改性纳米TiO_2的研究及在光催化处理矿井水中的应用
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摘要
纳米TiO_2光催化技术作为一种高级氧化技术,在污染物降解方面具有降解效率高、无二次污染等优点。但是,纯的纳米TiO_2光催化性能不强,限制了它的应用。为了提高纳米TiO_2的光催化活性,必须对其进行改性。矿井水是一种可重复利用的水资源。将改性纳米TiO_2应用于矿井水处理中,对缓解我国水资源紧张,实现矿区经济可持续发展具有重要意义。
采用溶胶-凝胶技术合成WO_3掺杂改性纳米TiO_2和改性聚乙二醇(PEG)的TiO_2。运用XRD、SEM、XPS、IR、TG-DTA等测试手段,研究了改性二氧化钛的物理化学性质。考察了改性纳米TiO_2对甲基橙的光催化降解情况和动力学:研究了催化剂投加量、溶液初始浓度、反应时间、反应温度、pH对甲基橙降解的影响,优选出最佳掺杂量的改性TiO_2。比较了在光催化和光氧化两种作用下甲基橙降解的动力学。
考察了7种无机离子对改性TiO_2光催化降解矿井水中COD的影响,HCO_3~-、SO_4~(2-)、Cl~-和Ca~(2+),在矿井水中的实际浓度时对两种光催化剂(PEG400-TiO_2和TiO_2)的性能均有抑制作用,抑制作用大小为HCO_3~-＞SO_4~(2-)＞Cl~-＞Ca~(2+);Cl~-在相对低浓度范围时(0.9～8.9mmol/l),对两种光催化剂的性能有促进作用;Mn~(2+)在矿井水中实际浓度时(0.0013mmol/L),对光催化性能没有影响,当Mn~(2+)浓度＞0.013mmol/L就对TiO_2光催化性能有抑制,当Mn~(2+)浓度＞0.039mmol/L才对PEG400-TiO_2光催化性能有抑制。Cu~(2+)在其浓度为0.008～0.072mmol/L对两种光催化剂性能有促进作用,其浓度＞0.072mmol/L对光催化性能有抑制作用;和Mn~(2+)、Cu~(2+)一样Fe~(3+)在矿井水中实际浓度时(0.0457mmol/L),对两种光催化剂没有影响,但在浓度(0.2～0.7mmol/L)对光催化剂的性能均有显著促进作用,但浓度＞0.8 mmol/L对光催化性能有抑制作用。
通过两因子方差分析,各离子浓度均与实际矿井水中离子浓度相近条件下,HCO_3~-和SO_4~(2-),HCO_3~-和Cl~-,SO_4~(2-)和Cl~-对两种光催化剂均降解率均有显著影响;Mn~(2+)和Cu~(2+)对两种光催化剂均降解率均没有显著影响;Mn~(2+)和Ca~(2+),Cu~(2+)和Ca~(2+)中的Ca~(2+)对两种光催化剂的降解率均有显著影响,而Mn~(2+)和Cu~(2+)没有影响。
研究了活性炭负载改性TiO_2处理矿井水的中试试验,针对超标严重的指标,氟化物、浊度、色度、Hg~(2+)、Cr~(6+)、大肠菌群、细菌总数等参数进行5d的试验,结果良好。并对其稳定性和工艺的经济效益进行了初步分析。
As an advanced oxidation technology,the nano-TiO_2 photocatalytic technology can degrade the pollutants effectively without secondary pollution.But the photocatalytic performance of pure nano-TiO_2 is not good, so its application is limited.In order to improve the photocatalytic activity,modification of pure nano-TiO_2 is an effective way.While the mine water is a kind of reusable water,in this way,using the nano-TiO_2 in the treatment of mine water will be significant to alleviate the shortage of water resources and achieve sustainable economic development of the mining areas.
The WO_3 modified and the PEG modified nano-TiO_2 were prepared with the sol-gel technology.Both were characterized or tested with XRD,SEM,XPS, IR,TG-DTA,etc.Research of the degradation of methyl orange caused by the photocatalysis of modified nano-TiO_2.The kinetics of photocatalysis in methyl orange were studied.The influence factors such as the amount of photocatalyst,initial concentration of the solution,reaction time, temperature and the pH on the degradation of methyl orange were also investigated and the optimum amount of WO_3 and PEG were determined.The dynamics of the degradation of methyl orange under photo-oxidation and photo-catalyze was compared.
