I-304 capillary tube Nanocomposites Isekelwe ku-Tungsten Oxide/Fullerene njengama-Electrocatalysts kanye nama-Inhibitors we-Parasitic VO2+/VO2+ Reactions in Mixed Acids

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I-Stainless Steel 304 Coil Tube Chemical Composition

I-304 Stainless Steel Coil Tube iwuhlobo lwe-austenitic chromium-nickel alloy.Ngokusho komkhiqizi we-Stainless Steel 304 Coil Tube, ingxenye eyinhloko kuyo i-Cr (17% -19%), kanye ne-Ni (8% -10.5%).Ukuze kuthuthukiswe ukumelana kwayo nokugqwala, kunezilinganiso ezincane ze-Mn (2%) kanye ne-Si (0.75%).

I-Stainless Steel 304 I-Coil Tube Mechanical Properties

Izakhiwo zemishini ye-304 stainless steel coil tube zimi kanje:

• Amandla okuqina: ≥515MPa
• Amandla okukhiqiza: ≥205MPa
• Ubude: ≥30%

Izicelo kanye nokusetshenziswa kwe-Stainless Steel 304 Coil Tube

Izindleko eziphakeme kakhulu zamabhethri e-vanadium redox flow battery (VRFBs) zikhawulela ukusetshenziswa kwawo okusabalele.I-kinetics of electrochemical reactions kumele ithuthukiswe ukuze kwandiswe ukuminyana kwamandla nokusebenza kahle kwamandla e-VRFB, ngaleyo ndlela kwehliswe izindleko ze-kWh ze-VRFB.Kulo msebenzi, i-hydrothermally synthesized hydrated tungsten oxide (HWO) nanoparticles, i-C76 ne-C76/HWO, yafakwa kuma-electrode endwangu ye-carbon futhi yahlolwa njengama-electrocatalysts ku-VO2+/VO2+ redox reaction.I-Field emission scanning electron microscopy (FESEM), i-energy dispersive X-ray spectroscopy (EDX), i-high-resolution transmission electron microscopy (HR-TEM), i-X-ray diffraction (XRD), i-X-ray photoelectron spectroscopy (XPS), i-Fourier ye-infrared guqula i-Spectroscopy (FTIR) kanye nezilinganiso ze-engeli yokuxhumana.Kutholwe ukuthi ukungezwa kwe-C76 fullerene ku-HWO kungathuthukisa i-kinetics ye-electrode ngokuphathelene nokusabela kwe-redox ye-VO2+/VO2+ ngokwandisa ukuqhutshwa nokuhlinzeka ngamaqembu asebenzayo aqukethe umoya-mpilo endaweni yayo.Inhlanganisela ye-HWO/C76 (50 wt% C76) ibonakale ifaneleka kakhulu ekuphenduleni kwe-VO2+/VO2+ nge-ΔEp engu-176 mV uma kuqhathaniswa no-365 mV wendwangu ye-carbon engalashwa (UCC).Ngaphezu kwalokho, inhlanganisela ye-HWO/C76 ibonise ukuvinjelwa okuphawulekayo kokusabela kwe-parasitic chlorine evolution ngenxa yamaqembu asebenzayo e-W-OH.
Umsebenzi oshubile wabantu kanye nenguquko esheshayo yezimboni kuholele esidingweni esikhulu ngokungenakuvinjelwa sikagesi, esikhula cishe ngama-3% ngonyaka1.Emashumini eminyaka, ukusetshenziswa kabanzi kwezinsalela ezimbiwa phansi njengomthombo wamandla kuye kwaholela ekukhishweni kwegesi ebamba ukushisa, okuholela ekufudumaleni komhlaba, ukungcoliswa kwamanzi nomoya, okusongela yonke imvelo.Ngenxa yalokho, ngo-2050 isabelo samandla ahlanzekile avuselelekayo namandla elanga kulindeleke ukuthi sifinyelele ku-75% wawo wonke ugesi1.Kodwa-ke, lapho ukukhiqizwa kwamandla avuselelekayo kudlula u-20% wengqikithi yokukhiqiza ugesi, igridi iba engazinzile 1. Ukuthuthukiswa kwezinhlelo zokulondoloza amandla ezisebenza kahle kubalulekile kulolu shintsho, njengoba kufanele zigcine ugesi owedlulele kanye nokulinganisa ukuhlinzekwa kanye nesidingo.
Phakathi kwazo zonke izinhlelo zokugcina amandla njenge-hybrid vanadium redox flow batterys2, wonke amabhethri e-vanadium redox flow (VRFBs) athuthuke kakhulu ngenxa yezinzuzo zawo eziningi3 futhi abhekwa njengesixazululo esingcono kakhulu sokugcina amandla isikhathi eside (~ iminyaka engu-30).Ukusetshenziswa kwemithombo yamandla avuselelekayo4.Lokhu kungenxa yokuhlukaniswa kwamandla namandla, ukuphendula okusheshayo, impilo ende kanye nezindleko zonyaka eziphansi kakhulu ze-$65/kWh uma kuqhathaniswa no-$93-140/kWh wamabhethri e-Li-ion namabhethri e-lead-acid kanye no-279-420 USD/kWh./kWh amabhethri ngokulandelana kwawo 4.
