CN112007612A - Magnetic compound MnO2@Fe3O4Research on adsorption performance of @ rGO uranium - Google Patents
Magnetic compound MnO2@Fe3O4Research on adsorption performance of @ rGO uranium Download PDFInfo
- Publication number
- CN112007612A CN112007612A CN202010979818.8A CN202010979818A CN112007612A CN 112007612 A CN112007612 A CN 112007612A CN 202010979818 A CN202010979818 A CN 202010979818A CN 112007612 A CN112007612 A CN 112007612A
- Authority
- CN
- China
- Prior art keywords
- rgo
- mno
- uranium
- temperature
- stirring
- 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.)
- Pending
Links
- NUJOXMJBOLGQSY-UHFFFAOYSA-N manganese dioxide Chemical compound O=[Mn]=O NUJOXMJBOLGQSY-UHFFFAOYSA-N 0.000 title claims abstract description 58
- 230000005291 magnetic effect Effects 0.000 title claims abstract description 18
- 150000001875 compounds Chemical class 0.000 title claims abstract description 12
- 238000001179 sorption measurement Methods 0.000 title abstract description 28
- 229910052770 Uranium Inorganic materials 0.000 title abstract description 22
- DNYWZCXLKNTFFI-UHFFFAOYSA-N uranium Chemical compound [U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U] DNYWZCXLKNTFFI-UHFFFAOYSA-N 0.000 title 1
- SZVJSHCCFOBDDC-UHFFFAOYSA-N iron(II,III) oxide Inorganic materials O=[Fe]O[Fe]O[Fe]=O SZVJSHCCFOBDDC-UHFFFAOYSA-N 0.000 claims abstract description 51
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 16
- 229910021389 graphene Inorganic materials 0.000 claims abstract description 13
- 238000000034 method Methods 0.000 claims abstract description 8
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 17
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 13
- 238000003756 stirring Methods 0.000 claims description 12
- 238000006243 chemical reaction Methods 0.000 claims description 11
- 239000002131 composite material Substances 0.000 claims description 10
- 238000001035 drying Methods 0.000 claims description 10
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 claims description 9
- 238000005406 washing Methods 0.000 claims description 9
- 239000008367 deionised water Substances 0.000 claims description 7
- 229910021641 deionized water Inorganic materials 0.000 claims description 7
- 238000002360 preparation method Methods 0.000 claims description 7
- 238000003786 synthesis reaction Methods 0.000 claims description 7
- 238000009210 therapy by ultrasound Methods 0.000 claims description 7
- 238000010438 heat treatment Methods 0.000 claims description 6
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims description 5
- 239000012286 potassium permanganate Substances 0.000 claims description 5
- 238000001914 filtration Methods 0.000 claims description 4
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 claims description 3
- WQZGKKKJIJFFOK-GASJEMHNSA-N Glucose Natural products OC[C@H]1OC(O)[C@H](O)[C@@H](O)[C@@H]1O WQZGKKKJIJFFOK-GASJEMHNSA-N 0.000 claims description 3
- 235000011114 ammonium hydroxide Nutrition 0.000 claims description 3
- 230000015572 biosynthetic process Effects 0.000 claims description 3
- 235000019441 ethanol Nutrition 0.000 claims description 3
- 239000008103 glucose Substances 0.000 claims description 3
- 229910002804 graphite Inorganic materials 0.000 claims 3
- 239000010439 graphite Substances 0.000 claims 3
- 239000000725 suspension Substances 0.000 claims 3
- 238000001816 cooling Methods 0.000 claims 2
- 239000006185 dispersion Substances 0.000 claims 1
- 239000007788 liquid Substances 0.000 claims 1
- 229910001220 stainless steel Inorganic materials 0.000 claims 1
- 239000010935 stainless steel Substances 0.000 claims 1
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 abstract description 19
- -1 uranium ions Chemical class 0.000 abstract description 7
- 239000003463 adsorbent Substances 0.000 abstract description 5
- 239000000463 material Substances 0.000 abstract description 3
- 230000007547 defect Effects 0.000 abstract description 2
- 238000000926 separation method Methods 0.000 abstract description 2
- 230000002194 synthesizing effect Effects 0.000 abstract description 2
- 238000012360 testing method Methods 0.000 abstract description 2
- 238000012512 characterization method Methods 0.000 abstract 1
- 238000001027 hydrothermal synthesis Methods 0.000 abstract 1
- 230000000877 morphologic effect Effects 0.000 abstract 1
