水质参数对功能化石墨烯在水中凝聚行为的影响

夏鹏; 张为波; 巢铸; 郭飞; 李忠玉; 白英臣

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中国环境科学 ›› 2022, Vol. 42 ›› Issue (10) : 4631-4638.

水污染与控制

水质参数对功能化石墨烯在水中凝聚行为的影响

夏鹏^1,2, 张为波³, 巢铸², 郭飞², 李忠玉¹, 白英臣^1,2

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Influence of water quality parameters on the aggregation behaviors of functionalized graphene in aquatic system

XIA Peng^1,2, ZHANG Wei-bo³, CHAO Zhu², GUO Fei², LI Zhong-yu¹, BAI Ying-chen^1,2

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摘要

采用动态光散射技术研究了不同价态阳离子、富里酸（FA）等对两种功能化石墨烯（FG）悬浮凝聚行为的影响机制.结果表明：FG分别在含不同浓度Na⁺、Ca²⁺和La³⁺的电解质溶液中，其临界聚集浓度（CCC）值范围为221~263，3~4，0.05~0.07mmol/L，符合经典的DLVO理论与Schulze-Hardy法则.5种FA亚组分均可显著抑制FG在水体中的凝聚，加入5mg/L的FA亚组分后，在不同浓度的Ca²⁺和La³⁺的电解质溶液中，FG-OH （FG-COOH）的CCC值分别增大12.5%~37.5%（3.2%~4.5%）和4.2%~25.7%（10%~46%）.FG的CCC值与FA亚组分的C、H含量和H/C比显著正相关（P<0.05），与O含量、O/C比和羧基C含量显著负相关（P<0.05）.差分荧光光谱研究表明随着FG的加入，FA的荧光强度逐渐降低，二者发生相互作用.

Abstract

The influence mechanisms of cations with different valences and fulvic acid (FA) on aggregation behaviours of two functionalized graphene (FG) were investigated by dynamic light scattering technique. The critical coagulation concentration (CCC) values of FG in electrolyte solutions containing Na⁺, Ca²⁺ and La³⁺ ranged from 221~263, 3~4 and 0.05~0.07mmol/L respectively, which were consistent with DLVO theory and Schulze-Hardy rule. The five FA sub-fractions can significantly inhibit the aggregation of FG in water. After adding 5mg/L FA sub-fractions, the CCC values of FG-OH (FG-COOH) increased 12.5%~37.5% (3.2%~4.5%) and 4.2%~25.7% (10%~46%), respectively in electrolyte solutions containing Ca²⁺ and La³⁺. The CCC values of FG were positively significantly correlated with the C content, H content and H/C ratio (P<0.05), and negatively significantly correlated with the O content, O/C ratio and carboxylic C of FA sub-fractions (P<0.05). The fluorescence intensity of FA gradually decreased with the addition of FG indicating the interactions between FG and FA.

导出引用

夏鹏, 张为波, 巢铸, 郭飞, 李忠玉, 白英臣. 水质参数对功能化石墨烯在水中凝聚行为的影响[J]. 中国环境科学. 2022, 42(10): 4631-4638

XIA Peng, ZHANG Wei-bo, CHAO Zhu, GUO Fei, LI Zhong-yu, BAI Ying-chen. Influence of water quality parameters on the aggregation behaviors of functionalized graphene in aquatic system[J]. China Environmental Science. 2022, 42(10): 4631-4638

