Zhang Beibei, Xiao Wen, Hu Jiawei, Liu Jinhong, Xu Hui, Zheng Xueqing, Wang Wuyou, Wu Haibo, Xi Xinguo, Dong Pengyu, Ji Hongbing
School of Chemistry and Chemical Engineering, Yancheng Institute of Technology, Yancheng 224051, PR China.
Advanced Energy Science and Technology Guangdong Laboratory, Research Institute of Sun Yat-sen University in Huizhou, Huizhou 516081, PR China.
J Colloid Interface Sci. 2023 Dec;651:948-958. doi: 10.1016/j.jcis.2023.08.057. Epub 2023 Aug 9.
To effectively separate electron-hole pairs produced by light, a heterojunction arrangement can be employed, thereby improving photocatalytic efficiency. In this study, a simple hydrothermal process is used to manufacture carbonized polymer dots/ZnInS (CPDs/ZIS) heterostructure, which enhances the light absorption and charge carrier lifetime in comparison to bare ZnInS (ZIS). Upon irradiation with visible light, the 3-CPDs/ZIS composite generates hydrogen at a rate of 133 μmol g h, which is 8.9 times faster than that of pure ZIS. The addition of CPDs can increase the range of light that can be absorbed, extend the service life of the optical charge, increase the specific surface area, and promote charge separation and transmission, which could effectively accelerate the photocatalytic reduction reaction. The presence of CPDs results in the introduction of multiple transition energy states and a decrease in the H* adsorption free energy, which enhances the hydrogen evolution activity according to the theoretical calculation findings of density functional theory (DFT) and Gibbs free energy of the hydrogen evolution process. Combining theoretical calculations and experimental results, a direct Z-type heterojunction mechanism is proposed for the hydrogen evolution promotion effectiveness of CPDs/ZIS under visible light.
为了有效分离光产生的电子 - 空穴对,可以采用异质结结构,从而提高光催化效率。在本研究中,采用简单的水热法制备碳化聚合物点/ ZnInS(CPDs/ZIS)异质结构,与裸ZnInS(ZIS)相比,该结构增强了光吸收和电荷载流子寿命。在可见光照射下,3-CPDs/ZIS复合材料产氢速率为133 μmol g⁻¹ h⁻¹,比纯ZIS快8.9倍。CPDs的加入可以增加可吸收光的范围,延长光生电荷的使用寿命,增加比表面积,并促进电荷分离和传输,从而有效加速光催化还原反应。根据密度泛函理论(DFT)的理论计算结果和析氢过程的吉布斯自由能,CPDs的存在导致引入多个跃迁能态并降低H*吸附自由能,从而增强析氢活性。结合理论计算和实验结果,提出了一种直接Z型异质结机理,用于解释CPDs/ZIS在可见光下促进析氢的有效性。