Water-Stable etb-MOFs for Methane and Carbon Dioxide Storage

Constantinos Tsangarakis; Ali Azmy; Christos Tampaxis; Nourdine Zibouche; Emmanuel Klontzas; Emmanuel Tylianakis; George E. Froudakis; Theodore Steriotis; Ioannis Spanopoulos; Pantelis N. Trikalitis

doi:10.1021/acs.inorgchem.2c04483

Water-Stable etb-MOFs for Methane and Carbon Dioxide Storage

Constantinos Tsangarakis, Ali Azmy, Christos Tampaxis, Nourdine Zibouche, Emmanuel Klontzas, Emmanuel Tylianakis, George E. Froudakis, Theodore Steriotis, Ioannis Spanopoulos, Pantelis N. Trikalitis

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

4 Citations (SciVal)

Abstract

We utilized the etb platform of MOFs for the synthesis of two new water-stable compounds based on amide functionalized trigonal tritopic organic linkers H₃BTBTB (L1), H₃BTCTB (L2) and Al³⁺ metal ions, namely, Al(L1) and Al(L2). The mesoporous Al(L1) material exhibits an impressive methane (CH₄) uptake at high pressures and ambient temperature. The corresponding values of 192 cm³ (STP) cm^-3, 0.254 g g^-1 at 100 bar, and 298 K are among the highest reported for mesoporous MOFs, while the gravimetric and volumetric working capacities (between 80 bar and 5 bar) can be well compared to the best MOFs for CH₄ storage. Furthermore, at 298 K and 50 bar, Al(L1) adsorbs 50 wt % (304 cm³ (STP) cm^-3) CO₂, values among the best recorded for CO₂ storage using porous materials. To gain insight into the mechanism accounting for the resultant enhanced CH₄ storage capacity, theoretical calculations were performed, revealing the presence of strong CH₄ adsorption sites near the amide groups. Our work demonstrates that amide functionalized mesoporous etb-MOFs can be valuable for the design of versatile coordination compounds with CH₄ and CO₂ storage capacities comparable to ultra-high surface area microporous MOFs.

Original language	English
Pages (from-to)	5496-5504
Number of pages	9
Journal	Inorganic Chemistry
Volume	62
Issue number	14
Early online date	28 Mar 2023
DOIs	https://doi.org/10.1021/acs.inorgchem.2c04483
Publication status	Published - 10 Apr 2023

Bibliographical note

Funding Information:
I.S. acknowledges financial support from ACS-PRF (65721-DNI5), acknowledgment is made to the donors of the American Chemical Society Petroleum Research Fund for support of this research. P.N.T. acknowledges the co-financial support by the European Regional Development Fund of the European Union and Greek national funds through the Operational Program Competitiveness, Entrepreneurship and Innovation, under the call RESEARCH─CREATE─INNOVATE (project code: T1EDK-00770). This work used the Isambard 2 UK National Tier-2 HPC Service operated by GW4 and the UK Met Office, and funded by EPSRC (EP/T022078/1).

ASJC Scopus subject areas

Physical and Theoretical Chemistry
Inorganic Chemistry

Access to Document

10.1021/acs.inorgchem.2c04483

Cite this

@article{cdf8994e38644b1ebf92620db71eb519,

title = "Water-Stable etb-MOFs for Methane and Carbon Dioxide Storage",

abstract = "We utilized the etb platform of MOFs for the synthesis of two new water-stable compounds based on amide functionalized trigonal tritopic organic linkers H3BTBTB (L1), H3BTCTB (L2) and Al3+ metal ions, namely, Al(L1) and Al(L2). The mesoporous Al(L1) material exhibits an impressive methane (CH4) uptake at high pressures and ambient temperature. The corresponding values of 192 cm3 (STP) cm-3, 0.254 g g-1 at 100 bar, and 298 K are among the highest reported for mesoporous MOFs, while the gravimetric and volumetric working capacities (between 80 bar and 5 bar) can be well compared to the best MOFs for CH4 storage. Furthermore, at 298 K and 50 bar, Al(L1) adsorbs 50 wt % (304 cm3 (STP) cm-3) CO2, values among the best recorded for CO2 storage using porous materials. To gain insight into the mechanism accounting for the resultant enhanced CH4 storage capacity, theoretical calculations were performed, revealing the presence of strong CH4 adsorption sites near the amide groups. Our work demonstrates that amide functionalized mesoporous etb-MOFs can be valuable for the design of versatile coordination compounds with CH4 and CO2 storage capacities comparable to ultra-high surface area microporous MOFs.",

author = "Constantinos Tsangarakis and Ali Azmy and Christos Tampaxis and Nourdine Zibouche and Emmanuel Klontzas and Emmanuel Tylianakis and Froudakis, {George E.} and Theodore Steriotis and Ioannis Spanopoulos and Trikalitis, {Pantelis N.}",

