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非均相催化剂催化臭氧产生·OH性能评价体系构建

中国给水排水[ISSN:1000-4062/CN:12-1073/TU] 卷: 第39卷 期数: 2023年第13期 页码: 25-31 栏目: 出版日期: 2023-07-01
Title:
Development and Application of Evaluation Method for Hydroxyl Radical Formation during Heterogeneous Catalytic Ozonation
作者:
沈方方1,2， 刘永泽1,2， 马军3， 江进4， 邹金儒1,2， 耿男男1,2， 封莉1,2， 张立秋1,2
（1.北京林业大学 水体污染源控制技术北京市重点实验室，北京 100083；2.北京林业大学环境科学与工程学院 污染水体源控制与生态修复技术北京市高等学校工程研究中心，北京 100083；3.哈尔滨工业大学 环境学院，黑龙江 哈尔滨 150090；4.广东工业大学 环境生态工程研究院，广东 广州 510006）
Author(s):
SHEN　Fang?fang1，2， LIU　Yong?ze1，2， MA　Jun3， JIANG　Jin4， ZOU　Jin?ru1，2， GENG　Nan?nan1，2， FENG　Li1，2， ZHANG　Li?qiu1，2
（1. Beijing Key Laboratory for Source Control Technology of Water Pollution， Beijing Forestry University， Beijing 100083， China； 2. Engineering Research Center for Water Pollution Source Control & Eco?remediation， College of Environmental Science and Engineering， Beijing Forestry University， Beijing 100083， China； 3. School of Environment， Harbin Institute of Technology， Harbin 150090， China； 4. Institute of Environmental and Ecological Engineering， Guangdong University of Technology， Guangzhou 510006， China）
关键词:
非均相催化剂;  臭氧催化氧化;  链反应机制;  ·OH产率;  ·OH产速
Keywords:
heterogeneous catalysts;  catalytic ozonation;  chain reactions;  hydroxyl radical yield;  hydroxyl radical formation rate
摘要:
非均相臭氧催化氧化技术在污（废）水深度处理中应用普遍，它利用非均相催化剂催化臭氧（O3）分解产生羟基自由基（·OH），从而强化对臭氧难降解有机物的氧化去除。然而目前催化剂种类繁多，且催化效果参差不齐，亟需建立一种横向比较其催化性能的评价体系，为工程中催化剂的筛选与优化应用提供依据。基于催化臭氧分解产生·OH的链反应机制，构建了非均相催化剂催化O3产生·OH性能（·OH产率和产速）评价体系并进行了验证，随后对两类6种催化剂（包括碳材料类，即碳纳米管MWCNTs和N原子掺杂碳纳米管N-CNTs；金属氧化物类，即Fe-Mn-Al2O3、FeOx-Al2O3、NiOx-Al2O3和CuMn2O4）诱发O3分解产生·OH的效能进行评价。结果表明，在O3投量约为3.8 mg/L的条件下，N-CNTs（0.01~0.06 g/L）的·OH产速快［2.52~8.61 μmol/（L·min）］，但产率低（50.20%~59.66%）；Fe-Mn-Al2O3、FeOx-Al2O3和NiOx-Al2O3（0.05~0.4 g/L）的·OH产率较高（72.51%~89.50%），但产速相比较慢［0.66~3.68 μmol/（L·min）］；而CuMn2O4（0.05~0.3 g/L）兼具·OH产率高（76.61%~89.46%）、产速快［1.10~5.87 μmol/（L·min）］且·OH产速提高快［0.014 6 μmol/（min·mg）］的特点，性能最佳。该评价方法的建立有助于筛选非均相催化剂，为臭氧催化氧化工艺的实际应用提供技术指导。
Abstract:
Heterogeneous catalytic ozonation technology is widely used in the advanced treatment of wastewater. Heterogeneous catalysts can induce ozone (O3) decomposition into hydroxyl radical (·OH), thus enhancing the oxidation of ozone-resistant organic matters. Nowadays, there are many kinds of catalysts and their catalytic performance are uneven in practical applications. Thus, it is urgent to establish an evaluation method to comparatively evaluate their catalytic performance, so as to provide a basis for the selection and optimization of catalysts in engineering application. In this study, based on the chain reaction of ·OH formation during catalytic ozonation, an evaluation method (taking both ·OH formation rate and ·OH yield into account) was developed and verified. Subsequently, catalytic performance of two classes of six catalysts were evaluated, including carbon materials such as carbon nanotubes (CNTs) and N-doped carbon nanotubes (N-CNTs), and metal oxides, such as Fe-Mn-, FeOx-Al2O3, NiOx-Al2O3 and CuMn2O4. The results showed that, at about 3.8 mg/L O3 dose, N-CNTs (0.01-0.06 g/L) induced fast ·OH formation [i.e., 2.52-8.61 μmol/(L·min)] while the ·OH yield was low (i.e., 50.20%-59.66%). Fe-Mn-Al2O3, FeOx-Al2O3 and NiOx-Al2O3 (0.05-0.4 g/L) had higher ·OH yield (i.e., 72.51%-89.50%), but with relatively slow ·OH formation rate [i.e., 0.66-3.68 μmol/(L·min)]. CuMn2O4 had the best performance with highest ·OH yield (i.e., 76.61%-89.46%), and fast ·OH formation rate [i.e., 1.10-5.87 μmol/(L·min)] and ·OH production rate increased rapidly along with the catalyst dosage [i.e., 0.014 6 μmol/(min·mg)]. The developed method and the results in this study are helpful for heterogeneous catalysts selection and can provide technical guidance for the practical application of catalytic ozonation process.

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更新日期/Last Update: 2023-07-01