Ultrafast electron transfer from CdS quantum dots to atomically-dispersed Pt for enhanced H2 evolution and value-added chemical synthesis

Abstract

Photocatalytic hydrogen production is enchanting in solar energy utilization. And mechanism elucidation in interfacial electron transfer rate is a prerequisite for performance improvement. Herein, atomically dispersed Pt-modified CdS quantum dots (Pt-CdS QDs), prepared by a facile one-step in-situ deposited method, are used as a prototype. Benefiting from the maximized utilization of Pt cocatalyst as well as the strong electronic metal-support interaction, ultrafast electron transfer from CdS to Pt (∼1.7 ps) is achieved, as revealed by femtosecond transient absorption spectra. The optimal sample simultaneously realizes photocatalytic hydrogen evolution coupled with selective oxidation of 2-thiophene methanol (TM) into 2-thiophenecarboxaldehyde (TD). Specifically, it exhibits an enhanced H2-evolution rate, which is 70-fold higher than pristine CdS QDs. Moreover, a TM conversion rate of 95.3 % with a TD selectivity of 87.2 % is reached after 4 h. This work will provide some guidance for the design of photocatalytic systems with efficient interfacial electron transfer.