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空化强化袋增强了 Pd/AlO 催化剂的超声先进氧化。

Cavitation intensifying bags improve ultrasonic advanced oxidation with Pd/AlO catalyst.

机构信息

Mesoscale Chemical Systems Group, Faculty of Science and Technology, MESA+ Institute for Nanotechnology, and University of Twente, PO Box 217, 7500 AE Enschede, The Netherlands; Delft University of Technology, Delft, The Netherlands.

Catalytic Processes and Materials Group, Faculty of Science and Technology, MESA+ Institute for Nanotechnology, University of Twente, PO Box 217, 7500 AE Enschede, The Netherlands.

出版信息

Ultrason Sonochem. 2021 Jan;70:105324. doi: 10.1016/j.ultsonch.2020.105324. Epub 2020 Sep 7.

Abstract

Advanced oxidation processes can potentially eliminate organic contaminants from industrial waste streams as well as persistent pharmaceutical components in drinking water. We explore for the first time the utilization of Cavitation Intensifying Bags (CIB) in combination with Pd/AlO catalyst as possible advanced oxidation technology for wastewater streams, oxidizing terephthalic acid (TA) to 2-hydroxyterephthalic acid (HTA). The detailed characterization of this novel reaction system reveals that, during sonication, the presence of surface pits of the CIB improves the reproducibility and thus the control of the sonication process, when compared to oxidation in non-pitted bags. Detailed reaction kinetics shows that in the CIB reactor the reaction order to TA is zero, which is attributed to the large excess of TA in the system. The rate of HTA formation increased ten-fold from ~0.01 μMmin during sonication in the CIB, to ~0.10 μMmin for CIB in the presence of the Pd/AlO catalyst. This enhancement was ascribed to a combination of improved mass transport, the creation of thermal gradients, and Pd/AlO catalyst near the cavitating bubbles. Further analysis of the kinetics of HTA formation on Pd/AlO indicated that initially the reaction underwent through an induction period of 20 min, where the HTA concentration was ~0.3 μM. After this, the reaction rate increased reaching HTA concentrations ~6 μM after 40 min. This behavior resembled that observed during oxidation of hydrocarbons on metal catalysts, where the slow rate formation of hydroperoxides on the metal surface is followed by rapid product formation upon reaching a critical concentration. Finally, a global analysis using the Intensification Factor (IF) reveals that CIB in combination with the Pd/AlO catalyst is a desirable option for the oxidation of TA when considering increased oxidation rates and costs.

摘要

高级氧化工艺有潜力消除工业废水中的有机污染物以及饮用水中持久性药物成分。我们首次探索了将空化强化袋(CIB)与 Pd/AlO 催化剂结合作为废水处理的先进氧化技术,用于氧化对苯二甲酸(TA)为 2-羟基对苯二甲酸(HTA)。该新型反应体系的详细特性表明,在超声过程中,CIB 的表面凹坑提高了可重复性,从而控制了超声过程,与非凹坑袋中的氧化相比。详细的反应动力学表明,在 CIB 反应器中,TA 的反应级数为零,这归因于体系中 TA 的大量过剩。在 CIB 反应器中,HTA 的形成速率从 CIB 中超声时的0.01 μM*min 增加到 10 倍,至0.10 μM*min,当存在 Pd/AlO 催化剂时。这种增强归因于传质的改善、热梯度的产生以及 Pd/AlO 催化剂在空化气泡附近。对 Pd/AlO 上 HTA 形成动力学的进一步分析表明,最初反应经历了 20 min 的诱导期,HTA 浓度约为0.3 μM。在此之后,反应速率增加,40 min 后达到 HTA 浓度6 μM。这种行为类似于在金属催化剂上氧化烃类时观察到的情况,其中金属表面上氢过氧化物的形成速率较慢,然后在达到临界浓度后快速形成产物。最后,使用强化因子(IF)进行的全局分析表明,当考虑到氧化速率和成本的提高时,CIB 与 Pd/AlO 催化剂结合是 TA 氧化的理想选择。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/464c/7786540/1262967860b6/ga1.jpg

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