新型光催化剂降解盐酸莫西沙星及灭活病原微生物研究
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摘要
自然水体中抗生素物残留及由此而引发的耐药菌群增加,成为两类新兴的环境污染物,采用高级氧化技术是去除这两类环境污染物的有效方法。其中Fenton试剂反应迅速、条件温和、无二次污染；光催化氧化技术氧化效率高,反应速度快,并且可有效利用太阳能,绿色环保,在处理这两类环境污染物中得到较为广泛的应用。本文以盐酸莫西沙星和四种常见致病性微生物为目标,研究了Fenton反应及可见光催化降解水环境中污染物的影响因素和动力学规律。主要研究内容为：
1.采用氧化褪色法建立了Fenton反应中羟基自由基的测定方法,对影响羟基自由基测定的溶液初始pH值、Fe2+浓度、反应温度、反应时间等因素进行了优化,结果表明在一定的浓度范围内,不同类型的染料在最大吸收波长处的吸光度的降低值与体系中加入的H202成线性关系,可以间接测定Fenton反应中羟基自由基的浓度。氧化褪色法方便、快捷可广泛应用于环境领域中羟基自由基、H202和金属离子的测定以及食品、药学领域中功能性物质对羟基自由基、H202清除能力的比较。
2.以盐酸莫西沙星的降解率及降解残留物的抑菌活性为指标,采用响应面分析法优化了Fenton反应降解盐酸莫西沙星的工艺,建立了Fenton反应降解盐酸莫西沙星的数学模型。在pH2.3,Fe2+浓度57μmol·L-1, H2O2浓度100μmol·L-1,温度44℃,降解时间30min的条件下,初始浓度30μmol·L1的盐酸莫西沙星的降解率为85.5%,降解残留物对大肠杆菌的抑菌圈减小至10.6mm。采用Fenton反应对四种致病性微生物大肠杆菌、肺炎克雷伯菌、金黄色葡萄球菌和绿脓假单胞菌进行了灭活,考察了反应体系初始pH、Fe2+浓度、H202浓度、菌体浓度及反应介质对灭活过程的影响,实验结果为城镇及医院污水中致病性病原微生物的灭活提供实验依据。
3.采用超声辅助原位离子交换法制备了AgBr@Ag3PO4(Ag2CO3)复合型光催化剂,采用XRD、SEM、DRS等方法研究其晶型结构、表面形态和吸光强度,探讨了在可见光照射下AgBr@Ag3PO4(Ag2CO3光催化降解盐酸莫西沙星的降解效率及动力学规律,考察复合型光催化剂摩尔比、催化剂用量、盐酸莫西沙星初始浓度、溶液pH值、光照强度对降解率的影响,并研究了其光催化反应机理。XRD分析结果表明,AgBr的复合并未改变本体Ag3PO4(Ag2CO3)的晶型结构,二者之间形成简单的物理复合物。光催化降解盐酸莫西沙星实验表明：AgBr与Ag3PO4(Ag2CO3)形成复合物,有利于光生电子和空穴对的迁移,从而使得复合物具有更高的光催化性能；盐酸莫西沙星的光催化反应符合Langmuir-Hinshelwood一级动力学数学模型。当复合物中Br与P(C)的摩尔比为0.6：1,催化剂浓度1.5gL-1,可见光照射10min, AgBr@Ag3PO4、AgBr@Ag2CO3对盐酸莫西沙星的降解率达到99.8%和95.9%。复合型光催化剂灭活病原微生物实验结果表明,0.2g·L-’的催化剂可在30min内将4种致病性微生物全部杀死。
4.采用Hummers方法制备氧化石墨烯,采用超声辅助共沉淀法制备氧化石墨烯基异质结光催化剂GO@Ag3PO4(Ag2CO3),并用XRD、SEM-TEM、DRS、FT-IR、拉曼光谱等手段对催化剂进行表征,探讨了GO@Ag3PO4光催化降解盐酸莫西沙星的活性及机理。实验结果表明：与氧化石墨烯形成异质结后,Ag3PO4(Ag2CO3)晶型及表面形貌没有发生变化,但是晶体粒径变小,在可见光区对光的吸收得到有效提高。光催化降解实验表明：氧化石墨烯作为有效的电子受体,在异质结中含量为2.5%时,使得光生电子和空穴得到最大程度的分离,催化活性最高,活性要高于AgBr@Ag3PO4(Ag2CO3)复合型光催化剂,并且光催化降解反应亦符合一级反应动力学特性。催化剂稳定性实验结果表明,GO@Ag3PO4、GO@Ag2CO3循环使用四次后,对盐酸莫西沙星的降解率分别为93.3%和89.3%,表现出较高的稳定性。异质结型光催化剂灭活病原微生物实验结果表明,0.2g.L-1的催化剂可在30min内将4种致病性微生物全部杀死,因自身有部分银离子溶解具有杀菌作用,对致病性微生物的灭活活性要高于复合型光催化剂。
Antibiotics residuals and resistant pathogenic bacteria induced by antibiotics residuals became new environmental pollutants. And Advanced Oxidation Processes including Fenton reaction and photocatalytic oxidation technology were pollution control technology for these pollutants. This paper is to study the influencing factors and kinetics properties of degradation Moxifloxacin Hydrochloride(MX) and inactivation of pathogenic bacteria by Fenton reaction and photocatalysts under visible-light irradiation.
