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.
Highlights
The conversion of carbon dioxide to high value chemicals is of global interest owing to the dangers posed by this greenhouse gas to the environment
Our results demonstrate that incorporation of the [Ru(II)Cl(p-cymene)] complex into the metal–organic framework (MOF) enhances the yield of formate produced
The structure of JMS-1 is made up of La2C3O6 secondary building unit (SBU) rod which grow along the b-axis (Fig. 1a)
Summary
The conversion of carbon dioxide to high value chemicals is of global interest owing to the dangers posed by this greenhouse gas to the environment. Carbon dioxide is considered as a cheap and renewable source of carbon and its conversion to formic acid is of interest to the chemical industry. The world production of formic acid is around 700 000 tons per year, mostly from combining methanol and carbon monoxide.[1] In addition to current use, one can view formic acid produced from renewable H2 and CO2 as a way to store energy.[2,3]. During the past decades extensive research on conversion of carbon dioxide to formate or methanol has been accomplished using both homogeneous catalysts and heterogeneous catalysts.[4,5,6] The challenge with using homogenous catalysts, which
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