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Experimental demonstration of dynamic temperature-dependent behavior of UiO-66 metal-organic framework: Compaction of hydroxylated and dehydroxylated forms of UiO-66 for high-pressure hydrogen storage

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dc.contributor.author Bambalaza, Sonwabo E
dc.contributor.author Langmi, HW
dc.contributor.author Mokaya, R
dc.contributor.author Musyoka, Nicholas M
dc.contributor.author Khotseng, LE
dc.date.accessioned 2021-04-23T09:45:30Z
dc.date.available 2021-04-23T09:45:30Z
dc.date.issued 2020-05
dc.identifier.citation Bambalaza, S.E., Langmi, H., Mokaya, R., Musyoka, N.M. & Khotseng, L. 2020. Experimental demonstration of dynamic temperature-dependent behavior of UiO-66 metal-organic framework: Compaction of hydroxylated and dehydroxylated forms of UiO-66 for high-pressure hydrogen storage. <i>ACS Applied Materials and Interfaces, 12(22).</i> http://hdl.handle.net/10204/11990 en_ZA
dc.identifier.issn 1944-8244
dc.identifier.issn 1944-8252
dc.identifier.uri https://doi.org/10.1021/acsami.0c06080
dc.identifier.uri http://hdl.handle.net/10204/11990
dc.description.abstract High-pressure (700 MPa or ∼100 000 psi) compaction of dehydroxylated and hydroxylated UiO-66 for H2 storage applications is reported. The dehydroxylation reaction was found to occur between 150 and 300 °C. The H2 uptake capacity of powdered hydroxylated UiO-66 reaches 4.6 wt % at 77 K and 100 bar, which is 21% higher than that of dehydroxylated UiO-66 (3.8 wt %). On compaction, the H2 uptake capacity of dehydroxylated UiO-66 pellets reduces by 66% from 3.8 to 1.3 wt %, while for hydroxylated UiO-66 the pellets show only a 9% reduction in capacity from 4.6 to 4.2 wt %. This implies that the H2 uptake capacity of compacted hydroxylated UiO-66 is at least three times higher than that of dehydroxylated UiO-66, and therefore, hydroxylated UiO-66 is more promising for hydrogen storage applications. The H2 uptake capacity is closely related to compaction-induced changes in the porosity of UiO-66. The effect of compaction is greatest in partially dehydroxylated UiO-66 samples that are thermally treated at 200 and 290 °C. These compacted samples exhibit XRD patterns indicative of an amorphous material, low porosity (surface area reduces from between 700 and 1300 m2/g to ca. 200 m2/g and pore volume from between 0.4 and 0.6 cm3/g to 0.1 and 0.15 cm3/g), and very low hydrogen uptake (0.7–0.9 wt % at 77 K and 100 bar). The observed activation-temperature-induced dynamic behavior of UiO-66 is unusual for metal–organic frameworks (MOFs) and has previously only been reported in computational studies. After compaction at 700 MPa, the structural properties and H2 uptake of hydroxylated UiO-66 remain relatively unchanged but are extremely compromised upon compaction of dehydroxylated UiO-66. Therefore, UiO-66 responds in a dynamic manner to changes in activation temperature within the range in which it has hitherto been considered stable. en_US
dc.format Abstract en_US
dc.language.iso en en_US
dc.relation.uri https://pubs.acs.org/doi/abs/10.1021/acsami.0c06080 en_US
dc.source ACS Applied Materials and Interfaces, 12(22) en_US
dc.subject Dehydroxylation en_US
dc.subject compaction en_US
dc.subject Hydroxylation en_US
dc.subject Hydrogen storage en_US
dc.subject Metal-organic framework en_US
dc.subject UiO-66 en_US
dc.title Experimental demonstration of dynamic temperature-dependent behavior of UiO-66 metal-organic framework: Compaction of hydroxylated and dehydroxylated forms of UiO-66 for high-pressure hydrogen storage en_US
dc.type Article en_US
dc.description.pages 24883-24894 en_US
dc.description.note © 2020 American Chemical Society. Due to copyright restrictions, the attached PDF file only contains the abstract of the full text item. For access to the full text item, please consult the publisher's website: https://pubs.acs.org/doi/abs/10.1021/acsami.0c06080 en_US
dc.description.cluster Chemicals en_US
dc.description.impactarea Hydrogen SA en_US
