CN106083224A - The method using carbon nanomaterial regulation and control compost extraction heavy metal adsorption - Google Patents
The method using carbon nanomaterial regulation and control compost extraction heavy metal adsorption Download PDFInfo
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- CN106083224A CN106083224A CN201610442900.0A CN201610442900A CN106083224A CN 106083224 A CN106083224 A CN 106083224A CN 201610442900 A CN201610442900 A CN 201610442900A CN 106083224 A CN106083224 A CN 106083224A
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Classifications
-
- C—CHEMISTRY; METALLURGY
- C05—FERTILISERS; MANUFACTURE THEREOF
- C05F—ORGANIC FERTILISERS NOT COVERED BY SUBCLASSES C05B, C05C, e.g. FERTILISERS FROM WASTE OR REFUSE
- C05F9/00—Fertilisers from household or town refuse
- C05F9/04—Biological compost
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/20—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising free carbon; comprising carbon obtained by carbonising processes
- B01J20/205—Carbon nanostructures, e.g. nanotubes, nanohorns, nanocones, nanoballs
-
- G—PHYSICS
- G06—COMPUTING; CALCULATING OR COUNTING
- G06Q—INFORMATION AND COMMUNICATION TECHNOLOGY [ICT] SPECIALLY ADAPTED FOR ADMINISTRATIVE, COMMERCIAL, FINANCIAL, MANAGERIAL OR SUPERVISORY PURPOSES; SYSTEMS OR METHODS SPECIALLY ADAPTED FOR ADMINISTRATIVE, COMMERCIAL, FINANCIAL, MANAGERIAL OR SUPERVISORY PURPOSES, NOT OTHERWISE PROVIDED FOR
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- G16C20/70—Machine learning, data mining or chemometrics
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- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A40/00—Adaptation technologies in agriculture, forestry, livestock or agroalimentary production
- Y02A40/10—Adaptation technologies in agriculture, forestry, livestock or agroalimentary production in agriculture
- Y02A40/20—Fertilizers of biological origin, e.g. guano or fertilizers made from animal corpses
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Abstract
The invention discloses the method using carbon nanomaterial regulation and control compost extraction heavy metal adsorption, it is that preparation is containing Cu2+、Pb2+、Cd2+The mixed solution of three heavy metal species ions, its concentration is than for 6:4:1；The heavy metal mixed solution of configuration is mixed for 1:2 in mass ratio with compost extraction；Weigh in 10mg carbon nanomaterial and conical flask, in conical flask, add compost extraction 20 ml of heavy metal mixed solution 20 ml or simple respectively, be measured after filtering after 6 h that vibrate.The present invention further discloses the method using carbon nanomaterial regulation and control compost extraction heavy metal adsorption application in terms of improving the adsorption rate of heavy metal.Wherein the adsorption rate of heavy metal refers to: the absorption to Cd, Cu, Pb of Graphene, graphene oxide, multi-walled carbon nano-tubes.
Description
Technical field
The invention belongs to environmental protection technical field, relate to a kind of employing carbon nanomaterial regulation and control compost extraction heavy metal
The method of absorption.
Background technology
House refuse refers mainly to the solid waste produced in resident's daily life, production.Whole world house refuse is from 2005
51% will be increased to 2025.China's house refuse grows beyond 15% every year, and whole nation sanitary fill adds up appropriation of land more than 500,000,000
Square metre.By 2015, the house refuse annual production of our urban is anticipated will be more than 10,000,000 tons.House refuse physics becomes
The Organic substances such as inorganic matter and plant, fiber, plastics, paper such as distribution predominantly glass, brick and tile, cinder dirt, wherein can heap corruption
Thing accounts for more than 30%.Chemical composition is mainly moisture, N, P, K, organic matter etc., and some areas garbage water content exceedes
50%。
The most conventional life refuse processing method mainly has sanitary landfills, burning and During High-Temperature Composting.Sanitary landfills becomes
For being mostly the main method of city process house refuse.But sanitary landfills occupies a large amount of land used, along with the house refuse daily output
Improving year by year, garbage-surrounded city phenomenon is further serious, and the Leachate site that the higher direct heap buried of rubbish of moisture content produces is more, its
In containing more harmful substance, and produce a large amount of greenhouse gases, easily cause secondary pollution.Burning disposal makes combustiblerefuse fire
Burning is converted into residue, reduces garbage loading embeading amount, and high-temp combustion kills pathogen therein and bacterial parasite, and the heat energy of generation can
Generate electricity for heat supply.But burning partial contamination thing by solid state transformed as gaseous state, tail gas contains the polluter of complexity, especially can
Produce dioxin extremely toxic substance, have the strongest anelasticity in the environment.Compost treatment refers to by microorganism certain artificial
Under the conditions of, the Organic substance in fermentative degradation rubbish forms the process of stable humus, is a kind of resource, stabilisation, harmless
The solidification disposal of waste mode changed.House refuse is after composting, rich in nutrients such as organic matter, nitrogen, phosphorus, and harmless treatment
After can improve soil environment as fertilizer, have a preferable application prospect, simultaneously also it is noted that consumer garbage compost is also deposited
The higher equivalent risk of content of beary metal wherein.Each processing mode requires that the composition of rubbish is different, and single-mode processes cannot
Realize real innoxious.Use multiple processing method to combine for rubbish difference main constituent, become present garbage disposal
Trend of the times.