Kodwa-ke, ukudayiswa kwabo okusabalele kuyaqhubeka nokuphazanyiswa yizindleko ezinkulu zemali yesistimu, ikakhulukazi ngenxa yamaphakethe amabhethri4,5.Ngakho-ke, ukuthuthukisa ukusebenza kwebhethri ngokwandisa i-kinetics yokusabela kwe-half cell reaction kunganciphisa usayizi webhethri futhi ngaleyo ndlela kunciphise izindleko.Ngakho-ke, ukudluliswa kwe-electron okusheshayo endaweni ye-electrode kuyadingeka, kuye ngokuthi ukuklama, ukwakheka kanye nesakhiwo se-electrode, okumele ilungiselelwe ngokucophelela.Nakuba ama-electrode asekelwe ku-carbon enokuqina okuhle kwamakhemikhali kanye ne-electrochemical kanye nokuhamba kahle kagesi, uma kushiywe kungalashwa, i-kinetics yabo izohamba kancane ngenxa yokungabikho kwamaqembu okusebenza kwe-oksijeni kanye ne-hydrophilicity7,8.Ngakho-ke, ama-electrocatalyst ahlukahlukene ahlanganiswa nama-electrode ekhabhoni, ikakhulukazi ama-carbon nanostructures nama-oxide ensimbi, ukuze kuthuthukiswe i-kinetics yawo womabili ama-electrode, ngaleyo ndlela kwandise i-kinetics yama-electrode e-VRFB.
Kusetshenziswe izinto eziningi zekhabhoni, njenge-carbon paper9, carbon nanotubes10,11,12,13, graphene-based nanostructures14,15,16,17, carbon nanofibers18 nezinye19,20,21,22,23, ngaphandle komndeni we-fulerene. .Esifundweni sethu sangaphambilini ku-C76, sibike ngokokuqala ngqa umsebenzi omuhle kakhulu we-electrocatalytic wale fullerene ukuya ku-VO2+/VO2+, uma kuqhathaniswa nendwangu yekhabhoni ephethwe ukushisa nengaphathwanga, ukumelana nokudlulisa icala kwehliswe ngo-99.5% no-97%24.Ukusebenza kwe-catalytic yezinto zekhabhoni zokusabela kwe-VO2+/VO2+ uma kuqhathaniswa ne-C76 kuboniswa kuThebula S1.Ngakolunye uhlangothi, ama-oxide amaningi ensimbi afana ne-CeO225, ZrO226, MoO327, NiO28, SnO229, Cr2O330 kanye ne-WO331, 32, 33, 34, 35, 36, 37, 38 asetshenziswa ngenxa yokwanda kokumanzisa kwawo kanye nokuqukethwe okuphezulu kwe-oxygen.amaqembu.Ithebula S2 libonisa ukusebenza okunamandla kwalawa ma-oxide ensimbi ekuphenduleni kwe-VO2+/VO2+.I-WO3 isetshenziswe enanini elibalulekile lemisebenzi ngenxa yezindleko zayo eziphansi, ukuzinza okuphezulu kwemithombo ye-acidic, kanye nomsebenzi ophezulu we-catalytic31,32,33,34,35,36,37,38.Kodwa-ke, i-WO3 ibonise ukuthuthukiswa okuncane ku-cathode kinetics.Ukuze kuthuthukiswe ukuqhutshwa kwe-WO3, umphumela wokusebenzisa i-tungsten oxide encishisiwe (W18O49) kumsebenzi we-electrode omuhle uhlolwe38.I-Hydrated tungsten oxide (HWO) ayikaze ihlolwe kuzinhlelo zokusebenza ze-VRFB, nakuba ibonise umsebenzi ophezulu kuzinhlelo zokusebenza ze-supercapacitor ngenxa yokusabalalisa kwe-cation okusheshayo uma kuqhathaniswa ne-anhydrous WOx39,40.Ibhethri lokugeleza kwesizukulwane sesithathu i-all-vanadium redox lisebenzisa i-electrolyte ye-asidi exubile eyakhiwe i-HCl ne-H2SO4 ukuze kuthuthukiswe ukusebenza kwebhethri futhi kuthuthukiswe ukunyibilika nokuzinza kwama-ion e-vanadium ku-electrolyte.Kodwa-ke, i-parasitic chlorine evolution reaction isibe enye yezinto ezimbi zesizukulwane sesithathu, ngakho-ke ukuthola izindlela zokucindezela ukusabela kokuhlolwa kwe-chlorine sekuwumsebenzi wamaqembu amaningana ocwaningo.
Lapha, ukuhlolwa kokusabela kwe-VO2+/VO2+ kwenziwa kuzinhlanganisela ze-HWO/C76 ezifakwe kuma-electrode endwangu ye-carbon ukuze kutholwe ibhalansi phakathi kokuhamba kukagesi kwezinhlanganisela kanye ne-redox reaction kinetics endaweni ye-electrode kuyilapho kucindezela ukufakwa kwe-chlorine eyipharamitha.ukusabela (KVR).Ama-nanoparticles e-tungsten oxide (HWO) afakwe emanzini ahlanganiswa ngendlela elula ye-hydrothermal.Ukuhlolwa kwenziwa ku-electrolyte ye-asidi exubile (H2SO4/HCl) ukuze kulingise isizukulwane sesithathu i-VRFB (G3) ukuze kube lula futhi kuphenywe umthelela we-HWO ekuphenduleni kokuvela kwe-chlorine eyisinambuzane42.
I-Vanadium(IV) sulfate oxide hydrate (VOSO4, 99.9%, Alfa-Aeser), sulfuric acid (H2SO4), hydrochloric acid (HCl), dimethylformamide (DMF, Sigma-Aldrich), polyvinylidene fluoride (PVDF, Sigma-Aldrich), sodium I-Tungsten oxide dihydrate (Na2WO4, 99%, Sigma-Aldrich) ne-hydrophilic carbon cloth ELAT (Fuel Cell Store) zisetshenziswe kulolu cwaningo.
I-tungsten oxide (HWO) ene-Hydrated yalungiselelwa ukusabela kwe-hydrothermal lapho u-2 g kasawoti we-Na2WO4 yancibilika ku-12 ml we-HO kuze kutholakale ikhambi elingenambala, bese kwengezwa u-12 ml we-2 M HCl kuze kube yilapho ukumiswa okuphuzi okukhanyayo. yatholwa.ukumiswa.Ukusabela kwe-hydrothermal kwenziwa ku-autoclave yensimbi engenasici e-Teflon kuhhavini engu-180 ºC amahora angu-3.Izinsalela ziqoqwe ngokuhlunga, zigezwe izikhathi ezingu-3 nge-ethanol namanzi, zomiswe kuhhavini ngo-70 ° C for ~ 3 h, bese zigaywa ukuze kutholwe i-HWO powder eluhlaza okwesibhakabhaka.