- 230000008929 regeneration Effects 0.000 abstract 1
- 238000011069 regeneration method Methods 0.000 abstract 1
- 239000000243 solution Substances 0.000 description 8
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 7
- AAORDHMTTHGXCV-UHFFFAOYSA-N uranium(6+) Chemical compound [U+6] AAORDHMTTHGXCV-UHFFFAOYSA-N 0.000 description 6
- 229910021578 Iron(III) chloride Inorganic materials 0.000 description 4
- RBTARNINKXHZNM-UHFFFAOYSA-K iron trichloride Chemical compound Cl[Fe](Cl)Cl RBTARNINKXHZNM-UHFFFAOYSA-K 0.000 description 4
- 239000003153 chemical reaction reagent Substances 0.000 description 3
- 230000006378 damage Effects 0.000 description 3
- 238000009792 diffusion process Methods 0.000 description 3
- 238000002474 experimental method Methods 0.000 description 3
- 230000005415 magnetization Effects 0.000 description 3
- 239000000203 mixture Substances 0.000 description 3
- 230000008569 process Effects 0.000 description 3
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 239000013078 crystal Substances 0.000 description 2
- 230000007423 decrease Effects 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- 230000036541 health Effects 0.000 description 2
- 229910001385 heavy metal Inorganic materials 0.000 description 2
- 239000000696 magnetic material Substances 0.000 description 2
- 239000011259 mixed solution Substances 0.000 description 2
- 238000002336 sorption--desorption measurement Methods 0.000 description 2
- 229910002589 Fe-O-Fe Inorganic materials 0.000 description 1
- 229910018663 Mn O Inorganic materials 0.000 description 1
- 229910003176 Mn-O Inorganic materials 0.000 description 1
- 238000003917 TEM image Methods 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 238000013459 approach Methods 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 150000001768 cations Chemical class 0.000 description 1
- 239000003245 coal Substances 0.000 description 1
- 230000005595 deprotonation Effects 0.000 description 1
- 238000010537 deprotonation reaction Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000005292 diamagnetic effect Effects 0.000 description 1
- WYICGPHECJFCBA-UHFFFAOYSA-N dioxouranium(2+) Chemical compound O=[U+2]=O WYICGPHECJFCBA-UHFFFAOYSA-N 0.000 description 1
- 238000004146 energy storage Methods 0.000 description 1
- 238000002329 infrared spectrum Methods 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- 231100000053 low toxicity Toxicity 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- 239000011159 matrix material Substances 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 229940031182 nanoparticles iron oxide Drugs 0.000 description 1
- 230000007935 neutral effect Effects 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 239000003208 petroleum Substances 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 230000035484 reaction time Effects 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- 238000005067 remediation Methods 0.000 description 1
- 230000008439 repair process Effects 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 238000001228 spectrum Methods 0.000 description 1
- 238000001308 synthesis method Methods 0.000 description 1
- 231100000331 toxic Toxicity 0.000 description 1
- 230000002588 toxic effect Effects 0.000 description 1
- 239000002351 wastewater Substances 0.000 description 1
Images
Classifications
-
- 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
-
- 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
- B01J20/06—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising oxides or hydroxides of metals not provided for in group B01J20/04
-
- 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
- B01J20/28—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof characterised by their form or physical properties
- B01J20/28002—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof characterised by their form or physical properties characterised by their physical properties
- B01J20/28009—Magnetic properties
-
- 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
- C02F1/28—Treatment of water, waste water, or sewage by sorption
- C02F1/283—Treatment of water, waste water, or sewage by sorption using coal, charred products, or inorganic mixtures containing them
-
- 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
- C02F2101/006—Radioactive compounds
-
