title: Graphene-Immobilized fac-Re(bipy)(CO)3Cl for Syngas Generation from Carbon Dioxide.
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.
authors.affiliation: Department of Chemistry, University of Chicago , 929 East 57th Street, Chicago, Illinois 60637, United States.|School of Chemistry and Chemical Engineering, South China University of Technology , Guangzhou, Guangdong 510640, People's Republic of China.
authors.forename: Xin
authors.initials: X
authors.lastname: Zhou
authors.affiliation: Department of Chemistry, University of Chicago , 929 East 57th Street, Chicago, Illinois 60637, United States.
authors.forename: Daniel
authors.initials: D
authors.lastname: Micheroni
authors.affiliation: Department of Chemistry, University of Chicago , 929 East 57th Street, Chicago, Illinois 60637, United States.
authors.forename: Zekai
authors.initials: Z
authors.lastname: Lin
authors.affiliation: Department of Chemistry, University of Chicago , 929 East 57th Street, Chicago, Illinois 60637, United States.
authors.forename: Christopher
authors.initials: C
authors.lastname: Poon
authors.affiliation: School of Chemistry and Chemical Engineering, South China University of Technology , Guangzhou, Guangdong 510640, People's Republic of China.
authors.forename: Zhong
authors.initials: Z
authors.lastname: Li
authors.affiliation: Department of Chemistry, University of Chicago , 929 East 57th Street, Chicago, Illinois 60637, United States.
authors.forename: Wenbin
authors.initials: W
authors.lastname: Lin
keywords: CO2 reduction; catalysis; diazonium grafting; graphene; syngas