Surface Phosphate Functionalization for Boosting Plasmon-Induced Water Oxidation on Au/TiO2
Surface Phosphate Functionalization for Boosting Plasmon-Induced Water Oxidation on Au/TiO2
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DOI：
10.1021/acs.jpcc.2c00206
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发表时间：
2022-03
期刊：
影响因子：
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通讯作者：
Bin Zeng;Shengyang Wang;Yejun Xiao;Guang Zeng;Xianwen Zhang;Rengui Li;Can Li
中科院分区：
文献类型：
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作者：
Bin Zeng;Shengyang Wang;Yejun Xiao;Guang Zeng;Xianwen Zhang;Rengui Li;Can Li
等离子体光催化剂存在电荷分离效率低、反应动力学慢等问题，导致其光催化性能较差，尤其是对热空穴参与的水氧化反应。在等离子体光催化剂上构建热空穴传输链和反应中心，为有效的等离子体诱导水氧化提供了令人兴奋的机会。然而，由于热空穴的快速弛豫动力学和低迁移率，调制热空穴的行为仍然具有挑战性。在此，通过引入表面磷酸盐基团以使等离子体光催化剂Au-TiO 2的表面官能化，与原始光催化剂相比，涉及水氧化的热空穴的活性增加到103倍。在520 nm处测得等离子体诱导水氧化的最佳表观量子效率为1.2%。研究发现，等离子体激元诱导的热空穴可以被固定在TiO 2表面的磷酸盐捕获，实现有效的稳定电荷分离，并且表面磷酸盐功能化也导致了与Au/TiO 2不同的多空穴反应途径.该研究为等离子体激元激发中热空穴的分离和催化反应的调控提供了一种新的途径。
Plasmonic photocatalysts suffer from inefficient charge separation and slow reaction kinetics, which result in poor plasmonic photocatalytic performance, especially for the hot hole involved water oxidation. Constructing a hot hole transfer chain and reaction center on plasmonic photocatalysts enables exciting opportunities for efficient plasmon-induced water oxidation. However, it is still challenging to modulate the behavior of the hot holes owing to the fast relaxation dynamics and low mobility. Herein, by introducing a surface phosphate group to functionalize the surface of the plasmonic photocatalyst Au-TiO2, the activity of hot hole involved water oxidation increases to ∼3 times as compared to the pristine photocatalyst. The optimized apparent quantum efficiency for plasmon-induced water oxidation was measured to be 1.2% at 520 nm. It is found that the plasmon-induced hot holes can be trapped by the phosphate anchored on the TiO2surface for efficient steady charge separation, and the surface phosphate functionalization also results in a different multi-hole reaction pathway as compared to the Au/TiO2. This study provides an alternative way to modulate the hot hole’s separation and catalytic reactions in plasmonic photocatalysis.