1. A new catalytic spectrophotometry method was developed for the determination of hydroxyl radical in Fenton reaction based on the Fe2+catalyzed depletion of dyes by hydrogen peroxide. The influencing factors such as pH、Fe2+concentration、reaction time and temperature were discussed. The proposed method applied to determination hydroxyl radical was simple, rapid and satisfactory, and could be used in environment field to determine hydroxyl radical and in food and pharmacy field to determine scavenging capacity of hydroxyl radical and hydrogen peroxide.
2. With the degradation rate of MX and antibacterial activity as response value, the pH, Fe2+concentration, temperature were optimized by response surface methodology based on single factor experiments in Fenton reaction. The optimal reacting conditions was found to be initial pH2.3,[Fe2+]057μmol·L-1,[H2O2]0100μmol·L-1for MX30μmol·L-1at temperature44℃. Under optimal conditions,85.5%degradation efficiency in aqueous solution was achieved after30min of reaction, which was agreed with model predictions. And the residuals inhibition zone reduced to10.6mm. The pH, Fe2+、H2O2concentration, reaction medium were discussed in inactivation of K. pneumoniae, S. aureus B. pyocyaneus and E. coli by Fenton reaction. The results showed that all the pathogenic bacteria were inactivated in30min.
3. A visible-light response photocatalyst AgBr@Ag3PO4(Ag2CO3) was prepared by in situ ultrasonic assisted anion-exchange method with Ag3PO4(Ag2CO3) as precursor.The synthesized samples were characterized by X-ray diffraction, scanning electron microscopy, and UV-Vis diffuse spectroscopy. The photocatalytic activity of the prepared samples were evaluated by the degradation of MX as simulation pollutant under the visible light (λ>420nm) irradiation. The effect of several parameters such as pH value, catalyst dosage, initial moxifloxacin hydrochloride concentration and recycling runs were discussed. The photocatalysis reactive mechanisms under visible light irradiation were investigated by adding different scavengers. The results indicated that the AgBr could not change the crystal structures of Ag3PO4(Ag2CO3), and a simple physical composite material were formed in each other. The highest efficiency was obtained when the sample with the proportion0.6of Br to P(C). The AgBr@Ag3PO、AgBr@Ag2CO3photocatalyst could degrade MX up to99.8%and95.9%under illumination with500W visible lights for10min when the concentration of photocatalyst was1.5gL-1The photocatalyst could kill all of K. pneumoniae, S. aureus B. pyocyaneus and E. coli in30min with its concentration0.2gL-1.
4. Graphene Oxide was prepared by Hummers method, and then GO@Ag3PO4(Ag2CO3) heterojunction was prepared by in situ ultrasonic assisted co-precipitation method. The synthesized samples were characterized by X-ray diffraction, scanning electron microscopy, UV-Vis diffuse spectroscopy, FT-IR spectroscopy and Roman spectroscopy. The photocatalytic activity and mechanisms of the prepared samples were discussed. The results indicated the efficiency enhanced with the he teroj unction structure formed between Ag3PO4(Ag2CO3) and GO because the enhanced capacity of hole and charge generation and separation.The highest efficiency was obtained when the sample with the proportion2.5of GO. The results indicated that degradation rate MX process conformed to the rule of Langmuir-Hinshelwood kinetics which followed the pseudo-first order reaction. Testing in4recycle experiments, the degradation rate of MX did not change significantly; indicating the excellent stability and reusability.The photocatalyst could kill all of K. pneumoniae, S. aureus B. pyocyaneus and E. coli in30min with its concentration0.2gL-1.
