State Key Laboratory of Environmental Aquatic Chemistry, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.
J Am Chem Soc. 2010 Jan 20;132(2):857-62. doi: 10.1021/ja907792d.
A plasmonic photocatalyst Ag-AgI supported on mesoporous alumina (Ag-AgI/Al(2)O(3)) was prepared by deposition-precipitation and photoreduction methods. The catalyst showed high and stable photocatalytic activity for the degradation and mineralization of toxic persistent organic pollutants, as demonstrated with 2-chlorophenol (2-CP), 2,4-dichlorophenol (2,4-DCP), and trichlorophenol (TCP) under visible light or simulated solar light irradiation. On the basis of electron spin resonance, cyclic voltammetry analyses under a variety of experimental conditions, two electron transfer processes were verified from the excited Ag NPs to AgI and from 2-CP to the Ag NPs, and the main active species of O(2)(*-) and excited h(+) on Ag NPs were involved in the photoreaction system of Ag-AgI/Al(2)O(3). A plasmon-induced photocatalytic mechanism was proposed. Accordingly, the plasmon-induced electron transfer processes elucidated the photostability of Ag-AgI/Al(2)O(3). This finding indicates that the high photosensitivity of noble metal NPs due to surface plasmon resonance could be applied toward the development of new plasmonic visible-light-sensitive photocatalysts and photovoltaic fuel cells.
一种负载在介孔氧化铝上的等离子体光催化剂 Ag-AgI(Ag-AgI/Al2O3),通过沉积沉淀和光还原法制备而成。该催化剂在可见光或模拟太阳光照射下,对有毒持久性有机污染物 2-氯苯酚(2-CP)、2,4-二氯苯酚(2,4-DCP)和三氯苯酚(TCP)的降解和矿化表现出高且稳定的光催化活性。基于电子自旋共振和在各种实验条件下的循环伏安分析,从激发的 Ag NPs 到 AgI 和从 2-CP 到 Ag NPs 的两个电子转移过程得到了验证,Ag NPs 上的主要活性物质 O2(*-)和激发态 h(+)参与了 Ag-AgI/Al2O3 的光反应体系。提出了一种等离子体诱导的光催化机制。因此,阐明的等离子体诱导电子转移过程解释了 Ag-AgI/Al2O3 的光稳定性。这一发现表明,由于表面等离子体共振,贵金属 NPs 的高灵敏度可以应用于开发新型等离子体可见光敏感光催化剂和光伏燃料电池。