天然沸石和粉煤灰的改性及在城市景观水体脱氮除磷中的应用研究
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摘要
城市景观水体具有封闭、纳污能力低,水质改变快等特点,极易发生富营养化。本论文针对富营养化的城市景观水体水质特征考察了天然沸石和粉煤灰的改性方法及其改性后的脱氮、除磷效果,所得结果及结论为:
天然沸石由于孔道堵塞和带电等原因,其脱氮能力受到限制,需要使用一定的改性方法充分挖掘其潜在的脱氮能力。采用NaCl、AlCl_3、MgCl_2、HCI、煅烧等改性方法改性沸石后,沸石的吸附容量均有了一定的提高,其中用NaCl改性的效果最好;选用1mol/L的NaCl溶液,在固液比1:5的情况下改性30min的沸石具有较好的脱氮性能;改性沸石处理低浓度氨氮废水时选用60-100目粒径的沸石、在pH在6-8之间、搅拌强度G值为126.2s~(-1)、搅拌25min时可达到较好的脱氨效果;改性沸石吸附氨氮的反应可以用Langmuir等温吸附方程式描述,拟合系数为0.9937,其氨氮吸附容量为2.42mg/g。改性沸石滤床的试验表明,在不改变水箱水pH值和温度的条件下,滤速对氨氮的去除率影响不大,当滤速在8m/h以下时,氨氮去除率均大于94%。在8m/h的流速进行模拟城市景观水处理且进水氨氮浓度在5.25-0.51mg/L变化时,沸石滤床对氨氮的去除率很高,最高去除率达95.6%,氨氮的浓度可降到0.23mg/L。
未经改性的粉煤灰去除水中的磷酸盐主要依靠粉煤灰中的CaO水解,因此必须在极高的pH值下才能有很好的去除效果,在实际的应用中受到很大限制,出水的pH值也因过高无法达标,为了进一步提高粉煤灰除磷的能力及解决出水的pH值过高的问题,必须对粉煤灰进行改性。采用硫酸改性后,粉煤灰具备了很好的除磷能力。用0.5mol/L的硫酸,在固液比1:4条件下干燥的粉煤灰具有良好的除磷性能;改性灰比原灰有更快的吸附速率,5min之内可基本达到磷吸附平衡;pH对磷吸附效果有很大影响,在pH值分别为6～7和12左右时改性灰有最好的吸附效果,但除磷的机理不同;原灰和改性灰的磷吸附反应均符合Langmuir方程,相关系数分别达到0.997和0.998。最大吸附容量分别达到14.88mg/g和9.34mg/g。改性灰的最大吸附容量虽在数值上有所下降,但其除磷机理却更有实际运用意义。模拟水体试验中,pH在6-7之间、搅拌强度G值为49.7s~(-1)、搅拌5min的条件下,当灰水比分别为1/1500、1/4500和1/10000时,磷浓度分别为1 mg/L、0.2mg/L和0.04mg/L的模拟城市景观水体出水磷浓度都下降到了富营养化的发生浓度0.02mg/L左右,而当灰水比分别提高到1/1000、1/4000和1/8000时,三种水体的出水磷浓度均无法检出。处理极低磷浓度的水体时,如果灰水比过低,出水磷浓度反而略微上升,因此在实际应用中应该避免这种情况的出现。实际景观水体实验中,不同富营养化程度的两种城市景观水体按1/4000的灰水比投加改性粉煤灰处理后,出水TP都降到了0.02mg/L的水平,DP则都为0.0101mg/L,而且当灰水比提高到1/2000时都可将TP降至0.01mg/L的水平。出水pH都呈中性,对COD也有很好的去除效果,两种水体的COD去除率分别达到88.81%和66.37%。实验结果表明,改性粉煤灰在控制城市景观水体的富营养化方面有很好的应用前景。
粉煤灰由于本身不具有类似沸石的结构,无法与氨氮发生离子交换吸附,因此未经过活化的粉煤灰几乎没有脱氮能力,需要使用一定的方法改性后才能具备脱氮能力。采用硫酸和氢氧化钠复合改性后,粉煤灰具备了较强的脱氮能力。硫酸改性的粉煤灰用3mol/L的NaOH溶液,在固液比1:4条件下回流反应1h即可具有较好的脱氮性能;用改性灰处理低浓度氨氮废水时,pH在6-8之间、搅拌强度G值为49.7s~(-1)、搅拌15min即可达到较好的脱氨效果;改性粉煤灰的脱氮过程可以用Langmuir等温吸附方程式描述,拟合系数为0.9924。其氨氮吸附容量达到26.18mg/g。改性粉煤灰滤床的试验表明,在不改变水箱水pH值和温度的条件下,滤速对氨氮的去除率影响不大,当过滤速度小于或等于8m/h时的脱氮效果较好,氨氮去除率大于97%。当选取8m/h的流速进行模拟城市景观水处理且进水氨氮浓度在5.25～0.32 mg/L变化时,改性粉煤灰滤床对氨氮的去除率很高,最高去除率达97.7%,氨氮的浓度可降到0.12mg/L。结果表明改性灰的脱氮效果要好于改性沸石。
The urban landscape water which is closed,of low-pollutant carrying capacity and rapid changes in water quality characteristics will be prone to eutrophication.This paper researched the modified method of natural zeolite and fly ash and the removal effect of ammonia nitrogen and phosphorus using modified zeolite and modified fly ash from the urban landscape eutrophication water.The result and conclusions were shown as follows:
It is difficult for ammonia nitrogen removal to use natural zeolite because of the structure and other reasons.In order to exploit its potential capacity fully it need modifying.After using NaCl,AlCl_3,MgCl_2,HCl,calcining and other modification methods to modified the zeolite,the absorption capacity of the zeolite was improved, and the study also showed that among all modification methods the effect of NaCl was the best.The experiment was carried out under the condition that the concentration of NaCl was 1mol/L,the ratio of solid to liquid was 1:5 in the case of the modified 30 min, which showed that the zeolite had a good performance of ammonia nitrogen removal; under the experimental condition that the size of zeolite was 60～100 mesh,pH was 6～8 and the G was 126.2s~(-1)and stirring time was 25 min,the good efficiency of ammonia nitrogen removal was achieved.This study also showed that the adsorption reaction of ammonia nitrogen by modified zeolite could be described through Langmuir formula with R~2 of 0.9937,and on