Containing the nutrient substance needed for abundant organic matter and plant growing in garbage compost.Research shows, life rubbish
Organic substance in rubbish compost, N, K, content of lignin are higher, add in soil using compost as fertilizer, it is possible to increase soil is fertile
Power, increase water retention in soil, improve soil physicochemical property, promote plant growing, improve crop yield.There are some researches show,
Farmland castoff compost and chemical fertilizer respectively and are manured into soil, and plant Caulis et Folium Brassicae capitatae, the upgrowth situation of contrast crop, number of pest
And economic benefit etc..Result shows, although apply to number of pest in the soil of compost the twice being to apply chemical fertilizer, but,
Economic benefit is its 3 times.Zhang Chunying[21]After different proportion composting compost and original soil, add the garbage compost of 5% ~ 20%
Organic matter, rapid available phosphorus and total nitrogen content can be significantly improved, increase flowers above and below ground dry weight；Wherein, when adding 10% compost,
Underground dry weight is 3.61 times of comparison.Research shows, utilizes compost to plant Herba Cichorii after improving soil, and the fertility of soil significantly increases
Adding, Herba Cichorii is significantly increased production.Tang Shaojie is crop rotation winter wheat and summer corn on the soil apply compost, crop applying house refuse heap
After fertilizer, corn yield increasing rate substantially increases, and reaches 43.4%, and in wheat increase yield rate 2008 year, 2009 years were respectively 53.6% He
99.2%.Research shows, uses compost and can improve the carbon-nitrogen ratio in soil in sand, increases P, K, Mg content, and
It is of value to increase agron.But, even if the compost from industrial occupancy applies on a small quantity, the aobvious of content of beary metal also can be caused
Write and increase.Discounting for the impact of heavy metal, add compost and can significantly improve soil quality.
China's consumer garbage compost is affected by the indefinite factor of source refuse classification, mixes electricity in house refuse
Pond, electronic equipments etc. are rich in the material of heavy metal.Li Qiwei etc. research show, house refuse after compost treatment, heavy metal
Total amount change is inconspicuous, and wherein the elemental stable state content such as Hg, Pb, Cr rises.Waiting research quietly shows, Pb, Cd, Zn are at compost
During by other forms to Fe-Mn combined state convert, but due in composting process pH reduce, the biologically effective of Pb, Cu, Zn
State is slightly increased.Use consumer garbage compost and can increase heavy metal in soil content, meanwhile add heavy metal in soil
Transfer in plant, thus bring certain ecological risk.Shao Huawei research applies each device of Semen Maydis after consumer garbage compost
The rule of official's heavy metal distribution is: root > stem > leaf > seed, result shows that the nutrient content in continuous 3 years fertilized soil improves, but
Being that content of beary metal also accumulates, wherein Cd content is 0.416 mg kg-1, Pb is 21.6 mg kg-1, temporarily will not in 3 years
Cause heavy metal pollution of soil.Similar result has been arrived in the research of Ge Chunhui, after using garbage compost, and the organic matter of soil and speed
Effect Nutrient compost content increases and increases, but, negative effect is that content of beary metal increases simultaneously therewith, Cr, Cd in seed
Amplification reach 38.6% ~ 450%, although have not exceeded national standard, but life-time service need monitoring further.As can be seen here, execute
Improve heavy metal content in soil with consumer garbage compost to a certain extent, and then increase long-term cropping in-vivo heavy metal content,
Compost is agricultural can increase soil fertility in a short time, but uses needs monitoring in time for many years.
Producing fertilizer from refuse in daily life application in turf establishment system, has important ecological significance.Lawn is as city
The key component of city's Urban Greening, provides the place of amusement and recreation to urbanite.The green grassland of high-quality can be had,
It it is one of the important criterion of urban modernization.Urban afforestation land used mostly is removal ground, old city or building site etc., soil now
Matter poor shortage fertility, tradition turf establishment uses entirety to lay roll of sod, consumes substantial amounts of high-quality farmland.Lawn fertilising can
Effectively to improve turf quality, supplement nutrient to lawn in time and can improve EDTA-Fe, after adding compost, grass can be improved
The germination percentage of level ground plant.Compost, to lawn plant is ecological and qualitative character has a significant impact, can improve the life of turfgrass after interpolation
Thing amount, promotes growth；And accelerate plant to turn green, the density of Second Year plant, quality, cover degree etc. are all had facilitation.Have
Research shows, adds the compost of 12.5%, it is possible to significantly improve turf quality in Indigofera pseudotinctoria turf establishment, promotes the growth of root leaf,
Garbage compost can be obviously improved soil, improve fertilizer efficiency, increases nutrient content in soil.Additionally, compost can be as without soil grass
Scytoblastema matter.Consumer garbage compost and beanstalk stalk are made composite interstitial substance, under the low proportioning joining beanstalk, seed germination, on the ground list
Strain net photosynthesis amount and chlorophyll are improved, it is possible to use compost and beanstalk stalk composite interstitial substance substitute soil lawn planting.Not
Planting Festuca Arundinacea with the consumer garbage compost of particle diameter, result shows, the consumer garbage compost of small particle (300-600nm) can carry
The chlorophyll content of high Festuca Arundinacea, and promote the growth of root, and arid injury can be alleviated under water stress, improve anti-
Drought.For microorganism and soil animal, add compost and can suppress lawn pathogen, not only can reduce lawn disease,
And slow down the Drug resistance on lawn.After adding compost, in the built-in value system of lawn, the dominant genera of soil nematodes there occurs change, presses down
The growth and breeding of phytotrophy monoid processed, has created good environment for lawn growth.
Consumer garbage compost is used for that turf establishment system can effectively improve the organic matter of soil, nutrient substance contains
Amount, and the heavy metal of lawn plant enrichment is not along food web enrichment, enters the healthy risk of harm and reduces.But, long
Phase uses the accumulation of heavy metal-polluted soil still can not little to peep, additionally, heavy metal in soil is migrated downward into by soil leaching,
Cause subsoil water heavy metal pollution.Reduce Heavy Metal Pollution in compost and will provide broader sky to the rational utilization of compost
Between.
Most of heavy metals are transitional elements.In soil environment, heavy metal can occur oxidoreduction in certain amplitude
Reaction, the heavy metal of different valence state has different activity and toxicity.Heavy metal pollution of soil has that scope is wide, the persistent period
Long, disguised strong, by features such as food chain enrichment, big, the irreversibilities of difficulty of governance.Large number of biological is analyzed and toxicological study table
Bright, the Transport And Transformation process of the biological activity of heavy metal element, toxicity and heavy metal and its existence in the environment in environment
Morphology is correlated with.Therefore rely only on total metals and be difficult to show the contamination characteristics of heavy metal.
