CN104624635B - A microbial nutrient for remediation of chromium-contaminated soil and sediments - Google Patents
A microbial nutrient for remediation of chromium-contaminated soil and sediments Download PDFInfo
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- 239000002689 soil Substances 0.000 title claims abstract description 56
- 230000000813 microbial effect Effects 0.000 title claims abstract description 31
- 239000013049 sediment Substances 0.000 title claims description 20
- 235000015097 nutrients Nutrition 0.000 title description 21
- 238000005067 remediation Methods 0.000 title description 8
- 244000005700 microbiome Species 0.000 claims abstract description 19
- 235000013379 molasses Nutrition 0.000 claims abstract description 16
- 239000000843 powder Substances 0.000 claims abstract description 14
- 239000003795 chemical substances by application Substances 0.000 claims abstract description 9
- 235000016709 nutrition Nutrition 0.000 claims abstract description 9
- 230000035764 nutrition Effects 0.000 claims abstract description 9
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- 235000010469 Glycine max Nutrition 0.000 claims abstract description 5
- 230000009467 reduction Effects 0.000 claims abstract description 5
- 231100000614 poison Toxicity 0.000 claims abstract description 3
- 231100000053 low toxicity Toxicity 0.000 claims abstract 2
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- CKUAXEQHGKSLHN-UHFFFAOYSA-N [C].[N] Chemical compound [C].[N] CKUAXEQHGKSLHN-UHFFFAOYSA-N 0.000 claims description 3
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- 238000002955 isolation Methods 0.000 claims 1
- 239000000203 mixture Substances 0.000 claims 1
- 239000011651 chromium Substances 0.000 abstract description 31
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 abstract description 27
- 229910052804 chromium Inorganic materials 0.000 abstract description 27
- 238000000034 method Methods 0.000 abstract description 13
- 238000001556 precipitation Methods 0.000 abstract description 3
- 230000008569 process Effects 0.000 abstract description 3
- 239000000463 material Substances 0.000 abstract description 2
- 238000010521 absorption reaction Methods 0.000 abstract 1
- JOPOVCBBYLSVDA-UHFFFAOYSA-N chromium(6+) Chemical compound [Cr+6] JOPOVCBBYLSVDA-UHFFFAOYSA-N 0.000 description 36
- 235000010627 Phaseolus vulgaris Nutrition 0.000 description 13
- 244000046052 Phaseolus vulgaris Species 0.000 description 13
- 238000002386 leaching Methods 0.000 description 13
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 3
- 229910052799 carbon Inorganic materials 0.000 description 3
- BFGKITSFLPAWGI-UHFFFAOYSA-N chromium(3+) Chemical compound [Cr+3] BFGKITSFLPAWGI-UHFFFAOYSA-N 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 239000002893 slag Substances 0.000 description 3
- 238000003756 stirring Methods 0.000 description 3
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 2
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- 239000006227 byproduct Substances 0.000 description 2
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- KSPIHGBHKVISFI-UHFFFAOYSA-N Diphenylcarbazide Chemical compound C=1C=CC=CC=1NNC(=O)NNC1=CC=CC=C1 KSPIHGBHKVISFI-UHFFFAOYSA-N 0.000 description 1
- 230000009471 action Effects 0.000 description 1
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Abstract
Description
技术领域 technical field
本发明涉及一种用于修复铬污染土壤和沉积物的微生物营养剂，属于环保技术领域。 The invention relates to a microbial nutrient for repairing chromium-polluted soil and deposits, and belongs to the technical field of environmental protection.
