腐殖酸对改性聚乙烯亚胺去除水中Cu(Ⅱ)的影响
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摘要
采用二硫化碳和氢氧化钠对聚乙烯亚胺进行改性,制备出一种新型高分子絮凝剂聚乙烯亚胺基黄原酸钠(PEX).以含Cu(Ⅱ)水样为处理对象,研究了腐殖酸(HA)的存在对改性聚乙烯亚胺(PEX)去除水样中Cu(Ⅱ)性能的影响,探讨了HA共存时PEX除Cu(Ⅱ)机理.结果表明,HA的存在对PEX去除Cu(Ⅱ)表现出一定的抑制作用,Cu(Ⅱ)去除率随着体系中共存HA浓度的增大而降低,随着PEX投加量的增加而升高,随着pH值的升高而升高;当PEX投加量增加到100 mg·L~(-1)以上或体系pH值升高到6.0时,可消除HA的抑制影响,Cu(Ⅱ)的最高去除率均可达到100%.絮体的Zeta电位随着共存HA浓度的增加而升高,PEX除Cu(Ⅱ)的絮凝作用机理以吸附架桥为主;PEX高分子链上的二硫代羧基与Cu(Ⅱ)发生了螯合沉淀反应,PEX对共存体系中Cu(Ⅱ)和HA均具有一定的去除效果.
A novel macromolecule flocculant, called polyethyleneimine-sodium xanthogenate(PEX), was prepared by modifying polyethyleneimine with carbon disulfide and sodium hydroxide, and it was applied in the treatment of water sample containing Cu(Ⅱ) ions. The effect of HA on the removal performance of Cu(Ⅱ) with PEX was studied, and the mechanism that Cu(Ⅱ) was removed by PEX with the coexistence of HA was also investigated. The results showed that the coexistence of HA would inhibit the removal of Cu(Ⅱ). The removal efficiency of Cu(Ⅱ) by PEX decreased with the increase of HA concentration, and increased with the increase of the dosage of PEX or the initial pH in the mixed system. However, the inhibiting effect of HA could be eliminated when the dosage of PEX was more than 100 mg·L~(-1) or the initial pH was 6.0, and reaching the highest removal rate of Cu(Ⅱ) at 100%. The zeta potential of floc increased with the increase of HA concentration, and the flocculation mechanism for the removal of Cu(Ⅱ) by PEX was mainly reflected in the adsorption bridging action. Moreover, the reaction of chelation precipitation existed between dithiocarboxylic acid groups of PEX and Cu(Ⅱ). In addition, Cu(Ⅱ) and HA could be removed simultaneously by PEX in the coexistence system.
A novel macromolecule flocculant, called polyethyleneimine-sodium xanthogenate(PEX), was prepared by modifying polyethyleneimine with carbon disulfide and sodium hydroxide, and it was applied in the treatment of water sample containing Cu(Ⅱ) ions. The effect of HA on the removal performance of Cu(Ⅱ) with PEX was studied, and the mechanism that Cu(Ⅱ) was removed by PEX with the coexistence of HA was also investigated. The results showed that the coexistence of HA would inhibit the removal of Cu(Ⅱ). The removal efficiency of Cu(Ⅱ) by PEX decreased with the increase of HA concentration, and increased with the increase of the dosage of PEX or the initial pH in the mixed system. However, the inhibiting effect of HA could be eliminated when the dosage of PEX was more than 100 mg·L~(-1) or the initial pH was 6.0, and reaching the highest removal rate of Cu(Ⅱ) at 100%. The zeta potential of floc increased with the increase of HA concentration, and the flocculation mechanism for the removal of Cu(Ⅱ) by PEX was mainly reflected in the adsorption bridging action. Moreover, the reaction of chelation precipitation existed between dithiocarboxylic acid groups of PEX and Cu(Ⅱ). In addition, Cu(Ⅱ) and HA could be removed simultaneously by PEX in the coexistence system.
