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ʻO ke kumu kūʻai kiʻekiʻe loa o nā pahu pahu redox holo-vanadium holoʻokoʻa (VRFBs) e kaupalena i kā lākou hoʻohana ākea.Pono ka hoʻomaikaʻi ʻana i nā kinetics o nā hopena electrochemical e hoʻonui i ka mana kikoʻī a me ka pono o ka ikehu o ka VRFB, a laila e hōʻemi i ke kumukūʻai o kWh o ka VRFB.Ma keia hana, hydrothermally synthesized hydrated tungsten oxide (HWO) nanoparticles, C76 a me C76/HWO, ua waiho ma ka kalapona lole electrodes a ho'āʻo e like me electrocatalysts no ka VO2+/VO2+ redox reaction.ʻO ka microscopy electron emission scanning electron microscopy (FESEM), ikehu dispersive X-ray spectroscopy (EDX), high-resolution transmission electron microscopy (HR-TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), infrared Fourier transform Spectroscopy ( FTIR) a me nā ana kihi kihi.Ua ʻike ʻia ʻo ka hoʻohui ʻana o C76 fullerenes i ka HWO hiki ke hoʻomaikaʻi i nā kinetics electrode ma ka hoʻonui ʻana i ka conductivity uila a me ka hāʻawi ʻana i nā pūʻulu hana oxidized ma luna o kona ʻili, a laila hoʻolaha i ka hopena redox VO2 +/VO2+.ʻO ka HWO/C76 composite (50 wt% C76) ka mea i koho maikaʻi loa no ka hopena VO2+/VO2+ me ΔEp o 176 mV, ʻoiai ʻo ka lole kalapona i mālama ʻole ʻia (UCC) he 365 mV.Eia hou, ua hōʻike ka HWO/C76 composite i ka hopena hoʻohiolo nui i ka hopena chlorine evolution parasitic ma muli o ka hui hana W-OH.
ʻO ka hana ikaika a ke kanaka a me ka wikiwiki o ka ʻenehana i alakaʻi i kahi koi kiʻekiʻe loa no ka uila, e piʻi ana ma kahi o 3% i kēlā me kēia makahiki1.No nā makahiki he nui, ʻo ka hoʻohana nui ʻana i nā wahie mōʻalihaku ma ke ʻano he kumu o ka ikehu, ua alakaʻi i ka hoʻokuʻu ʻana i ke kinoea hoʻomehana honua e kōkua i ka hoʻomehana honua, ka wai a me ka pollution ea, e hoʻoweliweli ana i nā kaiaola holoʻokoʻa.ʻO ka hopena, ʻo ke komo ʻana o ka makani maʻemaʻe a hiki ke hoʻololi hou ʻia a me ka ikehu o ka lā e manaʻo ʻia e hiki i ka 75% o ka nui o ka uila e 20501. Eia naʻe, i ka wā i ʻoi aku ai ka māhele o ka uila mai nā kumu hoʻololi hou i ka 20% o ka nui o ka hana uila, lilo ka grid i mea paʻa.
Ma waena o nā ʻōnaehana mālama ikehu a pau e like me ka hybrid vanadium redox flow battery2, ua hoʻomohala ʻo all-vanadium redox flow battery (VRFB) i ka wikiwiki loa ma muli o kona mau pono he nui a ua manaʻo ʻia ʻo ia ka hopena maikaʻi loa no ka mālama ʻana i ka ikehu lōʻihi (ma kahi o 30 mau makahiki).) Nā koho i hui pū ʻia me ka ikehu hou4.ʻO kēia ma muli o ka hoʻokaʻawale ʻana o ka mana a me ka ikehu, pane wikiwiki, ke ola lōʻihi o ka lawelawe ʻana, a me ke kumu kūʻai haʻahaʻa haʻahaʻa o $ 65/kWh i hoʻohālikelike ʻia me $ 93-140/kWh no nā pahu Li-ion a me ke alakaʻi-acid a me 279-420 US kālā no kWh.pākahi pākahi 4.
Eia nō naʻe, ke kāohi ʻia nei kā lākou ʻoihana kūʻai nui ma muli o kā lākou kumukūʻai ʻōnaehana kiʻekiʻe, ʻoi loa ma muli o nā cell stacks4,5.No laila, ʻo ka hoʻomaikaʻi ʻana i ka hana hoʻopaʻa ʻana ma o ka hoʻonui ʻana i nā kinetics o nā hopena ʻelua hapa-element hiki ke hōʻemi i ka nui o ka waihona a pēlā e hōʻemi ai i ke kumukūʻai.No laila, pono ka hoʻololi electron wikiwiki i ka ʻili electrode, e hilinaʻi ana i ka hoʻolālā, haku a me ke ʻano o ka electrode a pono i ka optimization akahele6.ʻOiai ka maikaʻi o ka kemika a me ka electrochemical paʻa a me ka conductivity uila maikaʻi o nā electrodes kalapona, ua lohi kā lākou kinetics i hoʻoponopono ʻole ʻia ma muli o ka nele o nā hui hana oxygen a me ka hydrophilicity7,8.No laila, hui pū ʻia nā electrocatalysts like ʻole me nā electrodes e pili ana i ke kalapona, ʻoi aku ka nui o nā nanostructures carbon a me nā oxides metala, e hoʻomaikaʻi i nā kinetics o nā electrodes ʻelua, a laila e hoʻonui ai i nā kinetics o ka VRFB electrode.
