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WO2002040409A1 - A remediatiation method of contaminated materials by using pd/fe bimetalic permeable geosynthetic metal liner for the reactive wall - Google Patents

A remediatiation method of contaminated materials by using pd/fe bimetalic permeable geosynthetic metal liner for the reactive wall Download PDF

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Publication number
WO2002040409A1
WO2002040409A1 PCT/KR2000/001307 KR0001307W WO0240409A1 WO 2002040409 A1 WO2002040409 A1 WO 2002040409A1 KR 0001307 W KR0001307 W KR 0001307W WO 0240409 A1 WO0240409 A1 WO 0240409A1
Authority
WO
WIPO (PCT)
Prior art keywords
reactive wall
palladium
metal liner
reactive
coated
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/KR2000/001307
Other languages
English (en)
French (fr)
Inventor
Jae-Won Lee
Jun-Boum Park
Tae-Sik Kim
Il-Chul Jung
Si-Hyun Kim
Sang-Su Lee
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
GEO WORKS CO Ltd
Halla Engineering & Industrial Development Co Ltd
Original Assignee
GEO WORKS CO Ltd
Halla Engineering & Industrial Development Co Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by GEO WORKS CO Ltd, Halla Engineering & Industrial Development Co Ltd filed Critical GEO WORKS CO Ltd
Priority to PCT/KR2000/001307 priority Critical patent/WO2002040409A1/ko
Priority to JP2002542743A priority patent/JP4041735B2/ja
Publication of WO2002040409A1 publication Critical patent/WO2002040409A1/ko
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

Links

Classifications

    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
    • B09C—RECLAMATION OF CONTAMINATED SOIL
    • B09C1/00—Reclamation of contaminated soil
    • B09C1/08—Reclamation of contaminated soil chemically
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
    • B09C—RECLAMATION OF CONTAMINATED SOIL
    • B09C1/00—Reclamation of contaminated soil
    • B09C1/002—Reclamation of contaminated soil involving in-situ ground water treatment
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/72—Treatment of water, waste water, or sewage by oxidation
    • C02F1/725—Treatment of water, waste water, or sewage by oxidation by catalytic oxidation
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2101/00—Nature of the contaminant
    • C02F2101/30—Organic compounds
    • C02F2101/36—Organic compounds containing halogen
    • C02F2101/363—PCB's; PCP's
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
    • C02F2103/06—Contaminated groundwater or leachate

