Fe(II)、Fe(III)对砷与不同分子量腐植酸络合性能的影响

姚淑华, 雍玉玲, 李士凤, 王海博, 吕洪涛, 石中亮

中国环境科学 ›› 2022, Vol. 42 ›› Issue (10) : 4650-4657.

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中国环境科学 ›› 2022, Vol. 42 ›› Issue (10) : 4650-4657.
水污染与控制

Fe(II)、Fe(III)对砷与不同分子量腐植酸络合性能的影响

  • 姚淑华1, 雍玉玲1, 李士凤1, 王海博1, 吕洪涛2, 石中亮1
作者信息 +

Effect of Fe(II)/Fe(III) on complexation properties of arsenic and humic acid with different molecular weights

  • YAO Shu-hua1, YONG Yu-ling1, LI Shi-feng1, WANG Hai-bo1, LV Hong-tao2, SHI Zhong-liang1
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摘要

以腐植酸(HA)代表天然有机质,采用平衡透析和超滤的方法研究铁离子(Fe (II)、Fe (III))对不同分子量HA与砷离子(As (V)、As (III))络合作用的影响,并利用红外光谱(FT-IR)表征其络合特征.结果发现,Fe (II)和Fe (III)均能增强HA络合As能力,且对As (V)络合能力的增强作用大于As (III);pH值显著影响HA络合As能力;溶解性有机碳(DOC)浓度由5mg/L增大到200mg/L,As络合百分比随之增加,此时HA-Fe (III)络合As (III)百分比最大,为24.55%;初始As浓度由10μg/L增加1000μg/L,As络合百分比随之降低,其中HA-Fe (III)络合As (III)百分比最低,为3.11%.相同环境条件下,分子量>100kDa络合As百分比最大,其中HA-Fe (II)络合As (III)的百分比最高为26.43%;分子量小于10kDa的HA络合As百分比明显高于其他分子量的HA.Fe的增强作用主要源于Fe与羧基形成桥梁再与As络合形成三元络合物.

Abstract

Humic acid (HA) was used to represent natural organic matter, and the effects of Iron ions (Fe(II)/Fe(III)) on the complexation of HA with arsenic (As(V)/As(III)) of different molecular weights were investigated by equilibrium dialysis and ultrafiltration, and the complexation characteristics were characterized by infrared spectroscopy (FT-IR). Both Fe(II) and Fe(III) enhanced the As complexation ability of HA, and the enhancement effect on As(V) complexation ability was greater than that of As(III); pH significantly affected the As complexation ability of HA; the percentage of As complexation increased with the increase of dissolved organic carbon (DOC) concentration of HA from 50 to 200mg/L, and the percentage of HA-Fe(III) complexation was the maximum at 24.55%. Increasing the initial As concentration from 10μg/L to 1000μg/L, the percentage of As complexation decreased, with the minimum As(III) complexation percentage by HA-Fe(III) at 3.11%. Under the same environmental conditions, the percentage of As complexed with molecular weight more than 100kDa was the highest, and the percentage of As(III) complexed at HA-Fe(II) was 26.43%; The percentage of As complexed at HA with molecular weight less than 10kDa was significantly higher than that at other molecular weights. The enhancement of Fe was mainly due to the formation of a bridge between Fe and carboxyl groups of HA and then complexation with As to form a ternary complex.

关键词

分子量 / 腐植酸 / 络合 / / 铁离子

Key words

arsenic / complexation / humic acid / iron ion / molecular weight

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姚淑华, 雍玉玲, 李士凤, 王海博, 吕洪涛, 石中亮. Fe(II)、Fe(III)对砷与不同分子量腐植酸络合性能的影响[J]. 中国环境科学. 2022, 42(10): 4650-4657
YAO Shu-hua, YONG Yu-ling, LI Shi-feng, WANG Hai-bo, LV Hong-tao, SHI Zhong-liang. Effect of Fe(II)/Fe(III) on complexation properties of arsenic and humic acid with different molecular weights[J]. China Environmental Science. 2022, 42(10): 4650-4657
中图分类号: X703.5   

