Water decontamination via C.SUB.3.N.SUB.4.@MoO.SUB.3./MgAl.SUB.2.O.SUB.4 .nanocomposite
12479741 ยท 2025-11-25
Assignee
Inventors
Cpc classification
B01J20/28019
PERFORMING OPERATIONS; TRANSPORTING
B01J20/3078
PERFORMING OPERATIONS; TRANSPORTING
C02F2101/22
CHEMISTRY; METALLURGY
B01J20/2809
PERFORMING OPERATIONS; TRANSPORTING
B01J20/3021
PERFORMING OPERATIONS; TRANSPORTING
B01J20/08
PERFORMING OPERATIONS; TRANSPORTING
C02F1/288
CHEMISTRY; METALLURGY
B01J20/0259
PERFORMING OPERATIONS; TRANSPORTING
B01J20/06
PERFORMING OPERATIONS; TRANSPORTING
International classification
B01J20/06
PERFORMING OPERATIONS; TRANSPORTING
B01J20/08
PERFORMING OPERATIONS; TRANSPORTING
B01J20/28
PERFORMING OPERATIONS; TRANSPORTING
Abstract
A method of removing a contaminant from water may include contacting contaminated water, including a heavy metal and/or an organic pollutant, with a nanocomposite including graphitic C.sub.3N.sub.4, MoO.sub.3, and MgAl.sub.2O.sub.4 in a mass relationship to each other in a range of from 5 to 15:2 to 7:75 to 95, thereby adsorbing the heavy metal and/or the organic pollutant onto the nanocomposite, as an adsorbed material. The method further includes removing the adsorbed material from the contaminated water, thereby reducing a concentration of the heavy metal in the contaminated water by at least 2 wt. %, the heavy metal includes Cd, Cr, Cu, Fe, Pb, Ni, Ag, Zn, and/or U, and the organic pollutant includes a dye.
Claims
1. A method of removing a contaminant from water, the method comprising: contacting contaminated water, comprising a heavy metal, with a nanocomposite comprising graphitic C.sub.3N.sub.4, MoO.sub.3, and MgAl.sub.2O.sub.4 in a mass relationship to each other in a range of from 5 to 15:2 to 7:75 to 95, thereby adsorbing the heavy metal onto the nanocomposite, as an adsorbed material; and removing the adsorbed material from the contaminated water, thereby reducing a concentration of the heavy metal in the contaminated water by at least 2 wt. %, wherein the heavy metal comprises Cd, Cr, Cu, Fe, Pb, Ni, Ag, Zn, and/or U.
2. The method of claim 1, wherein the nanocomposite comprises no MoS.sub.2 before the contacting.
3. The method of claim 1, wherein the nanocomposite comprises no sulfide before the contacting.
4. The method of claim 1, wherein the nanocomposite comprises less than 10 wt. % Co, relative to total nanocomposite weight before the contacting.
5. The method of claim 1, wherein the nanocomposite comprises less than 1 wt. % Co, relative to total nanocomposite weight before the contacting.
6. The method of claim 1, wherein the nanocomposite comprises no more than 1 wt. % potassium before the contacting.
7. The method of claim 1, wherein the nanocomposite comprises no more than 1 wt. % iron before the contacting.
8. The method of claim 1, wherein the nanocomposite comprises no more than 1 wt. % zinc before the contacting.
9. The method of claim 1, wherein the nanocomposite comprises no more than 1 wt. % carbonaceous material besides the graphitic carbon nitride before the contacting.
10. The method of claim 1, wherein the nanocomposite has a structure comprising a dispersion of homogeneous spherical metal oxides nanoparticles on a two-dimensional porous structure comprising curled and wrinkled nanosheets and platelets of the g-C.sub.3N.sub.4.
11. The method of claim 1, which removes no more than 0.001 wt. % of uranium, based on total water weight.
12. The method of claim 1, wherein at least 70 mg of the heavy metal are adsorbed per gram of the nanocomposite from the water within 30 minutes of the contacting.
Description
BRIEF DESCRIPTION OF THE DRAWINGS
(1) A more complete appreciation of this disclosure and many of the attendant advantages thereof will be readily obtained as the same becomes better understood by reference to the following detailed description when considered in connection with the accompanying drawings, wherein:
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DETAILED DESCRIPTION
(12) When describing the present disclosure, the terms used are to be construed in accordance with the following definitions, unless a context dictates otherwise.
(13) Embodiments of the present invention will now be described more fully hereinafter with reference to the accompanying drawings wherever applicable, in that some, but not all, embodiments of the disclosure are shown.
(14) In the drawings, like reference numerals designate identical or corresponding parts throughout the several views. Further, as used herein, the words a, an and the like generally carry a meaning of one or more, unless stated otherwise.
(15) Furthermore, the terms approximately, approximate, about, and similar terms generally refer to ranges that include the identified value within a margin of 20%, 10%, or preferably 5%, and any values therebetween.
(16) As used herein, the term room temperature refers to a temperature range of 25 degrees Celsius ( C.)3 C. in the present disclosure.
(17) As used herein, the term nanoparticles (NPs) refers to particles having a particle size of 1 nanometer (nm) to 500 nm within the scope of the present invention.
(18) As used herein, the term nanocomposite refers to a composite material that has at least one component with a grain size measured in nanometers.
(19) As used herein, the term nanohybrid composite refers to a material that combines nanomaterials (such as nanoparticles, nanotubes, or nanofibers) with another material, typically a polymer, metal, or ceramic, to form a composite structure. The nanomaterials are typically incorporated at the nanoscale level to enhance the properties of the base material, such as improving strength, conductivity, or flexibility, while maintaining the advantages of both components. The resulting nanohybrid composite exhibits unique properties that are superior to the individual materials alone.
(20) As used herein, the term porosity refers to a measure of the void or vacant spaces within a material.
(21) As used herein, the term pore diameter refers to an average width or size of the pores (void spaces) within a material, typically measured in nm or angstroms (). It is a key parameter in characterizing the texture and permeability of porous materials, influencing their adsorption, filtration, or catalytic properties. The pore diameter is often determined using methods such as nitrogen adsorption or mercury intrusion, which provide insights into the material's ability to absorb or interact with molecules of specific sizes.
(22) As used herein, the term pore volume refers to the total volume of void spaces (pores) within a material that is capable of being filled by a gas or liquid. It is typically expressed in cubic centimeters per gram (cm.sup.3/g) and is an important parameter in characterizing the porous structure of materials, such as adsorbents or catalysts.
(23) As used herein, the term photodegradation refers to the process by which a material undergoes chemical breakdown or alteration due to exposure to light. This process typically results in the breaking of molecular bonds within the material, leading to the formation of new compounds or the degradation of its physical and chemical properties.
(24) As used herein, the term contaminants refer to the harmful substances or contaminants that degrade the quality of water, air, soil, or food, making them unsafe or unsuitable for specific uses. In water, contaminants include biological agents like bacteria, viruses, and parasites; chemical substances such as heavy metals, pesticides, pharmaceuticals, and industrial chemicals; and physical materials like dirt, debris, and sediment. These contaminants can pose serious risks to human health, the environment, and ecosystems, depending on their type, concentration, and exposure levels.
(25) As used herein, the term organic contaminants refers to carbon-based compounds, typically derived from industrial, agricultural, or domestic activities, that are present as contaminants in water or the environment. These contaminants may include pesticides, pharmaceuticals, dyes, and other synthetic or natural organic substances that can pose environmental or health risks.
