Constructing an Active Sulfur-Vacancy-Rich Surface for Selective *CH3-CH3 Coupling in CO2-to-C2H6 Conversion With 92% Selectivity

Constructing an Active Sulfur-Vacancy-Rich Surface for Selective *CH3-CH3 Coupling in CO2-to-C2H6 Conversion With 92% Selectivity

© 2024 Wiley‐VCH GmbH.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - 37(2025), 1 vom: 06. Jan., Seite e2412299
1. Verfasser: Yang, Xiaonan (VerfasserIn)
Weitere Verfasser: Ren, Liteng, Chen, Zhiheng, Li, Huiquan, Yuan, Yupeng
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2025
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article *CH3‐CH3 coupling S vacancies ethane photocatalytic CO2 reduction reaction
Beschreibung
Zusammenfassung:© 2024 Wiley‐VCH GmbH.
To achieve high selectivity in photocatalytic CO2 reduction to C2+ products, increasing the number of CO2 adsorption sites and lowering the energy barriers for key intermediates are critical. A ZnIn2S4 (ZIS)/MoO3-x (Z-M) photocatalyst is presented, in which plasmonic MoO3-x generates hot electrons, creating a multielectron environment in ZIS that facilitates efficient C─C coupling reactions. Density functional theory (DFT) calculations reveal that MoO3-x reduces the formation energy of sulfur vacancies (SV) in ZIS, thereby enhancing CO2 adsorption and activation. The SV-rich surface lowers the energy barrier for forming HCOO* to -0.33 eV whereas the energy barrier for forming *COOH is 0.77 eV. Successive hydrogenation of HCOO* leads to *CH2, which converts to *CH3 with an energy barrier of -0.63 eV. The energy barrier for *CH3-CH3 coupling is 0.54 eV, which is lower than the 0.73 eV for *CH2-CH2 coupling to form *C2H4. Thus, Z-M preferentially produces C2H6 over C2H4. Under visible light, Z-M achieves a CO2-to-C2H6 conversion rate of 467.3 µmol g-1 h-1 with 92.0% selectivity. This work highlights the dual role of plasmonic photocatalysts in enhancing CO2 adsorption and improving C2+ production in CO2 reduction
Beschreibung:Date Revised 08.01.2025
published: Print-Electronic
Citation Status PubMed-not-MEDLINE
ISSN:1521-4095
DOI:10.1002/adma.202412299