| 郝家琛,杨强,崔培昕,王卫轩,罗小三,王玉军.单原子铜改性氮化碳光芬顿降解水体中盐酸四环素及其机理研究[J].农业环境科学学报,2023,42(9):2027-2037. |
| 单原子铜改性氮化碳光芬顿降解水体中盐酸四环素及其机理研究 |
| Photocatalytic degradation of tetracycline hydrochloride in water by single-atom copper-modified carbon nitride |
| 投稿时间：2023-05-06 修订日期：2023-07-06 |
| DOI：10.11654/jaes.2023-0350 |
| 中文关键词: 抗生素 水环境污染 单原子 氮化碳 光芬顿 |
| 英文关键词: antibiotic environmental water contamination single-atom material carbon nitride Photo-Fenton |
| 基金项目:国家自然科学基金项目（42225701，42077145）；土壤污染防治专项资金项目（新沂采单〔2021〕1468） |
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| 中文摘要: |
| 本研究采用一步热解法合成了单原子铜改性的氮化碳光催化材料（Cu-CN），并通过同步辐射X射线吸收谱、高分辨透射电子显微镜、电子顺磁波谱和光致发光光谱等表征手段对该催化剂性质及其光芬顿降解抗生素盐酸四环素（Tetracycline，TC）降解机理进行深入研究。结果表明： Cu-CN可以在30 min内降解超过90%的TC，反应速率常数达到0.009 93 min-1，是未改性氮化碳催化剂的7.76倍，单原子Cu的引入可以显著提升氮化碳的光催化活性。同步辐射X射线吸收谱结果显示形成的Cu-N键可快速将光生电子传递给Cu，促进电子空穴空间分离，从而提升光催化活性；同时Cu（Ⅰ）与Cu（Ⅱ）的循环还可以迅速活化双氧水产生羟基自由基（·OH）。光生电子、空穴和·OH参与了TC降解反应，其中空穴起主导作用。在实际水体中，Cu-CN光芬顿体系依然有良好的TC降解效果，说明该催化剂具有很好的环境适应能力和实际应用前景。 |
| 英文摘要: |
| This study focused on a single-atom, Cu-doped carbon nitride photocatalyst synthesized by a one-step pyrolysis method. The properties of the materials and mechanism of tetracycline hydrochloride(TC)degradation were investigated by synchrotron radiation-based X-ray absorption spectroscopy, scanning transmission electron microscopy, electron paramagnetic spectroscopy, and photoluminescence spectroscopy. Study findings showed that Cu-CN could degrade more than 90% TC within 30 minutes. The reaction rate constant values reached 0.009 93 min-1, which is 7.76 times higher than that of unmodified carbon nitride material. The single-atom Cu sites significantly improved the photocatalytic activity of carbon nitride. The results of synchrotron radiation X-ray absorption spectra showed that the formed Cu-N bond could rapidly transfer photogenerated electrons to Cu, promoting the separation of electrons and holes and enhancing photocatalytic activity. Further, Cu(Ⅰ)and Cu(Ⅱ)cycling could rapidly activate hydrogen peroxide to produce ·OH radicals. Electrons, holes, and ·OH radicals participated in TC degradation where holes played a leading role. In lake water, the Photo-Fenton system of CuCN had an excellent TC degradation effect, indicating that the material has outstanding environmental adaptability and practical application potential. |
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