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Solvent-Free Synthetic Route for Cerium(IV) Metal–Organic Frameworks with UiO-66 Architecture and Their Photocatalytic Applications

Matteo Campanelli, Tiziana Del Giacco, Filippo De Angelis, Edoardo Mosconi, Marco Taddei Orcid Logo, Fabio Marmottini, Roberto D’Amato, Ferdinando Costantino

ACS Applied Materials & Interfaces, Volume: 11, Issue: 48, Pages: 45031 - 45037

Swansea University Author: Marco Taddei Orcid Logo

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DOI (Published version): 10.1021/acsami.9b13730

Abstract

A near solvent-free synthetic route for Ce-UiO-66 metal–organic frameworks (MOFs) is presented. The MOFs are obtained by energetically grinding the reagents, cerium ammonium nitrate (CAN) and the carboxylic linkers, in a mortar for a few minutes with the addition of a small amount of acetic acid (Ac...

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Published in: ACS Applied Materials & Interfaces
ISSN: 1944-8244 1944-8252
Published: American Chemical Society (ACS) 2019
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URI: https://cronfa.swan.ac.uk/Record/cronfa53025
first_indexed 2019-12-12T19:16:18Z
last_indexed 2020-11-21T04:07:31Z
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spelling 2020-11-20T09:53:53.8493613 v2 53025 2019-12-12 Solvent-Free Synthetic Route for Cerium(IV) Metal–Organic Frameworks with UiO-66 Architecture and Their Photocatalytic Applications 5cffd1038508554d8596dee8b4e51052 0000-0003-2805-6375 Marco Taddei Marco Taddei true false 2019-12-12 A near solvent-free synthetic route for Ce-UiO-66 metal–organic frameworks (MOFs) is presented. The MOFs are obtained by energetically grinding the reagents, cerium ammonium nitrate (CAN) and the carboxylic linkers, in a mortar for a few minutes with the addition of a small amount of acetic acid (AcOH) as a modulator (8.75 equiv, 0.5 mL). The slurry is then transferred into a 2 mL vial and heated at 120 °C for 1 day. The MOFs have been characterized for their composition, crystallinity, and porosity and employed as heterogeneous catalysts for the photo-oxidation reaction of substituted benzylic alcohols to benzaldaldehydes under near-ultraviolet light irradiation. The catalytic performances, such as selectivity, conversion, and kinetics, exceed those of similar systems studied by chemical oxidation using similar Ce-MOFs as a catalyst. Moreover, the MOFs were found to be reusable up to three cycles without loss of activity. Density functional theory (DFT) calculations were used to fully describe the electronic structure of the best performing MOFs and to provide useful information on the catalytic activity experimentally observed. Journal Article ACS Applied Materials & Interfaces 11 48 45031 45037 American Chemical Society (ACS) 1944-8244 1944-8252 metal−organic frameworks, cerium, photocatalysis, DFT calculations, green syntheses 4 12 2019 2019-12-04 10.1021/acsami.9b13730 COLLEGE NANME COLLEGE CODE Swansea University 2020-11-20T09:53:53.8493613 2019-12-12T15:41:54.0734403 Professional Services ISS - Uncategorised Matteo Campanelli 1 Tiziana Del Giacco 2 Filippo De Angelis 3 Edoardo Mosconi 4 Marco Taddei 0000-0003-2805-6375 5 Fabio Marmottini 6 Roberto D’Amato 7 Ferdinando Costantino 8 53025__16091__34c75e3e737147f19e4f98a90339b441.pdf Campanelli2019.pdf 2019-12-13T10:30:15.4260066 Output 1245265 application/pdf Accepted Manuscript true 2020-11-08T00:00:00.0000000 true eng
title Solvent-Free Synthetic Route for Cerium(IV) Metal–Organic Frameworks with UiO-66 Architecture and Their Photocatalytic Applications
spellingShingle Solvent-Free Synthetic Route for Cerium(IV) Metal–Organic Frameworks with UiO-66 Architecture and Their Photocatalytic Applications
Marco Taddei
title_short Solvent-Free Synthetic Route for Cerium(IV) Metal–Organic Frameworks with UiO-66 Architecture and Their Photocatalytic Applications
title_full Solvent-Free Synthetic Route for Cerium(IV) Metal–Organic Frameworks with UiO-66 Architecture and Their Photocatalytic Applications
title_fullStr Solvent-Free Synthetic Route for Cerium(IV) Metal–Organic Frameworks with UiO-66 Architecture and Their Photocatalytic Applications
title_full_unstemmed Solvent-Free Synthetic Route for Cerium(IV) Metal–Organic Frameworks with UiO-66 Architecture and Their Photocatalytic Applications
title_sort Solvent-Free Synthetic Route for Cerium(IV) Metal–Organic Frameworks with UiO-66 Architecture and Their Photocatalytic Applications
author_id_str_mv 5cffd1038508554d8596dee8b4e51052
author_id_fullname_str_mv 5cffd1038508554d8596dee8b4e51052_***_Marco Taddei
author Marco Taddei
author2 Matteo Campanelli
Tiziana Del Giacco
Filippo De Angelis
Edoardo Mosconi
Marco Taddei
Fabio Marmottini
Roberto D’Amato
Ferdinando Costantino
format Journal article
container_title ACS Applied Materials & Interfaces
container_volume 11
container_issue 48
container_start_page 45031
publishDate 2019
institution Swansea University
issn 1944-8244
1944-8252
doi_str_mv 10.1021/acsami.9b13730
publisher American Chemical Society (ACS)
college_str Professional Services
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hierarchy_top_title Professional Services
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description A near solvent-free synthetic route for Ce-UiO-66 metal–organic frameworks (MOFs) is presented. The MOFs are obtained by energetically grinding the reagents, cerium ammonium nitrate (CAN) and the carboxylic linkers, in a mortar for a few minutes with the addition of a small amount of acetic acid (AcOH) as a modulator (8.75 equiv, 0.5 mL). The slurry is then transferred into a 2 mL vial and heated at 120 °C for 1 day. The MOFs have been characterized for their composition, crystallinity, and porosity and employed as heterogeneous catalysts for the photo-oxidation reaction of substituted benzylic alcohols to benzaldaldehydes under near-ultraviolet light irradiation. The catalytic performances, such as selectivity, conversion, and kinetics, exceed those of similar systems studied by chemical oxidation using similar Ce-MOFs as a catalyst. Moreover, the MOFs were found to be reusable up to three cycles without loss of activity. Density functional theory (DFT) calculations were used to fully describe the electronic structure of the best performing MOFs and to provide useful information on the catalytic activity experimentally observed.
published_date 2019-12-04T07:51:12Z
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score 11.04748

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