Design of highly efficient adsorbents for removal of gaseous methyl iodide using tertiary amine-impregnated activated carbon: Integrated experimental and first-principles approach

Keon Ho; Hoje Chun; Hyung Chae Lee; Yunjo Lee; Seulah Lee; Hyunwook Jung; Byungchan Han; Chang Ha Lee

doi:10.1016/j.cej.2019.05.115

Design of highly efficient adsorbents for removal of gaseous methyl iodide using tertiary amine-impregnated activated carbon: Integrated experimental and first-principles approach

Keon Ho, Hoje Chun, Hyung Chae Lee, Yunjo Lee, Seulah Lee, Hyunwook Jung, Byungchan Han, Chang Ha Lee

Department of Chemical and Biomolecular Engineering

Research output: Contribution to journal › Article › peer-review

17 Citations (Scopus)

Abstract

Activated carbons (ACs) impregnated with triethylenediamine (TEDA) and quinuclidine (QD) are prepared for the removal of methyl iodide (CH₃I) gas in the event of nuclear accidents. The effect of the tertiary amine loading (1, 5, and 10 wt.%) on the adsorption capability of the ACs is evaluated under dry and humid (RH 75%) conditions. Experimental evaluation of the 'breakthrough' combined with rigorous first-principles calculations enables us to identify the fundamental mechanism underlying the superior adsorption capability of QD to TEDA for real application, especially under humid conditions. The adsorption of CH₃I by the impregnated ACs under dry conditions strongly depends on the physical properties (porosity) of the adsorbent. On the other hand, the chemical properties and the tertiary amine loading play dominant roles in CH₃I adsorption at 75% RH. In particular, this study suggests a novel mechanism of the protonation reaction, rather than the already known alkylation of tertiary amines, to capture CH₃I chemically under humid conditions. The molecular-level behavior of amines and water is a key factor for the enhanced adsorption of methyl iodide. The adsorbents developed herein can be applied to the efficient removal of radioactive methyl iodide in severe accidents.

Original language	English
Pages (from-to)	1003-1011
Number of pages	9
Journal	Chemical Engineering Journal
Volume	373
DOIs	https://doi.org/10.1016/j.cej.2019.05.115
Publication status	Published - 2019 Oct 1

Bibliographical note

Funding Information:
This work was supported by the Defense Industry Technology Center (DITC) of Korea (contract grant number UC15000ID) and the Global Frontier Program through the Global Frontier Hybrid Interface Materials (GFHIM) of National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT (Project No. 2013M3A6B1078882 ).

Publisher Copyright:
© 2019 Elsevier B.V.

All Science Journal Classification (ASJC) codes

Chemistry(all)
Environmental Chemistry
Chemical Engineering(all)
Industrial and Manufacturing Engineering

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10.1016/j.cej.2019.05.115

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title = "Design of highly efficient adsorbents for removal of gaseous methyl iodide using tertiary amine-impregnated activated carbon: Integrated experimental and first-principles approach",

abstract = "Activated carbons (ACs) impregnated with triethylenediamine (TEDA) and quinuclidine (QD) are prepared for the removal of methyl iodide (CH3I) gas in the event of nuclear accidents. The effect of the tertiary amine loading (1, 5, and 10 wt.%) on the adsorption capability of the ACs is evaluated under dry and humid (RH 75%) conditions. Experimental evaluation of the 'breakthrough' combined with rigorous first-principles calculations enables us to identify the fundamental mechanism underlying the superior adsorption capability of QD to TEDA for real application, especially under humid conditions. The adsorption of CH3I by the impregnated ACs under dry conditions strongly depends on the physical properties (porosity) of the adsorbent. On the other hand, the chemical properties and the tertiary amine loading play dominant roles in CH3I adsorption at 75% RH. In particular, this study suggests a novel mechanism of the protonation reaction, rather than the already known alkylation of tertiary amines, to capture CH3I chemically under humid conditions. The molecular-level behavior of amines and water is a key factor for the enhanced adsorption of methyl iodide. The adsorbents developed herein can be applied to the efficient removal of radioactive methyl iodide in severe accidents.",

