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Atomic Layer Deposition of ZnO on CuO Enables Selective and Efficient Electroreduction of Carbon Dioxide to Liquid Fuels.

Abstract

Electrochemical reduction of carbon dioxide, if powered by renewable electricity, could serve as a sustainable technology for carbon recycling and energy storage. Among all the products, ethanol is an attractive liquid fuel. However, the maximum faradaic efficiency of ethanol is only ≈10 % on polycrystalline Cu. Here, CuZn bimetallic catalysts were synthesized by in situ electrochemical reduction of ZnO-shell/CuO-core bi-metal-oxide. Dynamic evolution of catalyst was revealed by STEM-EDS mapping, showing the migration of Zn atom and blending between Cu and Zn. CuZn bimetallic catalysts showed preference towards ethanol formation, with the ratio of ethanol/ethylene increasing over five times regardless of applied potential. We achieved 41 % faradaic efficiency for C2+ liquids with this catalyst. Transitioning from H-cell to an electrochemical flow cell, we achieved 48.6 % faradaic efficiency and -97 mA cm-2 partial current density for C2+ liquids at only -0.68 V versus reversible hydrogen electrode in 1 m KOH. Operando Raman spectroscopy showed that CO binding on Cu sites was modified by Zn. Free CO and adsorbed *CH3 are believed to combine and form *COCH3 intermediate, which is exclusively reduced to ethanol.

Authors+Show Affiliations

Laboratory of Photonics and Interfaces, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), 1015, Lausanne, Switzerland.Laboratory of Photonics and Interfaces, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), 1015, Lausanne, Switzerland.Laboratory of Photomolecular Science, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), 1015, Lausanne, Switzerland.Laboratory of Photomolecular Science, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), 1015, Lausanne, Switzerland.Laboratory of Photonics and Interfaces, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), 1015, Lausanne, Switzerland. Institute of Photoelectronic Thin Film Devices and Technology, College of Electronic Information and Optical Engineering, Nankai University, 300071, Tianjin, China.Laboratory of Photonics and Interfaces, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), 1015, Lausanne, Switzerland.Laboratory of Photomolecular Science, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), 1015, Lausanne, Switzerland.Laboratory of Photonics and Interfaces, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), 1015, Lausanne, Switzerland.

Pub Type(s)

Journal Article

Language

eng

PubMed ID

31433551

Citation

Ren, Dan, et al. "Atomic Layer Deposition of ZnO On CuO Enables Selective and Efficient Electroreduction of Carbon Dioxide to Liquid Fuels." Angewandte Chemie (International Ed. in English), 2019.
Ren D, Gao J, Pan L, et al. Atomic Layer Deposition of ZnO on CuO Enables Selective and Efficient Electroreduction of Carbon Dioxide to Liquid Fuels. Angew Chem Int Ed Engl. 2019.
Ren, D., Gao, J., Pan, L., Wang, Z., Luo, J., Zakeeruddin, S. M., ... Grätzel, M. (2019). Atomic Layer Deposition of ZnO on CuO Enables Selective and Efficient Electroreduction of Carbon Dioxide to Liquid Fuels. Angewandte Chemie (International Ed. in English), doi:10.1002/anie.201909610.
Ren D, et al. Atomic Layer Deposition of ZnO On CuO Enables Selective and Efficient Electroreduction of Carbon Dioxide to Liquid Fuels. Angew Chem Int Ed Engl. 2019 Aug 21; PubMed PMID: 31433551.
* Article titles in AMA citation format should be in sentence-case
TY - JOUR T1 - Atomic Layer Deposition of ZnO on CuO Enables Selective and Efficient Electroreduction of Carbon Dioxide to Liquid Fuels. AU - Ren,Dan, AU - Gao,Jing, AU - Pan,Linfeng, AU - Wang,Zaiwei, AU - Luo,Jingshan, AU - Zakeeruddin,Shaik M, AU - Hagfeldt,Anders, AU - Grätzel,Michael, Y1 - 2019/08/21/ PY - 2019/07/30/received PY - 2019/8/23/pubmed PY - 2019/8/23/medline PY - 2019/8/22/entrez KW - carbon dioxide KW - electrocatalysis KW - ethanol KW - flow cell KW - operando Raman spectroscopy JF - Angewandte Chemie (International ed. in English) JO - Angew. Chem. Int. Ed. Engl. N2 - Electrochemical reduction of carbon dioxide, if powered by renewable electricity, could serve as a sustainable technology for carbon recycling and energy storage. Among all the products, ethanol is an attractive liquid fuel. However, the maximum faradaic efficiency of ethanol is only ≈10 % on polycrystalline Cu. Here, CuZn bimetallic catalysts were synthesized by in situ electrochemical reduction of ZnO-shell/CuO-core bi-metal-oxide. Dynamic evolution of catalyst was revealed by STEM-EDS mapping, showing the migration of Zn atom and blending between Cu and Zn. CuZn bimetallic catalysts showed preference towards ethanol formation, with the ratio of ethanol/ethylene increasing over five times regardless of applied potential. We achieved 41 % faradaic efficiency for C2+ liquids with this catalyst. Transitioning from H-cell to an electrochemical flow cell, we achieved 48.6 % faradaic efficiency and -97 mA cm-2 partial current density for C2+ liquids at only -0.68 V versus reversible hydrogen electrode in 1 m KOH. Operando Raman spectroscopy showed that CO binding on Cu sites was modified by Zn. Free CO and adsorbed *CH3 are believed to combine and form *COCH3 intermediate, which is exclusively reduced to ethanol. SN - 1521-3773 UR - https://www.unboundmedicine.com/medline/citation/31433551/Atomic_Layer_Deposition_of_ZnO_on_CuO_Enables_Selective_and_Efficient_Electroreduction_of_Carbon_Dioxide_to_Liquid_Fuels L2 - https://doi.org/10.1002/anie.201909610 DB - PRIME DP - Unbound Medicine ER -