- 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
- C02F2101/10—Inorganic compounds
- C02F2101/20—Heavy metals or heavy metal compounds
-
- 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
- C02F2103/08—Seawater, e.g. for desalination
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Analytical Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Inorganic Chemistry (AREA)
- Life Sciences & Earth Sciences (AREA)
- Hydrology & Water Resources (AREA)
- Engineering & Computer Science (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
Abstract
The invention mainly relates to the removal problem of uranium ions and the adsorption behavior of uranyl ions. The invention aims to solve the defects of secondary pollution, weak mechanical strength and difficult separation of the existing part of the adsorbent, so that the adsorbent can be used for a long time by people. The method adopted by the invention mainly comprises the following steps: with graphene and MnO2Preparing Fe by hydrothermal method as basic material3O4@ rGO complex, RebarWater bath method for synthesizing MnO2@Fe3O4The @ rGO magnetic compound is subjected to morphological characterization and electrochemical testing, and the result proves that the compound has strong adsorption performance on uranium and MnO is generated after the peak value is reached2@Fe3O4The increase of the amount of @ rGO does not have obvious change on the uranium removal rate, and has stronger regeneration performance.
Description
Technical Field
The invention mainly relates to the removal problem of uranium ions and the adsorption action of uranyl ions.
Background
With the continuous development of modern industry, traditional non-renewable energy sources (such as petroleum, coal and the like) are continuously consumed, and the problem of resource exhaustion is faced. To alleviate this troublesome problem, researchers have conducted extensive research to find alternative, non-renewable energy sources to which nuclear energy has received much attention in recent years, and over the next decades, nuclear energy is considered to be the only mature, continuous, scalable energy source in order to meet the ever-increasing energy demands. In the process of developing nuclear energy, uranium can be effectively utilized, economic benefits are brought to people, and pollution is generated to harm human health. Uranium has a high radioactivity, a long half-life and biotoxicity and is considered to be one of the most dangerous heavy metals in the environment. The uranium has serious damage to underground water quality, is harmful to human bodies and needs hundreds of years to repair once the uranium is damaged, so that an efficient and economic method for treating uranium pollution becomes a hotspot.
Disclosure of Invention
In order to solve the problems of harm of uranium to the environment and human health and overcome the defects of secondary pollution and difficult separation of the existing adsorbent, the invention synthesizes a magnetic adsorption material MnO by taking graphene as a matrix2@Fe3O4@ rGO, the adsorption performance of the composite material to uranium is in an optimal state when the pH value is 6, and meanwhile, the temperature also influences MnO2@Fe3O4An important factor for the adsorption performance of @ rGO, the theoretical adsorption capacity of the composite is maximal at 55 ℃, MnO2@Fe3O4The @ rGO is a magnetic compound, can be easily separated from an aqueous solution by using an external magnetic field, and still can keep higher adsorption efficiency after multiple adsorption-desorption cycles, so that the possibility is provided for recycling, the treatment efficiency of uranium is improved, and a theoretical basis is provided for the treatment of other toxic metals.
The purpose of the invention is realized as follows:
magnetic compound MnO2@Fe3O4The preparation method of @ rGO comprises the following steps:
(1) the main reagents used for obtaining the invention comprise rGO and FeCl3·6H2O and KMnO4And the like.
(2) First, synthesis of graphene. And stripping the obtained graphene by ultrasonic, completely dissolving glucose in the graphene, stirring for 30min at room temperature, and adding ammonia water into the solution. After vigorous shaking the resulting mixture was stirred at 95 ℃ and the product was subsequently cooled, filtered and washed.