Heavy metal forms different chemical forms in soil, is easily adsorbed by soil media.But the shadow at various factors
Under sound, heavy metal can occur to migrate and conversion.Heavy metal migration in soil is a sufficiently complex process, is that physics moves
Shifting, physicochemical migration and three kinds of coefficient results of migration pattern of biogenic migration, result in heavy metal and migrate in soil
Be difficult to predictability.
In absorption research, adsorbance is critically important physical quantity.At a constant temperature, adsorbance and solution equilibria concentration
Relation curve be referred to as adsorption isotherm.Adsorbate and adsorbent is it will be seen that by the shape of adsorption isotherm and Changing Pattern
Effect power, the state of adsorbed on interfaces matter and adsorbed layer structure.
Solute in aqueous solution adsorbent surface Isothermal Adsorption Characteristics generally with Langmuir model,
Freundlich model describes, and below both model will be discussed in detail.Langmuir proposes monolayer first and inhales
Attached model.
Langmuir model is to assume according to the monolayer adsorption that gas-solid two is alternate and draw, and each suction in model
Attached room energy is identical, and adjacent adsorbent is intermolecular without interaction force.It is that monolayer is inhaled that Freundlich adsoption equation does not limit
Attached, can be used for uneven surface situation, be comparatively ideal experience isothermal adsorpting equation, in narrow concentration range, many
System meets model the most very much.The research such as Wang obtains Linesless charcoal to the absorption of Cd and Langmuir model, Freundlich model
Degree of fitting is preferable, R2Value is respectively 0.993 and 0.989.Cheng Jiemin etc. study discovery, Cu and Cd is at modified Nano carbon blacksurface
Reparation can be divided into two stages of speed, all can be with Langmuir model, Freundlich models fitting.Farghali etc. study
Show CoFe2O4Modifying oxidoreduction Graphene, the adsorption process to C.I. 42590 is physical absorption, meets Lang Gemiaoer isothermal bent
Line.This model is commonly used to explain that the situation of monolayer adsorption, custom are used for calculating maximal absorptive capacity.Wang etc. find oxidation
Graphene meets Lang Gemiaoer adsorption isothermal curve to the adsorption process of Zn, and maximal absorptive capacity is 246mg/g.Moreno etc. study
Show that repair process and the Lang Gemiaoer adsorption isothermal curve of activated carbon adsorption Cd and Pb have preferable degree of fitting.Deng etc. grind
Study carefully functionalization graphene the highest to Cd and Pb adsorption process and Langmuir model, Freundlich model-fitting degree, R2Value
Both greater than 0.9.Freundlich model is the most suitable as an experience adsorption isotherm of uneven surface.
The approach that artificial repairing heavy metal in soil pollutes can be summarized as 3 kinds: removes the heavy metal in soil, mainly with new soil
The methods such as displacement, plant extract；Heavy metal is polluted and is isolated；Change heavy metal existing forms, reduce its animal migration and
Bioavailability, to such an extent as to can be present in steadily in the long term in soil, it is main generation with fixation in situ and microorganism remediation
Table.
Heavy-metal contaminated soil fixation in situ reparation has irreplaceable effect in contaminated soil governance process.At soil
Earth adds different allogenic material, is changed the chemical form of heavy metal by series reaction, reduce its animal migration and biology has
Effect property, reduces heavy metallic poison and migrates accumulation.Conventional soil remediation material mainly has zeolite, Vermiculitum, Calx, phosphorus ore, stove
The inorganic matters such as slag, green manure, Organic substance and part rich in carbon content can be used for the nano material of repairing heavy metal pollution.Wu Lie
Kind grade carries out Rapid deactivation process to the heavy metal in contaminated soil, according to the passivation ability value of stabilization efficiency and passivator to respectively
The passivation ability of passivator and compounded combination carries out strong and weak sequence and understands lime inactivating ability value maximum, and liming can reduce soil
The bioavailability of Cu, Zn, As, Hg, Cd, Pb in earth.Flying dust has stronger absorption property to Zn and Pb in soil.Yin Fei
By applying 4 kinds of passivator respectively to heavy-metal composite pollution soil, exchangeable species and carbonate knot after the process of slag, ground phosphate rock
Closing state Zn content to significantly reduce, slag, ground phosphate rock can dramatically increase residual form Cu content, biological difficult absorption after adding ground phosphate rock
Calcium type arsenic content dramatically increases；Wherein, Linesless charcoal and Paligorskite are mainly based on passivation absorption and complexation, slag and the phosphorus of heavy metal
The repair mechanism of breeze heavy metal is mainly based on chemical precipitation.Repair after utilizing graininess slag and MgO to be mixed in proportion
Soil, slag heavy metal has good absorption property, it is possible to be effectively improved the soil of heavy metal and organic contamination.Soares
Etc. Pb and Zn utilized in eggshell compost absorption soil, after interpolation, it is possible to increase soil pH value, reduce exchangeable species Pb in soil
And Zn, it is possible to effectively repairing heavy metal in soil.Utilize the combine d bioremediation soil such as the carbon rich material matter such as green manure, fertilizer compost and mineral acid
Earth, can effectively reduce As and the Cu pollution to soil.Paper mill sludge and soil interaction can form new adsorption site, have
Help Zn fixing in soil, improve soil quality and reduce content of beary metal in effusion.Shaheen utilizes inorganic matter: boiling
Stone, AlO, MnO and carbonate and organic amendment: the Cu in activated carbon, oil plant remnants compost fixing soil maize planting.Knot
Fruit shows, after adding soil-repairing agent, in Corn, Cu content reduces, and organic amendment effect is better than inorganic amendment, wherein
Activated carbon is preferable with AlO effect.
