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Carbon nitride with a tailored electronic structure toward peroxymonosulfate activation: A direct electron transfer mechanism for organic pollutant degradation
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2023-09-19 , DOI: 10.1016/j.apcatb.2023.123314
Hongbo Ming , Xiaoqiong Bian , Jiajia Cheng , Can Yang , Yidong Hou , Kaining Ding , Jinshui Zhang , Masakazu Anpo , Xinchen Wang

The persulfate-based nonradical reaction process has gained increasing attention in removing organic contaminants, and the process dramatically needs affordable, robust, high-performance heterogeneous catalysts. Herein, dimethyl formamide (DMF) incorporated graphitic carbon nitride (DCN) was synthesized. The molecular engineering of the heptazine unit in DCN improves the electron mobility, strengthens the built-in electric field, and provides abundant active sites, thus enabling DCN to efficiently activate PMS for organic degradation, with 100 % removal of BPA within 12 min. The investigation of the reactive species and electrochemical properties confirmed the direct electron transfer in the PMS activation for organic degradation over DCN. More importantly, DCN can be used as a membrane catalyst in a flowing catalytic unit, enabling continuous water purification and catalyst regeneration. This work provides novel guidance for metal-free catalyst design and profound insights into the persulfate-based heterogeneous catalytic oxidation process for water decontamination technology.

中文翻译:

具有针对过一硫酸盐活化的定制电子结构的氮化碳:有机污染物降解的直接电子转移机制

基于过硫酸盐的非自由基反应过程在去除有机污染物方面受到越来越多的关注,并且该过程迫切需要经济实惠、坚固、高性能的多相催化剂。在此,合成了掺有石墨碳氮化物(DCN)的二甲基甲酰胺(DMF)。 DCN中七嗪单元的分子工程提高了电子迁移率,增强了内置电场,并提供了丰富的活性位点,从而使DCN能够有效激活PMS进行有机降解,在12分钟内100%去除BPA。对活性物质和电化学性质的研究证实了 DCN 上有机降解的 PMS 活化中的直接电子转移。更重要的是,DCN可以用作流动催化装置中的膜催化剂,实现连续的水净化和催化剂再生。这项工作为无金属催化剂设计提供了新颖的指导,并对水净化技术中基于过硫酸盐的非均相催化氧化过程提供了深刻的见解。
更新日期:2023-09-19
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