Ma waho aʻe o kā mākou hana mua ma C76, ua hōʻike mua mākou i ka hana electrocatalytic maikaʻi loa o kēia fullerene no ka VO2 + / VO2 +, ka hoʻoili kālā, ke hoʻohālikelikeʻia me ka lole kalapona i mālamaʻia me ka wela.Hoʻemi ʻia ke kūʻē ʻana e 99.5% a me 97%.Hōʻike ʻia ka hana catalytic o nā mea kalapona no ka hopena VO2+/VO2+ i hoʻohālikelike ʻia me C76 ma ka Papa S1.Ma ka lima 'ē aʻe, he nui metala oxides e like me CeO225, ZrO226, MoO327, NiO28, SnO229, Cr2O330 a me WO331, 32, 33, 34, 35, 36, 37 ua hoʻohana 'ia no ko lakou mahuahua wettability a me ka nui o ka oxygen functionality., 38. hui.Hōʻike ʻia ka hana catalytic o kēia mau oxide metala ma ka hopena VO2+/VO2+ ma ka Papa S2.Ua hoʻohana ʻia ʻo WO3 i kahi helu nui o nā hana ma muli o kāna kumu kūʻai haʻahaʻa, kūpaʻa kiʻekiʻe i ka media acidic, a me ka hana catalytic kiʻekiʻe31,32,33,34,35,36,37,38.Eia naʻe, ʻaʻole nui ka hoʻomaikaʻi ʻana i nā kinetics cathodic ma muli o WO3.No ka hoʻomaikaʻi ʻana i ka conductivity o WO3, ua hoʻāʻo ʻia ka hopena o ka hoʻohana ʻana i ka tungsten oxide (W18O49) ma ka hana cathodic.ʻAʻole i hoʻāʻo ʻia ʻo Hydrated tungsten oxide (HWO) i nā noi VRFB, ʻoiai e hōʻike ana i ka hoʻonui ʻana i ka hana ma nā noi supercapacitor ma muli o ka wikiwiki o ka cation diffusion i hoʻohālikelike ʻia me WOx39,40 anhydrous.Ke hoʻohana nei ke kolu o ka hanauna vanadium redox flow battery i ka huila ʻakika electrolyte i haku ʻia me HCl a me H2SO4 e hoʻomaikaʻi i ka hana pākaukau a hoʻomaikaʻi i ka solubility a me ka paʻa o nā ion vanadium i loko o ka electrolyte.Eia nō naʻe, ua lilo ka hopena o ka chlorine evolution i kekahi o nā hemahema o ke kolu o ka hanauna, no laila ua lilo ka ʻimi ʻana i nā ala e pale ai i ka hopena loiloi chlorine i mea nui o nā hui noiʻi.
Ma ʻaneʻi, ua hoʻokō ʻia nā hoʻokolohua VO2 +/VO2+ ma nā HWO/C76 composites i waiho ʻia ma luna o nā electrodes lole kalapona i mea e ʻike ai i ke kaulike ma waena o ka conductivity uila o nā composites a me nā kinetics redox o ka ʻili electrode i ka wā e kāohi ana i ka hoʻomohala chlorine parasitic.pane (CER).Ua hoʻohui ʻia nā nanoparticles tungsten oxide (HWO) i kahi ʻano hydrothermal maʻalahi.Ua hoʻokō ʻia nā hoʻokolohua i loko o kahi electrolyte acid hui ʻia (H2SO4/HCl) e hoʻohālikelike i ke kolu o ka hanauna VRFB (G3) no ka hoʻomaʻamaʻa a me ka noiʻi ʻana i ka hopena o ka HWO ma ka hopena o ka chlorine evolution.
ʻO Vanadium (IV) sulfate hydrate (VOSO4, 99.9%, Alfa-Aeser), sulfuric acid (H2SO4), hydrochloric acid (HCl), dimethylformamide (DMF, Sigma-Aldrich), polyvinylidene fluoride (PVDF, Sigma) -Aldrich), sodium Tungsten oxide dihydrate, 9LATrich carbon dihydrate (Naphilic% carbon dihydrate, 29A, 9, 2000) (Fuel Cell Store) i kēia haʻawina.
