滇池水葫芦富集砷、铅、镉形态模拟研究
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摘要
随着国内外对水葫芦的深入研究,水葫芦对重金属的耐受性和富集作用得到越来越多的重视。强繁殖能力是水葫芦的一大特性,利用其生物量大和漂浮的特点来去除滇池水体中的重金属能达到去除量大和不易造成二次污染的良好效果。滇池受到砷、铅、镉等重金属的污染较为严重,通过“疯长”的水葫芦进行富集去除是一个可行有效的方法,本文研究砷、铅、镉等重金属在水葫芦中的富集形态,为研究水葫芦净化富营养化水体提供了一定理论依据。
我国有大量工矿区土地和城市土地等非耕地受重金属的污染,直接影响农产品的卫生品质和地下水、地表水、大气等环境质量,对工农业生产、居民生活和人类健康已造成巨大的危害。尤其是中国加入WTO之后,农产品的重金属超标问题对为我国农业的冲击更大。因此,重金属污染治理是我国当前急需解决的任务。
国家近年来加大了对云南滇池的治理力度,水质也有所好转,但仍处于劣V类,各种污染还比较严重,重金属污染则是其中之一。进入湖泊水体中的重金属被悬浮物和沉积物吸附,这在一定程度上净化了上覆水,对上覆水中的重金属污染起到缓冲和稀释的作用。但沉积物对重金属的吸附能力是有限的,并决定于沉积物的最大吸附量。而沉积物的最大吸附量主要依赖于沉积物的矿物组成,沉积物的粒度及沉积物的有机质含量等各种理化性质。重金属被沉积物吸附后,在一定条件下会再次释放,造成水体的“二次污染”。因此滇池中的重金属污染急需得到一个有效的、不易产生二次污染的方法来解决。
通过实验分析,得出了水葫芦对重金属(砷、铅、镉)的富集量及富集形态。把滇池水葫芦分别置于1.0mg/L(As3+、Pb2+、Cd2+)的溶液中进行培植后,对其根、茎、叶分别预处理后用80%乙醇,去离子水,1mol/L NaCl溶液,2%乙酸,0.6mol/L HCl溶液逐级提取,并对提取液及提取残渣的消解液进行ICP-MS分析,测定出各个部位的提取液及消解液中三种金属离子的富集量。利用液质谱联用技术(HPLC-MS)分析水葫芦富集砷、铅、镉等重金属的形态。
采用GaussviewW3.0和Gaussian系列电子结构程序,通过实验及计算结果表明,重金属离子以不同形态存在,砷的富集形态130种以上；镉的富集形态30种以上；铅的富集形态1种。通过紫外光谱分析得出水葫芦富集重金属(砷、铅、镉)的形态以聚糖、苯醌、萘醌、烯醇、苯环及羟基等基团为主,重金属螯合物有草酸、组氨酸、苹果酸、柠檬酸及谷胱甘肽等小分子物质和金属硫蛋白、植物络合素、金属结合体及金属结合蛋白等大分子物质。
结论为：①实验分析得出水葫芦根、茎、叶对砷、铅、镉具有富集作用,且对砷和铅的富集能力根>叶>茎,对镉的富集能力根>茎>叶；三种重金属的富集量：砷的富集量>铅的富集量>镉的富集量；②富集量不随各种提取液的逐级提取而减少,证明每一种提取液只能提取相溶形态的砷、铅、镉三种元素的化合物和螯合物,每种重金属的富集形态都存在相异性,为HPLC-MS和紫外光谱(UV)分析提供了依据；③HPLC-MS和紫外光谱分析得出水葫芦富集三种重金属的富集形态存在多样性；砷的富集形态>镉的富集形态>铅的富集形态。
最后采用精确度高的从头计算方法、量子化学计算作为分析模拟的计算基础,选择一种HF方法计算出水解物种受亲电试剂攻击的活性顺序为：Pb(OH)42->Pb(OH)3->Pb(OH)2>PbOH+;受亲核试剂攻击的活性顺序为：PbOH+> Pb(OH)2>Pb(OH)3->Pb(OH)42-。
而对于三价砷物种,随着氢配位数的增大,As对前线轨道(HOMO和LUMO)的贡献先显著降低而后略有升高。对于五价砷物种,随着氢配位数的增大,As对HOMO轨道的贡献逐渐增大,对LUMO轨道的贡献逐渐减小,可见随着氢配位数的升高,As接受电子的倾向逐渐减小,即体系酸度增大使As钝化。
水合物种中Cd(Ⅱ)的活性顺序为:Cd(H2O)62+Cd(OH)3(H2O)2->Cd(OH)3(H2O)-> Cd(OH)2(H2O)4>Cd(OH)(H2O)5+。
结合实验及分析结果,采用从头计算量子化学方法,对水葫芦中各官能团富集重金属进行的量子化学分析计算,最终从理论上证实水葫芦具有富集重金属、消除水体重金属污染、净化水体的能力。
With the in-depth study of water hyacinth at home and abroad, the enrichment and tolerance to heavy metal of water hyacinth had got more and more attention. The ability to propagate is one of characteristics to the water hyacinth. Making use of its big haracteristic floating of living beings amount could remove large of heavy metals from water body and get rid of secondary pollution. Dian had been polluted seriously by arsenic, lead, cadmium and other heavy metals.Through "soaring" of water hyacinth to enrich and remove heavy metals in water body is an effective method.So in this paper studying on the shape of enriching in arsenic, lead, cadmium and other heavy metal in the water hyacinth to provide certain theory basis for further research on purification of entropic water body.