note = "Funding Information: I.S. acknowledges financial support from ACS-PRF (65721-DNI5), acknowledgment is made to the donors of the American Chemical Society Petroleum Research Fund for support of this research. P.N.T. acknowledges the co-financial support by the European Regional Development Fund of the European Union and Greek national funds through the Operational Program Competitiveness, Entrepreneurship and Innovation, under the call RESEARCH─CREATE─INNOVATE (project code: T1EDK-00770). This work used the Isambard 2 UK National Tier-2 HPC Service operated by GW4 and the UK Met Office, and funded by EPSRC (EP/T022078/1). ",

year = "2023",

month = apr,

day = "10",

doi = "10.1021/acs.inorgchem.2c04483",

language = "English",

volume = "62",

pages = "5496--5504",

journal = "Inorganic Chemistry",

issn = "0020-1669",

publisher = "American Chemical Society",

number = "14",

}

TY - JOUR

T1 - Water-Stable etb-MOFs for Methane and Carbon Dioxide Storage

AU - Tsangarakis, Constantinos

AU - Azmy, Ali

AU - Tampaxis, Christos

AU - Zibouche, Nourdine

AU - Klontzas, Emmanuel

AU - Tylianakis, Emmanuel

AU - Froudakis, George E.

AU - Steriotis, Theodore

AU - Spanopoulos, Ioannis

AU - Trikalitis, Pantelis N.

N1 - Funding Information: I.S. acknowledges financial support from ACS-PRF (65721-DNI5), acknowledgment is made to the donors of the American Chemical Society Petroleum Research Fund for support of this research. P.N.T. acknowledges the co-financial support by the European Regional Development Fund of the European Union and Greek national funds through the Operational Program Competitiveness, Entrepreneurship and Innovation, under the call RESEARCH─CREATE─INNOVATE (project code: T1EDK-00770). This work used the Isambard 2 UK National Tier-2 HPC Service operated by GW4 and the UK Met Office, and funded by EPSRC (EP/T022078/1).

PY - 2023/4/10

Y1 - 2023/4/10

N2 - We utilized the etb platform of MOFs for the synthesis of two new water-stable compounds based on amide functionalized trigonal tritopic organic linkers H3BTBTB (L1), H3BTCTB (L2) and Al3+ metal ions, namely, Al(L1) and Al(L2). The mesoporous Al(L1) material exhibits an impressive methane (CH4) uptake at high pressures and ambient temperature. The corresponding values of 192 cm3 (STP) cm-3, 0.254 g g-1 at 100 bar, and 298 K are among the highest reported for mesoporous MOFs, while the gravimetric and volumetric working capacities (between 80 bar and 5 bar) can be well compared to the best MOFs for CH4 storage. Furthermore, at 298 K and 50 bar, Al(L1) adsorbs 50 wt % (304 cm3 (STP) cm-3) CO2, values among the best recorded for CO2 storage using porous materials. To gain insight into the mechanism accounting for the resultant enhanced CH4 storage capacity, theoretical calculations were performed, revealing the presence of strong CH4 adsorption sites near the amide groups. Our work demonstrates that amide functionalized mesoporous etb-MOFs can be valuable for the design of versatile coordination compounds with CH4 and CO2 storage capacities comparable to ultra-high surface area microporous MOFs.

AB - We utilized the etb platform of MOFs for the synthesis of two new water-stable compounds based on amide functionalized trigonal tritopic organic linkers H3BTBTB (L1), H3BTCTB (L2) and Al3+ metal ions, namely, Al(L1) and Al(L2). The mesoporous Al(L1) material exhibits an impressive methane (CH4) uptake at high pressures and ambient temperature. The corresponding values of 192 cm3 (STP) cm-3, 0.254 g g-1 at 100 bar, and 298 K are among the highest reported for mesoporous MOFs, while the gravimetric and volumetric working capacities (between 80 bar and 5 bar) can be well compared to the best MOFs for CH4 storage. Furthermore, at 298 K and 50 bar, Al(L1) adsorbs 50 wt % (304 cm3 (STP) cm-3) CO2, values among the best recorded for CO2 storage using porous materials. To gain insight into the mechanism accounting for the resultant enhanced CH4 storage capacity, theoretical calculations were performed, revealing the presence of strong CH4 adsorption sites near the amide groups. Our work demonstrates that amide functionalized mesoporous etb-MOFs can be valuable for the design of versatile coordination compounds with CH4 and CO2 storage capacities comparable to ultra-high surface area microporous MOFs.

UR - http://www.scopus.com/inward/record.url?scp=85151395341&partnerID=8YFLogxK

U2 - 10.1021/acs.inorgchem.2c04483

DO - 10.1021/acs.inorgchem.2c04483

M3 - Article

C2 - 36976265

AN - SCOPUS:85151395341

SN - 0020-1669

VL - 62

SP - 5496

EP - 5504

JO - Inorganic Chemistry

JF - Inorganic Chemistry

IS - 14

ER -

Water-Stable etb-MOFs for Methane and Carbon Dioxide Storage

Abstract

Bibliographical note

ASJC Scopus subject areas

Access to Document

Other files and links

Fingerprint

Cite this