304 tube capillary Nanocomposites oo ku salaysan Tungsten Oxide/Fullerene sida Electrocatalysts iyo Inhibitors of Parasitic VO2+/VO2+ Reactions in Mixed Acids

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Birta Aan Lahayn 304 Tubbada Gariireedka Kiimikada

304 Steel Coil Tube waa nooc ka mid ah daawaha chromium-nickel austenitic.Marka loo eego soo saaraha 304 Coil Tube manufacturer, qaybta ugu muhiimsan ee ku jirta waa Cr (17%-19%), iyo Ni (8%-10.5%).Si loo hagaajiyo caabbinta daxalka, waxaa jira xaddi yar oo Mn (2%) iyo Si (0.75%).

Qalabka Makaanikada ah ee Birta 304 Gariiradda Tubada

Qalabka farsamada ee 304 tuubada gariiradda birta ah ee birta ah waa sida soo socota:

• Xoogga xajinta: ≥515MPa
• Awoodda wax-soo-saarka: ≥205MPa
• Kordhinta: ≥30%

Codsiyada & Isticmaalka Tuubbada Gariirada 304 ee birta ah

Qiimaha aadka u sarreeya ee baytariyada qulqulka qulqulka ee vanadium redox (VRFBs) ayaa xaddidaya isticmaalkooda baahsan.Kinetics-ka falcelinta elektiroonigga ah waa in la hagaajiyaa si loo kordhiyo cufnaanta awoodda iyo waxtarka tamarta VRFB, si loo yareeyo kWh qiimaha VRFB.Shaqadan, hydrothermally synthesized hydrated tungsten oxide (HWO) nanoparticles, C76 iyo C76 / HWO, ayaa lagu shubay korantada marada kaarboonka waxaana lagu tijaabiyay sida korantada falcelinta VO2 +/VO2+.Sawirka qiiqa hawada ee mikroskoobyada elektaroonigga ah (FESEM), tamarta kala firdhisa raajada spectroscopy (EDX), mikroskoobyada gudbinta xallinta sare ee elektiroonigga ah (HR-TEM), Diffraction X-ray (XRD), X-ray photoelectron spectroscopy (XPS), infrared Fourier beddel Spectroscopy (FTIR) iyo cabbirada xagasha xidhiidhka.Waxaa la ogaaday in ku darida C76 fullerene ee HWO ay kor u qaadi karto kinetics ee electrode marka loo eego VO2 +/VO2 + falcelinta redox by kordhinta conductivity iyo bixinta oksijiin-ku jira kooxo functional ah oogada.Isku-dhafka HWO/C76 (50 wt% C76) ayaa cadeeyay inuu yahay midka ugu habboon falcelinta VO2 +/VO2+ ee leh ΔEp ee 176 mV marka la barbar dhigo 365 mV ee marada kaarboonka ee aan la daweyn (UCC).Intaa waxaa dheer, isku-dhafka HWO/C76 wuxuu muujiyay xannibaad weyn oo ku saabsan falcelinta koloriinta koloriinta ee dulin sababtoo ah kooxaha shaqeeya ee W-OH.
Dhaqdhaqaaqa ba'an ee bini'aadamka iyo kacaanka warshadaha ee degdega ah ayaa horseeday baahida koronto oo aan la joojin karin, taasoo koraysa ilaa 3% sannadkii1.Tobanaan sano, isticmaalka baahsan ee shidaalka fosil ee ilaha tamarta ayaa horseeday qiiqa gaaska aqalka dhirta lagu koriyo, taasoo horseedaysa kulaylka caalamiga ah, wasakhowga biyaha iyo hawada, oo khatar gelinaya dhammaan noolaha deegaanka.Natiijo ahaan, sanadka 2050 saamiga tamarta nadiifka ah ee la cusboonaysiin karo iyo tamarta qoraxda ayaa la saadaalinayaa inay gaarto 75% wadarta koronta1.Si kastaba ha noqotee, marka wax soo saarka tamarta la cusboonaysiin karo uu ka sarreeyo 20% wadarta wax soo saarka korontada, shabaqyada ayaa noqda mid aan degganayn 1. Horumarinta hababka kaydinta tamarta hufan ayaa muhiim u ah isbeddelkan, sababtoo ah waa inay kaydiyaan koronto xad-dhaaf ah iyo dheelitirka sahayda iyo baahida.
Dhammaan nidaamyada kaydinta tamarta sida hybrid vanadium redox batariyada qulqulka 2, dhammaan baytariyada socodka vanadium redox (VRFBs) ayaa ah kuwa ugu horumarsan sababtoo ah faa'iidooyinkooda badan3 waxaana loo tixgeliyaa xalka ugu fiican ee kaydinta tamarta muddada dheer (~ 30 sano).Isticmaalka ilaha tamarta la cusboonaysiin karo4.Tan waxa u sabab ah kala soocida cufnaanta tamarta iyo tamarta, jawaab celinta degdega ah, nolosha dheer iyo kharashyada sanadlaha ah oo aad u hooseeya oo ah $65/kWh marka loo eego $93-140/kWh ee baytariyada Li-ion iyo acid-ashitada iyo 279-420 USD/kWh./kWh baytariyada siday u kala horreeyaan 4.