(26) In some embodiments, the organic contaminant may be a dye, a phenol, a polycyclic aromatic hydrocarbon, an herbicide, a pesticide, a persistent organic contaminant, or the like.
(27) In some embodiments, the organic contaminant is a dye. A dye is a colored substance that chemically binds to a material it may be intended to color. Generally, a dye is applied in solution, typically aqueous solution. Examples of dyes include, but are not limited to: acridine dyes, which are acridine and its derivatives such as acridine orange, acridine yellow, acriflavine, and gelgreen; anthraquinone dyes, which are anthroaquinone and its derivatives such as acid blue 25, alizarin, anthrapurpurin, carminic acid, 1,4-diamno-2,3-dihydroanthraquinone, 7,14-dibenzypyrenequinone, dibromoanthrone, 1,3-dihydroxyanthraquinone, 1,4-dihydroxyanthraquinone, disperse red 9, disperse red 11, indanthrone blue, morindone, oil blue 35, parietin, quinizarine green SS, remazol brilliant blue R, solvent violet 13, 1,2,4-trihydroxyanthraquinone, vat orange 1, and vat yellow 1; diaryl methane dyes such as auramine O, triarylmethane dyes such as acid fuchsin, aluminon, aniline blue WS, aurin, aurintricarboxylic acid, brilliant blue FCF, brilliant green, bromocresol green, bromocresol purple, bromocresol blue, bromophenol blue, bromopyrogallol red, chlorophenol red, coomassie brilliant blue, cresol red, O-cresolphthalein, crystal violet, dichlorofluorescein, ethyl green, fast green FCT, FIAsH-EDT2, fluoran, fuchsine, green S, light green SF, malachite green, merbromin, metacresol purple, methyl blue, methyl violet, naphtholphthalein, new fuchsine, pararosaniline, patent blue V, phenol red, phenolphthalein, phthalein dye, pittacal, spirit blue, thymol blue, thymolphthalein, Victoria blue BO, Victoria blue R, water blue, xylene cyanol, and xylenol orange; azo dyes such as acid orange 5, acid red 13, alican yellow, alizarine yellow R, allura red AC, amaranth, amido black 10B, aniline yellow, arylide yellow, azo violet, azorubine, basic red 18, biebrich scarlet, Bismarck brown Y, black 7984, brilliant black BN, brown FK, chrysoine resorcinol, citrus red 2, congo red, D&C red 33, direct blue 1, disperse orange 1, eriochrome black T, evans blue, fast yellow AB, orange 1, hydroxynaphthol blue, janus green B, lithol rubine BK, metanil yellow, methyl orange, methyl red, methyl yellow, mordant brown 33, mordant red 19, naphthol AS, oil red 0, oil yellow DE, orange B, orange G, orange GGN, para red, pigment yellow 10, ponceau 2R, prontosil, red 2G, scarlet GN, Sirius red, solvent red 26, solvent yellow 124, sudan black B, sudan I, sudan red 7B, sudan stain, tartrazine, tropaeolin, trypan blue, and yellow 2G; phthalocyanine dyes such as phthalocyanine blue BN, phthalocyanine Green G, Alcian blue, and naphthalocyanine, azin dyes such as basic black 2, mauveine, neutral red, Perkin's mauve, phenazine, and safranin; indophenol dyes such as indophenol and dichlorophenolindophenol; oxazin dyes; oxazone dyes; thiazine dyes such as azure A, methylene blue, methylene green, new methylene blue, and toluidine blue; thiazole dyes such as primuline, stains-all, and thioflavin; xanthene dyes such as 6-carboxyfluorescein, eosin B, eosin Y, erythosine, fluorescein, rhodamine B, rose bengal, and Texas red; fluorone dyes such as calcein, carboxyfluorescein diacetate succinimidyl ester, fluo-3, fluo-4, indian yellow, merbromin, pacific blue, phloxine, and seminaphtharhodafluor; or rhodamine dyes such as rhodamine, rhodamine 6G, rhodamine 123, rhodamine B, sulforhodamine 101, and sulforhodamine B.
(28) A phenol is an organic compound consisting of a hydroxyl group (OH) bonded directly to an aromatic hydrocarbon group. Examples of phenols include, but are not limited to, phenol (the namesake of the group of compounds), bisphenols (including bisphenol A), butylated hydroxytoluene (BHT), 4-nonylphenol, orthophenyl phenol, picric acid, phenolphthalein and its derivatives mentioned above, xylenol, diethylstilbestrol, L-DOPA, propofol, butylated hydroxyanisole, 4-tert-butylcatechol, tert-butylhydroquinone, carvacrol, chloroxyleol, cresol (including M-, O-, and P-cresol), 2,6-di-tert-butylphenol, 2,4-dimethyl-6-tert-butylphenol, 2-ethyl-4,5-dimethylphenol, 4-ethylguaiacol, 3-ethylphenol, 4-ethylphenol, flexirubin, mesitol, 1-nonyl-4-phenol, thymol, 2,4,6-tri-tert-butylphenol, chlorophenol (including 2-, 3-, and 4-chlorophenol), dichlorophenol (including 2,4- and 2,6-dichlorophenol), bromophenol, dibromophenol (including 2,4-dibromophenol), nitrophenol, norstictic acid, oxybenzone, and paracetamol (also known as acetoaminophen).
(29) A polycyclic aromatic hydrocarbon (PAH) is an aromatic hydrocarbon composed of multiple aromatic rings. Examples of polycyclic aromatic hydrocarbons include naphthalene, anthracene, phenanthrene, phenalene, tetracene, chrysene, triphenylene, pyrene, pentacene, benzo[a]pyrene, corannulene, benzo[g,h,i]perylene, coronene, ovalene, benzo[c]fluorine, acenaphthene, acenaphthylene, benz[a]anthracene, benzo[b]fluoranthene, benzo[j]fluoranthene, benzo[k]fluoranthene, benzo[e]pyrene, cyclopenta[c,d]pyrene, dibenz[a,h]anthracene, dibenzo[a,e]pyrene, dibenzo[a,h]pyrene, dibenzo[a,i]pyrene, dibenzo[a,l]pyrene, fluoranthene, fluorine, indeno[1,2,3-c,d]pyrene, 5-methylchrysene, naphthacene, pentaphene, picene, and biphenylene.
(30) An herbicide (also known as weedkiller) is a substance that is toxic to plants and may kill, inhibit the growth of, or prevent the germination of plants. Herbicides are typically used to control the growth of or remove unwanted plants from an area of land, particularly in an agricultural context. Examples of herbicides include, but are not limited to, 2,4-D, aminopyralid, chlorsulfuron, clopyralid, dicamba, diuron, glyphosate, hexazinone, imazapic, imazapyr, methsulfuron methyl, picloram, sulfometuron methyl, triclopyr, fenoxaprop, fluazifop, quizalofop, clethodim, sethoxydim, chlorimuron, foramsulfuron, halosulfuron, nicosulfuron, primisulfuron, prosulfuron, rimsulfuron, thofensulfuron, tribenuron, imazamox, imazaquin, flumetsulam, cloransulam, thiencarbazone, fluoxpyr, diflufenzopyr, atrazine, simazine, metribuzin, bromoxynil, bentazon, linuron, glufosinate, clomazone, isoxaflutole, topramezone, mesotrione, tembotrione, acifluorfen, formesafen, lactofen, flumiclorac, flumioxazin, fulfentrazone, carfentrazone, fluthiacet-ethyl, falufenacil, paraquat, ethalfluralin, pendimethalin, trifluralin, butylate, EPTC, ecetochlor, alachlor, metolachlor, dimethenamid, flufenacet, and pyroxasulfone.
