Xiao Mu, Lyu Miaoqiang, Wang Zitong, Wang Lianzhou
School of Chemical Engineering, Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, Queensland, 4072, Australia.
ChemSusChem. 2024 Dec 6;17(23):e202400937. doi: 10.1002/cssc.202400937. Epub 2024 Aug 7.
Carbon nitride photocatalysts are among the most studied candidates for efficient solar hydrogen (H) production due to their abundance of precursors, suitable bandgap, and visible light utilization. However, the polymeric nature of carbon nitride materials raises concerns regarding the self-decomposition during photocatalytic redox processes. Yet, the operational stability of carbon nitride photocatalysts for solar H production remains under-explored. Here we evaluate the photostability of carbon nitride photocatalysts with platinum (Pt) as the co-catalyst for solar H evolution and significant deactivation of this photocatalyst is observed under'accelerated' testing conditions. It is demonstrated that the detachment of the Pt co-catalyst on the surface of carbon nitride is the major reason for this deactivation, which can be attributed to a synergistic effect of photo-corrosion and mechanical stirring. The photo-corrosion weakens the interfacial bonding between carbon nitride and Pt co-catalyst, while continuous collisions from the mechanical stirring promote the detachment of co-catalysts from the surface of carbon nitride. These understandings provide insights into the rational design of photocatalysts and photocatalytic systems for improved operational stability.
由于其前驱体丰富、带隙合适且能利用可见光，氮化碳光催化剂是高效太阳能制氢（H）研究最多的候选材料之一。然而，氮化碳材料的聚合物性质引发了人们对光催化氧化还原过程中自分解的担忧。然而，氮化碳光催化剂用于太阳能制氢的操作稳定性仍未得到充分探索。在此，我们评估了以铂（Pt）作为共催化剂用于太阳能析氢的氮化碳光催化剂的光稳定性，并且在“加速”测试条件下观察到该光催化剂出现显著失活。结果表明，Pt共催化剂在氮化碳表面的脱离是这种失活的主要原因，这可归因于光腐蚀和机械搅拌的协同作用。光腐蚀削弱了氮化碳与Pt共催化剂之间的界面结合，而机械搅拌产生的持续碰撞促进了共催化剂从氮化碳表面脱离。这些认识为合理设计光催化剂和光催化系统以提高操作稳定性提供了见解。
