Effect of pore geometry on ultra-densified hydrogen in microporous carbons

Mi Tian; Matthew J. Lennox; Alexander J. O'Malley; Alexander J. Porter; Benjamin Krüner; Svemir Rudić; Timothy J. Mays; Tina Düren; Volker Presser; Lui R. Terry; Stephane Rols; Yanan Fang; Zhili Dong; Sebastien Rochat; Valeska P. Ting

doi:10.1016/j.carbon.2020.11.063

Effect of pore geometry on ultra-densified hydrogen in microporous carbons

Mi Tian, Matthew J. Lennox, Alexander J. O'Malley, Alexander J. Porter, Benjamin Krüner, Svemir Rudić, Timothy J. Mays, Tina Düren, Volker Presser, Lui R. Terry, Stephane Rols, Yanan Fang, Zhili Dong, Sebastien Rochat, Valeska P. Ting

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

29 Citations (SciVal)

Abstract

Our investigations into molecular hydrogen (H₂) confined in microporous carbons with different pore geometries at 77 K have provided detailed information on effects of pore shape on densification of confined H₂ at pressures up to 15 MPa. We selected three materials: a disordered, phenolic resin-based activated carbon, a graphitic carbon with slit-shaped pores (titanium carbide-derived carbon), and single-walled carbon nanotubes, all with comparable pore sizes of <1 nm. We show via a combination of in situ inelastic neutron scattering studies, high-pressure H₂ adsorption measurements, and molecular modelling that both slit-shaped and cylindrical pores with a diameter of ∼0.7 nm lead to significant H₂ densification compared to bulk hydrogen under the same conditions, with only subtle differences in hydrogen packing (and hence density) due to geometric constraints. While pore geometry may play some part in influencing the diffusion kinetics and packing arrangement of hydrogen molecules in pores, pore size remains the critical factor determining hydrogen storage capacities. This confirmation of the effects of pore geometry and pore size on the confinement of molecules is essential in understanding and guiding the development and scale-up of porous adsorbents that are tailored for maximising H₂ storage capacities, in particular for sustainable energy applications.

Original language	English
Pages (from-to)	968-979
Number of pages	12
Journal	Carbon
Volume	173
Early online date	23 Nov 2020
DOIs	https://doi.org/10.1016/j.carbon.2020.11.063
Publication status	Published - 31 Mar 2021

Bibliographical note

Funding Information:
The authors acknowledge funding from the EPSRC H2FC SUPERGEN Hub (EP/E040071/1, EP/L016354/1, EP/L08365/1, EP/K021109/1, EP/J016454/1) for VPT and MT, an EPSRC Research Fellowship for VPT (EP/R01650X/1), funding from the STFC for beamtime on TOSCA (RB1410602 and RB1610401) and from the ILL (7-05-468) for beamtime on IN4. We also thank Dr Chris Goodway and Dr Mark Kibble (STFC) for user support at ISIS, and Prof. Steve Tennison at CarbonTex for the TE7 carbon beads. VP and BK thank Eduard Arzt (INM) for his continuing support. AJOM acknowledges Roger and Sue Whorrod for the funding of the Whorrod Fellowship. This research made use of the Balena High Performance Computing (HPC) Service at the University of Bath.

Keywords

Confinement
High-pressure adsorption
Hydrogen storage
Inelastic neutron scattering
Microporous carbon
Molecular dynamic simulation