this condition the absorption capacity of ammonia nitrogen is 2.42 mg/g.The experiments of modified zeolite filter beds showed that the filtration rate plays a trivial role in the removal rate of ammonia nitrogen without changing the pH and temperature of the raw water,and when the filtration rate below 8m/h,the removal rate of ammonia nitrogen is more than 94%.When the experiment to treating the simulate urban landscape water was carried out with the filtration rate of 8m/h and the concentration of ammonia nitrogen changing between 5.25～0.51mg/L, the removal rate of ammonia nitrogen by zeolite filter bed is high,and the highest removal rate was up to 95.6%,then the concentration of ammonia nitrogen could be reduced to 0.23mg/L.
The fly ash remove phosphate from water rely mainly on the CaO hydrolysis,it is necessary of high pH to getting a good effect.So the practical applications is largely limited,and the pH of output water is too high to reach the standards.In order to further enhance the ability of removing phosphorus and solve the problem of high pH of output water,it has to modify,the fly ash.After Modified by sulfuric acid,the fly ash has a very.good capacity of phosphorus removal.under the condition that the concentration of sulfuric acid was 0.5mol/L and the ratio of solid to liquid was 1:4,the modified fly ash has a good performance to remove phosphorus.The experiment showed that the modified fly ash has much faster absorption rate than the fly ash,.and it takes less than 5 min to reach P-adsorption-Balance;pH plays an important role on the absorption of phosphorus,when the pH was 6～7 and about 12 respectively,the modified fly ash has the best absorption effect,but the mechanism of phosphorus removal is different from each other.The P-adsorption reaction of the fly ash and the modified fly ash are both follow with Langmuir equation with the R~2 of 0.997 and 0.998 respectively,and the greatest absorption capacity reached 14.88mg/g and 9.34mg/g respectively.The biggest absorption capacity of modified fly ash decline,but its mechanism of phosphorus removal has much more significance of practical application.When the ratio of ash to water was 1/500,1/4500 and 1/10000 respectively,and the phosphorus concentration of simulated urban landscape water was 1mg/L,0.2mg/L and 0.04mg/L respectively,the phosphorus concentration of output water dropped to about 0.02mg/L under the condition that the pH was 6～7,the G was 49.7s~(-1)and stirring time was 5 min.while the ratio of ash to water up to 1/1000,1/4000 and 1/8000 respectively,the concentrations of phosphorus of the three output water can not be detected,if the ratio of ash to water was too low,the phosphorus concentration of output water rise slightly When dealing with the water of very low phosphorus concentration,so we should avoid such a situation in practical application.After treating by adding modified fly ash with the ratio of ash to water at 1/4000,TP of both the two urban landscape water dropped to 0.02mg/L,and DP dropped to 0.0101mg/L;when the ratio of ash to water was enhanced to 1/2000,TP reduced to 0.01mg/L.The pH of effluent water all was neutral,and the COD also had a good removal effect,COD removal ratio were up to 88.81%and 66.37%respectively.Experimental results showed that the modified fly ash has a very good prospect in the eutrophication-control of the urban landscape water.
