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钴掺杂g-C_(3)N_(4)光催化降解盐酸多西环素的性能与机理研究

Photocatalytic degradation of doxycycline hydrochloride by cobalt-doped g-C_(3)N_(4):Performance and mechanism
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摘要 以三聚氰胺和六水合硝酸钴作为前驱体,通过高温煅烧-溶剂热法制备不同掺杂比例的Co/g-C_(3)N_(4)纳米材料。粉末X射线衍射(XRD)、X射线光电子能谱(XPS)、傅里叶变换红外光谱(FT-IR)、透射电镜(TEM)及稳态光致发光光谱(PL)等表征结果表明,Co以Co^(2+)/Co^(3+)混合价态成功锚定于g-C_(3)N_(4)表面,有效提升了光生载流子的分离效率。当Co掺杂量为0.90%时,材料表现出最优的光催化活性,其对DOH的降解效率常数(k=0.0158 min^(-1))较纯g-C_(3)N_(4)(k=0.0064 min^(-1))提升2.47倍(准一级动力学拟合)。通过价态分析发现,光催化过程中Co^(3+)被还原为Co^(2+)(Co^(2+)/Co^(3+)比例从1∶0.77变为1∶0.39)。自由基猝灭实验证实·O_(2)^(-)为关键活性氧物种。 Co/g-C_(3)N_(4)nanomaterials with varied doping ratios were synthesized using melamine and cobalt(Ⅱ)nitrate hexahydrate as precursors through a thermal calcination-solvothermal method.Characterization results obtained from powder X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),Fourier transform infrared spectroscopy(FT-IR),transmission electron microscopy(TEM),and steady-state photoluminescence spectroscopy(PL)demonstrate that cobalt species,predominantly in the mixed Co^(2+)/Co^(3+)valence states,were successfully anchored onto the surface of g-C_(3)N_(4),which effectively enhanced the separation efficiency of photogenerated charge carriers.Optimal photocatalytic activity was achieved at Co doping level of 0.90 wt%.The corresponding degradation rate constant for DOH(k=0.0158 min^(-1)),determined via pseudo-first-order kinetics fitting,was 2.47 times higher than that of pristine g-C_(3)N_(4)(k=0.0064 min^(-1)).Valence state analysis revealed that Co^(3+)was reduced to Co^(2+)during the photocatalytic process,with the Co^(2+)/Co^(3+)ratio increasing from 1∶0.77 to 1∶0.39.Radical quenching experiments confirmed that the·O_(2)^(-) was the predominant reactive oxygen species.
作者 刘青志 刘玉娇 王霞 符袅 邹亚 何洁丽 LIU Qing-zhi;LIU Yu-jiao;WANG Xia;FU Niao;ZOU Ya;HE Jie-li(Yunnan Provincial Key Laboratory of Entomological Biopharmaceutical R&D,College of Pharmacy,Dali University,Dali 671000,China)
机构地区 大理大学药学院
出处 《现代化工》 2026年第3期109-116,共8页 Modern Chemical Industry
基金 国家自然科学基金地区基金(22162002) 云南省科技厅基础研究计划项目(202501AT070426)。
关键词 钴掺杂氮化碳 盐酸多西环素 光催化降解 cobalt-doped graphitic carbon nitride doxycycline hyclate photocatalytic degradation

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