高氧空位催化剂CeO2/Al2O3-SiC的制备及其对煤化工废水中有机污染物的催化臭氧化作用机理

IF 6.3 2区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of water process engineering Pub Date : 2024-11-30 DOI:10.1016/j.jwpe.2024.106684

Pengfei Li , Yongjun Liu , Zhuangzhuang Yang , Lu Yang , Pan Liu , Zhe Liu , Xiaowei Li

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引用次数: 0

摘要

煤化工废水中芳香族有机物的完全无害化处理一直是水处理工程中的一大难题。本研究通过设计和制备一种基于SiC载体的高氧空位铈铝双金属催化剂来解决这一问题。结果表明：CeO2和Al2O3均匀地分散在SiC表面，复合材料呈现有序的立方结构；研究了臭氧氧化催化剂的降解效率和增强机理。当化学需氧量（COD）浓度超过600 mg/L时，O3与CeO2/Al2O3-SiC的协同作用使苯酚的降解效率从单独使用O3的50%提高到99%，COD从42%提高到78%。CeO2/Al2O3-SiC具有较高的氧空位浓度（OVs = 48.57%）。进一步研究表明，氧空位（OVs）是臭氧吸附和活性氧（ROSs）生成的主要活性位点。电子顺磁共振（EPR）和淬火实验也证实了O3、•O2−1、1O2是主要的活性氧化因子，而不是•OH。此外，即使在催化剂颗粒化之后，它仍然可以达到99%的酚类降解。因此，本研究为CCW的完全无害化处理提供了理论支持，具有广阔的工业应用前景。

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Preparation of high oxygen vacancies catalyst CeO2/Al2O3-SiC and its mechanism in enhancing the catalytic ozonation of organic pollutants in coal chemical wastewater

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Preparation of high oxygen vacancies catalyst CeO2/Al2O3-SiC and its mechanism in enhancing the catalytic ozonation of organic pollutants in coal chemical wastewater

The complete harmless treatment of aromatic organic compounds in coal chemical wastewater (CCW) has always been a big challenge in water process engineering. This study addresses the issue by designing and preparing a kind of Ce and Al bimetallic catalyst with high oxygen vacancies (OVs) based on SiC carrier. The results showed that CeO₂ and Al₂O₃ were uniformly dispersed on SiC, and the composite material exhibited an ordered cubic structure. The degradation efficiency and enhancement mechanism of the catalyst with ozone oxidation were investigated. When applied to actual CCW with a chemical oxygen demand (COD) concentration exceeding 600 mg/L, the synergy between O₃ and CeO₂/Al₂O₃-SiC increased the degradation efficiency of phenols from 50 % to 99 % and COD from 42 % to 78 % compared to using O₃ alone. CeO₂/Al₂O₃-SiC had a high concentration of oxygen vacancies (OVs = 48.57 %). Further research indicated that oxygen vacancies (OVs) were the main active sites for ozone adsorption and reactive oxygen species (ROSs) generation. Electron paramagnetic resonance (EPR) and quenching experiments also confirmed that O₃, •O₂⁻¹, ¹O₂ were the main active oxidation factors, rather than •OH. Additionally, even after granulating the catalyst, it still achieved 99 % degradation of phenols. Therefore, this study provides theoretical support for the complete harmless treatment of CCW and has broad prospects for industrial application.

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来源期刊

Journal of water process engineering Biochemistry, Genetics and Molecular Biology-Biotechnology

CiteScore

10.70

自引率

8.60%

发文量

846

审稿时长

24 days

期刊介绍： The Journal of Water Process Engineering aims to publish refereed, high-quality research papers with significant novelty and impact in all areas of the engineering of water and wastewater processing . Papers on advanced and novel treatment processes and technologies are particularly welcome. The Journal considers papers in areas such as nanotechnology and biotechnology applications in water, novel oxidation and separation processes, membrane processes (except those for desalination) , catalytic processes for the removal of water contaminants, sustainable processes, water reuse and recycling, water use and wastewater minimization, integrated/hybrid technology, process modeling of water treatment and novel treatment processes. Submissions on the subject of adsorbents, including standard measurements of adsorption kinetics and equilibrium will only be considered if there is a genuine case for novelty and contribution, for example highly novel, sustainable adsorbents and their use: papers on activated carbon-type materials derived from natural matter, or surfactant-modified clays and related minerals, would not fulfil this criterion. The Journal particularly welcomes contributions involving environmentally, economically and socially sustainable technology for water treatment, including those which are energy-efficient, with minimal or no chemical consumption, and capable of water recycling and reuse that minimizes the direct disposal of wastewater to the aquatic environment. Papers that describe novel ideas for solving issues related to water quality and availability are also welcome, as are those that show the transfer of techniques from other disciplines. The Journal will consider papers dealing with processes for various water matrices including drinking water (except desalination), domestic, urban and industrial wastewaters, in addition to their residues. It is expected that the journal will be of particular relevance to chemical and process engineers working in the field. The Journal welcomes Full Text papers, Short Communications, State-of-the-Art Reviews and Letters to Editors and Case Studies