Charcoal has that porosity is high, specific surface area is big, surface active groups many can adsorb a large amount of exchangeable species sun from
Son.It is to Cd2+Adsorbance first rise with the increase of pH and decline afterwards, be a kind of good adsorbing material, and increase soil and have
Machine matter, promotes crop yield.After biological carbon and mixing with soil, in soil, the toxicity of Cd, Zn and Pb is along with the increase of charcoal content
And reduce, in filter liquor, heavy metal toxicity reduces over time.Qihong Zhu etc. utilizes biological carbon repairing heavy metal pollution
Rice soil, when applied amount is 0.5%, exchangeable species Cr in soil, Ni, Cu, Pb, Zn and Cd content have dropped 18.8 respectively,
29.6,26.3,23.0,23.01 and 48.14%, in Oryza sativa L., Zn, Cd, Pb content decreases 10.96,8.89 and 8.33%.
Almaroai et al. compared for adding maize planting after charcoal, Os Bovis seu Bubali and eggshell in soil, analyzes the biology of Pb in soil
Effectiveness, research shows, after adding charcoal, in Semen Maydis branch and leaf, Pb content reduces.Liu Jingjing studies different types of charcoal
The repair response of heavy metal contaminated soil, tries soil sample with the rice soil of combined pollution for confession and uses the charcoal of different-grain diameter,
The interpolation of Caulis et Folium Oryzae charcoal significantly improves soil pH value, and acid solvent Cu, Cd and Zn convert to reduction-state and oxidable state.Apply
Charcoal can change soil enzyme activities, and wherein urase and peroxidase activity significantly improve, but activity of acid phosphatase
Reduce.
Carbon nanomaterial is the ingredient that field of nanometer material technology is important, mainly includes CNT, fullerene, Graphene
And derivant etc..Graphene (graphene, GE) is that a kind of carbon atom by sp2 hydridization is formed with hexagonal array
Periodic cellular shape two dimension carbonaceous new material, has the physico-chemical property of uniqueness.2004, Univ Manchester UK's physics and
Geim and Novoselov of astronomy system etc. peel off graphite crystal with adhesive tape and obtain Graphene first, and thereby is achieved
Nobel Prize in physics in 2010.Common preparation method mainly has micromechanics stripping method, chemical vapour deposition technique, crystalline epitaxial
Growth method, soliquid method etc..The specific surface area that Graphene is huge makes it high-quality adsorbent, and its adsorption operations letter
Just, the advantage such as high treating effect is widely used in aqueous environment pollution amelioration, primary attachment two pollutant: Organic substance and nothing
Machine anion.
Graphene oxide (graphene oxide, GO) is typically by graphite through chemical oxidation, ultrasonic prepares, oxygen
Functionalized graphene is easy to large-scale production.At present the conventional graphite oxidation method of report mainly have Brodie method,
Standenmaier method and Hummers method.Meanwhile, to have substantial amounts of hydroxyl, carboxyl, epoxy radicals etc. oxygen-containing for graphene oxide
Group, is a kind of hydroaropic substance, can be fixedly combined formation complex by the effect of functional group and other polymer.Cause
This, graphene oxide is highly suitable for application during water processes and removes the metal in water and organic pollution.
CNT is that graphite galvanized hexagonal wire mesh plane is rolled into the single-layer tubular material of seamless tubular or is wrapped in interior, layer by layer
The multilamellar " tube-like materials " of intussusception.CNT is divided into SWCN (SWNTs) and multi-walled carbon nano-tubes
(MWNTs).The diameter of SWCN is substantially between 0.4～2.5nm, and length is up to a few micrometers；Multi-walled carbon nano-tubes by
Multiple coaxial SWNTs form, and the number of plies can be between two-layer to tens layers, and distance 0.34nm between layers, diameter is permissible
Reach about 100nm.MWNTs specific surface is lower slightly, owing to there is more defect on MWNTs tube wall, thus has higher change
Learn activity.CNT contains abundant nanoaperture structure and huge specific surface area, and architectural feature determines its physics, chemistry
Character, is mainly manifested in it and has excellent absorbability, special electrical and mechanical character, and have excellent energy of adsorption
Power.
Graphene, graphene oxide and CNT are due to the surface texture of its uniqueness, huge specific surface area so that it is tool
There is the strongest absorbability, Organic substance, inorganic matter are all shown stronger absorption property.Numerous studies show, carbon nanometer material
Material is used for adsorbing organic contamination and has good adsorption effect, utilize Graphene formaldehyde adsorption, basic stain, containing phenyl ring Organic substance etc.
Polluter.The graphene oxide using wet method to prepare not only has good mechanical features, and can pollute by active adsorption
Dyestuff in solution.The research such as the Chen repair materials absorption sulfamethoxazole with Graphene as substrate, all material all shows
Go out stronger absorbability, maximal absorptive capacity successively: graphene (239.0mg g-1)>graphene–NH2 (40.6
mg·g-1) > graphene–COOH (20.5 mg·g-1)> graphene–OH(11.5 mg·g-1).Repairing performance is with ring
Border pH develops change, and when pH=2 when, its absorption property is the strongest, but as pH=9, then loses absorbability.
Farghali etc. use Hummer method to prepare graphene oxide and reduction obtains redox graphene, use CoFe2O4Modify oxidation
Reduced graphene, tests its adsorption to C.I. 42590, and result shows, graphenic surface is long-pending reaches 40.6m2/g.Additionally, oxidation
Graphene also has preferable adsorption to other basic stains, utilizes the methyl in 3DGO biopolymer gels absorption effluent
Indigo plant and crystal violet, by experimentation, be respectively 1100mg/g and 1350mg/g to the absorption maximal absorptive capacity of the two, and have
Absorption has the strongest selectivity.
In a word, current carbon nanomaterial adsorption technology is limited primarily to polluted-water and administers field, and is applied to turf establishment
Technology in terms of system consumer garbage compost substrate heavy metal adsorption, also there is no document report.
