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Catalytic wet peroxide oxidation with in-situ generated H2O2: An efficient strategy for improving the stability of metal-organic framework catalysts
Catalysis Today ( IF 5.2 ) Pub Date : 2023-08-02 , DOI: 10.1016/j.cattod.2023.114316
Viet Le Nam Vo , Thi-Thuy Luu , Young-Min Chung

Although catalytic wet peroxide oxidation (CWPO) may offer an efficient method for wastewater treatment, the use of metal-organic framework (MOF) catalysts for the CWPO reaction in the presence of H2O2 is challenging because the MOF structure is highly vulnerable to water and/or oxidizing agents. Herein, a range of M-1,3,5-benzenetricarboxylate (BTCs) (M = Fe, Co, Mn, and Cu) were prepared, and their catalytic activities in the CWPO of methyl orange (MO) were evaluated. To examine the stability of the M-BTCs under different reaction conditions, the CWPO reaction was performed with ready-made H2O2 (CWPO-I) or in-situ generated H2O2 using H2 and O2 (CWPO-II). In the latter, Pd was supported onto an M-BTC (Pd/M-BTC). The CWPO-I reaction rate was significantly affected by the metal nodes of the M-BTC, with the Fe-BTC catalyst showing the fastest MO degradation rate. However, regardless of the type of metal node, the M-BTC catalysts underwent significant decomposition during the CWPO-I reaction, leading to a considerable decrease in their textural properties. This result suggests that the M-BTC structure collapsed due to attack by the hydroxyl radicals generated during the reaction. Therefore, the activity of the regenerated Fe-BTC catalyst significantly decreased to 40% of that of the fresh catalyst. In contrast, the catalyst stability in CWPO-II outperformed that in CWPO-I. The Pd/Fe-BTC catalyst exhibited a moderate decrease in activity owing to the gradually reduced surface area of the catalyst during the recycling runs, and the crystallinity of Fe-BTC was preserved. Moreover, the content, particle size, and electronic properties of Pd supported on Fe-BTC showed little change after the reaction. These results demonstrate that the use of in-situ generated H2O2 is superior for impeding the catalyst deactivation caused by structural deformation of the MOF.



中文翻译:

原位生成 H2O2 的催化湿式过氧化物氧化:提高金属有机骨架催化剂稳定性的有效策略

虽然催化湿式过氧化物氧化 (CWPO) 可以为废水处理提供一种有效的方法,但在 H 2 O 2存在的情况下使用金属有机骨架 (MOF) 催化剂进行 CWPO 反应具有挑战性,因为 MOF 结构非常容易受到水和/或氧化剂。在此,制备了一系列 M-1,3,5-苯三甲酸酯 (BTC)(M = Fe、Co、Mn 和 Cu),并评估了它们在甲基橙 (MO) CWPO 中的催化活性。为了检查M-BTC在不同反应条件下的稳定性,使用现成的H 2 O 2 (CWPO-I)或使用H 2原位生成的H 2 O 2进行CWPO反应和氧气2(CWPO-II)。在后者中,Pd 由 M-BTC (Pd/M-BTC) 支持。CWPO-I 反应速率受 M-BTC 金属节点的显着影响,其中 Fe-BTC 催化剂表现出最快的 MO 降解速率。然而,无论金属节点的类型如何,M-BTC 催化剂在 CWPO-I 反应过程中都会发生明显的分解,导致其织构性能大幅下降。这一结果表明,M-BTC 结构由于反应过程中产生的羟基自由基的攻击而崩溃。因此,再生后的Fe-BTC催化剂的活性显着下降至新鲜催化剂的40%。相比之下,CWPO-II 的催化剂稳定性优于 CWPO-I。由于在回收过程中催化剂的表面积逐渐减小,Pd/Fe-BTC 催化剂的活性适度下降,并且 Fe-BTC 的结晶度得以保留。此外,反应后Fe-BTC负载的Pd含量、粒径和电子性能几乎没有变化。这些结果表明,使用原位产生的H 2 O 2对于阻止MOF结构变形引起的催化剂失活具有优异的作用。

更新日期:2023-08-05
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