改性茶叶对工业废水的吸附性能研究
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摘要
本文根据茶叶中含有大量的吸附活性中心,如-OH,=NH,>C=C <,>C=O,二氮杂环及多元酚类等,这些基团在适宜条件下与金属离子发生不同反应,即可将金属离子吸附在茶叶上,并且多元酚类物质具有活性羟基,可使多种金属离子沉淀,用甲醛处理后发生酚醛缩合,既提高了物理吸附能力又增强了化学吸附能力,探讨了改性茶叶吸附Fe3+的最佳工艺条件、吸附动力学及吸附热力学等,在最佳工艺条件下,制备了新型吸附剂茶叶质铁,然后考察了茶叶质铁对模拟工业废水(苯酚废水、萘酚废水、活性嫩黄K-6G废水和活性艳红K-2BP废水)的吸附性能、吸附活化能及吸附热力学参数等。主要的实验结果如下：
1、考察改性茶叶吸附Fe3+的吸附性能、热力学及动力学
最佳吸附工艺条件：Fe3+初始浓度大于1.40mol/L时,溶液吸附温度范围为50-60℃,调节溶液pH为0.8-0.9之间；吸附60min基本达到饱和,饱和吸附量可达到863mg/g。改性茶叶吸附Fe3+很好的符合Langmuir等温吸附方程,热力学参数吸附自由能变ΔG<0,吸附焓变ΔH=340.61 J/mol,吸附熵变ΔS=1.18 J/mol·K;改性茶叶吸附水溶液中Fe3+的反应动力学过程均很好地符合准二级吸附速率方程,反应活化能Ea=28.41kJ/mol,活化能较小,表明改性茶叶吸附水溶液中Fe3+是容易进行的吸热过程。
2、考察茶叶质铁对模拟苯酚废水的吸附性能、热力学及动力学
最佳吸附工艺条件：最佳溶液pH为9.0；吸附温度为50℃,在吸附60min吸附量最大,当溶液初始浓度为200mg/L时,吸附都达到了饱和,饱和吸附量为4.78mg/g。茶叶质铁吸附苯酚的过程符合Langmuir等温吸附方程,热力学参数吸附自由能变AG<0,吸附焓变ΔH=38.10kJ/mol,吸附熵变ΔS=0.15kJ/mol·K;茶叶质铁吸附苯酚的吸附动力学反应级数为2,反应活化能Ea=92.04kJ/mol。
3、考察茶叶质铁对模拟萘酚废水的吸附性能、热力学及动力学
最佳吸附工艺条件：最佳溶液pH为11.0；吸附温度为50℃,在吸附120min吸附量最大,当溶液初始浓度为900mg/L时,吸附都达到了饱和,饱和吸附量为21.24mg/g。茶叶质铁吸附苯酚的过程符合Langmuir等温吸附方程,热力学参数吸附自由能变AG<0,吸附焓变ΔH=9.86kJ/mol,吸附熵变ΔS=0.053kJ/mol·K;茶叶质铁吸附萘酚的吸附动力学反应级数为2,反应活化能Ea=35.49kJ/mol。
4、考察茶叶质铁对模拟活性嫩黄K-6G废水的吸附性能、热力学及动力学
最佳吸附工艺条件：最佳溶液pH为0.5；吸附温度为60℃,在吸附11h吸附量最大,当溶液初始浓度为500mg/L时,吸附都达到了饱和,饱和吸附量为23.56mg/g。茶叶质铁吸附活性嫩黄K-6G的过程符合Langmuir等温吸附方程,热力学参数吸附自由能变ΔG<0,吸附焓变ΔH=57.12kJ/mol,吸附熵变ΔS=0.22kJ/mol·K;茶叶质铁吸附活性嫩黄K-6G的吸附动力学反应级数为1,反应活化能Ea=48.91 kJ/mol。
5、考察茶叶质铁对模拟活性艳红K-2BP废水的吸附性能、热力学及动力学
最佳吸附工艺条件：最佳溶液pH为0.8；吸附温度为50℃,在吸附120min吸附量最大,当溶液初始浓度为2000mg/L时,吸附都达到了饱和,饱和吸附量为95.32mg/g。茶叶质铁吸附活性艳红K-2BP的过程符合Langmuir等温吸附方程,热力学参数吸附自由能变ΔG<0,吸附焓变ΔH=16.49kJ/mol,吸附熵变ΔS=0.074KJ/mol·K;茶叶质铁吸附活性艳红K-2BP的吸附动力学反应级数为1,反应活化能Ea=44.13 kJ/mol。
A large number of adsorption active sites were contained on the tea, such as-OH,=NH,> C=C<,> C=O,2-aza-ring and multi-phenols, etc.. These groups reacted with metal ions in appropriate conditions, for example, metal ions could be adsorbed on the tea. Metal ions also could be precipitated because of polyhydric phenol with active hydroxyl. The physical and chemical adsorption capacities were enhanced after treated with phenolic formaldehyde condensation by formaldehyde. The main content was described as follows:adsorption kinetics, adsorption thermodynamics and the adsorption conditions of Fe3+ with modified tea, The new kind of adsorbent of Tea-Fe(Ⅲ) was synthesized under suitable condition. In addtion adsorption capacity, adsorption activation energy and adsorption thermodynamic parameters were studied on industrial wastewater (phenol wastewater naphthol wastewater, Reactive Yellow K-6G wastewater and Reactive Brilliant Red K-2BP wastewater) removal using Tea-Fe(Ⅲ). The main results obtained were as follows:
