Co-pelletization of a zirconium-based metal-organic framework (UiO-66) with polymer nanofibers for improved useable capacity in hydrogen storage

Sonwabo E. Bambalaza; Henrietta W. Langmi; Robert Mokaya; Nicholas M. Musyoka; Lindiwe E. Khotseng

doi:10.1016/j.ijhydene.2020.12.049

Co-pelletization of a zirconium-based metal-organic framework (UiO-66) with polymer nanofibers for improved useable capacity in hydrogen storage

Sonwabo E. Bambalaza, Henrietta W. Langmi, Robert Mokaya, Nicholas M. Musyoka, Lindiwe E. Khotseng

Research output: Journal Publication › Article › peer-review

16 Citations (Scopus)

Abstract

We report on a concept of co-pelletization using mechanically robust hydroxylated UiO-66 to develop a metal-organic framework (MOF) monolith that contains 5 wt% electrospun polymer nanofibers, and consists of an architecture with alternating layers of MOF and nanofiber mats. The polymers of choice were the microporous Polymer of Intrinsic Microporosity (PIM-1) and non-porous polyacrylonitrile (PAN). Co-pelletized UiO-66/PIM-1 and UiO-66/PAN monoliths retain no less than 85% of the porosity obtained in pristine powder and pelletized UiO-66. The composition of the pore size distribution in co-pelletized UiO-66/PIM-1 and UiO-66/PAN monoliths is significantly different to that of pristine UiO-66 forms, with pristine UiO-66 forms showing 90% of the pore apertures in the micropore region and both UiO-66/nanofiber monoliths showing a composite micro-mesoporous pore size distribution. The co-pelletized UiO-66/nanofiber monoliths obtained improved useable H₂ capacities in comparison to pristine UiO-66 forms, under isothermal pressure swing conditions. The UiO-66/PIM-1 monolith constitutes the highest gravimetric (and volumetric) useable capacities at 2.3 wt% (32 g L⁻¹) in comparison to 1.8 wt% (12 g L⁻¹) and 1.9 wt% (29 g L⁻¹) obtainable in pristine UiO-66 powder and UiO-66 pellet, respectively. The co-pelletized UiO-66/PAN monolith, however, shows a significantly reduced surface area by up to 50% less in comparison to pristine UiO-66, but its pore volume only 13% less in comparison to pristine UiO-66. As a result, total gravimetric H₂ capacity of the co-pelletized UiO-66/PAN monolith is 50% less in comparison to that of pristine UiO-66, but crucially the useable volumetric H₂ capacity is 50% higher for the UiO-66/PAN monolith in comparison to pristine UiO-66 powder. The co-pelletization strategy provides a simple method for generating hierarchical porosity into an initially highly microporous MOF without changing the structure of the MOF through complex chemical modifications. The UiO-66/nanofiber monoliths offer improvements to the typically low H₂ useable capacities in highly microporous MOFs, and open new opportunities towards achieving system-level H₂ storage targets.

Original language	English
Pages (from-to)	8607-8620
Number of pages	14
Journal	International Journal of Hydrogen Energy
Volume	46
Issue number	12
DOIs	https://doi.org/10.1016/j.ijhydene.2020.12.049
Publication status	Published - 16 Feb 2021
Externally published	Yes

Keywords

Co-pelletization
Hierarchical porosity
Hydrogen useable capacity
Metal-organic framework
UiO-66

ASJC Scopus subject areas

Renewable Energy, Sustainability and the Environment
Fuel Technology
Condensed Matter Physics
Energy Engineering and Power Technology

