锦州市铁合金厂土壤重金属污染分析、修复及植物产后利用的研究
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摘要
本论文针对目前锦州市铁合金厂周边土壤及蔬菜重金属污染严重、土壤重金属污染修复效率低及修复植物产后处理困难等问题,分别研究了锦州市铁合金厂周边及农田(大田、大棚内)土壤中典型重金属(Cu、Zn、Cr及Cd)的含量及分布,分析了Cu、Zn、Cr及Cd对土壤酶(脲酶、蛋白酶、蔗糖酶、过氧化氢酶)活性的影响,揭示了叶菜类蔬菜(不同生长期)及杂草对Cu、Zn、Cr及Cd的吸收、分布及富集规律,并对该地区叶菜类蔬菜重金属污染程度进行了系统评价,探讨了钼酸铵、邻苯二甲酸氢钾-氢氧化钠、磷酸二氢钠-柠檬酸对土壤重金属化学形态变化的影响,以及化学强化物质(钼酸铵及磷酸二氢钠-柠檬酸)对植物修复重金属污染土壤的诱导规律,发现了灯笼草是一种新的Zn超累积植物,以富集Zn的灯笼草为原料,成功制备了氧化锌纳米粒子与多壁碳纳米管。具体研究结果如下:
1、重金属复合污染对土壤酶活性的影响
(1)铁合金厂不同区域土壤酶活性存在较大差异。随土壤样品和酶类型不同,酶活性变化幅度相差较大。其中过氧化氢酶变化幅度最大,蛋白酶变化幅度最小。铁合金厂土壤环境下,随着土壤中Cu、Zn、Cr及Cd浓度增加,脲酶、蛋白酶、蔗糖酶、过氧化氢酶活性显著降低。
(2)在钼酸铵作用下,四种酶活性均呈不规律变化。其中,蔗糖酶与脲酶活性基本呈上升趋势(激活效应),过氧化氢酶和蛋白酶活性均减小(抑制效应)。
2、重金属在土壤-植物体系中的迁移转化研究
(1)苦苣、生菜、菠菜及小白菜对土壤中重金属的吸收规律不同。铁合金厂周边农田种植的四种叶菜类蔬菜均受到重金属严重污染。其中Cr与Cd对四种叶菜类蔬菜的污染贡献最大。
(2)车前草、蒲公英、野艾蒿、皱叶酸模及灯笼草五种杂草对土壤中的重金属有一定的富集作用。同种杂草对不同重金属的富集作用不同,不同杂草对不同重金属的富集作用也不同。五种杂草中灯笼草叶对Zn和Cd的富集作用最强;野艾蒿根对Cr的富集作用最强;车前草根对Cu的富集作用最强。
3、铁合金厂土壤重金属污染的修复
(1)钼酸铵对土壤中的Cr与Zn起固定作用,而对Cd、Cu、Ni起活化作用。
(2)邻苯二甲酸氢钾-氢氧化钠缓冲体系(pH=5.2-6.2)对土壤中Cr、Cu、Hg、Pb的酸可提取态的转化有明显的促进作用;对土壤中As、Hg的氧化结合态及有机结合态的转化有明显的促进作用。
(3)磷酸二氢钠-柠檬酸缓冲体系(pH=5.2-7.2)可提高土壤中Zn、Mo、Ni、Pb、Cu、As、Cr、Cd和Hg酸可提取态的含量。其中,柠檬酸对土壤重金属化学形态变化起主要作用。
(4)在土壤Zn含量为5000 mg/kg的条件下,植物生长12周后,灯笼草地上部Zn含量达到10976 mg/kg,对土壤中Zn的富集系数及转运系数均大于1,由此证明灯笼草是一种Zn的超累积植物。
(5)钼酸铵有助于苜蓿草对生物量的积累,而且增强了苜蓿草对重金属的富集能力。磷酸二氢钠-柠檬酸(pH=5.2-7.2)也有助于苜蓿草对生物量的积累。在磷酸二氢钠-柠檬酸的影响下,苜蓿草对As、Cr、Hg、Mo和Zn的转运系数增加,但降低了对Cd、Cu、Ni和Pb的转运系数。
4、修复植物的产后处理
(1)以富集Zn的灯笼草地上部分为原料,制得较纯净的氧化锌纳米粒子,其平均粒径为72.5 nm。
(2)以灯笼草体内的维管束为原料,制备了纯净的多壁碳纳米管。多壁碳纳米管的结构为:中空、外径范围为20-500 nm,内径范围为10-200 nm,管壁上存在着缺陷,且直径与管长不统一。
In this thesis, we focus on the problem in the soil and vegetables contaminated seriously by heavy metals, the low efficiency of remediation, and difficulty of the reuse phytoremediation. The contents and distributions of heavy metals (Cu, Zn, Cr, and Cd) in the farmland (field and greenhouse) and soil around ferroalloy plant (Jinzhou, China) were studied. The influences of Cu, Zn, Cr, and Cd on soil enzyme (urease, protease, sucrose, and catalase) activities were analyzed. The regular patterns of absorption, distribution, and enrichment of heavy metals (Cu, Zn, Cr, and Cd) in leafy vegetables (in different growth phase) and weeds were revealed. The pollution degree of vegetables by heavy metals was assessed. The effects of ammonium molybdate, potassium acid phthalate-sodium hydroxide, and sodium dihydrogen phosphate-citric acid on the transformation of chemical states in heavy metals were discussed. The inducement patterns of chemical substances (ammonium molybdate and sodium dihydrogen phosphate-citric acid) on phytoremediation of soil contaminated by heavy metals were studied. Physalis alkekengi L. was a newly found zinc hyperaccumulator. ZnO nanoparticles and multi-walled carbon nanotubes were synthesized using Physalis alkekengi L. which had enriched Zn fron soil. The findings are shown as follows:
1. Effect of combined heavy metal contamination on soil enzyme activities