In China, a large number of non-cultivated land that is polluted by the heavy metal, for example industrial and mining land and urban land.have affected directly the health of agricultural products quality and environmental quality of groundwater, surface water, atmospheric and has caused great harm agricultural production, living and human health Especially after China accessed to the WTO, the heavy metals exceeded in agricultural products, so it have impacted on China's agriculture. Therefore, the heavy metal pollution is the task of China's current need to be resolved.
In recent years the management strength in Yunnan Dianchi have increased,the water quality has also improved, but it's still in inferior Vclass. Heavy metals that enter in the water body of the lake was suspended by SS and sediment sorption, it purificated of overlying water on some exten. But the adsorption capacity of the sediment decided in the maximum adsorption capacity of sediments,so it's limited, and the maximum adsorption capacity of sediment depended mainly on the mineral composition, particle size and organic matter content for various Organic matter of sediment. Heavy metal that was adsorpted by sediment could be released again in certain conditions,than it caused secondary pollution. Therefore the Dianchi heavy metal pollution was in urgent need of an effective solution.
Analyzing the experiment, had obtained the enrichments quantity and the enrichments shape of water hyacinth to heavy metal (arsenic, lead, cadmium). Put in1.0mg/L separately of the Dian water hyacinth (As3+, Pb2+, Cd2+) in the solution carries on the cultivation, after its, the stem, the leaf pretreats separately with80%ethanol, the deionized water, lmol/L the NaCl(sodium chloride solution),2%Acetic Acid,0.6mol/L the HC1(Hydrochloride). The digestion solution of the extraction and residues were used for measuring the enrichment amount of arsenic in the different parts of water hyacinth by ICP-MS and analyzing the molecular formulas by HPLC-MS.
The experimental results and calculation showed that arsenic had different enrichment conformations in water hyacinth. The conformations of arsenic are130above, cadmium are30above,and lead is only1. By using Ultraviolet Spectrum Analysis, we concluded that enrichment conformations of heavy metal (arsenic, lead, cadmium)in water hyacinth were mainly exist in the forms of polysaccharide, benzoquinone, naphthoquinone, enol, phenyl and hydroxy. Chelates of heavy metals enriched in water hyacinth contains small molecular substances such as oxalic acid, histidine, malic acid, citric acid, Glutathione and macromolecule substances such as metallothionein, foliage Complex, metallic, albumen.
The conclusion is:The experiment analyzes obtained the water hyacinth root, the stem, the leaf have truly enriched to As, Cd, Pb. The enrichments of arsenic and lead were root>leat>stem. The enrichment of cadmium was root> stem>leat.The quantity of three kind of heavy metals enrichments:As> Pb> Cd.2The quantity of enrichments did not descend with Sequential Extraction.It demonstrated that each extract of compatibility can only be extracted one kind of compounds and chelate of arsenic, lead, cadmium, and each shape of heavy metal enrichments exist diversity.It provided the basis for the next analysis of HPLC-MS and Ultraviolet Spectrum Analysis.③HPLC-MS and UV analysis obtained three kinds of water hyacinth accumulation of heavy metals accumulation patterns exist diversity;Enrichments are As>Cd>Pb.
Finally, using the high accuracy ab initio methods, quantum chemical alculations as the analysis simulation calculation basis and choosing a HF method calculated the order of activity that was regulated by the electrophiles attack activity:Pb(OH)42->Pb(OH)3-> Pb(OH)2>PbOH+; the order of activity that was regulated by the nucleophile attacks: PbOH+>Pb(OH)2>Pb(OH)3->Pb(OH)42-.
And along with hydrogen coordination number of the trivalent arsenic species,increased, it's On the contribution of the frontier molecular orbital (HOMO and LUMO) was significantly reduce,and then slightly elevated., along with hydrogen coordination number of the pentavalent arsenic species increased, it's on HOMO orbital contribution increases gradually and the LUMO orbital contributions decreases gradually.visiblely, as the hydrogen coordination number increased, the As accept electronic tendency decreased gradually, namely the acidity of the system increased, As be passived.
