TY - JOUR
T1 - A Porphyrin/Graphene Framework
T2 - A Highly Efficient and Robust Electrocatalyst for Carbon Dioxide Reduction
AU - Choi, Jay
AU - Wagner, Pawel
AU - Jalili, Rouhollah
AU - Kim, Jeonghun
AU - MacFarlane, Douglas R.
AU - Wallace, Gordon G.
AU - Officer, David L.
PY - 2018/9/14
Y1 - 2018/9/14
N2 -
Developing immobilized molecular complexes, which demonstrate high product efficiencies at low overpotential in the electrochemical reduction of CO
2
in aqueous media, is essential for the practical production of reduction products. In this work, a simple and facile self-assembly method is demonstrated by electrostatic interaction and π–π stacking for the fabrication of a porphyrin/graphene framework (FePGF) composed of Fe(III) tetraphenyltrimethylammonium porphyrin and reduced liquid crystalline graphene oxide that can be utilized for the electrocatalytic reduction of CO
2
to CO on a glassy carbon electrode in aqueous electrolyte. The FePGF results in an outstanding robust catalytic performance for the production of CO with 97.0% faradaic efficiency at an overpotential of 480 mV and superior long-term stability relative to other heterogeneous molecular complexes of over 24 h (cathodic energy efficiency: 58.1%). In addition, a high surface area carbon fiber paper is used as a substrate for FePGF catalyst, resulting in enhanced current density of 1.68 mA cm
−2
with 98.7% CO faradaic efficiency at an overpotential of 430 mV for 10 h, corresponding to a turnover frequency of 2.9 s
−1
and 104 400 turnover number. Furthermore, FePGF/CFP has one of the highest cathodic energy efficiencies (60.9%) reported for immobilized metal complex catalysts.
AB -
Developing immobilized molecular complexes, which demonstrate high product efficiencies at low overpotential in the electrochemical reduction of CO
2
in aqueous media, is essential for the practical production of reduction products. In this work, a simple and facile self-assembly method is demonstrated by electrostatic interaction and π–π stacking for the fabrication of a porphyrin/graphene framework (FePGF) composed of Fe(III) tetraphenyltrimethylammonium porphyrin and reduced liquid crystalline graphene oxide that can be utilized for the electrocatalytic reduction of CO
2
to CO on a glassy carbon electrode in aqueous electrolyte. The FePGF results in an outstanding robust catalytic performance for the production of CO with 97.0% faradaic efficiency at an overpotential of 480 mV and superior long-term stability relative to other heterogeneous molecular complexes of over 24 h (cathodic energy efficiency: 58.1%). In addition, a high surface area carbon fiber paper is used as a substrate for FePGF catalyst, resulting in enhanced current density of 1.68 mA cm
−2
with 98.7% CO faradaic efficiency at an overpotential of 430 mV for 10 h, corresponding to a turnover frequency of 2.9 s
−1
and 104 400 turnover number. Furthermore, FePGF/CFP has one of the highest cathodic energy efficiencies (60.9%) reported for immobilized metal complex catalysts.
KW - electrochemical CO reduction
KW - graphene frameworks
KW - heterogeneous catalysts
KW - water-soluble porphyrins
UR - http://www.scopus.com/inward/record.url?scp=85050860864&partnerID=8YFLogxK
U2 - 10.1002/aenm.201801280
DO - 10.1002/aenm.201801280
M3 - Article
AN - SCOPUS:85050860864
VL - 8
JO - Advanced Energy Materials
JF - Advanced Energy Materials
SN - 1614-6840
IS - 26
M1 - 1801280
ER -