Issue 6, 2020

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.

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

Supplementary files

Article information

Article type
Paper
Submitted
27 Nov 2019
Accepted
14 Jan 2020
First published
22 Jan 2020
This article is Open Access
Creative Commons BY license

RSC Adv., 2020,10, 3593-3605

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

P. Tshuma, B. C. E. Makhubela, L. Öhrström, S. A. Bourne, N. Chatterjee, I. N. Beas, J. Darkwa and G. Mehlana, RSC Adv., 2020, 10, 3593 DOI: 10.1039/C9RA09938G

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