Format

Send to

Choose Destination
J Am Chem Soc. 2017 Jan 11;139(1):47-50. doi: 10.1021/jacs.6b10740. Epub 2016 Dec 27.

Electroreduction of Carbon Dioxide to Hydrocarbons Using Bimetallic Cu-Pd Catalysts with Different Mixing Patterns.

Author information

1
Dept. of Chemistry and Chemical and Biomolecular Engineering, UIUC , 600 S. Mathews Ave., Urbana, Illinois 61801, United States.
2
International Institute for Carbon-Neutral Energy Research (WPI-I2CNER), Kyushu University , 744 Moto-oka, Nishi-ku, Fukuoka 819-0395, Japan.
3
CREST, JST, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012, Japan.
4
Frederick Seitz Materials Research Laboratory, UIUC , 104 S. Goodwin Ave., Urbana, Illinois 61801, United States.

Abstract

Electrochemical conversion of CO2 holds promise for utilization of CO2 as a carbon feedstock and for storage of intermittent renewable energy. Presently Cu is the only metallic electrocatalyst known to reduce CO2 to appreciable amounts of hydrocarbons, but often a wide range of products such as CO, HCOO-, and H2 are formed as well. Better catalysts that exhibit high activity and especially high selectivity for specific products are needed. Here a range of bimetallic Cu-Pd catalysts with ordered, disordered, and phase-separated atomic arrangements (Cuat:Pdat = 1:1), as well as two additional disordered arrangements (Cu3Pd and CuPd3 with Cuat:Pdat = 3:1 and 1:3), are studied to determine key factors needed to achieve high selectivity for C1 or C2 chemicals in CO2 reduction. When compared with the disordered and phase-separated CuPd catalysts, the ordered CuPd catalyst exhibits the highest selectivity for C1 products (>80%). The phase-separated CuPd and Cu3Pd achieve higher selectivity (>60%) for C2 chemicals than CuPd3 and ordered CuPd, which suggests that the probability of dimerization of C1 intermediates is higher on surfaces with neighboring Cu atoms. Based on surface valence band spectra, geometric effects rather than electronic effects seem to be key in determining the selectivity of bimetallic Cu-Pd catalysts. These results imply that selectivities to different products can be tuned by geometric arrangements. This insight may benefit the design of catalytic surfaces that further improve activity and selectivity for CO2 reduction.

PMID:
27958727
DOI:
10.1021/jacs.6b10740

Supplemental Content

Full text links

Icon for American Chemical Society
Loading ...
Support Center