UN SDGs

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

Access to Document

10.1016/j.ijhydene.2020.12.049

Cite this

@article{56542dfa04ec48599cdc068b6fd2a23f,

title = "Co-pelletization of a zirconium-based metal-organic framework (UiO-66) with polymer nanofibers for improved useable capacity in hydrogen storage",

abstract = "We report on a concept of co-pelletization using mechanically robust hydroxylated UiO-66 to develop a metal-organic framework (MOF) monolith that contains 5 wt% electrospun polymer nanofibers, and consists of an architecture with alternating layers of MOF and nanofiber mats. The polymers of choice were the microporous Polymer of Intrinsic Microporosity (PIM-1) and non-porous polyacrylonitrile (PAN). Co-pelletized UiO-66/PIM-1 and UiO-66/PAN monoliths retain no less than 85% of the porosity obtained in pristine powder and pelletized UiO-66. The composition of the pore size distribution in co-pelletized UiO-66/PIM-1 and UiO-66/PAN monoliths is significantly different to that of pristine UiO-66 forms, with pristine UiO-66 forms showing 90% of the pore apertures in the micropore region and both UiO-66/nanofiber monoliths showing a composite micro-mesoporous pore size distribution. The co-pelletized UiO-66/nanofiber monoliths obtained improved useable H2 capacities in comparison to pristine UiO-66 forms, under isothermal pressure swing conditions. The UiO-66/PIM-1 monolith constitutes the highest gravimetric (and volumetric) useable capacities at 2.3 wt% (32 g L−1) in comparison to 1.8 wt% (12 g L−1) and 1.9 wt% (29 g L−1) obtainable in pristine UiO-66 powder and UiO-66 pellet, respectively. The co-pelletized UiO-66/PAN monolith, however, shows a significantly reduced surface area by up to 50% less in comparison to pristine UiO-66, but its pore volume only 13% less in comparison to pristine UiO-66. As a result, total gravimetric H2 capacity of the co-pelletized UiO-66/PAN monolith is 50% less in comparison to that of pristine UiO-66, but crucially the useable volumetric H2 capacity is 50% higher for the UiO-66/PAN monolith in comparison to pristine UiO-66 powder. The co-pelletization strategy provides a simple method for generating hierarchical porosity into an initially highly microporous MOF without changing the structure of the MOF through complex chemical modifications. The UiO-66/nanofiber monoliths offer improvements to the typically low H2 useable capacities in highly microporous MOFs, and open new opportunities towards achieving system-level H2 storage targets.",

keywords = "Co-pelletization, Hierarchical porosity, Hydrogen useable capacity, Metal-organic framework, UiO-66",

author = "Bambalaza, {Sonwabo E.} and Langmi, {Henrietta W.} and Robert Mokaya and Musyoka, {Nicholas M.} and Khotseng, {Lindiwe E.}",

note = "Publisher Copyright: {\textcopyright} 2020 Hydrogen Energy Publications LLC",

year = "2021",

month = feb,

day = "16",

doi = "10.1016/j.ijhydene.2020.12.049",

language = "English",

volume = "46",

pages = "8607--8620",

journal = "International Journal of Hydrogen Energy",

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TY - JOUR

T1 - Co-pelletization of a zirconium-based metal-organic framework (UiO-66) with polymer nanofibers for improved useable capacity in hydrogen storage

AU - Bambalaza, Sonwabo E.

AU - Langmi, Henrietta W.

AU - Mokaya, Robert

AU - Musyoka, Nicholas M.

AU - Khotseng, Lindiwe E.

