Abstract
Herein, we reported a octahedral Cd3(C3N3S3)2 coordination polymer as a new noble metal-free photocatalyst for robust photocatalytic H2O2 production from methanol/water solution. The coordination polymer can give an unprecedented H2O2 yield of ca. 110.0 mmol • L−1 • g−1 at pH = 2.8 under visible light illumination. The characterization results clearly revealed that the photocatalytic H2O2 production proceeds by a pathway of two-electron reduction of O2 on the catalyst surface. This work showed the potential perspective of Mx(C3N3S3)y (M = transitional metals) coordination polymers as a series of new materials for solar energy storage and conversion.
Highlights
We reported a octahedral Cd3(C3N3S3)[2] coordination polymer as a new noble metal-free photocatalyst for robust photocatalytic H2O2 production from methanol/water solution
By suppressing the back reaction, the photocatalytic H2O2 yield can be upgraded to a millimolar level over a surface-fluorinated TiO2, but along with a large amount of fluorine contaminant emitted into the aqueous solution[18]
It appears that the triangular surface of these octahedrons is sporadically covered by some irregular-shaped nanoparticles, which suggests that the formation of the octahedral nanocrystals maybe follow the “Oriented attachment” mechanism, just similar to the case of a previous work by Zeng and coworkers[29]
Summary
It appears that the H2O2 amount produced in the system decreases with increasing the incident light wavelength, matching well with the optical spectrum This result clearly indicates that the H2O2 production is intrinsically a photocatalytic process driven by photoexcitation of the coordination polymer semiconductor. Its crystal structure does not change after photocatalytic reaction, as shown in Fig. S10 (Supporting Information) Those results indicate that the Cd3(TMT)[2] polymer is able to serve as a stable, reusable photocatalyst for H2O2 generation from methanol/water solution. This work shows the potential promising of the transitional metal coordination polymers in solar energy storage and conversion, especially organic photosynthesis
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