Definitions

  • the present invention relates to a remediation method of contaminated materials by using reactive wall and, more particularly, to a remediation method of contaminated materials by using reactive wall built under the ground where contaminated materials exist, whereby contaminated materials are eliminated by the chemical reaction of reactive media and contaminated materials induced by hydraulical flow of contaminant band of underground water.
  • the present invention uses flexible reactive wall to reduce the shock load of reacting materials due to the contaminated materials such as various organic materials and floating materials in the underground water, fn the flexible reactive wall, mixture of granular iron on which palladium is coated to directly react with contaminated materials, and soil fills two fold non- woven fabric like sandwich, and crushed non-woven geotextiles are attached.
  • the present invention uses permeable geosynthetic metal liner (PGML) with two metals of palladium and iron which can be applicable to materials such as PCBs which require high redox potential, and can be produced in a large scale.
  • PGML permeable geosynthetic metal liner
  • USP 5,575,927 discloses a method for faster reduction of halogenated hydrocarbon by the use of mixture of iron and ferrous sulfide in relative quantities as reactive media than when either of these materials was used separately.
  • USP 5,543,059 discloses a method for purification by passing contaminated material containing halogenated hydrocarbon through a tiered iron wall or column, comprising at least three zones of granule sizes of iron particles as reactive media.
  • Fig. 1 is a diagram of the process of dechlorination of PCE (C C-U, tetrachloroethylene) and its standard redox potential.
  • PCE C C-U, tetrachloroethylene
  • C indicates the point where the oxidation rate is the highest
  • D the point where it is the lowest.
  • major reductants capable of reacting with organic chlorides are Fe°, Fe 2+ , and H 2 .
  • the reaction is generally achieved by direct electron exchange between Fe° and alkyl chlorides adsorbed on the surface (Formula 2) but the reaction also may occur by Fe 2+ produced from the corrosion (Formula 3), H 2 (Fonnula 4) and H 2 O, etc.
  • Fig. 2 shows the reductive dechlorination of organic chlorides by exchange of electrons in corrosion of Fe°; Fig. 2A showing the reductive reaction of organic chlorides by Fe° which occurs on its surface; Fig. 2B, the reductive reaction of organic chlorides which occurs indirectly by way of ferrous ions; while Fig. 2C shows the role played by
  • the conventional reactive wall methods can only be applicable to the contaminated materials such as PCE, TCE, DCE, NC, CT and the like, but not to the contaminated materials such as PCBs which need high redox potential, because the granular iron has limited redox potential when used without additional treatment or addition of other materials. Furthermore, another problem was that against such contaminated materials which contain organic matters to a high degree, the surface energy of the iron particles used as reactive materials was found insufficient for satisfactory dechlorination. And, when the reactive wall is outworn, the conventional method has the problem of reconstructing the whole reactive wall system.
  • One object of the present invention is to solve problems as mentioned above and to provide reactive wall which can eliminate such material as PCBs that require high energy, and which includes reactive material that has reaction velocity of about 500 ⁇ 1000 times faster than conventional material which uses only granular iron so greatly reducing the thickness of reactive wall to 0.02 ⁇ 0.03 m while conventional reactive wall which uses granular iron of slow reaction velocity requires thickness of about 1 m to eliminate materials such as PCE, TCE, DCE, NC and CT.
  • Another object of the present invention is to provide flexible reactive wall to reduce the shock load of reacting materials due to the contaminated materials such as various organic materials and floating materials in the underground water.
  • this flexible reactive wall mixture of granular iron on which palladium is coated to directly react with contaminated materials, and soil fills two fold non-woven fabric like sandwich, and crushed non- oven fabrics are attached.
  • the remediation method of contaminated materials by using Pd/Fe bimetalic permeable geosynthetic metal liner for the reactive wall of the present invention comprises the steps of preparing a permeable geosynthetic metal liner (PGML) for the reactive wall wherein non-woven geotextiles with crashed blast furnace slag attached thereon are adhered on both sides of reactive wall materials including mixture of iron which is coated with palladium which directly react with contaminant and soil, and installing the reactive wall at the area where contaminated materials pass, and eliminating contaminant by passing contaminated materials through the reactive wall.
  • PGML permeable geosynthetic metal liner
  • the palladium which is used in the remediation method of contaminated materials by using Pd/Fe bimetalic permeable geosynthetic metal liner for the reactive wall of the present invention, is a metal which has atomic weight of 106.42 amu, melting point of
  • the palladium is used as a catalyst to maximize the effect of the reductive dechlorination of organic chlorides.
