Synergistic Effect of Atomically Dispersed Ni-Zn Pair Sites for Enhanced CO2 Electroreduction
© 2021 Wiley-VCH GmbH.
| Publié dans: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 33(2021), 41 vom: 18. Okt., Seite e2102212 |
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| Auteur principal: | |
| Autres auteurs: | , , , , , , , , , |
| Format: | Article en ligne |
| Langue: | English |
| Publié: |
2021
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| Accès à la collection: | Advanced materials (Deerfield Beach, Fla.) |
| Sujets: | Journal Article atomic-level Ni-Zn pair sites enhanced CO2 electroreduction kinetic pathways mechanistic understanding synergistic effects thermodynamic pathways |
| Résumé: | © 2021 Wiley-VCH GmbH. Dual-atom catalysts have the potential to outperform the well-established single-atom catalysts for the electrochemical conversion of CO2 . However, the lack of understanding regarding the mechanism of this enhanced catalytic process prevents the rational design of high-performance catalysts. Herein, an obvious synergistic effect in atomically dispersed Ni-Zn bimetal sites is observed. In situ characterization combined with density functional theory (DFT) calculations reveals that heteronuclear coordination modifies the d-states of the metal atom, narrowing the gap between the d-band centre (εd ) of the Ni (3d) orbitals and the Fermi energy level (EF ) to strengthen the electronic interaction at the reaction interface, resulting in a lower free energy barrier (ΔG) in the thermodynamic pathway and a reduced activation energy (Ea ) as well as fortified metal-C bonding in the kinetic pathway. Consequently, a CO faradaic efficiency of >90% is obtained across a broad potential window from -0.5 to -1.0 V (vs RHE), reaching a maximum of 99% at -0.8 V, superior to that of the Ni/Zn single-metal sites |
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| Description: | Date Revised 13.10.2021 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
| ISSN: | 1521-4095 |
| DOI: | 10.1002/adma.202102212 |