The fly ash almost has no capacity of exchanging adsorption with ammonia nitrogen since lacking the structure of zeolite,After using H_2SO_4 and NaOH to modify the fly ash,the absorption capacity of the fly ash had great increase,The experiment was carried out under the condition that the concentration of NaOH was 3mol/L,the ratio of solid to liquid was 1:4 in the case of the modified 1h,which showed that the fly ash has a good performance of ammonia nitrogen removal;under the experimental condition that the pH was 6～8 and the G was 49.7 s~(-1)and stirring time was 15 min,the good efficiency of ammonia nitrogen was achieved.This study also showed that the adsorption reaction of ammonia nitrogen by modified fly ash could be described through Langmuir formula with R~2 of 0.9924,and on this condition the absorption capacity of ammonia nitrogen is 26.18mg/g.The experiments of modified fly ash filter beds showed that the filtration rate plays a trivial role in the removal rate of ammonia nitrogen without changing the pH and temperature of the raw water,and when the filtration rate below 8m/h,the removal rate of ammonia nitrogen is more than 97%. When the experiment to treating the simulate urban landscape water was carried out with filtration rate of 8m/h and the concentration of ammonia nitrogen changing between 5.25～0.32 mg/L,the removal rate of ammonia nitrogen by fly ash filter bed is high,and the highest removal rate was up to 97.7%,then the concentration of ammonia nitrogen could be reduced to 0.12 mg/L.
天然沸石由于孔道堵塞和带电等原因,其脱氮能力受到限制,需要使用一定的改性方法充分挖掘其潜在的脱氮能力。采用NaCl、AlCl_3、MgCl_2、HCI、煅烧等改性方法改性沸石后,沸石的吸附容量均有了一定的提高,其中用NaCl改性的效果最好;选用1mol/L的NaCl溶液,在固液比1:5的情况下改性30min的沸石具有较好的脱氮性能;改性沸石处理低浓度氨氮废水时选用60-100目粒径的沸石、在pH在6-8之间、搅拌强度G值为126.2s~(-1)、搅拌25min时可达到较好的脱氨效果;改性沸石吸附氨氮的反应可以用Langmuir等温吸附方程式描述,拟合系数为0.9937,其氨氮吸附容量为2.42mg/g。改性沸石滤床的试验表明,在不改变水箱水pH值和温度的条件下,滤速对氨氮的去除率影响不大,当滤速在8m/h以下时,氨氮去除率均大于94%。在8m/h的流速进行模拟城市景观水处理且进水氨氮浓度在5.25-0.51mg/L变化时,沸石滤床对氨氮的去除率很高,最高去除率达95.6%,氨氮的浓度可降到0.23mg/L。
未经改性的粉煤灰去除水中的磷酸盐主要依靠粉煤灰中的CaO水解,因此必须在极高的pH值下才能有很好的去除效果,在实际的应用中受到很大限制,出水的pH值也因过高无法达标,为了进一步提高粉煤灰除磷的能力及解决出水的pH值过高的问题,必须对粉煤灰进行改性。采用硫酸改性后,粉煤灰具备了很好的除磷能力。用0.5mol/L的硫酸,在固液比1:4条件下干燥的粉煤灰具有良好的除磷性能;改性灰比原灰有更快的吸附速率,5min之内可基本达到磷吸附平衡;pH对磷吸附效果有很大影响,在pH值分别为6～7和12左右时改性灰有最好的吸附效果,但除磷的机理不同;原灰和改性灰的磷吸附反应均符合Langmuir方程,相关系数分别达到0.997和0.998。最大吸附容量分别达到14.88mg/g和9.34mg/g。改性灰的最大吸附容量虽在数值上有所下降,但其除磷机理却更有实际运用意义。模拟水体试验中,pH在6-7之间、搅拌强度G值为49.7s~(-1)、搅拌5min的条件下,当灰水比分别为1/1500、1/4500和1/10000时,磷浓度分别为1 mg/L、0.2mg/L和0.04mg/L的模拟城市景观水体出水磷浓度都下降到了富营养化的发生浓度0.02mg/L左右,而当灰水比分别提高到1/1000、1/4000和1/8000时,三种水体的出水磷浓度均无法检出。处理极低磷浓度的水体时,如果灰水比过低,出水磷浓度反而略微上升,因此在实际应用中应该避免这种情况的出现。实际景观水体实验中,不同富营养化程度的两种城市景观水体按1/4000的灰水比投加改性粉煤灰处理后,出水TP都降到了0.02mg/L的水平,DP则都为0.0101mg/L,而且当灰水比提高到1/2000时都可将TP降至0.01mg/L的水平。出水pH都呈中性,对COD也有很好的去除效果,两种水体的COD去除率分别达到88.81%和66.37%。实验结果表明,改性粉煤灰在控制城市景观水体的富营养化方面有很好的应用前景。