背景技术 Background technique
铬（Cr）是自然环境中常见的一种金属污染物，也是美国超级基金优先控制的前20种有毒物质之一。我国自1958年建成第一条铬盐生产线至今，先后有70余家企业生产过铬盐，现存25家，根据《铬渣污染综合整治方案》的统计数据，我国累计产生铬渣量约为600万t。铬渣中含有0.3～1.5%可溶性六价铬，经降水和地表水冲刷，进入周围土壤和地下水，造成了环境严重的铬污染。目前我国受六价铬严重污染的土壤达1250万吨，对铬污染土壤的治理刻不容缓，急需修复铬污染土壤的关键技术。 Chromium (Cr) is a common metal pollutant in the natural environment, and it is also one of the top 20 toxic substances prioritized by the US Superfund. Since my country built the first chromium salt production line in 1958, more than 70 enterprises have produced chromium salts, and there are 25 existing ones. According to the statistics of the "Comprehensive Treatment Plan for Chromium Slag Pollution", the cumulative amount of chromium slag produced in my country is about 600 million. million t. Chromium slag contains 0.3-1.5% soluble hexavalent chromium, which is washed by precipitation and surface water and enters the surrounding soil and groundwater, causing serious chromium pollution to the environment. At present, the soil seriously polluted by hexavalent chromium in my country has reached 12.5 million tons, and the treatment of chromium-contaminated soil is urgent, and the key technology for repairing chromium-contaminated soil is urgently needed.
修复六价铬污染土壤的传统方法有化学固定法、化学还原法、土壤淋洗法和电动修复法等。而这些方法大多数需要高能耗或者需要大量的化学试剂，成本高且易造成二次污染。近年来，微生物修复法由于其环境友好性和较低成本等优点备受关注。微生物修复铬污染土壤主要是利用土壤中的土著微生物或加入经驯化的高效微生物，通过微生物还原反应，将有毒的、可移动的Cr(Ⅵ)还原为低毒的、不易移动的Cr(Ⅲ)，达到治理铬污染土壤的目的。而应用土著微生物进行有毒废物解毒与污染土壤修复在环境安全性、环境适应性与种群协调性以及应用成本方面具有其他异地菌种不可比拟的优越性。但由于环境中营养物质的缺乏，有效的土著微生物的生长较为缓慢，使得铬污染土壤的修复受到限制。因此，本发明提供一种用于修复铬污染土壤和沉积物的微生物营养剂，通过为土著铬还原微生物提供营养物质，刺激其生长，进行铬污染土壤的修复。另外，本发明同样适用于铬污染沉积物的修复。 Traditional methods for remediating hexavalent chromium-contaminated soil include chemical fixation, chemical reduction, soil leaching, and electrokinetic remediation. Most of these methods require high energy consumption or a large amount of chemical reagents, which are costly and easily cause secondary pollution. In recent years, microbial remediation has attracted much attention due to its environmental friendliness and low cost. Microbial remediation of chromium-contaminated soil mainly uses indigenous microorganisms in the soil or adding domesticated and efficient microorganisms to reduce toxic and mobile Cr(VI) to low-toxic and non-mobile Cr(III) through microbial reduction reaction. , to achieve the purpose of controlling chromium-contaminated soil. The use of indigenous microorganisms for toxic waste detoxification and contaminated soil remediation has incomparable advantages over other exotic strains in terms of environmental safety, environmental adaptability, population coordination, and application cost. However, due to the lack of nutrients in the environment, the growth of effective indigenous microorganisms is relatively slow, which limits the remediation of chromium-contaminated soils. Therefore, the present invention provides a microbial nutrient for remediating chromium-contaminated soil and sediments, which can remediate chromium-contaminated soil by providing nutrients for indigenous chromium-reducing microorganisms and stimulating their growth. In addition, the present invention is also applicable to the remediation of chromium-contaminated deposits.
