Tracking a common surface-bound intermediate during CO2-to- fuels catalysis

Anna Wuttig, Can Liu, Qiling Peng, Momo Yaguchi, Christopher H. Hendon, Kenta Motobayashi, Shen Ye, Masatoshi Osawa, Yogesh Surendranath

研究成果: Article査読

117 被引用数 (Scopus)

抄録

Rational design of selective CO2-to-fuels electrocatalysts requires direct knowledge of the electrode surface structure during turnover. Metallic Cu is the most versatile CO2-to-fuels catalyst, capable of generating a wide array of value-added products, including methane, ethylene, and ethanol. All of these products are postulated to form via a common surface-bound CO intermediate. Therefore, the kinetics and thermodynamics of CO adsorption to Cu play a central role in determining fuel-formation selectivity and efficiency, highlighting the need for direct observation of CO surface binding equilibria under catalytic conditions. Here, we synthesize nanostructured Cu films adhered to IR-transparent Si prisms, and we find that these Cu surfaces enhance IR absorption of bound molecules. Using these films as electrodes, we examine Cu-catalyzed CO2 reduction in situ via IR spectroelectrochemistry. We observe that Cu surfaces bind electrogenerated CO, derived from CO2, beginning at -0.60 V vs RHE with increasing surface population at more negative potentials. Adsorbed CO is in dynamic equilibrium with dissolved 13CO and exchanges rapidly under catalytic conditions. The CO adsorption profiles are pH independent, but adsorbed CO species undergo a reversible transformation on the surface in modestly alkaline electrolytes. These studies establish the potential, concentration, and pH dependencies of the CO surface population on Cu, which serve to maintain a pool of this vital intermediate primed for further reduction to higher order fuel products.

本文言語English
ページ(範囲)522-528
ページ数7
ジャーナルACS Central Science
2
8
DOI
出版ステータスPublished - 2016 8 24
外部発表はい

ASJC Scopus subject areas

  • 化学 (全般)
  • 化学工学(全般)

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