(31) A pesticide is a substance meant to prevent, destroy, or control pests including, but not limited to algae, bacteria, fungi, plants, insects, mites, snails, rodents, and viruses.
(32) A pesticide intended for use against algae is known as an algicide. Examples of algicides include benzalkonium chloride, bethoxazin, cybutryne, dichlone, dichlorophen, diuron, endothal, fentin, isoproturon, methabenthiazuron, nabam, oxyfluorfen, pentachlorophenyl laurate, quinoclamine, quinonamid, simazine, terbutryn, and tiodonium.
(33) A pesticide intended for use against bacteria is known as a bactericide. Examples of bactericides include antibiotics such as: aminoglycosides such as amikacin, gentamicin, kanamycin, neomycin, netilmicin, tobramycin, paromomycin, streptomycin, and spectinomycin; ansamycins such as geldanamycin, herbimycin, and rifaximin; carbacephems such as loracarbef; carbapenems such as ertapenem, doripenem, imipenem, and meropenem; cephalosporins such as cefadroxil, cefazolin, cephradine, cephapirin, cephalothin, cephalexin, cefaclor, cefoxitin, cefotetan, cefamandole, cefmetazole, cefonicid, cefprozil, cefuroxime, cefixime, cefdinir, cefditoren, cefoperazone, cefotaxime, cefpodoxime, cefazidime, ceftibuten, ceftizoxime, moxalactam, ceftriaxone, cefepime, cefaroline fosamil, and ceftobiprole; glycopeptides such as teicoplanin, vancomycin, telavancin, dalbavancin, and oritavancin; lincosamides such as clindamycin and lincomycin; lipopeptides such as daptomycin; macrolides such as azithromycin, clarithromycin, erythromycin, roxithromycin, telithromycin, spiramycin, and fidoxamicin; monobactams such as aztreonam; nitrofurans such as furazolidone and nitrofurantoin; oxazolidinones such as linezolid, posizolid, radezolid, and torezolid; penicillins such as amoxicillin, ampicillin, azlocillin, dicloxacillin, flucloxacillin, mezlocillin, methicillin, nafcillin, oxacillin, penicillins (including penicillin G and V), piperacillin, temocillin, and ticarcillin; polypeptides such as bacitracin, colistin, and polymyxin B; quinolones such as ciproflaxacin, enoxacin, gatifloxacin, gemifloxacin, levofloxacin, lomefloxacin, moxifloxacin, nadifloxacin, nalidixic acid, norfloxacin, ofloxacin, trovafloxacin, gepafloxacin, sparfloxacin, and temafloxacin; sulfonamides such as mafenide, sulfacetamide, sulfadiazine, sulfadithoxine, sulfamethizole, sulfamethoxazole, sulfanilamide, sulfasalazine, sulfisoxazole, and sulfonamidochrysoidine; tetracyclines such as demeclocycline, doxycycline, metacycline, minocycline, oxytetracycline, and tetracycline.
(34) A pesticide intended for use against fungi is known as a fungicide. Examples of fungicides include acibenzolar, acypetacs, aldimorph, anilazine, aureofungin, azaconazole, azithiram, azoxystrobin, benalaxyl, benodanil, benomyl, benquinox, benthiavalicarb, binapacryl, biphenyl, bitertanol, bixafen, blasticidin-S, boscalid, bromuconazole, captafol, captan, carbendazim, carboxin, carpropamid, chloroneb, chlorothalonil, chlozolinate, cyazofamid, cymoxanil, cyprodinil, dichlofluanid, diclocymet, dicloran, diethofencarb, difenoconazole, diflumetorim, dimethachlone, dimethomorph, diniconazole, dinocap, dodemorph, edifenphos, enoxastrobin, epoxiconazole, etaconazole, ethaboxam, ethirimol, etridiazole, famoxadone, fenamidone, fenarimol, fenbuconazole, fenfuram, fenhexamid, fenoxanil, fenpropidin, fenpropimorph, ferbam, fluazinam, fludioxonil, flumorph, fluopicolide, fluopyram, fluoroimide, fluoxastrobin, flusilazole, flutianil, flutolain, flopet, fthalide, furalaxyl, guazatine, hexaconazole, hymexazole, imazalil, imibenconazole, iminoctadine, iodocarb, ipconazole, iprobenfos, iprodione, iprovalicarb, siofetamid, isoprothiolane, isotianil, kasugamycin, laminarin, mancozeb, mandestrobin, mandipropamid, maneb, mepanypyrim, mepronil, meptyldinocap, mealaxyl, metominostrobin, metconazole, methafulfocarb, metiram, metrafenone, myclobutanil, naftifine, nuarimol, octhilinone, ofurace, orysastrobin, oxadixyl, oxathiapiprolin, oxolinic acid, oxpoconazole, oxycarboxin, oxytetracycline, pefurazate, penconazole, pencycuron, penflufen, penthiopyrad, phenamacril, picarbutrazox, picoxystrobin, piperalin, polyoxin, probenzole, prochloraz, procymidone, propamocarb, propiconazole, propineb, proquinazid, prothiocarb, prothioconazole, pydiflumetofen, pyraclostrobin, pyrametostrobin, pyraoxystrobin, pyrazophos, pyribencarb, pyributicarb, pyrifenox, pyrimethanil, pyrimorph, pyriofenone, pyroquilon, quinoxyfen, quintozene, sedaxane, silthiofam, simeconazole, spiroxamine, streptomycin, tebuconazole, tebufloquin, teclofthalam, tecnazene, terbinafine, tetraconazole, thiabendazole, thifluzamide, thiphanate, thiram, tiadinil, tolclosfos-methyl, folfenpyrid, tolprocarb, tolylfluanid, triadimefon, triadimenol, triazoxide, triclopyricarb, tricyclazole, tridemorph, trifloxystrobin, triflumizole, triforine, validamycin, and vinclozolin.
(35) A pesticide intended for use against plants is known as an herbicide as described above.
(36) A pesticide intended for use against insects is known as an insecticide. Examples of insecticides are: organochlorides such as Aldrin, chlordane, chlordecone, DDT, dieldrin, endofulfan, endrin, heptachlor, hexachlorobenzene, lindane, methoxychlor, mirex, pentachlorophenol, and TDE; organophosphates such as acephate, azinphos-methyl, bensulide, chlorethoxyfos, chlorpyrifos, diazinon, chlorvos, dicrotophos, dimethoate, disulfoton, ethoprop, fenamiphos, fenitrothion, fenthion, malathion, methamdophos, methidathion, mevinphos, monocrotophos, naled, omethoate, oxydemeton-methyl, parathion, phorate, phosalone, phosmet, phostebupirim, phoxim, pirimiphos-methyl, profenofos, terbufos, and trichlorfon; carbamates such as aldicarb, bendiocarb, carbofuran, carbaryl, dioxacarb, fenobucarb, fenoxycarb, isoprocarb, methomyl; pyrethroids such as allethrin, bifenthrin, cyhalothrin, cypermethrin, cyfluthrin, deltamethrin, etofenprox, fenvalerate, permethrin, phenothrin, prallethrin, resmethrin, tetramethrin, tralomethrin, and transfluthrin; neonicotinoids such as acetamiprid, clothiandin, imidacloprid, nithiazine, thiacloprid, and thiamethoxam; ryanoids such as chlorantraniliprole, cyanthaniliprole, and flubendiamide.
