Stability of Residual Oxides in Oxide‐Derived Copper Catalysts for Electrochemical CO 2 Reduction Investigated with 18 O Labeling

Lum, Yanwei; Ager, Joel W.

doi:10.1002/ange.201710590

Title: Stability of Residual Oxides in Oxide‐Derived Copper Catalysts for Electrochemical CO ₂ Reduction Investigated with ¹⁸ O Labeling

Abstract

Abstract Oxide‐derived (OD) Cu catalysts have high selectivity towards the formation of multi‐carbon products (C ₂ /C ₃ ) for aqueous electrochemical CO ₂ reduction (CO ₂ R). It has been proposed that a large fraction of the initial oxide can be surprisingly resistant to reduction, and these residual oxides play a crucial catalytic role. The stability of residual oxides was investigated by synthesizing ¹⁸ O‐enriched OD Cu catalysts and testing them for CO ₂ R. These catalysts maintain a high selectivity towards C ₂ /C ₃ products (ca. 60 %) for up to 5 h in 0.1 m KHCO ₃ at −1.0 V vs. RHE. However, secondary‐ion mass spectrometry measurements show that only a small fraction (<1 %) of the original ¹⁸ O content remains, showing that residual oxides are not present in significant amounts during CO ₂ R. Furthermore, we show that OD Cu can reoxidize rapidly, which could compromise the accuracy of ex situ methods for determining the true oxygen content.

Authors:

^[1];

^[1]

Joint Center for Artificial Photosynthesis and Materials Sciences Division Lawrence Berkeley National Laboratory Berkeley CA 94720 USA, Department of Materials Science and Engineering University of California Berkeley CA 94720 USA

Publication Date:: Fri Dec 08 00:00:00 EST 2017

Sponsoring Org.:: USDOE

OSTI Identifier:: 1412579

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: Angewandte Chemie

Additional Journal Information:: Journal Name: Angewandte Chemie Journal Volume: 130 Journal Issue: 2; Journal ID: ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)

Country of Publication:: Germany

Language:: English

Citation Formats


                    Lum, Yanwei, and Ager, Joel W. Stability of Residual Oxides in Oxide‐Derived Copper Catalysts for Electrochemical CO 2 Reduction Investigated with 18 O Labeling.  Germany: N. p., 2017. 
Web.  doi:10.1002/ange.201710590.

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                    Lum, Yanwei, & Ager, Joel W. Stability of Residual Oxides in Oxide‐Derived Copper Catalysts for Electrochemical CO 2 Reduction Investigated with 18 O Labeling.  Germany.  https://doi.org/10.1002/ange.201710590

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                    Lum, Yanwei, and Ager, Joel W. Fri .  
"Stability of Residual Oxides in Oxide‐Derived Copper Catalysts for Electrochemical CO 2 Reduction Investigated with 18 O Labeling".  Germany.  https://doi.org/10.1002/ange.201710590.

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@article{osti_1412579,

  title        = {Stability of Residual Oxides in Oxide‐Derived Copper Catalysts for Electrochemical CO 2 Reduction Investigated with 18 O Labeling},

  author       = {Lum, Yanwei and Ager, Joel W.},

  abstractNote = {Abstract Oxide‐derived (OD) Cu catalysts have high selectivity towards the formation of multi‐carbon products (C 2 /C 3 ) for aqueous electrochemical CO 2 reduction (CO 2 R). It has been proposed that a large fraction of the initial oxide can be surprisingly resistant to reduction, and these residual oxides play a crucial catalytic role. The stability of residual oxides was investigated by synthesizing 18 O‐enriched OD Cu catalysts and testing them for CO 2 R. These catalysts maintain a high selectivity towards C 2 /C 3 products (ca. 60 %) for up to 5 h in 0.1  m KHCO 3 at −1.0 V vs. RHE. However, secondary‐ion mass spectrometry measurements show that only a small fraction (<1 %) of the original 18 O content remains, showing that residual oxides are not present in significant amounts during CO 2 R. Furthermore, we show that OD Cu can reoxidize rapidly, which could compromise the accuracy of ex situ methods for determining the true oxygen content.},

  doi          = {10.1002/ange.201710590},

  journal      = {Angewandte Chemie},

  number       = 2,

  volume       = 130,

  place        = {Germany},

  year         = {Fri Dec 08 00:00:00 EST 2017},

  month        = {Fri Dec 08 00:00:00 EST 2017}

}

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Title: Stability of Residual Oxides in Oxide‐Derived Copper Catalysts for Electrochemical CO 2 Reduction Investigated with 18 O Labeling

Abstract

Citation Formats

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