参考文献

[1] Wang C, Jiang H.Real-time monitoring of sediment bulking through a multi-anode sediment microbial fuel cell as reliable biosensor[J].Science of the Total Environment, 2019,697:134009.
[2] Chen S C, Sun G X, Yan Y, et al.The great oxidation event expanded the genetic repertoire of arsenic metabolism and cycling[J].Proceedings of the National Academy of Sciences, 2020,117(19):10414-10421.
[3] Sharma P, Ofner J, Kappler A.Formation of binary and ternary colloids and dissolved complexes of organic matter, Fe and As[J].Environmental Science and Technology, 2010,44(12):4479-4485.
[4] Ehlert K, Mikutta C, Kretzschmar R.Impact of birnessite on arsenic and iron speciation during microbial reduction of arsenic-bearing ferrihydrite[J].Environmental Science and Technology, 2014,48(19):11320-11329.
[5] 吴丰昌,王立英,黎文,等.天然有机质及其在地表环境中的重要性[J].湖泊科学, 2008,20(1):12.Wu F C, Wang L Y, Li W, el al.Natural organic matter and its importance in the surface environment[J].Lake Science, 2008,20(1):12.
[6] Liu X, Zhang W, Hu Y, et al.Extraction and detection of organoarsenic feed additives and common arsenic species in environmental matrices by HPLC-ICP-MS[J].Microchemical Journal, 2013,108:38-45.
[7] Jackson B P, Seaman J C, Bertsch P M.Fate of arsenic compounds in poultry litter upon land application[J].Chemosphere, 2006,65(11):2028-2034.
[8] 易层,严玉鹏,王小明,等.天然有机质和金属离子在矿物表面的共吸附[J].农业环境科学学报, 2018,37(8):1574-1583.Yi C, Yan Y P, Wang X M, el al.Co-sorption of natural organic matter and metal ions on minerals[J].Journal of Agro-Environment Science, 2018,37(8):1574-1583.
[9] Pfeiffer M, Batbayar G, Hofmann J, et al.Investigating arsenic (As) occurrence and sources in ground, surface, waste and drinking water in northern Mongolia[J].Environmental Earth Sciences, 2015,73(2):649-662.
[10] Catrouillet C, Davranche M, Dia A, et al.Does As(III) interact with Fe(II), Fe(III) and organic matter through ternary complexes[J].Journal of Colloid and Interface Science, 2016,470:153-161.
[11] Hoffmann M, Mikutta C, Kretzschmar R.Arsenite binding to natural organic matter:spectroscopic evidence for ligand exchange and ternary complex formation[J].Environmental Science & Technology, 2013,47(21):12165-12173.
[12] Catrouillet C, Davranche M, Dia A, et al.Thiol groups controls on arsenite binding by organic matter:New experimental and modeling evidence[J].Journal of Colloid and Interface Science, 2015,460:310-320.
[13] Shaw P J, Jones R I, Haan H D.The influence of humic substances on the molecular weight distributions of phosphate and iron in epilimnetic lake waters[J].Freshwater Biology, 2010,45(4):393.
[14] Gao Z, Guéguen C.Size distribution of absorbing and fluorescing DOM in beaufort sea, Canada Basin[J].Deep Sea Research Part I Oceanographic Research Papers, 2016,121:30-37.
[15] Chen T C, Hseu Z Y, Jean J S, et al.Association between arsenic and different-sized dissolved organic matter in the groundwater of black-foot disease area, Taiwan[J].Chemosphere, 2016,159:214-220.
[16] Bauer M, Blodau C.Arsenic distribution in the dissolved, colloidal and particulate size fraction of experimental solutions rich in dissolved organic matter and ferric iron[J].Geochimica et Cosmochimica Acta, 2009,73(3):529-542.