Si kastaba ha ahaatee, ganacsigeyntooda baahsan ayaa weli waxaa caqabad ku ah kharashaadka raasamaal ee nidaamka oo sarreeya, inta badanna waxaa ugu wacan xirmooyinka baytariga4,5.Sidaa darteed, hagaajinta waxqabadka batteriga iyadoo la kordhinayo kinetics ee laba falcelin unug nus unug ah waxay yareyn kartaa cabbirka batteriga oo sidaas darteed hoos u dhigi kara qiimaha.Sidaa darteed, wareejinta degdega ah ee elektarooniga ah ee dusha elektiroonigga ah ayaa loo baahan yahay, taas oo ku xidhan naqshadaynta, halabuurka iyo qaab-dhismeedka korantada, taas oo ay tahay in si taxadar leh loo hagaajiyo.Inkasta oo electrodes-ku salaysan kaarboonku ay leeyihiin xasilooni kiimikaad iyo kiimikaad wanaagsan iyo korantada wanaagsan, haddii aan la daweyn, kinetics-kooda ayaa noqon doona mid gaabis ah sababtoo ah maqnaanshaha kooxaha shaqada oksijiinta iyo hydrophilicity7,8.Sidaa darteed, electrocatalysts kala duwan ayaa lagu daraa korantada kaarboonka, gaar ahaan kaarboon nanostructures iyo birta oxides, si loo hagaajiyo kinetics ee labada electrodes, taas oo kordhinaysa kinetics ee electrodes VRFB.
Qalab badan oo kaarboon ah ayaa la isticmaalay, sida carbon paper9, carbon nanotubes10,11,12,13, nanostructures graphene-based14,15,16,17, carbon nanofibers18 iyo others19,20,21,22,23, marka laga reebo qoyska fullerene .Daraasaddeenii hore ee C76, waxaanu soo sheegnay markii ugu horeysay waxqabadka ugu fiican ee korantada ee fullerene ee ku wajahan VO2 +/VO2 +, marka la barbardhigo kulaylka-la daaweeyay iyo marada kaarboonka, caabbinta wareejinta kharashka ayaa hoos loo dhigay 99.5% iyo 97%24.Waxqabadka catalytic ee walxaha kaarboonka ee falcelinta VO2+/VO2+ marka la barbar dhigo C76 ayaa lagu muujiyay shaxda S1.Dhanka kale, oksaydhooyin badan oo bir ah sida CeO225, ZrO226, MoO327, NiO28, SnO229, Cr2O330 iyo WO331, 32, 33, 34, 35, 36, 37, 38 ayaa loo isticmaalaa sababtoo ah qoyaankooda oo kordhay iyo waxa ku jira oksijiinta sare.kooxaha.Shaxda S2 waxay ku tusinaysaa waxqabadka firfircoonida ee oksaydhyada birta ah ee falcelinta VO2+/VO2+.WO3 waxaa loo adeegsaday tiro shaqo oo aad u tiro badan iyadoo ay ugu wacan tahay qiimo jaban, xasiloonida sare ee warbaahinta acidic, iyo dhaqdhaqaaqa sare ee catalytic31,32,33,34,35,36,37,38.Si kastaba ha ahaatee, WO3 waxay muujisay horumar yar oo ku saabsan kinetics cathode.Si loo hagaajiyo dhaqdhaqaaqa WO3, saamaynta isticmaalka tungsten oxide (W18O49) ee hoos u dhaca dhaqdhaqaaqa korantada ayaa la tijaabiyay38.Oksijiinta tungsten-ka ah (HWO) waligiis laguma tijaabin codsiyada VRFB, in kasta oo ay muujisay firfircooni sare ee codsiyada supercapacitor sababtoo ah faafinta degdega ah ee cation marka la barbar dhigo anhydrous WOx39,40.Jiilka saddexaad oo dhan-vanadium redox batteriga wuxuu isticmaalaa korantada aashitada isku dhafan ee ka kooban HCl iyo H2SO4 si loo hagaajiyo waxqabadka batteriga loona hagaajiyo milanka iyo xasilloonida ions vanadium ee elektrolytka.Si kastaba ha ahaatee, falcelinta koloriinta koloriinta ee dulinku waxay noqotay mid ka mid ah khasaarooyinka jiilka saddexaad, sidaa darteed helidda habab lagu cabudhiyo falcelinta qiimaynta koloriinta waxay noqotay hawsha dhawr kooxood oo cilmi-baadhiseed.
Halkan, tijaabooyinka falcelinta VO2 +/VO2+ ayaa lagu sameeyay isku-dhafka HWO/C76 ee lagu shubay electrodes-ka marada kaarboonka si loo helo isku dheelitirnaanta udhaxeeya korantada korantada ee isku-dhafka iyo kinetics falcelinta redox ee dusha sare ee elektiroonigga iyada oo la xakameynayo kaydinta koloriinta dulinka.falcelinta (KVR).Nanoparticles tungsten oxide (HWO) ayaa lagu soo saaray hab fudud oo biyo-dhaliye ah.Tijaabooyin ayaa lagu sameeyay electrolyte acid isku dhafan (H2SO4 / HCl) si loogu ekaado jiilka saddexaad ee VRFB (G3) ee ku habboonaanta iyo in la baaro saameynta HWO ee falcelinta koloriinta koloriinta.
Vanadium (IV) sulfate oxide hydrate (VOSO4, 99.9%, Alfa-Aeser), sulfuric acid (H2SO4), hydrochloric acid (HCl), dimethylformamide (DMF, Sigma-Aldrich), fluoride polyvinylidene (PVDF, Sigma-Aldrich), sodium), Tungsten oxide dihydrate (Na2WO4, 99%, Sigma-Aldrich) iyo maro kaarboon ah ELAT (Bakhaarka Unugyada Shidaalka) ayaa loo adeegsaday daraasaddan.
Hudheelka tungsten oxide (HWO) waxaa lagu diyaariyey fal-celin biyo-mareen ah kaas oo 2 g oo cusbo Na2WO4 ah lagu milmay 12 ml H O ilaa xal aan midab lahayn, ka dibna 12 ml 2 M HCl ayaa lagu daray hoos u dhac ilaa huruud khafiif ah la hakiyo. ayaa la helay.ka joojinta.Dareen-celinta hydrothermal-ka waxaa lagu sameeyay Teflon oo dahaarka leh oo birta aan lahayn autoclave foornada 180 ºC muddo 3 saacadood ah.Hadhaaga waxaa lagu soo ururiyay sifeyn, lagu dhaqay 3 jeer ethanol iyo biyo, lagu qalajiyey foornada 70 ° C ilaa ~ 3 h, ka dibna dhulka si aad u hesho budada HWO buluug-cawlan.