Ua hoʻomākaukau ʻia ka tungsten oxide (HWO) i hoʻomākaukau ʻia e ka hopena hydrothermal 43 kahi i hoʻoheheʻe ʻia ai 2 g o ka paʻakai Na2WO4 i 12 ml o H2O no ka hāʻawi ʻana i kahi hopena kala ʻole, a laila ua hoʻohui ʻia he 12 ml o 2 M HCl i kahi dropwise e hāʻawi i kahi hoʻomaha melemele haʻahaʻa.Hoʻokomo ʻia ka slurry i loko o kahi autoclave i uhi ʻia ʻo Teflon a mālama ʻia i loko o ka umu ma 180 ° C. no 3 mau hola no ka hopena hydrothermal.Ua hōʻiliʻili ʻia ke koena ma ka kānana ʻana, holoi ʻia i 3 mau manawa me ka ethanol a me ka wai, maloʻo i loko o ka umu ma 70 ° C no ~3 mau hola, a laila triturated e hāʻawi i ka pauka HWO polū-hina.
Ua hoʻohana ʻia nā electrodes lole kalapona i loaʻa (ʻaʻole i hoʻomaʻamaʻa ʻia) e like me ke ʻano a i ʻole ka wela i mālama ʻia i loko o kahi umu pahu ma 450°C i ka lewa me ka wikiwiki hoʻomehana o 15 ºC/min no 10 mau hola e loaʻa ai nā CC i mālama ʻia (TCC).e like me ka mea i wehewehe ʻia ma ka ʻatikala mua 24.Ua ʻoki ʻia ʻo UCC a me TCC i mau electrodes ma kahi o 1.5 knm ka laulā a me 7 knm ka lōʻihi.Hoʻokuʻu ʻia o C76, HWO, HWO-10% C76, HWO-30% C76 a me HWO-50% C76 i hoʻomākaukau ʻia ma ka hoʻohui ʻana i 20 mg .% (~ 2.22 mg) o PVDF binder i ~ 1 ml DMF a sonicated no 1 hola e hoʻomaikaʻi i ka like ʻole.2 mg o C76, HWO a me HWO-C76 composites i hoʻopili ʻia i kahi UCC ikaika electrode wahi ma kahi o 1.5 cm2.Ua hoʻouka ʻia nā catalysts a pau ma luna o nā electrodes UCC a ua hoʻohana ʻia ʻo TCC no nā kumu hoʻohālikelike wale nō, ʻoiai ua hōʻike kā mākou hana mua ʻaʻole koi ʻia ka mālama wela24.Ua hoʻokō ʻia ka hoʻonā manaʻo ma ke kāhili ʻana i 100 µl o ka hoʻokuʻu ʻia (hoʻouka 2 mg) no ka hopena ʻoi aku ka maikaʻi.A laila ua maloʻo nā electrodes a pau i ka umu ma 60 ° C. i ka pō.Ana ʻia nā electrodes i mua a i hope e hōʻoia i ka hoʻouka ʻana i nā waihona.No ka loaʻa ʻana o kahi ʻāpana geometric (~ 1.5 cm2) a pale i ka piʻi ʻana o ka vanadium electrolyte i ka electrode ma muli o ka hopena capillary, ua hoʻopili ʻia kahi ʻāpana lahilahi o ka paraffin ma luna o ka mea hana.
