Journal
JOURNAL OF ENERGY CHEMISTRY
Volume 66, Issue -, Pages 68-73Publisher
ELSEVIER
DOI: 10.1016/j.jechem.2021.06.031
Keywords
Impurity on Cu film; Zr-based MOFs; Electrocatalysts; CO2 reduction; Hydrocarbon
Funding
- Basic Science Research Program of the National Research Foundation of Korea [NRF-2021R1A2C4001777, NRF-2021R1A2C2007823]
- Carbon to X Project - Ministry of Science and ICT, Republic of Korea [NRF-2020M3H7A1098231]
- Technology Innovation Program - Ministry of Trade, Industry & Energy (MOTIE), Republic of Korea [20013794]
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By forming a compensating layer of nano-sized metal-organic frameworks (MOFs) on copper film, the impact of iron impurities on the copper surface in CO2RR is effectively blocked, resulting in improved efficiency and selectivity in the production of hydrocarbons.
Copper (Cu) provides a cost-effective means of producing value-added fuels through the electrochemical reduction of carbon dioxide (CO2RR). However, we observed the production of hydrocarbons via CO2RR on commercial Cu films is less efficient because of the surface impurities, i.e., Fe. Carbon monoxide (CO), a reaction intermediate of CO2RR to hydrocarbons, binds strongly to the Fe sites and interrupts the production of hydrocarbons, resulting in an active hydrogen evolution reaction (HER). Herein, we report a method of blocking the effect of Fe impurities on the Cu surface through the preferential growth of nano-sized metal-organic frameworks (MOFs) on Fe site. When zirconium (Zr)-based MOFs (UiO-66) forms a compensating layer on Cu film via the terephthalic acid (TPA)-Fe coordination bond, the UiO66 coated Cu film (UiO-66@Cu) presents significantly improved hydrocarbon Faradaic efficiency (FE) of 37.59% compared to 14.68% FE on commercial Cu film (99.9% purity) by suppressing HER. According to X-ray photoelectron spectroscopy (XPS) analysis, the UiO-66 ligand binds to entire metallic Fe site on the Cu surface, while metallic Cu is retained. Thus, UiO-66@Cu provides active sites of Cu for CO2RR and leads to highly efficient and selective production of hydrocarbons. (C) 2021 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
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