臭氧/多相催化氧化去除水中有机污染物效能与机理
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摘要
近年来，饮用水污染问题已引起人们的广泛重视，特别是饮用水中一些微量难降解有机物是导致饮用水水质恶化的主要污染物质，因而研究开发应用于大规模水处理中的新型水处理工艺，有效去除水中微量难降解有机物，已成为当务之急。本文利用蜂窝陶瓷具有蜂窝状的多孔整体结构，只有比表面积大、高强度、低膨胀、扩散距离短、耐磨拟、压力降小等特点，制备了一种新型Mn-Cu-K负载蜂窝陶瓷催化剂，并开发了臭氧／Mn-Cu-K负载蜂窝陶瓷催化氧化体系去除水中难降解有机物的水处理技术；同时首次将蜂窝陶瓷和臭氧结合获得新的臭氧催化氧化技术，可直接应用于去除水中难降解有机物。该类催化剂只有来源易得、制备简单、生产成本低、使用方便和催化剂使用寿命长等优点，只有较好的市场应用前景。
实验中采用半连续流动的运行方式，选用了难降解的硝基苯作为典型有机物，考察了臭氧／蜂窝陶瓷和臭氧／Mn-Cu-K蜂窝陶瓷对有机污染物的降解效能。
在臭氧／蜂窝陶瓷催化氧化体系中，蜂窝陶瓷的存在对高稳定性有机物具有较好的去除效果，在相同条件下比单独臭氧对硝基苯的降解效率提高近15％，而蜂窝陶瓷本身对硝基苯的吸附能力较弱。蜂窝陶瓷的存在显著地提高了臭氧的利用率，提高近26％，并有效地促进了臭氧分解。实验中考察了反应条件对臭氧／蜂窝陶瓷体系的影响，包括催化剂用量、体系温度、体系pH值变化、硝基苯初始浓度、水质本底变化、臭氧投加工艺和投加量，并发现硝基苯的初始浓度与反应速率常数成线性关系。在臭氧／蜂窝陶瓷催化体系中水中低浓度的无机金属离子存在有利于催化反应，此时金属离子相当于均相催化剂起到协同作用，高浓度金属离子存在会对催化体系有一定的抑制作用；同样，低浓度HCO_3~-离子和天然有机物腐殖酸存在能促进反应，高浓度HCO_3~-离子和腐殖酸存在能抑制反应，间接表明催化反应遵循自由基作用机理。臭氧／蜂窝陶瓷催化体系对有机物具有较强的矿化能力，与单独臭氧体系相比，TOC的降解率提高近19％；另外，对小分子酸草酸的TOC的降解能力明显优于单独臭氧体系。
以蜂窝陶瓷为载体通过负载主族、过渡金属氧化物形成新型的催化剂，并进行了筛选、评价和表征。单组分负载的金属氧化物只有如下活性顺序：Ba＞Ca＞Zn＞Ni＞Mn＞Cu＞Fe＞Sr＞Ag＞Cd；负载主族元素的催化剂活性较高。
Special concern has been paid to the pollution of drinking water sources in recent years. Especially some refractory organics in drinking water could directly cause the deterioration of water quality. Accordingly, it is urgently needed to develop new advanced water treatment technology that is applicable in large-scale water treatment to remove refractory organics in water effectively.
Ceramic honeycombs with porous gross structure have the characteristic of large specific surface area, high intensity, low expansion, short diffusion length, high abrasive resistance and low pressure drop. Based on above concern, a new type of ceramic honeycombs catalyst loaded with Mn-Cu-K has been prepared to catalyze the ozonation process in drinking water treatment. Ozone/Mn-Cu-K loaded ceramic honeycombs system is thus developed for removing the refractory organics with high stability in water. At the same time the new catalytic ozonation technology with the combination of ceramic honeycombs and ozone has been first directly applied to remove the refractory organics in drinking water. The catalysts showed long lifetime, being readily available, and less cost, easy to be prepared and handled, which have good
application potential in drinking water treatment process.
Semi-continuous flow process is adopted in the experiments to study the effectiveness and mechanism of ozone/ceramic honeycombs and ozone/Mn-Cu-K loaded ceramic honeycombs toward nitrobenzene removing in drinking water.
