Strategic defect engineering in TiO2 catalysts through electron beam irradiation: Unraveling enhanced photocatalytic pathways for multicomponent VOCs degradation

IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Separation and Purification Technology Pub Date : 2024-11-27 DOI:10.1016/j.seppur.2024.130804
Jianghua Huang, Xiangbo Feng, Fukun Bi, Genghuai Huang, Renzhi Rao, Rong Qiao, Xiaodong Zhang
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Abstract

Defect engineering improves catalytic activity, electron transport efficiency, and stability by introducing defects such as oxygen vacancies, offering significant potential for applications in environmental remediation and energy conversion. Electron beam (EB) irradiation has emerged as a key technique in defect engineering, renowned for its mild reaction conditions and precise defect construction capabilities. This study synthesized defect-rich commercial TiO2 catalysts (P25) using high-energy EB irradiation to investigate the photodegradation efficiency of multicomponent VOCs. The EB irradiation technique promoted the formation of oxygen vacancies, which played a key role in the adsorption and activation of pollutant molecules. DFT calculations further confirmed the superior photocatalytic activity of the irradiated P25 catalyst. The photodegradation experiments showed that the 300P25 degraded pure ethyl acetate up to 99.05 % (40 min) and acetone up to 97.14 % (60 min), but toluene only up to 7.34 % (60 min). Interestingly, in acetone and toluene mixture, 300P25 achieved toluene removal as high as 68 % (60 min) with a rate constant (k) of 0.0181 min−1, a 12.1-fold than pure toluene (0.0015 min−1). In-situ infrared spectroscopy analysis revealed that during the simultaneous degradation of toluene and acetone, acetone significantly promoted the deep oxidation of toluene, leading to the rapid oxidation of intermediate products (benzyl alcohol and benzaldehyde) to benzoic acid and smaller molecules. This work provides important guidance for developing efficient and stable photocatalysts for degrading multicomponent VOCs.

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通过电子束辐照对二氧化钛催化剂进行战略性缺陷工程:揭示多组分挥发性有机化合物降解的增强型光催化途径
缺陷工程通过引入氧空位等缺陷来提高催化活性、电子传输效率和稳定性,为环境修复和能源转换领域的应用提供了巨大潜力。电子束(EB)辐照因其温和的反应条件和精确的缺陷构建能力而成为缺陷工程的关键技术。本研究利用高能电子束辐照合成了富缺陷商用二氧化钛催化剂(P25),以研究多组分挥发性有机化合物的光降解效率。EB 辐照技术促进了氧空位的形成,而氧空位在污染物分子的吸附和活化过程中发挥了关键作用。DFT 计算进一步证实了经过辐照的 P25 催化剂具有优异的光催化活性。光降解实验表明,300P25 对纯乙酸乙酯的降解率高达 99.05%(40 分钟),对丙酮的降解率高达 97.14%(60 分钟),但对甲苯的降解率仅为 7.34%(60 分钟)。有趣的是,在丙酮和甲苯混合物中,300P25 对甲苯的去除率高达 68%(60 分钟),速率常数 (k) 为 0.0181 min-1,是纯甲苯(0.0015 min-1)的 12.1 倍。原位红外光谱分析显示,在甲苯和丙酮同时降解的过程中,丙酮显著促进了甲苯的深度氧化,导致中间产物(苯甲醇和苯甲醛)迅速氧化为苯甲酸和更小的分子。这项工作为开发高效稳定的光催化剂降解多组分挥发性有机化合物提供了重要指导。
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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