]
Mendes, Adelio [1 ]
机构
[1] Univ Porto, Fac Engn, LEPABE Lab Proc Engn Biotechnol & Energy, Rua Dr Roberto Frias, P-4200465 Porto, Portugal
关键词
Carbon molecular sieve membranes; Cellulose; Propylene; Aging; Stability; SEPARATION PERFORMANCE; CO2; SEPARATION; TEMPERATURE; GRAPHENE; DECONVOLUTION; SORPTION; DEFECTS; WATER; AIR;
D O I
10.1016/j.memsci.2021.119852
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
Carbon molecular sieve membranes (CMSMs) with a remarkable separation performance and stability were prepared from an ionic liquid regenerated cellulose precursor. Extremely high selectivities to H2 and CO2 are reported (H2/CH4 > 206 000 and CO2/CH4 > 14 600) due to the precise pore size of the produced membranes. Selectivity results >3590 are reported for the first time for the C3H6/C3H8 separation using cellulose-based CMSMs. However, after one year exposed to ambient air the permeability of these CMSMs to O2 reduced approximately 62% and the O2/N2 selectivity increased 72% due to the chemisorption of oxygen. In this work it is demonstrated that exposure to propylene can not only regenerate the aged CMSMs but, more importantly, it can passivate them in a long-lasting way. CMSMs exposed to propylene for 10 days acquired aging-resistant properties that last for more than 1 year, i.e. they preserve their separation performances after 1 year exposed to ambient air. The regeneration of these CMSMs using propylene causes an increase in the permeability to O2 and in the O2/N2 selectivity of aged CMSMs. The effect of oxygen chemisorption and the passivation and regeneration by propylene post-treatment were evaluated by adsorption isotherms, FTIR, XPS and Raman spectra. Transport properties were evaluated for O2 and N2. The propylene post-treatment reduced the fraction of oxygenated groups on the surface of the CMSM, causing the widening of the pores, changing the adsorption kinetics of the gases. The results presented in this work demonstrate the industrial attractiveness of this type of membranes for the separation of gases with high performance and stability.
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页数:10
相关论文
共 76 条
[1]  
Andrade M.R.S.d, 2019, CARBON MOL SIEVE MAT
[2]   Propane selective carbon adsorbents from phenolic resin precursor [J].
Andrade, Marcia ;
Parnell, Andrew J. ;
Bernardo, Gabriel ;
Mendes, Adelio .
MICROPOROUS AND MESOPOROUS MATERIALS, 2021, 320
[3]   Highly propylene equilibrium selective carbon molecular sieve adsorbent [J].
Andrade, Marcia ;
Relvas, Frederico ;
Mendes, Adelio .
SEPARATION AND PURIFICATION TECHNOLOGY, 2020, 245
[4]   High performing CMS adsorbent for O2/N2 separation [J].
Andrade, Marcia ;
Rodrigues, Sandra C. ;
Mendes, Adelio .
MICROPOROUS AND MESOPOROUS MATERIALS, 2020, 296
[5]  
[Anonymous], 2019, GAS SEPARATION MEMBR
[6]   Cellulose-Based Carbon Molecular Sieve Membranes for Gas Separation: A Review [J].
Araujo, Tiago ;
Bernardo, Gabriel ;
Mendes, Adelio .
MOLECULES, 2020, 25 (15)
[7]   Future directions of membrane gas separation technology [J].
Baker, RW .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2002, 41 (06) :1393-1411
[8]   Recent advances in membrane technologies for hydrogen purification [J].
Bernardo, Gabriel ;
Araujo, Tiago ;
Lopes, Telmo da Silva ;
Sousa, Jose ;
Mendes, Adelio .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2020, 45 (12) :7313-7338
[9]   Defining the challenges for C3H6/C3H8 separation using polymeric membranes [J].
Burns, RL ;
Koros, WJ .
JOURNAL OF MEMBRANE SCIENCE, 2003, 211 (02) :299-309
[10]   Carbon molecular sieve membranes from cellophane paper [J].
Campo, M. C. ;
Magalhaes, F. D. ;
Mendes, A. .
JOURNAL OF MEMBRANE SCIENCE, 2010, 350 (1-2) :180-188