I-carbon cloth electrode (CCTs) etholiwe (engaphathwanga) isetshenziswe ngendlela etholwe ngayo noma ifakwe ngaphansi kokwelashwa kokushisa esithandweni somlilo ku-450 ° C ngamahora angu-10 ngesilinganiso sokushisa esingu-15 ° C / min emoyeni kuya thola i-UCC (TCC) eyalashwayo, s Ngokufanayo nomsebenzi wangaphambilini 24. I-UCC ne-TCC zasikwa zaba ama-electrode acishe abe ngu-1.5 cm ububanzi no-7 cm ubude.Ukumiswa kwe-C76, HWO, HWO-10% C76, HWO-30% C76 kanye ne-HWO-50% C76 kwalungiselelwa ngokwengeza u-20 mg wempushana esebenzayo kanye no-10 wt% (~2.22 mg) we-PVDF binder ku-~1 ml ye I-DMF ilungiselelwe futhi ifakwe i-sonicated ihora elingu-1 ukuze kuthuthukiswe ukufana.Khona-ke u-2 mg wezinhlanganisela ze-C76, i-HWO ne-HWO-C76 zasetshenziswa cishe ku-1.5 cm2 wendawo ye-electrode esebenzayo ye-UCC.Wonke ama-catalysts alayishwa kuma-electrode e-UCC futhi i-TCC yasetshenziselwa izinjongo zokuqhathanisa kuphela, njengoba umsebenzi wethu wangaphambili ubonise ukuthi ukwelashwa kokushisa akudingeki i-24.Ukulungiswa kombono kwafinyelelwa ngokuxubha i-100 µl yokumiswa (umthwalo 2 mg) ukuze kufane kakhulu.Khona-ke wonke ama-electrode omiswa kuhhavini ngobusuku obungama-60 ° C.Ama-electrode akalwa ngaphambi nangemuva kokuqinisekisa ukulayishwa kwesitoko okunembile.Ukuze ube nendawo ethile yejometri (~ 1.5 cm2) futhi uvimbele ukuphakama kwe-vanadium electrolyte kuma-electrodes ngenxa yomphumela we-capillary, ungqimba omncane weparafini wasetshenziswa phezu kwezinto ezisebenzayo.
Isibonakhulu se-electron emission scanning (FESEM, Zeiss SEM Ultra 60.5 kV) yasetshenziswa ukuze kubhekwe i-HWO surface morphology.I-spectroscopy ye-X-ray ehlakaza amandla efakwe i-Feii8SEM (EDX, Zeiss AG) yasetshenziswa ukwenza imephu yezinto ze-HWO-50%C76 kuma-electrode e-UCC.Isibonakhulu se-electron edlulisa ukulungiswa okuphezulu (HR-TEM, JOEL JEM-2100) esebenza ngevolthi esheshayo engu-200 kV yasetshenziswa ukuze kutholwe izithombe zokucaca okuphezulu namaringi e-diffraction ezinhlayiya ze-HWO.Sebenzisa isofthiwe ye-Crystallographic Tool Box (CrysTBox) ukuze uhlaziye izindandatho ze-HWO diffraction usebenzisa umsebenzi we-ringGUI futhi uqhathanise imiphumela namamodeli we-XRD.Isakhiwo kanye ne-graphitization ye-UCC ne-TCC kunqunywe yi-X-ray diffraction (XRD) ngesilinganiso sokuskena esingu-2.4°/min kusuka ku-5° kuya ku-70° nge-Cu Kα (λ = 1.54060 Å) kusetshenziswa i-Panalytical X-ray diffractometer.(Imodeli 3600).I-XRD ikhombisa ukwakheka kwekristalu nezigaba ze-HWO.Isofthiwe ye-PANalytical X'Pert HighScore isetshenziselwe ukufanisa iziqongo ze-HWO namamephu we-tungsten oxide atholakala kusizindalwazi45.Qhathanisa imiphumela ye-HWO nemiphumela ye-TEM.Ukwakheka kwamakhemikhali nesimo samasampuli e-HWO kunqunywe i-X-ray photoelectron spectroscopy (XPS, ESCALAB 250Xi, ThermoScientific).Isofthiwe ye-CASA-XPS (v 2.3.15) isetshenziselwe ukukhishwa kwe-deconvolution nokuhlaziya idatha.Ukulinganisa kwe-Fourier transform infrared spectroscopy (FTIR, kusetshenziswa i-Perkin Elmer class KBr FTIR spectrometer) kwenziwa ukuze kutholwe amaqembu asebenza phezulu e-HWO ne-HWO-50% C76.Qhathanisa imiphumela nemiphumela ye-XPS.Izilinganiso zama-engeli othintana naye (KRUSS DSA25) nazo zasetshenziswa ukukhombisa ukumanzisa kwama-electrode.