粉煤灰由于本身不具有类似沸石的结构,无法与氨氮发生离子交换吸附,因此未经过活化的粉煤灰几乎没有脱氮能力,需要使用一定的方法改性后才能具备脱氮能力。采用硫酸和氢氧化钠复合改性后,粉煤灰具备了较强的脱氮能力。硫酸改性的粉煤灰用3mol/L的NaOH溶液,在固液比1:4条件下回流反应1h即可具有较好的脱氮性能;用改性灰处理低浓度氨氮废水时,pH在6-8之间、搅拌强度G值为49.7s~(-1)、搅拌15min即可达到较好的脱氨效果;改性粉煤灰的脱氮过程可以用Langmuir等温吸附方程式描述,拟合系数为0.9924。其氨氮吸附容量达到26.18mg/g。改性粉煤灰滤床的试验表明,在不改变水箱水pH值和温度的条件下,滤速对氨氮的去除率影响不大,当过滤速度小于或等于8m/h时的脱氮效果较好,氨氮去除率大于97%。当选取8m/h的流速进行模拟城市景观水处理且进水氨氮浓度在5.25～0.32 mg/L变化时,改性粉煤灰滤床对氨氮的去除率很高,最高去除率达97.7%,氨氮的浓度可降到0.12mg/L。结果表明改性灰的脱氮效果要好于改性沸石。
The urban landscape water which is closed,of low-pollutant carrying capacity and rapid changes in water quality characteristics will be prone to eutrophication.This paper researched the modified method of natural zeolite and fly ash and the removal effect of ammonia nitrogen and phosphorus using modified zeolite and modified fly ash from the urban landscape eutrophication water.The result and conclusions were shown as follows:
It is difficult for ammonia nitrogen removal to use natural zeolite because of the structure and other reasons.In order to exploit its potential capacity fully it need modifying.After using NaCl,AlCl_3,MgCl_2,HCl,calcining and other modification methods to modified the zeolite,the absorption capacity of the zeolite was improved, and the study also showed that among all modification methods the effect of NaCl was the best.The experiment was carried out under the condition that the concentration of NaCl was 1mol/L,the ratio of solid to liquid was 1:5 in the case of the modified 30 min, which showed that the zeolite had a good performance of ammonia nitrogen removal; under the experimental condition that the size of zeolite was 60～100 mesh,pH was 6～8 and the G was 126.2s~(-1)and stirring time was 25 min,the good efficiency of ammonia nitrogen removal was achieved.This study also showed that the adsorption reaction of ammonia nitrogen by modified zeolite could be described through Langmuir formula with R~2 of 0.9937,and on this condition the absorption capacity of ammonia nitrogen is 2.42 mg/g.The experiments of modified zeolite filter beds showed that the filtration rate plays a trivial role in the removal rate of ammonia nitrogen without changing the pH and temperature of the raw water,and when the filtration rate below 8m/h,the removal rate of ammonia nitrogen is more than 94%.When the experiment to treating the simulate urban landscape water was carried out with the filtration rate of 8m/h and the concentration of ammonia nitrogen changing between 5.25～0.51mg/L, the removal rate of ammonia nitrogen by zeolite filter bed is high,and the highest removal rate was up to 95.6%,then the concentration of ammonia nitrogen could be reduced to 0.23mg/L.
