氧化石墨烯对沉积物中重金属Cu的稳定固化研究
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摘要
以一种新型碳基材料——氧化石墨烯(GO)为吸附剂,以乌梁素海表层沉积物中重金属Cu为研究对象,考察了GO投加量、沉积物pH值、有机质种类及其质量分数在35 d老化时间内对Cu稳定固化效果的影响。实验中利用电位法测定沉积物的pH值和氧化还原电位值(ORP),通过BCR连续提取法分析Cu各形态含量的分布。研究结果表明,随着GO投加量(2%、4%、6%、8%和10%)的增加,GO可以有效地将Cu从不稳定状态转化为稳定状态。在质量分数为10%时,Cu的酸可提取态较原始状态减少3.76%,残渣态增加28.16%。另外在不同pH(6、7、8和9)下,GO对Cu的稳定效果不同,表现出pH=9>pH=8>pH=7>pH=6的递减关系;并且当pH=9时,沉积物的ORP值在整个老化时间内最低。选用腐殖酸(HA)和富里酸(FA)两种有机质研究其对GO稳定沉积物中Cu的影响。结果发现,加入HA和FA后,GO对沉积物中Cu的稳定效果明显提高,且随着HA和FA质量分数(1%、5%、10%和15%)的增加而增加,当质量分数为15%时固定效果最好。GO+15%HA使重金属Cu的残渣态增加了34.95%,GO+15%FA使重金属Cu残渣态增加了32.96%。以上实验数据表明,GO可以有效地将沉积物中Cu从不稳定态转化为稳定合态,降低沉积物中Cu向上覆水释放的风险。该研究围绕乌梁素海上覆水环境开展实验,以期望对高寒地区重金属污染沉积物的修复提供一种新的思路。
In recent years, river sediments had been polluting by heavy metals due to large amounts of industrial wastewater, the migration and bioavailability of heavy metals in sediments adversely affect ecosystem health. In order to reduce the harm of heavy metals to the environment, a new carbon-based material, graphene oxide(GO), was used as an adsorbent to study stable curing of the heavy metal Cu in the surface sediments of Wuliangsuhai. The dosage of GO, pH value of sediment, organic matter type(HA or FA)and percentages were investigated to determine their effects for Stabilization of Cu on 35 days aging period. In the experiment, the pH value and Oxidation reduction potential(ORP) of the sediment were determined using potentiometry. The percentages of acid-soluble, reducible, oxidizable and residual Cu were analyzed by BCR continuous extraction method. The dosage of GO increased from 2% to 10% and unstable Cu was successfully transformed into stable Cu. For example, the percentages of the acid-soluble Cu decreased by 3.76% and the residual Cu increased by 28.16%. Furthermore, the stabilization of Cu varied with pH value, the large pH value is, the more stable Cu can be gained when pH value was 9, the ORP of the sediment was the lowest. Humic acid(HA) and fulvic acid(FA) were chosen to be added with GO, and it is found that the stablization of Cu became better with more HA or FA addition. And when the percentages of HA and FA were both 15%, the residual Cu increased by 34.95% and 32.96%,respectively. The results of this study indicated that GO can effectively transform unstable Cu into stable Cu, and can reduce the risk of Cu in the sediment releasing into surfacing water. The paper presents a new view for the restoration of heavy metal contaminated sediment in alpine regions.
In recent years, river sediments had been polluting by heavy metals due to large amounts of industrial wastewater, the migration and bioavailability of heavy metals in sediments adversely affect ecosystem health. In order to reduce the harm of heavy metals to the environment, a new carbon-based material, graphene oxide(GO), was used as an adsorbent to study stable curing of the heavy metal Cu in the surface sediments of Wuliangsuhai. The dosage of GO, pH value of sediment, organic matter type(HA or FA)and percentages were investigated to determine their effects for Stabilization of Cu on 35 days aging period. In the experiment, the pH value and Oxidation reduction potential(ORP) of the sediment were determined using potentiometry. The percentages of acid-soluble, reducible, oxidizable and residual Cu were analyzed by BCR continuous extraction method. The dosage of GO increased from 2% to 10% and unstable Cu was successfully transformed into stable Cu. For example, the percentages of the acid-soluble Cu decreased by 3.76% and the residual Cu increased by 28.16%. Furthermore, the stabilization of Cu varied with pH value, the large pH value is, the more stable Cu can be gained when pH value was 9, the ORP of the sediment was the lowest. Humic acid(HA) and fulvic acid(FA) were chosen to be added with GO, and it is found that the stablization of Cu became better with more HA or FA addition. And when the percentages of HA and FA were both 15%, the residual Cu increased by 34.95% and 32.96%,respectively. The results of this study indicated that GO can effectively transform unstable Cu into stable Cu, and can reduce the risk of Cu in the sediment releasing into surfacing water. The paper presents a new view for the restoration of heavy metal contaminated sediment in alpine regions.