Electrodes-ka marada kaarboonka ah ee la helay (aan la daawayn) ayaa loo isticmaalay qaabka lagu helay ama lagu daaweeyay kulaylka foornada tuubada 450°C ee 10 h heerka kulaylka 15°C/min hawada Hel daweeyay UCC (TCC), s La mid ah shaqadii hore 24. UCC iyo TCC ayaa la gooyay electrodes qiyaastii 1.5 cm ballaaran iyo 7 cm dheer.Joojinta C76, HWO, HWO-10% C76, HWO-30% C76 iyo HWO-50% C76 ayaa la diyaariyey iyadoo lagu daray 20 mg oo ah budada walxaha firfircoon iyo 10 wt% (~ 2.22 mg) ee PVDF xiraha ~ 1 ml oo ah DMF waxay diyaarisay oo codsatay 1 saac si loo horumariyo labbiska.Kadibna 2 mg ee C76, HWO iyo HWO-C76 isku dhafan ayaa lagu dabaqay qiyaastii 1.5 cm2 ee aagga korantada firfircoon ee UCC.Dhammaan kicinta ayaa lagu dhejiyay electrodes UCC iyo TCC waxaa loo isticmaalay ujeeddooyin isbarbardhigga oo keliya, sida shaqadeenii hore ay muujisay in daaweynta kuleylka aan loo baahnayn 24.Dejinta aragtida waxaa lagu gaadhay cadayashada 100 µl ee hakinta (load 2 mg) si loo mideeyo.Kadibna dhammaan electrodes-ka ayaa lagu qallajiyey foornada habeenkii oo dhan 60 ° C.Electrodes-ka waxa la cabbiraa ka hor iyo ka dib si loo hubiyo in kaydka saxda ah uu soo shubo.Si loo helo aag joomatari gaar ah (~ 1.5 cm2) loogana hortago kor u kaca vanadium electrolyte ee electrodes sababtoo ah saamaynta capillary, lakabka khafiifka ah ee paraffin ayaa lagu dabaqay walxaha firfircoon.
Mikroskoob elektaroonik ah (FESEM, Zeiss SEM Ultra 60.5 kV) ayaa la isticmaalay si loo eego qaab-dhismeedka HWO.Tamarta kala firdhisa raajada spectroscopy oo ku qalabaysan Feii8SEM (EDX, Zeiss AG) ayaa loo isticmaalay in lagu khariideeyo walxaha HWO-50%C76 ee korantada UCC.Mikroskoob gudbinta xallinta sare ee elektarooniga ah (HR-TEM, JOEL JEM-2100) oo ku shaqeynaya korantada dardargelinta ee 200 kV ayaa loo adeegsaday si loo helo sawirro xallin sare leh iyo giraangiraha kala-soocidda ee qaybaha HWO.Isticmaal barnaamijka Crystallographic Tool Box (CrysTBox) si aad u falanqeyso siddooyinka kala duwanaanta HWO adoo isticmaalaya shaqada ringGUI oo barbardhig natiijooyinka moodooyinka XRD.Qaab dhismeedka iyo garaafyada UCC iyo TCC waxaa lagu go'aamiyay kala-duwanaanta raajada (XRD) ee qiyaasta sawirka 2.4 ° / min min 5 ° ilaa 70 ° oo leh Cu Kα (λ = 1.54060 Å) iyadoo la adeegsanayo diffractometer X-ray Panalytical.(Model 3600).XRD waxay muujinaysaa qaab dhismeedka crystal iyo wejiyada HWO.Software-ka PANalytical X'Pert HighScore waxaa loo isticmaalay in lagu waafajiyo meelaha ugu sarreeya ee HWO iyo khariidadaha tungsten oxide ee laga heli karo database45.Is barbar dhig natiijooyinka HWO iyo natiijooyinka TEM.Halabuurka kiimikaad iyo xaaladda shaybaarrada HWO waxaa lagu go'aamiyay raajada sawir-qaadista sawirka (XPS, ESCALAB 250Xi, ThermoScientific).Software-ka CASA-XPS (v 2.3.15) waxa loo isticmaalay deconvolution iyo falanqaynta xogta ugu sarreysa.Fourier transforming infrared spectroscopy (FTIR, iyadoo la isticmaalayo fasalka Perkin Elmer KBr FTIR spectrometer) cabbirada ayaa la sameeyay si loo go'aamiyo kooxaha shaqada dusha ee HWO iyo HWO-50% C76.Is barbar dhig natiijooyinka iyo natiijooyinka XPS.Cabbirrada xagasha xidhiidhka (KRUSS DSA25) ayaa sidoo kale loo isticmaalay in lagu garto qoyaanka korantada.
