Journal
CHEMSUSCHEM
Volume 10, Issue 2, Pages 387-393Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.201601144
Keywords
carbon dioxide; electroreduction; density functional theory; solid liquid interface; intermediates
Funding
- Program for the Thousand Young Talents Plan
- Program for New Century Excellent Talents in University [NCET-13-0255]
- National Natural Science Foundation of China [21673095, 51631004]
Ask authors/readers for more resources
Cu demonstrates a unique capability towards CO2 electroreduction that can close the anthropogenic carbon cycle; however, its reaction mechanism remains elusive, owing to the obscurity of the solid-liquid interface on Cu surfaces where electrochemical reactions occur. Using a genetic algorithm method in addition to density functional theory, we explicitly identify the configuration of a water bilayer on Cu(211) and build electrochemical models. These enable us to reveal a mechanistic picture for CO2 electroreduction, finding the key intermediates CCO* for the C2H4 pathway and CH* for the CH4 pathway, which rationalize a series of experimental observations. Furthermore, we find that the interplay between the Cu surfaces, carbon monomers, and water network (but not the binding of CO*) essentially determine the unique capability of Cu towards CO2 electroreduction, proposing a new and effective descriptor for exploiting optimal catalysts.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available