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

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

^*Corresponding author for this work

Chemistry

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

227 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 - Dec 1 2018

Bibliographical note

Publisher Copyright:
© 2018, The Author(s), under exclusive licence to Springer Nature Limited.

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
Energy Engineering and Power Technology
Fuel Technology
Renewable Energy, Sustainability and the Environment

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1038/s41560-018-0267-0

Cite this

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

note = "Publisher Copyright: {\textcopyright} 2018, The Author(s), under exclusive licence to Springer Nature Limited.",

year = "2018",

month = dec,

day = "1",

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

language = "English (US)",

volume = "3",

pages = "1059--1066",

journal = "NATURE ENERGY",

issn = "2058-7546",

publisher = "Springer Nature",

number = "12",

}

TY - JOUR

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

AU - Belmabkhout, Youssef

AU - Bhatt, Prashant M.

AU - Adil, Karim

AU - Pillai, Renjith S.

AU - Cadiau, Amandine

AU - Shkurenko, Aleksander

AU - Maurin, Guillaume

AU - Liu, Gongping

AU - Koros, William J.

AU - Eddaoudi, Mohamed

PY - 2018/12/1

Y1 - 2018/12/1

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://www.scopus.com/inward/record.url?scp=85056003652&partnerID=8YFLogxK

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

Abstract

Bibliographical note

ASJC Scopus subject areas

UN SDGs

Access to Document

Other files and links

Fingerprint

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

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)]

Cite this

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

Abstract

Bibliographical note

ASJC Scopus subject areas

UN SDGs

Access to Document

Other files and links

Fingerprint

Datasets

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

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)]

Cite this

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