Premium
Atomic‐Scale Spacing between Copper Facets for the Electrochemical Reduction of Carbon Dioxide
Author(s) -
Jeong Hyung Mo,
Kwon Youngkook,
Won Jong Ho,
Lum Yanwei,
Cheng MuJeng,
Kim Kwang Ho,
HeadGordon Martin,
Kang Jeung Ku
Publication year - 2020
Publication title -
advanced energy materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.08
H-Index - 220
eISSN - 1614-6840
pISSN - 1614-6832
DOI - 10.1002/aenm.201903423
Subject(s) - faraday efficiency , copper , materials science , electrochemistry , electrochemical reduction of carbon dioxide , selectivity , catalysis , metal , absorption (acoustics) , density functional theory , carbon dioxide , lithium (medication) , nanoparticle , analytical chemistry (journal) , inorganic chemistry , nanotechnology , carbon monoxide , chemistry , electrode , computational chemistry , metallurgy , organic chemistry , composite material , medicine , endocrinology
Copper (Cu) offers a means for producing value‐added fuels through the electrochemical reduction of carbon dioxide (CO 2 ), i.e., the CO 2 reduction reaction (CO 2 RR), but designing Cu catalysts with significant Faradaic efficiency to C 2+ products remains as a great challenge. This work demonstrates that the high activity and selectivity of Cu to C 2+ products can be achieved by atomic‐scale spacings between two facets of Cu particles. These spacings are created by lithiating CuO x particles, removing lithium oxides formed, and electrochemically reducing CuO x to metallic Cu. Also, the range of spacing ( d s ) is confirmed via the 3D tomographs using the Cs‐corrected scanning transmission electron microscopy (3D tomo‐STEM), and the operando X‐ray absorption spectra show that oxidized Cu reduces to the metallic state during the CO 2 RR. Moreover, control of d s to 5–6 Å allows a current density exceeding that of unmodified CuO x nanoparticles by about 12 folds and a Faradaic efficiency of ≈80% to C 2+ . Density functional theory calculations support that d s of 5–6 Å maximizes the binding energies of CO 2 reduction intermediates and promotes C–C coupling reactions. Consequently, this study suggests that control of d s can be used to realize the high activity and C 2+ product selectivity for the CO 2 RR.