引文
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TONG X J,LI J Y,YUAN J H,et al.,2011.Adsorption of Cu(II)by biochars generated from three crop straws[J].Chemical Engineering Journal,172(2-3):828-834.
VIJAY B H,YADAVA R G,SIPPY K,2019.Clay based nanocomposites for removal of heavy metals from water:Areview[J].Journal of Environmental Management,232:803-817.
WANG F,ZHANG L,WANG Y,et al.,2017.Fe3O4@Si O2@CS-TETAfunctionalized graphene oxide for the adsorption of methylene blue(MB)and Cu(II)[J].Applied Surface Science,420:970-981.
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WEN J,YI Y J,ZENG G M,2016.Effects of modified zeolite on the removal and stabilization of heavy metals in contaminated lake sediment using BCR sequential extraction[J].Journal of Environmental Management,178:63-69.
XIONG T,YUAN X,WANG H,et al.,2018.Implication of graphene oxide in Cd-contaminated soil:A case study of bacterial communities[J].Journal of Environmental Management,205:99-106.
YIN X Q,JIANG Y J,TAN Y H,et al.,2019.Co-transport of graphene oxide and heavy metal ions in surfacemodified porous media[J].Chemosphere,218:1-13.
DAVIDSON C M,DUNCAN A L,LITTLEJOHN D,et al.,1998.A critical evaluation of the three-stage BCR sequential extraction procedure to assess the potential mobility and toxicity of heavy metals in industrially-contaminated land[J].Analytica Chimica Acta,363:45-55.
XU J,ZHANG Y P,GUTHA Y,et al.,2017.Antibacterial property and biocompatibility of Chitosan/Poly(vinyl alcohol)/ZnO(CS/PVA/ZnO)beads as an efficient adsorbent for Cu(II)removal from aqueous solution[J].Colloids and Surfaces B:Biointerfaces,156:340-348.
ZAHED M,PARSAMEHR P S,TOFIGHY M A,et al.,2018.Synthesis and functionalization of graphene oxide(GO)for salty water desalination as adsorbent[J].Chemical Engineering Research and Design,138:358-365.
ZHA J R,HIANG Y J,XIA W Q,et al.,2018.Effect of mineral reaction between calcium and aluminosilicate on heavy metal behavior during sludge incineration[J].Fuel,229:241-247.
ZHAO G M,YE S Y,YUAN H M,et al.,2018.Surface sediment properties and heavy metal contamination assessment in river sediments of the Pearl River Delta,China[J].Marine Pollution Bulletin,136:300-308.
付绪金,贾克力,史小红,等,2013.乌梁素海沉积物腐殖质的组成及分布特征[J].湖泊科学,25(4):489-496.FU X J,JIA K L,SHI X H,et al.,2013.The humus composition and distribution of Lake Wuliangsuhai sediment[J].Journal of Lake Sciences,25(4):489-496.
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HE Y,MEN B,YANG X F,et a.,2019.Relationship between heavy metals and dissolved organic matter released from sediment by bioturbation/bioirrigation[J].Journal of Environmental Sciences,75:216-223.
HU X J,LIU Y G,WANG H,et al.,2013.Removal of Cu(II)ions from aqueous solution using sulfonated magnetic graphene oxide composite[J].Separation and Purification Technology,108:189-195.
JOHN U,KENNEDY O,ZAGABATHUNI V P,et al.,2010.Removal of Cu(II)and Zn(II)from industrial wastewater by acid-activated montmorillonite-illite type of clay[J].Comptes Rendus Chimie,13:1359-1363.
WEN J,YI Y J,ZENG G M,2016.Effects of modified zeolite on the removal and stabilization of heavy metals in contaminated lake sediment using BCR sequential extraction[J].Journal of Environmental Management,178:63-69.