发明内容 Contents of the invention
本发明旨在提供一种用于修复铬污染土壤和沉积物的微生物营养剂，由豆饼粉和糖蜜以一定配比组成，其中豆饼粉和糖蜜的配比及用量根据土壤中六价铬的污染浓度而定。通过向土壤或沉积物中加入本发明的微生物营养剂，促进土壤或沉积物中土著微生物的大量生长，利用微生物的还原作用将土壤或沉积物中有毒的、可移动的Cr(Ⅵ)还原为低毒的、不易移动的Cr(Ⅲ)，同时，微生物会通过吸附、沉淀等过程，将三价铬固定，减少其移动性和生物可利用性，也避免三价铬再次被氧化为六价铬。本发明具有成本低、效果好、材料易得、使用方便、环境友好等优点。 The present invention aims to provide a microbial nutrient for repairing chromium-contaminated soil and deposits, which is composed of bean cake powder and molasses in a certain proportion, wherein the proportion and dosage of bean cake powder and molasses are based on the pollution of hexavalent chromium in the soil Concentration depends. By adding the microbial nutrient of the present invention to the soil or sediment, the mass growth of indigenous microorganisms in the soil or sediment is promoted, and the toxic and mobile Cr(VI) in the soil or sediment is reduced to Low-toxic, non-mobile Cr(Ⅲ), at the same time, microorganisms will fix trivalent chromium through adsorption, precipitation and other processes, reducing its mobility and bioavailability, and also avoiding the oxidation of trivalent chromium to hexavalent again chromium. The invention has the advantages of low cost, good effect, readily available materials, convenient use, and environmental friendliness.
本发明中的微生物营养剂选用糖蜜，一是因为糖蜜可以增加土壤或沉积物中六价铬的浸出；二是可直接作为还原Cr(Ⅵ)的电子供体；三是糖蜜也可以作为微生物利用的碳源，促进微生物的生长。豆饼粉的碳氮比约6.76，可为微生物提供氮源。糖蜜和豆饼粉以一定配比组成的微生物营养剂碳氮比约15～40，非常有利于土著微生物对其矿化，从而促进土著微生物的生长，提高六价铬的还原稳定化效率。 The microbial nutrition agent among the present invention selects molasses, the one, because molasses can increase the leaching of hexavalent chromium in soil or sediment; A carbon source that promotes the growth of microorganisms. The carbon-to-nitrogen ratio of bean cake flour is about 6.76, which can provide nitrogen source for microorganisms. The carbon-to-nitrogen ratio of microbial nutrients composed of molasses and bean cake powder is about 15-40, which is very conducive to the mineralization of indigenous microorganisms, thereby promoting the growth of indigenous microorganisms and improving the reduction and stabilization efficiency of hexavalent chromium.
本发明提供的一种用于修复铬污染土壤和沉积物的微生物营养剂，其优选的使用方法如下： A kind of microbial nutrient for repairing chromium-contaminated soil and sediment provided by the invention, its preferred method of use is as follows:
将土壤或沉积物破碎至直径小于2mm，向土壤或沉积物中添加糖蜜和豆饼粉以一定配比组成的微生物营养剂，搅拌均匀，调节含水率，隔绝空气养护20天以上，既得修复后土壤或沉积物。其中，上述微生物营养剂中豆饼粉和糖蜜的质量比为1：2～10，所加微生物营养剂的用量为土壤或沉积物质量的2%～20%，含水率控制为25%～40%，温度在20℃～30℃为宜。 Crush the soil or sediment to a diameter of less than 2mm, add microbial nutrients composed of molasses and bean cake powder to the soil or sediment, stir evenly, adjust the moisture content, isolate the air for more than 20 days, and obtain the repaired soil or sediment. Among them, the mass ratio of bean cake powder and molasses in the above-mentioned microbial nutrient is 1:2-10, the amount of added microbial nutrient is 2%-20% of the soil or sediment mass, and the moisture content is controlled at 25%-40%. , the temperature is preferably between 20°C and 30°C.
