Modulating pollutant adsorption and peroxymonosulfate activation sites on Co3O4@N,O doped-carbon shell for boosting catalytic degradation activity

IF 5.9 4区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR 结构化学 Pub Date : 2024-08-01 DOI:10.1016/j.cjsc.2024.100332
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Abstract

The construction of double active sites for pollutant adsorption and peroxymonosulfate (PMS) activation on the surface of catalyst is conducive to further enhancing the pollutant-removing effect. Herein, a N,O co-doped carbon-encapsulated tricobalt tetraoxide (Co3O4@N,O–C) with double active sites is prepared by a one-step laser carbonization method. The optimized Co3O4@N,O–C shows excellent tetracycline (TC) removal ability, in which the k value reaches 0.608 min−1. On the surface of Co3O4@N,O–C, TC is adsorbed to the N site, and PMS is activated at the O site. Building double active sites on the catalyst surface not only avoids competition for the active site, but also confines the pollutant molecules to the surface of the catalyst, thus shortening the migration distance between reactive oxygen species (ROS) and the pollutant and boosting the removal efficiency of pollutants. In addition, the Co3O4@N,O–C/PMS system exhibits both good resistance to environmental interference and cyclic stability. Finally, a practical continuous flow reactor based on Co3O4@N,O–C catalyst is built, which shows a stable and efficient TC degradation performance.

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调节掺杂碳壳 Co3O4@N,O 上的污染物吸附和过一硫酸盐活化位点以提高催化降解活性
在催化剂表面构建吸附污染物和过一硫酸盐(PMS)活化的双活性位点有利于进一步提高除污效果。本文采用一步激光碳化法制备了具有双活性位点的 N、O 共掺碳包封四氧化三钴(Co3O4@N,O-C)。优化后的 Co3O4@N,O-C 具有优异的四环素(TC)去除能力,其 k 值达到 0.608 min-1。在 Co3O4@N,O-C 表面,TC 被吸附在 N 位点上,而 PMS 则在 O 位点上被活化。在催化剂表面建立双活性位点不仅可以避免活性位点的竞争,还能将污染物分子限制在催化剂表面,从而缩短活性氧(ROS)与污染物之间的迁移距离,提高污染物的去除效率。此外,Co3O4@N,O-C/PMS 系统还具有良好的抗环境干扰能力和循环稳定性。最后,基于 Co3O4@N,O-C 催化剂构建了一个实用的连续流反应器,该反应器具有稳定高效的 TC 降解性能。
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来源期刊
结构化学
结构化学 化学-晶体学
CiteScore
4.70
自引率
22.70%
发文量
5334
审稿时长
13 days
期刊介绍: Chinese Journal of Structural Chemistry “JIEGOU HUAXUE ”, an academic journal consisting of reviews, articles, communications and notes, provides a forum for the reporting and discussion of current novel research achievements in the fields of structural chemistry, crystallography, spectroscopy, quantum chemistry, pharmaceutical chemistry, biochemistry, material science, etc. Structural Chemistry has been indexed by SCI, CA, and some other prestigious publications.
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