定制 C 缺陷 O 掺杂和 n-π* 过渡唤醒多孔超薄氮化碳,实现高效过一硫酸盐活化:性能和机理洞察

IF 5.9 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES
Meng Tai , Guangbo Che , Tianyu Zhou , Honghui Teng , Chunbo Liu , Bo Hu
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引用次数: 0

摘要

将光催化技术与过氧化单硫酸盐氧化技术相结合,在降解顽固污染物方面具有巨大潜力。本文通过熔融尿素与多聚甲醛的一锅热诱导聚合,定制了一种具有C缺陷O掺杂和高级n-π*转变的多孔超薄氮化碳。通过可见光耦合过氧单硫酸盐活化,DCN-100 可完全光降解 2,4-二氯苯酚,速率常数分别是无过氧单硫酸盐的 CN 和 DCN-100 的 136.6 倍和 37.9 倍。DCN-100 的光吸收波长超过 550 nm,比表面积从 45.03 m2/g 上升到 98.58 m2/g,电荷行为明显改善。详细探讨了多聚甲醛用量、PMS用量、pH值、2,4-二氯苯酚浓度、不同水体、波长和循环时间对光降解性能的影响。通过捕获实验、ESR、LC-MS、福井函数、TEXT毒性评估和DFT理论计算,阐明了DCN-100的主要活性物质、降解途径、中间毒性和活性增强机理。该研究为活化过硫酸盐进行水质修复提供了一种经济、高效、环保的光催化剂。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Tailoring C-defect O-doping and n-π* transition awakened porous ultra-thin carbon nitride for efficient peroxymonosulfate activation: Performances and mechanism insight

Integrating photocatalysis technology with peroxymonosulfate oxidation possesses huge potential for degrading stubborn pollutant. Herein, a porous ultra-thin carbon nitride with C-defect O-doping and advanced n-π* transition was customized by one-pot thermal-induced polymerization of molten urea assisted with paraformaldehyde. Via visible-light coupling peroxymonosulfate activation, the DCN-100 can completely photodegrade 2,4-dichlorophenol, and rate constant is 136.6 and 37.9 times that of CN and DCN-100 without peroxymonosulfate. The light-absorption of DCN-100 surpasses 550 nm, specific surface area rises from 45.03 to 98.58 m2/g, and charge behaviors are significantly improved. The effects of paraformaldehyde amount, PMS dosage, pH, 2,4-dichlorophenol concentration, different water-body, wavelength and recycling times on photodegradation performance were explored in detail. Via capture experiments, ESR, LC-MS, Fukui-function, TEXT toxicity assessment and DFT theoretical calculation, the main active substances, degradation pathway, intermediate toxicity and enhanced activity mechanism of DCN-100 were clarified. The research provides a cost-effective, high-efficiency and environmental-friendly photocatalysts to activate peroxymonosulfate for water remediating.

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来源期刊
Journal of Environmental Sciences-china
Journal of Environmental Sciences-china 环境科学-环境科学
CiteScore
13.70
自引率
0.00%
发文量
6354
审稿时长
2.6 months
期刊介绍: The Journal of Environmental Sciences is an international journal started in 1989. The journal is devoted to publish original, peer-reviewed research papers on main aspects of environmental sciences, such as environmental chemistry, environmental biology, ecology, geosciences and environmental physics. Appropriate subjects include basic and applied research on atmospheric, terrestrial and aquatic environments, pollution control and abatement technology, conservation of natural resources, environmental health and toxicology. Announcements of international environmental science meetings and other recent information are also included.
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