水热合成Ag~+掺杂SrTiO_3可见光催化降解四环素性能和机制
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摘要
采用一步水热法制备纳米Ag-SrTiO_3可见光催化剂,利用X射线衍射、X射线光电子能谱、扫描电镜和紫外可见光吸收光谱等对Ag-SrTiO_3的组成、形貌及吸光性进行表征,通过对四环素(TC)的降解实验研究了其在可见光下的光催化活性和稳定性,并进一步通过光致发光光谱、电子自旋共振和自由基捕获实验探究了其对TC的降解机制。结果表明,Ag+可成功掺杂到SrTiO_3中,且Ag-SrTiO_3的吸收光较纯SrTiO_3明显发生红移;当AgNO_3与Sr(NO_3)_2的摩尔分数为3%时,制备的Ag-SrTiO_3对TC的光降解效果最好,120min内降解率可达79.63%,较纯SrTiO_3提高13倍,光催化降解TC反应过程符合准一级动力学模型,且重复使用8次后仍具有较高光催化活性;Ag-SrTiO_3中Ag+捕获了SrTiO_3产生的电子,有效抑制了电子和空穴的复合概率,从而增加其光催化活性,且其主要活性物种为·O_2~–。
Nano-Ag-SrTiO_3 visible-light catalyst was prepared by one-step hydrothermal method. Composition, morphology and structure, visible-light absorption performance of Ag-SrTiO_3 were characterized by X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS), scanning electron microscopy(SEM), and ultraviolet visible absorption spectra(UV-vis), respectively. Photocatalytic property and stability of Ag-SrTiO_3 in visible-light were studied by tetracycline(TC) degradation experiment, and its degradation mechanism for TC was also investigated by photoluminescence spectra(PL), electron spin resonance(ESR) analysis and free radical capture experiment. The results showed that Ag~+ could be well doped in SrTiO_3, and the absorption spectra of Ag-SrTiO_3 significantly redshifted compared with pure SrTiO_3. The photocatalytic property of Ag-SrTiO_3 for TC degradation was optimal while the molar ratio of AgNO_3 and Sr(NO_3)_2 was 3%, and its degradation rate could reach 79.63% within 120 min, 13 times higher than pure SrTiO_3. Furthermore, TC degradation of Ag-SrTiO_3 showed a good compliance with the pseudo-first-order kinetic model. Ag-SrTiO_3 still had excellent photocatalytic degradation activity after 8 times reuse. Electronics generated in SrTiO_3 was captured by Ag+ in Ag-SrTiO_3. The compound probability of electron and hole could be effectively restrained, which resulted in the increase of photocatalytic properties. The main active species of Ag-SrTiO_3 was ·O_2~–.
Nano-Ag-SrTiO_3 visible-light catalyst was prepared by one-step hydrothermal method. Composition, morphology and structure, visible-light absorption performance of Ag-SrTiO_3 were characterized by X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS), scanning electron microscopy(SEM), and ultraviolet visible absorption spectra(UV-vis), respectively. Photocatalytic property and stability of Ag-SrTiO_3 in visible-light were studied by tetracycline(TC) degradation experiment, and its degradation mechanism for TC was also investigated by photoluminescence spectra(PL), electron spin resonance(ESR) analysis and free radical capture experiment. The results showed that Ag~+ could be well doped in SrTiO_3, and the absorption spectra of Ag-SrTiO_3 significantly redshifted compared with pure SrTiO_3. The photocatalytic property of Ag-SrTiO_3 for TC degradation was optimal while the molar ratio of AgNO_3 and Sr(NO_3)_2 was 3%, and its degradation rate could reach 79.63% within 120 min, 13 times higher than pure SrTiO_3. Furthermore, TC degradation of Ag-SrTiO_3 showed a good compliance with the pseudo-first-order kinetic model. Ag-SrTiO_3 still had excellent photocatalytic degradation activity after 8 times reuse. Electronics generated in SrTiO_3 was captured by Ag+ in Ag-SrTiO_3. The compound probability of electron and hole could be effectively restrained, which resulted in the increase of photocatalytic properties. The main active species of Ag-SrTiO_3 was ·O_2~–.
引文
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