Electrochemical Activation of CO2 through Atomic Ordering Transformations of AuCu Nanoparticles

作者：Dohyung Kim, Chenlu Xie, Nigel Becknell, Yi Yu, Mohammadreza Karamad, Karen Chan, Ethan J. Crumlin, Jens K. Nørskov, Peidong Yang · 发表于：Journal of the American Chemical Society · 年份：2017 · DOI：10.1021/jacs.7b03516 · 被引用次数：678 · 研究领域：CO2 Reduction Techniques and Catalysts、Electrocatalysts for Energy Conversion、Advanced battery technologies research

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 CO 2 reduction. In contrast to the disordered alloy NP, which is catalytically active for hydrogen evolution, ordered AuCu NPs selectively converted CO 2 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.