首页|Substituent Modulated Electronic Properties of Cu(Ⅰ)Active Site in Metal-Organic Halides for Boosting Hydrogen Evolution Reaction
Substituent Modulated Electronic Properties of Cu(Ⅰ)Active Site in Metal-Organic Halides for Boosting Hydrogen Evolution Reaction
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Development of heterogeneous molecular photocatalysts for promising light-driven hydrogen evolution reaction(HER)is highly de-manding but still challenging.Here,we report the blue-greenish emitting dinuclear metal-organic halides as photocatalyst by incor-porating site-specific single copper(Ⅰ)atoms that exhibit an efficient carbon-negative H2 production.Interestingly,the electronic prop-erties,including the spin and charge density of central Cu(Ⅰ)active site,can be triggered by substituent modulation in metal-organic halides,which greatly affect the exciton dissociation kinetics and thus the HER reactivity.The optimized spin density in these hetero-geneous photocatalysts drastically boosts the hydrogen production rate from 1250 to 3130 pmol·g-1·h-1.Our molecular strategy pro-vides a platform that rationally facilitates electronic modulation of copper(Ⅰ)atoms,tunes the macroscopic optoelectronic properties of photocatalystsand boosts carbon-negative HER activity,extending the boundaries of conventional molecular-based photocatalysts.
Metal-organic halidesPhotocatalysisHydrogen evolutionMicroenvironment modulationHybrid copper(Ⅰ)halidsLigand effectsSubstituent effectsSpin density
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