LU K P,XING Y,GERTY G,et al.,2017.Effect of bamboo and rice straw biochars on the mobility and redistribution of heavy metals(Cd,Cu,Pb and Zn)in contaminated soil[J].Journal of Environmental Management,186:285-292.
LIANG Y Z,DING Y,WANG P,et al.,2019.Molecular characteristics,proton dissociation properties,and metal binding properties of soil organic matter:A theoretical study[J].Science of The Total Environment,656:521-530.
LIU M,CHEN J B,SUN X S,et al.,2019.Accumulation and transformation of heavy metals in surface sediments from the Yangtze River estuary to the East China Sea shelf[J].Environmental Pollution,245:111-121.
MONSER L,NAFA?A,2001.Modified activated carbon for the removal of copper,zinc,chromium and cyanide from wastewater[J].Separation and Purification Technology,26(2-3):137-146.
LU K P,YANG X,GIELEN G,et al.,2017.Effect of bamboo and rice straw biochars on the mobility and redistribution of heavy metals(Cd,Cu,Pb and Zn)in contaminated soil[J].Journal of Environmental Management,186(Part 2):285-292.
PENG J F,SONG Y H,YUAN P,et al.,2009.The remediation of heavy metals contaminated sediment[J].Journal of Hazardous Materials,161(2-3):633-640.
PENG W J,LI H Q,LIU Y Y,et al.,2017.A review on heavy metal ions adsorption from water by graphene oxide and its composites[J].Journal of Molecular Liquids,230:496-504.
QUE W,ZHOU Y H,LIU Y G,et al.,2018.Appraising the effect of in-situ remediation of heavy metal contaminated sediment by biochar and activated carbon on Cu immobilization and microbial community[J].Ecological Engineering,127:519-526.
SHAHEEN S M,TSADILAS C D,RINKLEBE J,2013.A review of the distribution coefficients of trace elements in soils:Influence of sorption system,element characteristics,and soil colloidal properties[J].Advances in Colloid and Interface Science,201-202:43-56.
SIMAIO F A,BLETSA E,DELI G Y,et al.,2017.Functionalized graphene oxides stabilizing Cu ions under ambient O2[J].Materials&Design,116:227-237.
SUN C Y,ZHANG Z X,CAO H N,et al.,2019.Concentrations,speciation,and ecological risk of heavy metals in the sediment of the Songhua River in an urban area with petrochemical industries[J].Chemosphere,219:538-545.
SZKOKAN-EMILSON E J,WATMOUGH S A,GUNN J M,2014.Wetlands as long-term sources of metals to receiving waters in mining-impacted landscapes[J].Environmental Pollution,192:91-103.
TONG X J,LI J Y,YUAN J H,et al.,2011.Adsorption of Cu(II)by biochars generated from three crop straws[J].Chemical Engineering Journal,172(2-3):828-834.
VIJAY B H,YADAVA R G,SIPPY K,2019.Clay based nanocomposites for removal of heavy metals from water:Areview[J].Journal of Environmental Management,232:803-817.
WANG F,ZHANG L,WANG Y,et al.,2017.Fe3O4@Si O2@CS-TETAfunctionalized graphene oxide for the adsorption of methylene blue(MB)and Cu(II)[J].Applied Surface Science,420:970-981.
WANG L,HU D,KONG X,et al.,2018.Anionic polypeptide poly(γ-glutamic acid)-functionalized magnetic Fe3O4-GO-(o-MWCNTs)hybrid nanocomposite for high-efficiency removal of Cd(II),Cu(II)and Ni(II)heavy metal ions[J].Chemical Engineering Journal,346:38-49.
WEN J,YI Y J,ZENG G M,2016.Effects of modified zeolite on the removal and stabilization of heavy metals in contaminated lake sediment using BCR sequential extraction[J].Journal of Environmental Management,178:63-69.
XIONG T,YUAN X,WANG H,et al.,2018.Implication of graphene oxide in Cd-contaminated soil:A case study of bacterial communities[J].Journal of Environmental Management,205:99-106.
YIN X Q,JIANG Y J,TAN Y H,et al.,2019.Co-transport of graphene oxide and heavy metal ions in surfacemodified porous media[J].Chemosphere,218:1-13.
