期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 43, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202211848
关键词
CO2 Reduction; Core-Shell Composites; Photocatalysis; Zr-MOFs; In Situ Spectroscopies
资金
- CSC [201706140196]
- CNRS
- European Union [837975, EUR2020-112294]
- Spanish Ministry of Science and Innovation for a Ramon y Cajal fellowship [RYC2018-024328-I]
- MCIN/AEI
- FPI-UAM fellowship UAM
- Shenzhen Key Laboratory of Micro/Nano-Porous Functional Materials (SKLPM) [ZDSYS20210709112802010]
- H2020 Societal Challenges Programme [837975] Funding Source: H2020 Societal Challenges Programme
This study successfully encapsulates ultrasmall Cu nanoparticles inside Zr-MOFs to form core-shell composites, which exhibit enhanced reactivity compared to Cu nanoparticles confined in the pores of MOFs. Introducing polar groups on the MOF structure further improves catalytic reactivity and selectivity. Mechanistic investigation reveals the active role of Cu-I sites at the interface between Cu nanoparticles and the support in CO2 photoreduction.
Encapsulating ultrasmall Cu nanoparticles inside Zr-MOFs to form core-shell architecture is very challenging but of interest for CO2 reduction. We report for the first time the incorporation of ultrasmall Cu NCs into a series of benchmark Zr-MOFs, without Cu NCs aggregation, via a scalable room temperature fabrication approach. The Cu NCs@MOFs core-shell composites show much enhanced reactivity in comparison to the Cu NCs confined in the pore of MOFs, regardless of their very similar intrinsic properties at the atomic level. Moreover, introducing polar groups on the MOF structure can further improve both the catalytic reactivity and selectivity. Mechanistic investigation reveals that the Cu-I sites located at the interface between Cu NCs and support serve as the active sites and efficiently catalyze CO2 photoreduction. This synergetic effect may pave the way for the design of low-cost and efficient catalysts for CO2 photoreduction into high-value chemical feedstock.
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