1.采用氧化褪色法建立了Fenton反应中羟基自由基的测定方法,对影响羟基自由基测定的溶液初始pH值、Fe2+浓度、反应温度、反应时间等因素进行了优化,结果表明在一定的浓度范围内,不同类型的染料在最大吸收波长处的吸光度的降低值与体系中加入的H202成线性关系,可以间接测定Fenton反应中羟基自由基的浓度。氧化褪色法方便、快捷可广泛应用于环境领域中羟基自由基、H202和金属离子的测定以及食品、药学领域中功能性物质对羟基自由基、H202清除能力的比较。
2.以盐酸莫西沙星的降解率及降解残留物的抑菌活性为指标,采用响应面分析法优化了Fenton反应降解盐酸莫西沙星的工艺,建立了Fenton反应降解盐酸莫西沙星的数学模型。在pH2.3,Fe2+浓度57μmol·L-1, H2O2浓度100μmol·L-1,温度44℃,降解时间30min的条件下,初始浓度30μmol·L1的盐酸莫西沙星的降解率为85.5%,降解残留物对大肠杆菌的抑菌圈减小至10.6mm。采用Fenton反应对四种致病性微生物大肠杆菌、肺炎克雷伯菌、金黄色葡萄球菌和绿脓假单胞菌进行了灭活,考察了反应体系初始pH、Fe2+浓度、H202浓度、菌体浓度及反应介质对灭活过程的影响,实验结果为城镇及医院污水中致病性病原微生物的灭活提供实验依据。
3.采用超声辅助原位离子交换法制备了AgBr@Ag3PO4(Ag2CO3)复合型光催化剂,采用XRD、SEM、DRS等方法研究其晶型结构、表面形态和吸光强度,探讨了在可见光照射下AgBr@Ag3PO4(Ag2CO3光催化降解盐酸莫西沙星的降解效率及动力学规律,考察复合型光催化剂摩尔比、催化剂用量、盐酸莫西沙星初始浓度、溶液pH值、光照强度对降解率的影响,并研究了其光催化反应机理。XRD分析结果表明,AgBr的复合并未改变本体Ag3PO4(Ag2CO3)的晶型结构,二者之间形成简单的物理复合物。光催化降解盐酸莫西沙星实验表明：AgBr与Ag3PO4(Ag2CO3)形成复合物,有利于光生电子和空穴对的迁移,从而使得复合物具有更高的光催化性能；盐酸莫西沙星的光催化反应符合Langmuir-Hinshelwood一级动力学数学模型。当复合物中Br与P(C)的摩尔比为0.6：1,催化剂浓度1.5gL-1,可见光照射10min, AgBr@Ag3PO4、AgBr@Ag2CO3对盐酸莫西沙星的降解率达到99.8%和95.9%。复合型光催化剂灭活病原微生物实验结果表明,0.2g·L-’的催化剂可在30min内将4种致病性微生物全部杀死。
4.采用Hummers方法制备氧化石墨烯,采用超声辅助共沉淀法制备氧化石墨烯基异质结光催化剂GO@Ag3PO4(Ag2CO3),并用XRD、SEM-TEM、DRS、FT-IR、拉曼光谱等手段对催化剂进行表征,探讨了GO@Ag3PO4光催化降解盐酸莫西沙星的活性及机理。实验结果表明：与氧化石墨烯形成异质结后,Ag3PO4(Ag2CO3)晶型及表面形貌没有发生变化,但是晶体粒径变小,在可见光区对光的吸收得到有效提高。光催化降解实验表明：氧化石墨烯作为有效的电子受体,在异质结中含量为2.5%时,使得光生电子和空穴得到最大程度的分离,催化活性最高,活性要高于AgBr@Ag3PO4(Ag2CO3)复合型光催化剂,并且光催化降解反应亦符合一级反应动力学特性。催化剂稳定性实验结果表明,GO@Ag3PO4、GO@Ag2CO3循环使用四次后,对盐酸莫西沙星的降解率分别为93.3%和89.3%,表现出较高的稳定性。异质结型光催化剂灭活病原微生物实验结果表明,0.2g.L-1的催化剂可在30min内将4种致病性微生物全部杀死,因自身有部分银离子溶解具有杀菌作用,对致病性微生物的灭活活性要高于复合型光催化剂。
Antibiotics residuals and resistant pathogenic bacteria induced by antibiotics residuals became new environmental pollutants. And Advanced Oxidation Processes including Fenton reaction and photocatalytic oxidation technology were pollution control technology for these pollutants. This paper is to study the influencing factors and kinetics properties of degradation Moxifloxacin Hydrochloride(MX) and inactivation of pathogenic bacteria by Fenton reaction and photocatalysts under visible-light irradiation.
