Natural gas upgrading using a fluorinated MOF with tuned H2S and CO2 adsorption selectivity

Youssef Belmabkhout; Prashant Bhatt; Karim Adil; Renjith S. Pillai; Amandine Cadiau; Aleksander Shkurenko; Guillaume Maurin; Liu Gongping; William J. Koros; Mohamed Eddaoudi

doi:10.1038/s41560-018-0267-0

Natural gas upgrading using a fluorinated MOF with tuned H2S and CO2 adsorption selectivity

Youssef Belmabkhout, Prashant Bhatt, Karim Adil, Renjith S. Pillai, Amandine Cadiau, Aleksander Shkurenko, Guillaume Maurin, Liu Gongping, William J. Koros, Mohamed Eddaoudi

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168 Scopus citations

Abstract

The process used to upgrade natural gas, biogas and refinery-off-gas directly influences the cost of producing the fuel and often requires complex separation strategies and operational systems to remove contaminants such as hydrogen sulfide (H2S) and carbon dioxide (CO2). Here we report a fluorinated metal–organic framework (MOF), AlFFIVE-1-Ni, that allows simultaneous and equally selective removal of CO2 and H2S from CH4-rich streams in a single adsorption step. The simultaneous removal is possible for a wide range of H2S and CO2 compositions and concentrations of the gas feed. Pure component and mixed gas adsorption, single-crystal X-ray diffraction and molecular simulation studies were carried out to elucidate the mechanism governing the simultaneous adsorption of H2S and CO2. The results suggest that concurrent removal of CO2 and H2S is achieved via the integrated favourable sites for H2S and CO2 adsorption in a confined pore system. This approach offers the prospect of simplifying the complex schemes for removal of acid gases.

Original language	English (US)
Pages (from-to)	1059-1066
Number of pages	8
Journal	Nature Energy
Volume	3
Issue number	12
DOIs	https://doi.org/10.1038/s41560-018-0267-0
State	Published - Oct 29 2018

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10.1038/s41560-018-0267-0

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@article{5d76ac1b9a1943649733bb547b3d8811,

title = "Natural gas upgrading using a fluorinated MOF with tuned H2S and CO2 adsorption selectivity",

abstract = "The process used to upgrade natural gas, biogas and refinery-off-gas directly influences the cost of producing the fuel and often requires complex separation strategies and operational systems to remove contaminants such as hydrogen sulfide (H2S) and carbon dioxide (CO2). Here we report a fluorinated metal–organic framework (MOF), AlFFIVE-1-Ni, that allows simultaneous and equally selective removal of CO2 and H2S from CH4-rich streams in a single adsorption step. The simultaneous removal is possible for a wide range of H2S and CO2 compositions and concentrations of the gas feed. Pure component and mixed gas adsorption, single-crystal X-ray diffraction and molecular simulation studies were carried out to elucidate the mechanism governing the simultaneous adsorption of H2S and CO2. The results suggest that concurrent removal of CO2 and H2S is achieved via the integrated favourable sites for H2S and CO2 adsorption in a confined pore system. This approach offers the prospect of simplifying the complex schemes for removal of acid gases.",

author = "Youssef Belmabkhout and Prashant Bhatt and Karim Adil and Pillai, {Renjith S.} and Amandine Cadiau and Aleksander Shkurenko and Guillaume Maurin and Liu Gongping and Koros, {William J.} and Mohamed Eddaoudi",

note = "KAUST Repository Item: Exported on 2021-01-19 Acknowledged KAUST grant number(s): URF/1/2222-01, CPF-2910 Acknowledgements: Y.B., P.M.B., A.C. and M.E. thank the Aramco sponsored research fund (contract 66600024505). M.E., Y.B., G.L. and W.J.K acknowledge support from KAUST CRG Research Grant URF/1/2222-01. G.M. and M.E. acknowledge the KAUST Center Partnership Fund Program (CPF-2910). We also acknowledge support by King Abdullah University of Science and Technology. We thank S.R. Tavares for fruitful discussions on the computation work.",

year = "2018",

month = oct,

day = "29",

doi = "10.1038/s41560-018-0267-0",

language = "English (US)",

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TY - JOUR

T1 - Natural gas upgrading using a fluorinated MOF with tuned H2S and CO2 adsorption selectivity

AU - Belmabkhout, Youssef

AU - Bhatt, Prashant

AU - Adil, Karim

AU - Pillai, Renjith S.

AU - Cadiau, Amandine

AU - Shkurenko, Aleksander

AU - Maurin, Guillaume

AU - Gongping, Liu

AU - Koros, William J.