1. Investigation of modified tea on adsorption capacity, adsorption kinetics and adsorption thermodynamics with Fe3+
The optimal conditions were the initial concention of Fe3+ larger than 1.40 mol/L, the reaction temperature 50-60℃, pH 0.8-0.9; adsorption 60 min reaching to saturation, the saturated adsorption capacity 863mg/g. The adsorption behavior of modified tea with Fe3+ showed a good fit with Langmuir isotherm equation, Thermodynamic parameters of Gibbs free energy(AG) was less than zero. Enthaly of adsorption (AH) value was 340.61J/mol and the entropy (ΔS) value was 1.18 J/mol·K. The dynamic adsorption model of modified tea on Fe3+ ions was well accorded with quasi-second dynamic equation. The activation energy (Ea) was determined to be only 28.74 kJ/mol, indicated that the adsorption is endothermic process.
2. Investigation of adsorption capacity, adsorption kinetics and adsorption thermodynamics of simulated phenol wastewater onto Tea-Fe(Ⅲ)
The optimum conditions of adsorption technology were as follows: pH 9.0, the temperature 50℃, adsorption time 60 min. If the initial concention of phenol wastewater was 200mg/L, the saturated adsorption capacity was 4.78 mg/g on the above conditions. The adsorption behavior of Tea-Fe(Ⅲ) with phenol shows a good fit with Langmuir isotherm equation, Thermodynamic parameters of Gibbs free energy(ΔG) was less than zero. Enthaly of adsorption (ΔH) value was 38.10 kJ/mol and the entropy (ΔS) value was 0.15 kJ/mol·K. The dynamic adsorption model of Tea-Fe(Ⅲ) on phenol was accorded with the character of the second-order reaction, and the activation energy (Ea) was determined to be 92.04 kJ/mol.
3. Investigation of adsorption capacity, adsorption kinetics and adsorption thermodynamics of simulated naphthol wastewater onto Tea-Fe(Ⅲ)
The optimum conditions of adsorption technology were as follows: pH 11.0, the temperature 50℃, adsorption time 120min. If the initial concention of phenol wastewater were 900 mg/L, the saturated adsorption capacity was 21.24 mg/g on the above conditions. The adsorption behavior of Tea-Fe(Ⅲ) with naphthol shows a good fit with Langmuir isotherm equation, Thermodynamic parameters of Gibbs free energy(ΔG) was less than zero. Enthaly of adsorption (ΔH) value was 9.86 kJ/mol and the entropy (ΔS) value was 0.053 kJ/mol·K. The dynamic adsorption model of Tea-Fe(Ⅲ) on naphthol was accorded with the character of the second-order reaction, and the activation energy (Ea) was determined to be 35.49 kJ/mol.