Dhammaan cabbiraadaha korantada kiimikaad, Biologic SP 300 goobta shaqada ayaa la isticmaalay.Cyclic voltammetry (CV) iyo electrochemical impedance spectroscopy (EIS) ayaa loo isticmaalay in lagu barto kinetics electrode ee falcelinta redox VO2 +/VO2+ iyo saamaynta faafinta reagent (VOSO4 (VO2+)) ee heerka falcelinta.Labada teknoolajiyada waxay isticmaalaan unug saddex-electrode ah oo leh fiirsashada elektrolytka ee 0.1 M VOSO4 (V4+) oo lagu milmay 1 M H2SO4 + 1 M HCl (acid isku dhafan).Dhammaan xogta korantada kiimikada ee la soo bandhigay waa IR la saxay.Dhererka calomel-ka buuxa (SCE) iyo platinum (Pt) gariiradda ayaa loo isticmaalay tixraac ahaan iyo korantada counterde, siday u kala horreeyaan.CV-ga, heerarka iskaanka (ν) ee 5, 20, iyo 50 mV/s ayaa lagu dabaqay daaqad suurtagal ah (0-1) V marka la barbar dhigo SCE ee VO2+/VO2+, ka dibna lagu saxay miisaanka SHE si loo sawiro (VSCE = 0.242). V marka loo eego HSE).Si loo baaro haynta dhaqdhaqaaqa korantada, dib u warshadaynta CV-ga ayaa lagu sameeyay UCC, TCC, UCC-C76, UCC-HWO iyo UCC-HWO-50% C76 at ν oo u dhiganta 5 mV/s.Qiyaasta EIS ee falcelinta VO2+/VO2+, kala duwanaansho joogto ah oo ah 0.01-105 Hz iyo khalkhal korantada furan (OCV) ee 10 mV ayaa la isticmaalay.Tijaabo kasta ayaa lagu soo celiyay 2-3 jeer si loo hubiyo joogtaynta natiijooyinka.Heterogeneous heerka joogtada ah (k0) waxaa lagu helay habka Nicholson46,47.
Oksijiinta tungsten (HVO) ayaa si guul leh u soo saartay habka biyo-dhaliye.Sawirka SEM ee fig.1a waxay tusinaysaa in HWO la kaydiyay ay ka kooban tahay rucubyo nanoparticles oo leh cabbirro qaybeed oo u dhexeeya 25-50 nm.
Habka kala-duwanaanta raajada ee HWO waxay muujinaysaa ugu sarreeya (001) iyo (002) at ~ 23.5 ° iyo ~ 47.5 °, siday u kala horreeyaan, kuwaas oo sifo aan stoichiometric WO2.63 (W32O84) (PDF 077-0810, a = 21.4 Å, b = 17.8 Å, c = 3.8 Å, α = β = γ = 90 °), taas oo u dhiganta midab buluug ah oo muuqda (Jaantus 1b) 48,49.Kuwa kale ee ugu sarreeya ee qiyaastii ah 20.5°, 27.1°, 28.1°, 30.8°, 35.7°, 36.7° iyo 52.7° waxa ay joogan (140), (620), (350), (720), (740), (560).iyo (970) diyaaradaha diffraction, siday u kala horreeyaan, 49 orthorhombic WO2.63.Songara iyo al.43 waxay isticmaashay habka synthetic ee isku midka ah si ay u hesho badeecad cad, taas oo loo aaneynayo joogitaanka WO3 (H2O) 0.333.Si kastaba ha noqotee, shaqadan, xaalado kala duwan awgeed, badeecad buluug-cawlan ayaa la helay, taasoo muujinaysa wada noolaanshaha WO3 (H2O) 0.333 (PDF 087-1203, a = 7.3 Å, b = 12.5 Å, c = 7.7) ee Å. , α = β = γ = 90 °) iyo qaabka la dhimay ee tungsten oxide.Falanqaynta semiquantitative ee software-ka X'Pert HighScore waxay muujisay 26% WO3 (H2O) 0.333: 74% W32O84.Maadaama W32O84 ay ka kooban tahay W6+ iyo W4+ (1.67:1 W6+:W4+), waxa lagu qiyaasay W6+ iyo W4+ waa qiyaastii 72% W6+ iyo 28% W4+, siday u kala horreeyaan.Sawirada SEM, 1-ilbiriqsi XPS spectra ee heerka nukleus, sawirada TEM, FTIR spectra iyo Raman spectra ee qaybaha C76 ayaa lagu soo bandhigay warqadayadii hore24.Sida laga soo xigtay Kawada et al.50,51, qaabka kala-duwanaanta raajada ee C76 waxay muujinaysaa qaabka monoclinic ee FCC ka dib markii laga saaro toluene.
Sawirada SEM ee fig.2a iyo b waxay muujinayaan meel dhigista guusha leh ee HWO iyo HWO-50% C76 iyo inta u dhaxaysa fiilooyinka kaarboon ee korantada UCC.Khariidaynta curiyaha ah ee tungsten, kaarboon iyo ogsijiin ee sawirka SEM ee sawirka 2c ayaa lagu muujiyay berdaha.2d-f tusinaya in tungsten-ka iyo kaarboonku si isku mid ah isugu dhafan yihiin (muujinaya qaybinta la mid ah) dusha korantada oo isku-dhafka aan si siman loo dhigin.iyadoo ay ugu wacan tahay dabeecadda habka roobabka.
Sawirada SEM ee qaybaha HWO ee kaydsan (a) iyo qaybaha HWO-C76 (b).Khariidadda EDX oo lagu shubay HWO-C76 ee UCC iyadoo la adeegsanayo aagga sawirka (c) waxay muujinaysaa qaybinta tungsten (d), kaarboon (e), iyo ogsijiin (f) ee muunadda.
