Abstract
The discovery of graphene and graphene-like two-dimensional materials has brought fresh vitality to the field of photocatalysis. Bandgap engineering has always been an effective way to make semiconductors more suitable for specific applications such as photocatalysis and optoelectronics. Achieving control over the bandgap helps to improve the light absorption capacity of the semiconductor materials, thereby improving the photocatalytic performance. This work reports two-dimensional −H/−OH terminal-substituted siligenes (gersiloxenes) with tunable bandgap. All gersiloxenes are direct-gap semiconductors and have wide range of light absorption and suitable band positions for light driven water reduction into H2, and CO2 reduction to CO under mild conditions. The gersiloxene with the best performance can provide a maximum CO production of 6.91 mmol g−1 h−1, and a high apparent quantum efficiency (AQE) of 5.95% at 420 nm. This work may open up new insights into the discovery, research and application of new two-dimensional materials in photocatalysis.
Highlights
The discovery of graphene and graphene-like two-dimensional materials has brought fresh vitality to the field of photocatalysis
Most 2D materials have several structural limitations as photocatalysts, for example, graphene is zero-bandgap material[4], which is not sufficient to absorb light to drive photocatalytic oxidation or reduction reaction; the absorption range of g-C3N4 is mainly limited in the ultraviolet region[2]; the monolayer of transition-metal chalcogenides represented by MoS2 and WS2 is direct-bandgap semiconductor, while the bilayer and multilayer are indirect semiconductors[5], which will affect the energy conversion efficiency of light
Another hydrogenation product of silicene is siloxene (Si6H3(OH)3) which has been synthesized by the similar methods26. 2D
Summary
The discovery of graphene and graphene-like two-dimensional materials has brought fresh vitality to the field of photocatalysis. The N2 Adsorption/desorption isotherms and poresize distribution curves (Supplementary Fig. 7a–d) indicate that all gersiloxenes, GeH, and Si6H3(OH)[3] have mesoporous structure and gersiloxene with x = 0.5 exhibits the most extensive size distribution (details in Supplementary Note 2).
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