The order of Cd(II) in Hydrate's activity:Cd(H2O)62+Cd(OH)3(H2O)2->Cd(OH)3(H2O)3-> Cd(OH)2(H2O)4> Cd(OH)(H2O)5+.
In order to confirm the result of experiment and analysis, Ab initio quantum chemistry methods of calculating are made use. Theoretically it confirmed water hyacinth has ability to enrich heavy metals, eliminate heavy metals pollution, and make water purification.
我国有大量工矿区土地和城市土地等非耕地受重金属的污染,直接影响农产品的卫生品质和地下水、地表水、大气等环境质量,对工农业生产、居民生活和人类健康已造成巨大的危害。尤其是中国加入WTO之后,农产品的重金属超标问题对为我国农业的冲击更大。因此,重金属污染治理是我国当前急需解决的任务。
国家近年来加大了对云南滇池的治理力度,水质也有所好转,但仍处于劣V类,各种污染还比较严重,重金属污染则是其中之一。进入湖泊水体中的重金属被悬浮物和沉积物吸附,这在一定程度上净化了上覆水,对上覆水中的重金属污染起到缓冲和稀释的作用。但沉积物对重金属的吸附能力是有限的,并决定于沉积物的最大吸附量。而沉积物的最大吸附量主要依赖于沉积物的矿物组成,沉积物的粒度及沉积物的有机质含量等各种理化性质。重金属被沉积物吸附后,在一定条件下会再次释放,造成水体的“二次污染”。因此滇池中的重金属污染急需得到一个有效的、不易产生二次污染的方法来解决。
通过实验分析,得出了水葫芦对重金属(砷、铅、镉)的富集量及富集形态。把滇池水葫芦分别置于1.0mg/L(As3+、Pb2+、Cd2+)的溶液中进行培植后,对其根、茎、叶分别预处理后用80%乙醇,去离子水,1mol/L NaCl溶液,2%乙酸,0.6mol/L HCl溶液逐级提取,并对提取液及提取残渣的消解液进行ICP-MS分析,测定出各个部位的提取液及消解液中三种金属离子的富集量。利用液质谱联用技术(HPLC-MS)分析水葫芦富集砷、铅、镉等重金属的形态。
采用GaussviewW3.0和Gaussian系列电子结构程序,通过实验及计算结果表明,重金属离子以不同形态存在,砷的富集形态130种以上；镉的富集形态30种以上；铅的富集形态1种。通过紫外光谱分析得出水葫芦富集重金属(砷、铅、镉)的形态以聚糖、苯醌、萘醌、烯醇、苯环及羟基等基团为主,重金属螯合物有草酸、组氨酸、苹果酸、柠檬酸及谷胱甘肽等小分子物质和金属硫蛋白、植物络合素、金属结合体及金属结合蛋白等大分子物质。
结论为：①实验分析得出水葫芦根、茎、叶对砷、铅、镉具有富集作用,且对砷和铅的富集能力根>叶>茎,对镉的富集能力根>茎>叶；三种重金属的富集量：砷的富集量>铅的富集量>镉的富集量；②富集量不随各种提取液的逐级提取而减少,证明每一种提取液只能提取相溶形态的砷、铅、镉三种元素的化合物和螯合物,每种重金属的富集形态都存在相异性,为HPLC-MS和紫外光谱(UV)分析提供了依据；③HPLC-MS和紫外光谱分析得出水葫芦富集三种重金属的富集形态存在多样性；砷的富集形态>镉的富集形态>铅的富集形态。
最后采用精确度高的从头计算方法、量子化学计算作为分析模拟的计算基础,选择一种HF方法计算出水解物种受亲电试剂攻击的活性顺序为：Pb(OH)42->Pb(OH)3->Pb(OH)2>PbOH+;受亲核试剂攻击的活性顺序为：PbOH+> Pb(OH)2>Pb(OH)3->Pb(OH)42-。
而对于三价砷物种,随着氢配位数的增大,As对前线轨道(HOMO和LUMO)的贡献先显著降低而后略有升高。对于五价砷物种,随着氢配位数的增大,As对HOMO轨道的贡献逐渐增大,对LUMO轨道的贡献逐渐减小,可见随着氢配位数的升高,As接受电子的倾向逐渐减小,即体系酸度增大使As钝化。
水合物种中Cd(Ⅱ)的活性顺序为:Cd(H2O)62+
结合实验及分析结果,采用从头计算量子化学方法,对水葫芦中各官能团富集重金属进行的量子化学分析计算,最终从理论上证实水葫芦具有富集重金属、消除水体重金属污染、净化水体的能力。
With the in-depth study of water hyacinth at home and abroad, the enrichment and tolerance to heavy metal of water hyacinth had got more and more attention. The ability to propagate is one of characteristics to the water hyacinth. Making use of its big haracteristic floating of living beings amount could remove large of heavy metals from water body and get rid of secondary pollution. Dian had been polluted seriously by arsenic, lead, cadmium and other heavy metals.Through "soaring" of water hyacinth to enrich and remove heavy metals in water body is an effective method.So in this paper studying on the shape of enriching in arsenic, lead, cadmium and other heavy metal in the water hyacinth to provide certain theory basis for further research on purification of entropic water body.