1. A new catalytic spectrophotometry method was developed for the determination of hydroxyl radical in Fenton reaction based on the Fe2+catalyzed depletion of dyes by hydrogen peroxide. The influencing factors such as pH、Fe2+concentration、reaction time and temperature were discussed. The proposed method applied to determination hydroxyl radical was simple, rapid and satisfactory, and could be used in environment field to determine hydroxyl radical and in food and pharmacy field to determine scavenging capacity of hydroxyl radical and hydrogen peroxide.
2. With the degradation rate of MX and antibacterial activity as response value, the pH, Fe2+concentration, temperature were optimized by response surface methodology based on single factor experiments in Fenton reaction. The optimal reacting conditions was found to be initial pH2.3,[Fe2+]057μmol·L-1,[H2O2]0100μmol·L-1for MX30μmol·L-1at temperature44℃. Under optimal conditions,85.5%degradation efficiency in aqueous solution was achieved after30min of reaction, which was agreed with model predictions. And the residuals inhibition zone reduced to10.6mm. The pH, Fe2+、H2O2concentration, reaction medium were discussed in inactivation of K. pneumoniae, S. aureus B. pyocyaneus and E. coli by Fenton reaction. The results showed that all the pathogenic bacteria were inactivated in30min.
3. A visible-light response photocatalyst AgBr@Ag3PO4(Ag2CO3) was prepared by in situ ultrasonic assisted anion-exchange method with Ag3PO4(Ag2CO3) as precursor.The synthesized samples were characterized by X-ray diffraction, scanning electron microscopy, and UV-Vis diffuse spectroscopy. The photocatalytic activity of the prepared samples were evaluated by the degradation of MX as simulation pollutant under the visible light (λ>420nm) irradiation. The effect of several parameters such as pH value, catalyst dosage, initial moxifloxacin hydrochloride concentration and recycling runs were discussed. The photocatalysis reactive mechanisms under visible light irradiation were investigated by adding different scavengers. The results indicated that the AgBr could not change the crystal structures of Ag3PO4(Ag2CO3), and a simple physical composite material were formed in each other. The highest efficiency was obtained when the sample with the proportion0.6of Br to P(C). The AgBr@Ag3PO、AgBr@Ag2CO3photocatalyst could degrade MX up to99.8%and95.9%under illumination with500W visible lights for10min when the concentration of photocatalyst was1.5gL-1The photocatalyst could kill all of K. pneumoniae, S. aureus B. pyocyaneus and E. coli in30min with its concentration0.2gL-1.
4. Graphene Oxide was prepared by Hummers method, and then GO@Ag3PO4(Ag2CO3) heterojunction was prepared by in situ ultrasonic assisted co-precipitation method. The synthesized samples were characterized by X-ray diffraction, scanning electron microscopy, UV-Vis diffuse spectroscopy, FT-IR spectroscopy and Roman spectroscopy. The photocatalytic activity and mechanisms of the prepared samples were discussed. The results indicated the efficiency enhanced with the he teroj unction structure formed between Ag3PO4(Ag2CO3) and GO because the enhanced capacity of hole and charge generation and separation.The highest efficiency was obtained when the sample with the proportion2.5of GO. The results indicated that degradation rate MX process conformed to the rule of Langmuir-Hinshelwood kinetics which followed the pseudo-first order reaction. Testing in4recycle experiments, the degradation rate of MX did not change significantly; indicating the excellent stability and reusability.The photocatalyst could kill all of K. pneumoniae, S. aureus B. pyocyaneus and E. coli in30min with its concentration0.2gL-1.
引文
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