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Integration of Plasmonic Ag(I) Clusters and Fe(II) Porphyrinates into Metal–Organic Frameworks for Efficient Photocatalytic CO2 Reduction Coupling with Photosynthesis of Pure H2O2.

Authors :
Chen, Hui‐Ying
Huang, Jia‐Run
Liu, Jia‐Chuan
Huang, Ning‐Yu
Chen, Xiao‐Ming
Liao, Pei‐Qin
Source :
Angewandte Chemie; 11/18/2024, Vol. 136 Issue 47, p1-7, 7p
Publication Year :
2024

Abstract

Efficient photocatalytic CO2 reduction coupled with the photosynthesis of pure H2O2 is a challenging and significant task. Herein, using classical CO2 photoreduction site iron porphyrinate as the linker, Ag(I) clusters were spatially separated and evenly distributed within a new metal–organic framework (MOF), namely Ag27TPyP‐Fe. With water as electron donors, Ag27TPyP‐Fe exhibited remarkable performances in artificial photosynthetic overall reaction with CO yield of 36.5 μmol g−1 h−1 and ca. 100 % selectivity, as well as H2O2 evolution rate of 35.9 μmol g−1 h−1. Since H2O2 in the liquid phase can be more readily separated from the gaseous products of CO2 photoreduction, high‐purity H2O2 with a concentration up to 0.1 mM was obtained. Confirmed by theoretical calculations and the established energy level diagram, the reductive iron(II) porphyrinates and oxidative Ag(I) clusters within an integrated framework functioned synergistically to achieve artificial photosynthesis. Furthermore, photoluminescence spectroscopy and photoelectrochemical measurements revealed that the robust connection of Ag(I) clusters and iron porphyrinate ligands facilitated efficient charge separation and rapid electron transfer, thereby enhancing the photocatalytic activity. [ABSTRACT FROM AUTHOR]

Details

Language :
English
ISSN :
00448249
Volume :
136
Issue :
47
Database :
Complementary Index
Journal :
Angewandte Chemie
Publication Type :
Academic Journal
Accession number :
180803137
Full Text :
https://doi.org/10.1002/ange.202412553