HR-TEM waxa loo isticmaalay sawirka waynaynta sare iyo macluumaadka crystallographic (Jaantuska 3).HWO waxay muujinaysaa qaab-dhismeedka nanocube sida ku cad Jaantuska 3a oo si cad ugu muuqda Jaantuska 3b.Iyada oo la weyneynayo nanocube loogu talagalay kala-soocidda aag la doortay, qaab-dhismeedka qashinka iyo dayuuradaha kala-baxa ee qancinaya sharciga Bragg waa la arki karaa sida ku cad Jaantuska 3c, iyada oo xaqiijinaysa crystallinity ee walxaha.Gelitaanka Jaantuska 3c waxay muujinaysaa masaafada d 3.3 Å u dhiganta (022) iyo (620) dayuuradaha kala duwan ee WO3(H2O)0.333 iyo W32O84, 43, 44, 49, siday u kala horreeyaan.Tani waxay la socotaa falanqaynta sare ee XRD (Jaantus. 1b) tan iyo fogaanta diyaaradda grating ee la arkay d (Jaantus. 3c) waxay u dhigantaa heerka ugu sarreeya XRD ee muunadda HWO.Siddooyinka tusaalaha ah ayaa sidoo kale lagu muujiyay berdaha.3d, halkaas oo giraanti kasta u dhiganto diyaarad gaar ah.Diyaaradaha WO3(H2O) 0.333 iyo W32O84 waa midabyo cad iyo buluug, siday u kala horreeyaan, heerarkooda ugu sarreeya ee XRD ayaa sidoo kale lagu muujiyey sawirka 1b.Giraanta ugu horreysa ee lagu muujiyey qaabka giraanta waxay u dhigantaa meesha ugu sarreysa ee calaamadsan ee qaabka raajada ee (022) ama (620).Laga soo bilaabo (022) ilaa (402) faraanti, d-fogaanshaha 3.30, 3.17, 2.38, 1.93, iyo 1.69 Å ayaa la helay, kuwaas oo la jaan qaadaya qiimaha XRD ee 3.30, 3.17, 2.45, 1.93 iyo 1.66.Å, 44, 45, siday u kala horreeyaan.
(a) Sawirka HR-TEM ee HWO, (b) wuxuu muujinayaa sawir la weynaaday.Sawirada dayuuradaha grating ayaa lagu muujiyay (c), iyo inset (c) waxay muujinayaan sawirka la weynaaday ee diyaaradaha iyo inta u dhaxaysa d 0.33 nm oo u dhiganta (002) iyo (620) diyaaradaha.(d) Habka giraanta HWO oo muujinaya diyaaradaha la xidhiidha WO3 (H2O) 0.333 (caddaan) iyo W32O84 (buluug).
Falanqaynta XPS ayaa la sameeyay si loo go'aamiyo kiimikada dusha sare iyo xaaladda oksaydhka ee tungsten (Jaantusyada S1 iyo 4).Kala duwanaanshaha baaxadda ballaaran ee sawirka XPS ee HWO la isku daray ayaa lagu muujiyey shaxanka.S1, taas oo muujinaysa joogitaanka tungsten.Sawirka dhuuban ee XPS ee heerarka W 4f iyo O 1s ee ugu muhiimsan ayaa lagu muujiyay berdihii.4a iyo b, siday u kala horreeyaan.Muuqaalka W 4f wuxuu u kala qaybsan yahay laba laab-orbit-orbit oo u dhiganta tamarta isku-xidhka ah ee gobolka oksaydheynta W. Meesha ugu sarreysa W 4f5/2 iyo W 4f7/2 ee isku xidhka tamarta ee 37.8 iyo 35.6 eV waxay iska leeyihiin W6+, iyo meelaha ugu sarreeya W. 4f5/2 iyo W 4f7/2 at 36.6 iyo 34.9 eV waa sifada gobolka W4+, siday u kala horreeyaan.Joogitaanka gobolka oksaydhka (W4 +) ayaa sii xaqiijinaysa samaynta WO2.63 aan ahayn stoichiometric, halka joogitaanka W6 + ay muujinayso stoichiometric WO3 sababtoo ah WO3 (H2O) 0.333.Xogta ku habboon ayaa muujisay in boqolleyda atomigga ee W6+ iyo W4+ ay ahaayeen 85% iyo 15%, siday u kala horreeyaan, kuwaas oo aad ugu dhow qiyamka lagu qiyaasay xogta XRD, marka la eego farqiga u dhexeeya labada tignoolajiyada.Labada habba waxay bixiyaan macluumaadka tirada leh saxsanaan hoose, gaar ahaan XRD.Intaa waxaa dheer, labada hab waxay falanqeeyaan qaybaha kala duwan ee walxaha sababtoo ah XRD waa hab badan halka XPS ay tahay habka dusha sare oo kaliya oo ku wajahan dhowr nanometer.Muuqaalka O 1s wuxuu u kala baxaa laba meelood oo ugu sarreeya 533 (22.2%) iyo 530.4 eV (77.8%).Midka kowaad wuxuu u dhigmaa OH, ka labaadna xidhidhiyaha ogsijiinta ee xabagta WO.Joogitaanka kooxaha shaqada OH waxay la socotaa sifooyinka fuuq-celinta ee HWO.
Falanqaynta FTIR ayaa sidoo kale lagu sameeyay labadan muunado si loo baaro joogitaanka kooxaha shaqeeya iyo molecules biyaha isku dubaridan ee qaab dhismeedka HWO fuuqbaxay.Natiijooyinku waxay muujinayaan in HWO-50% C76 muunad iyo natiijooyinka FT-IR HWO ay isku mid yihiin sababtoo ah joogitaanka HWO, laakiin xoojinta ugu sarreysa ayaa ka duwan sababtoo ah qiyaaso kala duwan oo muunad ah oo loo isticmaalo inta lagu jiro diyaarinta falanqaynta (Jaantus. 5a). ).HWO-50% C76 Dhammaan fullerene 24 ugu sarreeya ayaa la muujiyay marka laga reebo tungsten oxide ugu sarreeya.Tafatiran ee fig.5a waxay muujineysaa in labada muunadba ay muujinayaan koox aad u xoog badan oo ah ~ 710 / cm, oo loo aaneynayo gariirrada fidinta OWO ee qaab dhismeedka HWO, iyo garabka adag ee ~ 840 / cm, oo loo aaneynayo WO.band fiiqan ee ~ 1610 / cm waxay la xiriirtaa gariir foorarsiga OH, iyo qaybta nuugista ballaaran ee ~ 3400 / cm waxay la xiriirtaa gariirka fidinta OH ee kooxda hydroxyl43.Natiijooyinkani waxay la socdaan spectrum XPS ee Jaantuska 4b, halkaas oo kooxda shaqada ee WO ay ku siin karaan goobo firfircoon falcelinta VO2+/VO2+.