PY - 2021/2/16

Y1 - 2021/2/16

N2 - We report on a concept of co-pelletization using mechanically robust hydroxylated UiO-66 to develop a metal-organic framework (MOF) monolith that contains 5 wt% electrospun polymer nanofibers, and consists of an architecture with alternating layers of MOF and nanofiber mats. The polymers of choice were the microporous Polymer of Intrinsic Microporosity (PIM-1) and non-porous polyacrylonitrile (PAN). Co-pelletized UiO-66/PIM-1 and UiO-66/PAN monoliths retain no less than 85% of the porosity obtained in pristine powder and pelletized UiO-66. The composition of the pore size distribution in co-pelletized UiO-66/PIM-1 and UiO-66/PAN monoliths is significantly different to that of pristine UiO-66 forms, with pristine UiO-66 forms showing 90% of the pore apertures in the micropore region and both UiO-66/nanofiber monoliths showing a composite micro-mesoporous pore size distribution. The co-pelletized UiO-66/nanofiber monoliths obtained improved useable H2 capacities in comparison to pristine UiO-66 forms, under isothermal pressure swing conditions. The UiO-66/PIM-1 monolith constitutes the highest gravimetric (and volumetric) useable capacities at 2.3 wt% (32 g L−1) in comparison to 1.8 wt% (12 g L−1) and 1.9 wt% (29 g L−1) obtainable in pristine UiO-66 powder and UiO-66 pellet, respectively. The co-pelletized UiO-66/PAN monolith, however, shows a significantly reduced surface area by up to 50% less in comparison to pristine UiO-66, but its pore volume only 13% less in comparison to pristine UiO-66. As a result, total gravimetric H2 capacity of the co-pelletized UiO-66/PAN monolith is 50% less in comparison to that of pristine UiO-66, but crucially the useable volumetric H2 capacity is 50% higher for the UiO-66/PAN monolith in comparison to pristine UiO-66 powder. The co-pelletization strategy provides a simple method for generating hierarchical porosity into an initially highly microporous MOF without changing the structure of the MOF through complex chemical modifications. The UiO-66/nanofiber monoliths offer improvements to the typically low H2 useable capacities in highly microporous MOFs, and open new opportunities towards achieving system-level H2 storage targets.

AB - We report on a concept of co-pelletization using mechanically robust hydroxylated UiO-66 to develop a metal-organic framework (MOF) monolith that contains 5 wt% electrospun polymer nanofibers, and consists of an architecture with alternating layers of MOF and nanofiber mats. The polymers of choice were the microporous Polymer of Intrinsic Microporosity (PIM-1) and non-porous polyacrylonitrile (PAN). Co-pelletized UiO-66/PIM-1 and UiO-66/PAN monoliths retain no less than 85% of the porosity obtained in pristine powder and pelletized UiO-66. The composition of the pore size distribution in co-pelletized UiO-66/PIM-1 and UiO-66/PAN monoliths is significantly different to that of pristine UiO-66 forms, with pristine UiO-66 forms showing 90% of the pore apertures in the micropore region and both UiO-66/nanofiber monoliths showing a composite micro-mesoporous pore size distribution. The co-pelletized UiO-66/nanofiber monoliths obtained improved useable H2 capacities in comparison to pristine UiO-66 forms, under isothermal pressure swing conditions. The UiO-66/PIM-1 monolith constitutes the highest gravimetric (and volumetric) useable capacities at 2.3 wt% (32 g L−1) in comparison to 1.8 wt% (12 g L−1) and 1.9 wt% (29 g L−1) obtainable in pristine UiO-66 powder and UiO-66 pellet, respectively. The co-pelletized UiO-66/PAN monolith, however, shows a significantly reduced surface area by up to 50% less in comparison to pristine UiO-66, but its pore volume only 13% less in comparison to pristine UiO-66. As a result, total gravimetric H2 capacity of the co-pelletized UiO-66/PAN monolith is 50% less in comparison to that of pristine UiO-66, but crucially the useable volumetric H2 capacity is 50% higher for the UiO-66/PAN monolith in comparison to pristine UiO-66 powder. The co-pelletization strategy provides a simple method for generating hierarchical porosity into an initially highly microporous MOF without changing the structure of the MOF through complex chemical modifications. The UiO-66/nanofiber monoliths offer improvements to the typically low H2 useable capacities in highly microporous MOFs, and open new opportunities towards achieving system-level H2 storage targets.

KW - Co-pelletization

KW - Hierarchical porosity

KW - Hydrogen useable capacity

KW - Metal-organic framework

KW - UiO-66

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U2 - 10.1016/j.ijhydene.2020.12.049

DO - 10.1016/j.ijhydene.2020.12.049

M3 - Article

AN - SCOPUS:85098541522

SN - 0360-3199

VL - 46

SP - 8607

EP - 8620

JO - International Journal of Hydrogen Energy

JF - International Journal of Hydrogen Energy

IS - 12

ER -

Co-pelletization of a zirconium-based metal-organic framework (UiO-66) with polymer nanofibers for improved useable capacity in hydrogen storage

Abstract

Keywords

ASJC Scopus subject areas

UN SDGs

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