dc.identifier.apacitation Bambalaza, S. E., Langmi, H., Mokaya, R., Musyoka, N. M., & Khotseng, L. (2020). Experimental demonstration of dynamic temperature-dependent behavior of UiO-66 metal-organic framework: Compaction of hydroxylated and dehydroxylated forms of UiO-66 for high-pressure hydrogen storage. <i>ACS Applied Materials and Interfaces, 12(22)</i>, http://hdl.handle.net/10204/11990 en_ZA
dc.identifier.chicagocitation Bambalaza, Sonwabo E, HW Langmi, R Mokaya, Nicholas M Musyoka, and LE Khotseng "Experimental demonstration of dynamic temperature-dependent behavior of UiO-66 metal-organic framework: Compaction of hydroxylated and dehydroxylated forms of UiO-66 for high-pressure hydrogen storage." <i>ACS Applied Materials and Interfaces, 12(22)</i> (2020) http://hdl.handle.net/10204/11990 en_ZA
dc.identifier.vancouvercitation Bambalaza SE, Langmi H, Mokaya R, Musyoka NM, Khotseng L. Experimental demonstration of dynamic temperature-dependent behavior of UiO-66 metal-organic framework: Compaction of hydroxylated and dehydroxylated forms of UiO-66 for high-pressure hydrogen storage. ACS Applied Materials and Interfaces, 12(22). 2020; http://hdl.handle.net/10204/11990. en_ZA
dc.identifier.ris TY - Article AU - Bambalaza, Sonwabo E AU - Langmi, HW AU - Mokaya, R AU - Musyoka, Nicholas M AU - Khotseng, LE AB - High-pressure (700 MPa or ∼100 000 psi) compaction of dehydroxylated and hydroxylated UiO-66 for H2 storage applications is reported. The dehydroxylation reaction was found to occur between 150 and 300 °C. The H2 uptake capacity of powdered hydroxylated UiO-66 reaches 4.6 wt % at 77 K and 100 bar, which is 21% higher than that of dehydroxylated UiO-66 (3.8 wt %). On compaction, the H2 uptake capacity of dehydroxylated UiO-66 pellets reduces by 66% from 3.8 to 1.3 wt %, while for hydroxylated UiO-66 the pellets show only a 9% reduction in capacity from 4.6 to 4.2 wt %. This implies that the H2 uptake capacity of compacted hydroxylated UiO-66 is at least three times higher than that of dehydroxylated UiO-66, and therefore, hydroxylated UiO-66 is more promising for hydrogen storage applications. The H2 uptake capacity is closely related to compaction-induced changes in the porosity of UiO-66. The effect of compaction is greatest in partially dehydroxylated UiO-66 samples that are thermally treated at 200 and 290 °C. These compacted samples exhibit XRD patterns indicative of an amorphous material, low porosity (surface area reduces from between 700 and 1300 m2/g to ca. 200 m2/g and pore volume from between 0.4 and 0.6 cm3/g to 0.1 and 0.15 cm3/g), and very low hydrogen uptake (0.7–0.9 wt % at 77 K and 100 bar). The observed activation-temperature-induced dynamic behavior of UiO-66 is unusual for metal–organic frameworks (MOFs) and has previously only been reported in computational studies. After compaction at 700 MPa, the structural properties and H2 uptake of hydroxylated UiO-66 remain relatively unchanged but are extremely compromised upon compaction of dehydroxylated UiO-66. Therefore, UiO-66 responds in a dynamic manner to changes in activation temperature within the range in which it has hitherto been considered stable. DA - 2020-05 DB - ResearchSpace DP - CSIR J1 - ACS Applied Materials and Interfaces, 12(22) KW - Dehydroxylation KW - compaction KW - Hydroxylation KW - Hydrogen storage KW - Metal-organic framework KW - UiO-66 LK - https://researchspace.csir.co.za PY - 2020 SM - 1944-8244 SM - 1944-8252 T1 - Experimental demonstration of dynamic temperature-dependent behavior of UiO-66 metal-organic framework: Compaction of hydroxylated and dehydroxylated forms of UiO-66 for high-pressure hydrogen storage TI - Experimental demonstration of dynamic temperature-dependent behavior of UiO-66 metal-organic framework: Compaction of hydroxylated and dehydroxylated forms of UiO-66 for high-pressure hydrogen storage UR - http://hdl.handle.net/10204/11990 ER - en_ZA
dc.identifier.worklist 24302 en_US


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