Chen Ao, Chen Chuang, Shao Shuai, Lian Yang, Du Yunlong, Gao Yunna, Yi Jinwen, Zheng Wei
School of Material Science and Chemical Engineering, Harbin University of Science and Technology, Harbin 150040, China.
Dalton Trans. 2025 Jul 8;54(27):10710-10718. doi: 10.1039/d5dt00955c.
Regular shape and size regularity of quantum dots (QDs) significantly influence the photoelectrical properties of solar photoelectrochemical (PEC) cells. Two types of green CuSnS (CTS) QDs, sphere-like and bullet-like, were synthesized the hot injection method by modulating the ratio of sulfur precursors. Compared with bullet-like CTS QDs, sphere-like CTS QDs exhibit a more negative conduction-band minimum and a narrower bandgap, enhancing sunlight absorption and utilization efficiency. These QDs were deposited onto TiO nanorod arrays individually to form p-n heterojunction photoanodes, which were assembled into PEC cells with Pt-plate counter electrodes for water-splitting H production. The experimental results demonstrate that the sphere-like CTS/TiO photoanode exhibits excellent PEC performance due to its more systematical spherical structure and homogeneous size distribution, achieving a photocurrent density of 2.54 mA cm, a hydrogen production yield of 162.1 μmol cm within 4-hour illumination (AM 1.5G, 100 mW cm), and, especially, long-term high stability of hydrogen production for 16 consecutive hours. The enhanced performance of the sphere-like CTS/TiO photoanode is attributed to its superior photoabsorption, shorter charge-carrier diffusion length and improved charge-separation efficiency. By modulating the morphology and size uniformity of CTS QDs as photosensitizers, this work demonstrates a viable strategy to boost the charge separation kinetics and light-harvesting capacity of PEC systems, thereby achieving efficient solar-to-hydrogen conversion.
量子点(QD)的规则形状和尺寸规整性对太阳能光电化学(PEC)电池的光电性能有显著影响。通过调节硫前驱体的比例,采用热注入法合成了两种类型的绿色CuSnS(CTS)量子点,即球状和子弹状。与子弹状CTS量子点相比,球状CTS量子点表现出更负的导带最小值和更窄的带隙,提高了太阳光的吸收和利用效率。这些量子点分别沉积在TiO纳米棒阵列上,形成p-n异质结光阳极,将其与铂板对电极组装成用于水分解制氢的PEC电池。实验结果表明,球状CTS/TiO光阳极由于其更规则的球形结构和均匀的尺寸分布而表现出优异的PEC性能,在4小时光照(AM 1.5G,100 mW/cm²)下实现了2.54 mA/cm²的光电流密度、162.1 μmol/cm²的产氢量,尤其是连续16小时的长期高产氢稳定性。球状CTS/TiO光阳极性能的提高归因于其优异的光吸收、较短的电荷载流子扩散长度和改进的电荷分离效率。通过调节作为光敏剂的CTS量子点的形貌和尺寸均匀性,这项工作展示了一种可行的策略来提高PEC系统的电荷分离动力学和光捕获能力,从而实现高效的太阳能到氢能的转换。