Atomically precise metal nanoclusters (NCs) have recently been unleashed as an emerging sector of metal nanomaterials but suffer from light-induced poor stability, giving rise to the detrimental self-transformation to metal nanocrystals (NYs), losing the photosensitization effect and ultimately retarding their widespread applications in photoredox catalysis. Are the metal NCs definitely superior to metal NYs in heterogeneous photocatalysis in terms of structural merits? To unlock this mystery, herein, we conceptually demonstrate how to rationally manipulate the instability of metal NCs to construct high-efficiency artificial photosystems and unleash how the metal NYs self-transformed from metal NCs influence the charge transfer in photoredox selective organic transformation. To our surprise, the results indicate that the Schottky-type electron-trapping ability of Au NYs surpasses the photosensitization effect of glutathione (GSH)-protected Au clusters [Au25(GSH)18 NCs] in mediating the charge separation and enhancing the photoactivities towards selective photoreduction of aromatic nitro compounds to amino derives and photocatalytic oxidation of aromatic alcohols to aldehydes under visible light irradiation. This work strategically provides new insights into the inherent instability of metal NCs utilized for photocatalysis and reinforce our fundamental understanding on metal NCs-based artificial photosystems for solar energy conversion.

This article is Open Access

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