State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University , Beijing 100084, China.
Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China , Chengdu 610054, China.
ACS Nano. 2017 Dec 26;11(12):12753-12763. doi: 10.1021/acsnano.7b07512. Epub 2017 Nov 28.
A highly efficient low-band-gap (1.2-0.8 eV) photoelectrode is critical for accomplishing efficient conversion of visible-near-infrared sunlight into storable hydrogen. Herein, we report an SbSe polycrystalline thin-film photocathode having a low band gap (1.2-1.1 eV) for efficient hydrogen evolution for wide solar-spectrum utilization. The photocathode was fabricated by a facile thermal evaporation of a single SbSe powder source onto the Mo-coated soda-lime glass substrate, followed by annealing under Se vapor and surface modification with an antiphotocorrosive CdS/TiO bilayer and Pt catalyst. The fabricated SbSe(Se-annealed)/CdS/TiO/Pt photocathode achieves a photocurrent density of ca. -8.6 mA cm at 0 V, an onset potential of ca. 0.43 V, a stable photocurrent for over 10 h, and a significant photoresponse up to the near-infrared region (ca. 1040 nm) in near-neutral pH buffered solution (pH 6.5) under AM 1.5G simulated sunlight. The obtained photoelectrochemical performance is attributed to the reliable synthesis of a micrometer-sized SbSe (Se-annealed) thin film as photoabsorber and the successful construction of an appropriate p-n heterojunction at the electrode-liquid interface for effective charge separation. The demonstration of a low-band-gap and high-performance SbSe photocathode with facile fabrication might facilitate the development of cost-effective PEC devices for wide solar-spectrum utilization.
一种高效的低带隙(1.2-0.8 eV)光电阴极对于实现可见光-近红外太阳光向可储存氢的高效转化至关重要。在此,我们报告了一种 SbSe 多晶薄膜光电阴极,具有低带隙(1.2-1.1 eV),可用于高效的氢析出,实现宽太阳光谱的利用。该光电阴极是通过将单一 SbSe 粉末源在 Mo 涂层的钠钙玻璃衬底上进行简单的热蒸发,然后在 Se 蒸气下退火,并通过抗光腐蚀性的 CdS/TiO 双层和 Pt 催化剂进行表面修饰来制备的。所制备的 SbSe(Se-annealed)/CdS/TiO/Pt 光电阴极在 0 V 时达到约-8.6 mA cm 的光电流密度,起始电位约为 0.43 V,在近中性 pH 缓冲溶液(pH 6.5)中,在 AM 1.5G 模拟太阳光下稳定的光电流超过 10 小时,并在近红外区域(约 1040nm)具有显著的光响应。所获得的光电化学性能归因于可靠合成作为光吸收体的微米级 SbSe(Se-annealed)薄膜,以及在电极-液体界面成功构建适当的 p-n 异质结,以实现有效的电荷分离。具有低成本和高性能 SbSe 光电阴极的高效制备的展示可能会促进具有宽太阳光谱利用的经济高效的 PEC 器件的发展。