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

Zhou, Xin; Micheroni, Daniel; Lin, Zekai; Poon, Christopher; Li, Zhong; Lin, Wenbin

doi:10.1021/acsami.5b11958

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

Journal Article · Thu Jan 21 23:00:00 EST 2016 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.5b11958· OSTI ID:1330243

Zhou, Xin ^[1]; Micheroni, Daniel ^[2]; Lin, Zekai ^[2]; Poon, Christopher ^[2]; Li, Zhong ^[3]; Lin, Wenbin ^[2]

Univ. of Chicago, IL (United States); South China University of Technology, Guangzhou (People's Republic of China)
Univ. of Chicago, IL (United States)
South China University of Technology, Guangzhou (People's Republic of China)

We report herein 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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: National Science Foundation (NSF); Oversea Study Program of Guangzhou Elite Project; USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1330243

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 6 Vol. 8; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: ENGLISH

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