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...

Full description

Saved in:
Bibliographic Details
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
Subjects:
Online Access:https://pubs.rsc.org/en/content/articlepdf/2020/ra/c9ra09938g
http://hdl.handle.net/11408/4329
Tags: Add Tag
No Tags, Be the first to tag this record!
Description
Summary: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.