(3)Fe3O4Synthesis of @ rGO. Graphene was added to the ethylene glycol solution and sonicated. Then FeCl3·6H2And adding O and NaAc into the mixed solution for dissolving, stirring for 30min, transferring the solution into a reaction kettle, reacting for 6h at 200 ℃, repeatedly washing the obtained product with ethanol and deionized water, and drying at 60 ℃.
(4) Magnetic composite MnO2@Fe3O4Synthesis of @ rGO. The compound is synthesized by a water bath synthesis method. KMnO4Heating to 75 ℃ in water bath, and reacting for 3h to obtain Fe3O4@ rGO was added to the above solution and pH adjusted with hydrochloric acid. Continuously heating in 75 deg.C water bath for 3 hr, filtering, washing with deionized water and anhydrous ethanol, and drying at 80 deg.C for 12 hr.
The second stirring temperature in the step (2) is 95 ℃, and the stirring time is 30 min;
the ultrasonic treatment time in the step (3) is 3 hours, the reaction temperature is 200 ℃ after the ultrasonic treatment time is transferred to a reaction kettle, the reaction time is 6 hours, absolute ethyl alcohol and deionized water are selected for washing, and the drying temperature is 60 ℃;
KMnO in the step (4)4Heating in water bath at 75 deg.C for 3 hr, adjusting pH to about 5, and adding Fe3O4Keeping the temperature at 75 ℃ after @ rGO and reacting for 3h, wherein the drying temperature is 80 ℃ and the time is 12 h.
Compared with the prior art, the invention has the beneficial effects that;
the invention selects MnO2Is one of the original reagents, utilizes the low cost and synthesis thereofThe method is simple, can provide an effective surface to adsorb heavy metal elements in the wastewater, and develops a new generation of magnetic material which is a new material for environmental purification. The adsorption-desorption of the magnetic material can be realized only by a simple external magnetic field, namely iron oxide nano-particles (Fe)3O4) The magnetic composite has the characteristics of low toxicity and superparamagnetism, and the magnetic composite formed by skillfully combining the three components not only improves the uranium removal rate and the reproducibility, but also can be applied to the fields of adsorption, magnetic energy storage, catalysis, environmental remediation and the like.
Drawings
FIG. 1 shows Fe prepared in example 1 of the present invention3O4@ rGO and MnO2@Fe3O4The XRD pattern of @ rGO;
FIG. 2 shows GO, Fe prepared in example 1 of the present invention3O4@ rGO and MnO2@Fe3O4Infrared spectrogram of @ rGO;
FIG. 3 shows MnO prepared in example 1 of the present invention2@Fe3O4TEM image of @ rGO;
FIG. 4 shows Fe prepared in example 1 of the present invention3O4@ rGO and MnO2@Fe3O4A hysteresis loop of @ rGO;
FIG. 5 shows MnO prepared in example 1 of the present invention2@Fe3O4@ rGO uranium adsorption performance curves at different pH's; MnO2@Fe3O4@ rGO adsorption isotherms and linear fitting graphs of uranium at different temperatures;
FIG. 6 is a Zata potential measurement curve before and after uranium adsorption at different pH values, prepared in example 1 of the present invention;
FIG. 7 shows different MnO prepared in example 1 of the present invention2@Fe3O4The effect of the amount of @ rGO adsorbent on uranium adsorption performance;
FIG. 8 shows MnO prepared in example 1 of the present invention2@Fe3O4The relationship between the adsorption capacity and adsorption time of @ rGO to uranium;
FIG. 9 shows MnO prepared in example 1 of the present invention2@Fe3O4The intragranular diffusion model of @ rGO;
Detailed Description
The present invention will be described in detail below with reference to the accompanying drawings and examples.
