碘化褐煤、硫酸掺杂聚苯胺纤维、紫茎泽兰活性炭对产价铬离子的吸附研究
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摘要
水是一种最重要和最基本的自然资源,不仅是人类赖以生存的根本,而且是社会和经济持续发展的关键。我国不仅面临着水资源短缺的问题,而且水体的污染也越来越引起人们的关注和重视。铬是重要的工业原料,在生产中得到广泛的应用,而且在众多的领域没有替代的材料。铬的大量使用以及不合理的排放,造成了地表水和地下水的污染。
通常处理含铬废水的方法有化学沉淀法,电化学法,离子交换法,膜分离法,生物法以及吸附法等,各种方法各有优缺点。吸附法广泛的被用于工业废水的处理。吸附过程操作简单,吸附剂可再生重复使用。需找廉价,吸附能力好的吸附剂用于污水处理已成为国内外研究的热点。考虑到云南省褐煤储量丰富,而磺化煤很早就用作离子交换剂用于硬水的软化,本文用云南先锋褐煤制备磺化煤吸附剂。紫茎泽兰是在云南省大量存在的一种外侵植物。紫茎泽兰生长的地方其他植物不会生长,而且紫茎泽兰传播速度很快。控制紫茎泽兰传播已成为难点,紫茎泽兰本身还有较高的木质素,从变废为宝,变害为宝的思想出发,本文用紫茎泽兰制备活性炭材料。聚苯胺以其良好的热稳定性、化学稳定性和电化学可逆性,优良的电磁微波吸收性能,潜在的溶液和熔融加工性能,原料易得,合成方法简便,还有独特的掺杂现象等特性,成为现在研究进展最快的导电高分子材料之一。国内外将聚苯胺用于重金属废水处理的研究较少,本文以快速混合的制备方法制备了硫酸掺杂聚苯胺纤维。
本文以含六价铬离子模拟废水为研究对象,研究先锋磺化褐煤、硫酸掺杂聚苯胺纤维和紫茎泽兰活性炭三种吸附材料对水中六价铬离子的去除作用,探讨三种吸附剂对重金属离子的吸附机理。对硫酸掺杂聚苯胺纤维和紫茎泽兰活性炭吸附剂的比表面积、表面形态结构等进行了测定和分析。制备的紫茎泽兰活性炭比表面积为1184.2m2·g-1,分析认为用紫茎泽兰制备活性炭从原料到制备方法是可行的。硫酸掺杂聚苯胺纤维具有较大的比表面积(203.7m2.g-1)、较好的机械性能和较高的热学稳定性能。
研究了先锋磺化褐煤、硫酸掺杂聚苯胺纤维和紫茎泽兰活性炭对六价铬离子吸附性能。研究包括等温吸附研究,吸附剂用量、pH值、时间、温度因素对吸附的影响。探讨了吸附剂的吸附机理,研究了六价铬离子的吸附热力学和动力学行为。结果表明：
先锋磺化褐煤吸附Cr(Ⅵ),吸附时间1小时即可达到吸附平衡。在pH为2左右时,先锋磺化煤对Cr(Ⅵ)的去除效果较好。在pH较小时,可能涉及六价铬的还原。吸附过程中,ΔG=-4.43～-5.71kJ·mol-1,ΔH=14.16kJ·mol-1,ΔS=63.42J·K-1mol-1,说明先锋磺化煤吸附水中Cr(Ⅵ)为自发、吸热、熵增过程。Elovich方程能更好地描述Cr(Ⅵ)在先锋磺化煤上的吸附动力学行为,吸附平衡数据符合Langmuir方程,高温有利于吸附。
硫酸掺杂聚苯胺纤维吸附Cr(Ⅵ),吸附时间1.5h即可达到吸附平衡。在pH小于3时,硫酸掺杂聚苯胺纤维对Cr(Ⅵ)的去除效果较好,去除率达到99%。对于给定的实验条件下4g·L-1的硫酸掺杂聚苯胺纤维是适宜的。吸附过程中,ΔG=-10.76kJ·mol-1～-13.13kJ·mol-1, Δ:23.87kJ·mol-1,ΔS=118.20J·K-1.mol-1,说明硫酸掺杂聚苯胺纤维吸附水中Cr(Ⅵ)为自发、吸热、熵增过程。准二级方程能更好地描述Cr(Ⅵ)在硫酸掺杂聚苯胺纤维上的吸附动力学行为,吸附平衡数据符合Langmuir方程,高温有利于吸附。颗粒内扩散方程研究表明,Cr(Ⅵ)在硫酸掺杂聚苯胺纤维上的吸附不仅仅内扩散是速率控制过程,可能还有其它类型自发进行的动力学控制过程。
紫茎泽兰活性炭对水中Cr(Ⅵ)的最大吸附量为36.22mmg·g-1,吸附时间40min即可达到吸附平衡。在pH为2左右时,紫茎泽兰活性炭对Cr(Ⅵ)的去除效果较好。吸附过程中,△G=-0.76kJ.mol-1～-2.91kJ·mol-1,ΔH=15.02kJ·mol-1,ΔS=53.85J.K-·mol-1,说明紫茎泽兰活性炭吸附水中Cr(Ⅵ)为自发、吸热、熵增过程。准二级方程能更好地描述Cr(Ⅵ)在紫茎泽兰活性炭上的吸附动力学行为,吸附平衡数据符合Langmuir方程,高温有利于吸附。颗粒内扩散方程研究表明,六价铬在紫茎泽兰活性炭上的吸附前期由颗粒内扩散控制,后期由颗粒内扩散控制与膜扩散共同控制。
Water is one of the most important and basic natural resources. It is not only a fundament of human survival, but also is a key of social and economic sustainable development. China is not only facing the problem of water shortage, water pollution, and more and more cause for concern and attention. Chromium is an important industrial raw material in the production; there is no alternative in many areas of the material. Chromium emissions from extensive use and unreasonable emissions, resulting in surface water and groundwater pollution.
Usually chromium-containing wastewater treatment methods are chemical precipitation, electrochemical method, ion exchange, membrane separation, biological and adsorption; various methods have advantages and disadvantages. Adsorption is widely used in the treatment of industrial wastewater emissions. Adsorption process is simple, repeated use of renewable sorbent. Finding cheap, good adsorption capacity of adsorbent for wastewater treatment has become a hot research at home and abroad. Lignite reserves is very rich in Yunnan