Kuzo zonke izilinganiso ze-electrochemical, indawo yokusebenza ye-Biologic SP 300 yasetshenziswa.I-Cyclic voltammetry (CV) kanye ne-electrochemical impedance spectroscopy (EIS) zisetshenziswe ukutadisha i-electrode kinetics ye-VO2+/VO2+ redox reaction kanye nomthelela we-reagent diffusion (VOSO4 (VO2+)) kwizinga lokusabela.Bobabili ubuchwepheshe busebenzisa iseli lama-electrode amathathu ane-electrolyte concentration engu-0.1 M VOSO4 (V4+) encibilike ku-1 M H2SO4 + 1 M HCl (i-asidi exutshiwe).Yonke idatha ye-electrochemical eyethulwa i-IR ilungisiwe.Ikhoyili ye-calomel egcwele (SCE) kanye nekhoyili yeplatinamu (Pt) kwasetshenziswa njengereferensi ne-counter electrode, ngokulandelana.Ku-CV, amanani wokuskena (ν) we-5, 20, kanye no-50 mV/s asetshenziswe efasiteleni elingaba khona (0–1) V uma kuqhathaniswa ne-SCE ye-VO2+/VO2+, bese elungiswa esikalini se-SHE ukuze kufakwe itulo (VSCE = 0.242 V uma kuqhathaniswa ne-HSE) .Ukuze kuphenywe ukugcinwa komsebenzi we-electrode, ukugaywa kabusha kwe-CV kwenziwa ku-UCC, TCC, UCC-C76, UCC-HWO kanye ne-UCC-HWO-50% C76 ngo-ν elingana no-5 mV/s.Ezilinganisweni ze-EIS zokusabela kwe-VO2+/VO2+ redox, ububanzi befrikhwensi obungu-0.01-105 Hz kanye nokuphazamiseka kwamandla wesekethe evulekile (OCV) okungu-10 mV.Ukuhlolwa ngakunye kwaphindwa izikhathi ezingu-2-3 ukuze kuqinisekiswe ukuhambisana kwemiphumela.Izilinganiso zesilinganiso ezingafani (k0) zitholwe ngendlela ye-Nicholson46,47.
I-tungsten oxide enamanzi (HVO) yenziwe ngempumelelo ngendlela ye-hydrothermal.Isithombe se-SEMI-1a ibonisa ukuthi i-HWO efakiwe iqukethe amaqoqo ama-nanoparticles anosayizi bezinhlayiyana kububanzi obungu-25–50 nm.
Iphethini ye-X-ray diffraction ye-HWO ibonisa iziqongo (001) kanye (002) kokuthi ~23.5° kanye no-~47.5°, ngokulandelana, okuyisici se-nonstoichiometric WO2.63 (W32O84) (PDF 077–0810, a = 21.4 Å, b = 17.8 Å, c = 3.8 Å, α = β = γ = 90 °), ehambisana nombala wayo oluhlaza okwesibhakabhaka obonakalayo (Fig. 1b)48,49.Ezinye iziqongo ezicishe zibe ngu-20.5°, 27.1°, 28.1°, 30.8°, 35.7°, 36.7° kanye no-52.7° ziku-(140), (620), (350), (720), (740), (560).kanye (970) nezindiza ze-diffraction, ngokulandelana, 49 orthorhombic WO2.63.Songara et al.43 isebenzise indlela yokwenziwa efanayo ukuze kutholwe umkhiqizo omhlophe, okwakubalulwe ukuba khona kwe-WO3(H2O)0.333.Kodwa-ke, kulo msebenzi, ngenxa yezimo ezihlukene, kutholwe umkhiqizo ompunga oluhlaza okwesibhakabhaka, obonisa ukuhlalisana kwe-WO3(H2O) 0.333 (PDF 087-1203, a = 7.3 Å, b = 12.5 Å, c = 7.7) ku-Å , α = β = γ = 90°) kanye nesimo esincishisiwe se-tungsten oxide.Ukuhlaziywa kwe-semiquantitative ngesofthiwe ye-X'Pert HighScore kubonise u-26% WO3(H2O)0.333: 74% W32O84.Njengoba i-W32O84 iqukethe i-W6+ ne-W4+ (1.67:1 W6+:W4+), okuqukethwe okulinganiselwe kwe-W6+ ne-W4+ cishe ku-72% W6+ no-28% W4+, ngokulandelanayo.Izithombe ze-SEM, i-spectra ye-XPS yesekhondi elingu-1 ezingeni le-nucleus, izithombe ze-TEM, i-FTIR spectra kanye ne-Raman spectra yezinhlayiya ze-C76 zethulwe ephepheni lethu langaphambilini24.Ngokuka-Kawada et al.50,51, iphethini ye-X-ray diffraction ye-C76 ibonisa isakhiwo se-monoclinic se-FCC ngemva kokususwa kwe-toluene.
Izithombe ze-SEM ku-fig.2a kanye no-b kubonisa ukufakwa ngempumelelo kwe-HWO ne-HWO-50% C76 phakathi naphakathi kwama-carbon fibers ama-electrode e-UCC.Imephu ye-elemental ye-tungsten, ikhabhoni nomoya-mpilo emfanekisweni we-SEM ku-Fig. 2c iboniswa kufig.I-2d–f ebonisa ukuthi i-tungsten nekhabhoni kuxutshwe ngokulinganayo (kubonisa ukusatshalaliswa okufanayo) phezu kwendawo ye-electrode futhi inhlanganisela ayifakwanga ngokulinganayo.ngenxa yemvelo yendlela yezulu.
Izithombe ze-SEM zezinhlayiya ezifakiwe ze-HWO (a) nezinhlayiyana ze-HWO-C76 (b).Imephu ye-EDX elayishwe ku-HWO-C76 e-UCC kusetshenziswa indawo esesithombeni (c) ibonisa ukusatshalaliswa kwe-tungsten (d), ikhabhoni (e), nomoya-mpilo (f) kusampula.
