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山东大学黄柏标课题组报道了一种通过设计亲核和亲电位点修饰TiO2以增强光催化臭氧化反应的策略。与TiO2相比，表面羟基修饰的TiO2与臭氧之间的相互作用大大提高，促进了其对臭氧吸附和活化能力、同时增强了光生载流子的分离，展现出优异的污染物降解效率。
光催化臭氧氧化(Photocatalytic Ozonation)作为一种强大的高级氧化工艺，在室温下处理难以降解的有机污染物方面受到了广泛的关注。尽管该技术的整体降解效率很高，但仍存在臭氧利用率低等问题，其主要原因是臭氧的活化效率低。通常，光催化臭氧化反应发生在催化剂表面，臭氧吸附随后转化为活性氧 (Reactive Oxide Species)。因此，在催化剂表面设计高效的活性位点对于提高臭氧利用率至关重要。 表面改性是改变材料表面性质的一种有效方法，它可以通过调整材料表面的能带结构和电子结构来提高催化活性。臭氧分子的特殊结构允许它作为亲电和亲核试剂。这启发我们，合理设计催化剂表面的亲核和亲电位点将有利于促进臭氧的吸附与活化。表面羟基已被证明在多种催化过程中促进物质活化，同时具有亲核和亲电位点。但据我们所知，羟基在光催化臭氧活化中的作用并不清晰，有待深入的研究。 基于以上考虑，山东大学黄柏标课题组设计了表面羟基修饰的TiO2(记为TiO2-OH)，用于光催化臭氧氧化，并研究了表面羟基对臭氧活化和分解转化的作用。基于密度泛函理论的计算、原位漫反射傅立叶变换红外光谱和电子顺磁共振的结果表明，由于亲核O位和亲电H位的存在，表面羟基极大地促进了臭氧的吸附。此外，表面羟基修饰使催化剂表面电子云密度增加，导致表面吸附的臭氧内部发生极化；同时表面羟基增强了光生载流子的分离，这都有利于促进臭氧的活化和活性氧的形成。因此，TiO2-OH表现出优异的污染物去除效率。这项工作系统阐明了在光催化臭氧化过程中，表面羟基在臭氧活化和分解转化中的作用，并对其进行了深入的研究，为设计高效的光催化臭氧化催化剂提供了思路。 论文信息 Enhanced Photocatalytic Ozonation Using Modified TiO2 With Designed Nucleophilic and Electrophilic Sites Shaozhi Liu, Guangyao Zhai, Honggang Zhang, Shenghe Si, Yuanyuan Liu, Yuyin Mao, Zeyan Wang, Hefeng Cheng, Peng Wang, Zhaoke Zheng, Ying Dai, Baibiao Huang Chemistry – A European Journal DOI: 10.1002/chem.202401380
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