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氮化碳中的掺杂和缺陷导致原位高效合成羟基自由基,从而实现高效的光催化杀菌。

Doping and defects in carbon nitride cause efficient in situ HO synthesis to allow efficient photocatalytic sterilization.

作者信息

Li Xinyu, Wang Hui, Li Shunlin, Xu Ye, Bian Zhaoyong

机构信息

Beijing Key Lab for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, China; Engineering Research Center for Water Pollution Source Control & Eco-remediation, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, China.

Beijing Key Lab for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, China; Engineering Research Center for Water Pollution Source Control & Eco-remediation, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, China.

出版信息

Sci Total Environ. 2024 May 20;926:172109. doi: 10.1016/j.scitotenv.2024.172109. Epub 2024 Mar 30.

Abstract

In situ photocatalytic synthesis of HO for disinfection has attracted widespread attention because it is a clean and environmentally friendly sterilization method. Graphitic carbon nitride has been used as a very selective photocatalyst for HO generation but has some limitations (e.g., insufficient light absorption, rapid electron-hole recombination, and slow direct two-electron reduction processes) that prevent efficient HO production. In this study, potassium-doped graphite carbon nitride with nitrogen vacancies (NDKCN) was prepared using a simple method involving a thermal fusion salt and N calcination, which possessed an ultrathin nanosheet structure (1.265 nm) providing abundant active sites. Synergistic effects caused by nitrogen vacancies and K and I doping in the NDKCN photocatalyst gave the NDKCN a good ability to absorb light, undergo fast charge transfer, and give a high photoelectric current response. The optimized photocatalytic HO yield of the NDKCN was 780.1 μM·g·min, which was 10 times the yield of the pristine g-CN. Tests involving quenching reactive species, electron spin resonance, and rotating disk electrodes indicated that one-step two-electron direct reduction on the NDKCN caused excellent HO generation performance. The ability to efficiently generate HO in situ gave NDKCN an excellent bactericidal performance, and 7.3 log (colony-forming units·mL) of Escherichia coli were completely eliminated within 80 min. Scanning electron microscopy images before and after sterilization indicated the changes in bacteria caused by the catalytic activity. The new g-CN-based photocatalyst and similar rationally designed photocatalysts with doping and defects offer efficient and simple in situ HO sterilization.

摘要

原位光催化合成用于消毒的羟基自由基(HO)因其是一种清洁环保的杀菌方法而备受关注。石墨相氮化碳已被用作一种非常有选择性的用于生成HO的光催化剂,但存在一些局限性(例如,光吸收不足、快速的电子 - 空穴复合以及缓慢的直接双电子还原过程),这阻碍了高效的HO生成。在本研究中,采用一种涉及热熔盐和N煅烧的简单方法制备了具有氮空位的钾掺杂石墨相氮化碳(NDKCN),其具有超薄纳米片结构(1.265纳米),提供了丰富的活性位点。NDKCN光催化剂中氮空位以及K和I掺杂所引起的协同效应赋予了NDKCN良好的光吸收能力、快速的电荷转移能力以及高的光电流响应。NDKCN优化后的光催化HO产率为780.1 μM·g·min,是原始g - CN产率的10倍。涉及猝灭活性物种、电子自旋共振和旋转圆盘电极的测试表明,NDKCN上的一步双电子直接还原导致了优异的HO生成性能。原位高效生成HO的能力赋予了NDKCN优异的杀菌性能,在80分钟内可完全消除7.3 log(菌落形成单位·mL)的大肠杆菌。杀菌前后的扫描电子显微镜图像显示了催化活性引起的细菌变化。这种新型的基于g - CN的光催化剂以及类似的经过合理设计的具有掺杂和缺陷的光催化剂提供了高效且简单的原位HO杀菌方法。

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