4. Investigation of adsorption capacity, adsorption kinetics and adsorption thermodynamics of simulated Reactive Yellow K-6G wastewater onto Tea-Fe(Ⅲ)
The optimum conditions of adsorption technology were as follows: pH 0.5, the reaction temperature 60℃, adsorption time 11h. If the initial concention of Reactive Yellow K-6G wastewater was 500 mg/L, the saturated adsorption capacity was 23.56 mg/g on the above conditions. The adsorption behavior of Tea-Fe(Ⅲ) with Reactive Yellow K-6G shows a good fit with Langmuir isotherm equation. Thermodynamic parameters of Gibbs free energy(ΔG) was less than zero. Enthaly of adsorption (ΔH) value was 57.12 kJ/mol and the entropy (ΔS) value was 0.22 kJ/mol·K. The dynamic adsorption model of Tea-Fe(Ⅲ) on Reactive Yellow K-6G was accorded with the character of the first-order reaction, and the activation energy (Ea) was determined to be 48.91 kJ/mol.
5. Investigation of adsorption capacity, adsorption kinetics and adsorption thermodynamics of simulated Reactive Brilliant Red K-2BP wastewater onto Tea-Fe(Ⅲ)
The optimum conditions of adsorption technology were as follows: pH 0.8, the reaction temperature 50℃, adsorption time 120 min. If the initial concention of Reactive Brilliant Red K-2BP wastewater 2000mg/L, the saturated adsorption capacity was 95.32 mg/g on the above conditions. The adsorption behavior of Tea-Fe(Ⅲ) with Reactive Brilliant Red K-2BP shows a good fit with Langmuir isotherm equation. Thermodynamic parameters of Gibbs free energy(ΔG) was less than zero. Enthaly of adsorption (ΔH) value was 16.49 kJ/mol and the entropy (ΔS) value was 0.074 kJ/mol·K. The dynamic adsorption model of Tea-Fe(Ⅲ) on Reactive Brilliant Red K-2BP was accorded with the character of the first-order reaction, and the activation energy (Ea) was determined to be 44.13 kJ/mol.
1、考察改性茶叶吸附Fe3+的吸附性能、热力学及动力学
最佳吸附工艺条件：Fe3+初始浓度大于1.40mol/L时,溶液吸附温度范围为50-60℃,调节溶液pH为0.8-0.9之间；吸附60min基本达到饱和,饱和吸附量可达到863mg/g。改性茶叶吸附Fe3+很好的符合Langmuir等温吸附方程,热力学参数吸附自由能变ΔG<0,吸附焓变ΔH=340.61 J/mol,吸附熵变ΔS=1.18 J/mol·K;改性茶叶吸附水溶液中Fe3+的反应动力学过程均很好地符合准二级吸附速率方程,反应活化能Ea=28.41kJ/mol,活化能较小,表明改性茶叶吸附水溶液中Fe3+是容易进行的吸热过程。
2、考察茶叶质铁对模拟苯酚废水的吸附性能、热力学及动力学
最佳吸附工艺条件：最佳溶液pH为9.0；吸附温度为50℃,在吸附60min吸附量最大,当溶液初始浓度为200mg/L时,吸附都达到了饱和,饱和吸附量为4.78mg/g。茶叶质铁吸附苯酚的过程符合Langmuir等温吸附方程,热力学参数吸附自由能变AG<0,吸附焓变ΔH=38.10kJ/mol,吸附熵变ΔS=0.15kJ/mol·K;茶叶质铁吸附苯酚的吸附动力学反应级数为2,反应活化能Ea=92.04kJ/mol。
3、考察茶叶质铁对模拟萘酚废水的吸附性能、热力学及动力学
