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微波合成碘掺杂的氯氧铋微球用于可见光光催化去除对羟基苯甲酸酯类有毒含羟基中间产物:催化剂合成、表征和机理研究。

Microwave synthesis of iodine-doped bismuth oxychloride microspheres for the visible light photocatalytic removal of toxic hydroxyl-contained intermediates of parabens: catalyst synthesis, characterization, and mechanism insight.

机构信息

School of Chemistry and Environment, South China Normal University, Guangzhou, 510006, People's Republic of China.

出版信息

Environ Sci Pollut Res Int. 2019 Oct;26(28):28871-28883. doi: 10.1007/s11356-019-06074-1. Epub 2019 Aug 5.

DOI:10.1007/s11356-019-06074-1
PMID:31385253
Abstract

The iodine-doped bismuth oxychloride (I-doped BiOCl) microspheres are synthesized as the visible light photocatalysts for the photocatalytic removal of three toxic hydroxyl-contained intermediates of parabens. With the aid of the unique heating mode of microwave method, the I-doped BiOCl photocatalysts with tunable iodine contents and dispersed energy bands, instead of a mixture of BiOI and BiOCl or solid solution, are synthesized under the controllable conditions. Due to the stretched architectures, high specific surface area, and effective separation of photogenerated carriers, they exhibit high activity to the photocatalytic degradation of methyl 2,4-dihydroxybenzoate (MDB), methyl 3,4-dihydroxybenzoate (MDHB), and ethyl 2,4-dihydroxybenzoate (EDB). As a typical result, it is indicated that though MDB as the most difficult intermediate of parabens to be degraded, a 91.2% removal ratio can still be achieved over the I-doped BiOCl with an energy band of 2.79 eV within 60 min. In addition, it is also confirmed that these photocatalysts remain stable throughout the photocatalytic reaction and can be reused, and more importantly, the photogenerated h and •O are the key reactive species, while •OH plays a negligible role in the photocatalytic reaction. Resorcinol was identified as the main photodegraded intermediate. These results demonstrate that this photocatalytic system not only exhibit a high efficiency but also avoid the consequent secondary pollutions due to the no formation of complex hydroxyl derivatives.

摘要

碘掺杂的氧氯化铋(I 掺杂 BiOCl)微球被合成作为可见光光催化剂,用于光催化去除对羟基苯甲酸酯的三种有毒羟基中间体。借助微波法独特的加热方式,在可控条件下合成了具有可调碘含量和分散能带的 I 掺杂 BiOCl 光催化剂,而不是 BiOI 和 BiOCl 的混合物或固溶体。由于其伸展的结构、高比表面积和光生载流子的有效分离,它们对甲基 2,4-二羟基苯甲酸酯(MDB)、甲基 3,4-二羟基苯甲酸酯(MDHB)和乙基 2,4-二羟基苯甲酸酯(EDB)的光催化降解表现出很高的活性。作为一个典型的结果,表明尽管 MDB 是最难降解的对羟基苯甲酸酯中间体,但在能带为 2.79eV 的 I 掺杂 BiOCl 中,在 60min 内仍可达到 91.2%的去除率。此外,还证实这些光催化剂在整个光催化反应过程中保持稳定且可重复使用,更重要的是,光生 h 和 •O 是关键的反应性物质,而 •OH 在光催化反应中起微不足道的作用。间苯二酚被确定为主要的光降解中间产物。这些结果表明,该光催化体系不仅表现出高效率,而且由于没有形成复杂的羟基衍生物,避免了随之产生的二次污染。

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