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CO 2 Conversion on Ligand‐Protected Au 25 Nanoparticle: The Role of Structural Inhomogeneity in the Promotion of the Electrocatalytic Process
Author(s) -
Alfonso Dominic R.
Publication year - 2021
Publication title -
physica status solidi (b)
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.51
H-Index - 109
eISSN - 1521-3951
pISSN - 0370-1972
DOI - 10.1002/pssb.202000387
Subject(s) - nanoclusters , electrochemistry , catalysis , ligand (biochemistry) , adsorption , electrocatalyst , materials science , hydrogen , active site , combinatorial chemistry , chemistry , nanotechnology , chemical physics , electrode , organic chemistry , biochemistry , receptor
The possibility of direct integration with renewable electric sources adds more potential to the electrochemical method as a promising route for CO 2 conversion. Previous experimental breakthrough reveals that Au 25 (SR) 18 − nanoclusters having 25 gold atoms and 18 protecting thiolate ligands can be utilized as catalysts for CO 2 electroreduction to CO. The reason for its observed activity toward CO 2 conversion is of fundamental importance that needs to be explained. Herein, the progress made in the first‐principles mechanistic studies of the reduction process is described. Contrary to long‐standing assumptions, the fully ligand protected version is not the active catalyst because of the weak adsorption of the relevant intermediates. Instead, the calculations based on computational hydrogen electrode method reveal that the reduction process is facilitated by a thermodynamically stable yet structurally inhomogeneous active site. This reaction center binds the intermediates in such a way that the process can occur at low overpotentials. The results point to the role of inhomogeneity in the surface region for this class of materials as a critical factor promoting the CO 2 conversion process under electrochemical environment.