Ua hoʻohana ʻia ke kahua emission scanning electron microscopy (FESEM, Zeiss SEM Ultra 60, 5 kV) no ka nānā ʻana i ka morphology surface HWO.Ua ho'ohana 'ia ka ikehu dispersive X-ray spectrometer me Feii8SEM (EDX, Zeiss Inc.) no ka palapala 'ana i nā mea HWO-50%C76 ma nā electrodes UCC.Ua hoʻohana ʻia kahi microscope electron hoʻonā kiʻekiʻe (HR-TEM, JOEL JEM-2100) e hana ana ma kahi voli wikiwiki o 200 kV e kiʻi i nā ʻāpana HWO hoʻonā kiʻekiʻe a me nā apo diffraction.Hoʻohana ka lako polokalamu Crystallography Toolbox (CrysTBox) i ka hana ringGUI e kālailai i ke ʻano hoʻohālikelike apo apo HWO a hoʻohālikelike i nā hopena me ke kumu XRD.Hoʻopili ʻia ke ʻano a me ka graphitization o UCC a me TCC e ka X-ray diffraction (XRD) ma ka helu scan o 2.4 ° / min mai 5 ° a i 70 ° me Cu Kα (λ = 1.54060 Å) me ka hoʻohana ʻana i ka Panalytical X-ray diffractometer (Model 3600).Ua hōʻike ʻo XRD i ke ʻano aniani a me ka pae o HWO.Ua hoʻohana ʻia ka polokalamu PANalytical X'Pert HighScore e hoʻohālikelike i nā piko o ka HWO i nā palapala ʻāina tungsten oxide i loaʻa ma ka waihona45.Ua hoʻohālikelike ʻia nā hopena HWO me nā hopena TEM.Ua hoʻoholo ʻia ke ʻano kemika a me ke kūlana o nā laʻana HWO e ka X-ray photoelectron spectroscopy (XPS, ESCALAB 250Xi, ThermoScientific).Ua hoʻohana ʻia ka polokalamu CASA-XPS (v 2.3.15) no ka deconvolution kiʻekiʻe a me ka ʻikepili ʻikepili.No ka hoʻoholo ʻana i nā pūʻulu hana ili o HWO a me HWO-50%C76, ua hana ʻia nā ana me ka hoʻohana ʻana i ka Fourier transform infrared spectroscopy (FTIR, Perkin Elmer spectrometer, me ka KBr FTIR).Ua hoʻohālikelike ʻia nā hopena me nā hopena XPS.Ua hoʻohana pū ʻia nā ana kihi pili (KRUSS DSA25) e ʻike i ka pulu o nā electrodes.
No nā ana electrochemical a pau, ua hoʻohana ʻia kahi hale hana Biologic SP 300.Ua hoʻohana ʻia ka cyclic voltammetry (CV) a me ka electrochemical impedance spectroscopy (EIS) no ke aʻo ʻana i nā kinetics electrode o ka VO2 +/VO2+ redox reaction a me ka hopena o ka reagent diffusion (VOSO4(VO2+)) ma ka helu pane.Ua hoʻohana ʻia nā ʻano ʻelua i ke kelepona ʻekolu-electrode me kahi ʻano electrolyte o 0.1 M VOSO4 (V4+) ma 1 M H2SO4 + 1 M HCl (hui ʻia o nā waikawa).Hoʻoponopono ʻia nā ʻikepili electrochemical a pau i hōʻike ʻia.Ua hoʻohana ʻia ka saturated calomel electrode (SCE) a me ka platinum (Pt) coil ma ke ʻano he reference a counter electrode.No ka CV, ua hoʻohana ʻia nā helu scan (ν) o 5, 20, a me 50 mV/s i ka puka makani VO2+/VO2+ no (0-1) V vs. SCE, a laila hoʻoponopono ʻia no SHE e hoʻolālā (VSCE = 0.242 V vs. HSE) .No ke aʻo ʻana i ka mālama ʻana i ka hana electrode, ua hana ʻia nā CV cyclic hou ma ν 5 mV/s no UCC, TCC, UCC-C76, UCC-HWO, a me UCC-HWO-50% C76.No nā ana EIS, he 0.01-105 Hz ke alapinepine o ka hopena redox VO2+/VO2+, a he 10 mV ka hoʻololi ʻana o ka volta ma ka puka makani kaapuni (OCV).Ua hana hou ʻia kēlā me kēia hoʻokolohua 2-3 mau manawa e hōʻoia i ka kūlike o nā hopena.Ua loaʻa nā mea hoʻomau heterogeneous rate (k0) e ke ala Nicholson46,47.
Ua hoʻohui maikaʻi ʻia ʻo Hydrated tungsten oxide (HVO) e ke ʻano hydrothermal.kiʻi SEM ma ka fig.Hōʻike ka 1a i ka HWO i waiho ʻia he mau pūʻulu o nā nanoparticles me nā nui ma ka laulā o 25-50 nm.