(1) The soil enzyme activities in different areas were extremely different. The change amplitudes of soil enzyme activities were varied significantly with different soil and enzyme: the change amplitudes of catalase activities were significant, but the change amplitudes of protease activities were minimum. In the soil of ferroalloy plant, the activities of urease, protease, sucrose, and catalase were decreasing significantly with the increasing of the contents of Cu, Zn, Cr, and Cd in soil.
(2) With the additions of ammonium molybdate into soil, the changes of soil enzyme (urease, protease, sucrose, and catalase) activities were not regulation. The activities of urease and sucrose were increased (activate effect), but the activities of protease and catalase were decreased (inhibit effect).
2. The study of the migration and transformation of heavy metals in soil-plant
(1) The regular patterns of absorption of heavy metals by Endive, Lettuce, Spinach, and Chinese Cabbage were different. Endive, Lettuce, Spinach, and Chinese Cabbage growing in the soil of ferroalloy plant were contaminated seriously by heavy metals. The contributions of Cd and Cr on contamination in four leafy vegetables were maximum.
(2) The heavy metals in soil were accumulated in Plantago asiatica L., Taraxacum mongolicum, Artemisia lavandula, Artemisia Lavandulaefolia and Physalis alkekengi L.. The enrichment on different heavy metals by the same weed and different weeds were not alike. For the five kinds of weeds, enrichment on Zn and Cd by leaf of Physalis alkekengi L. was powerful; enrichment on Cr by root of Artemisia lavandula was powerful; enrichment on Cu by root of Plantago asiatica L. was powerful.
3. The remediation of soil contaminated by heavy metals in ferroalloy plant
(1) The effects of ammonium molybdate on Cr and Zn in soil were immobilization, but the effects of it on Cd, Cu, and Ni in soil were mobilization.
(2) The promoting effects of potassium acid phthalate-sodium hydroxide (pH ranged from 5.2 to 6.2) on the transformation of both the acid soluble fractions in Cr, Cu, Hg, Pb and the oxidation associated as well as organic associated fractions in As, Hg were significant.
(3) With addition of sodium dihydrogen phosphate-citric acid (pH ranged from 5.2 to 7.2) into soil, the contents of acid soluble fractions in Zn, Mo, Ni, Pb, Cu, As, Cr, Cd, and Hg were increased. Citric acid played a leading role in the transformation of chemical states in heavy metals.
(4) The zinc concentrations in the aerial parts of P. alkekengi plants growing in soil spiked with 5000 mg/kg zinc increased to 10976 mg/kg (dry weight) within 12 weeks. The values of bioconcentration factor and translocation factor were greater than 1, which confirmed that Physalis alkekengi L. was a zinc hyperaccumulator.
(5) With addition of ammonium molybdate into soil, both the biomass of alfalfa and the enrichment on heavy metals by alfalfa were enhanced. The sodium dihydrogen phosphate-citric acid (pH ranged from 5.2 to 7.2) could promote alfalfa to produce more biomass. The translocation factors of As, Cr, Hg, Mo, and Zn in alfalfa were increased, but them of Cd, Cu, Ni, and Pb were decreased after sodium dihydrogen phosphate-citric acid was added into soil.