Falanqaynta FTIR ee HWO iyo HWO-50% C76 (a) oo muujinaya kooxo shaqeynaya iyo cabbirada xagasha xidhiidhka (b, c).
Kooxda OH waxay sidoo kale kicin kartaa falcelinta VO2+/VO2+, taas oo kordhinaysa hydrophilicity ee korantada, taas oo kor u qaadeysa faafinta iyo heerka wareejinta elektaroonigga ah.Muunada HWO-50% C76 waxay muujinaysaa ugu sarreeya C76 dheeraad ah sida ku cad shaxanka.Meelaha ugu sarreeya ee ~ 2905, 2375, 1705, 1607, iyo 1445 cm3 waxaa lagu meelayn karaa CH, O=C=O, C=O, C=C,iyo CO, siday u kala horreeyaan.Waxaa si fiican loo og yahay in kooxaha shaqada oksijiinta C = O iyo CO ay u adeegi karaan sidii xarumo firfircoon oo loogu talagalay falcelinta redox ee vanadium.Si loo tijaabiyo loona isbarbardhigo qoyaanka labada electrodes, cabbirada xagasha xidhiidhka ayaa la isticmaalay sida ku cad sawirka 5b, c.Electrode-ka HWO isla markiiba wuxuu nuugaa dhibcaha biyaha, taas oo muujinaysa superhydrophilicity sababtoo ah kooxaha shaqeeya ee OH ee la heli karo.HWO-50% C76 waa hydrophobic ka badan, oo leh xagal xiriir ah oo ku saabsan 135 ° 10 ilbiriqsi ka dib.Si kastaba ha ahaatee, marka la eego cabbirada korantada, HWO-50% C76 electrode si buuxda ayaa loo qooyay in ka yar hal daqiiqo.Cabbirrada qoynta ayaa la socda natiijooyinka XPS iyo FTIR, taasoo soo jeedinaysa in kooxo badan oo OH ah oo ku yaal dusha HWO ay ka dhigayaan mid aad u badan.
Dareen-celinta VO2 +/VO2+ ee HWO iyo HWO-C76 nanocomposites ayaa la tijaabiyay waxaana la filayay in HWO ay xakameyn doonto kobcinta gaasta koloriinta ee dhacda inta lagu jiro falcelinta VO2 +/ VO2 + ee asiidhyada isku dhafan, halka C76 ay sii kordhin doonto VO2 +/ VO2+ la doonayo.Joojinta HWO oo ka kooban 10%, 30% iyo 50% C76 ayaa lagu dabaqay korantada UCC oo wadata culeys dhan 2 mg/cm2.
Sida ku cad fig.6, Kinetics ee falcelinta VO2 +/VO2+ ee dusha sare ee korantada ayaa la baaray iyadoo la adeegsanayo CV-yada elektarolytka isku dhafan.Hadda waxa loo tusay I/Ipa si loo fududeeyo isbarbardhigga ΔEp iyo Ipa/Ipc.Kataliyeyaal kala duwan ayaa si toos ah looga helay shaxanka.Xogta unugga aagga hadda waxa lagu muujiyey Jaantuska 2S.On berde.Jaantus 6a waxay muujinaysaa in HWO ay wax yar kordhiso heerka wareejinta elektaroonigga ah ee VO2 +/VO2+ falcelinta redox ee dusha elektiroonigga ah waxayna xakameysaa falcelinta koloriinta koloriinta.Si kastaba ha noqotee, C76 waxay si weyn u kordhisaa heerka wareejinta elektaroonigga waxayna kicisaa falcelinta koloriinta.Sidaa darteed, isku-dhafan oo leh qaabka saxda ah ee HWO iyo C76 waa inay lahaadaan waxqabadka ugu fiican iyo awoodda ugu sareysa ee lagu xakameynayo falcelinta koloriinta.Waxaa la ogaaday in ka dib markii la kordhiyey nuxurka C76, dhaqdhaqaaqa korantada ee korantada ayaa soo hagaagtay, sida caddaynta hoos u dhaca ΔEp iyo korodhka saamiga Ipa / Ipc (Shaxda S3).Tan waxaa sidoo kale lagu xaqiijiyay qiyamka RCT ee laga soo saaray goobta Nyquist ee sawirka 6d (miiska S3), halkaas oo la ogaaday in qiimaha RCT uu hoos u dhacay iyada oo korodhka content ee C76.Natiijooyinkani waxay sidoo kale la socdaan daraasadda Lee taas oo ku darista kaarboonka mesoporous ee mesoporous WO3 ay hagaajisay kinetics wareejinta kharashka ee VO2+/VO2+35.Tani waxay soo jeedinaysaa in falcelinta togani ay ku xirnaan karto wax badan oo ku saabsan korantada korantada (C=C bond)18,24,35,36,37.Sababtoo ah isbeddelka joomatari isuduwidda ee u dhexeeya [VO(H2O)5]2+ iyo [VO2(H2O)4]+, C76 waxa kale oo ay yarayn kartaa jawaabta xad-dhaafka ah iyada oo la yareynayo tamarta unugyada.Si kastaba ha ahaatee, tani waxaa laga yaabaa inaanay suurtogal ahayn qalabka HWO.
(a) Dabeecada wareega wareega ee UCC iyo HWO-C76 isku dhafan oo leh HWO kala duwan: C76 saamiga VO2+/VO2+ ee 0.1 M VOSO4/1 M H2SO4 + 1 M HCl electrolyte (at ν = 5 mV/s).(b) Randles-Sevchik iyo (c) Habka Nicholson ee VO2+/VO2+ ee lagu qiyaaso waxtarka faafinta iyo helitaanka qiimaha k0 (d).
