Journal
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
Volume 305, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2022.121069
Keywords
Stacking design; Interfacial charge polarization; Photocatalysis; CO2 reduction; Surface and interfacial engineering
Funding
- National Natural Science Foundation of China [21603191, 21803063]
- Zhejiang Provincial Natural Science Foundation of China [LY20B030003, LQ16B010001]
- Public Welfare Technology Application Research Plan Project of Zhejiang Province (Analysis Test Item) [2017C37024]
- Foundation of Science and Technology Bureau of Jinhua [20204185]
- Self-Topic Fund of Zhejiang Normal University [2020ZS04]
- Open Research Fund of Key Laboratory of the Ministry of Education
- Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces, Zhejiang Normal University
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This study reports a layered graphene/Pd@PtCu nanostructure for high-efficient CO2-to-CH4 photoreduction. The smart design utilizes the excitation of Ru complex with broad visible absorption, smooth movement of photoelectrons, and highly selective CO2 reduction on the PtCu surface. The improved photocatalytic performance is achieved through cooperative surface and interfacial modulations.
Photocatalytic conversion of CO2 to chemical feedstocks represents an intriguing approach to address the energy and environmental crisis, but faces low conversion efficiencies resulted from unsatisfied light absorption, charge recombination and surface reactivity of traditional semiconductor photocatalysts. Herein, we report stacked graphene/Pd@PtCu nanostructures with atomically thin PtCu shell to overcome above challenges and realize high-efficient CO2-to-CH4 photoreduction. The smart design begins with the excitation of Ru complex with broad visible absorption, which is followed by the smooth movement of photoelectrons via the graphene & RARR;Pd & RARR;PtCu pathway, and then the highly selective CO2 reduction on the PtCu surface. As the PtCu thickness decreases, the strengthened Pd-PtCu interfacial charge polarization contributes to improved charge separation/migration. Meanwhile, CO2 adsorption on the PtCu surface is ameliorated owing to increased electron accumulation and compressive strain. This work provides a new design for boosting the photocatalytic performance by cooperative surface and interfacial modulations.
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