DAVIDSON C M,DUNCAN A L,LITTLEJOHN D,et al.,1998.A critical evaluation of the three-stage BCR sequential extraction procedure to assess the potential mobility and toxicity of heavy metals in industrially-contaminated land[J].Analytica Chimica Acta,363:45-55.
XU J,ZHANG Y P,GUTHA Y,et al.,2017.Antibacterial property and biocompatibility of Chitosan/Poly(vinyl alcohol)/ZnO(CS/PVA/ZnO)beads as an efficient adsorbent for Cu(II)removal from aqueous solution[J].Colloids and Surfaces B:Biointerfaces,156:340-348.
ZAHED M,PARSAMEHR P S,TOFIGHY M A,et al.,2018.Synthesis and functionalization of graphene oxide(GO)for salty water desalination as adsorbent[J].Chemical Engineering Research and Design,138:358-365.
ZHA J R,HIANG Y J,XIA W Q,et al.,2018.Effect of mineral reaction between calcium and aluminosilicate on heavy metal behavior during sludge incineration[J].Fuel,229:241-247.
ZHAO G M,YE S Y,YUAN H M,et al.,2018.Surface sediment properties and heavy metal contamination assessment in river sediments of the Pearl River Delta,China[J].Marine Pollution Bulletin,136:300-308.
付绪金,贾克力,史小红,等,2013.乌梁素海沉积物腐殖质的组成及分布特征[J].湖泊科学,25(4):489-496.FU X J,JIA K L,SHI X H,et al.,2013.The humus composition and distribution of Lake Wuliangsuhai sediment[J].Journal of Lake Sciences,25(4):489-496.
郭嘉,韦玮,于一雷,等,2015.乌梁素海湿地富营养化研究进展[J].生态学杂志,34(1):3244-3252.GUO J,WEI W,YU Y L,et al.,2015.Research progress on the eutrophication of Wuliangsuhai wetland[J].Chinese Journal of Ecology,34(11):3244-3252.
姜忠峰,张生,李畅游,等,2012.乌梁素海表层沉积物重金属分布特征及生态风险评价[J].环境工程学报,6(6):1673-9108.JIANG Z F,ZHANG S,LI C Y,et al.,2012.Distribution features and ecological risk assessment of heavy metals in surface sediments of Wuliangsuhai Lake[J].Chinese Journal of Environmental Engineering,6(6):1673-9108.
吕杰,2018.环境条件变化下乌梁素海沉积物重金属释放机制研究[D].呼和浩特市:内蒙古农业大学:17-22.LV J,2018.Release mechanism of heavy metals from sediments in wuliangsuhai under environmental changes[D].Huhhot:Inner Mongolia Agricultural University:17-22.
罗高节,黄志宏,2018.生物炭和腐殖质联合修复重金属污染土壤研究进展[J].河南科技学院学报,46(6):1008-7516.LUO G J,HUANG Z H,2018.Research progress on combined remediation of heavy metal contaminated soil by biochar and humus[J].Journal of Henan Institute of Science and Technology(Natural Science Edition),46(6):1008-7516.
李卫平,王晓云,段浩洁,等,2017.乌梁素海表层水中重金属元素的空间分布及生态风险评估[J].环境监测管理与技术,29(5):21-32.LI W P,WANG X Y,DUAN H J,et al.,2017.Spatial distribution and ecological risk assessment of heavy metal elements in surface water of Ulansuhai Lake[J].The Administration and Technique of Environmental Monitoring,29(5):21-32.
孙斌斌,张寅清,王坤坤,等,2018.有机质和阳离子对氧化石墨烯团聚行为的影响[J].中国环境科学,38(3):985-992.SUN B B,ZHANG Y Q,WANG K K,et al.,2018.Impacts of natural organic matter and electrolytes on aggregation kinetics of graphene oxide[J].China Environmental Science,38(3):985-992.
孙丽华,刘华民,王世冬,等,2014.乌梁素海流域土壤盐分和pH值空间分布格局研究[J].湖南生态科学学报,3(1):1-6.SUN L H,LIU H M,WANG S D,et al.,2014.Investigation of Spatial Distribution Pattern of Soil Salinity and pH in the Wuliangsuhai Basin[J].Journal of Hunan Ecological Science,3(1):1-6.
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