Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 14, Issue 24, Pages 27882-27890Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c05654
Keywords
photosensitizers; polyoxometalates; POM-based metal-organic frameworks; photocatalytic; oxidative coupling of amines
Funding
- National Natural Science Foundation of China [22071044, 22171071, 21571050, 21771054]
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Researchers have developed two crystalline metal-organic frameworks based on polyoxometalate, which enhance light absorption and carrier separation efficiency. These frameworks also demonstrate excellent photocatalytic activity.
Photocatalytic technology is widely studied, while it comes with drawbacks such as low sunlight utilization efficiency and high carrier recombination rates. Herein, for the first time, we present two crystalline polyoxometalate (POM)-based metal-organic frameworks (POMOFs), {[Cd(DMF)(2)Ru(bpy)(2)(dcbpy)](2)(POMs)(DMF)2} xDMF (PMo-1, POMs = [(PMo11MoO40)-Mo-VI-O-V](4-), x = 5; SiW-2, POMs = [SiW12O40](4-), x = 4) through assembling the photosensitizer [Ru(bpy)(2)(H(2)dcbpy)]Cl-2 and POMs into a single framework. The assembly not only enhances light absorption in the visible light regime but also improves carrier separation efficiency; atop of that, both POMOFs demonstrate activities in the photocatalytic oxidative coupling of amines. Particularly, PMo-1 enables the quantitative completion of oxidative coupling of benzylamine reaction within 30 min (yield = 99.6%) with a high turnover frequency (TOF = 6631.6 h(-1)). To our knowledge, the PMo-1 catalyst outperforms any other photocatalysts previously reported in similar use cases where TOF values were usually obtained <2000 h(-1).
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