Province, and sulphonated coal have been used as ion exchanger for softening hard water long time ago, here sulfonation lignite derived from Yunnan Xianfeng lignite was prepared and investigated. Eupatorium is a kind of weed where it grows no other plant can grow. It spreads fastly and difficulty to control in China. Activated carbon derived from Eupatorium was prepared in this research. With good thermal stability, chemical stability and electrochemical reversibility, polyaniline show good microwave absorption properties of the electromagnetic potential solution and melt processing performance, easy to obtain and simple synthesis method etc. Due to the unique phenomenon of polyaniline doping characteristics, it is now the hottest conductive polymer material. Polyaniline at home and abroad for heavy metal removal from wastewater treatment was less reported, here the sulfuric acid doped polyaniline was prepared by rapid mixing method.
In this research, hexavalent chromium ion in wastewater was selected as the research object, sulfonated lignite, polyaniline doped with sulfuric acid and activated carbon derived from Eupatorium were used as the sorbent to remove hexavalent chromium ions in water and its adsorption mechanism were studied. The surface area and surface morphology of sulfuric acid doped polyaniline fibers and activated carbon derived from Eupatorium adsorbent were measured and analyzed. The results show that the surface area of activated carbon derived from Eupatorium is1184.19m2·g-1and the preparation method is feasible. Polyaniline doped with sulfuric acid has a large surface area (203.7m2·g-1), good mechanical properties and high thermal stability.
The properties of sulfuric acid doped polyaniline fibers and activated carbon derived from Eupatorium in removal of hexavalent chromium ion from wastewater were studied in batch studies, including the adsorption isotherms, adsorbent dosage, pH, adsorption time and temperature. The mechanism, thermodynamics and dynamics of the hexavalent chromium ion adsorption were also studied, the results showed that:The adsorption behavavior of Cr (VI) onto the sulfonated lignite show that the time reached adsorption equilibrium is1hour. When the pH is around2, the highest removal efficiency was obtained, maybe involving the reduction of hexavalent chromium in the low pH. Thermodynamic parameters for the adsorption system were determinated, ΔG=-4.43kJ·mol-1to-5.71kJ·mol-1,ΔH=14.16kJ·mol-1, ΔS=63.42J·K-1·mol-1. The positive values of both AH and AS suggest the adsorption process is an endothermic reaction with increasing in randomness at the solid-liquid interface. AG values obtained were negative, indicated that the adsorption of Cr (VI) ion on the sulphonated lignite was a spontaneous adsorption process. The kinetics process can be described by Elovich equation. The adsorption equilibrium data are consistent with Langmuir equation. Adsorption process can be promoted at higher temperature.