Hōʻike ke kumu hoʻohālikelike X-ray o HWO i nā piko (001) a me (002) ma ~23.5° a me ~47.5°, kēlā me kēia, ʻo ia ke ʻano o nonstoichiometric WO2.63 (W32O84) (PDF 077–0810, a = 21.4 Å.β = Å.8 γ = Å, β = Å. 90°), e pili ana i ko lakou kala uliuli akaka (Fig. 1b) 48.49.ʻO nā piko ʻē aʻe ma kahi o 20.5°, 27.1°, 28.1°, 30.8°, 35.7°, 36.7° a me 52.7° ua hāʻawi ʻia iā (140), (620), (350), (720), (740), (560°).) ) a me (970) nā mokulele ʻokoʻa i ka WO2.63.Ua hoʻohana ʻia ke ʻano hana synthetic e Songara et al.43 no ka loaʻa ʻana o kahi huahana keʻokeʻo, i hoʻopili ʻia i ka loaʻa ʻana o WO3(H2O)0.333.Eia nō naʻe, ma kēia hana, ma muli o nā kūlana like ʻole, ua loaʻa kahi huahana polū-hina, e hōʻike ana he WO3(H2O)0.333 (PDF 087-1203, a = 7.3 Å, b = 12.5 Å, c = 7 .7 Å, α = β = γ = 90°) a me ke ano hoemi o tungstend.Ua hōʻike ʻia ka hōʻike Semiquantitative me ka hoʻohana ʻana i ka polokalamu X'Pert HighScore he 26% WO3(H2O)0.333:74% W32O84.No ka mea aia ʻo W32O84 me W6+ a me W4+ (1.67:1 W6+:W4+), ʻo ka maʻiʻo i manaʻo ʻia o W6+ a me W4+ ma kahi o 72% W6+ a me 28% W4+.Ua hōʻike ʻia nā kiʻi SEM, 1-kekona XPS spectra ma ka pae nucleus, nā kiʻi TEM, FTIR spectra, a me Raman spectra o nā ʻāpana C76 i hōʻike ʻia i kā mākou ʻatikala mua.Wahi a Kawada et al., 50,51 X-ray diffraction o C76 ma hope o ka wehe ʻana o toluene i hōʻike i ke ʻano monoclinic o FCC.
Nā kiʻi SEM ma ka fig.2a a me b hōʻike i ka HWO a me ka HWO-50%C76 i waiho maikaʻi ʻia ma waena a ma waena o nā kaula kalapona o ka UCC electrode.Nā palapala 'āina EDX o ka tungsten, carbon, a me ka oxygen ma nā kiʻi SEM ma ka fig.2c ua hoikeia ma ka fig.2d-f e hōʻike ana i ka hui like ʻana o ka tungsten a me ke kalapona (e hōʻike ana i ka puʻunaue like) ma luna o ka ʻili electrode holoʻokoʻa a ʻaʻole like ka waiho ʻana o ka composite ma muli o ke ʻano o ke ʻano deposition.
Nā kiʻi SEM o nā ʻāpana HWO i waiho ʻia (a) a me nā ʻāpana HWO-C76 (b).ʻO ka palapala ʻāina ʻo EDX ma HWO-C76 i hoʻouka ʻia ma UCC me ka hoʻohana ʻana i ka ʻāpana o ke kiʻi (c) e hōʻike ana i ka puʻunaue o ka tungsten (d), kalapona (e), a me ka oxygen (f) i ka hāpana.
Ua hoʻohana ʻia ʻo HR-TEM no ke kiʻi kiʻi kiʻekiʻe a me ka ʻike crystallographic (Figure 3).Hōʻike ʻo HWO i ka morphology nanocube e like me ka hōʻike ʻana ma ka Fig. 3a a me ka maopopo loa ma ka Fig. 3b.Ma ka hoʻonui ʻana i ka nanocube no ka ʻokoʻa o nā wahi i koho ʻia, hiki i kekahi ke nānā i ke ʻano o ka grating a me nā mokulele ʻokoʻa e hoʻokō ai i ke kānāwai Bragg, e like me ka hōʻike ʻana ma ka Fig. 3c, e hōʻoia ana i ka crystallinity o ka mea.Ma ka hoʻokomo i ka Fig. 3c e hōʻike ana i ka mamao d 3.3 Å e pili ana i nā (022) a me (620) nā mokulele ʻokoʻa i loaʻa ma nā māhele WO3(H2O)0.333 a me W32O84, pakahi43,44,49.Kūlike kēia me ka hōʻike XRD i hōʻike ʻia ma luna (Fig. 1b) ʻoiai ʻo ka mamao o ka mokulele grating i ʻike ʻia d (Fig. 3c) pili i ka piko XRD ikaika loa i ka hāpana HWO.Hōʻike ʻia nā apo laʻana ma ka fig.3d, kahi e pili ai kēlā me kēia apo i kahi mokulele ʻokoʻa.ʻO nā mokulele WO3(H2O)0.333 a me W32O84 he keʻokeʻo a me ka uliuli, a ua hōʻike pū ʻia ko lākou mau piko XRD e pili ana i ke kiʻi 1b.ʻO ke apo mua i hōʻike ʻia ma ke kiʻikuhi apo e pili ana i ka piko i kaha mua ʻia ma ke ʻano x-ray o ka (022) a i ʻole (620).Mai nā apo (022) a i (402), ʻo nā helu d-spacing he 3.30, 3.17, 2.38, 1.93, a me 1.69 Å, e like me nā helu XRD o 3.30, 3.17, 2, 45, 1.93.a me 1.66 Å, ua like ia me 44, 45.
