Rapid photocatalytic debromination on TiO2 with in-situ formed copper co-catalyst: Enhanced adsorption and visible light activity
Rapid photocatalytic debromination on TiO2 with in-situ formed copper co-catalyst: Enhanced adsorption and visible light activity
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原位形成的铜助催化剂对 TiO2 进行快速光催化脱溴：增强吸附和可见光活性
DOI：
10.1016/j.apcatb.2016.04.053
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发表时间：
2016-10-05
影响因子：
22.1
通讯作者：
Zhao, Jincai
中科院分区：
文献类型：
--
作者：
Lv, Yanhui;Cao, Xiaofeng;Zhao, Jincai
廉价的金属Cu原位负载在TiO 2表面能够协同催化多溴污染物的光催化脱溴。结果表明，Cu/TiO 2催化剂对十溴二苯醚（BDE 209）的还原脱溴反应的催化活性是裸TiO 2催化剂的15倍以上.此外，金属铜的存在显着改变了形成的中间体的分布，表明由于金属铜的助催化作用，脱溴机理发生了变化。详细的非原位和原位表征的Cu/TiO 2光催化剂表明，铜保持其Cu的价态在光催化周转。机理研究表明，金属铜纳米粒子的存在大大增强了疏水性BDE 209在光催化剂上的吸附，促进了电子从TiO 2导带向污染物的转移。我们的实验结果还表明，BDE 209与金属铜助催化剂的相互作用将在解离电子转移过程中位置特异性地激活C-Br键。我们进一步表明，金属铜的表面等离子体共振可以通过利用可见光照射的一部分，有助于提高光催化活性。本研究为有机溴污染物的去除提供了一种简单、经济的方法，也为其他技术的还原脱卤提供了一种新的途径。(C)2016爱思唯尔B. V.保留所有权利。
The cheap metal Cu particles in-situ loaded on TiO2 surface is able to co-catalyze the photocatalytic debromination of polybrominated pollutants. Over 15 times of enhancement for the reductive debromination of deca-brominated diphenyl ether (BDE209) over Cu/TiO2 is achieved, relative to that on the bare TiO2. Moreover, the presence of metal copper markedly changes the distribution of the formed intermediates, indicating the change in the debromination mechanism because of the co-catalysis of metal Cu. The detailed ex-situ and in-situ characterizations of the Cu/TiO2 photocatalyst indicate that the copper remains its Cu valence state in photocatalytic turnover. The mechanistic investigation suggests that the presence of metal copper nanoparticles greatly enhance the adsorption of hydrophobic BDE209 on the photocatalyst, which facilitates the electron transfer from the conduction band of TiO2 to the pollutants. Our experimental results also implies that the interaction of BDE209 with metal copper co-catalyst would position-specifically activate the C-Br bonds during the dissociative electron transfer. We further show that the surface plasmon resonance of metal copper can contribute to the enhancement of photocatalytic activity by utilizing the visible-light part of the irradiation. The present study provides a simple and economic method for elimination of organobromide pollutants, and would be promising in reductive dehalogenation by other techniques. (C) 2016 Elsevier B.V. All rights reserved.