最佳吸附工艺条件：最佳溶液pH为11.0；吸附温度为50℃,在吸附120min吸附量最大,当溶液初始浓度为900mg/L时,吸附都达到了饱和,饱和吸附量为21.24mg/g。茶叶质铁吸附苯酚的过程符合Langmuir等温吸附方程,热力学参数吸附自由能变AG<0,吸附焓变ΔH=9.86kJ/mol,吸附熵变ΔS=0.053kJ/mol·K;茶叶质铁吸附萘酚的吸附动力学反应级数为2,反应活化能Ea=35.49kJ/mol。
4、考察茶叶质铁对模拟活性嫩黄K-6G废水的吸附性能、热力学及动力学
最佳吸附工艺条件：最佳溶液pH为0.5；吸附温度为60℃,在吸附11h吸附量最大,当溶液初始浓度为500mg/L时,吸附都达到了饱和,饱和吸附量为23.56mg/g。茶叶质铁吸附活性嫩黄K-6G的过程符合Langmuir等温吸附方程,热力学参数吸附自由能变ΔG<0,吸附焓变ΔH=57.12kJ/mol,吸附熵变ΔS=0.22kJ/mol·K;茶叶质铁吸附活性嫩黄K-6G的吸附动力学反应级数为1,反应活化能Ea=48.91 kJ/mol。
5、考察茶叶质铁对模拟活性艳红K-2BP废水的吸附性能、热力学及动力学
最佳吸附工艺条件：最佳溶液pH为0.8；吸附温度为50℃,在吸附120min吸附量最大,当溶液初始浓度为2000mg/L时,吸附都达到了饱和,饱和吸附量为95.32mg/g。茶叶质铁吸附活性艳红K-2BP的过程符合Langmuir等温吸附方程,热力学参数吸附自由能变ΔG<0,吸附焓变ΔH=16.49kJ/mol,吸附熵变ΔS=0.074KJ/mol·K;茶叶质铁吸附活性艳红K-2BP的吸附动力学反应级数为1,反应活化能Ea=44.13 kJ/mol。
A large number of adsorption active sites were contained on the tea, such as-OH,=NH,> C=C<,> C=O,2-aza-ring and multi-phenols, etc.. These groups reacted with metal ions in appropriate conditions, for example, metal ions could be adsorbed on the tea. Metal ions also could be precipitated because of polyhydric phenol with active hydroxyl. The physical and chemical adsorption capacities were enhanced after treated with phenolic formaldehyde condensation by formaldehyde. The main content was described as follows:adsorption kinetics, adsorption thermodynamics and the adsorption conditions of Fe3+ with modified tea, The new kind of adsorbent of Tea-Fe(Ⅲ) was synthesized under suitable condition. In addtion adsorption capacity, adsorption activation energy and adsorption thermodynamic parameters were studied on industrial wastewater (phenol wastewater naphthol wastewater, Reactive Yellow K-6G wastewater and Reactive Brilliant Red K-2BP wastewater) removal using Tea-Fe(Ⅲ). The main results obtained were as follows:
1. Investigation of modified tea on adsorption capacity, adsorption kinetics and adsorption thermodynamics with Fe3+
The optimal conditions were the initial concention of Fe3+ larger than 1.40 mol/L, the reaction temperature 50-60℃, pH 0.8-0.9; adsorption 60 min reaching to saturation, the saturated adsorption capacity 863mg/g. The adsorption behavior of modified tea with Fe3+ showed a good fit with Langmuir isotherm equation, Thermodynamic parameters of Gibbs free energy(AG) was less than zero. Enthaly of adsorption (AH) value was 340.61J/mol and the entropy (ΔS) value was 1.18 J/mol·K. The dynamic adsorption model of modified tea on Fe3+ ions was well accorded with quasi-second dynamic equation. The activation energy (Ea) was determined to be only 28.74 kJ/mol, indicated that the adsorption is endothermic process.
