Cs-RHO Goes from Worst to Best as Water Enhances Equilibrium CO2 Adsorption via Phase Change

The strong affinity of water to zeolite adsorbents has made adsorption of CO2 from humid gas mixtures such as flue gas nearly impossible under equilibrated conditions. Here, in this manuscript, we describe a unique cooperative adsorption mechanism between H2O and Cs+ cations on Cs-RHO zeolite, which...

Ausführliche Beschreibung

Bibliographische Detailangaben
Veröffentlicht in:Langmuir : the ACS journal of surfaces and colloids. - 1992. - 37(2021), 47 vom: 30. Nov., Seite 13903-13908
1. Verfasser: Xu, Le (VerfasserIn)
Weitere Verfasser: Okrut, Alexander, Tate, Gregory L, Ohnishi, Ryohji, Wu, Kun-Lin, Xie, Dan, Kulkarni, Ambarish, Takewaki, Takahiko, Monnier, John R, Katz, Alexander
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2021
Zugriff auf das übergeordnete Werk:Langmuir : the ACS journal of surfaces and colloids
Schlagworte:Journal Article
LEADER 01000naa a22002652 4500
001 NLM333299639
003 DE-627
005 20231225221357.0
007 cr uuu---uuuuu
008 231225s2021 xx |||||o 00| ||eng c
024 7 |a 10.1021/acs.langmuir.1c02430  |2 doi 
028 5 2 |a pubmed24n1110.xml 
035 |a (DE-627)NLM333299639 
035 |a (NLM)34792360 
040 |a DE-627  |b ger  |c DE-627  |e rakwb 
041 |a eng 
100 1 |a Xu, Le  |e verfasserin  |4 aut 
245 1 0 |a Cs-RHO Goes from Worst to Best as Water Enhances Equilibrium CO2 Adsorption via Phase Change 
264 1 |c 2021 
336 |a Text  |b txt  |2 rdacontent 
337 |a ƒaComputermedien  |b c  |2 rdamedia 
338 |a ƒa Online-Ressource  |b cr  |2 rdacarrier 
500 |a Date Revised 30.11.2021 
500 |a published: Print-Electronic 
500 |a Citation Status PubMed-not-MEDLINE 
520 |a The strong affinity of water to zeolite adsorbents has made adsorption of CO2 from humid gas mixtures such as flue gas nearly impossible under equilibrated conditions. Here, in this manuscript, we describe a unique cooperative adsorption mechanism between H2O and Cs+ cations on Cs-RHO zeolite, which actually facilitates the equilibrium adsorption of CO2 under humid conditions. Our data demonstrate that, at a relative humidity of 5%, Cs-RHO adsorbs 3-fold higher amounts of CO2 relative to dry conditions, at a temperature of 30 °C and CO2 pressure of 1 bar. A comparative investigation of univalent cation-exchanged RHO zeolites with H+, Li+, Na+, K+, Rb+, and Cs+ shows an increase of equilibrium CO2 adsorption under humid versus dry conditions to be unique to Cs-RHO. In situ powder X-ray diffraction indicates the appearance of a new phase with Im3̅m symmetry after H2O saturation of Cs-RHO. A mixed-cation exchanged NaCs-RHO exhibits similar phase transitions after humid CO2 adsorption; however, we found no evidence of cooperativity between Cs+ and Na+ cations in adsorption, in single-component H2O and CO2 adsorption. We hypothesize based on previous Rietveld refinements of CO2 adsorption in Cs-RHO zeolite that the observed phase change is related to solvation of extra-framework Cs+ cations by H2O. In the case of Cs-RHO, molecular modeling results suggest that hydration of these cations favors their migration from an original D8R position to S8R sites. We posit that this movement enables a trapdoor mechanism by which CO2 can interact with Cs+ at S8R sites to access the α-cage 
650 4 |a Journal Article 
700 1 |a Okrut, Alexander  |e verfasserin  |4 aut 
700 1 |a Tate, Gregory L  |e verfasserin  |4 aut 
700 1 |a Ohnishi, Ryohji  |e verfasserin  |4 aut 
700 1 |a Wu, Kun-Lin  |e verfasserin  |4 aut 
700 1 |a Xie, Dan  |e verfasserin  |4 aut 
700 1 |a Kulkarni, Ambarish  |e verfasserin  |4 aut 
700 1 |a Takewaki, Takahiko  |e verfasserin  |4 aut 
700 1 |a Monnier, John R  |e verfasserin  |4 aut 
700 1 |a Katz, Alexander  |e verfasserin  |4 aut 
773 0 8 |i Enthalten in  |t Langmuir : the ACS journal of surfaces and colloids  |d 1992  |g 37(2021), 47 vom: 30. Nov., Seite 13903-13908  |w (DE-627)NLM098181009  |x 1520-5827  |7 nnns 
773 1 8 |g volume:37  |g year:2021  |g number:47  |g day:30  |g month:11  |g pages:13903-13908 
856 4 0 |u http://dx.doi.org/10.1021/acs.langmuir.1c02430  |3 Volltext 
912 |a GBV_USEFLAG_A 
912 |a SYSFLAG_A 
912 |a GBV_NLM 
912 |a GBV_ILN_22 
912 |a GBV_ILN_350 
912 |a GBV_ILN_721 
951 |a AR 
952 |d 37  |j 2021  |e 47  |b 30  |c 11  |h 13903-13908