Cyclometalation of lanthanum(iii) based MOF for catalytic hydrogenation of carbon dioxide to formate

Piwai Tshuma; Banothile C.E. Makhubela; Lars Öhrström; Susan A. Bourne; Nabanita Chatterjee; Isaac N. Beas; James Darkwa; Gift Mehlana

doi:10.1039/c9ra09938g

Cyclometalation of lanthanum(iii) based MOF for catalytic hydrogenation of carbon dioxide to formate

Piwai Tshuma, Banothile C.E. Makhubela, Lars Öhrström, Susan A. Bourne, Nabanita Chatterjee, Isaac N. Beas, James Darkwa, Gift Mehlana

Chemical Sciences

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Abstract

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 = 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.

Original language	English
Pages (from-to)	3593-3605
Number of pages	13
Journal	RSC Advances
Volume	10
Issue number	6
DOIs	https://doi.org/10.1039/c9ra09938g
Publication status	Published - 2020

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General Chemistry
General Chemical Engineering

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title = "Cyclometalation of lanthanum(iii) based MOF for catalytic hydrogenation of carbon dioxide to formate",

abstract = "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 = 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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AU - Tshuma, Piwai

AU - Makhubela, Banothile C.E.

AU - Öhrström, Lars

AU - Bourne, Susan A.

AU - Chatterjee, Nabanita

AU - Beas, Isaac N.

AU - Darkwa, James

AU - Mehlana, Gift

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N2 - 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 = 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.

AB - 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 = 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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Cyclometalation of lanthanum(iii) based MOF for catalytic hydrogenation of carbon dioxide to formate

Abstract

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