The influences of 7 kinds of inorganic ions to the activity of the modified TiO_2 on catalyzing and degrading the COD in the water were studied. It is found that HCO_3~-,SO_4~(2-),Cl~-and Ca~(2+) all can restrain the two photocatalysts PEG400-TiO_2 and TiO_2 when they reach the actual concentration in the coal mine water,and the order of their restraining capacities is HCO_3~-＞SO_4~(2-)＞Cl~-＞Ca~(2+).The Cl~- can improve the performances of the two photocatalysts when its concentration is low(0.9～8.9mmol/l); Mn~(2+) has no influence on the photocatalysts when it reaches the actual concentration(0.0013mol/L),while when its concentration is more than 0.013mol/L,it could restrain the photocatalytic performance of TiO_2,and it can restrain the catalytic performance of PEG400-TiO_2 only when its concentration is more than 0.039mmol/L.The Cu~(2+) can improve the performances of the two photocatalysts when its concentration is 0.008～0.072mmol/L,while when its concentration is more than 0.072mol/L,it can restrain the photocatalytic performance;Like Mn~(2+) and Cu~(2+),Fe~(3+) has no influence on the photocatalysts when it reaches the actual concentration (0.0457mmol/L),and it can greatly improve the performances of the two photocatalysts when its concentration is 0.2～0.7mmol/L,but it can restrain the photocatalytic performance when its concentration is more than 0.8mmol/L.
When the concentration of each ion is very close to the one in the actual mine water,it shows that HCO_3~- and SO_4~(2-),HCO_3~- and Cl~-,SO_4~(2-) and Cl~- all have obvious influences on the degradation rate of the two photocatalysts through the two-factor analysis of variance;Both Mn~(2+) and Cu~(2+) have no influence on the degradation rate of the two photocatalysts;When the Mn~(2+) and Ca~(2+) coexist or Cu~(2+) and Ca~(2+) coexists,it is Ca~(2+) that influences the degradation rate of the both photocatalysts.
Experimentation of the activated carbon load modified Ti_2 on the coal mine water has been researched.5d experiment on the serious against standard indicators,such as fluoride,nephelometer,chroma,Hg~(2+),Cr~(6+), coliform bacteria and parameters of the total number of the bacteria has been carried out.The results are satisfying and its stability and the economic benefits are preliminarily analyzed.
采用溶胶-凝胶技术合成WO_3掺杂改性纳米TiO_2和改性聚乙二醇(PEG)的TiO_2。运用XRD、SEM、XPS、IR、TG-DTA等测试手段,研究了改性二氧化钛的物理化学性质。考察了改性纳米TiO_2对甲基橙的光催化降解情况和动力学:研究了催化剂投加量、溶液初始浓度、反应时间、反应温度、pH对甲基橙降解的影响,优选出最佳掺杂量的改性TiO_2。比较了在光催化和光氧化两种作用下甲基橙降解的动力学。
考察了7种无机离子对改性TiO_2光催化降解矿井水中COD的影响,HCO_3~-、SO_4~(2-)、Cl~-和Ca~(2+),在矿井水中的实际浓度时对两种光催化剂(PEG400-TiO_2和TiO_2)的性能均有抑制作用,抑制作用大小为HCO_3~-＞SO_4~(2-)＞Cl~-＞Ca~(2+);Cl~-在相对低浓度范围时(0.9～8.9mmol/l),对两种光催化剂的性能有促进作用;Mn~(2+)在矿井水中实际浓度时(0.0013mmol/L),对光催化性能没有影响,当Mn~(2+)浓度＞0.013mmol/L就对TiO_2光催化性能有抑制,当Mn~(2+)浓度＞0.039mmol/L才对PEG400-TiO_2光催化性能有抑制。Cu~(2+)在其浓度为0.008～0.072mmol/L对两种光催化剂性能有促进作用,其浓度＞0.072mmol/L对光催化性能有抑制作用;和Mn~(2+)、Cu~(2+)一样Fe~(3+)在矿井水中实际浓度时(0.0457mmol/L),对两种光催化剂没有影响,但在浓度(0.2～0.7mmol/L)对光催化剂的性能均有显著促进作用,但浓度＞0.8 mmol/L对光催化性能有抑制作用。
通过两因子方差分析,各离子浓度均与实际矿井水中离子浓度相近条件下,HCO_3~-和SO_4~(2-),HCO_3~-和Cl~-,SO_4~(2-)和Cl~-对两种光催化剂均降解率均有显著影响;Mn~(2+)和Cu~(2+)对两种光催化剂均降解率均没有显著影响;Mn~(2+)和Ca~(2+),Cu~(2+)和Ca~(2+)中的Ca~(2+)对两种光催化剂的降解率均有显著影响,而Mn~(2+)和Cu~(2+)没有影响。
研究了活性炭负载改性TiO_2处理矿井水的中试试验,针对超标严重的指标,氟化物、浊度、色度、Hg~(2+)、Cr~(6+)、大肠菌群、细菌总数等参数进行5d的试验,结果良好。并对其稳定性和工艺的经济效益进行了初步分析。