本发明与现有技术相比具有下列优点和效果： Compared with the prior art, the present invention has the following advantages and effects:
1、修复效果好：微生物的还原作用可将有毒的、可移动的Cr(Ⅵ)还原为低毒的、不易移动的Cr(Ⅲ)，同时，微生物会通过吸附、沉淀等过程，将三价铬固定，减少其移动性和生物可利用性，避免三价铬再次被氧化为六价铬。本发明对土壤或沉积物中六价铬的去除率可达96%以上，总铬和六价铬的稳定化效率（浸出液中总铬或六价铬浓度的减少比率）可达95%以上，大大降低了毒性和危害； 1. Good repair effect: The reduction of microorganisms can reduce the toxic and mobile Cr(Ⅵ) to low-toxic and non-mobile Cr(Ⅲ). At the same time, the microorganisms will convert the trivalent Chromium is fixed, reducing its mobility and bioavailability, avoiding the re-oxidation of trivalent chromium to hexavalent chromium. The removal rate of hexavalent chromium in soil or sediment can reach more than 96%, and the stabilization efficiency of total chromium and hexavalent chromium (the reduction rate of total chromium or hexavalent chromium concentration in the leach solution) can reach more than 95%. Greatly reduced toxicity and hazards;
2、成本低：本发明所述糖蜜为制糖过程的副产物，豆饼粉为大豆(主要是黄豆和黑豆)榨油后的副产品，来源广泛、价格低廉； 2, cost is low: molasses described in the present invention is the by-product of sugar-making process, and bean cake powder is the by-product after soybean (mainly soybean and black soybean) oil extraction, and source is extensive, cheap;
3、使用方便：本发明所述微生物营养剂在使用过程中涉及的机械设备主要有挖掘机、粉碎机和搅拌机，操作简便； 3. Easy to use: The mechanical equipment involved in the use of the microbial nutrient of the present invention mainly includes excavators, pulverizers and mixers, which are easy to operate;
4、环境友好：本发明通过微生物的作用还原稳定化六价铬，避免了化学试剂的使用，具有环境安全性，另外，本发明是通过刺激土著微生物的生长起作用，不添加异地菌，在环境适应性与种群协调性方面更具优势。 4. Environmentally friendly: the present invention reduces and stabilizes hexavalent chromium through the action of microorganisms, avoids the use of chemical reagents, and has environmental safety. In addition, the present invention works by stimulating the growth of indigenous microorganisms without adding foreign bacteria. It has more advantages in environmental adaptability and population coordination.
具体实施方式 detailed description
以下实施例用于说明本发明，但不用来限制本发明的范围。 The following examples are used to illustrate the present invention, but are not intended to limit the scope of the present invention.
实施例中所有样品的分析方法如下：依据《土壤水分测定法》（NY/T52-1987）测定土壤含水率，依据《固体废物六价铬的测定碱消解/火焰原子吸收分光光度法》（HJ687-2014）测定土壤六价铬浓度；依据《固体废物浸出毒性浸出方法—硫酸硝酸法》（HJ/T299-2007）制备浸出液，并根据《水质六价铬的测定二苯碳酰二肼分光光度法》（GB7467-87）测定浸出液中六价铬的浓度，采用火焰原子吸收分光光度法测定浸出液中总铬的浓度。 The analysis method of all samples in the embodiment is as follows: according to " soil moisture determination method " (NY/T52-1987 ) Determination of soil moisture content, according to " determination of hexavalent chromium in solid waste Alkali digestion/flame atomic absorption spectrophotometry " (HJ687 -2014) to determine the concentration of hexavalent chromium in soil; prepare the leach solution according to "Solid Waste Leaching Toxic Leaching Method-Sulfuric Acid Nitric Acid Method" (HJ/T299-2007), and according to "Determination of Hexavalent Chromium in Water Quality Diphenylcarbazide Spectrophotometry "Method" (GB7467-87) to determine the concentration of hexavalent chromium in the leaching solution, and use flame atomic absorption spectrophotometry to determine the concentration of total chromium in the leaching solution.
实施例1 Example 1
本实施例选取的污染土壤取自山东省济南市某化工厂区内的表层污染土，土壤风干、磨细过100目筛，储存备用。经测定，实施例1所取污染土壤基本性质如表1，其中污染土壤中六价铬的浓度为2655.6mg/kg，浸出液中总铬浓度为179.49mg/L，浸出液中六价铬浓度为119.88mg/L。 The polluted soil selected in this example was taken from the surface polluted soil in a chemical factory area in Jinan City, Shandong Province. The soil was air-dried, ground and passed through a 100-mesh sieve, and stored for future use. After determination, the basic properties of the polluted soil taken in Example 1 are shown in Table 1, wherein the concentration of hexavalent chromium in the polluted soil is 2655.6mg/kg, the total chromium concentration in the leachate is 179.49mg/L, and the hexavalent chromium concentration in the leachate is 119.88 mg/L.