  • the palladium-coated bimetal iron can be produced by putting 5,000 wt parts of Fe into a solution which includes 10 wt parts of potassium hexachloropalladate (K PdCl 6 ) and 90 wt parts of water and by having the surface of Fe coated with palladium until its orange color turns bright yellow. The following formula (1) shows this coating process.
  • the reactivity can be increased up to 500 ⁇ 1,000 times higher by using above mentioned palladium-coated iron, than that of the conventional method using elemental iron because the palladium/iron bimetal of the present invention undergoes zero order reaction rather than 1 st order reaction of the conventional elemental iron.
  • Figs. 3 and 4 illustrate one example of the permeable geosynthetic metal liner used in the remediation method of contaminated materials by using Pd/Fe bimetalic permeable geosynthetic metal liner for the reactive wall of the present invention.
  • Fig. 3 illustrates one example of the permeable geosynthetic metal liner of steel wool type.
  • non-woven geotextiles 20 are adhered on both sides of reactive wall materials including Pd/Fe bimetal which directly react with the contaminant.
  • the non-woven geotextile 20 of the present invention is adhered to reduce the shock load of reacting materials due to the contaminated materials.
  • Crashed blast furnace slag which is a byproduct of steelmaking process in the steel industry and is very cheap and has excellent absorption characteristics, can be attached on the non- woven geotextile 20.
  • Steelwool 10 coated with palladium is used as Pd/Fe bimetal.
  • Fig. 4 illustrates one example of the permeable geosynthetic metal liner of granular iron type.
  • granular iron 30 coated with palladium is used as Pd/Fe bimetal.
  • iron of steelwool type since the strength of reactive media can be maintained against twist of the ground, and when contaminated ground is composed mainly of sandy soil it is desirable to use granular iron type.
  • Both type of iron is coated with palladium as a catalyst.
  • the present invention attaches, on both sides of reactive wall materials, non-woven geotextiles with crashed blast furnace slag, which is a byproduct of steehnaking process in the steel industry and is very cheap and has excellent absorption characteristics of the floating materials, nutrient salts and heavy metals, attached thereon in order to prevent the lowering of effectiveness of reaction of reactive media composed of Pd/Fe bimetal due to the introduction of impurities into the system.
  • the absorption characteristics of the nutrient salts by blast furnace slag can be shown from Figs. 5 and 6. Figs.
  • blast furnace slag has excellent absorption characteristics on the floating materials, nutrient salts and heavy metals, and is appropriate for eliminating these materials by absorption.
  • the content of nanometer scale iron coated with palladium of the present invention is preferably 5 ⁇ 20 wt% and most favorably 20 wt% of the whole reactive materials. If the content is larger than 20 wt%, the permeability of the reactive wall is lowered, reducing the effectiveness of remediation of contaminated materials. And if the content is smaller than 5 wt%, the amount of palladium coated iron becomes too small, also reducing the effectiveness of remediation of contaminated materials.
  • the permeable geosynthetic metal liner (PGML) for the reactive wall with Pd Fe bimetal can be made in any form and can be made in a certain standard to be made in a large scale installed at the site easily.
  • the method of the present invention can be applicable to contaminated materials of organic compounds such as PCE(C 2 Cl4 . tetrachloroethylene), TCE(C 2 HC1 3 , trichloroethylene), DCE(C 2 H 2 C1 2 , dichloroethylene), NC(C 2 H 3 C1, vinyl chloride),
  • organic compounds such as PCE(C 2 Cl4 . tetrachloroethylene), TCE(C 2 HC1 3 , trichloroethylene), DCE(C 2 H 2 C1 2 , dichloroethylene), NC(C 2 H 3 C1, vinyl chloride),
  • These organic compounds are converted into harmless materials such as ethane through reductive dehalogenation reaction which replaces Cl " ion with H " ion by the electron generated by corrosion process of Fe°.
  • the palladium coated iron used in the present invention as reactive material is much more reactive than the conventional reactive wall system using only soil and Fe°, the thickness of the reactive wall can be reduced. Also, by using the method of the present invention, organic chloride such as PCBs which requires high dechlorination energy can be effectively eliminated.
  • the permeable geosynthetic metal liner (PGML) for the reactive wall with Pd/Fe bimetal can be made in a predetermined form, it can be standardized and can be made in a large scale and easily installed at the site.
  • Fig. 1 illustrates the process of dechlorination of PCE and the standard redox potential
  • Fig. 2A is a drawing to show the reductive reaction of an organic chloride directly taking place by virtue of elemental iron over its surface;
  • Fig. 2B illustrates the role of elemental iron in a reductive reaction of an organic chloride indirectly taking place by virtue of ferrous ion
  • Fig. 2C illustrates the role of elemental iron in a reductive reaction of an organic chloride by H 2 in the presence of catalyst
  • Fig. 3 illustrates one example of the permeable geosynthetic metal liner of steel wool type
  • Fig. 4 illustrates one example of the permeable geosynthetic metal liner of granular iron type
  • Fig. 5 shows the change of concentration of TCE after passing the 100 ⁇ M solution of TCE through the reactive wall of Pd/Fe bimetalic permeable geosynthetic metal liner
  • Fig. 6A is a chromatogram of the components of congener of 20 ppm PCB(arochlor- 1254);