Example 1 magnetic composite MnO2@Fe3O4The preparation method of @ rGO comprises the following preparation steps:
(1) the main reagents used for obtaining the invention comprise rGO and FeCl3·6H2O and KMnO4Etc.;
(2) and (3) synthesizing graphene. And stripping the obtained graphene by ultrasonic, completely dissolving glucose in the graphene, stirring for 30min at room temperature, and adding ammonia water into the solution. The mixture obtained after vigorous shaking was stirred at 95 ℃ and the product was subsequently cooled, filtered and washed;
(3) adding graphene into an ethylene glycol solution and carrying out ultrasonic treatment. Then FeCl3·6H2Adding O and NaAc into the mixed solution for dissolving, transferring the solution into a reaction kettle after stirring, reacting for 6 hours at 200 ℃, repeatedly washing the obtained product with ethanol and deionized water, and drying at 60 ℃ to obtain Fe3O4@rGO；
(4) Fe prepared in the step (3)3O4@ rGO addition of KMnO4The water bath was heated to a solution of 75 deg.C and the pH was adjusted with hydrochloric acid. Continuously keeping the same temperature for heating in water bath for 3h, filtering the mixture, washing with deionized water and absolute ethyl alcohol, and drying at 80 ℃ for 12 h;
the invention is further described with reference to the following drawings and examples:
as shown in fig. 1, Fe was analyzed by XRD test3O4@ rGO and MnO2@Fe3O4The crystal structure of the @ rGO compound, and the results show that MnO2@Fe3O4@ rGO exhibits a new diffraction peak at 37.64 deg. 2 θ, which is attributed to MnO2(131) crystal face of (1), and MnO2@Fe3O4The XRD spectrum of the @ rGO compound has a plurality of obvious characteristic peaksFalls under MnO2(JCPDS14-664), these results show MnO2@Fe3O4The @ rGO complex has been successfully prepared.
As shown in FIG. 2, at 1385cm-1The characteristic peak of (A) should be assigned to C-H vibration at MnO2@Fe3O4In the IR spectrum of the @ rGO complex, about 624cm in the low frequency region was observed-1The presence of which is attributed to the vibration of Mn-O, Mn-O-Mn and Fe-O-Fe.
As shown in FIG. 3, MnO was exhibited2@Fe3O4Structure of @ rGO, Fe3O4@ rGO by MnO2Complete coating to form a very thin, continuous uniform MnO2And (4) coating.
As shown in FIG. 4, Fe was obtained3O4@ rGO and MnO2@Fe3O4The saturation magnetization of @ rGO is 62.4 emu/g and 13.9emu/g, respectively. With Fe3O4Comparison of saturation magnetization of @ rGO, MnO2@Fe3O4The saturation magnetization of @ rGO is reduced, mainly by diamagnetic MnO2Coated with Fe3O4@ rGO.
As shown in FIG. 5, MnO was observed in the graph2@Fe3O4The adsorption capacity for uranium of @ rGO increases gradually from 2.0 to 6.0, but decreases gradually with increasing pH from 6.0 to 12.0. In the pH range from 2 to 12, the pH of the best adsorbed uranium (VI) was 6.0 and the pH of the least adsorbed uranium (VI) was 2.0. MnO with increasing pH2@Fe3O4The @ rGO is subjected to a deprotonation process to enable the surface of the @ rGO to be negatively charged, so that the coulomb attraction between the compound and uranium (VI) is increased, the interaction between the compound and the uranium (VI) is strengthened, and the adsorption performance is further improved.
As shown in FIG. 6, at a certain pH range, the magnetic composite MnO was present at a pH of 3.92@Fe3O4The isoelectric point of @ rGO and MnO when the pH value is more than 3.92@Fe3O4@ rGO surface charge is negative. When the pH value is less than 6.0, the uranyl ions are absorbed after being adsorbedMnO before attachment2@Fe3O4The higher zeta potential values of @ rGO indicate that the uranyl ion is present as a cation or as a neutral complex that attenuates the surface charge by positive conversion. MnO at pH greater than 6.02@Fe3O4The @ rGO complex is highly electronegative and the effect of adsorption of uranyl ions on its zeta potential becomes less pronounced.
