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

Journal Article · · ACS Applied Materials and Interfaces
 [1];  [2];  [2];  [2];  [3];  [2]
  1. Univ. of Chicago, IL (United States); South China University of Technology, Guangzhou (People's Republic of China)
  2. Univ. of Chicago, IL (United States)
  3. 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.

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, Vol. 8, Issue 6; ISSN 1944-8244
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
ENGLISH
Citation Metrics:
Cited by: 18 works
Citation information provided by
Web of Science

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Nitrogen-doped tubular carbon foam electrodes for efficient electroreduction of CO 2 to syngas with potential-independent CO/H 2 ratios journal January 2019
Electrocatalytic reduction of carbon dioxide: opportunities with heterogeneous molecular catalysts journal January 2020
Rhenium-modified porous covalent triazine framework for highly efficient photocatalytic carbon dioxide reduction in a solid–gas system journal January 2018
Carbon Solving Carbon's Problems: Recent Progress of Nanostructured Carbon-Based Catalysts for the Electrochemical Reduction of CO 2 journal July 2017
Immobilizing Re(CO) 3 Br(dcbpy) Complex on CsPbBr 3 Nanocrystal for Boosted Charge Separation and Photocatalytic CO 2 Reduction journal September 2019
Electrocatalytic reduction of CO 2 with CCC-NHC pincer nickel complexes journal January 2017
Elucidating the Electrocatalytic CO 2 Reduction Reaction over a Model Single‐Atom Nickel Catalyst journal December 2019
Elucidating the Electrocatalytic CO 2 Reduction Reaction over a Model Single‐Atom Nickel Catalyst journal January 2020
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Figures / Tables (7)