In ozone/ ceramic honeycombs system the removal of nitrobenzene is enhanced by the presence of ceramic honeycombs. The removal ratio of nitrobenzene increased by 15% compared with the system of ozone alone. However, it is found that ceramic honeycombs have quite low absorbability toward nitrobenzene. The application rate of ozone is increased to 26% in the presence of ceramic honeycombs. At the same time, the decomposition of ozone is also enhanced effectively. The effect of reaction conditions toward ozone/
实验中采用半连续流动的运行方式，选用了难降解的硝基苯作为典型有机物，考察了臭氧／蜂窝陶瓷和臭氧／Mn-Cu-K蜂窝陶瓷对有机污染物的降解效能。
在臭氧／蜂窝陶瓷催化氧化体系中，蜂窝陶瓷的存在对高稳定性有机物具有较好的去除效果，在相同条件下比单独臭氧对硝基苯的降解效率提高近15％，而蜂窝陶瓷本身对硝基苯的吸附能力较弱。蜂窝陶瓷的存在显著地提高了臭氧的利用率，提高近26％，并有效地促进了臭氧分解。实验中考察了反应条件对臭氧／蜂窝陶瓷体系的影响，包括催化剂用量、体系温度、体系pH值变化、硝基苯初始浓度、水质本底变化、臭氧投加工艺和投加量，并发现硝基苯的初始浓度与反应速率常数成线性关系。在臭氧／蜂窝陶瓷催化体系中水中低浓度的无机金属离子存在有利于催化反应，此时金属离子相当于均相催化剂起到协同作用，高浓度金属离子存在会对催化体系有一定的抑制作用；同样，低浓度HCO_3~-离子和天然有机物腐殖酸存在能促进反应，高浓度HCO_3~-离子和腐殖酸存在能抑制反应，间接表明催化反应遵循自由基作用机理。臭氧／蜂窝陶瓷催化体系对有机物具有较强的矿化能力，与单独臭氧体系相比，TOC的降解率提高近19％；另外，对小分子酸草酸的TOC的降解能力明显优于单独臭氧体系。
以蜂窝陶瓷为载体通过负载主族、过渡金属氧化物形成新型的催化剂，并进行了筛选、评价和表征。单组分负载的金属氧化物只有如下活性顺序：Ba＞Ca＞Zn＞Ni＞Mn＞Cu＞Fe＞Sr＞Ag＞Cd；负载主族元素的催化剂活性较高。
Special concern has been paid to the pollution of drinking water sources in recent years. Especially some refractory organics in drinking water could directly cause the deterioration of water quality. Accordingly, it is urgently needed to develop new advanced water treatment technology that is applicable in large-scale water treatment to remove refractory organics in water effectively.
Ceramic honeycombs with porous gross structure have the characteristic of large specific surface area, high intensity, low expansion, short diffusion length, high abrasive resistance and low pressure drop. Based on above concern, a new type of ceramic honeycombs catalyst loaded with Mn-Cu-K has been prepared to catalyze the ozonation process in drinking water treatment. Ozone/Mn-Cu-K loaded ceramic honeycombs system is thus developed for removing the refractory organics with high stability in water. At the same time the new catalytic ozonation technology with the combination of ceramic honeycombs and ozone has been first directly applied to remove the refractory organics in drinking water. The catalysts showed long lifetime, being readily available, and less cost, easy to be prepared and handled, which have good
application potential in drinking water treatment process.
Semi-continuous flow process is adopted in the experiments to study the effectiveness and mechanism of ozone/ceramic honeycombs and ozone/Mn-Cu-K loaded ceramic honeycombs toward nitrobenzene removing in drinking water.
In ozone/ ceramic honeycombs system the removal of nitrobenzene is enhanced by the presence of ceramic honeycombs. The removal ratio of nitrobenzene increased by 15% compared with the system of ozone alone. However, it is found that ceramic honeycombs have quite low absorbability toward nitrobenzene. The application rate of ozone is increased to 26% in the presence of ceramic honeycombs. At the same time, the decomposition of ozone is also enhanced effectively. The effect of reaction conditions toward ozone/
引文
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