碳酸氢盐活化的过氧化氢:一种有机废水处理的新技术

doi:10.1016/S1872-2067(15)61100-7

摘要/Abstract

摘要：

水污染问题已成为影响我国可持续发展的关键问题之一, 为有效提高现有污水处理的效率及其回收利用, 各种催化氧化技术受到了广泛的关注. 目前发展的各类高级氧化技术在实际的应用过程中明显受到了氧化剂的利用率、催化剂的浸出、寿命及成本等问题的严重限制. 因此基于新的理念、发展新的催化氧化技术仍然受到广泛的关注.
最近几年, 利用碳酸氢盐活化过氧化氢, 应用于有机废水的降解逐渐受到环境催化领域的关注. 碳酸氢盐本身是一种低毒性、广泛存在于环境及生物体系的化学物质, 通过它活化过氧化氢产生过碳酸氢盐氧化剂, 该氧化剂能够直接氧化有机物. 同时, 在各种过渡金属催化剂的存在下, 通过该过碳酸氢盐可以形成氧化能力更强的各种自由基 (如羟基自由基等) 及高价态的过渡金属离子参与有机废水的降解. 虽然传统认为碳酸盐及碳酸氢盐对高级氧化法降解有机废水不利, 原因是认为它们能捕捉羟基自由基, 形成氧化能力更低的碳酸根自由基. 现有的研究已充分表明, 较低浓度的碳酸氢盐能够加快有机废水的氧化降解, 而且通常比单独使用过氧化氢效率更高, 这些新的发现已明显突破了传统意义上对碳酸氢盐作用的理解. 更为重要的是, 在微量碳酸氢盐的存在下, 其产生的微碱性环境极大地消除了负载型氧化物催化剂在废水降解过程中的金属离子流失、从而极大地延长了催化剂的寿命. 该缺点是各种基于过渡金属氧化物催化剂的高级氧化技术难以广泛推广的关键性挑战, 原因是随着氧化降解的进行, 废水体系由于有机酸的生成而逐渐酸化, 进而引发氧化物催化剂的酸溶而流失. 在这点上, 碳酸氢盐活化过氧化氢系统由于其天然的微碱性环境体现出了其明显的优势.
本文即是在本课题组工作基础上, 对该领域内国内外研究进展加以总结, 以期获得国内外同行的进一步关注. 综述的主要内容包括: (1) 碳酸氢氧活化过氧化氢的相关知识介绍, (2) 均相碳酸氢氧活化过氧化氢降解有机废水的研究进展, (3) 基于金属氧化物催化剂的碳酸氢氧活化过氧化氢降解有机废水的研究进展, 和 (4) 碳酸氢盐在其他高级氧化技术中的应用. 虽然基于碳酸氢氧活化过氧化氢降解有机废水的研究还处于早期探索阶段, 还有很多基础科学问题如降解机理等值得进一步探索, 期望通过该综述的介绍能够让同行对碳酸氢氧活化过氧化氢降解有机废水有一个比较全面的了解, 进而推动该研究方向的发展, 为有机废水的催化处理提供新的机会.

关键词: 废水处理, 碳酸氢盐活化过氧化氢, 催化剂浸出, 污染降解, 催化氧化

Abstract:

The serious limitations of available technologies for decontamination of wastewater have compelled researchers to search for alternative solutions. Catalytic treatment with hydrogen peroxide, which appears to be one of the most efficient treatment systems, is able to degrade various organics with the help of powerful ·OH radicals. This review focuses on recent progress in the use of bicarbonate activated hydrogen peroxide for wastewater treatment. The introduction of bicarbonate to pollutant treatment has led to appreciable improvements, not only in process efficiency, but also in process stability. This review describes in detail the applications of this process in homogeneous and heterogeneous systems. The enhanced degradation, limited or lack of leaching during heterogeneous degradation, and prolonged catalysts stability during degradation are salient features of this system. This review provides readers with new knowledge regarding bicarbonate, including the fact that it does not always harm pollutant degradation, and can significantly benefit degradation under some conditions.

Key words: Wastewater treatment, Bicarbonate activated hydrogen peroxide, Catalyst leaching, Pollutant degradation, Catalytic oxidation

Ali Jawad, 陈朱琦, 尹国川. 碳酸氢盐活化的过氧化氢:一种有机废水处理的新技术[J]. 催化学报, 2016, 37(6): 810-825.

Ali Jawad, Zhuqi Chen, Guochuan Yin. Bicarbonate activation of hydrogen peroxide: A new emerging technology for wastewater treatment[J]. Chinese Journal of Catalysis, 2016, 37(6): 810-825.

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