The adsorption behavavior of Cr (VI) onto the polyaniline fibers doped with sulfuric acid show that adsorption time is1.5hours to reach the equilibrium. In less than3in the pH, the highest removal efficiency was obtained.4g·L-1of adsorbent is enough for the quantitative removal of Cr (VI) ions for the given experimental conditions. Thermodynamic parameters for the adsorption system is AG=-10.76kJ·mol-1to-13.13kJ·mol-1, ΔH=23.87kJ·mol-1, AS=118.20J·K-1mol-1, which shows the adsorption of Cr (VI) ion on the sulfuric acid doped polyaniline is a spontaneous, endothermic, entropy process. Pseudo second equation can describe the adsorption of Cr (VI) in sulfuric acid doped polyaniline fibers, the adsorption equilibrium data are consistent with Langmuir equation, and adsorption process can be promoted at higher temperature. The results of using intraparticle diffusion equation show that the rate of diffusion is not only the control process; there may be other types of spontaneous dynamic control process.
The Cr (Ⅵ) maximum adsorption capacity of eupatorium activated carbon is36.22mg·g-1Adsorption time is40minutes to reach that equilibrium. When the pH is around2, the highest removal efficiency was obtained. Thermodynamics parameters for the adsorption system is ΔG=-0.76kJ·mol-1to-2.91kJ·mol-1, AH=15.02kJ·mol-1, ΔS=53.85J·K-1·mol-1, which shows the adsorption of the Cr (Ⅵ) ion on Eupatorium activated carbon is spontaneous, endothermic Pseudo second equation can describe the Cr (Ⅵ) adsorption on the eupatorium activated carbon in dynamic behavior. The adsorption equilibrium data are consistent with Langmuir equation. Adsorption process can be promoted at higher temperature. The results of using intraparticle diffusion equation show that the adsorption of the Cr (Ⅵ) ion on Eupatorium activated carbon is controled by diffusion of particles in the early, and late is controled by diffusion of particles and film diffusion.
通常处理含铬废水的方法有化学沉淀法,电化学法,离子交换法,膜分离法,生物法以及吸附法等,各种方法各有优缺点。吸附法广泛的被用于工业废水的处理。吸附过程操作简单,吸附剂可再生重复使用。需找廉价,吸附能力好的吸附剂用于污水处理已成为国内外研究的热点。考虑到云南省褐煤储量丰富,而磺化煤很早就用作离子交换剂用于硬水的软化,本文用云南先锋褐煤制备磺化煤吸附剂。紫茎泽兰是在云南省大量存在的一种外侵植物。紫茎泽兰生长的地方其他植物不会生长,而且紫茎泽兰传播速度很快。控制紫茎泽兰传播已成为难点,紫茎泽兰本身还有较高的木质素,从变废为宝,变害为宝的思想出发,本文用紫茎泽兰制备活性炭材料。聚苯胺以其良好的热稳定性、化学稳定性和电化学可逆性,优良的电磁微波吸收性能,潜在的溶液和熔融加工性能,原料易得,合成方法简便,还有独特的掺杂现象等特性,成为现在研究进展最快的导电高分子材料之一。国内外将聚苯胺用于重金属废水处理的研究较少,本文以快速混合的制备方法制备了硫酸掺杂聚苯胺纤维。
本文以含六价铬离子模拟废水为研究对象,研究先锋磺化褐煤、硫酸掺杂聚苯胺纤维和紫茎泽兰活性炭三种吸附材料对水中六价铬离子的去除作用,探讨三种吸附剂对重金属离子的吸附机理。对硫酸掺杂聚苯胺纤维和紫茎泽兰活性炭吸附剂的比表面积、表面形态结构等进行了测定和分析。制备的紫茎泽兰活性炭比表面积为1184.2m2·g-1,分析认为用紫茎泽兰制备活性炭从原料到制备方法是可行的。硫酸掺杂聚苯胺纤维具有较大的比表面积(203.7m2.g-1)、较好的机械性能和较高的热学稳定性能。
研究了先锋磺化褐煤、硫酸掺杂聚苯胺纤维和紫茎泽兰活性炭对六价铬离子吸附性能。研究包括等温吸附研究,吸附剂用量、pH值、时间、温度因素对吸附的影响。探讨了吸附剂的吸附机理,研究了六价铬离子的吸附热力学和动力学行为。结果表明：