AU - Eddaoudi, Mohamed

N1 - KAUST Repository Item: Exported on 2021-01-19 Acknowledged KAUST grant number(s): URF/1/2222-01, CPF-2910 Acknowledgements: Y.B., P.M.B., A.C. and M.E. thank the Aramco sponsored research fund (contract 66600024505). M.E., Y.B., G.L. and W.J.K acknowledge support from KAUST CRG Research Grant URF/1/2222-01. G.M. and M.E. acknowledge the KAUST Center Partnership Fund Program (CPF-2910). We also acknowledge support by King Abdullah University of Science and Technology. We thank S.R. Tavares for fruitful discussions on the computation work.

PY - 2018/10/29

Y1 - 2018/10/29

N2 - The process used to upgrade natural gas, biogas and refinery-off-gas directly influences the cost of producing the fuel and often requires complex separation strategies and operational systems to remove contaminants such as hydrogen sulfide (H2S) and carbon dioxide (CO2). Here we report a fluorinated metal–organic framework (MOF), AlFFIVE-1-Ni, that allows simultaneous and equally selective removal of CO2 and H2S from CH4-rich streams in a single adsorption step. The simultaneous removal is possible for a wide range of H2S and CO2 compositions and concentrations of the gas feed. Pure component and mixed gas adsorption, single-crystal X-ray diffraction and molecular simulation studies were carried out to elucidate the mechanism governing the simultaneous adsorption of H2S and CO2. The results suggest that concurrent removal of CO2 and H2S is achieved via the integrated favourable sites for H2S and CO2 adsorption in a confined pore system. This approach offers the prospect of simplifying the complex schemes for removal of acid gases.

AB - The process used to upgrade natural gas, biogas and refinery-off-gas directly influences the cost of producing the fuel and often requires complex separation strategies and operational systems to remove contaminants such as hydrogen sulfide (H2S) and carbon dioxide (CO2). Here we report a fluorinated metal–organic framework (MOF), AlFFIVE-1-Ni, that allows simultaneous and equally selective removal of CO2 and H2S from CH4-rich streams in a single adsorption step. The simultaneous removal is possible for a wide range of H2S and CO2 compositions and concentrations of the gas feed. Pure component and mixed gas adsorption, single-crystal X-ray diffraction and molecular simulation studies were carried out to elucidate the mechanism governing the simultaneous adsorption of H2S and CO2. The results suggest that concurrent removal of CO2 and H2S is achieved via the integrated favourable sites for H2S and CO2 adsorption in a confined pore system. This approach offers the prospect of simplifying the complex schemes for removal of acid gases.

UR - http://hdl.handle.net/10754/630587

UR - https://www.nature.com/articles/s41560-018-0267-0

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U2 - 10.1038/s41560-018-0267-0

DO - 10.1038/s41560-018-0267-0

M3 - Article

AN - SCOPUS:85056003652

SN - 2058-7546

VL - 3

SP - 1059

EP - 1066

JO - Nature Energy

JF - Nature Energy

IS - 12

ER -

Natural gas upgrading using a fluorinated MOF with tuned H2S and CO2 adsorption selectivity

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CCDC 1843110: Experimental Crystal Structure Determination : catena-[(mu-fluoro)-bis(mu-pyrazine)-tetrafluoro-aluminium(iii)-nickel(ii) (hydrogen sulfide)]

CCDC 1859923: Experimental Crystal Structure Determination : catena-[(mu-fluoro)-bis(mu-pyrazine)-tetrafluoro-aluminium(iii)-nickel(ii) (carbon dioxide)]

CCDC 1843109: Experimental Crystal Structure Determination : catena-[bis(mu-pyrazine)-(mu-fluoro)-tetrakis(fluoro)-(mu-oxido)-niobium-nickel dihydrogen sulfide]

Cite this

Natural gas upgrading using a fluorinated MOF with tuned H2S and CO2 adsorption selectivity

Abstract

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Datasets

CCDC 1843110: Experimental Crystal Structure Determination : catena-[(mu-fluoro)-bis(mu-pyrazine)-tetrafluoro-aluminium(iii)-nickel(ii) (hydrogen sulfide)]

CCDC 1859923: Experimental Crystal Structure Determination : catena-[(mu-fluoro)-bis(mu-pyrazine)-tetrafluoro-aluminium(iii)-nickel(ii) (carbon dioxide)]

CCDC 1843109: Experimental Crystal Structure Determination : catena-[bis(mu-pyrazine)-(mu-fluoro)-tetrakis(fluoro)-(mu-oxido)-niobium-nickel dihydrogen sulfide]

Cite this