Summary of the invention
The present invention mainly uses the heavy metal that carbon nanomaterial is fixed, repaired in consumer garbage compost, probes into carbon nanometer material
Material is to the fixed effect of heavy metal in consumer garbage compost.In turf establishment system, apply carbon nanomaterial, analyze it to grass
The impact of level ground plant Adsorption of Heavy Metals, and on the impact of the different shape of heavy metal in consumer garbage compost.Numerous studies table
Bright, owing to compost percolate environment relatively water body environment is more complicated, containing gas chromatography matter, have with compost for the application of this technology
Carbon nanomaterial adsorption under machine environment.By this technical research, on the one hand for solving heavy metal from consumer garbage compost problem
Provide technical support.This technology uses consumer garbage compost lixiviating solution and heavy metal mixed solution simulation soil environment, develops
The adsorption technology of carbon nanomaterial heavy metal, should have significant application value.
The invention discloses following technology contents for achieving the above object:
A kind of method using carbon nanomaterial regulation and control compost extraction heavy metal adsorption, it is characterised in that by following step
Suddenly carry out:
(1) material is developed
Take from Tianjin little Dian consumer garbage compost treatment plant for examination garbage compost, cross 2mm sieve standby；Little shallow lake consumer garbage compost
Its basic physical and chemical is: the content of organic matter 22.00%, unit weight 0.79g/cm3, porosity 67.98%, saturation moisture content
0.67ml·g-1, pH value 7.49, full nitrogen 0.57%, full phosphorus 0.34%, full potassium 1. 21%, available phosphorus 0.078 g kg-1, C/N
Being 8.37, wherein tenor is respectively as follows: Ca 23.23 mg/kg, Fe 30.49g/kg, Mg 5. 78 g/kg, Cu
341.34 mg/kg, Zn 677.33 mg/kg, Pb 216.98 mg/kg, Cd 5.02 mg/kg, Mn 437.88 mg/kg,
Cr 702.6 mg/kg, Ni 41.82 mg/kg.
The grass seeds northern common grass Festuca Arundinacea of selection (Festuca arundinacea)；
The flit size of graphene microchip: 0.5-20 μm；Microplate thickness: 5-25 nm；Specific surface area: 40-60 m2/g；Density:
About 2.25 g/cm3；Electrical conductivity: 8000-10000 S/m；Phosphorus content: > 99.5%.
The average thickness of graphene oxide: 3.4-7 nm；Lamella diameter: 10-50 μm；The number of plies: 5-10 layer；Specific surface area:
100-300 m2/g；Purity > 90%.
The diameter of functionalized multi-wall carbonnanotubes: 20-40 nm；Length: 10-30 μm；-COOH content: 1.43%；Purity:
>90 wt%；Ashes: < 8 wt%；Specific surface area: > 110 m2/g；Conductivity: > 102 s/cm。
The diameter of hydroxylating multi-walled carbon nano-tubes: 20-40 nm；Length: 10-30 μm；-OH content: 1.63%；Purity: >
90 wt%；Ashes: < 8 wt%；Specific surface area: > 110 m2/g；Conductivity: > 102 s/cm；
(2) method:
1) weigh 50 mg carbon nanomaterials in the conical flask of 150 ml, add 100 ml, 100 mg L-1Cu2+、Pb2+、
Cd2Single ionic solution, adjust pH be 6,1 min that vibrates the most respectively, 3 min, 5 min, 10 min, 15 min, 30
min、1 h、2 h、4 h、8 h、24 h.Rapid filtration solution, with metal ion in atomic absorption spectroscopy determination filtrate
Residual concentration.
2) preparation is containing Cu2+、Pb2+、Cd2+The mixed solution of three heavy metal species ions, its concentration is than for 6:4:1；To join
The heavy metal mixed solution put is mixed for 1:2 in mass ratio with compost extraction；
3) weigh in 10mg carbon nanomaterial and conical flask, in conical flask, add step 2 respectively) heavy metal mixed solution 20
Compost extraction 20 ml of ml or simple, filters after 6 h that vibrate, and filtrate is measured with atomic absorption spectrophotometer (TAS-990)
Heavy metal concentration, according to its adsorbance of the mathematic interpolation of concentration of heavy metal ion before and after adsorption experiment.
The present invention further discloses and use the method for carbon nanomaterial regulation and control compost extraction heavy metal adsorption improving
Application in terms of the adsorption rate of heavy metal.Wherein the adsorption rate of heavy metal refers to: absorption affinity is respectively carbon
Nanotube and Cd affinity are strong, and graphene oxide and Cu affinity are strong, and Graphene and Pb absorption affinity are strong.Described heavy metal
Refer to: Cd, Cu, Pb.
More detailed description of the present invention is as follows:
1 develops materials and methods
1.1 materials and reagent
Take from Tianjin little Dian consumer garbage compost treatment plant for examination garbage compost, cross 2mm sieve standby.Its basic physical and chemical
For: the content of organic matter 22.00%, unit weight 0.79g/cm3, porosity 67.98%, saturation moisture content 0.67ml g-1, pH value 7.49,
Full nitrogen 0.57%, full phosphorus 0.34%, full potassium 1. 21%, available phosphorus 0.078 g kg-1, C/N is 8.37, and wherein tenor divides
It is not: Ca 23.23 mg/kg, Fe 30.49g/kg, Mg 5. 78 g/kg, Cu 341.34 mg/kg, Zn 677.33 mg/
Kg, Pb 216.98 mg/kg, Cd 5.02 mg/kg, Mn 437.88 mg/kg, Cr 702.6 mg/kg, Ni 41.82 mg/
kg。
Graphene microchip (Graphene) is purchased from Nanjing Ji Cang nanosecond science and technology company limited, for black, random flake
Structure, flit size: 0.5-20 μm；Microplate thickness: 5-25 nm；Specific surface area: 40-60 m2/g；Density: about 2.25 g/
cm3；Electrical conductivity: 8000-10000 S/m；Phosphorus content: > 99.5%.
Graphene oxide (Graphene oxide) is purchased from Suzhou Heng Qiu nanometer company, for black or brownish yellow powder, puts down
All thickness: 3.4-7 nm；Lamella diameter: 10-50 μm；The number of plies: 5-10 layer；Specific surface area: 100-300 m2/g；Purity > 90%.
