Multifunctional composite materials are currently highly desired for sustainable energy applications. A general strategy to integrate atomically precise Au (SG) with ZIF-8 (Zn(MeIm) , MeIm = 2-methylimidazole), is developed via the typical Zn-carboxylate type of linkage. Au (SG) are uniformly encapsulated into a ZIF-8 framework (Au (SG) @ZIF-8) by coordination-assisted self-assembly. In contrast, Au (SG) integrated by simple impregnation is oriented along the outer surface of ZIF-8 (Au (SG) /ZIF-8). The porous structure and thermal stability of these nanocomposites are characterized by N adsorption-desorption isothermal analysis and thermal gravimetric analysis. The distribution of Au (SG) in the two nanocomposites is confirmed by electron microscopy, and the accessibility of Au (SG) is evaluated by the 4-nitrophenol reduction reaction. The as-prepared nanocomposites retain the high porosity and thermal stability of the ZIF-8 matrix, while also exhibiting the desired catalytic and optical properties derived from the integrated Au (SG) nanoclusters (NCs). Au (SG) @ZIF-8 with isolated Au sites is a promising heterogenous catalyst with size selectivity imparted by the ZIF-8 matrix. The structural distinction between Au (SG) @ZIF-8 and Au (SG) /ZIF-8 determines their different emission features, and provides a new strategy to adjust the optical behavior of Au (SG) for applications in bioimaging and biotherapy.
Hydrogenated ZnO nanorod arrays (NRAs) grown on F-doped SnO(2) (FTO) glass substrates yield a benchmark specific hydrogen production rate of 122,500 μmol h(-1) g(-1), and exhibit excellent stability and recyclability.
Photocatalytic water splitting is a natural but challenging chemical way of harnessing renewable solar power to generate clean hydrogen energy. Here we report a potential hydrogen-evolving photochemical molecular device based on a self-assembled ruthenium–palladium heterometallic coordination cage, incorporating multiple photo- and catalytic metal centres. The photophysical properties are investigated by absorption/emission spectroscopy, electrochemical measurements and preliminary DFT calculations and the stepwise electron transfer processes from ruthenium-photocentres to catalytic palladium-centres is probed by ultrafast transient absorption spectroscopy. The photocatalytic hydrogen production assessments reveal an initial reaction rate of 380 μmol h−1 and a turnover number of 635 after 48 h. The efficient hydrogen production may derive from the directional electron transfers through multiple channels owing to proper organization of the photo- and catalytic multi-units within the octahedral cage, which may open a new door to design photochemical molecular devices with well-organized metallosupramolecules for homogenous photocatalytic applications.
This work aims to investigate the role that defect states play in photoelectric and photocatalytic processes. Ternary Zn x Cd 1Àx S with wurtzite structure is firstly synthesized, and then the defect is characterized by photoluminescence (PL) spectroscopy. It is found that the photoelectrons trapped in surface defect states exhibit different behavior in the processes of photoelectric transfer and photocatalytic hydrogen evolution. During the photocatalytic process, the surface defect states in Zn x Cd 1Àx S act as the electron pool to improve the photocatalytic activity of water-splitting reaction. In comparison, the surface defect states serve as the recombination center that decreases the efficiency of photoelectric transfer. This finding is of great significance for the design of effective photoelectric and photocatalytic material in the field of solar energy conversion.
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