[17] 李士凤,周杨,姚淑华,等.腐植酸中不同分子量组分与As(Ⅲ)的络合性能[J].中国环境科学, 2020,40(10):4395-4401.Li S F, Zhou Y, Yao S H, et al.Complex properties of different molecular weight components in humic acid and As(Ⅲ)[J].China Environmental Science, 2020,40(10):4395-4401.
[18] Zhang F, Li X, Duan L, et al.Effect of different DOM components on arsenate complexation in natural water[J].Environmental Pollution, 2021,270:116221.
[19] Li X, Guo H, Zheng H, et al.Roles of different molecular weights of dissolved organic matter in arsenic enrichment in groundwater:Evidences from ultrafiltration and EEM-PARAFAC[J].Applied Geochemistry, 2019,104:124-134.
[20] Liu G, Fernandez A, Cai Y.Complexation of arsenite with humic acid in the presence of ferric Iron[J].Environmental Science and Technology, 2011,45(8):3210-3216.
[21] Gontijo E S J, Watanabe C H, Monteiro A S C, et al.Effects of Fe(III) and quality of humic substances on As(V) distribution in freshwater:use of ultrafiltration and kohonen neural network[J].Chemosphere, 2017,188:208-217.
[22] Jackson A, Gaffney J W, Boult S, et al.Subsurface interactions of Fe(II) with humic acid or landfill leachate do not control subsequent iron(III) (hydr)oxide production at the surface[J].Environmental Science and Technology, 2012,46(14):7543-7550.
[23] Liao P, Li W, Jiang Y, et al.Formation, aggregation, and deposition dynamics of NOM-iron colloids at anoxic-oxic interfaces[J].Environmental Science and Technology, 2017,51(21):12235-12245.
[24] Ren J, Fan W, Wang X, et al.Influences of size-fractionated humic acids on arsenite and arsenate complexation and toxicity to Daphnia magna[J].Water Res., 2017,108:68-77.
[25] Buschmann J, Sigg L.Antimony(III) binding to humic substances:influence of pH and type of humic acid[J].Environmental Science and Technology, 2004,38(17):4535-4541.
[26] 周述琼,章骅,但德忠.水中总有机碳测定方法研究进展[J].四川环境, 2006,25(2):111-115.Zhou S Q, Zhang H, Dan D Z.Progress on methods for determination of TOC in water[J].Sichuan Environment, 2006,25(2):111-115.
[27] Johanna B, Alexandra K, Ursula L, et al.Arsenite and arsenate binding to dissolved humic acids:  Influence of pH, type of humic acid, and aluminum[J].Environmental Science and Technology, 2006,40(19):6015-6020.
[28] Bauer M, Blodau C.Arsenic distribution in the dissolved, colloidal and particulate size fraction of experimental solutions rich in dissolved organic matter and ferric iron[J].Geochimica et Cosmochimica Acta, 2009,73(3):529-542.
[29] Mona Z, Zeeshan A, Javaid A, et al.Extraction and characterization of humic acid from Pakistani lignite coals[Z].Energy Sources, Part A:Recovery, Utilization, and Environmental Effects, 2017.
[30] Dick D P, Mangrich A S, Menezes S M C, et al.Chemical and spectroscopical characterization of humic acids from two south brazilian coals of different ranks[J].Journal of the Brazilian Chemical Society, 2002,13(2):177-182.
[31] Guardado I, Urrutia O, Garcia-Mina J M.Some Structural and electronic features of the interaction of phosphate with metal−humic complexes[J].Journal of Agricultural and Food Chemistry, 2008, 56(3):1035-1042.
[32] Rao P, Mak M S H, Liu T, et al.Effects of humic acid on arsenic(V) removal by zero-valent iron from groundwater with special references to corrosion products analyses[J].Chemosphere, 2009,75(2):156-162.

基金

辽宁省高等学校创新团队项目(LT2020016);辽宁省教育厅科学研究项目(LQ2020027,LQ2020023,LJ2020008)

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