Functionalized multi-wall carbonnanotubes (carboxylic multi-walled carbon nanotubes) is purchased from Beijing
Rich space high-tech new material technology company limited, diameter: 20-40 nm；Length: 10-30 μm；-COOH content: 1.43%；Pure
Degree: > 90 wt%；Ashes: < 8 wt%；Specific surface area: > 110 m2/g；Conductivity: > 102 s/cm.
Hydroxylating multi-walled carbon nano-tubes (Hydroxylation multi-walled carbon nanotubes) is purchased from north
Space high-tech new material technology company limited, diameter: 20-40 nm are won in capital；Length: 10-30 μm；-OH content: 1.63%；Pure
Degree: > 90 wt%；Ashes: < 8 wt%；Specific surface area: > 110 m2/g；Conductivity: > 102 s/cm。
1.2 method for designing
1.2.1 the adsorption time impact on adsorption effect
Weigh 50 mg carbon nanomaterials in the conical flask of 150 ml, add 100 ml, 100 mg L-1Cu2+、Pb2+、Cd2
Single ionic solution, adjust pH be 6,1 min that vibrates the most respectively, 3 min, 5 min, 10 min, 15 min, 30 min, 1
h、2 h、4 h、8 h、24 h.Rapid filtration solution, by the residual of metal ion in atomic absorption spectroscopy determination filtrate
Concentration.
1.2.2 mixture-metal competitive Adsorption is tested
1) preparation is containing Cu2+、Pb2+、Cd2+The mixed solution of three heavy metal species ions, its concentration is than for 6:4:1；
2) the heavy metal mixed solution of configuration is mixed for 1:2 in mass ratio with compost extraction；
3) weigh in 10mg carbon nanomaterial and conical flask, in conical flask, add step 2 respectively) heavy metal mixed solution 20
Compost extraction 20 ml of ml or simple, filters after 6 h that vibrate, and filtrate is measured with atomic absorption spectrophotometer (TAS-990)
Heavy metal concentration, according to its adsorbance of the mathematic interpolation of concentration of heavy metal ion before and after adsorption experiment.
1.3 data analysis
According to balance quality calculation adsorbance:
In formula,Initial concentration solution before absorptionIt is adsorbed toMoment solution concentrationAdsorb molten
Liquid amasss L；W adsorbent massAdsorbance mg/g.
Desorption quantity, desorption efficiency is calculated according to content of beary metal after desorbing.
Desorption efficiency=(desorption quantity/adsorbance) 100%
The experimental data of isothermal adsorption Langmuir model, the 2 kinds of isotherm adsorption model simulations of Freundlich model:
Langmuir equation:
In formula,For unit mass carbon nanomaterial absorption Solute mass during balanceFor having with absorbability
The constant of the Langmuir equation closed；Represent adsorption capacityDense for heavy metal ion in balance solution
Degree (mg L-1).
Freundlich equation:
In formula, KFWith the constant that n is Freundlich equation, it is respectively used to evaluate absorbability and the intensity of adsorbent.
Owing in experiment, the concentration of three heavy metal species ions of absorption differs, therefore can not directly judge from adsorbance
Cd, Cu, Pb tri-Competitive adsorption of heavy metal species ion, absorption competition coefficient can directly reflect that interionic effect is strong
Degree, eliminates the impact of concentration.
Its formula is:
In formula, KiAbsorption competition coefficient for heavy metal element；Weight, in this article
Individual elementFor the number of heavy metal element in system.
Data process and use Origin 8.6 to carry out adsorbing dynamic curve matching.
2 development results analyses
In the compound system containing various heavy, after adding Graphene, graphene oxide and CNT respectively, Cd2+'s
Adsorbance with the change of equilibrium concentration as it is shown in figure 1, when concentration is relatively low, each process between show identical trend, along with dense
The increase adsorbance of degree is continuously increased, and wherein, graphene oxide adsorbs Cd in lixiviating solution system2+Inhale with the increase of equilibrium concentration
Attached amount quickly raises, and subsequent concn continues to increase adsorbance and substantially remains unchanged, and other process groups all increase absorption with concentration
Amount is gradually increased.Further, in general, three kinds of carbon nanomaterials of compost extraction compound system are to Cd2+Adsorbance less than mixed
Fit system.Comparing with unitary system adsorbance, initial concentration is 100 mg g-1In the case of, in mixed system, Graphene,
Graphene oxide, the adsorbance of CNT reduce 28.7%, 14.75%, 30.95%；In lixiviating solution system, Graphene, carbon are received
The adsorbance of mitron reduces 46.35%, 54.04% respectively, but the adsorbance of graphene oxide does not decline.
In mixed system and compost extraction system, three kinds of carbon nanomaterials are to Cu2+Adsorbance with the change of equilibrium concentration
Change curve, as shown in Figure 2.In two kinds of systems, the adsorbance of Cu ion is all increased with concentration and increases by carbon nanomaterial, low dense
When spending, in mixed system and lixiviating solution system, the adsorbance difference of Cu ion is little, along with the increase of concentration, equilibrium concentration > 200
mg·g-1After, in mixed system, adsorbance increases sharply, but the adsorbance in lixiviating solution still maintains and is slowly increased, it is seen that lixiviating solution
System is to material with carbon element Adsorption of Cu2+There is certain inhibitory action.With Cu under single ionic2+Absorption compare, initial concentration is 150
mg·g-1Time, in mixed system, Graphene, graphene oxide, carbon nanotube adsorption amount reduce 36.33% respectively, 74.18%,
56.63%；Lixiviating solution system have dropped 7.09%, 56.92%, 19.92% respectively.