(37) A pesticide intended for use against mites is known as a miticide. Examples of miticides are permethrin, ivermectin, carbamate insecticides as described above, organophosphate insecticides as described above, dicofol, abamectin, chlorfenapyr, cypermethrin, etoxazole, hexythiazox, imidacloprid, propargite, and spirotetramat.
(38) A pesticide intended for use against snails and other mollusks is known as a molluscicide. Examples of molluscicides are metaldehyde and methiocarb.
(39) A pesticide intended for use against rodents is known as a rodenticide. Examples of rodenticides are warfarin, coumatetralyl, difenacoum, brodifacoum, flocoumafen, bromadiolone, diphacinone, chlorophacinone, pindone, difethialone, cholecalciferol, ergocalciferol, ANTU, chloralose, crimidine, 1,3-difluoro-2-propanol, endrin, fluroacetamide, phosacetim, pyrinuron, scilliroside, strychnine, tetramethylenedisulfotetramine, bromethalin, 2,4-dinitrophenol, and uragan D2.
(40) A pesticide intended for use against viruses is known as a virucide. Examples of virucides are cyanovirin-N, griffithsin, interferon, NVC-422, scytovirin, urumin, virkon, zonroz, and V-bind viricie.
(41) A persistent organic contaminant is a toxic organic chemical that adversely affects human and environmental health, can be transported by wind and water, and can persist for years, decades, or centuries owing to resistance to environmental degradation by natural chemical, biological, or photolytic processes. Persistent organic contaminants are regulated by the United Nations Environment Programme 2001 Stockholm Convention on Persistent Organic Contaminants. Examples of persistent organic contaminants are Aldrin, chlordane, dieldrin, endrin, heptachlor, hexachlorobenzene, mirex, toxaphene, polychlorinated biphenyl (PCBs), dichlorodiphenyltrichloroethane (DDT), dioxins, polychlorinated dibenzofurans, chlordecone, hexachlorocyclohexane (- and -), hexabromodiphenyl ether, lindane, pentachlorobenzene, tetrabromodiphenyl ether, perfluorooctanesulfonic acid, endosulfans, and hexabromocyclododecane.
(42) As used herein, the term unimodal refers to a distribution or pattern that has a single peak or mode. In the context of particle size or material properties, it indicates that the sample consists of particles or components that are primarily of one size or characteristic, rather than varying widely in size or composition.
(43) As used herein, the term spinel interplanar spacing refers to the distance between parallel planes of atoms in the crystal structure of a spinel material. Spinel is a type of mineral with a specific crystalline arrangement, represented by the general formula AB.sub.2O.sub.4, where A and B are metal ions. The interplanar spacing is crucial for understanding the material's structural properties and is typically measured using X-ray diffraction (XRD) techniques.
(44) A weight percent of a component, unless specifically stated to the contrary, is based on the total weight of the formulation or composition in which the component is included. For example, if a particular element or component in a composition or article is said to have 5 wt. %, it is understood that this percentage is in relation to a total compositional percentage of 100%.
(45) The present disclosure is intended to include all hydration states of a given compound or formula, unless otherwise noted or when heating a material.
(46) In addition, the present disclosure is intended to include all isotopes of atoms occurring in the present compounds and complexes. Isotopes include those atoms having the same atomic number but different mass numbers. By way of general example, and without limitation, isotopes of hydrogen include deuterium and tritium, and isotopes of carbon include .sup.13C and .sup.14C. Isotopes of oxygen include .sup.16O, .sup.17O, and .sup.18O. Isotopically-labeled compounds of the disclosure may generally be prepared by conventional techniques known to those skilled in the art or by processes analogous to those described herein, using an appropriate isotopically-labeled reagent in place of the non-labeled reagent otherwise employed.
(47) Aspect of the present disclosure is directed to a method of forming a nanocomposite of graphitic carbon nitride (g-C.sub.3N.sub.4), molybdenum oxide (MoO.sub.3), and magnesium aluminate (MgAl.sub.2O.sub.4) (g-C.sub.3N.sub.4@MoO.sub.3/MgAl.sub.2O.sub.4). Each component of the nanocomposite, when used in appropriate ratios, is effective in the removal of organic contaminants in water with high efficiency and removal activity.
(48) A nanocomposite (g-C.sub.3N.sub.4@MoO.sub.3/MgAl.sub.2O.sub.4) including g-C.sub.3N.sub.4, MoO.sub.3, and MgAl.sub.2O.sub.4 is described. The nanocomposite includes a coating of g-C.sub.3N.sub.4 on MoO.sub.3 and MgAl.sub.2O.sub.4. The g-C.sub.3N.sub.4, MoO.sub.3, and MgAl.sub.2O.sub.4 are present in the nanocomposite in a mass relationship to each other in a range of from 5 to 15:2 to 7:75 to 95, preferably 7 to 13:3 to 6:80 to 90, and preferably 9 to 11:4 to 5:84 to 86. The g-C.sub.3N.sub.4, MoO.sub.3, and MgAl.sub.2O.sub.4 may be present in the nanocomposite in a mass relationship to each other of 10:5:85, while tolerable variations of any of these values may be 2.5, 2, 1.5, 1, 0.75, 0.5, 0.25, 0.1, 0.5, or 0.1. When each component of the nanocomposite is used in desired weight ratios, the nanocomposite exhibits excellent performance in photodegradation of organic pollutants owing to its enhanced catalytic properties, high surface reactivity, and efficient adsorption, making it suitable for applications in environmental remediation, energy production, and biomedical treatments.
(49) The nanocomposite may contain g-C.sub.3N.sub.4 in an amount ranging from 5 to 15 wt. %, including 5 to 7 wt. %, 7 to 9 wt. %, 9 to 11 wt. %, 11 to 13 wt. %, and 13 to 15 wt. % based on the total weight of the nanocomposite. The nanocomposite may contain 102.5, 2, 1.5, 1, 0.5, or 0.1 wt. % of graphite-phase carbon nitride (g-C.sub.3N.sub.4).
(50) The nanocomposite may contain MO.sub.3 in an amount ranging from 2 to 7 wt. %, including 3 to 7 wt. %, 7 to 11 wt. %, 11 to 13 wt. %, 13 to 15 wt. %, and 15 to 17 wt. % based on the total weight of the nanocomposite. The nanocomposite may contain 52.5, 2, 1.5, 1, 0.5, or 0.1 wt. % of MO.sub.3.
(51) The nanocomposite may contain magnesium aluminum oxide (MgAl.sub.2O.sub.4) in an amount ranging from 75 to 95 wt. %, including 80 to 82 wt. %, 82 to 84 wt. %, 84 to 86 wt. %, 86 to 88 wt. %, and 88 to 90 wt. % based on the total weight of the nanocomposite. The nanocomposite contains 852.5, 2, 1.5, 1, 0.5, or 0.1 wt. % of magnesium aluminum oxide (MgAl.sub.2O.sub.4).