The fly ash remove phosphate from water rely mainly on the CaO hydrolysis,it is necessary of high pH to getting a good effect.So the practical applications is largely limited,and the pH of output water is too high to reach the standards.In order to further enhance the ability of removing phosphorus and solve the problem of high pH of output water,it has to modify,the fly ash.After Modified by sulfuric acid,the fly ash has a very.good capacity of phosphorus removal.under the condition that the concentration of sulfuric acid was 0.5mol/L and the ratio of solid to liquid was 1:4,the modified fly ash has a good performance to remove phosphorus.The experiment showed that the modified fly ash has much faster absorption rate than the fly ash,.and it takes less than 5 min to reach P-adsorption-Balance;pH plays an important role on the absorption of phosphorus,when the pH was 6～7 and about 12 respectively,the modified fly ash has the best absorption effect,but the mechanism of phosphorus removal is different from each other.The P-adsorption reaction of the fly ash and the modified fly ash are both follow with Langmuir equation with the R~2 of 0.997 and 0.998 respectively,and the greatest absorption capacity reached 14.88mg/g and 9.34mg/g respectively.The biggest absorption capacity of modified fly ash decline,but its mechanism of phosphorus removal has much more significance of practical application.When the ratio of ash to water was 1/500,1/4500 and 1/10000 respectively,and the phosphorus concentration of simulated urban landscape water was 1mg/L,0.2mg/L and 0.04mg/L respectively,the phosphorus concentration of output water dropped to about 0.02mg/L under the condition that the pH was 6～7,the G was 49.7s~(-1)and stirring time was 5 min.while the ratio of ash to water up to 1/1000,1/4000 and 1/8000 respectively,the concentrations of phosphorus of the three output water can not be detected,if the ratio of ash to water was too low,the phosphorus concentration of output water rise slightly When dealing with the water of very low phosphorus concentration,so we should avoid such a situation in practical application.After treating by adding modified fly ash with the ratio of ash to water at 1/4000,TP of both the two urban landscape water dropped to 0.02mg/L,and DP dropped to 0.0101mg/L;when the ratio of ash to water was enhanced to 1/2000,TP reduced to 0.01mg/L.The pH of effluent water all was neutral,and the COD also had a good removal effect,COD removal ratio were up to 88.81%and 66.37%respectively.Experimental results showed that the modified fly ash has a very good prospect in the eutrophication-control of the urban landscape water.
The fly ash almost has no capacity of exchanging adsorption with ammonia nitrogen since lacking the structure of zeolite,After using H_2SO_4 and NaOH to modify the fly ash,the absorption capacity of the fly ash had great increase,The experiment was carried out under the condition that the concentration of NaOH was 3mol/L,the ratio of solid to liquid was 1:4 in the case of the modified 1h,which showed that the fly ash has a good performance of ammonia nitrogen removal;under the experimental condition that the pH was 6～8 and the G was 49.7 s~(-1)and stirring time was 15 min,the good efficiency of ammonia nitrogen was achieved.This study also showed that the adsorption reaction of ammonia nitrogen by modified fly ash could be described through Langmuir formula with R~2 of 0.9924,and on this condition the absorption capacity of ammonia nitrogen is 26.18mg/g.The experiments of modified fly ash filter beds showed that the filtration rate plays a trivial role in the removal rate of ammonia nitrogen without changing the pH and temperature of the raw water,and when the filtration rate below 8m/h,the removal rate of ammonia nitrogen is more than 97%. When the experiment to treating the simulate urban landscape water was carried out with filtration rate of 8m/h and the concentration of ammonia nitrogen changing between 5.25～0.32 mg/L,the removal rate of ammonia nitrogen by fly ash filter bed is high,and the highest removal rate was up to 97.7%,then the concentration of ammonia nitrogen could be reduced to 0.12 mg/L.
引文
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