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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Main Authors: Tshuma, Piwai, Makhubela, Banothile C. E., Ohrstr ¨ om, Lars, Bourne, Susan A., Chatterjee, Nabanita, Beas, Isaac N., Darkwa, James, Mehlana, Gift
Format: Article
Language:English
Published: 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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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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