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. 2016 Dec 13:7:13869.
doi: 10.1038/ncomms13869.

A metal-free electrocatalyst for carbon dioxide reduction to multi-carbon hydrocarbons and oxygenates

Jingjie Wu  1 , Sichao Ma  2   3 , Jing Sun  4 , Jake I Gold  2 , ChandraSekhar Tiwary  1 , Byoungsu Kim  2   3 , Lingyang Zhu  2 , Nitin Chopra  5 , Ihab N Odeh  5 , Robert Vajtai  1 , Aaron Z Yu  2 , Raymond Luo  2 , Jun Lou  1 , Guqiao Ding  4 , Paul J A Kenis  2   3 , Pulickel M Ajayan  1
Affiliations

A metal-free electrocatalyst for carbon dioxide reduction to multi-carbon hydrocarbons and oxygenates

Jingjie Wu et al. Nat Commun. .

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.

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Figures

Figure 1
Figure 1. Nanostructure and specific nitrogen dopant configurations of NGQDs.
(a) Low-magnification TEM image of NGQDs. Scale bar, 50 nm. (b) High-magnification TEM image of NGQDs. Scale bar, 2 nm. Inset shows a single NGQD containing zigzag edges as circled. The yellow line outlines the zigzag edge. Scale bar in inset, 1 nm. (c) Raman spectrum of NGQDs as compared with that of pristine GQDs. (d) High-resolution N 1s spectrum for NGQDs, deconvoluted into three sub-peaks representing pyridinic, pyrrolic and graphitic N. The value in parentheses is the corresponding N atomic concentration calculated based on N/(N+C). The inset is a schematic demonstrating zigzag edges and the N-bonding configuration with respect to pyridinic (black), pyrrolic (blue) and graphitic (pink) N. In comparison, the N 1s peak does not appear in GQDs sample.
Figure 2
Figure 2. Electrocatalytic activity of carbon nanostructures towards CO2 reduction.
(a) FEs of carbon monoxide (CO), methane (CH4), ethylene (C2H4), formate (HCOO−), ethanol (EtOH), acetate (AcO−) and n-propanol (n-PrOH) at various applied cathodic potential for NGQDs. (b) FE of CO2 reduction products for pristine GQDs. (c) Selectivity to CO2 reduction products for NRGOs. (d) Tafel plots of partial current density of CO2 reduction versus applied cathodic potential for three nanostructured carbon catalysts. The error bar represents the s.d. of three separate measurements for an electrode.
Figure 3
Figure 3. Partial current densities as a function of cathode potential for various products from electrochemical CO2 reduction.
(a) When using NGQDs as cathode catalyst. (b) When using GQDs as cathode catalyst.
See this image and copyright information in PMC

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