Fig. 3 show in compound system carbon nanomaterial to Pb2+Adsorbance with equilibrium concentration change curve, have the figure can
Know, in mixed system, Pb2+The adsorbance of ion is all slowly increased with the increase of equilibrium concentration, wherein the adsorbance of Graphene
Average higher than graphene oxide, CNT.But in lixiviating solution system, equilibrium concentration is less than 90mg g-1Time, adsorbance is delayed
Slow increase, along with being continuously increased of concentration, adsorbance increases rapidly, and adsorbance has exceeded the isolated son of identical initial concentration
Absorption, on the one hand the reason producing this situation is likely to be due in lixiviating solution containing certain Pb2+, increase the Pb in solution2+
Concentration, the organic matter being on the other hand likely to be due in lixiviating solution adds Pb2+Precipitation capacity.
3 develop conclusion
Graphene, graphene oxide, multi-walled carbon nano-tubes all have stronger absorbability to Cd, Cu, Pb.Relatively different metal from
Son absorbability on carbon nanomaterial of the same race, the absorbability of Graphene and carbon nano tube metal ion all shows as Pb >
Cu > Cd, but graphene oxide then shows themselves in that Pb > Cd > Cu, and, the absorbability to Pb and Cd, graphene oxide is superior to
Other two material.
Accompanying drawing illustrates:
Cd in Fig. 1 Compound Heavy Metals ionic system2+Absorption；Note: G, GO, CNT are Graphene, graphite oxide in mixed system
The Cd of absorption on alkene, CNT2+Adsorption curve.G-C, GO-C, CNT-C are Graphene, graphite oxide in compost acid soil
The Cd of absorption on alkene, CNT2+Adsorption curve, lower same；
Cu in Fig. 2 Compound Heavy Metals ionic system2+Absorption；
Pb in Fig. 3 Compound Heavy Metals ionic system2+Absorption.
Detailed description of the invention
The present invention is described below by specific embodiment.Unless stated otherwise, technological means used in the present invention
It is method known in those skilled in the art.It addition, embodiment is interpreted as illustrative, and the unrestricted present invention
Scope, the spirit and scope of the invention are limited only by the claims that follow.To those skilled in the art, without departing substantially from this
On the premise of invention spirit and scope, the various changes carrying out the material component in these embodiments and consumption or change are also
Belong to protection scope of the present invention.The present invention is raw materials used, reagent is commercially available.
Embodiment 1
(1) material is developed
Take from Tianjin little Dian consumer garbage compost treatment plant for examination garbage compost, cross 2mm sieve standby；Little shallow lake consumer garbage compost
Its basic physical and chemical is: the content of organic matter 22.00%, unit weight 0.79g/cm3, porosity 67.98%, saturation moisture content
0.67ml·g-1, pH value 7.49, full nitrogen 0.57%, full phosphorus 0.34%, full potassium 1. 21%, available phosphorus 0.078 g kg-1, C/N
Being 8.37, wherein tenor is respectively as follows: Ca 23.23 mg/kg, Fe 30.49g/kg, Mg 5. 78 g/kg, Cu
341.34 mg/kg, Zn 677.33 mg/kg, Pb 216.98 mg/kg, Cd 5.02 mg/kg, Mn 437.88 mg/kg,
Cr 702.6 mg/kg, Ni 41.82 mg/kg.
The grass seeds northern common grass Festuca Arundinacea of selection (Festuca arundinacea)；
The flit size of graphene microchip: 10 μm；Microplate thickness: 5 nm；Specific surface area: 40m2/g；Density: about 2.25 g/
cm3；Electrical conductivity: 8000 S/m；Phosphorus content: > 99.5%.
The average thickness of graphene oxide: 3.4nm；Lamella diameter: 10 μm；The number of plies: 5 layers；Specific surface area: 100-300
m2/g；Purity > 90%.
The diameter of functionalized multi-wall carbonnanotubes: 20nm；Length: 10 μm；-COOH content: 1.43%；Purity: > 90
wt%；Ashes: < 8 wt%；Specific surface area: > 110 m2/g；Conductivity: > 102 s/cm。
The diameter of hydroxylating multi-walled carbon nano-tubes: 20nm；Length: 10 μm；-OH content: 1.63%；Purity: > 90 wt%；
Ashes: < 8 wt%；Specific surface area: > 110 m2/g；Conductivity: > 102 s/cm；
(2) method:
1) weigh 50 mg carbon nanomaterials in the conical flask of 150 ml, add 100 ml, 100 mg L-1Cu2+、Pb2+、
Cd2Single ionic solution, adjust pH be 6,1 min that vibrates the most respectively, 3 min, 5 min, 10 min, 15 min, 30
min、1 h、2 h、4 h、8 h、24 h.Rapid filtration solution, with metal ion in atomic absorption spectroscopy determination filtrate
Residual concentration.
2) preparation is containing Cu2+、Pb2+、Cd2+The mixed solution of three heavy metal species ions, its concentration is than for 6:4:1；To join
The heavy metal mixed solution put is mixed for 1:2 in mass ratio with compost extraction；
3) weigh in 10mg carbon nanomaterial and conical flask, in conical flask, add step 2 respectively) heavy metal mixed solution 20
Compost extraction 20 ml of ml or simple, filters after 6 h that vibrate, and filtrate is measured with atomic absorption spectrophotometer (TAS-990)
Heavy metal concentration, according to its adsorbance of the mathematic interpolation of concentration of heavy metal ion before and after adsorption experiment.
Embodiment 2
(1) material is developed
Take from Tianjin little Dian consumer garbage compost treatment plant for examination garbage compost, cross 2mm sieve standby；Little shallow lake consumer garbage compost
Its basic physical and chemical is: the content of organic matter 22.00%, unit weight 0.79g/cm3, porosity 67.98%, saturation moisture content
0.67ml·g-1, pH value 7.49, full nitrogen 0.57%, full phosphorus 0.34%, full potassium 1. 21%, available phosphorus 0.078 g kg-1, C/N
Being 8.37, wherein tenor is respectively as follows: Ca 23.23 mg/kg, Fe 30.49g/kg, Mg 5. 78 g/kg, Cu
341.34 mg/kg, Zn 677.33 mg/kg, Pb 216.98 mg/kg, Cd 5.02 mg/kg, Mn 437.88 mg/kg,
Cr 702.6 mg/kg, Ni 41.82 mg/kg.