Ma aha oo kaliya HWO-50% C76 waxay soo bandhigtay ku dhawaad ​​isla dhaqdhaqaaqa elektiroonigga ah ee C76 ee falcelinta VO2 +/VO2+, laakiin, aad u xiiso badan, waxay sidoo kale xakamaysay kobcinta gaasta koloriin marka la barbar dhigo C76, sida ku cad shaxanka.6a, marka lagu daro muujinta wareega-yar ee fig.6g (RCT hoose).C76 waxay muujisay Ipa/Ipc ka muuqda mid ka sarreeya HWO-50% C76 (Shaxda S3), ma aha sababtoo ah dib-u-celinta falcelinta oo soo hagaagtay, laakiin sababtoo ah isku-dhafka ugu sarreeya ee yaraynta koloriinta ee 1.2 V marka la barbardhigo SHE.Waxqabadka ugu fiican ee HWO-50% C76 waxaa loo aaneynayaa isdhexgalka ka dhexeeya C76 si xun loo dallaco iyo qoynta sare iyo hawlaha firfircoonida ee W-OH ee HWO.Iyadoo sii daynta koloriin yar ay wanaajin doonto wax ku oolnimada ku dallacaadda unugga buuxa, kaniiniyada la roonaaday waxay kordhin doontaa waxtarka tamarta unugga oo buuxa.
Marka loo eego isla'egta S1, falcelinta quasi-la beddeli karo (wareejinta elektarooniga ah ee tartiib tartiib ah) falcelinta ay maamusho faafinta, hadda ugu sarreeya (IP) waxay kuxirantahay tirada elektaroonigga (n), aagga elektiroonigga (A), iskudhafka faafinta (D), lambar Xawaaraha wareejinta elektarooniga ah (α) iyo xawaaraha iskaanka (ν).Si loo barto habdhaqanka la xakameeyey faafinta ee alaabta la tijaabiyay, xidhiidhka ka dhexeeya IP iyo ν1/2 ayaa la qorsheeyay oo lagu muujiyay sawirka 6b.Maadaama dhammaan agabku ay muujinayaan xiriir toos ah, falcelinta waxaa lagu xakameynayaa faafinta.Maaddaama falcelinta VO2+/VO2+ ay tahay mid dib loo rogi karo, jiirada xariiqdu waxay kuxirantahay iskudarka faafinta iyo qiimaha α (isla'egta S1).Sababtoo ah isku-dhafka joogtada ah ee faafinta (≈ 4 × 10-6 cm2 / s) 52, farqiga u dhexeeya xariiqda xariiqda ayaa si toos ah u muujinaya qiimaha kala duwan ee α iyo markaa heerarka kala duwan ee wareejinta elektaroonigga ah ee dusha sare ee elektiroonigga, oo leh C76 iyo HWO -50 % C76, oo muujinaya jiirarrada ugu dhaadheer (heerka wareejinta elektaroonigga ugu sarreeya).
Jiidadka Warburg ee hooseeya ee la xisaabiyay (W) ee lagu muujiyey Shaxda S3 (Jaantus. 6d) waxay leeyihiin qiyam ku dhow 1 dhammaan agabka, taasoo muujinaysa faafinta qumman ee qaybaha redox iyo xaqiijinta habdhaqanka tooska ah ee IP iyo ν1 / 2 ee CV.cabbirada .HWO-50% C76, jiirada Warburg waxay ka leexataa midnimada ilaa 1.32, oo soo jeedinaysa wax ku biirinta ma aha oo kaliya faafinta semi-infinite reactants (VO2+), laakiin sidoo kale suurtagal ahaan dabeecad khafiif ah oo ku jirta habdhaqanka faafinta sababtoo ah porosity electrode.
Si loo sii falanqeeyo dib-u-celinta (heerka wareejinta elektiroonigga ah) ee falcelinta redox-ka ee VO2+/VO2+, habka fal-celinta ka-soo-noqoshada ee Nicholson ayaa sidoo kale loo adeegsaday si loo go'aamiyo heerka caadiga ah ee joogtada ah k041.42.Tan waxaa lagu sameeyaa iyadoo la sawirayo cabbirka kinetic-ka aan cabbir lahayn Ψ oo ah shaqada ΔEp ee shaqada ν−1/2 iyadoo la adeegsanayo isla'egta S2.Jadwalka S4 wuxuu muujinayaa natiijada Ψ qiyamka alaab kasta oo korantada ah.Qor natiijada (Jaantuska 6c) si aad u heshid k0 × 104 cm/s (oo ku qoran saf kasta oo ku xiga oo lagu soo bandhigay shaxda S4) adoo isticmaalaya isla'egta S3 ee jiirada goob kasta.HWO-50% C76 waxaa la ogaaday inuu leeyahay jiirada ugu sarreysa (Jaantus. 6c) oo markaa qiimaha k0 ugu sarreeya ee 2.47 × 10-4 cm/s.Tani waxay ka dhigan tahay in korantadani ay bixiso kaniiniga ugu dhaqsaha badan si waafaqsan CV iyo natiijooyinka EIS ee Jaantusyada 6a iyo d iyo Shaxda S3.Intaa waxaa dheer, qiimaha k0 ayaa sidoo kale laga helay sawirada Nyquist (Jaantus. 6d) ee isla'egta S4 iyadoo la adeegsanayo qiimaha RCT (Shaxda S3).Natiijooyinkan k0 ee EIS waxaa lagu soo koobay Jadwalka S4 waxayna sidoo kale muujinayaan in HWO-50% C76 ay muujiso heerka ugu sarreeya ee wareejinta elektaroonigga ah sababtoo ah saameynta isdhexgalka.Inkasta oo qiimaha k0 uu ku kala duwan yahay asalka kala duwan ee hab kasta, weli waxay muujinaysaa isku xigxiga xajmiga waxayna muujinaysaa joogteynta.