I-HR-TEM isetshenziselwe ukuthwebula isithombe sokukhulisa okuphezulu nolwazi lwecrystallographic (Umfanekiso 3).I-HWO ibonisa i-nanocube morphology njengoba kukhonjisiwe kuMfanekiso 3a futhi ngokucacile kuMfanekiso 3b.Ngokukhulisa i-nanocube yokuhlukanisa indawo ekhethiwe, ukwakheka kwegrayiti kanye nezindiza ezihlukanisayo ezanelisa umthetho kaBragg zingabonwa ngeso lengqondo njengoba kuboniswe kuMfanekiso 3c, okuqinisekisa ubucwebe bento.Esihlokweni esikuFig. 3c sikhombisa ibanga d 3.3 Å elihambisana nezindiza ze-diffraction (022) kanye (620) ezigabeni ezingu-WO3(H2O)0.333 kanye ne-W32O84, 43, 44, 49, ngokulandelana.Lokhu kuhambisana nokuhlaziywa kwe-XRD okungenhla (I-Fig. 1b) njengoba ibanga lendiza eligayiwe eliqashiwe d (Umfanekiso 3c) lihambisana nenani eliphakeme le-XRD eliqine kakhulu kusampula ye-HWO.Izindandatho zesampula nazo zikhonjiswe emkhiwaneni.3d, lapho indandatho ngayinye ihambisana nendiza ehlukile.Izindiza ze-WO3(H2O) 0.333 kanye ne-W32O84 zinemibala emhlophe neluhlaza okwesibhakabhaka, ngokulandelana, futhi iziqongo zazo ezihambisanayo ze-XRD nazo ziboniswa ku-Fig. 1b.Iringi yokuqala eboniswe kuphethini yendandatho ihambisana nenani eliphakeme lokuqala elimakiwe kuphethini ye-x-ray yendiza ye-diffraction (022) noma (620).Ukusuka ku-(022) kuye ku-(402) izindandatho, amabanga angu-d-3.30, 3.17, 2.38, 1.93, kanye no-1.69 Å atholwe, ahambisana namanani e-XRD angu-3.30, 3.17, 2 .45, 1.66 kanye no-1.63.Å, 44, 45, ngokulandelana.
(a) Isithombe se-HR-TEM se-HWO, (b) sibonisa isithombe esinwetshiwe.Izithombe zezindiza ezisanhlamvu ziboniswa ku-(c), futhi inset (c) ibonisa isithombe esikhulisiwe sezindiza kanye nesikhawu esingu-d 0.33 nm esihambisana nezindiza (002) kanye (620).(d) Iphethini yeringi ye-HWO ebonisa izindiza ezihlotshaniswa nezigaba ze-WO3(H2O)0.333 (ezimhlophe) kanye ne-W32O84 (eluhlaza okwesibhakabhaka).
Ukuhlaziywa kwe-XPS kwenziwa ukuze kunqunywe ikhemistri engaphezulu nesimo se-oxidation se-tungsten (Izibalo S1 no-4).I-spectrum yokuskena kwe-XPS yobubanzi obubanzi be-HWO ehlanganisiwe iboniswa ku-Fig.I-S1, ekhombisa ukuba khona kwe-tungsten.I-spectra ye-XPS yokuskena encane yamazinga amakhulu we-W 4f kanye ne-O 1s iboniswa ku-Fig.4a kanye b, ngokulandelana.I-spectrum ye-W 4f ihlukaniswe yaba ama-spin-orbit double double ahambisana namandla abophayo wesimo se-oxidation W. Iziqongo ezingu-W 4f5/2 kanye ne-W 4f7/2 emandleni ahlanganisayo angu-37.8 no-35.6 eV ngeze-W6+, kanti iziqongo ezingu-W I-4f5/2 kanye ne-W 4f7/2 ku-36.6 kanye ne-34.9 eV ziyisici sesimo se-W4+, ngokulandelanayo.Ukuba khona kwesimo se-oxidation (W4 +) kuqinisekisa ngokuqhubekayo ukwakheka kwe-WO2.63 engeyona i-stoichiometric, kuyilapho ukuba khona kwe-W6 + kubonisa i-stoichiometric WO3 ngenxa ye-WO3 (H2O) 0.333.Idatha efakiwe ibonise ukuthi amaphesenti e-athomu e-W6+ ne-W4+ ayengama-85% kanye no-15%, ngokulandelana, ayesondele kakhulu kumanani alinganiselwe kusukela kudatha ye-XRD, uma kubhekwa umehluko phakathi kobuchwepheshe obubili.Zombili izindlela zinikeza ulwazi lobuningi ngokunemba okuphansi, ikakhulukazi i-XRD.Ngaphezu kwalokho, lezi zindlela ezimbili zihlaziya izingxenye ezihlukene zezinto ezibonakalayo ngoba i-XRD iyindlela yobuningi kuyilapho i-XPS iyindlela engaphezulu esondela kuma-nanometer ambalwa kuphela.I-spectrum ye-O 1s ihlukana ibe iziqongo ezimbili ku-533 (22.2%) kanye no-530.4 eV (77.8%).Eyokuqala ihambisana ne-OH, kanti eyesibili ihambisana ne-oxygen bond ku-lattice ku-WO.Ukuba khona kwamaqembu e-OH asebenzayo kuhambisana nezakhiwo ze-hydration ze-HWO.
Ukuhlaziywa kwe-FTIR kuphinde kwenziwa kulawa masampuli amabili ukuze kuhlolwe ubukhona bamaqembu asebenzayo kanye nama-molecule amanzi adidiyelwe esakhiweni se-HWO esinamanzi.Imiphumela ibonisa ukuthi isampula ye-HWO-50% C76 kanye nemiphumela ye-FT-IR HWO ibukeka ngokufanayo ngenxa yokuba khona kwe-HWO, kodwa ukushuba kweziqongo kuyahluka ngenxa yamanani ahlukene esampula asetshenziswa ngesikhathi sokulungiselelwa ukuhlaziya (Fig. 5a ).HWO-50% C76 Zonke iziqongo ze-fulerene 24 ziyaboniswa ngaphandle kwesiqongo se-tungsten oxide.Inemininingwane emkhiwaneni.I-5a ibonisa ukuthi womabili amasampula abonisa ibhendi ebanzi eqinile kakhulu ku-~710/cm, abalulwe ukudlidliza okwelula kwe-OWO esakhiweni se-lattice se-HWO, kanye nehlombe eliqinile elingu-~840/cm, elibalelwa ku-WO.ibhendi ecijile kokuthi ~1610/cm ihlobene nokudlidliza okugobayo kwe-OH, futhi ibhendi yokumunca ebanzi kokuthi ~3400/cm ihlobene nokudlidliza okunwebekayo kwe-OH kuqembu le-hydroxyl43.Le miphumela ihambisana ne-XPS spectrum ku-Fig. 4b, lapho iqembu elisebenzayo le-WO linganikeza amasayithi asebenzayo wokusabela kwe-VO2+/VO2+.