中图分类号： X131.2

参考文献

[1] Yang Q Q, Li X G, Chen G C, et al.Effect of humic acid on the sulfamethazine adsorption by functionalized multi-walled carbon nanotubes in aqueous solution:mechanistic study[J].Rsc.Advances, 2016,6(18):84-91.
[2] Wang Y L, Lei C, Lin D H.Environmental behaviors and biological effects of engineered nanomaterials:important roles of interfacial interactions and dissolved organic matter[J].Chinese Journal of Chemistry, 2021,39(2):32-42.
[3] 方华,孙宇心,于江华,等.腐殖酸对水中多壁碳纳米管凝聚特性的影响[J].中国环境科学, 2015,35(5):1410-1415.Fang H, Sun Y X, Yu J H, et al.Influence of humic acid on the aggregation of multi-walled carbon nanotubes (MWNTs) in aquatic systems[J].China Environmental Science, 2015,35(5):1410-1415.
[4] Zhao J, Wang Z Y, Jason C W, et al.Graphene in the aquatic environment:adsorption, dispersion, toxicity and transformation[J].Environmental Science & Technology, 2014,48(17):9995-10009.
[5] 蒋丹烈,胡霞林,王锐,等.离子对氧化铁纳米颗粒水中聚集作用的影响[J].中国环境科学, 2014,34(10):2545-2550.Jiang D L, Hu X L, Wang R, et al.Influence of ions on the aggregation behavior of hematite nanoparticle in aqueous system[J].China Environmental Science, 2014,34(10):2545-2550.
[6] Forney M, Anderson J, Ameen A, et al.Aggregation kinetics of single-walled carbon nanotubes in nonaqueous solvents:critical coagulation concentrations and transient dispersion stability[J].The Journal of Physical Chemistry C, 2011,115(47):67-72.
[7] 毛翰,董蕙,Ghosh Saikat,等.pH值、离子强度和粒径对氧化石墨烯稳定性的影响[J].环境化学, 2019,38(10):2300-2305.Mao H, Dong H, Ghosh Saikat, et al.The effects of pH, ionic strength and particle size on the stability of graphene oxide[J].Environmental Chemistry, 2019,38(10):2300-2305.
[8] Chen M, Wang D J, Xu X Y, et al.Biochar nanoparticles with different pyrolysis temperatures mediate cadmium transport in water-saturated soils:effects of ionic strength and humic acid[J].Science of The Total Environment, 2022,806:150668.
[9] Cheng H J, Yang T, Ma J, et al.The aggregation kinetics of manganese oxides nanoparticles in Al (III) electrolyte solutions:roles of distinct Al (III) species and natural organic matters[J].Science of The Total Environment, 2020,744:8-14.
[10] Chowdhury I, Duch M C, Mansukhani N D, et al.Colloidal properties and stability of graphene oxide nanomaterials in the aquatic environment[J].Environmental Science & Technology, 2013,47(12):88-96.
[11] Li T T, Song F H, Zhang J, et al.Experimental and modeling study of proton and copper binding properties onto fulvic acid fractions using spectroscopic techniques combined with two-dimensional correlation analysis[J].Environmental Pollution, 2020,256:113465.
[12] Kim J Y, Kim K T, Lee B, et al.Developmental toxicity of Japanese medaka embryos by silver nanoparticles and released ions in the presence of humic acid[J].Ecotoxicology and Environmental Safety, 2013,92:57-63.
[13] Ali J, Li Y, Wang X J, et al.Climate-zone-dependent effect mechanism of humic acid and fulvic acid extracted from river sediments on aggregation behavior of graphene oxide[J].Science of The Total Environment, 2020,721:137682.
[14] Hyung H, Kim J.Natural organic matter (NOM) adsorption to multi-walled carbon nanotubes:effect of NOM characteristics and water quality parameters[J].Environmental Science & Technology, 2008,42(12):4416-4421.
[15] Hyung H, Fortner J D, Hughes J B.et al.Natural organic matter stabilizes carbon nanotubes in the aqueous phase[J].Environmental Science & Technology, 2007,41(1):179-184.
[16] Song F H, Wu F C, Feng W Y, et al.Fluorescence regional integration and differential fluorescence spectroscopy for analysis of structural characteristics and proton binding properties of fulvic acid sub-fractions[J].Journal of Environmental Sciences, 2018,74:16-25.