Si aad si buuxda u fahamto kinetics-ka ugu fiican ee la gaari karo, waxaa muhiim ah in la isbarbar dhigo qalabka elektaroonigga ah ee ugu fiican ee leh UCC iyo TCC Electrodes oo aan la daboolin.Dareen-celinta VO2 +/VO2 +, HWO-C76 kaliya ma muujin ΔEp ugu hooseeya iyo dib-u-celinta ka wanaagsan, laakiin sidoo kale waxay si weyn u xakamaysay falcelinta koloriinta koloriinta marka la barbar dhigo TCC, sida lagu muujiyay hoos u dhac weyn oo hadda ah 1.45 V marka la barbardhigo OHA (Berdihii. 7a)Marka la eego xasilloonida, waxaan u maleynay in HWO-50% C76 ay jir ahaan deggan tahay sababtoo ah kicinta ayaa lagu qasi jiray xiraha PVDF ka dibna lagu dabaqay qalabka korontada ku shaqeeya ee dharka kaarboon.Marka la barbardhigo 50 mV ee UCC, HWO-50% C76 waxay muujisay isbeddelka ugu sarreeya ee 44 mV ka dib wareegyada 150 (heerka hoos u dhaca 0.29 mV / wareegga) (Jaantus 7b).Waxaa laga yaabaa inaysan farqi weyn u ahayn, laakiin kinetics ee electrodes UCC waa mid aad u gaabis ah waxayna hoos u dhigtaa baaskiilka, gaar ahaan falcelinta dhabarka.Inkasta oo dib-u-celinta TCC ay aad uga fiican tahay kan UCC, TCC waxaa la ogaaday in ay leedahay isbeddelka ugu sarreeya ee 73 mV ka dib 150 wareegyo, taas oo laga yaabo inay sabab u tahay qadarka badan ee koloriinta ee laga sii daayo dusha sare.Si loo hubiyo in kataliyuhu uu si fiican ugu dheggan yahay dusha sare ee korantada.Sida lagu arki karo dhammaan electrodes-ka la tijaabiyay, xitaa kuwa aan lahayn kiciyayaal la taageeray waxay muujinayaan heerar kala duwan oo xasiloonida baaskiilka, taasoo soo jeedinaysa in isbeddelada kala soocida ugu sarreysa inta lagu jiro baaskiil wadida ay sabab u tahay wax-ka-qabashada walxaha sababtoo ah isbeddelada kiimikaad halkii ay ka ahaan lahaayeen kala-soocidda kicinta.Sidoo kale, haddii xaddi badan oo walxaha kicinta ah laga sooci lahaa dusha sare ee korantada, tani waxay horseedi doontaa koror weyn oo kala-soocidda ugu sarreysa (ma ahan oo keliya 44 mV), maadaama substrate (UCC) uu yahay mid aan firfircooneyn VO2 +/VO2+ falcelinta redox.
Isbarbardhigga CV (a) iyo xasilloonida falcelinta redox VO2+/VO2+ (b) ee walxaha korantada ugu fiican marka loo eego CCC.Qalabka elektrolytka 0.1 M VOSO4/1 M H2SO4 + 1 M HCl, dhammaan CV-yada waxay la mid yihiin ν = 5 mV/s.
Si loo kordhiyo soo jiidashada dhaqaale ee tignoolajiyada VRFB, wanaajinta iyo fahamka kinetics ee falcelinta redox ee vanadium waa lama huraan si loo gaaro hufnaanta tamarta sare.Isku-dhafka HWO-C76 ayaa la diyaariyey iyo saameyntooda korantada ee falcelinta VO2 +/ VO2 + ayaa la darsay.HWO waxay muujisay kor u qaadis yar laakiin waxay si weyn u xakamaysay koloriinta koloriinta ee korantada isku dhafan.Saamiyada kala duwan ee HWO:C76 ayaa loo isticmaalay si loo sii wanaajiyo kinetics ee korantada ku salaysan HWO.Kordhinta waxa ku jira C76 ilaa HWO waxay hagaajin kartaa dhaqdhaqaaqa wareejinta elektaroonigga ah ee VO2 +/VO2+ falcelinta elektiroonigga ah ee la beddelay, oo ay ka mid yihiin HWO-50% C76 waa walxaha ugu fiican sababtoo ah waxay hoos u dhigtaa iska caabbinta wareejinta kharashka waxayna sii kordhisaa xakamaynta koloriin gaaska marka la barbar dhigo C76.iyo TCC waa la sii daayay.Tani waxay sabab u ahayd saamaynta isku-dhafan ee u dhaxaysa C=C sp2 hybridization, OH iyo W-OH kooxaha shaqeeya.Heerka hoos u dhaca HWO-50% C76 waxaa lagu ogaadey inuu yahay 0.29mV/wareegga baaskiilka badan halka UCC iyo TCC ay yihiin 0.33mV/wareegga iyo 0.49mV/wareegga siday u kala horreeyaan, taasoo ka dhigaysa mid aad u deggan electrolytes acid isku dhafan.Natiijooyinka la soo bandhigay ayaa si guul leh u aqoonsanaya qalabka korantada ee waxqabadka sare leh ee falcelinta VO2 +/VO2+ oo leh kinetics degdeg ah iyo xasillooni sare.Tani waxay kordhin doontaa tamarta wax soo saarka, taas oo kor u qaadaysa waxtarka awoodda VRFB, taas oo hoos u dhigi doonta kharashka ganacsigeeda mustaqbalka.
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