Ukuhlaziywa kwe-FTIR kwe-HWO ne-HWO-50% C76 (a) okubonisa amaqembu asebenzayo nezilinganiso ze-engeli yokuxhumana (b, c).
Iqembu le-OH lingakwazi futhi ukugqugquzela ukusabela kwe-VO2+/VO2+, ngaleyo ndlela likhulise i-hydrophilicity ye-electrode, ngaleyo ndlela likhuthaze amazinga okusabalalisa kanye nokudlulisa ama-electron.Isampula ye-HWO-50% C76 ibonisa ukuphakama kwe-C76 eyengeziwe njengoba kuboniswe esithombeni.Iziqongo kokuthi ~2905, 2375, 1705, 1607, and 1445 cm3 zingabelwa ukudlidliza okunwebekayo okungu-CH, O=C=O, C=O, C=C, kanye ne-CO, ngokulandelana.Kuyaziwa ukuthi amaqembu asebenza komoyampilo C=O kanye ne-CO angasebenza njengezikhungo ezisebenzayo zokusabela kwe-redox ye-vanadium.Ukuze kuhlolwe futhi kuqhathaniswe ukumanzisa kwama-electrode amabili, izilinganiso ze-engeli yokuxhumana zisetshenziswe njengoba kuboniswe ku-Fig. 5b, c.I-electrode ye-HWO imunca ngokushesha amaconsi amanzi, okubonisa i-superhydrophilicity ngenxa yamaqembu asebenzayo we-OH atholakalayo.I-HWO-50% C76 i-hydrophobic kakhulu, ine-engeli yokuxhumana cishe engu-135° ngemva kwemizuzwana engu-10.Kodwa-ke, ezilinganisweni ze-electrochemical, i-electrode ye-HWO-50% C76 yayimanziswe ngokuphelele ngaphansi komzuzu.Izilinganiso zokumanzisa ziyahambisana nemiphumela ye-XPS ne-FTIR, okuphakamisa ukuthi amaqembu e-OH engeziwe endaweni ye-HWO ayenza ibe ne-hydrophilic kakhulu.
Ukusabela kwe-VO2+/VO2+ kwe-HWO kanye ne-HWO-C76 nanocomposites kwahlolwa futhi kwakulindeleke ukuthi i-HWO icindezele ukuvela kwegesi ye-chlorine okwenzeka ngesikhathi sokusabela kwe-VO2+/VO2+ kuma-asidi axubile, kuyilapho i-C76 izoqhubekisela phambili i-VO2+/ VO2+ efunwayo.Ukumiswa kwe-HWO okuqukethe u-10%, 30% no-50% C76 kusetshenziswe kuma-electrode e-UCC anomthwalo ophelele ongaba ngu-2 mg/cm2.
Njengoba kuboniswe emkhiwaneni.6, i-kinetics yokusabela kwe-VO2+/VO2+ endaweni ye-electrode yahlolwa kusetshenziswa i-CV kuma-electrolyte ane-asidi exubile.I-Currents iboniswa njenge-I/Ipa ukuze kube lula ukuqhathanisa i-ΔEp ne-Ipa/Ipc.Ama-catalysts ahlukahlukene atholakala ngokuqondile kumfanekiso.Idatha yendawo yamanje ikhonjisiwe kuMfanekiso 2S.Emkhiwaneni.Umfanekiso 6a ubonisa ukuthi i-HWO inyusa kancane izinga lokudlulisa i-electron ye-VO2+/VO2+ redox yokusabela endaweni ye-electrode futhi icindezela ukusabela kwe-parasitic chlorine evolution.Kodwa-ke, i-C76 inyusa kakhulu izinga lokudlulisa ama-electron futhi igqugquzela ukusabela kokuvela kwe-chlorine.Ngakho-ke, inkimbinkimbi enokwakheka okulungile kwe-HWO ne-C76 kufanele ibe nomsebenzi omuhle kakhulu kanye nekhono eliphakeme kakhulu lokuvimbela ukusabela kwe-chlorine.Kutholakale ukuthi ngemva kokwandisa okuqukethwe kwe-C76, umsebenzi we-electrochemical we-electrode uthuthukisiwe, njengoba kuboniswa ukwehla kwe-ΔEp kanye nokwanda kwesilinganiso se-Ipa / Ipc (Ithebula S3).Lokhu kuphinde kwaqinisekiswa amanani e-RCT akhishwe esakhiweni se-Nyquist ku-Fig. 6d (ithebula S3), lapho kutholakale khona ukuthi amanani e-RCT ehla ngokuqukethwe okwandayo kwe-C76.Le miphumela ibuye ihambisane nocwaningo luka-Lee lapho ukungezwa kwekhabhoni ye-mesoporous ku-mesoporous WO3 kuthuthukise indlela yokudlulisa ukushaja ku-VO2+/VO2+35.Lokhu kuphakamisa ukuthi ukusabela okuhle kungase kuncike kakhulu ekuphatheni kwe-electrode (C=C bond)18,24,35,36,37.Ngenxa yoshintsho ku-geometry yokuxhumanisa phakathi kwe-[VO(H2O)5]2+ ne-[VO2(H2O)4]+, i-C76 ingaphinda inciphise ukusabela ngokweqile ngokunciphisa amandla ezicubu.Nokho, lokhu kungase kungenzeki ngama-electrode e-HWO.