author = "Keon Ho and Hoje Chun and Lee, {Hyung Chae} and Yunjo Lee and Seulah Lee and Hyunwook Jung and Byungchan Han and Lee, {Chang Ha}",

note = "Funding Information: This work was supported by the Defense Industry Technology Center (DITC) of Korea (contract grant number UC15000ID) and the Global Frontier Program through the Global Frontier Hybrid Interface Materials (GFHIM) of National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT (Project No. 2013M3A6B1078882 ). Publisher Copyright: {\textcopyright} 2019 Elsevier B.V.",

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doi = "10.1016/j.cej.2019.05.115",

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T2 - Integrated experimental and first-principles approach

AU - Ho, Keon

AU - Chun, Hoje

AU - Lee, Hyung Chae

AU - Lee, Yunjo

AU - Lee, Seulah

AU - Jung, Hyunwook

AU - Han, Byungchan

AU - Lee, Chang Ha

N1 - Funding Information: This work was supported by the Defense Industry Technology Center (DITC) of Korea (contract grant number UC15000ID) and the Global Frontier Program through the Global Frontier Hybrid Interface Materials (GFHIM) of National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT (Project No. 2013M3A6B1078882 ). Publisher Copyright: © 2019 Elsevier B.V.

PY - 2019/10/1

Y1 - 2019/10/1

N2 - Activated carbons (ACs) impregnated with triethylenediamine (TEDA) and quinuclidine (QD) are prepared for the removal of methyl iodide (CH3I) gas in the event of nuclear accidents. The effect of the tertiary amine loading (1, 5, and 10 wt.%) on the adsorption capability of the ACs is evaluated under dry and humid (RH 75%) conditions. Experimental evaluation of the 'breakthrough' combined with rigorous first-principles calculations enables us to identify the fundamental mechanism underlying the superior adsorption capability of QD to TEDA for real application, especially under humid conditions. The adsorption of CH3I by the impregnated ACs under dry conditions strongly depends on the physical properties (porosity) of the adsorbent. On the other hand, the chemical properties and the tertiary amine loading play dominant roles in CH3I adsorption at 75% RH. In particular, this study suggests a novel mechanism of the protonation reaction, rather than the already known alkylation of tertiary amines, to capture CH3I chemically under humid conditions. The molecular-level behavior of amines and water is a key factor for the enhanced adsorption of methyl iodide. The adsorbents developed herein can be applied to the efficient removal of radioactive methyl iodide in severe accidents.

AB - Activated carbons (ACs) impregnated with triethylenediamine (TEDA) and quinuclidine (QD) are prepared for the removal of methyl iodide (CH3I) gas in the event of nuclear accidents. The effect of the tertiary amine loading (1, 5, and 10 wt.%) on the adsorption capability of the ACs is evaluated under dry and humid (RH 75%) conditions. Experimental evaluation of the 'breakthrough' combined with rigorous first-principles calculations enables us to identify the fundamental mechanism underlying the superior adsorption capability of QD to TEDA for real application, especially under humid conditions. The adsorption of CH3I by the impregnated ACs under dry conditions strongly depends on the physical properties (porosity) of the adsorbent. On the other hand, the chemical properties and the tertiary amine loading play dominant roles in CH3I adsorption at 75% RH. In particular, this study suggests a novel mechanism of the protonation reaction, rather than the already known alkylation of tertiary amines, to capture CH3I chemically under humid conditions. The molecular-level behavior of amines and water is a key factor for the enhanced adsorption of methyl iodide. The adsorbents developed herein can be applied to the efficient removal of radioactive methyl iodide in severe accidents.

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Design of highly efficient adsorbents for removal of gaseous methyl iodide using tertiary amine-impregnated activated carbon: Integrated experimental and first-principles approach

Abstract

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