(52) The nanocomposite obtained may include no molybdenum sulfide (MoS.sub.2) and/or sulfide. The nanocomposite obtained may include no molybdenum sulfide (MoS.sub.2), or may exclude added MoS.sub.2, such as no detectable amounts thereof by, e.g., combustion analysis and/or spectroscopic analysis (e.g., UV-vis, fluorescence, XPS, IR, ESR, etc.). The nanocomposite obtained may include no sulfide, exclude added sulfide or metal sulfide, such as no detectable amounts thereof by, e.g., combustion analysis and/or spectroscopic analysis (e.g., UV-vis, fluorescence, XPS, IR, ESR, etc.). The nanocomposite obtained may include no sulfide, particularly no added Mo.sub.2S and/or sulfide. The nanocomposite may include no more than 0.1, 0.01, 0.001, or 0.0001 wt. % Mo.sub.2S and/or sulfide, e.g., no detectable Mo.sub.2S and/or sulfide, based on total nanocomposite weight.
(53) The nanocomposite obtained may include less than 10 wt. % Co, preferably less than 9 wt. % Co, preferably less than 8 wt. % Co, preferably less than 7 wt. % Co, preferably less than 6 wt. % Co, preferably less than 5 wt. % Co, preferably less than 4 wt. % Co, preferably less than 3 wt. % Co, preferably less than 2 wt. % Co, and preferably less than 1 wt. % Co, relative to total nanocomposite weight. The nanocomposite obtained may include less than 1 wt. % Co, preferably less than 0.9 wt. % Co, preferably less than 0.8 wt. % Co, preferably less than 0.7 wt. % Co, preferably less than 0.6 wt. % Co, preferably less than 0.5 wt. % Co, preferably less than 0.4 wt. % Co, preferably less than 0.3 wt. % Co, preferably less than 0.2 wt. % Co, preferably less than 0.1 wt. % Co, preferably less than 0.05 wt. % Co, and preferably less than 0.01 wt. % Co. The nanocomposite may contain no added Co (e.g., only inevitable traces). The exclusion of MoS.sub.2 and sulfides and the minimization of Co content in the nanocomposite can ensure the preservation of its desired catalytic properties, stability, and reactivity. The absence of MoS.sub.2 and sulfide may prevent undesirable side reactions, while limiting the Co content to less than 1 wt. % prevents interference and potential toxicity, thereby potentially enhancing the performance and applicability of the nanocomposite. In some embodiments, the nanocomposite obtained comprises no more than 1 wt. % potassium, preferably less than 0.9 wt. % potassium, preferably less than 0.8 wt. % potassium, preferably less than 0.7 wt. % potassium, preferably less than 0.6 wt. % potassium, preferably less than 0.5 wt. % potassium, preferably less than 0.4 wt. % potassium, preferably less than 0.3 wt. % potassium, preferably less than 0.2 wt. % potassium, preferably less than 0.1 wt. % potassium, preferably less than 0.05 wt. % potassium, and preferably less than 0.01 wt. % potassium. In some embodiments, the nanocomposite obtained comprises no more than 1 wt. % iron, preferably less than 0.9 wt. % iron, preferably less than 0.8 wt. % iron, preferably less than 0.7 wt. % iron, preferably less than 0.6 wt. % iron, preferably less than 0.5 wt. % iron, preferably less than 0.4 wt. % iron, preferably less than 0.3 wt. % iron, preferably less than 0.2 wt. % iron, preferably less than 0.1 wt. % iron, preferably less than 0.05 wt. % iron, and preferably less than 0.01 wt. % iron. In some embodiments, nanocomposite obtained comprises no more than 1 wt. % zinc, preferably less than 0.9 wt. % zinc, preferably less than 0.8 wt. % zinc, preferably less than 0.7 wt. % zinc, preferably less than 0.6 wt. % zinc, preferably less than 0.5 wt. % zinc, preferably less than 0.4 wt. % zinc, preferably less than 0.3 wt. % zinc, preferably less than 0.2 wt. % zinc, preferably less than 0.1 wt. % zinc, preferably less than 0.05 wt. % zinc, and preferably less than 0.01 wt. % zinc. In some embodiments, the nanocomposite obtained comprises no more than 1 wt. % of carbonaceous material, preferably less than 0.9 wt. % g-C.sub.3N.sub.4, preferably less than 0.8 wt. % g-C.sub.3N.sub.4, preferably less than 0.7 wt. % g-C.sub.3N.sub.4, preferably less than 0.6 wt. % g-C.sub.3N.sub.4, preferably less than 0.5 wt. % g-C.sub.3N.sub.4, preferably less than 0.4 wt. % g-C.sub.3N.sub.4, preferably less than 0.3 wt. % g-C.sub.3N.sub.4, preferably less than 0.2 wt. % g-C.sub.3N.sub.4, preferably less than 0.1 wt. % g-C.sub.3N.sub.4, preferably less than 0.05 wt. %, and preferably less than 0.01 wt. % of carbonaceous material besides the graphitic carbon nitride. The nanocomposite obtained may include less than 10 wt. % Co, or less than 7.5, 5, 2.5, 1, 0.5, 0.25, 0.1, 0.01, 0.001, 0.0001, or 0.00001 wt. % Co or any of the above-mentioned metals, relative to total nanocomposite weight.
(54) The nanocomposite may be porous. A porous material is the one that forms a porous bulk solid. Pores may be micropores, mesopores, macropores, and/or a combination thereof. The pores exist in the bulk material, not necessarily in the molecular structure of the material. The term microporous means that nanocomposite have pores with an average pore width (i.e. diameter) of less than 2 nm, e.g., in a range with an upper limit of 2, 1, 0.9, 0.75, 0.5, 0.25, 0.1, 0.05, or 0.01 nm, and/or a lower limit of 0.00001, 0.0001, 0.001, 0.01, 0.1, 0.25, 0.5, 0.75, or 1 nm. The term mesoporous means the pores of the nanocomposite have an average pore width of 2 to 50 nm, though this may include subranges within this general range, e.g., a minimum diameter of 2, 3, 5, 10, 15, 20, 25, or 35 m, and/or a maximum diameter of 50, 45, 40, 35, 30, 25, 20, 15, or 10 nm. The term macroporous means the pores of nanocomposite have an average pore width larger than 50 nm, e.g., at least 55, 75, 100, 250, 500, 750, or 1000 nm. Pore size may be determined by methods including, but not limited to, gas adsorption (e.g. N.sub.2 adsorption), mercury intrusion porosimetry, and imaging techniques such as scanning electron microscopy (SEM), and X-ray computed tomography (XRCT).
(55) The Brunauer-Emmett-Teller (BET) surface area of the nanocomposite may be in a range of from 8 to 12 square meters per gram (m.sup.2/g), preferably 9 to 11 m.sup.2/g, and preferably 10 m.sup.2/g. The surface area on the nanocomposite may be 10.12.5, 2, 1.5, 1, 0.75, 0.5, 0.25, 0.2, or 0.1 m.sup.2/g. The BET hypothesis is the foundation for a significant analysis method for determining the specific surface area of a material. It attempts to explain the physical adsorption of gas molecules on a solid surface. Specific surface area is a property of solids, which is the total surface area of a material per unit of mass, solid or bulk volume, or cross-sectional area. Pore diameter, pore volume, and BET surface area may be measured by gas adsorption analysis, preferably N.sub.2 adsorption analysis (e.g., N.sub.2 adsorption isotherms).