2. Investigation of adsorption capacity, adsorption kinetics and adsorption thermodynamics of simulated phenol wastewater onto Tea-Fe(Ⅲ)
The optimum conditions of adsorption technology were as follows: pH 9.0, the temperature 50℃, adsorption time 60 min. If the initial concention of phenol wastewater was 200mg/L, the saturated adsorption capacity was 4.78 mg/g on the above conditions. The adsorption behavior of Tea-Fe(Ⅲ) with phenol shows a good fit with Langmuir isotherm equation, Thermodynamic parameters of Gibbs free energy(ΔG) was less than zero. Enthaly of adsorption (ΔH) value was 38.10 kJ/mol and the entropy (ΔS) value was 0.15 kJ/mol·K. The dynamic adsorption model of Tea-Fe(Ⅲ) on phenol was accorded with the character of the second-order reaction, and the activation energy (Ea) was determined to be 92.04 kJ/mol.
3. Investigation of adsorption capacity, adsorption kinetics and adsorption thermodynamics of simulated naphthol wastewater onto Tea-Fe(Ⅲ)
The optimum conditions of adsorption technology were as follows: pH 11.0, the temperature 50℃, adsorption time 120min. If the initial concention of phenol wastewater were 900 mg/L, the saturated adsorption capacity was 21.24 mg/g on the above conditions. The adsorption behavior of Tea-Fe(Ⅲ) with naphthol shows a good fit with Langmuir isotherm equation, Thermodynamic parameters of Gibbs free energy(ΔG) was less than zero. Enthaly of adsorption (ΔH) value was 9.86 kJ/mol and the entropy (ΔS) value was 0.053 kJ/mol·K. The dynamic adsorption model of Tea-Fe(Ⅲ) on naphthol was accorded with the character of the second-order reaction, and the activation energy (Ea) was determined to be 35.49 kJ/mol.
4. Investigation of adsorption capacity, adsorption kinetics and adsorption thermodynamics of simulated Reactive Yellow K-6G wastewater onto Tea-Fe(Ⅲ)
The optimum conditions of adsorption technology were as follows: pH 0.5, the reaction temperature 60℃, adsorption time 11h. If the initial concention of Reactive Yellow K-6G wastewater was 500 mg/L, the saturated adsorption capacity was 23.56 mg/g on the above conditions. The adsorption behavior of Tea-Fe(Ⅲ) with Reactive Yellow K-6G shows a good fit with Langmuir isotherm equation. Thermodynamic parameters of Gibbs free energy(ΔG) was less than zero. Enthaly of adsorption (ΔH) value was 57.12 kJ/mol and the entropy (ΔS) value was 0.22 kJ/mol·K. The dynamic adsorption model of Tea-Fe(Ⅲ) on Reactive Yellow K-6G was accorded with the character of the first-order reaction, and the activation energy (Ea) was determined to be 48.91 kJ/mol.
5. Investigation of adsorption capacity, adsorption kinetics and adsorption thermodynamics of simulated Reactive Brilliant Red K-2BP wastewater onto Tea-Fe(Ⅲ)
The optimum conditions of adsorption technology were as follows: pH 0.8, the reaction temperature 50℃, adsorption time 120 min. If the initial concention of Reactive Brilliant Red K-2BP wastewater 2000mg/L, the saturated adsorption capacity was 95.32 mg/g on the above conditions. The adsorption behavior of Tea-Fe(Ⅲ) with Reactive Brilliant Red K-2BP shows a good fit with Langmuir isotherm equation. Thermodynamic parameters of Gibbs free energy(ΔG) was less than zero. Enthaly of adsorption (ΔH) value was 16.49 kJ/mol and the entropy (ΔS) value was 0.074 kJ/mol·K. The dynamic adsorption model of Tea-Fe(Ⅲ) on Reactive Brilliant Red K-2BP was accorded with the character of the first-order reaction, and the activation energy (Ea) was determined to be 44.13 kJ/mol.
引文
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