(a) Ukuziphatha kwe-voltammetric ye-cyclic ye-UCC ne-HWO-C76 enezilinganiso ezihlukile ze-HWO:C76 ekuphenduleni kwe-VO2+/VO2+ ku-0.1 M VOSO4/1 M H2SO4 + 1 M HCl electrolyte (ku-ν = 5 mV/s).(b) I-Randles-Sevchik kanye (c) nendlela ka-Nicholson ye-VO2+/VO2+ yokulinganisa ukusebenza kahle kokusabalalisa kanye nokuthola amanani we-k0 (d).
Akukhona nje kuphela ukuthi i-HWO-50% C76 yayibonisa cishe umsebenzi ofanayo we-electrocatalytic njenge-C76 yokusabela kwe-VO2+/VO2+, kodwa, okuthakazelisa nakakhulu, iphinde yacindezela ukuvela kwegesi ye-chlorine uma kuqhathaniswa ne-C76, njengoba kuboniswe esithombeni.6a, ngaphezu kokubonisa ingxenye encane yesiyingi kufig.6g (RCT ephansi).I-C76 ibonise i-Ipa/Ipc esobala ephakeme kune-HWO-50% C76 (Ithebula S3), hhayi ngenxa yokuhlehla kokusabela okuthuthukisiwe, kodwa ngenxa yokugqagqana nenani eliphakeme lokunciphisa i-chlorine ku-1.2 V uma kuqhathaniswa ne-SHE.Ukusebenza okuhle kakhulu kwe-HWO-50% C76 kubalulwe ekusebenzisaneni phakathi kwe-C76 ekhokhiswa kabi eqhuba kahle kanye nokumanzisa okuphezulu nokusebenza kwe-catalytic kwe-W-OH ku-HWO.Nakuba ukukhishwa kwe-chlorine encane kuzothuthukisa ukusebenza kahle kokushaja kweseli eligcwele, i-kinetics ethuthukisiwe izokwandisa ukusebenza kahle kwe-voltage yeseli egcwele.
Ngokusho kwe-equation S1, ekuphenduleni okungahlehliswa kabusha (okulinganiselwe ngokulinganiswa kwe-electron) okulawulwa ukusabalalisa, umthamo wamanje (IP) uncike enanini lama-electron (n), indawo ye-electrode (A), i-diffusion coefficient (D), inombolo yama-electron adlulisa i-coefficient (α) nesivinini sokuskena (ν).Ukuze kufundwe ukuziphatha okulawulwayo kokusatshalaliswa kwezinto ezihloliwe, ubudlelwano phakathi kwe-IP ne-ν1/2 bahlelwa futhi baboniswa ku-Fig. 6b.Njengoba zonke izinto ezisetshenziswayo zibonisa ubudlelwano bomugqa, ukusabela kulawulwa ukusabalalisa.Njengoba impendulo ye-VO2+/VO2+ ikwazi ukuhlehliswa ngendlela efanayo, ukuthambeka komugqa kuncike ku-coefficient yokusabalalisa kanye nenani lika-α (isibalo S1).Ngenxa ye-coefficient yokusabalalisa engashintshi (≈ 4 × 10–6 cm2/s) 52, umehluko emthambekeni womugqa ubonisa ngokuqondile amanani ahlukene ka-α ngakho-ke amazinga ahlukene okudluliselwa kwe-electron endaweni ye-electrode, ne-C76 ne-HWO -50 % C76, ekhombisa izindawo eziphakeme kakhulu (izinga eliphakeme kakhulu lokudlulisa ama-electron).
Imithambeka ebaliwe yemvamisa ephansi ye-Warburg (W) eboniswe kuThebula S3 (Fig. 6d) inamanani asondele koku-1 kuzo zonke izinto zokwakha, ebonisa ukusakazeka okuphelele kwezinhlayiya ze-redox futhi iqinisekisa ukuziphatha okuqondile kwe-IP ngokumelene no-ν1/2 ku-CV .izilinganiso .Ku-HWO-50% C76, i-Warburg slope ichezuka ebunyeni iye ku-1.32, iphakamisa umnikelo hhayi kuphela kusukela ekusakazeni okungapheli kwama-reactants (VO2+), kodwa futhi nokuziphatha okungenzeka kongqimba oluncane ekuziphatheni kokusabalalisa ngenxa ye-electrode porosity.
Ukuze kuqhutshekwe kuhlaziywe ukuhlehla (isilinganiso sokudlulisa ama-electron) sokusabela kwe-VO2+/VO2+ redox, indlela yokusabela ye-Nicholson quasi-reversible reversible nayo yasetshenziswa ukuze kunqunywe izinga elijwayelekile elingu-k041.42.Lokhu kwenziwa ngokuhlela ipharamitha yekinetic engena-dimensionless Ψ njengomsebenzi we-ΔEp njengomsebenzi ka-ν−1/2 kusetshenziswa isibalo se-S2.Ithebula S4 libonisa amanani angu-Ψ avelayo wento ngayinye ye-electrode.Hlela imiphumela (Umdwebo 6c) ukuze uthole u-k0 × 104 cm/s (obhalwe eduze komugqa ngamunye futhi wethulwe kuThebula u-S4) usebenzisa i-equation S3 emthambekeni wesakhiwo ngasinye.I-HWO-50% C76 itholwe inomthambeka ophakeme kakhulu (Fig. 6c) ngakho-ke inani eliphakeme kakhulu le-k0 lika-2.47 × 10-4 cm/s.Lokhu kusho ukuthi le electrode inikeza ama-kinetics ashesha kakhulu ahambisana nemiphumela ye-CV ne-EIS ku-Figure 6a no-d kanye neThebula S3.Ngaphezu kwalokho, amanani we-k0 aphinde atholakala ku-Nyquist plots (Fig. 6d) ye-Equation S4 kusetshenziswa amanani e-RCT (Ithebula S3).Le miphumela ye-k0 evela ku-EIS ifingqwe kuThebula S4 futhi iphinde ibonise ukuthi i-HWO-50% C76 ibonisa izinga eliphezulu lokudlulisa ama-electron ngenxa yomphumela we-synergistic.Ngisho noma inani le-k0 lihluka ngenxa yemvelaphi ehlukile yendlela ngayinye, lisabonisa ukuhleleka okufanayo kobukhulu futhi libonisa ukungaguquguquki.