The grass seeds northern common grass Festuca Arundinacea of selection (Festuca arundinacea)；
The flit size of graphene microchip: 20 μm；Microplate thickness: 25 nm；Specific surface area: 60 m2/g；Density: about 2.25
g/cm3；Electrical conductivity: 10000 S/m；Phosphorus content: > 99.5%.
The average thickness of graphene oxide: 7 nm；Lamella diameter: 50 μm；The number of plies: 10 layers；Specific surface area: 300
m2/g；Purity > 90%.
The diameter of functionalized multi-wall carbonnanotubes: 40 nm；Length: 30 μm；-COOH content: 1.43%；Purity: > 90
wt%；Ashes: < 8 wt%；Specific surface area: > 110 m2/g；Conductivity: > 102 s/cm。
The diameter of hydroxylating multi-walled carbon nano-tubes: 40 nm；Length: 30 μm；-OH content: 1.63%；Purity: > 90
wt%；Ashes: < 8 wt%；Specific surface area: > 110 m2/g；Conductivity: > 102 s/cm；
(2) method:
1) weigh 50 mg carbon nanomaterials in the conical flask of 150 ml, add 100 ml, 100 mg L-1Cu2+、Pb2+、
Cd2Single ionic solution, adjust pH be 6,1 min that vibrates the most respectively, 3 min, 5 min, 10 min, 15 min, 30
min、1 h、2 h、4 h、8 h、24 h.Rapid filtration solution, with metal ion in atomic absorption spectroscopy determination filtrate
Residual concentration.
2) preparation is containing Cu2+、Pb2+、Cd2+The mixed solution of three heavy metal species ions, its concentration is than for 6:4:1；To join
The heavy metal mixed solution put is mixed for 1:2 in mass ratio with compost extraction；
3) weigh in 10mg carbon nanomaterial and conical flask, in conical flask, add step 2 respectively) heavy metal mixed solution 20
Compost extraction 20 ml of ml or simple, filters after 6 h that vibrate, and filtrate is measured with atomic absorption spectrophotometer (TAS-990)
Heavy metal concentration, according to its adsorbance of the mathematic interpolation of concentration of heavy metal ion before and after adsorption experiment.
Claims (5)
1. the method using carbon nanomaterial regulation and control compost extraction heavy metal adsorption, it is characterised in that by the steps
Carry out:
(1) material is developed
Take from Tianjin little Dian consumer garbage compost treatment plant for examination garbage compost, cross 2mm sieve standby；
The grass seeds northern common grass Festuca Arundinacea of selection (Festuca arundinacea)；
The flit size of graphene microchip: 0.5-20 μm；Microplate thickness: 5-25 nm；Specific surface area: 40-60 m2/g；Density:
About 2.25 g/cm3；Electrical conductivity: 8000-10000 S/m；Phosphorus content: > 99.5%；
The average thickness of graphene oxide: 3.4-7 nm；Lamella diameter: 10-50 μm；The number of plies: 5-10 layer；Specific surface area: 100-
300 m2/g；Purity > 90%；
The diameter of functionalized multi-wall carbonnanotubes: 20-40 nm；Length: 10-30 μm；-COOH content: 1.43%；Purity: > 90
wt%；Ashes: < 8 wt%；Specific surface area: > 110 m2/g；Conductivity: > 102s/cm；
The diameter of hydroxylating multi-walled carbon nano-tubes: 20-40 nm；Length: 10-30 μm；-OH content: 1.63%；Purity: > 90
wt%；Ashes: < 8 wt%；Specific surface area: > 110 m2/g；Conductivity: > 102 s/cm；
(2) method:
1) weigh 50 mg carbon nanomaterials in the conical flask of 150 ml, add 100 ml, 100 mg L-1Cu2+、Pb2+、
Cd2Single ionic solution, adjust pH be 6,1 min that vibrates the most respectively, 3 min, 5 min, 10 min, 15 min, 30
Min, 1 h, 2 h, 4 h, 8 h, 24 h, rapid filtration solution, with metal ion in atomic absorption spectroscopy determination filtrate
Residual concentration；
2) preparation is containing Cu2+、Pb2+、Cd2+The mixed solution of three heavy metal species ions, its concentration is than for 6:4:1；By configuration
Heavy metal mixed solution is mixed for 1:2 in mass ratio with compost extraction；
3) weigh in 10mg carbon nanomaterial and conical flask, in conical flask, add step 2 respectively) heavy metal mixed solution 20
Compost extraction 20 ml of ml or simple, filters after 6 h that vibrate, and filtrate is measured with atomic absorption spectrophotometer (TAS-990)
Heavy metal concentration, according to its adsorbance of the mathematic interpolation of concentration of heavy metal ion before and after adsorption experiment.
2. the method described in claim 1, wherein said little shallow lake its basic physical and chemical of consumer garbage compost is: organic matter contains
Amount 22.00%, unit weight 0.79g/cm3, porosity 67.98%, saturation moisture content 0.67ml g-1, pH value 7.49, full nitrogen 0.57%,
Full phosphorus 0.34%, full potassium 1. 21%, available phosphorus 0.078 g kg-1, C/N is 8.37, and wherein tenor is respectively as follows: Ca
23.23 mg/kg, Fe 30.49g/kg, Mg 5. 78 g/kg, Cu 341.34 mg/kg, Zn 677.33 mg/kg, Pb
216.98 mg/kg, Cd 5.02 mg/kg, Mn 437.88 mg/kg, Cr 702.6 mg/kg, Ni 41.82 mg/kg.
3. the method using carbon nanomaterial regulation and control compost extraction heavy metal adsorption described in claim 1 is improving heavy metal
Adsorption rate in terms of application.
4. the application described in claim 3, wherein the adsorption rate of heavy metal refers to: Graphene, graphene oxide, Duo Bi
The CNT absorption to Cd, Cu, Pb.
5. the application described in claim 3, wherein said adsorption rate refers to the graphene oxide absorption to Pb and Cd.
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