表1土壤基本理化性质 Table 1 Basic physical and chemical properties of soil
取1kg风干的铬污染土壤置于2L的塑料桶中，添加糖蜜和豆饼粉以一定配比组成的微生物营养剂150g，搅拌均匀，调节含水率为38%，隔绝空气，于25℃恒温培养箱中养护21天，既得修复后土壤。其中，上述微生物营养剂中豆饼粉和糖蜜的质量比为1：4，微生物营养剂的碳氮比约23.5:1。 Take 1kg of air-dried chromium-contaminated soil and put it in a 2L plastic bucket, add 150g of microbial nutrition agent composed of molasses and bean cake powder in a certain ratio, stir evenly, adjust the moisture content to 38%, isolate the air, and place in a constant temperature incubator at 25°C Medium-maintenance for 21 days, and the repaired soil will be obtained. Among them, the mass ratio of bean cake powder and molasses in the above-mentioned microbial nutrient is 1:4, and the carbon-nitrogen ratio of the microbial nutrient is about 23.5:1.
经测定，修复后土壤中六价铬的浓度为66.82mg/kg，土壤中六价铬的去除率达97.48%；按照《固体废物浸出毒性浸出方法—硫酸硝酸法》（HJ/T299-2007）制备的浸出液中六价铬的浓度为未检出，总铬的浓度为4.4mg/L，总铬的稳定化效率为97.55%。 It was determined that the concentration of hexavalent chromium in the soil after remediation was 66.82mg/kg, and the removal rate of hexavalent chromium in the soil reached 97.48%; according to the "Solid Waste Leaching Toxic Leaching Method-Sulphuric Nitric Acid Method" (HJ/T299-2007) The concentration of hexavalent chromium in the prepared leachate was not detected, the concentration of total chromium was 4.4mg/L, and the stabilization efficiency of total chromium was 97.55%.
实施例2 Example 2
本实施例中，选取的污染土壤类型、操作步骤及相关测定方法均同实施例1，区别在于：所加微生物营养剂中豆饼粉和糖蜜的质量比为1:9，微生物营养剂的碳氮比约36.16:1，调节含水率为37%。经测定，修复后的土壤中六价铬的浓度为65.43mg/kg，土壤中六价铬的去除率达97.54%；按照《固体废物浸出毒性浸出方法—硫酸硝酸法》（HJ/T299-2007）制备的浸出液中六价铬的浓度为未检出，总铬的浓度为7.33mg/L，总铬的稳定化效率为95.91%。 In this embodiment, the selected polluted soil type, operation steps and related measurement methods are all the same as in Example 1, the difference is that the mass ratio of bean cake powder and molasses in the added microbial nutrient is 1:9, and the carbon and nitrogen content of the microbial nutrient is 1:9. The ratio is about 36.16:1, and the moisture content is adjusted to 37%. It was determined that the concentration of hexavalent chromium in the repaired soil was 65.43mg/kg, and the removal rate of hexavalent chromium in the soil reached 97.54%; ) The concentration of hexavalent chromium in the leachate prepared was not detected, the concentration of total chromium was 7.33mg/L, and the stabilization efficiency of total chromium was 95.91%.
实施例3 Example 3
本实施例选取山东省济南市某化工厂区内一基坑的水下沉积物，风干、磨细过100目筛，储存备用。经测定，实施例3所取沉积物的基本性质如表2，其中沉积物中六价铬的浓度为126.09mg/kg，浸出液中总铬浓度为8.41mg/L，浸出液中六价铬浓度为5.93mg/L。 In this embodiment, the underwater sediments of a foundation pit in a chemical factory area in Jinan City, Shandong Province were selected, air-dried, ground and passed through a 100-mesh sieve, and stored for future use. After measurement, the basic properties of the deposits taken in Example 3 are as shown in Table 2, wherein the concentration of hexavalent chromium in the deposits is 126.09mg/kg, the total chromium concentration in the leach solution is 8.41mg/L, and the concentration of hexavalent chromium in the leach solution is 5.93mg/L.