  • Figs. 6B and 6C are chromatograms of the components of PCBs after passing 20 ppm solution of PCBs through the reactive wall of Pd/Fe bimetalic permeable geosynthetic metal liner of example 2 for 10 and 24 hours respectively;
  • Fig. 7 shows the change of concentration of PCE after passing 100 ⁇ M solution of
  • Pd/Fe bimetalic permeable geosynthetic metal liner which includes palladium coated granular iron and normal granular iron;
  • Fig. 8 shows the change of concentration of TCE after passing 100 ⁇ M. solution of TCE through the reactive wall of Pd/Fe bimetalic permeable geosynthetic metal liner which includes palladium coated granular iron and normal granular iron;
  • Fig. 9 shows the change of concentration of ammonia when the solution of ammonia with initial solution of 20mg/l is in equilibrium with blast furnace slag.
  • Fig. 10 shows the change of concentration of phosphate when the solution of phosphate with initial solution of 500mg/l is in equilibrium with blast furnace slag.
  • the reactive wall of Pd Fe bimetalic permeable geosynthetic metal liner is installed with breadth lm, length 0.5m and thickness 0.005m, and solutions of lOOi/M of TCE and 20 ppm of PCBs(Arochlor-1254) are passed through the reactive wall.
  • the effect of the remediation method of contaminated materials by using Pd/Fe bimetalic permeable geosynthetic metal liner for the reactive wall of the present invention is evaluated by measuring the concentration of TCE and PCBs of the passed solution as time goes by.
  • the content of palladium coated iron in the metal liner of this example is 20wt%.
  • the hydraulic conductivity of the reactive wall of Pd/Fe bimetalic permeable geosynthetic metal liner is measured as 5cm/hr, and the hydraulic gradient 1/50.
  • Darcy flow velocity calculated from above data is O.lcm/hr and maximum velocity of the underground water is set as lcm hr which is 10 times the above flow velocity.
  • the solution of 100 /M TCE used in this example is prepared by stirring for 12 hours in zero headspace state by using 0.61 of Teflon gas sampling bag (Alltech, USA). Also, the solution of 20mg/l PCBs is mixed with 1 ml of Arochlor-1254 (lOOi/g/ml methanol, ACS reagent, 99.8%+, Sigma, USA) and 3ml of 20% methanol solution, and 1 ml of acetone (ACS reagent, 99.8%+, Sigma, USA) is added to the solution for complete dissolution of Arochlor-1254. The ratio of concentration of methanol/water/acetone is 1 : 3: l(v/v/v).
  • the concentration of TCE used in this example is analyzed by using gas chromatography (6890 series, Hewlett Packard Co, USA). The condition for gas chromatography is shown in Table 1.
  • the concentration of Arochlor-1254 used in this example is analyzed by using gas chromatography (6890 series, Hewlett Packard Co, USA) according to the extraction method of hexane (reagent grade, showa chem., Japan).
  • the condition for gas chromatography is shown in Table 2. Table 2. condition for gas chromatography
  • Figs. 7 and 8 show the results of this example.
  • Fig. 7 shows the change of concentration of TCE after passing 100 ⁇ M solution of TCE through the reactive wall of Pd/Fe bimetalic permeable geosynthetic metal liner which includes palladium coated iron.
  • the reactive wall of steelwool type is lower in effectiveness than the reactive wall of granular iron type. From this result it can be directly confirmed that the mechanism of remediation is closely related with the size of reactive materials.
  • Fig. 8 shows the change of concentration of PCBs after passing 20ppm solution of PCBs through the reactive wall of Pd/Fe bimetalic permeable geosynthetic metal liner which includes palladium coated iron. As shown in the figure, it can be known from the relative peak area of PCBs, namely the concentration of PCBs remaining in the solution, that most PCBs in the solution are eliminated after 24 hours.
  • Fig. 8 A in Fig. 8 illustrates the peak area of each single element of 20ppm PCBs (arochlor-1254) congener.
  • 8C illustrate the peak area of each single element of PCBs after passing solution of 20ppm PCBs (arochlor-1254) congener through the reactive wall of Pd/Fe bimetalic permeable geosynthetic metal liner for 10 and 24 hours.
  • example 2 The purpose of example 2 is to compare the reaction velocity of Pd/Fe bimetalic permeable geosynthetic metal liner which uses palladium coated iron as a reactive material, and conventional permeable geosynthetic metal liner which uses elemental iron Fe° as a reactive material.
  • Pd/Fe bimetalic permeable geosynthetic metal liner which uses palladium coated iron as a reactive material
  • conventional permeable geosynthetic metal liner which uses elemental iron Fe as a reactive material
  • PCE and TCE of 100 ⁇ M are passed through each of two metal liners, and the concentration is measured after predetermined time.
  • Figs. 9 and 10 show the change of concentration of PCE in this example and Fig. 10 shows the change of concentration of TCE in this example.
  • initial lOOi M of PCE is reduced to 28.8 /M after 50 hours in the case of onventional permeable geosynthetic metal liner showing elimination of 71.2%, while the concentration is reduced to 5.44 /M after 0.017 hours in the case of Pd/Fe bimetalic permeable geosynthetic metal liner showing elimination of 94.5%.
  • initial 100 . / of TCE is reduced to
  • the present invention relates to environmental industries, and especially to land environmental industries, thus being applicable to industrial estates and military facilities such as underground oil storage facilities, semi-conductor plants, areas of heaving populated with plants, petrochemical engineering facilities, etc. for instance.