(56) The average pore distribution of the nanocomposite may include, but is not limited to, crystalline average pore distribution, bimodal, trimodal, multimodal, narrow, broad, and Gaussian. The average pore distribution of nanocomposite may be (only) unimodal, indicating a single dominant pore size within the material. This unimodal distribution suggests that the nanocomposites possess a relatively narrow pore size range, resulting in more uniform pore structures and enhancing specific properties such as adsorption capacity, catalytic activity, or surface reactivity.
(57) The average pore diameter of the nanocomposite, according to Barrett-Joyner-Halenda (BJH) measurement method, may be in a range of from 5 to 15 nm, preferably 6 to 14 nm, preferably 7 to 13 nm, preferably 8 to 12 nm, and preferably 9 to 11 nm. The nanocomposite may have an average pore diameter of 8.342.5, 2, 1.5, 1, 0.5, 0.1, 0.05, 0.025, or 0.01 nm nm.
(58) The average pore volume of the nanocomposite, according to the BJH measurement method, may be in a range of from 0.01 to 0.5 cm.sup.3/g, preferably 0.02 to 0.4 cm.sup.3/g, preferably 0.03 to 0.3 cm.sup.3/g, preferably 0.04 to 0.2 cm.sup.3/g, and preferably 0.05 to 0.1 cm.sup.3/g. The average pore volume of the nanocomposite may be 0.033 cm.sup.3/g0.1, 0.05, 0.025, or 0.01 cm.sup.3/g.
(59) The mass relationship of the nanocomposite may be in a range of from 9 to 11:4 to 6:84 to 86, and preferably 9.5 to 10.5:4.5 to 5.5:84.5 to 85.5. The mass relationship of the nanocomposite may be 10:5:85, wherein the ratios may vary by 3, 2.5, 2, 1.5, 1, 0.5, 0.25, or 0.1.
(60) The nanocomposite may have a (311) spinel interplanar spacing in a range of from 0.205 to 0.285 nm, preferably 0.215 to 0.275 nm, preferably 0.225 to 0.265 nm, and preferably 0.235 to 0.255 nm; (411) MoO.sub.3 interplanar spacing in a range of from 0.150 to 0.230 nm, preferably 0.160 to 0.220 nm, preferably 0.170 to 0.210 nm, and preferably 0.180 to 0.200 nm; (511) spinel interplanar spacing in a range of from 0.115 to 0.195 nm, preferably 0.125 to 0.185 nm, preferably 0.135 to 0.175 nm, and preferably 0.145 to 0.165 nm; (311) MgO interplanar spacing in a range of from 0.087 to 0.167 nm, preferably 0.097 to 0.157 nm, preferably 0.107 to 0.147 nm, and preferably 0.117 to 0.137 nm; and/or (622) spinel interplanar spacing in a range of from 0.080 to 0.160 nm, preferably 0.090 to 0.150 nm, preferably 0.100 to 0.140 nm, and preferably 0.110 to 0.130 nm, according to SAED.
(61) The nanocomposite may have a (311) spinel interplanar spacing of 0.2452, 1, 0.5, or 0.1% nm, (411) MoO.sub.3 interplanar spacing of 0.192% nm, (511) spinel interplanar spacing of 0.1552, 1, 0.5, or 0.1% nm, (311) MgO interplanar spacing of 0.1272, 1, 0.5, or 0.1% nm, and/or (622) spinel interplanar spacing of 0.122, 1, 0.5, or 0.1% nm, according to selected area diffraction (SAED).
(62) The XRD spectrum of the nanocomposite under Cu-filtered CuK radiation (1.5418 A) powered at 45 kilovolt (kV) and 10 milliampere (mA) may have 2 peaks of an MoO.sub.3 hexagonal phase at 18.71, 28.71, 33.01, 33.81, 36.81, and/or 42.81, an MgAl.sub.2O.sub.4 spinel phase at 19.31, 36.81, 44.61, 59.31, and/or 65.01; an MgO cubic phase at 42.81, 62.21, and/or 74.61; and g-C.sub.3N.sub.4-related diffractions at 27.81, 36.81, 44.61, and/or 59.31. No more than 1% relative intensity Al.sub.2O.sub.3, e.g., less than 0.5, 0.25, 0.1, or 0.1%, may be detected in the XRD spectrum. The minimal presence of Al.sub.2O.sub.3 (less than 1%) in the nanocomposite is critical to maintaining its enhanced catalytic properties, high surface reactivity, and efficient adsorption. This may ensure desired performance in environmental remediation, energy production, and biomedical applications, free from interference by less reactive Al.sub.2O.sub.3 phases. The MoO.sub.3 in the nanocomposite may have a hexagonal crystal structure. In alternate embodiments, MoO.sub.3 may exist in other crystal phases including cubic, monoclinic, tetragonal, rhombohedral, and orthorhombic phases. The hexagonal phase of MoO.sub.3 may be represented by diffractions at 2.6 values of 18.7, 28.7, 33.0, 33.8, 36.8, and/or 42.8. At 2 values of 42.8, 62.2, and/or 74.6, the cubic phase of MgO is detected. At 2 values of 19.3, 36.8, 44.6, 59.3, and/or 65.01, MgAl.sub.2O.sub.4 spinel is detected. At 2 values of 27.8, 36.8, 44.6, and/or 59.3 g-C.sub.3N.sub.4-related diffractions is detected. MgAl.sub.2O.sub.4 may have a spinel phase, for example at least 95, 97.5, 99, 99.9%, or exclusively. The spinel phase is a mixed oxide with the general formula AB.sub.2O.sub.4, including one divalent cation (A.sup.2+) and two trivalent cations (B.sup.3+). The unit cell consists of a face-centered cubic arrangement of oxygen ions, containing 32 O.sup.2 ions, with 64 tetrahedral and 32 octahedral sites occupied by A.sup.2+ and B.sup.3+ cations. When one half of the octahedral interstices are occupied by B.sup.3+ cations and one-eighth of the tetrahedral sites are occupied by A.sup.2+ cations, the spinel phase is termed normal. Conversely, when tetrahedral sites are occupied by half of the B.sup.3+ and octahedral sites by the other half along with A.sup.2+, the spinel phase is termed inverse.
(63) The spinel phase with the chemical formula MgAl.sub.2O.sub.4 is a mineral type of this oxide family. MgAl.sub.2O.sub.4 has been widely used in various applications, such as in metallurgical, electrochemical, radio-technical, and chemical industrial fields owing to its high thermal stability (melting point at 2135 C., high hardness (16 gigapascal (GPa)), high mechanical resistance, high resistance against chemical attack, wide band gap energy, high electrical resistivity, relatively low thermal expansion coefficient (9.Math.10.sup.6 m/m C.) between 3 and 1400 C., low dielectric constant, low density (3.58 gram per cubic centimeter (g/cm.sup.3)), high thermal shock resistance, hydrophobicity, and low surface acidity.
(64) The nanocomposite may consist essentially of sheet morphologies, i.e., such that at least 98% of the adsorption capacity is retained relative to exclusive sheet morphology, preferably nanosheets, although other morphologies such as nanowires, nanospheres, nanocrystals, nanorectangles, nanotriangles, nanopentagons, nanohexagons, nanoprisms, nanodisks, nanocubes, nanoribbons, nanoblocks, nanotoroids, nanodiscs, nanobarrels, nanogranules, nanowhiskers, nanoflakes, nanofoils, nanopowders, nanoboxes, nanobeads, nanobelts, nano-urchins, nanoflowers, nanostars, tetrapods, and their mixtures thereof are also possible. Any of these may be excluded from the composition, however. The nanocomposite may have a structure including a dispersion of homogeneous spherical metal oxides nanoparticles on a two-dimensional porous structure including curled and wrinkled nanosheets and platelets of the g-C.sub.3N.sub.4.