表2沉积物基本理化性质 Table 2 Basic physical and chemical properties of sediments
取1kg风干的铬污染沉积物置于2L的塑料桶中，添加糖蜜和豆饼粉以一定配比组成的微生物营养剂20g，搅拌均匀，调节含水率为30%，隔绝空气，于25℃恒温培养箱中养护21天，既得修复后沉积物。其中，上述微生物营养剂中豆饼粉和糖蜜的质量比为1：4，微生物营养剂的碳氮比约23.5:1。 Take 1 kg of air-dried chromium-contaminated sediment and put it in a 2L plastic bucket, add 20 g of microbial nutrition agent composed of molasses and bean cake powder in a certain ratio, stir evenly, adjust the moisture content to 30%, isolate the air, and place in a constant temperature incubator at 25 °C After 21 days of medium maintenance, the repaired deposits were obtained. Among them, the mass ratio of bean cake powder and molasses in the above-mentioned microbial nutrient is 1:4, and the carbon-nitrogen ratio of the microbial nutrient is about 23.5:1.
经测定，修复后沉积物中六价铬未检出，按照《固体废物浸出毒性浸出方法—硫酸硝酸法》（HJ/T299-2007）制备的浸出液中六价铬的浓度为未检出，总铬的浓度为0.025mg/L，总铬的稳定化效率为99.7%。 It was determined that hexavalent chromium was not detected in the remediation sediment, and the concentration of hexavalent chromium in the leaching solution prepared in accordance with "Solid Waste Leaching Toxic Leaching Method-Sulphuric Nitric Acid Method" (HJ/T299-2007) was not detected, and the total The concentration of chromium is 0.025mg/L, and the stabilization efficiency of total chromium is 99.7%.
实施例4 Example 4
本实施例中，选取的污染沉积物类型、操作步骤及相关测定方法均同实施例3，区别在于：所加微生物营养剂中豆饼粉和糖蜜的质量比为1:10，微生物营养剂的碳氮比约38.04：1。经测定，修复后的沉积物中六价铬的浓度为4.08mg/kg，土壤中六价铬的去除率达96.77%；按照《固体废物浸出毒性浸出方法—硫酸硝酸法》（HJ/T299-2007）制备的浸出液中六价铬的浓度为未检出，总铬的浓度为0.08mg/L，总铬的稳定化效率为99.05%。 In this embodiment, the selected pollution sediment type, operation steps and related determination methods are all the same as in Example 3, the difference is that the mass ratio of bean cake powder and molasses in the added microbial nutrient is 1:10, and the carbon content of the microbial nutrient is 1:10. The nitrogen ratio is about 38.04:1. It was determined that the concentration of hexavalent chromium in the restored sediment was 4.08mg/kg, and the removal rate of hexavalent chromium in the soil reached 96.77%; 2007) the concentration of hexavalent chromium in the leach solution prepared was not detected, the concentration of total chromium was 0.08mg/L, and the stabilization efficiency of total chromium was 99.05%.
上述一般性说明、实施例只为说明本发明的技术构思及特点，其目的在于让熟悉此领域技术的人士能够了解本发明的内容并加以实施，并不能以此限制本发明的保护范围。凡根据本发明精神实质所作的修改或改进，都应涵盖在本发明的保护范围内。 The above-mentioned general description and examples are only to illustrate the technical concept and characteristics of the present invention, and its purpose is to enable those skilled in the art to understand and implement the content of the present invention, and cannot limit the scope of protection of the present invention. All modifications or improvements made according to the spirit of the present invention shall fall within the protection scope of the present invention.
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