缺陷工程调控ZnIn_(2)S_(4)纳米片用于增强近红外驱动制氢

Facile defect engineering in ZnIn_(2)S_(4) nanosheets for enhanced NIR-driven H2 evolution

近红外(NIR)光驱动水分解产生氢气(H_(2))一直以来都是光催化领域备受关注的问题,但由于其动力学和热力学方面的缺陷,迄今为止仍是一项艰巨的挑战.为了突破这一限制,我们通过简便的水热法设计出了富含硫空位的无贵金属二维(2D)ZnIn_(2)S_(4)-基光催化剂,并首次使用单组分ZnIn_(2)S_(4)-基材料实现了波长大于800 nm的近红外驱动制氢性能.根据价带光谱、紫外-可见-近红外DRS光谱、稳态PL光谱、瞬态光电流响应和EPR表征,我们揭示了存在一个高效的Urbach带尾吸收用于捕获近红外光.硫空位在ZnIn_(2)S_(4)纳米片中的成功构建不仅扩展了光谱吸收范围,而且具有出色的载流子扩散特性和丰富的活性位点.因此,我们的研究结果可能会为未来开发近红外响应的ZnIn_(2)S_(4)-基光催化剂用于实现高效近红外驱动制氢提供一定的指导.

Near-infrared(NIR)light-driven water splitting to produce hydrogen(H_(2))has long been of great interest in photocatalysis,but it remains a formidable challenge so far due to both kinetic and thermodynamic shortcomings.To break through this limitation,we demonstrate a noble metal-free two-dimensional ZnIn_(2)S_(4)-based photocatalyst rich in sulfur vacancies via a facile hydrothermal method and firstly realized NIR-driven H_(2) production beyond 800 nm using single component ZnIn_(2)S_(4)-based materials.We disclosed the existence of an efficient Urbach tail transition to absorb long-wavelength NIR light according to the valence-band spectra,ultraviolet-visible-NIR diffuse reflectance spectra,steady-state photoluminescence spectra,transient photocurrent response,and electron paramagnetic resonance measurements.The successful construction of sulfur vacancies in ZnIn_(2)S_(4) na-nosheets not only extends the spectral absorption range but also has an excellent carrier diffusion property as well as an abundance of active sites.Therefore,our findings may provide an effective and promising perspective for the future devel-opment of NIR-responsive ZnIn_(2)S_(4)-based photocatalysts for highly efficient H_(2) production.