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  • Life Sciences & Earth Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Environmental & Geological Engineering (AREA)
  • Chemical & Material Sciences (AREA)
  • Hydrology & Water Resources (AREA)
  • Water Supply & Treatment (AREA)
  • Soil Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Organic Chemistry (AREA)
  • Fire-Extinguishing Compositions (AREA)
  • Treatment Of Water By Oxidation Or Reduction (AREA)
  • Processing Of Solid Wastes (AREA)

Abstract

The present invention relates to the remediation method of the contaminated materials by using the reactive barriers ,which is comprised of the following steps; (i) preparing the reactive barriers containing palladium coated iron as reactive component and then establishing this reactive barriers at the place where the contaminated materials are passing through; (ii) eliminating the contaminating components from the contaminated materials by passing the contaminated materials through the reactive barriers. According to this invention the chlorinated organocompounds which needs a higher energy to dechlorinate can be effectively eliminated from the contaminated materials.
PCT/KR2000/001307 2000-11-16 2000-11-16 A remediatiation method of contaminated materials by using pd/fe bimetalic permeable geosynthetic metal liner for the reactive wall Ceased WO2002040409A1 (ko)

Priority Applications (2)

Application Number Priority Date Filing Date Title
PCT/KR2000/001307 WO2002040409A1 (ko) 2000-11-16 2000-11-16 A remediatiation method of contaminated materials by using pd/fe bimetalic permeable geosynthetic metal liner for the reactive wall
JP2002542743A JP4041735B2 (ja) 2000-11-16 2000-11-16 反応壁にＰｄ／Ｆｅ二元金属の透過性ジオシンセティックメタルシートを使用する汚染物質の浄化方法

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PCT/KR2000/001307 WO2002040409A1 (ko) 2000-11-16 2000-11-16 A remediatiation method of contaminated materials by using pd/fe bimetalic permeable geosynthetic metal liner for the reactive wall

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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR100380549B1 (ko) * 2000-11-16 2003-04-26 한라산업개발 주식회사 팔라듐/철 이원금속의 투과성 지합성 메탈라이너를 이용한오염물의 정화방법
WO2007136757A3 (en) * 2006-05-19 2008-01-10 Usa As Represented By The Admi Mechanical alloying of a hydrogenation catalyst used for the remediation of contaminated compounds
US8163972B2 (en) 2005-08-11 2012-04-24 The United States Of America As Represented By The Administrator Of The National Aeronautics And Space Administration Zero-valent metallic treatment system and its application for removal and remediation of polychlorinated biphenyls (PCBs)

Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5543059A (en) * 1995-03-31 1996-08-06 General Electric Company Enhanced reactive metal wall for dehalogenation of hydrocarbons
US5575927A (en) * 1995-07-06 1996-11-19 General Electric Company Method for destruction of halogenated hydrocarbons

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5543059A (en) * 1995-03-31 1996-08-06 General Electric Company Enhanced reactive metal wall for dehalogenation of hydrocarbons
US5575927A (en) * 1995-07-06 1996-11-19 General Electric Company Method for destruction of halogenated hydrocarbons

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR100380549B1 (ko) * 2000-11-16 2003-04-26 한라산업개발 주식회사 팔라듐/철 이원금속의 투과성 지합성 메탈라이너를 이용한오염물의 정화방법
US8163972B2 (en) 2005-08-11 2012-04-24 The United States Of America As Represented By The Administrator Of The National Aeronautics And Space Administration Zero-valent metallic treatment system and its application for removal and remediation of polychlorinated biphenyls (PCBs)
WO2007136757A3 (en) * 2006-05-19 2008-01-10 Usa As Represented By The Admi Mechanical alloying of a hydrogenation catalyst used for the remediation of contaminated compounds
US7842639B2 (en) 2006-05-19 2010-11-30 The United States Of America As Represented By The Administrator Of The National Aeronautics And Space Administration Mechanical alloying of a hydrogenation catalyst used for the remediation of contaminated compounds
US8288307B2 (en) 2006-05-19 2012-10-16 The United States Of America As Represented By The Administrator Of The National Aeronautics And Space Administration Mechanical alloying of a hydrogenation catalyst used for the remediation of contaminated compounds

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Publication number Publication date
JP4041735B2 (ja) 2008-01-30
JP2004529745A (ja) 2004-09-30

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