Zhang Xi, Pollitt Stephan, Jung Gihun, Niu Wenzhe, Adams Pardis, Bühler Jan, Grundmann Nora S, Erni Rolf, Nachtegaal Maarten, Ha Neul, Jung Jisu, Shin Byungha, Yang Wooseok, Tilley S David
Department of Chemistry, University of Zurich, Winterthurerstrasse 190, 8057 Zurich, Switzerland.
Paul Scherrer Institut (PSI), Forschungsstrasse 111, 5232 Villigen, Switzerland.
Chem Mater. 2023 Mar 8;35(6):2371-2380. doi: 10.1021/acs.chemmater.2c03489. eCollection 2023 Mar 28.
CuS is a promising solar energy conversion material due to its suitable optical properties, high elemental earth abundance, and nontoxicity. In addition to the challenge of multiple stable secondary phases, the short minority carrier diffusion length poses an obstacle to its practical application. This work addresses the issue by synthesizing nanostructured CuS thin films, which enables increased charge carrier collection. A simple solution-processing method involving the preparation of CuCl and CuCl molecular inks in a thiol-amine solvent mixture followed by spin coating and low-temperature annealing was used to obtain phase-pure nanostructured (nanoplate and nanoparticle) CuS thin films. The photocathode based on the nanoplate CuS (FTO/Au/CuS/CdS/TiO/RuO ) reveals enhanced charge carrier collection and improved photoelectrochemical water-splitting performance compared to the photocathode based on the non-nanostructured CuS thin film reported previously. A photocurrent density of 3.0 mA cm at -0.2 versus a reversible hydrogen electrode ( ) with only 100 nm thickness of a nanoplate CuS layer and an onset potential of 0.43 were obtained. This work provides a simple, cost-effective, and high-throughput method to prepare phase-pure nanostructured CuS thin films for scalable solar hydrogen production.
硫化铜因其合适的光学性质、高的地壳元素丰度和无毒特性，是一种很有前景的太阳能转换材料。除了存在多个稳定次生相的挑战外，少数载流子扩散长度较短也对其实际应用构成了障碍。这项工作通过合成纳米结构的硫化铜薄膜来解决这一问题，从而增加电荷载流子的收集。采用一种简单的溶液处理方法，即在硫醇 - 胺溶剂混合物中制备氯化铜和氯化铜分子墨水，然后旋涂并进行低温退火，以获得纯相纳米结构（纳米片和纳米颗粒）的硫化铜薄膜。与之前报道的基于非纳米结构硫化铜薄膜的光阴极相比，基于纳米片硫化铜的光阴极（FTO/Au/CuS/CdS/TiO/RuO ）显示出增强的电荷载流子收集能力和改善的光电化学水分解性能。在相对于可逆氢电极（ ）为 -0.2时，仅100纳米厚的纳米片硫化铜层获得了3.0 mA cm的光电流密度，起始电位为0.43 。这项工作提供了一种简单、经济高效且高通量的方法来制备用于可扩展太阳能制氢的纯相纳米结构硫化铜薄膜。