As shown in FIG. 7, it can be concluded that uranium (VI) removal efficiency varies with MnO2@Fe3O4The increase in the amount of @ rGO increases rapidly and then approaches equilibrium, but the adsorption capacity decreases. With MnO2@Fe3O4Increase of @ rGO content, in MnO2@Fe3O4The functional groups and adsorption sites available on the surface of @ rGO are increased, resulting in increased adsorption performance of the adsorbent for uranium (VI) ions.
As shown in FIG. 8, it can be seen that MnO was present during the first 240min contact time2@Fe3O4The rate of uranium adsorption is very fast for @ rGO, with the subsequent reaction proceeding at a slower rate, eventually reaching equilibrium at 360 min. Therefore, in the later experiments, in order to ensure that the adsorption balance can be achieved in each step of experiment, the adsorption experiment time is set to be 360 min. Furthermore, a maximum adsorption capacity of 110.6mg/g was obtained at an initial uranium (VI) concentration of 120 mg/L.
As shown in FIG. 9, the straight line portion does not pass through the origin, indicating MnO2@Fe3O4The @ rGO adsorption process is co-controlled by intra-particle diffusion and membrane diffusion.
Claims (4)
1. Magnetic compound MnO2@Fe3O4The preparation method of @ rGO comprises the following steps:
(1) synthesis of graphene (rGO). Dispersing the synthesized graphite oxide in water, stripping by an ultrasonic method to obtain uniform graphite oxide dispersion liquid, completely dissolving glucose in the stripped graphite oxide solution, stirring and adding ammonia water. And then shaking, stirring, cooling, filtering and washing to obtain the product graphene.
(2)Fe3O4Synthesis of @ rGO. Adding graphene into an ethylene glycol solution, and performing ultrasonic treatment. Then FeCl is added3·6H2And adding O and NaAc into the solution, stirring, transferring into a stainless steel high-pressure reaction kettle, reacting at a certain temperature, naturally cooling, washing and drying.
(3)MnO2@Fe3O4Synthesis of @ rGO. KMnO4Heating in water bath, reacting at a certain temperature, and obtaining Fe3O4@ rGO was added to the above solution and the pH of the solution was adjusted with dilute hydrochloric acid. And after the reaction is finished, filtering the suspension, washing the suspension for several times by using deionized water and absolute ethyl alcohol, and drying the suspension.
2. The magnetic composite MnO of claim 12@Fe3O4The preparation method of @ rGO is characterized by comprising the following steps: in the step (1), the stirring time at room temperature for the first time is 30min, the stirring temperature after shaking is 95 ℃, and the stirring time is 60 min.
3. The magnetic composite MnO of claim 12@Fe3O4The preparation method of @ rGO is characterized by comprising the following steps: the ultrasonic treatment time in the step (2) is 3 hours, the reaction temperature is 200 ℃ after the ultrasonic treatment time is transferred to a reaction kettle, the ultrasonic treatment time is 6 hours, ethanol and deionized water are selected for washing, and the drying temperature is 60 ℃.