ASJC Scopus subject areas

General Chemistry
General Materials Science

Access to Document

10.1016/j.carbon.2020.11.063Licence: CC BY

Cite this

@article{9d9b38413f11485ba8f83ef75783010b,

title = "Effect of pore geometry on ultra-densified hydrogen in microporous carbons",

abstract = "Our investigations into molecular hydrogen (H2) confined in microporous carbons with different pore geometries at 77 K have provided detailed information on effects of pore shape on densification of confined H2 at pressures up to 15 MPa. We selected three materials: a disordered, phenolic resin-based activated carbon, a graphitic carbon with slit-shaped pores (titanium carbide-derived carbon), and single-walled carbon nanotubes, all with comparable pore sizes of <1 nm. We show via a combination of in situ inelastic neutron scattering studies, high-pressure H2 adsorption measurements, and molecular modelling that both slit-shaped and cylindrical pores with a diameter of ∼0.7 nm lead to significant H2 densification compared to bulk hydrogen under the same conditions, with only subtle differences in hydrogen packing (and hence density) due to geometric constraints. While pore geometry may play some part in influencing the diffusion kinetics and packing arrangement of hydrogen molecules in pores, pore size remains the critical factor determining hydrogen storage capacities. This confirmation of the effects of pore geometry and pore size on the confinement of molecules is essential in understanding and guiding the development and scale-up of porous adsorbents that are tailored for maximising H2 storage capacities, in particular for sustainable energy applications.",

keywords = "Confinement, High-pressure adsorption, Hydrogen storage, Inelastic neutron scattering, Microporous carbon, Molecular dynamic simulation",

author = "Mi Tian and Lennox, {Matthew J.} and O'Malley, {Alexander J.} and Porter, {Alexander J.} and Benjamin Kr{\"u}ner and Svemir Rudi{\'c} and Mays, {Timothy J.} and Tina D{\"u}ren and Volker Presser and Terry, {Lui R.} and Stephane Rols and Yanan Fang and Zhili Dong and Sebastien Rochat and Ting, {Valeska P.}",

note = "Funding Information: The authors acknowledge funding from the EPSRC H2FC SUPERGEN Hub (EP/E040071/1, EP/L016354/1, EP/L08365/1, EP/K021109/1, EP/J016454/1) for VPT and MT, an EPSRC Research Fellowship for VPT (EP/R01650X/1), funding from the STFC for beamtime on TOSCA (RB1410602 and RB1610401) and from the ILL (7-05-468) for beamtime on IN4. We also thank Dr Chris Goodway and Dr Mark Kibble (STFC) for user support at ISIS, and Prof. Steve Tennison at CarbonTex for the TE7 carbon beads. VP and BK thank Eduard Arzt (INM) for his continuing support. AJOM acknowledges Roger and Sue Whorrod for the funding of the Whorrod Fellowship. This research made use of the Balena High Performance Computing (HPC) Service at the University of Bath. ",

year = "2021",

month = mar,

day = "31",

doi = "10.1016/j.carbon.2020.11.063",

language = "English",

volume = "173",

pages = "968--979",

journal = "Carbon",

issn = "0008-6223",

publisher = "Elsevier",

}

TY - JOUR

T1 - Effect of pore geometry on ultra-densified hydrogen in microporous carbons

AU - Tian, Mi

AU - Lennox, Matthew J.

AU - O'Malley, Alexander J.

AU - Porter, Alexander J.

AU - Krüner, Benjamin

AU - Rudić, Svemir

AU - Mays, Timothy J.

AU - Düren, Tina

AU - Presser, Volker

AU - Terry, Lui R.

AU - Rols, Stephane

AU - Fang, Yanan

AU - Dong, Zhili

AU - Rochat, Sebastien

AU - Ting, Valeska P.

N1 - Funding Information: The authors acknowledge funding from the EPSRC H2FC SUPERGEN Hub (EP/E040071/1, EP/L016354/1, EP/L08365/1, EP/K021109/1, EP/J016454/1) for VPT and MT, an EPSRC Research Fellowship for VPT (EP/R01650X/1), funding from the STFC for beamtime on TOSCA (RB1410602 and RB1610401) and from the ILL (7-05-468) for beamtime on IN4. We also thank Dr Chris Goodway and Dr Mark Kibble (STFC) for user support at ISIS, and Prof. Steve Tennison at CarbonTex for the TE7 carbon beads. VP and BK thank Eduard Arzt (INM) for his continuing support. AJOM acknowledges Roger and Sue Whorrod for the funding of the Whorrod Fellowship. This research made use of the Balena High Performance Computing (HPC) Service at the University of Bath.