(65) A method 50 for removing contaminants from water is described. The order in which the method 50 is described is not intended to be construed as a limitation, and any number of the described method steps can be combined to implement the method 50. Additionally, individual steps may be removed or skipped from the method 50 without departing from the spirit and scope of the present disclosure.
(66) At step 52, the method 50 includes contacting contaminated water, comprising a heavy metal and/or an organic pollutant, with the nanocomposite, thereby adsorbing the heavy metal and/or the organic pollutant onto the nanocomposite, as an adsorbed material. This interaction facilitates the adsorption of heavy metals and/or organic pollutants onto the nanocomposite. In some embodiments, the nanocomposite preferentially adsorbs charged indigo-derivative dyes to radioactive metals. The nanocomposite may adsorb organic dyes as the organic pollutant. The organic pollutant may be a dye, a phenol, a polycyclic aromatic hydrocarbon, an herbicide, a pesticide, a persistent organic contaminant, or the like. The removed dye may be indigo carmine dye. The dye or organic pollutant may also be decomposed by irradiation of the nanocomposite in its presence.
(67) The organic pollutant may be adsorbed, e.g., as an indolinone sulfonate substructure (e.g., Indigo carmine), in a mass ratio of 0.01 to 0.2 parts, preferably 0.05 parts, preferably 0.1 parts, preferably 0.15 parts, preferably 0.2 parts, of the organic molecules per part of the nanocomposite. The organic pollutant adsorbed may include an indolinone sulfonate substructure (Indigo carmine) in a mass ratio of 0.0982 parts of the organic molecules per part of the nanocomposite.
(68) The average adsorption rate of the organic pollutant on the nanocomposite may be in a range of from 3 to 4 mg/min, preferably 3.2 to 4 mg/min, preferably 3.6 to 4 mg/min, preferably 3.8 to 4 mg/min from an initiation of the contacting over 30 minutes. In some embodiment, at least 70 mg, preferably at least 75, at least 80 mg, at least 85 mg, at least 90 mg, at least 95 mg of the organic pollutant is adsorbed per gram of nanocomposite within 30 minutes of the contacting the organic pollutant with the nanocomposite. 98.25, 2.5, 2, 1.5, 1, 0.75, 0.5, 0.25, or 0.1 mg per gram of nanocomposite may be adsorbed from the water within 30 minutes of contacting the organic pollutant with the nanocomposite. The adsorption profile may be twice, thrice, 3.5-fold, etc., as fast over the first 30 minutes than over the subsequent 10 minutes, then again , , or , etc., as fast over the subsequent 10 minutes.
(69) The contaminant may be a heavy metal. Suitable examples of the heavy metals include, but are not limited to, Cd, Cr, Cu, Fe, Pb, Ni, Ag, Zn, and/or U. The heavy metal may be uranium. Contacting the contaminated water with the nanocomposite results in removal of no more than 0.001 wt. % of uranium, or other heavy metal(s), preferably no more than 0.0009 wt. % of uranium, preferably no more than 0.0008 wt. % of uranium, preferably no more than 0.0006 wt. % of uranium, preferably no more than 0.0005 wt. % of uranium, preferably no more than 0.0002 wt. % of uranium, based on total water weight.
(70) At step 54, the method 50 includes removing the adsorbed material from the contaminated water, thereby reducing the concentration of the heavy metal in the contaminated water by at least 2 wt. %. The adsorbed materials may be separated from the contaminated water and reducing a concentration of the heavy metal in the contaminated water by at least 2 wt. %, preferably at least 2.5 wt. %, preferably at least 3 wt. %, preferably at least 3.5 wt. %, preferably at least 4 wt. %, preferably at least 5 wt. %.
(71) Fabrication of g-C.sub.3N.sub.4@MoO.sub.3/MgAl.sub.2O.sub.4 (10:5:8 5, Wt. %) Nanohybrid
(72) According to the present disclosure, magnesium nitrate, and aluminum nitrate can be added together in one beaker with ammonium molybdate, in predetermined amounte.g., stoichiometric, to produce a 10% MoO.sub.3/MgAl.sub.2O.sub.4. Further, about 10 g of menthol (e.g., 100:1 to 1:1, 25:1 to 1:1, or 10:1 to 1:1, by weight) as fuel was added to the beaker, followed by 30 milliliters (mL) of distilled water. The beaker was heated till a clear solution was obtained, heated further till dryness. The product was ground in a mortar, transferred to a 150 mL porcelain dish, and calcined at 700 C. for 3.0 hours (h). Furthermore, the 10% MoO.sub.3/MgAl.sub.2O.sub.4 product was cooled down to room temperature and weighed, ground with urea in an amount suitable (depending upon the reaction conditions, this may be 5, 10, 15, 20, 25, 33, 50, 100, 150, 250, 500, or 1000 parts by weight of urea to 100 parts by weight of 10% MoO.sub.3/MgAl.sub.2O.sub.4, and optionally no more than 100,000, 50,000, 25,000, 10,000, 5,000, 1,000, 750, 500, 400, 333, 250, 125, 100, 75, 50, or 25 parts by weight urea to 100 parts) to produce g-C.sub.3N.sub.4@MoO.sub.3/MgAl.sub.2O.sub.4 (10:5:85, wt. %) nanohybrid. The quadruple mixture was returned, and heated to 600 C. for 1.0 h in a covered porcelain crucible, and subsequently, the g-C.sub.3N.sub.4@MoO.sub.3/MgAl.sub.2O.sub.4 (10:5:85, wt. %) nanohybrid was collected.
(73) X-ray diffraction (XRD) was used to identify the crystalline states in each specimen studied, employing the JDX-8030 X-ray (JEOL), made in Japan. Cu-filtered Cu-K radiation (1.5418 angstroms ()) powered at 45 kV and 10 mA was used to run the patterns. The specimens were tested at ambient temperatures in a range of 2=5 to 80. The surface morphologies of the obtained samples were analyzed by transmission electron microscopy (TEM), selected area electron diffraction (SAED), and high-resolution transmission electron microscopy (HRTEM) images, obtained using a Tecnai-G20 (USA) transmission electron microscope with a 200 kV speed voltage. Nitrogen (N.sub.2) adsorption isotherm obtained at 77 K using Micrometrics ASAP 2020 Brnauer-Emmett-Teller (BET) analyzer was used to calculate the surface characteristics, specifically the BET surface area, total pore volume (Vp), and mean pore radius (r). Before beginning the measurement, the samples were outgassed for three h at 200 C. with a decreased pressure of 10.sup.5 Torr.