(a) kiʻi HR-TEM o HWO, (b) hōʻike i kahi kiʻi i hoʻonui ʻia.Hōʻike ʻia nā kiʻi o nā mokulele paʻi ma (c), hōʻike ʻia ka inset (c) i kahi kiʻi i hoʻonui ʻia o nā mokulele a me kahi pitch d o 0.33 nm e pili ana i nā mokulele (002) a me (620).(d) HWO kiʻi apo e hōʻike ana i nā mokulele pili me WO3(H2O)0.333 (keʻokeʻo) a me W32O84 (uliuli).
Ua hana ʻia ka loiloi XPS no ka hoʻoholo ʻana i ka kemika o ka ʻili a me ke kūlana oxidation o tungsten (Nā Kiʻi S1 a me 4).Hōʻike ʻia ka laulā ākea XPS scan spectrum o ka HWO synthesized ma ke Kiʻi S1, e hōʻike ana i ke alo o ka tungsten.Hōʻike ʻia nā kikoʻī kikoʻī XPS o nā pae kumu W 4f a me O1s ma Fig.4a a me b.Hoʻokaʻawale ʻia ka spectrum W 4f i ʻelua pālua spin-orbit e pili ana i ka ikehu hoʻopaʻa ʻana o ke kūlana W oxidation.a me W 4f7/2 ma 36.6 a me 34.9 eV ke ano o ka mokuaina W4+ o 40.)0.333.Hōʻike ka ʻikepili i hoʻopili ʻia ʻo nā pākēneka atomic o W6+ a me W4+ he 85% a me 15%, kēlā me kēia, kahi kokoke i nā waiwai i manaʻo ʻia mai ka ʻike XRD e noʻonoʻo ana i nā ʻokoʻa ma waena o nā ʻano ʻelua.Hāʻawi nā ʻano ʻelua i ka ʻike nui me ka pololei haʻahaʻa, ʻoi aku ka XRD.Eia kekahi, ʻike kēia mau ʻano ʻelua i nā ʻāpana like ʻole o ka mea no ka mea he ʻano nui ka XRD aʻo XPS kahi ʻano ʻili e hoʻokokoke wale ana i nā nanometer.Ua māhele ʻia ka spectrum O 1s i ʻelua mau piko ma 533 (22.2%) a me 530.4 eV (77.8%).Ua pili ka mua me OH, a o ka lua me na mea paa o ka oxygen ma ka lattice ma WO.ʻO ka loaʻa ʻana o nā pūʻulu hana OH e kūlike me nā waiwai hydration o HWO.
Ua hana pū ʻia kahi loiloi FTIR ma kēia mau laʻana ʻelua e nānā i ke alo o nā pūʻulu hana a me ka hoʻonohonoho ʻana i nā molekole wai i loko o ka hale HWO hydrated.Hōʻike nā hualoaʻa i ka HWO-50% C76 hāpana a me ka FT-IR HWO nā hopena ma muli o ka loaʻa ʻana o HWO, akā ʻokoʻa ka ikaika o nā piko ma muli o ka nui o ka hāpana i hoʻohana ʻia no ka hoʻomākaukau ʻana no ka nānā ʻana (Fig. 5a).) Hōʻike ka HWO-50% C76 i nā piko a pau, koe ka piko o ka tungsten oxide, pili i ka fullerene 24.Hōʻike ka 5a e hōʻike ana nā laʻana ʻelua i kahi hui ākea ikaika loa ma ~ 710/cm i hoʻoili ʻia i nā oscillations hoʻolōʻihi ʻia ʻo OWO i ka hoʻolālā lattice HWO, me kahi poʻohiwi ikaika ma ~ 840/cm i hāʻawi ʻia iā WO.No nā haʻalulu hoʻopololei, ʻike ʻia kahi kaula ʻoi ma kahi o 1610/cm i nā haʻalulu o ka OH, ʻoiai ʻo ka pūʻali hoʻoheheʻe ākea ma kahi o 3400/cm e pili ana i nā haʻalulu o OH i nā hui hydroxyl43.Kūlike kēia mau hopena me ka XPS spectra ma Fig.4b, kahi e hiki ai i nā hui hana WO ke hāʻawi i nā wahi hana no ka pane VO2+/VO2+.
ʻIkepili FTIR o HWO a me HWO-50% C76 (a), hōʻike ʻia nā pūʻulu hana a me nā ana kihi pili (b, c).
