A single site catalyst supported in mesoporous UiO-66 for catalytic conversion of carbon dioxide to formate

被引:3
作者
Gumbo, Maureen [1 ,2 ]
Ocansey, Edward [2 ]
Makhubela, Banothile C. E. [2 ]
Amombo Noa, Francoise M. [3 ]
Ohrstrom, Lars [3 ]
Mudraj, Obieda S. [4 ]
Mehlana, Gift [1 ]
机构
[1] Midlands State Univ, Fac Sci & Technol, Dept Chem Sci, Private Bag 9055,Senga Rd, Gweru, Zimbabwe
[2] Univ Johannesburg, Res Ctr Synth & Catalysis, Dept Chem Sci, Auckland Pk Kingsway Campus, ZA-2006 Auckland Pk, South Africa
[3] Chalmers Univ Technol, Dept Chem & Chem Engn, SE-41296 Gothenburg, Sweden
[4] Royal Sci Soc, Adv Res Ctr, Mat Discovery Res Unit, Amman 11941, Jordan
基金
瑞典研究理事会;
关键词
METAL-ORGANIC FRAMEWORK; CO2; HYDROGENATION; IRIDIUM COMPLEXES; NICKEL-CATALYSTS; CHEMISTRY; METHANOL; LIGANDS; PROTON; MOFS;
D O I
10.1039/d3se01465g
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Carbon dioxide utilisation strategies are of paramount importance, yielding various products such as methanol and formate. Formate is an excellent hydrogen carrier in fuel cells, making it a highly exploitable chemical on the hydrogen energy storage front. Formate has an energy content that is at least five times greater than that of commercially available lithium-ion batteries. Herein, we have prepared mesoporous metal-organic frameworks (MOFs) (m-UiO-66 and m-UiO-66-NH2), using a Zr-based secondary building unit (SBU) and terephthalate linkers. The MOFs were used to support the half-sandwich (tetrazolylpyridyl)iridium(iii) complex to make single-site catalyst (Ir(iii)@m-UiO-66 and Ir(iii)@m-UiO-66-NH2) for CO2 conversion to formate. Both Ir(iii)@m-UiO-66 and Ir(iii)@m-UiO-66-NH2 exhibited improved activity for CO2 hydrogenation to formate in a heterogeneous system. Ir(iii)@m-UiO-66-NH2 and Ir(iii)@m-UiO-66 had turnover numbers of 3313 and 3076 TON, respectively, under optimized conditions. X-ray photoelectron spectroscopy (XPS) showed possible interaction of the complex with the MOF as evidenced by a downfield shift in the binding energies of the Ir 4f electronic environment. The catalysts showed post-catalysis stability, as confirmed by PXRD, FTIR, and XPS. The Ir 4f binding energies of the materials after catalysis showed an up-field shift confirming the presence of Ir-H species which are the active species for catalysis. The half-sandwich (tetrazolylpyridyl)iridium(iii) complex shows improved catalytic activity towards hydrogenation of carbon dioxide to formate when supported in a mesoporous m-UiO-66 MOF.
引用
收藏
页码:777 / 788
页数:12
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