引文
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Maghsoodloo S, Noroozi B, Haghi A K, et al. 2011. Consequence of chitosan treating on the adsorption of humic acid by granular activated carbon [J]. Journal of Hazardous Materials,191(1/3):380-387
Manzak A, Kur?un C, Y?ld?z Y. 2017. Characterization of humic acid extracted from aqueous solutions with polymer inclusion membranes [J]. Journal of the Taiwan Institute of Chemical Engineers,81:14-20
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谢彬彬,廖建波,胡芸,等.2017.腐殖酸对巯基功能化离子印迹聚合物吸附Cd2+的增效作用[J].环境化学,36(6):1213-1225
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杨虎城,龚继来,曾光明.2017.掺杂聚乙烯醇的壳聚糖小球对铜离子-腐殖酸的单一和连续吸附行为[J].环境科学学报,37(10):3735-3745
Yang S, Li L Y, Pei Z G, et al. 2014. Effects of humic acid on copper adsorption onto few-layer reduced graphene oxide and few-layer graphene oxide [J]. Carbon,75:227-235
袁斌,吕松,张卫红.2010.紫外分光光度法测定水中微量腐殖酸的研究[J].工业水处理,30(4):75-77
Zhou H B, Meng H B, Zhao L X, et al. 2018. Effect of biochar and humic acid on the copper, lead, and cadmium passivation during composting [J]. Bioresource Technology,258:279-286
Zhou P, Yan H, Gu B H. 2005. Competitive complexation of metal ions with humic substances[J]. Chemosphere,58(10):1327-1337
周霞萍.2007.腐植酸应用中的化学基础[M].北京:化学工业出版社.49-51
Bilal M, Shah J A, Ashfaq T, et al. 2013. Waste biomass adsorbents for copper removal from industrial wastewater—A review [J]. Journal of Hazardous Materials, 263: 322-333
常青.2015.絮凝学研究的新领域—具有重金属捕集功能的高分子絮凝剂[J].环境科学学报,35(1):1-11
Chang Q, Zhang M, Wang J X. 2009. Removal of Cu2+ and turbidity from wastewater by mercaptoacetyl chitosan [J]. Journal of Hazardous Materials,169(1/3):621-625
丁文川,田秀美,王定勇,等.2012.腐殖酸对生物炭去除水中Cr(Ⅵ)的影响机制研究[J].环境科学,33(11):3847-3853
顾时国,延克军,谭啸.2015.响应曲面优化MIEX去除水中腐殖酸的工艺研究[J].离子交换与吸附,31(5):401-409
ková M, Kalina M. 2015. Diffusivity of Cu(II) ions in humic gels-influence of reactive functional groups of humic acids [J]. Colloids and Surfaces A: Physicochemical and Engineering Aspects,483:162-170
Li Y, Yue Q Y, Gao B Y. 2010. Adsorption kinetics and desorption of Cu(II) and Zn(II) from aqueous solution onto humic acid [J]. Journal of Hazardous Materials,178(1/3):455-461
Liu L H, Wu J, Ling Y L, et al. 2014. Synthesis of a novel amphoteric chelating polymer flocculant and its performance in Cu2+ removal [J]. Journal of Applied Polymer Science,127(3):2082-2094
龙良俊,王里奥,余纯丽,等.2017.改性污泥腐殖酸的表征及其对Cu2+的吸附特性[J].中国环境科学,37(3):1016-1023
卢涌泉,邓振华.1989.实用红外光谱解析[M].北京:电子工业出版社.176-178
Maghsoodloo S, Noroozi B, Haghi A K, et al. 2011. Consequence of chitosan treating on the adsorption of humic acid by granular activated carbon [J]. Journal of Hazardous Materials,191(1/3):380-387
Manzak A, Kur?un C, Y?ld?z Y. 2017. Characterization of humic acid extracted from aqueous solutions with polymer inclusion membranes [J]. Journal of the Taiwan Institute of Chemical Engineers,81:14-20
邱阳.2015.含铜废水处理法的研究进展[J].污染防治技术,28(3):22-24
Wang G, Chang Q, Han X T, et al. 2013. Removal of Cr(VI) from aqueous solution by flocculant with the capacity of reduction and chelation [J]. Journal of Hazardous Materials,248-249:115-121
王刚,王志科,常青,等.2017.改性聚乙烯亚胺捕集和回收水中的Cu2+[J].环境科学研究,30(6):953-959
Whitby H, van den Berg C M G. 2015. Evidence for copper-binding humic substances in seawater [J]. Marine Chemistry,173:282-290
谢彬彬,廖建波,胡芸,等.2017.腐殖酸对巯基功能化离子印迹聚合物吸附Cd2+的增效作用[J].环境化学,36(6):1213-1225
谢发之,谢志勇,李国莲,等.2017.腐植酸对氧化锌吸附Cu(II)的影响[J].中国环境科学,37(8):2970-2977
熊英禹,付忠田,黄戊生.2014.化学沉淀法处理模拟含铜废水的研究[J].环境保护科学,40(2):35-38
杨虎城,龚继来,曾光明.2017.掺杂聚乙烯醇的壳聚糖小球对铜离子-腐殖酸的单一和连续吸附行为[J].环境科学学报,37(10):3735-3745
Yang S, Li L Y, Pei Z G, et al. 2014. Effects of humic acid on copper adsorption onto few-layer reduced graphene oxide and few-layer graphene oxide [J]. Carbon,75:227-235
袁斌,吕松,张卫红.2010.紫外分光光度法测定水中微量腐殖酸的研究[J].工业水处理,30(4):75-77
Zhou H B, Meng H B, Zhao L X, et al. 2018. Effect of biochar and humic acid on the copper, lead, and cadmium passivation during composting [J]. Bioresource Technology,258:279-286
Zhou P, Yan H, Gu B H. 2005. Competitive complexation of metal ions with humic substances[J]. Chemosphere,58(10):1327-1337
周霞萍.2007.腐植酸应用中的化学基础[M].北京:化学工业出版社.49-51