4. The reuse of phytoremediation
(1) The pure ZnO nanoparticles were synthesized using the shoot of Physalis alkekengi L., which had enriched Zn from soil, as material. ZnO nanoparticles had a mean size of 72.5 nm.
(2) The pure multi-walled carbon nanotubes were synthesized using the vascular bundles in Physalis alkekengi L. as material. The structure of synthesized multi-walled carbon nanotubes was middle-hollow. The inner diameter ranged from 10 to 200 nm, and the outer diameter ranged from 20 to 500 nm. There were a few defects in the walls of the multi-walled carbon nanotubes. The diameter and length of the multi-walled carbon nanotubes were ununiform.
1、重金属复合污染对土壤酶活性的影响
(1)铁合金厂不同区域土壤酶活性存在较大差异。随土壤样品和酶类型不同,酶活性变化幅度相差较大。其中过氧化氢酶变化幅度最大,蛋白酶变化幅度最小。铁合金厂土壤环境下,随着土壤中Cu、Zn、Cr及Cd浓度增加,脲酶、蛋白酶、蔗糖酶、过氧化氢酶活性显著降低。
(2)在钼酸铵作用下,四种酶活性均呈不规律变化。其中,蔗糖酶与脲酶活性基本呈上升趋势(激活效应),过氧化氢酶和蛋白酶活性均减小(抑制效应)。
2、重金属在土壤-植物体系中的迁移转化研究
(1)苦苣、生菜、菠菜及小白菜对土壤中重金属的吸收规律不同。铁合金厂周边农田种植的四种叶菜类蔬菜均受到重金属严重污染。其中Cr与Cd对四种叶菜类蔬菜的污染贡献最大。
(2)车前草、蒲公英、野艾蒿、皱叶酸模及灯笼草五种杂草对土壤中的重金属有一定的富集作用。同种杂草对不同重金属的富集作用不同,不同杂草对不同重金属的富集作用也不同。五种杂草中灯笼草叶对Zn和Cd的富集作用最强;野艾蒿根对Cr的富集作用最强;车前草根对Cu的富集作用最强。
3、铁合金厂土壤重金属污染的修复
(1)钼酸铵对土壤中的Cr与Zn起固定作用,而对Cd、Cu、Ni起活化作用。
(2)邻苯二甲酸氢钾-氢氧化钠缓冲体系(pH=5.2-6.2)对土壤中Cr、Cu、Hg、Pb的酸可提取态的转化有明显的促进作用;对土壤中As、Hg的氧化结合态及有机结合态的转化有明显的促进作用。
(3)磷酸二氢钠-柠檬酸缓冲体系(pH=5.2-7.2)可提高土壤中Zn、Mo、Ni、Pb、Cu、As、Cr、Cd和Hg酸可提取态的含量。其中,柠檬酸对土壤重金属化学形态变化起主要作用。
(4)在土壤Zn含量为5000 mg/kg的条件下,植物生长12周后,灯笼草地上部Zn含量达到10976 mg/kg,对土壤中Zn的富集系数及转运系数均大于1,由此证明灯笼草是一种Zn的超累积植物。
(5)钼酸铵有助于苜蓿草对生物量的积累,而且增强了苜蓿草对重金属的富集能力。磷酸二氢钠-柠檬酸(pH=5.2-7.2)也有助于苜蓿草对生物量的积累。在磷酸二氢钠-柠檬酸的影响下,苜蓿草对As、Cr、Hg、Mo和Zn的转运系数增加,但降低了对Cd、Cu、Ni和Pb的转运系数。
4、修复植物的产后处理
(1)以富集Zn的灯笼草地上部分为原料,制得较纯净的氧化锌纳米粒子,其平均粒径为72.5 nm。
(2)以灯笼草体内的维管束为原料,制备了纯净的多壁碳纳米管。多壁碳纳米管的结构为:中空、外径范围为20-500 nm,内径范围为10-200 nm,管壁上存在着缺陷,且直径与管长不统一。
In this thesis, we focus on the problem in the soil and vegetables contaminated seriously by heavy metals, the low efficiency of remediation, and difficulty of the reuse phytoremediation. The contents and distributions of heavy metals (Cu, Zn, Cr, and Cd) in the farmland (field and greenhouse) and soil around ferroalloy plant (Jinzhou, China) were studied. The influences of Cu, Zn, Cr, and Cd on soil enzyme (urease, protease, sucrose, and catalase) activities were analyzed. The regular patterns of absorption, distribution, and enrichment of heavy metals (Cu, Zn, Cr, and Cd) in leafy vegetables (in different growth phase) and weeds were revealed. The pollution degree of vegetables by heavy metals was assessed. The effects of ammonium molybdate, potassium acid phthalate-sodium hydroxide, and sodium dihydrogen phosphate-citric acid on the transformation of chemical states in heavy metals were discussed. The inducement patterns of chemical substances (ammonium molybdate and sodium dihydrogen phosphate-citric acid) on phytoremediation of soil contaminated by heavy metals were studied. Physalis alkekengi L. was a newly found zinc hyperaccumulator. ZnO nanoparticles and multi-walled carbon nanotubes were synthesized using Physalis alkekengi L. which had enriched Zn fron soil. The findings are shown as follows:
1. Effect of combined heavy metal contamination on soil enzyme activities
(1) The soil enzyme activities in different areas were extremely different. The change amplitudes of soil enzyme activities were varied significantly with different soil and enzyme: the change amplitudes of catalase activities were significant, but the change amplitudes of protease activities were minimum. In the soil of ferroalloy plant, the activities of urease, protease, sucrose, and catalase were decreasing significantly with the increasing of the contents of Cu, Zn, Cr, and Cd in soil.