PY - 2021/3/31

Y1 - 2021/3/31

N2 - Our investigations into molecular hydrogen (H2) confined in microporous carbons with different pore geometries at 77 K have provided detailed information on effects of pore shape on densification of confined H2 at pressures up to 15 MPa. We selected three materials: a disordered, phenolic resin-based activated carbon, a graphitic carbon with slit-shaped pores (titanium carbide-derived carbon), and single-walled carbon nanotubes, all with comparable pore sizes of <1 nm. We show via a combination of in situ inelastic neutron scattering studies, high-pressure H2 adsorption measurements, and molecular modelling that both slit-shaped and cylindrical pores with a diameter of ∼0.7 nm lead to significant H2 densification compared to bulk hydrogen under the same conditions, with only subtle differences in hydrogen packing (and hence density) due to geometric constraints. While pore geometry may play some part in influencing the diffusion kinetics and packing arrangement of hydrogen molecules in pores, pore size remains the critical factor determining hydrogen storage capacities. This confirmation of the effects of pore geometry and pore size on the confinement of molecules is essential in understanding and guiding the development and scale-up of porous adsorbents that are tailored for maximising H2 storage capacities, in particular for sustainable energy applications.

AB - Our investigations into molecular hydrogen (H2) confined in microporous carbons with different pore geometries at 77 K have provided detailed information on effects of pore shape on densification of confined H2 at pressures up to 15 MPa. We selected three materials: a disordered, phenolic resin-based activated carbon, a graphitic carbon with slit-shaped pores (titanium carbide-derived carbon), and single-walled carbon nanotubes, all with comparable pore sizes of <1 nm. We show via a combination of in situ inelastic neutron scattering studies, high-pressure H2 adsorption measurements, and molecular modelling that both slit-shaped and cylindrical pores with a diameter of ∼0.7 nm lead to significant H2 densification compared to bulk hydrogen under the same conditions, with only subtle differences in hydrogen packing (and hence density) due to geometric constraints. While pore geometry may play some part in influencing the diffusion kinetics and packing arrangement of hydrogen molecules in pores, pore size remains the critical factor determining hydrogen storage capacities. This confirmation of the effects of pore geometry and pore size on the confinement of molecules is essential in understanding and guiding the development and scale-up of porous adsorbents that are tailored for maximising H2 storage capacities, in particular for sustainable energy applications.

KW - Confinement

KW - High-pressure adsorption

KW - Hydrogen storage

KW - Inelastic neutron scattering

KW - Microporous carbon

KW - Molecular dynamic simulation

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U2 - 10.1016/j.carbon.2020.11.063

DO - 10.1016/j.carbon.2020.11.063

M3 - Article

AN - SCOPUS:85097563797

SN - 0008-6223

VL - 173

SP - 968

EP - 979

JO - Carbon

JF - Carbon

ER -

Effect of pore geometry on ultra-densified hydrogen in microporous carbons

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

Access to Document

Other files and links

Fingerprint

UK SUSTAINABLE HYDROGEN ENERGY CONSORTIUM CORE PROGRAMME

3Flex+ 1MP Analyser with flow degasser

High Pressure Gas Absorption Apparatus

Raman confocal microscope RENISHAM INVIA

Cite this

Effect of pore geometry on ultra-densified hydrogen in microporous carbons

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

Access to Document

Other files and links

Fingerprint

Projects

UK SUSTAINABLE HYDROGEN ENERGY CONSORTIUM CORE PROGRAMME

Equipment

3Flex+ 1MP Analyser with flow degasser

High Pressure Gas Absorption Apparatus

Raman confocal microscope RENISHAM INVIA

Cite this