title: A metal-free electrocatalyst for carbon dioxide reduction to multi-carbon hydrocarbons and oxygenates.
abstract: Electroreduction of carbon dioxide into higher-energy liquid fuels and chemicals is a promising but challenging renewable energy conversion technology. Among the electrocatalysts screened so far for carbon dioxide reduction, which includes metals, alloys, organometallics, layered materials and carbon nanostructures, only copper exhibits selectivity towards formation of hydrocarbons and multi-carbon oxygenates at fairly high efficiencies, whereas most others favour production of carbon monoxide or formate. Here we report that nanometre-size N-doped graphene quantum dots (NGQDs) catalyse the electrochemical reduction of carbon dioxide into multi-carbon hydrocarbons and oxygenates at high Faradaic efficiencies, high current densities and low overpotentials. The NGQDs show a high total Faradaic efficiency of carbon dioxide reduction of up to 90%, with selectivity for ethylene and ethanol conversions reaching 45%. The C2 and C3 product distribution and production rate for NGQD-catalysed carbon dioxide reduction is comparable to those obtained with copper nanoparticle-based electrocatalysts.
authors.affiliation: Department of Materials Science and NanoEngineering, Rice University, 6100 Main Street, Houston, Texas 77005, USA.
authors.forename: Jingjie
authors.initials: J
authors.lastname: Wu
authors.affiliation: School of Chemical Sciences, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA.|International Institute for Carbon-Neutral Energy Research (WPI-I2CNER), Kyushu University, 744 Moto-oka, Nishi-ku, Fukuoka 819-0395, Japan.
authors.forename: Sichao
authors.initials: S
authors.lastname: Ma
authors.affiliation: State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, Shanghai 200050, China.
authors.forename: Jing
authors.initials: J
authors.lastname: Sun
authors.affiliation: School of Chemical Sciences, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA.
authors.forename: Jake I
authors.initials: JI
authors.lastname: Gold
authors.affiliation: Department of Materials Science and NanoEngineering, Rice University, 6100 Main Street, Houston, Texas 77005, USA.
authors.forename: ChandraSekhar
authors.initials: C
authors.lastname: Tiwary
authors.affiliation: School of Chemical Sciences, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA.|International Institute for Carbon-Neutral Energy Research (WPI-I2CNER), Kyushu University, 744 Moto-oka, Nishi-ku, Fukuoka 819-0395, Japan.
authors.forename: Byoungsu
authors.initials: B
authors.lastname: Kim
authors.affiliation: School of Chemical Sciences, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA.
authors.forename: Lingyang
authors.initials: L
authors.lastname: Zhu
authors.affiliation: Saudi Basic Industries Corporation (SABIC), Sugar Land, Texas 77478, USA.
authors.forename: Nitin
authors.initials: N
authors.lastname: Chopra
authors.affiliation: Saudi Basic Industries Corporation (SABIC), Sugar Land, Texas 77478, USA.
authors.forename: Ihab N
authors.initials: IN
authors.lastname: Odeh
authors.affiliation: Department of Materials Science and NanoEngineering, Rice University, 6100 Main Street, Houston, Texas 77005, USA.
authors.forename: Robert
authors.identifier: 0000-0002-3942-8827
authors.initials: R
authors.lastname: Vajtai
authors.affiliation: School of Chemical Sciences, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA.
authors.forename: Aaron Z
authors.initials: AZ
authors.lastname: Yu
authors.affiliation: School of Chemical Sciences, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA.
authors.forename: Raymond
authors.initials: R
authors.lastname: Luo
authors.affiliation: Department of Materials Science and NanoEngineering, Rice University, 6100 Main Street, Houston, Texas 77005, USA.
authors.forename: Jun
authors.initials: J
authors.lastname: Lou
authors.affiliation: State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, Shanghai 200050, China.
authors.forename: Guqiao
authors.initials: G
authors.lastname: Ding
authors.affiliation: School of Chemical Sciences, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA.|International Institute for Carbon-Neutral Energy Research (WPI-I2CNER), Kyushu University, 744 Moto-oka, Nishi-ku, Fukuoka 819-0395, Japan.
authors.forename: Paul J A
authors.initials: PJ
authors.lastname: Kenis
authors.affiliation: Department of Materials Science and NanoEngineering, Rice University, 6100 Main Street, Houston, Texas 77005, USA.
authors.forename: Pulickel M
authors.initials: PM
authors.lastname: Ajayan