(2) With the additions of ammonium molybdate into soil, the changes of soil enzyme (urease, protease, sucrose, and catalase) activities were not regulation. The activities of urease and sucrose were increased (activate effect), but the activities of protease and catalase were decreased (inhibit effect).
2. The study of the migration and transformation of heavy metals in soil-plant
(1) The regular patterns of absorption of heavy metals by Endive, Lettuce, Spinach, and Chinese Cabbage were different. Endive, Lettuce, Spinach, and Chinese Cabbage growing in the soil of ferroalloy plant were contaminated seriously by heavy metals. The contributions of Cd and Cr on contamination in four leafy vegetables were maximum.
(2) The heavy metals in soil were accumulated in Plantago asiatica L., Taraxacum mongolicum, Artemisia lavandula, Artemisia Lavandulaefolia and Physalis alkekengi L.. The enrichment on different heavy metals by the same weed and different weeds were not alike. For the five kinds of weeds, enrichment on Zn and Cd by leaf of Physalis alkekengi L. was powerful; enrichment on Cr by root of Artemisia lavandula was powerful; enrichment on Cu by root of Plantago asiatica L. was powerful.
3. The remediation of soil contaminated by heavy metals in ferroalloy plant
(1) The effects of ammonium molybdate on Cr and Zn in soil were immobilization, but the effects of it on Cd, Cu, and Ni in soil were mobilization.
(2) The promoting effects of potassium acid phthalate-sodium hydroxide (pH ranged from 5.2 to 6.2) on the transformation of both the acid soluble fractions in Cr, Cu, Hg, Pb and the oxidation associated as well as organic associated fractions in As, Hg were significant.
(3) With addition of sodium dihydrogen phosphate-citric acid (pH ranged from 5.2 to 7.2) into soil, the contents of acid soluble fractions in Zn, Mo, Ni, Pb, Cu, As, Cr, Cd, and Hg were increased. Citric acid played a leading role in the transformation of chemical states in heavy metals.
(4) The zinc concentrations in the aerial parts of P. alkekengi plants growing in soil spiked with 5000 mg/kg zinc increased to 10976 mg/kg (dry weight) within 12 weeks. The values of bioconcentration factor and translocation factor were greater than 1, which confirmed that Physalis alkekengi L. was a zinc hyperaccumulator.
(5) With addition of ammonium molybdate into soil, both the biomass of alfalfa and the enrichment on heavy metals by alfalfa were enhanced. The sodium dihydrogen phosphate-citric acid (pH ranged from 5.2 to 7.2) could promote alfalfa to produce more biomass. The translocation factors of As, Cr, Hg, Mo, and Zn in alfalfa were increased, but them of Cd, Cu, Ni, and Pb were decreased after sodium dihydrogen phosphate-citric acid was added into soil.
4. The reuse of phytoremediation
(1) The pure ZnO nanoparticles were synthesized using the shoot of Physalis alkekengi L., which had enriched Zn from soil, as material. ZnO nanoparticles had a mean size of 72.5 nm.
(2) The pure multi-walled carbon nanotubes were synthesized using the vascular bundles in Physalis alkekengi L. as material. The structure of synthesized multi-walled carbon nanotubes was middle-hollow. The inner diameter ranged from 10 to 200 nm, and the outer diameter ranged from 20 to 500 nm. There were a few defects in the walls of the multi-walled carbon nanotubes. The diameter and length of the multi-walled carbon nanotubes were ununiform.
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