Cyclometalation of lanthanum(III) based MOF for catalytic hydrogenation of carbon dioxide to formate
The hydrogenation of carbon dioxide (CO2) to formic acid is of great importance due to its useful properties in the chemical industry. In this work, we have prepared a novel metal–organic framework (MOF), JMS-1, using bipyridyl dicarboxylate linkers, with molecular formula [La2(bpdc)3(DMF)3]n. Netwo...
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Royal Society of Chemistry
2021
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Online Access: | https://pubs.rsc.org/en/content/articlepdf/2020/ra/c9ra09938g http://hdl.handle.net/11408/4329 |
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author | Tshuma, Piwai Makhubela, Banothile C. E. Ohrstr ¨ om, Lars Bourne, Susan A. Chatterjee, Nabanita Beas, Isaac N. Darkwa, James Mehlana, Gift |
author_facet | Tshuma, Piwai Makhubela, Banothile C. E. Ohrstr ¨ om, Lars Bourne, Susan A. Chatterjee, Nabanita Beas, Isaac N. Darkwa, James Mehlana, Gift |
author_sort | Tshuma, Piwai |
collection | DSpace |
description | The hydrogenation of carbon dioxide (CO2) to formic acid is of great importance due to its useful properties in the chemical industry. In this work, we have prepared a novel metal–organic framework (MOF), JMS-1, using bipyridyl dicarboxylate linkers, with molecular formula [La2(bpdc)3(DMF)3]n. Network analysis of JMS-1 revealed a new 7-connected topology (zaz). The MOF backbone of the activated phase (JMS-1a) was functionalized by cyclometalation using [RuCl2(p-cymene)]2 to produce Ru(II)@JMS-1a. Both JMS-1a and Ru(II)@JMS-1a were able to convert CO2 in the presence of hydrogen to formate. Ru(II)@JMS-1a displayed outstanding conversion evidenced by a yield of 98% of formate under optimized conditions of total pressure 50 bar (CO2/H2 ¼ 1 : 4, temperature 110 C, time 24 h, 5 mmol KOH, 8 mL ethanol). This work is significant in providing new strategies of incorporating active catalytic centres in MOFs for efficient and selective conversion of CO2 to formate. |
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id | ir-11408-4329 |
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language | English |
publishDate | 2021 |
publisher | Royal Society of Chemistry |
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spelling | ir-11408-43292022-06-27T13:49:06Z Cyclometalation of lanthanum(III) based MOF for catalytic hydrogenation of carbon dioxide to formate Tshuma, Piwai Makhubela, Banothile C. E. Ohrstr ¨ om, Lars Bourne, Susan A. Chatterjee, Nabanita Beas, Isaac N. Darkwa, James Mehlana, Gift Cyclometalation of lanthanum(III) MOF for catalytic hydrogenation carbon dioxide to formate The hydrogenation of carbon dioxide (CO2) to formic acid is of great importance due to its useful properties in the chemical industry. In this work, we have prepared a novel metal–organic framework (MOF), JMS-1, using bipyridyl dicarboxylate linkers, with molecular formula [La2(bpdc)3(DMF)3]n. Network analysis of JMS-1 revealed a new 7-connected topology (zaz). The MOF backbone of the activated phase (JMS-1a) was functionalized by cyclometalation using [RuCl2(p-cymene)]2 to produce Ru(II)@JMS-1a. Both JMS-1a and Ru(II)@JMS-1a were able to convert CO2 in the presence of hydrogen to formate. Ru(II)@JMS-1a displayed outstanding conversion evidenced by a yield of 98% of formate under optimized conditions of total pressure 50 bar (CO2/H2 ¼ 1 : 4, temperature 110 C, time 24 h, 5 mmol KOH, 8 mL ethanol). This work is significant in providing new strategies of incorporating active catalytic centres in MOFs for efficient and selective conversion of CO2 to formate. 2021-06-02T13:18:37Z 2021-06-02T13:18:37Z 2020 Article 2046-2069 https://pubs.rsc.org/en/content/articlepdf/2020/ra/c9ra09938g http://hdl.handle.net/11408/4329 en RSC Advances;Vol.10 ; No.3593 open Royal Society of Chemistry |
spellingShingle | Cyclometalation of lanthanum(III) MOF for catalytic hydrogenation carbon dioxide to formate Tshuma, Piwai Makhubela, Banothile C. E. Ohrstr ¨ om, Lars Bourne, Susan A. Chatterjee, Nabanita Beas, Isaac N. Darkwa, James Mehlana, Gift Cyclometalation of lanthanum(III) based MOF for catalytic hydrogenation of carbon dioxide to formate |
title | Cyclometalation of lanthanum(III) based MOF for catalytic hydrogenation of carbon dioxide to formate |
title_full | Cyclometalation of lanthanum(III) based MOF for catalytic hydrogenation of carbon dioxide to formate |
title_fullStr | Cyclometalation of lanthanum(III) based MOF for catalytic hydrogenation of carbon dioxide to formate |
title_full_unstemmed | Cyclometalation of lanthanum(III) based MOF for catalytic hydrogenation of carbon dioxide to formate |
title_short | Cyclometalation of lanthanum(III) based MOF for catalytic hydrogenation of carbon dioxide to formate |
title_sort | cyclometalation of lanthanum(iii) based mof for catalytic hydrogenation of carbon dioxide to formate |
topic | Cyclometalation of lanthanum(III) MOF for catalytic hydrogenation carbon dioxide to formate |
url | https://pubs.rsc.org/en/content/articlepdf/2020/ra/c9ra09938g http://hdl.handle.net/11408/4329 |
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