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J Am Chem Soc. 2017 Jun 21;139(24):8329-8336. doi: 10.1021/jacs.7b03516. Epub 2017 Jun 7.

Electrochemical Activation of CO2 through Atomic Ordering Transformations of AuCu Nanoparticles.

Author information

1
Department of Materials Science and Engineering, University of California , Berkeley, California 94720, United States.
2
Kavli Energy Nanosciences Institute , Berkeley, California 94720, United States.
3
Department of Chemistry, University of California , Berkeley, California 94720, United States.
4
Department of Chemical Engineering, Stanford University , Stanford, California 94305, United States.
5
SLAC National Accelerator Laboratory , Menlo Park, California 94025, United States.
6
Advanced Light Source, Lawrence Berkeley National Laboratory , Berkeley, California 94720, United States.
7
Chemical Sciences Division, Lawrence Berkeley National Laboratory , Berkeley, California 94720, United States.

Abstract

Precise control of elemental configurations within multimetallic nanoparticles (NPs) could enable access to functional nanomaterials with significant performance benefits. This can be achieved down to the atomic level by the disorder-to-order transformation of individual NPs. Here, by systematically controlling the ordering degree, we show that the atomic ordering transformation, applied to AuCu NPs, activates them to perform as selective electrocatalysts for CO2 reduction. In contrast to the disordered alloy NP, which is catalytically active for hydrogen evolution, ordered AuCu NPs selectively converted CO2 to CO at faradaic efficiency reaching 80%. CO formation could be achieved with a reduction in overpotential of ∼200 mV, and catalytic turnover was enhanced by 3.2-fold. In comparison to those obtained with a pure gold catalyst, mass activities could be improved as well. Atomic-level structural investigations revealed three atomic gold layers over the intermetallic core to be sufficient for enhanced catalytic behavior, which is further supported by DFT analysis.

PMID:
28551991
DOI:
10.1021/jacs.7b03516

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