Ukuze uqonde ngokugcwele ama-kinetics amahle kakhulu angafinyelelwa, kubalulekile ukuqhathanisa impahla ye-electrode efanele ne-UCC engafakwanga kanye nama-electrode e-TCC.Ekuphenduleni kwe-VO2+/VO2+, i-HWO-C76 ayizange ibonise kuphela i-ΔEp ephansi kakhulu kanye nokuhlehla okungcono, kodwa futhi yacindezela kakhulu ukusabela kokuvela kwe-chlorine eyi-parasitic uma kuqhathaniswa ne-TCC, njengoba kuboniswa ukwehla okuphawulekayo kwamanje ku-1.45 V uma kuqhathaniswa nokubona i-OHA (Fig. 7a).Mayelana nokuzinza, sicabange ukuthi i-HWO-50% C76 izinzile ngokomzimba ngoba i-catalyst yayixutshwe ne-PVDF binder bese isetshenziswa kuma-electrode endwangu ye-carbon.Uma kuqhathaniswa ne-50 mV ye-UCC, i-HWO-50% C76 ibonise ukushintshwa okuphezulu kwe-44 mV ngemva kwemijikelezo engu-150 (izinga lokuwohloka 0.29 mV/umjikelezo) (Umfanekiso 7b).Kungase kungabi umehluko omkhulu, kodwa i-kinetics yama-electrode e-UCC ihamba kancane futhi ilulaza ngokuhamba ngebhayisikili, ikakhulukazi ukusabela emuva.Nakuba ukubuyiselwa emuva kwe-TCC kungcono kakhulu kunaleyo ye-UCC, i-TCC itholwe inokushintsha okukhulu kwe-73 mV ngemva kwemijikelezo engu-150, okungenzeka kube ngenxa yenani elikhulu le-chlorine ekhishwe ebusweni bayo.Ukuqinisekisa ukuthi i-catalyst ibambelela kahle endaweni ye-electrode.Njengoba kungabonakala kuwo wonke ama-electrode ahloliwe, ngisho nalawo angenawo ama-catalyst asekelwe abonisa amazinga ahlukene okungazinzi kokuhamba ngebhayisikili, okuphakamisa ukuthi izinguquko ekuhlukaniseni okuphezulu ngesikhathi sokugibela ibhayisikili kungenxa yokuvalwa kwempahla ngenxa yokushintsha kwamakhemikhali kunokuhlukana kwe-catalyst.Futhi, uma inani elikhulu lezinhlayiya ze-catalyst belizohlukaniswa endaweni ye-electrode, lokhu bekuzoholela ekwenyukeni okukhulu kokuhlukaniswa okuphezulu (hhayi nje ngo-44 mV), njengoba i-substrate (UCC) ingasebenzi ku-VO2+/VO2++ ukusabela kwe-redox.
Ukuqhathaniswa kwe-CV (a) nokuzinza kwe-redox reaction VO2+/VO2+ (b) yezinto ezisebenza kahle ze-electrode ngokuphathelene ne-CCC.Ku-electrolyte engu-0.1 M VOSO4/1 M H2SO4 + 1 M HCl, wonke ama-CV alingana no-ν = 5 mV/s.
Ukwandisa ukukhanga kwezomnotho kobuchwepheshe be-VRFB, ukuthuthukisa nokuqonda i-kinetics ye-vanadium redox reaction kubalulekile ekuzuzeni ukusebenza kahle kwamandla okuphezulu.Izinhlanganisela ze-HWO-C76 zalungiswa futhi umphumela wazo we-electrocatalytic ekuphenduleni kwe-VO2+/VO2+ wacwaningwa.I-HWO ibonise ukuthuthukiswa okuncane kwe-kinetic kodwa yacindezela kakhulu ukuvela kwe-chlorine kuma-electrolyte ane-asidi exubile.Izilinganiso ezihlukahlukene ze-HWO:C76 zisetshenzisiwe ukuze kuthuthukiswe i-kinetics yama-electrode asekelwe ku-HWO.Ukwandisa okuqukethwe kwe-C76 kuya ku-HWO kungathuthukisa i-electron transfer kinetics ye-VO2+/VO2+ reaction on the modified electrode, phakathi kwayo i-HWO-50% C76 iyimpahla engcono kakhulu ngoba yehlisa ukumelana nokushaja futhi icindezela nakakhulu ukuvela kwegesi ye-chlorine uma kuqhathaniswa C76.futhi i-TCC iyakhululwa.Lokhu kube ngenxa yomphumela we-synergistic phakathi kwe-C=C sp2 hybridization, i-OH kanye namaqembu asebenzayo e-W-OH.Izinga lokuwohloka kwe-HWO-50% C76 litholakale liyi-0.29mV/umjikelezo ngaphansi kokuhamba ngamabhayisikili amaningi kuyilapho i-UCC ne-TCC ingu-0.33mV/umjikelezo kanye no-0.49mV/umjikelezo ngokulandelanayo, okwenza izinze kakhulu kuma-electrolyte e-asidi exubile.Imiphumela ethulwe ihlonze ngempumelelo izinto zokwenziwa kwama-electrode ezisezingeni eliphezulu zokusabela kwe-VO2+/VO2+ nge-kinetics esheshayo nokuzinza okuphezulu.Lokhu kuzokhuphula amandla kagesi okukhiphayo, ngaleyo ndlela kuthuthukise ukusebenza kahle kwamandla kwe-VRFB, ngaleyo ndlela kunciphise izindleko zokudayiswa kwayo esikhathini esizayo.
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