非均相催化臭氧氧化反应机制

刘莹; 何宏平; 吴德礼; 张亚雷

doi:10.7536/PC160118

化学进展 ›› 2016, Vol. 28 ›› Issue (7) :1112-1120 DOI: 10.7536/PC160118

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非均相催化臭氧氧化反应机制

刘莹, 何宏平, 吴德礼*, 张亚雷

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Heterogeneous Catalytic Ozonation Reaction Mechanism

Liu Ying, He Hongping, Wu Deli*, Zhang Yalei

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摘要

臭氧催化氧化作为高级氧化技术是目前水处理领域研究的热点，其中非均相臭氧催化氧化技术因其氧化能力强、降低臭氧投加量特别是能显著提高有机物矿化率等优点而备受关注。非均相催化臭氧氧化领域不断研究新的催化剂，但是其反应过程及机制更加复杂。催化臭氧氧化的性能很大程度上取决于催化剂及其表面性质。污染物在催化剂表面形成络合物，或者臭氧在催化剂表面分解产生不同的含氧物种如表面氧原子、过氧化物和羟基自由基等。本文评述了非均相臭氧催化氧化反应中存在的多种机理，主要是自由基理论、氧空位理论、表面原子氧理论、表面络合物理论和臭氧直接氧化理论。催化剂表面的羟基基团是主要的催化活性中心，本文探讨了表面羟基基团催化反应机制，得出催化剂表面性质决定其表面活性位点的特性及含量，对诱导臭氧分解产生含氧活性物种起了关键作用；概述了催化剂改性后的结构形态、比表面积及其性能和作用机制；并讨论了非均相臭氧催化氧化反应催化剂未来的发展趋势，为催化臭氧氧化污水处理技术提供了理论参考。

Abstract

As one of advanced oxidation processes(AOPs), catalytic ozonation has recently gained significant attention in the field of wastewater treatment. Heterogeneous catalytic ozonation have notable advantages of strong oxidation, less ozone dosage and especially its potentially greater effectiveness in the mineralization of organic matter. New catalysts have been studied world widely, but the reaction process and mechanisms are much more complicated. The efficiency of catalytic ozonation process depends to a great extent on the catalyst and its surface properties. On the surface active sites of catalyst,pollutants adsorbed form surface complexes or ozone decomposes to various reactive oxygen species such as surface atomic oxygen (^*O), surface peroxide (O₂^·-), hydroxyl radical (·OH). Thus the main mechanisms of heterogeneous catalytic ozonation are reviewed, including radical mechanism, oxygen vacancies theory, surface atomic oxygen mechanism, surface complexes theory and direct ozonation mechanism. The hydroxyl groups on the surface of catalyst are mainly catalytic active centers. The catalytic reaction mechanisms by hydroxyl groups are introduced in this paper. Surface properties of the catalysts determine the properties of the surface active sites and its amount, which play a key role in ozone decomposition. The structure and morphology, the specially surface area, the catalytic performance as well as reaction mechanisms of modified catalysts are reviewed. The future development of heterogeneous catalysts are also discussed to provide a theoretical reference of heterogeneous catalytic ozonation.

Contents
1 Introduction
2 Mechanism of heterogeneous catalytic ozonation
2.1 Radical mechanism
2.2 Oxygen vacancies mechanism
2.3 Surface atomic oxygen mechanism
2.4 Surface complexes mechanism
2.5 Direct ozonation mechanism
3 Catalytic reaction mechanisms by hydroxyl groups on the surface of catalyst
4 Heterogeneous catalytic ozonation mechanism after modification of the catalysts
4.1 Catalytic performance of modified catalysts
4.2 Reaction mechanism of modified catalysts
5 Conclusion and outlook

关键词

高级氧化技术 / 臭氧 / 非均相催化臭氧反应 / 催化剂 / 反应机制

Key words

advanced oxidation processes / ozone / heterogeneous catalytic ozonation / catalyst / reaction mechanism

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刘莹, 何宏平, 吴德礼, 张亚雷. 非均相催化臭氧氧化反应机制[J]. 化学进展, 2016, 28(7): 1112-1120 DOI:10.7536/PC160118

Liu Ying, He Hongping, Wu Deli, Zhang Yalei. Heterogeneous Catalytic Ozonation Reaction Mechanism[J]. Progress in Chemistry, 2016, 28(7): 1112-1120 DOI:10.7536/PC160118

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Received	Published	Revised
2016-01-01	2016-07-15	2016-03-01
Online Date
2016-05-17

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