Hiki i ka hui OH ke hoʻoikaika i ka hopena VO2 + / VO2 +, me ka hoʻonui ʻana i ka hydrophilicity o ka electrode, ma laila e hoʻoikaika ai i ka wikiwiki o ka diffusion a me ka hoʻoili electron.E like me ka hōʻike ʻana, hōʻike ka laʻana HWO-50% C76 i kahi kiʻekiʻe kiʻekiʻe no C76.ʻO nā piko ma ~2905, 2375, 1705, 1607, a me 1445 cm3 hiki ke hāʻawi ʻia i ka CH, O=C=O, C=O, C=C, a me CO stretching vibrations.Ua ʻike ʻia ʻo nā hui hana oxygen C=O a me CO hiki ke lawelawe ma ke ʻano he mau kikowaena ikaika no nā hopena redox o vanadium.No ka ho'āʻo a hoʻohālikelike i ka pulu o nā electrodes ʻelua, ua lawe ʻia nā ana kihi pili e like me ka hōʻike ʻana ma ka Fig. 5b,c.Hoʻopili koke ka HWO electrode i nā kulu wai, e hōʻike ana i ka superhydrophilicity ma muli o nā pūʻulu hana OH i loaʻa.ʻOi aku ka hydrophobic HWO-50% C76, me kahi kihi pili ma kahi o 135° ma hope o 10 kekona.Eia nō naʻe, ma nā ana electrochemical, ua pulu loa ka HWO-50%C76 electrode ma lalo o hoʻokahi minuke.Ua kūlike nā ana wai me nā hualoaʻa XPS a me FTIR, e hōʻike ana i ka nui o nā pūʻulu OH ma ka ʻili HWO e ʻoi aku ka hydrophilic.
Ua ho'āʻo ʻia nā hopena VO2+/VO2+ o nā nanocomposites HWO a me HWO-C76 a ua manaʻo ʻia e hoʻopau ʻo HWO i ka chlorine evolution i ka hopena VO2+/VO2+ i loko o ka ʻakika hui ʻia, a na C76 e hoʻoikaika hou i ka hopena redox VO2+/VO2+ i makemake ʻia.%, 30%, a me 50% C76 i HWO hoʻokuʻu ʻia a me CCC i waiho ʻia ma nā electrodes me ka hoʻouka ʻana o kahi o 2 mg/cm2.
E like me ka hoike ana ma ka fig.6, ua nānā ʻia nā kinetics o ka hopena VO2+/VO2+ ma ka ʻili electrode e CV i loko o kahi electrolyte acidic hui ʻia.Hōʻike ʻia nā au i ka I/Ipa no ka hoʻohālikelike maʻalahi o ΔEp a me Ipa/Ipc no nā catalysts like ʻole ma ka pakuhi.Hōʻike ʻia ka ʻikepili ʻāpana ʻāpana o kēia manawa ma ke Kiʻi 2S.Ma ka fig.Hōʻike ka Figure 6a i ka hoʻonui iki ʻana o ka HWO i ka hoʻololi electron o ka hopena redox VO2+/VO2+ ma ka ʻili electrode a hoʻopaʻa i ka hopena o ka evolution chlorine parasitic.Eia naʻe, hoʻonui nui ʻo C76 i ka helu hoʻololi electron a hoʻopaʻa i ka hopena o ka chlorine evolution.No laila, mana'o 'ia ka 'oihana maika'i loa a me ka 'oi loa o ka hiki ke pale i ka hopena o ka chlorine evolution.Uaʻikeʻia ma hope o ka hoʻonuiʻana i ka mea o C76, ua hoʻonuiʻia ka hana electrochemical o nā electrodes, e like me ka hōʻikeʻana i ka emiʻana o ka ΔEp a me ka piʻiʻana o ka ratio Ipa / Ipc (Table S3).Ua hōʻoia pū ʻia kēia e nā waiwai RCT i unuhi ʻia mai ka ʻāpana Nyquist ma Fig. 6d (Table S3), i ʻike ʻia e emi me ka hoʻonui ʻana i ka ʻike C76.Ua kūlike pū kēia mau hopena me ka haʻawina a Li, kahi i hōʻike ʻia ai ka hoʻohui ʻana o ka kalapona mesoporous i ka mesoporous WO3 i ka hoʻomaikaʻi ʻana i nā kinetics hoʻoili kālā ma VO2+/VO2+35.Hōʻike kēia e hilinaʻi ʻoi aku ka hopena pololei i ka conductivity electrode (C=C bond) 18, 24, 35, 36, 37. ʻO kēia paha ma muli o ka hoʻololi ʻana i ka geometry coordination ma waena o [VO(H2O)5]2+ a me [VO2(H2O)4]+, C76 hōʻemi i ka overvoltage o ka ʻili.Eia naʻe, ʻaʻole hiki ke hana me nā electrodes HWO.
(a) Ka hana voltammetric Cyclic (ν = 5 mV/s) o ka pane VO2+/VO2+ o UCC a me HWO-C76 composites me HWO: C76 ratio like ole ma 0.1 M VOSO4/1 M H2SO4 + 1 M HCl electrolyte.(b) Randles-Sevchik a me (c) Nicholson VO2+/VO2+ ala no ka loiloi ʻana i ka pono diffusion a loaʻa nā waiwai k0(d).