4. The magnetic composite MnO of claim 12@Fe3O4The preparation method of @ rGO is characterized by comprising the following steps: KMnO in the step (3)4The water bath heating temperature is 75 ℃ and is kept for 3h, the pH value is adjusted to about 5, and Fe3O4After the @ rGO is added, the reaction is continued for 3h at the temperature of 75 ℃, and the drying temperature is 80 ℃ for 12 h.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202010979818.8A CN112007612A (en) | 2020-09-17 | 2020-09-17 | Magnetic compound MnO2@Fe3O4Research on adsorption performance of @ rGO uranium |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202010979818.8A CN112007612A (en) | 2020-09-17 | 2020-09-17 | Magnetic compound MnO2@Fe3O4Research on adsorption performance of @ rGO uranium |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN112007612A true CN112007612A (en) | 2020-12-01 |
Family
ID=73521811
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN202010979818.8A Pending CN112007612A (en) | 2020-09-17 | 2020-09-17 | Magnetic compound MnO2@Fe3O4Research on adsorption performance of @ rGO uranium |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN112007612A (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113089016A (en) * | 2021-03-10 | 2021-07-09 | 西南科技大学 | Preparation method of high-performance single-center uranium-based supported catalyst |
-
2020
- 2020-09-17 CN CN202010979818.8A patent/CN112007612A/en active Pending
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113089016A (en) * | 2021-03-10 | 2021-07-09 | 西南科技大学 | Preparation method of high-performance single-center uranium-based supported catalyst |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| CN110813251B (en) | Modified nano material and application thereof in antimony-containing wastewater treatment | |
| CN110694583B (en) | Preparation method and application of magnetic recyclable lanthanum oxide phosphate removal adsorbent | |
| CN109569548B (en) | Magnetic nano functional material for extracting uranium from seawater and preparation method thereof | |
| US11384444B2 (en) | Method for electrochemical extraction of uranium from seawater using oxygen vacancy (OV)-containing metal oxide | |
| CN113198507A (en) | Preparation method of nitrogen-doped graphene-loaded iron-cobalt bimetallic single-atom catalyst | |
| CN104826599A (en) | Preparation method of magnetic composite organic bentonite | |
| CN104275196A (en) | Ferroferric oxide/carbon/cadmium sulfide composite nano material and preparation method thereof | |
| CN109499520A (en) | A kind of amino functional manganese dioxide load nano-magnetic preparation method for bentonite and its application | |
| CN112742340A (en) | S-ZVI magnetic environment restoration material and preparation method and application thereof | |
| CN111825260B (en) | Method for regulating and controlling selective adsorption of Cu2+, Pb2+ and Zn2+ from wastewater by carbon nanotubes | |
| CN111298760A (en) | Preparation method of flower-like aluminum oxide-magnesium oxide composite adsorbent, product and application thereof | |
| CN108147518B (en) | Modified starch water treatment agent and preparation method and application thereof | |
| CN112007612A (en) | Magnetic compound MnO2@Fe3O4Research on adsorption performance of @ rGO uranium | |
| CN113877549A (en) | Selective composite microsphere adsorption material and preparation method and application thereof | |
| CN113385139B (en) | Schweitmann stone prepared by alkali neutralization method and application thereof | |
| CN114225897A (en) | Modified attapulgite loaded nano zero-valent iron composite material and preparation method and application thereof | |
| CN116651474B (en) | Preparation method of ferric hydroxide quantum dot modified BiOX photocatalytic material | |
| CN113413869A (en) | Preparation method of magnetic Mg-La-Fe/zeolite composite material and dephosphorization application thereof | |
| CN115920834B (en) | Composite defluorinating agent for water purification and preparation method thereof | |
| CN108043371A (en) | A kind of double-template is oriented to the preparation method and applications of trace composite membrane | |
| CN113952939A (en) | Preparation method and application of amino modified ferrihydrite material | |
| CN109046265B (en) | Preparation method of magnetic carboxymethyl chitosan adsorbent | |
| CN115101736B (en) | Three-dimensional NiPc-NiFe@Ti 3 C 2 T x Preparation method of MXene composite material, and product and application thereof | |
| CN115498299A (en) | Method for recovering Prussian positive electrode material and manganese-based Prussian white positive electrode material prepared by same | |
| CN113289570B (en) | Arsenic adsorbing material and preparation method and application thereof |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| PB01 | Publication | ||
| PB01 | Publication | ||
| WD01 | Invention patent application deemed withdrawn after publication |
Application publication date: 20201201 |
|
| WD01 | Invention patent application deemed withdrawn after publication |