[17] 宋凡浩,吴丰昌,冯伟莹,等.差分吸收光谱-高斯拟合法研究富里酸质子化[J].中国环境科学, 2017,37(12):4571-4577.Song F H, Wu F C, Feng W Y, et al.Study on protonation of fulvic acid using differential absorption spectroscopy coupled with Gaussian fitting method[J].China Environmental Science, 2017,37(12):4571-4577.
[18] 简正军,徐健.基于三维荧光光谱的鄱阳湖湿地水体有色可溶性有机物组成特征和来源[J].环境科学学报, 2022,42(2):213-223.Jian Z J, Xu J.Composition characteristics and source of chromophoric dissolved organic matter in Poyang Lake wetland based on three-dimensional fluorescence excitation-emission matrix spectroscopy[J].Acta Scientiae Circumstantiae, 2022,42(2):213-223.
[19] Song F H, Wu F C, Guo F, et al.Interactions between stepwise-eluted sub-fractions of fulvic acids and protons revealed by fluorescence titration combined with EEM-PARAFAC[J].Science of The Total Environment, 2017,605:58-65.
[20] Zhu B Q, Ryan D K.Characterizing the interaction between uranyl ion and fulvic acid using regional integration analysis (RIA) and fluorescence quenching[J].Journal of Environmental Radioactivity, 2016,153:97-103.
[21] Bai Y C, Wu F C, Xing B S, et al.Isolation and characterization of Chinese standard fulvic acid sub-fractions separated from forest soil by stepwise elution with pyrophosphate buffer[J].Scientific Reports, 2015,5(1):1-8.
[22] 施国兰.土壤有机质分级提取及其与氨基甲酸酯类农药相互作用的研究[D].南昌:南昌大学, 2012.Shi G L.Study on isolation of organic matter subfractions obtained from soil and interaction with carbamate pesticides[D].Nanchang:Nanchang University, 2012.
[23] Mohona T M, Gupta A, Masud A, et al.Aggregation behavior of inorganic 2D nanomaterials beyond graphene:insights from molecular modeling and modified DLVO theory[J].Environmental Science & Technology, 2019,53(8):61-72.
[24] Gao Q, Wu F, Hu J, et al.Chemical composition-dependent removal of cationic surfactants by carbon nanotubes[J].Science of the Total Environment, 2020,716:137017.
[25] Aich N, Boateng L K, Sabaraya I V, et al.Aggregation kinetics of higher-order fullerene clusters in aquatic systems[J].Environmental Science & Technology, 2016,50(7):62-71.
[26] Wang L X, Yang X Z, Wang Q, et al.Effects of ionic strength and temperature on the aggregation and deposition of multi-walled carbon nanotubes[J].Journal of Environmental Sciences, 2017,51(1):48-55.
[27] Kennedy A J, Hull M S, Steevens J A, et al.Factors influencing the partitioning and toxicity of nanotubes in the aquatic environment[J].Environmental Toxicology and Chemistry, 2008,27(9):1932-1941.
[28] Sun B B, Zhang Y Q, Chen W, et al.Concentration dependent effects of bovine serum albumin on graphene oxide colloidal stability in aquatic environment[J].Environmental Science & Technology, 2018,52(13):2-9.
[29] Lin D H, Liu N, Yang K, et al.The effect of ionic strength and pH on the stability of tannic acid-facilitated carbon nanotube suspensions[J].Carbon, 2009,47(12):75-82.
[30] Yang K J, Chen B L, Zhu X Y, et al.Aggregation, adsorption, and morphological transformation of graphene oxide in aqueous solutions containing different metal cations[J].Environmental Science & Technology, 2016,50(20):66-75.
[31] Saleh N B, Pfefferle L D, Elimelech M.Aggregation kinetics of multiwalled carbon nanotubes in aquatic systems:measurements and environmental implications[J].Environmental Science & Technology, 2008,42(21):3-9.
[32] Chowdhury I, Mansukhani N D, Guiney L M, et al.Aggregation and stability of reduced graphene oxide:complex roles of divalent cations, pH, and natural organic matter[J].Environmental Science & Technology, 2015,49(18):86-93.
[33] Bai Y C, Wu F C, Lin D H, et al.Aqueous stabilization of carbon nanotubes:effects of surface oxidization and solution chemistry[J].Environmental Science and Pollution Research, 2014,21(6):58-65.
[34] Lee B M, Seo Y S, Hur J.Investigation of adsorptive fractionation of humic acid on graphene oxide using fluorescence EEM-PARAFAC[J].Water Research, 2015,73:42-51.