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Construction of solid frustrated-Lewis-pairs in porous nanoceria for boosting catalytic ozonation of refractory organic pollutants
Separation and Purification Technology ( IF 8.1 ) Pub Date : 2024-11-19 , DOI: 10.1016/j.seppur.2024.130613 Shujuan Zhan, Yiqing Li, Lianpeng Sun, Chun He, Ya Xiong, Shuanghong Tian
Separation and Purification Technology ( IF 8.1 ) Pub Date : 2024-11-19 , DOI: 10.1016/j.seppur.2024.130613 Shujuan Zhan, Yiqing Li, Lianpeng Sun, Chun He, Ya Xiong, Shuanghong Tian
Catalytic ozonation is an efficient method to eliminate refractory organic pollutants from wastewater. Defect engineering of metal oxides can construct new actives and regulate catalytic performance. Herein abundant solid frustrated Lewis pairs (FLPs) were constructed in porous nanoceria by surface defect engineering. The obtained FLPs-CeO2 had a high reaction rate constant of 7.99 × 10-2 min−1 towards the oxidation of refractory pollutants, and boosted the mineralization rate within 90 min from 14.2 ± 2.7 % to 72.4 ± 3 %. The experimental and DFT calculation investigations reveal that FLPs significantly decreased the energy barrier of the adsorption and activation of ozone over CeO2. Thus, a large amount of reactive oxygen species, especially surface oxygen atom (*O) and •OH, were produced for the efficient oxidation of refractory pollutants. As a proof of concept, this study paves the way for rational design of active FLP-catalysts for catalytic ozonation applied in efficient wastewater treatment
中文翻译:
在多孔纳米铈中构建固体受挫路易斯对,促进难降解有机污染物的催化臭氧化
催化臭氧化是去除废水中难降解有机污染物的有效方法。金属氧化物的缺陷工程可以构建新的活性物质并调节催化性能。本文通过表面缺陷工程在多孔纳米氧化铈中构建了丰富的固体受挫路易斯对 (FLP)。所得的 FLPs-CeO2 对难降解污染物的氧化反应速率常数为 7.99 × 10-2 min−1,并在 90 分钟内将矿化速率从 14.2 ± 2.7 % 提高到 72.4 ± 3 %。实验和 DFT 计算研究表明,FLPs 显着降低了 CeO2 对臭氧吸附和活化的能垒。因此,产生了大量的活性氧,特别是表面氧原子 (*O) 和 •OH,用于有效氧化难降解污染物。作为概念验证,本研究为合理设计用于高效废水处理的催化臭氧化活性 FLP 催化剂铺平了道路
更新日期:2024-11-20
中文翻译:
在多孔纳米铈中构建固体受挫路易斯对,促进难降解有机污染物的催化臭氧化
催化臭氧化是去除废水中难降解有机污染物的有效方法。金属氧化物的缺陷工程可以构建新的活性物质并调节催化性能。本文通过表面缺陷工程在多孔纳米氧化铈中构建了丰富的固体受挫路易斯对 (FLP)。所得的 FLPs-CeO2 对难降解污染物的氧化反应速率常数为 7.99 × 10-2 min−1,并在 90 分钟内将矿化速率从 14.2 ± 2.7 % 提高到 72.4 ± 3 %。实验和 DFT 计算研究表明,FLPs 显着降低了 CeO2 对臭氧吸附和活化的能垒。因此,产生了大量的活性氧,特别是表面氧原子 (*O) 和 •OH,用于有效氧化难降解污染物。作为概念验证,本研究为合理设计用于高效废水处理的催化臭氧化活性 FLP 催化剂铺平了道路