As an advanced oxidation technology,the nano-TiO_2 photocatalytic technology can degrade the pollutants effectively without secondary pollution.But the photocatalytic performance of pure nano-TiO_2 is not good, so its application is limited.In order to improve the photocatalytic activity,modification of pure nano-TiO_2 is an effective way.While the mine water is a kind of reusable water,in this way,using the nano-TiO_2 in the treatment of mine water will be significant to alleviate the shortage of water resources and achieve sustainable economic development of the mining areas.
The WO_3 modified and the PEG modified nano-TiO_2 were prepared with the sol-gel technology.Both were characterized or tested with XRD,SEM,XPS, IR,TG-DTA,etc.Research of the degradation of methyl orange caused by the photocatalysis of modified nano-TiO_2.The kinetics of photocatalysis in methyl orange were studied.The influence factors such as the amount of photocatalyst,initial concentration of the solution,reaction time, temperature and the pH on the degradation of methyl orange were also investigated and the optimum amount of WO_3 and PEG were determined.The dynamics of the degradation of methyl orange under photo-oxidation and photo-catalyze was compared.
The influences of 7 kinds of inorganic ions to the activity of the modified TiO_2 on catalyzing and degrading the COD in the water were studied. It is found that HCO_3~-,SO_4~(2-),Cl~-and Ca~(2+) all can restrain the two photocatalysts PEG400-TiO_2 and TiO_2 when they reach the actual concentration in the coal mine water,and the order of their restraining capacities is HCO_3~-＞SO_4~(2-)＞Cl~-＞Ca~(2+).The Cl~- can improve the performances of the two photocatalysts when its concentration is low(0.9～8.9mmol/l); Mn~(2+) has no influence on the photocatalysts when it reaches the actual concentration(0.0013mol/L),while when its concentration is more than 0.013mol/L,it could restrain the photocatalytic performance of TiO_2,and it can restrain the catalytic performance of PEG400-TiO_2 only when its concentration is more than 0.039mmol/L.The Cu~(2+) can improve the performances of the two photocatalysts when its concentration is 0.008～0.072mmol/L,while when its concentration is more than 0.072mol/L,it can restrain the photocatalytic performance;Like Mn~(2+) and Cu~(2+),Fe~(3+) has no influence on the photocatalysts when it reaches the actual concentration (0.0457mmol/L),and it can greatly improve the performances of the two photocatalysts when its concentration is 0.2～0.7mmol/L,but it can restrain the photocatalytic performance when its concentration is more than 0.8mmol/L.
When the concentration of each ion is very close to the one in the actual mine water,it shows that HCO_3~- and SO_4~(2-),HCO_3~- and Cl~-,SO_4~(2-) and Cl~- all have obvious influences on the degradation rate of the two photocatalysts through the two-factor analysis of variance;Both Mn~(2+) and Cu~(2+) have no influence on the degradation rate of the two photocatalysts;When the Mn~(2+) and Ca~(2+) coexist or Cu~(2+) and Ca~(2+) coexists,it is Ca~(2+) that influences the degradation rate of the both photocatalysts.
Experimentation of the activated carbon load modified Ti_2 on the coal mine water has been researched.5d experiment on the serious against standard indicators,such as fluoride,nephelometer,chroma,Hg~(2+),Cr~(6+), coliform bacteria and parameters of the total number of the bacteria has been carried out.The results are satisfying and its stability and the economic benefits are preliminarily analyzed.
引文
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