In China, a large number of non-cultivated land that is polluted by the heavy metal, for example industrial and mining land and urban land.have affected directly the health of agricultural products quality and environmental quality of groundwater, surface water, atmospheric and has caused great harm agricultural production, living and human health Especially after China accessed to the WTO, the heavy metals exceeded in agricultural products, so it have impacted on China's agriculture. Therefore, the heavy metal pollution is the task of China's current need to be resolved.
In recent years the management strength in Yunnan Dianchi have increased,the water quality has also improved, but it's still in inferior Vclass. Heavy metals that enter in the water body of the lake was suspended by SS and sediment sorption, it purificated of overlying water on some exten. But the adsorption capacity of the sediment decided in the maximum adsorption capacity of sediments,so it's limited, and the maximum adsorption capacity of sediment depended mainly on the mineral composition, particle size and organic matter content for various Organic matter of sediment. Heavy metal that was adsorpted by sediment could be released again in certain conditions,than it caused secondary pollution. Therefore the Dianchi heavy metal pollution was in urgent need of an effective solution.
Analyzing the experiment, had obtained the enrichments quantity and the enrichments shape of water hyacinth to heavy metal (arsenic, lead, cadmium). Put in1.0mg/L separately of the Dian water hyacinth (As3+, Pb2+, Cd2+) in the solution carries on the cultivation, after its, the stem, the leaf pretreats separately with80%ethanol, the deionized water, lmol/L the NaCl(sodium chloride solution),2%Acetic Acid,0.6mol/L the HC1(Hydrochloride). The digestion solution of the extraction and residues were used for measuring the enrichment amount of arsenic in the different parts of water hyacinth by ICP-MS and analyzing the molecular formulas by HPLC-MS.
The experimental results and calculation showed that arsenic had different enrichment conformations in water hyacinth. The conformations of arsenic are130above, cadmium are30above,and lead is only1. By using Ultraviolet Spectrum Analysis, we concluded that enrichment conformations of heavy metal (arsenic, lead, cadmium)in water hyacinth were mainly exist in the forms of polysaccharide, benzoquinone, naphthoquinone, enol, phenyl and hydroxy. Chelates of heavy metals enriched in water hyacinth contains small molecular substances such as oxalic acid, histidine, malic acid, citric acid, Glutathione and macromolecule substances such as metallothionein, foliage Complex, metallic, albumen.
The conclusion is:The experiment analyzes obtained the water hyacinth root, the stem, the leaf have truly enriched to As, Cd, Pb. The enrichments of arsenic and lead were root>leat>stem. The enrichment of cadmium was root> stem>leat.The quantity of three kind of heavy metals enrichments:As> Pb> Cd.2The quantity of enrichments did not descend with Sequential Extraction.It demonstrated that each extract of compatibility can only be extracted one kind of compounds and chelate of arsenic, lead, cadmium, and each shape of heavy metal enrichments exist diversity.It provided the basis for the next analysis of HPLC-MS and Ultraviolet Spectrum Analysis.③HPLC-MS and UV analysis obtained three kinds of water hyacinth accumulation of heavy metals accumulation patterns exist diversity;Enrichments are As>Cd>Pb.
Finally, using the high accuracy ab initio methods, quantum chemical alculations as the analysis simulation calculation basis and choosing a HF method calculated the order of activity that was regulated by the electrophiles attack activity:Pb(OH)42->Pb(OH)3-> Pb(OH)2>PbOH+; the order of activity that was regulated by the nucleophile attacks: PbOH+>Pb(OH)2>Pb(OH)3->Pb(OH)42-.
And along with hydrogen coordination number of the trivalent arsenic species,increased, it's On the contribution of the frontier molecular orbital (HOMO and LUMO) was significantly reduce,and then slightly elevated., along with hydrogen coordination number of the pentavalent arsenic species increased, it's on HOMO orbital contribution increases gradually and the LUMO orbital contributions decreases gradually.visiblely, as the hydrogen coordination number increased, the As accept electronic tendency decreased gradually, namely the acidity of the system increased, As be passived.
The order of Cd(II) in Hydrate's activity:Cd(H2O)62+
In order to confirm the result of experiment and analysis, Ab initio quantum chemistry methods of calculating are made use. Theoretically it confirmed water hyacinth has ability to enrich heavy metals, eliminate heavy metals pollution, and make water purification.
引文
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