(74) XRD can be used to examine the crystallinity and phase identification of the g-C.sub.3N.sub.4@MoO.sub.3/MgAl.sub.2O.sub.4 catalyst. A high crystalline nature of the powders may be indicated by the strong peaks. MoO.sub.3, MgO, MgAl.sub.2O.sub.4, and g-C.sub.3N.sub.4 phases are detected when the diffraction patterns are compared to the normal JCPDS cards. The hexagonal phase of MoO.sub.3 is represented by diffractions at 2.6 values of 18.7, 28.7, 33.0, 33.8, 36.8, and 42.8 (JCPDS No. 00-021-0569). At 20 values of 42.8, 62.2, and 74.6, the cubic phase of MgO (JCPDS card, No. 45-0946) was detected. At 20 values of 19.3, 36.8, 44.6, 59.3, and 65.01, MgAl.sub.2O.sub.4 spinel was discovered. The cubic phase of MgAl.sub.2O.sub.4 spinel is identified by these diffractions (JCPDS card, No. 21-1152). It was previously reported that MgO was present together with the MgAl.sub.2O.sub.4 spinel phase. The g-C.sub.3N.sub.4-related diffractions were detected at 27.8, 36.8, 44.6, and 59.3. The production of g-C.sub.3N.sub.4@MoO.sub.3/MgAl.sub.2O.sub.4 was shown by the absence of additional phases (such as Al.sub.2O.sub.3).
(75) Further, TEM images of a g-C.sub.3N.sub.4@MoO.sub.3/MgAl.sub.2O.sub.4 within the claims shows the dispersion of homogeneous spherical metal oxides nanoparticles with size 9.4 nm on two-dimensional porous structure constructed with curled and wrinkled nanosheets and platelets of the g-C.sub.3N.sub.4. The corresponding SAED pattern reveals diffraction spots with interplanar spacing of 0.245 nm, 0.19 nm, 0.155 nm, 0.127 nm, 0.12 nm, due to (311, spinel), (411, MoO.sub.3), (511, spinel), (311, MgO), and (622, spinel) diffraction planes. The corresponding HRTEM of the composite shows a plane spacing of 0.34 nm related to the (002) of CN, where 0.25 nm and 0.24 nm relates to (311) planes of spinel as well as (410) of MoO.sub.3, and 0.32 nm relates to (210) plane of MoO.sub.3, characterizing the heterostructure formation, as shown in
(76) The nitrogen sorption isotherm of the composite relates to type IV with clear hysteresis loop, indicating the formation of mesoporous structures. However, shifting the loop to a relatively lower pressure (P/P=0.51 to 1) suggests a decrease in the size of the mesopores, which may result from the deposition of metal oxides particles in the wide pores of g-C.sub.3N.sub.4. Furthermore, the BET surface area of the g-C.sub.3N.sub.4@MoO.sub.3/MgAl.sub.2O.sub.4 sample was calculated to be 10.1 m.sup.2/g. The marked high specific surface area reflects the good dispersion of the aforementioned metal oxides nanoparticles on g-C.sub.3N.sub.4. Moreover, the pore size distribution curves, plotted using the BJH method, for the g-C.sub.3N.sub.4@MoO.sub.3/MgAl.sub.2O.sub.4 sample exhibited unimodal distribution with average pore diameters maximized at 8.34 nm and pore volume of 0.033 cm.sup.3/g. The isotherm belongs to the category H3 type of pores, which do not exhibit limiting adsorption at high P/P and may arise due to aggregation of plate-like particles giving rise to slit-shaped pores. The aforementioned observation indicates that the assembly of g-C.sub.3N.sub.4@MoO.sub.3/MgAl.sub.2O.sub.4 composite provoked a mesoporous array.
(77) The following examples are provided solely for illustration and are not to be construed as limitations of the present disclosure, as many variations thereof are possible without departing from the spirit and scope of the present disclosure.
EXAMPLES
(78) The following examples demonstrate a method of removing contaminants from water using a nanocomposite. The examples are provided solely for illustration and are not to be construed as limitations of the present disclosure, as many variations thereof are possible without departing from the spirit and scope of the present disclosure.
Example 1: Fabrication of g-C.SUB.3.N.SUB.4.@MoO.SUB.3./MgAl.SUB.2.O.SUB.4 .(10:5:8 5, Wt. %) Nanocomposite
(79) According to the present disclosure, magnesium nitrate, and aluminum nitrate were added together in one beaker with ammonium molybdate, in predetermined amount (here stoichiometric), to produce a 10% MoO.sub.3/MgAl.sub.2O.sub.4. Further, about 10 g of menthol as fuel was added to the beaker, followed by 30 mL of distilled water. The beaker was heated till a clear solution was obtained, heated further till dryness. The product was ground in a mortar, transferred to a 150 mL porcelain dish, and calcined at 700 C. for 3.0 hours. Furthermore, the 10% MoO.sub.3/MgAl.sub.2O.sub.4 product was cooled down to room temperature and weighed, ground with urea in an amount suitable (here, 2 g urea to 20 g of the 10% V.sub.2O.sub.5/MgAl.sub.2O.sub.4 product, but depending upon the reaction conditions, this may be 5, 10, 15, 20, 25, 33, 50, 100, 150, 250, 500, or 1000 parts by weight of urea to 100 parts by weight of 10% V.sub.2O.sub.5/MgAl.sub.2O.sub.4, and optionally no more than 100,000, 50,000, 25,000, 10,000, 5,000, 1,000, 750, 500, 400, 333, 250, 125, 100, 75, 50, 25, 20, 15, or 10 parts by weight urea to 100 parts) to produce g-C.sub.3N.sub.4@MoO.sub.3/MgAl.sub.2O.sub.4 (10:5:85, wt. %) nanohybrid/nanocomposite. The quadruple mixture was returned, and heated to 600 C. for 1.0 h in a covered porcelain crucible, and subsequently, the g-C.sub.3N.sub.4@MoO.sub.3/MgAl.sub.2O.sub.4 (10:5:85, wt. %) nanocomposite was collected.
Example 2: Characterization
(80) According to the present disclosure, X-ray diffraction (XRD) was used to identify the crystalline states in each specimen studied, employing the JDX-8030 X-ray (JEOL), made in Japan. Cu-filtered Cu-K radiation (1.5418 ) powered at 45 kV and 10 mA was used to run the patterns. The specimens were tested at ambient temperatures in a range of 2=5 to 80. The surface morphologies of the obtained samples were analyzed by transmission electron microscopy (TEM), selected area electron diffraction (SAED), and high-resolution transmission electron microscopy (HRTEM) images, obtained using a Tecnai-G20 (USA) transmission electron microscope with a 200 kV speed voltage. Nitrogen (N.sub.2) adsorption isotherm obtained at 77 K using Micrometrics ASAP 2020 Brnauer-Emmett-Teller (BET) analyzer was used to calculate the surface characteristics, specifically the BET surface area, total pore volume (Vp), and mean pore radius (r).
RESULTS AND DISCUSSION
(81) As mentioned above, XRD was used to examine the crystallinity and phase identification of the g-C.sub.3N.sub.4@MoO.sub.3/MgAl.sub.2O.sub.4 catalyst, the results are depicted in
(82) Further, TEM images of g-C.sub.3N.sub.4@MoO.sub.3/MgAl.sub.2O.sub.4 nanocomposite are shown in
(83) According to the present disclosure,
(84) An accurate mass of 50 mg of the g-C.sub.3N.sub.4@MoO.sub.3/MgAl.sub.2O.sub.4 was transferred to a 120 mL beaker to which 100 mL of 50 mg/L indigo carmine dye was added, and an aliquot was picked at serial time intervals till about 2.0 hours. The portion of the solution was filtered through a 0.22 m syringe filter, and the absorbance of the dye in the solution was measured with a ultraviolet visible (UV-vis) spectrophotometer, as shown in
(85) Numerous modifications and variations of the present disclosure are possible in light of the above teachings. It is therefore to be understood that within the scope of the appended claims, the invention may be practiced otherwise than as specifically described herein.