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

Abstract

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.

Authors:
 [1];  [2];  [2];  [2];  [3];  [2]
+ Show Author Affiliations
  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)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
National Science Foundation (NSF); Oversea Study Program of Guangzhou Elite Project; USDOE Office of Science (SC)
OSTI Identifier:
1330243
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 8; Journal Issue: 6; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
ENGLISH
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO2 reduction; syngas; graphene; diazonium grafting; catalysis

Citation Formats

Zhou, Xin, Micheroni, Daniel, Lin, Zekai, Poon, Christopher, Li, Zhong, and Lin, Wenbin. Graphene-Immobilized fac-Re(bipy)(CO)3 Cl for Syngas Generation from Carbon Dioxide. United States: N. p., 2016. Web. doi:10.1021/acsami.5b11958.
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Zhou, Xin, Micheroni, Daniel, Lin, Zekai, Poon, Christopher, Li, Zhong, & Lin, Wenbin. Graphene-Immobilized fac-Re(bipy)(CO)3 Cl for Syngas Generation from Carbon Dioxide. United States. https://doi.org/10.1021/acsami.5b11958
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Zhou, Xin, Micheroni, Daniel, Lin, Zekai, Poon, Christopher, Li, Zhong, and Lin, Wenbin. Fri . "Graphene-Immobilized fac-Re(bipy)(CO)3 Cl for Syngas Generation from Carbon Dioxide". United States. https://doi.org/10.1021/acsami.5b11958. https://www.osti.gov/servlets/purl/1330243.
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@article{osti_1330243,
title = {Graphene-Immobilized fac-Re(bipy)(CO)3 Cl for Syngas Generation from Carbon Dioxide},
author = {Zhou, Xin and Micheroni, Daniel and Lin, Zekai and Poon, Christopher and Li, Zhong and Lin, Wenbin},
abstractNote = {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.},
doi = {10.1021/acsami.5b11958},
journal = {ACS Applied Materials and Interfaces},
number = 6,
volume = 8,
place = {United States},
year = {Fri Jan 22 00:00:00 EST 2016},
month = {Fri Jan 22 00:00:00 EST 2016}
}
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https://doi.org/10.1021/acsami.5b11958
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Figures / Tables:

Scheme 1 Scheme 1: The synthesis of 4-amino-bipy.
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