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Atomic Layer Deposition of ZnO on CuO Enables Selective and Efficient Electroreduction of Carbon Dioxide to Liquid Fuels
Author(s) -
Ren Dan,
Gao Jing,
Pan Linfeng,
Wang Zaiwei,
Luo Jingshan,
Zakeeruddin Shaik M.,
Hagfeldt Anders,
Grätzel Michael
Publication year - 2019
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201909610
Subject(s) - faraday efficiency , catalysis , electrochemistry , electrochemical reduction of carbon dioxide , bimetallic strip , chemical engineering , inorganic chemistry , reversible hydrogen electrode , chemistry , materials science , electrode , carbon monoxide , working electrode , organic chemistry , engineering
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 C 2+ 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 C 2+ 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 *CH 3 are believed to combine and form *COCH 3 intermediate, which is exclusively reduced to ethanol.