Zheng Xinlong, Song Yiming, Liu Yuhao, Li Jing, Yang Yingjie, Wu Daoxiong, Liu Weifeng, Shen Yijun, Tian Xinlong
State Key Laboratory of Marine Resource Utilization in South China Sea, Hainan Provincial Key Lab of Fine Chemistry, School of Science, Hainan University, Haikou, 570228, China.
Mechanical and Electrical Engineering College, Hainan University, Haikou, 570228, China.
Small. 2023 May;19(19):e2207623. doi: 10.1002/smll.202207623. Epub 2023 Feb 9.
Photocatalyst with excellent semiconductor properties is the key point to realize the efficient photocatalytic hydrogen evolution (PHE). As a representative binary metal sulfide (BMS) semiconductor, cadmium sulfide (CdS) possesses suitable bandgap of 2.4 eV and negative conduction band potential, which has a great potential to realize efficient visible-light PHE performance. In this work, CdS with unique cubic/hexagonal phase junction is facilely synthesized through a sulfur-rich butyldithiocarbamate acid (BDCA) solution process. The results illustrate that the phase junction can efficiently enhance the separation and transfer of photogenerated electron-hole pairs, resulting in an excellent PHE performance. In addition, the sulfur-rich property of BDCA solution leads to the absence of additional sulfur sources during the synthesis of CdS photocatalyst, which greatly simplifies the fabrication process. The optimal PHE rate of the BDCA-synthesized phase junction CdS photocatalyst is 7.294 mmol g h and exhibits a favorable photostability. Moreover, density function theory calculations indicated that the apparent redistribution of charge density in the cubic/hexagonal phase junction regions gives a suitable hydrogen adsorption capacity, which is responsible for the enhanced PHE activity.
具有优异半导体性能的光催化剂是实现高效光催化析氢（PHE）的关键。作为一种典型的二元金属硫化物（BMS）半导体，硫化镉（CdS）具有2.4 eV的合适带隙和负导带电位，在实现高效可见光PHE性能方面具有巨大潜力。在这项工作中，通过富硫的丁基二硫代氨基甲酸（BDCA）溶液法轻松合成了具有独特立方/六方相结的CdS。结果表明，相结可以有效地增强光生电子-空穴对的分离和转移，从而产生优异的PHE性能。此外，BDCA溶液的富硫特性导致在CdS光催化剂合成过程中无需额外的硫源，这极大地简化了制备过程。BDCA合成的相结CdS光催化剂的最佳PHE速率为7.294 mmol g h，并且表现出良好的光稳定性。此外，密度泛函理论计算表明，立方/六方相结区域中电荷密度的明显重新分布赋予了合适的氢吸附能力，这是PHE活性增强的原因。