先锋磺化褐煤吸附Cr(Ⅵ),吸附时间1小时即可达到吸附平衡。在pH为2左右时,先锋磺化煤对Cr(Ⅵ)的去除效果较好。在pH较小时,可能涉及六价铬的还原。吸附过程中,ΔG=-4.43～-5.71kJ·mol-1,ΔH=14.16kJ·mol-1,ΔS=63.42J·K-1mol-1,说明先锋磺化煤吸附水中Cr(Ⅵ)为自发、吸热、熵增过程。Elovich方程能更好地描述Cr(Ⅵ)在先锋磺化煤上的吸附动力学行为,吸附平衡数据符合Langmuir方程,高温有利于吸附。
硫酸掺杂聚苯胺纤维吸附Cr(Ⅵ),吸附时间1.5h即可达到吸附平衡。在pH小于3时,硫酸掺杂聚苯胺纤维对Cr(Ⅵ)的去除效果较好,去除率达到99%。对于给定的实验条件下4g·L-1的硫酸掺杂聚苯胺纤维是适宜的。吸附过程中,ΔG=-10.76kJ·mol-1～-13.13kJ·mol-1, Δ:23.87kJ·mol-1,ΔS=118.20J·K-1.mol-1,说明硫酸掺杂聚苯胺纤维吸附水中Cr(Ⅵ)为自发、吸热、熵增过程。准二级方程能更好地描述Cr(Ⅵ)在硫酸掺杂聚苯胺纤维上的吸附动力学行为,吸附平衡数据符合Langmuir方程,高温有利于吸附。颗粒内扩散方程研究表明,Cr(Ⅵ)在硫酸掺杂聚苯胺纤维上的吸附不仅仅内扩散是速率控制过程,可能还有其它类型自发进行的动力学控制过程。
紫茎泽兰活性炭对水中Cr(Ⅵ)的最大吸附量为36.22mmg·g-1,吸附时间40min即可达到吸附平衡。在pH为2左右时,紫茎泽兰活性炭对Cr(Ⅵ)的去除效果较好。吸附过程中,△G=-0.76kJ.mol-1～-2.91kJ·mol-1,ΔH=15.02kJ·mol-1,ΔS=53.85J.K-·mol-1,说明紫茎泽兰活性炭吸附水中Cr(Ⅵ)为自发、吸热、熵增过程。准二级方程能更好地描述Cr(Ⅵ)在紫茎泽兰活性炭上的吸附动力学行为,吸附平衡数据符合Langmuir方程,高温有利于吸附。颗粒内扩散方程研究表明,六价铬在紫茎泽兰活性炭上的吸附前期由颗粒内扩散控制,后期由颗粒内扩散控制与膜扩散共同控制。
Water is one of the most important and basic natural resources. It is not only a fundament of human survival, but also is a key of social and economic sustainable development. China is not only facing the problem of water shortage, water pollution, and more and more cause for concern and attention. Chromium is an important industrial raw material in the production; there is no alternative in many areas of the material. Chromium emissions from extensive use and unreasonable emissions, resulting in surface water and groundwater pollution.
Usually chromium-containing wastewater treatment methods are chemical precipitation, electrochemical method, ion exchange, membrane separation, biological and adsorption; various methods have advantages and disadvantages. Adsorption is widely used in the treatment of industrial wastewater emissions. Adsorption process is simple, repeated use of renewable sorbent. Finding cheap, good adsorption capacity of adsorbent for wastewater treatment has become a hot research at home and abroad. Lignite reserves is very rich in Yunnan Province, and sulphonated coal have been used as ion exchanger for softening hard water long time ago, here sulfonation lignite derived from Yunnan Xianfeng lignite was prepared and investigated. Eupatorium is a kind of weed where it grows no other plant can grow. It spreads fastly and difficulty to control in China. Activated carbon derived from Eupatorium was prepared in this research. With good thermal stability, chemical stability and electrochemical reversibility, polyaniline show good microwave absorption properties of the electromagnetic potential solution and melt processing performance, easy to obtain and simple synthesis method etc. Due to the unique phenomenon of polyaniline doping characteristics, it is now the hottest conductive polymer material. Polyaniline at home and abroad for heavy metal removal from wastewater treatment was less reported, here the sulfuric acid doped polyaniline was prepared by rapid mixing method.
