Efficient
solar-to-H2 conversion coupled with high-value
multicarbon chemical production is an appealing strategy to meet the
demands in energy and environment; unfortunately, it remains a great
challenge because of insufficient effective photocatalysts and vague
catalytic mechanism. Here, Pt single sites are dispersed on a two-dimensional
CdS nanosheet (PtSS-CdS) for simultaneous photocatalytic
H2 and 1,1-diethoxyethane (DEE) evolution from ethanol.
Structural characterizations elucidate that each Pt single atom is
bonded with three surface S atoms in CdS, forming a Pt–S3 tetrahedron coordination structure. The strong semiconductor
(CdS) and metal (Pt) interface interaction not only endows efficient
migration of photoexcited electron from CdS to Pt single atom via
Pt–S bonds but also promises Pt centers with optimized H adsorption
energy, thus accelerating the H2 evolution reaction. Moreover,
in situ electron spin resonance measurements reveal that the α-C–H
bond rather than the O–H in ethanol prefers to be dehydrogenated
by the surface holes of PtSS-CdS. Therefore, a remarkably
promoted H2 generation rate (11.5 mmol g–1 h–1) is observed on PtSS-CdS under
simulated solar light, and continuous H2 bubbles are generated
over PtSS-CdS thin film upon light irradiation. Meanwhile,
DEE is also formed with the selectivity of 97.9%. This study affords
a promising strategy to develop high-performance catalysts toward
photocatalytic H2 evolution and organic synthesis in a
sustainable manner.