Key Laboratory for Advanced Materials, Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Shanghai Engineering Research Center for Multi-media Environmental Catalysis and Resource Utilization, School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai 200237, P. R. China.
School of Chemistry and Chemical Engineering, Queen's University of Belfast, University Road, Belfast BT9 5AG, Northern Ireland, U.K.
ACS Nano. 2023 Jun 27;17(12):11655-11664. doi: 10.1021/acsnano.3c02092. Epub 2023 Jun 5.
Incorporation of plasmonic metal nanomaterials can significantly enhance the visible light response of semiconductor photocatalysts via localized surface plasmon resonance (LSPR) mechanisms. However, the surfaces of plasmonic metal nanomaterials are often covered with surfactant molecules, which is undesired when the nanomaterials are used for photocatalytic hydrogen evolution, since surfactant molecules could significantly compromise the nanomaterials' cocatalyst functionalities by blocking the active sites and/or by inhibiting the surface charge transfer process. Herein, we demonstrate a method that assembles Au nanoparticles (NPs) into Au colloidosomes (AuCSs) without modifying their surfaces with surfactants. The resulting AuCSs were then coupled with CdS for the formation of Au-CdS composite photocatalysts through an deposition method. The assembly of Au NPs induced a broader and stronger LSPR response for AuCSs, while the absence of surfactants allowed them to act efficiently as cocatalysts. This essentially enhanced the electron-hole pair generation rate and further their utilization efficiency, leading to an extremely high hydrogen evolution rate of 235.8 mmol·g·h under simulated sunlight excitation.
将等离子体金属纳米材料纳入半导体光催化剂中,可以通过局域表面等离子体共振(LSPR)机制显著增强可见光响应。然而,当等离子体金属纳米材料用于光催化析氢时,纳米材料的表面通常会被表面活性剂分子覆盖,这是不理想的,因为表面活性剂分子会通过覆盖活性位点和/或抑制表面电荷转移过程,极大地损害纳米材料的助催化剂功能。在此,我们展示了一种方法,即不使用表面活性剂对 Au 纳米颗粒(NPs)进行修饰,将其组装成 Au 胶束(AuCSs)。然后,通过沉积法将得到的 AuCSs 与 CdS 耦合,形成 Au-CdS 复合光催化剂。Au NPs 的组装诱导了 AuCSs 更宽和更强的 LSPR 响应,而表面活性剂的缺失使其能够有效地作为助催化剂发挥作用。这从本质上提高了电子-空穴对的产生速率,并进一步提高了它们的利用效率,在模拟太阳光激发下,产生了 235.8 mmol·g·h 的极高析氢速率。