Graphene-Immobilized fac-Re(bipy)(CO)3Cl for Syngas Generation from Carbon Dioxide

ACS Applied Materials & Interfaces
Xin ZhouWenbin Lin

Abstract

We report the synthesis of fac-M(4-amino-bipy)(CO)3X (M = Mn and X = Br or M = Re and X = Cl, with bipy = 2,2'-bipyridine), their immobilization on graphene oxide (GrO) via diazonium grafting, and the use of Re-functionalized GrO for electrocatalytic syngas production. Infrared (IR) spectroscopy, X-ray absorption fine structure (XAFS) spectroscopy, and electrocatalysis indicated successful grafting of the Re catalyst onto GrO. Re-functionalized GrO was then deposited onto a glassy carbon electrode (GCE) for CO2 reduction. Investigation of the Re-functionalized GCE for syngas production was performed in a CO2-saturated acetonitrile solution with 3.1 M H2O as the proton source and 0.1 M tetrabutylammonium hexafluorophosphate (TBAPF6) as the supporting electrolyte. Cyclic voltammetry (CV), controlled potential electrolysis (CPE), and gas chromatography (GC) were employed to determine its CO2-to-CO conversion performance. The Re catalyst shows a turnover frequency (TOF) for generating CO up to 4.44 s(-1) with a CO/H2 ratio of 7:5.

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Citations

Aug 10, 2017·Chemical Communications : Chem Comm·James D CopeT Keith Hollis
Jul 22, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Nicholas M OrchanianSmaranda C Marinescu
Oct 4, 2019·Journal of the American Chemical Society·Almagul ZhanaidarovaClifford P Kubiak
Dec 12, 2017·The Journal of Physical Chemistry Letters·Aimin GeTianquan Lian

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