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Exclusive Recognition of CO 2 from Hydrocarbons by Aluminum Formate with Hydrogen-Confined Pore Cavities.

Authors :
Zhang Z
Deng Z
Evans HA
Mullangi D
Kang C
Peh SB
Wang Y
Brown CM
Wang J
Canepa P
Cheetham AK
Zhao D
Source :
Journal of the American Chemical Society [J Am Chem Soc] 2023 May 31; Vol. 145 (21), pp. 11643-11649. Date of Electronic Publication: 2023 May 17.
Publication Year :
2023

Abstract

Exclusive capture of carbon dioxide (CO <subscript>2</subscript> ) from hydrocarbons via adsorptive separation is an important technology in the petrochemical industry, especially for acetylene (C <subscript>2</subscript> H <subscript>2</subscript> ) production. However, the physicochemical similarities between CO <subscript>2</subscript> and C <subscript>2</subscript> H <subscript>2</subscript> hamper the development of CO <subscript>2</subscript> -preferential sorbents, and CO <subscript>2</subscript> is mainly discerned via C recognition with low efficiency. Here, we report that the ultramicroporous material Al(HCOO) <subscript>3</subscript> , ALF, can exclusively capture CO <subscript>2</subscript> from hydrocarbon mixtures, including those containing C <subscript>2</subscript> H <subscript>2</subscript> and CH <subscript>4</subscript> . ALF shows a remarkable CO <subscript>2</subscript> capacity of 86.2 cm <superscript>3</superscript> g <superscript>-1</superscript> and record-high CO <subscript>2</subscript> /C <subscript>2</subscript> H <subscript>2</subscript> and CO <subscript>2</subscript> /CH <subscript>4</subscript> uptake ratios. The inverse CO <subscript>2</subscript> /C <subscript>2</subscript> H <subscript>2</subscript> separation and exclusive CO <subscript>2</subscript> capture performance from hydrocarbons are validated via adsorption isotherms and dynamic breakthrough experiments. Notably, the hydrogen-confined pore cavities with appropriate dimensional size provide an ideal pore chemistry to specifically match CO <subscript>2</subscript> via a hydrogen bonding mechanism, with all hydrocarbons rejected. This molecular recognition mechanism is unveiled by in situ Fourier-transform infrared spectroscopy, X-ray diffraction studies, and molecular simulations.

Details

Language :
English
ISSN :
1520-5126
Volume :
145
Issue :
21
Database :
MEDLINE
Journal :
Journal of the American Chemical Society
Publication Type :
Academic Journal
Accession number :
37196352
Full Text :
https://doi.org/10.1021/jacs.3c01705