In this research, hexavalent chromium ion in wastewater was selected as the research object, sulfonated lignite, polyaniline doped with sulfuric acid and activated carbon derived from Eupatorium were used as the sorbent to remove hexavalent chromium ions in water and its adsorption mechanism were studied. The surface area and surface morphology of sulfuric acid doped polyaniline fibers and activated carbon derived from Eupatorium adsorbent were measured and analyzed. The results show that the surface area of activated carbon derived from Eupatorium is1184.19m2·g-1and the preparation method is feasible. Polyaniline doped with sulfuric acid has a large surface area (203.7m2·g-1), good mechanical properties and high thermal stability.
The properties of sulfuric acid doped polyaniline fibers and activated carbon derived from Eupatorium in removal of hexavalent chromium ion from wastewater were studied in batch studies, including the adsorption isotherms, adsorbent dosage, pH, adsorption time and temperature. The mechanism, thermodynamics and dynamics of the hexavalent chromium ion adsorption were also studied, the results showed that:The adsorption behavavior of Cr (VI) onto the sulfonated lignite show that the time reached adsorption equilibrium is1hour. When the pH is around2, the highest removal efficiency was obtained, maybe involving the reduction of hexavalent chromium in the low pH. Thermodynamic parameters for the adsorption system were determinated, ΔG=-4.43kJ·mol-1to-5.71kJ·mol-1,ΔH=14.16kJ·mol-1, ΔS=63.42J·K-1·mol-1. The positive values of both AH and AS suggest the adsorption process is an endothermic reaction with increasing in randomness at the solid-liquid interface. AG values obtained were negative, indicated that the adsorption of Cr (VI) ion on the sulphonated lignite was a spontaneous adsorption process. The kinetics process can be described by Elovich equation. The adsorption equilibrium data are consistent with Langmuir equation. Adsorption process can be promoted at higher temperature.
The adsorption behavavior of Cr (VI) onto the polyaniline fibers doped with sulfuric acid show that adsorption time is1.5hours to reach the equilibrium. In less than3in the pH, the highest removal efficiency was obtained.4g·L-1of adsorbent is enough for the quantitative removal of Cr (VI) ions for the given experimental conditions. Thermodynamic parameters for the adsorption system is AG=-10.76kJ·mol-1to-13.13kJ·mol-1, ΔH=23.87kJ·mol-1, AS=118.20J·K-1mol-1, which shows the adsorption of Cr (VI) ion on the sulfuric acid doped polyaniline is a spontaneous, endothermic, entropy process. Pseudo second equation can describe the adsorption of Cr (VI) in sulfuric acid doped polyaniline fibers, the adsorption equilibrium data are consistent with Langmuir equation, and adsorption process can be promoted at higher temperature. The results of using intraparticle diffusion equation show that the rate of diffusion is not only the control process; there may be other types of spontaneous dynamic control process.
The Cr (Ⅵ) maximum adsorption capacity of eupatorium activated carbon is36.22mg·g-1Adsorption time is40minutes to reach that equilibrium. When the pH is around2, the highest removal efficiency was obtained. Thermodynamics parameters for the adsorption system is ΔG=-0.76kJ·mol-1to-2.91kJ·mol-1, AH=15.02kJ·mol-1, ΔS=53.85J·K-1·mol-1, which shows the adsorption of the Cr (Ⅵ) ion on Eupatorium activated carbon is spontaneous, endothermic Pseudo second equation can describe the Cr (Ⅵ) adsorption on the eupatorium activated carbon in dynamic behavior. The adsorption equilibrium data are consistent with Langmuir equation. Adsorption process can be promoted at higher temperature. The results of using intraparticle diffusion equation show that the adsorption of the Cr (Ⅵ) ion on Eupatorium activated carbon is controled by diffusion of particles in the early, and late is controled by diffusion of particles and film diffusion.
引文
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