ʻAʻole wale ʻo HWO-50% C76 e hōʻike ana i ka hana electrocatalytic like me C76 no ka hopena VO2+/VO2+, akā, ʻoi aku ka hoihoi, ua hoʻopau ʻo ia i ka ulu ʻana o ka chlorine i hoʻohālikelike ʻia me C76, e like me ka hōʻike ʻana ma ka Fig.6d (RCT haʻahaʻa).Ua hōʻike ʻo C76 i kahi Ipa/Ipc kiʻekiʻe aʻe ma mua o HWO-50% C76 (Table S3), ʻaʻole ma muli o ka hoʻomaikaʻi ʻana i ka hoʻohuli ʻana, akā no ka piʻi ʻana o ka hopena o ka hoʻohaʻahaʻa chlorine me SHE ma 1.2 V. ʻO ka hana maikaʻi loa o HWO- ʻO ka 50% C76 i pili i ka synergistic hopena ma waena o ka hopena C76 kiʻekiʻe. O.ʻO ka liʻiliʻi o ka chlorine e hoʻomaikaʻi i ka pono o ka hoʻopiʻi ʻana o ke kelepona piha, ʻoiai ka hoʻomaikaʻi ʻana i nā kinetics e hoʻomaikaʻi i ka pono o ka volta cell piha.
E like me ka hoohalike S1, no ka ho'ololi 'ana i ka quasi-reversible (relatively slow electron transfer) i ho'omalu 'ia e ka diffusion, 'o ka peak current (IP) ma muli o ka helu o nā electrons (n), electrode area (A), diffusion coefficient (D), helu o nā electrons transfer coefficient (α) a me ka scanning speed (ν).No ke aʻo ʻana i ke ʻano hoʻokalakupua o nā mea i hoʻāʻo ʻia, ua kuhi ʻia ka pilina ma waena o IP a me ν1/2 a hōʻike ʻia ma Fig. 6b.No ka mea, hōʻike nā mea a pau i ka pilina laina, hoʻomalu ʻia ka hopena e ka diffusion.No ka mea hiki ke hoʻohuli ʻia ka hopena o VO2+/VO2+, pili ka slope o ka laina i ka diffusion coefficient a me ka waiwai o α (equation S1).No ka mea he mau ka diffusion coefficient (≈ 4 × 10–6 cm2/s)52, ʻo ka ʻokoʻa o ka pali o ka laina e hōʻike pololei ana i nā waiwai like ʻole o α, a no laila ke ʻano o ka hoʻololi electron ma ka ʻili electrode, i hōʻike ʻia no C76 a me HWO -50% C76 Steepest slope.
ʻO nā pali o Warburg (W) i helu ʻia no nā alapine haʻahaʻa i hōʻike ʻia ma ka Papa S3 (Fig. 6d) he mau waiwai kokoke i ka 1 no nā mea āpau, e hōʻike ana i ka diffusion kūpono o nā ʻano redox a me ka hōʻoia ʻana i ke ʻano linear o IP i hoʻohālikelike ʻia me ν1/2. Ua ana ʻia ʻo CV.No ka HWO-50% C76, ua ha'alele ka pali o Warburg mai ka 1 a i ka 1.32, e hō'ike ana 'a'ole wale ka diffusion semi-infinite o ka reagent (VO2+), akā, he ha'awina hiki nō ho'i o ka 'ano lahilahi i ka hana diffusion ma muli o ka electrode porosity.
No ka hoʻopili hou ʻana i ka hoʻololi ʻana (ka hoʻololi uila) o ka hopena redox VO2+/VO2+, ua hoʻohana pū ʻia ka Nicholson quasi-reversible reaction method no ka hoʻoholo ʻana i ka helu maʻamau k041.42.Hana ʻia kēia me ka hoʻohana ʻana i ka hoohalike S2 ​​no ke kūkulu ʻana i ka ʻāpana kinetic dimensionless Ψ, he hana ia o ΔEp, ma ke ʻano he hana o ν-1/2.Hōʻike ka papa S4 i nā waiwai Ψ i loaʻa no kēlā me kēia mea electrode.Hoʻolālā ʻia nā hopena (Fig 6c) e loaʻa k0 × 104 cm / s mai ka pali o kēlā me kēia pā e hoʻohana ana i ka Equation S3 (kākau ʻia ma hope o kēlā me kēia lālani a hōʻike ʻia ma ka Papa S4).Ua ʻike ʻia ʻo HWO-50% C76 ka piʻi kiʻekiʻe loa (Fig. 6c), no laila ʻo ka waiwai nui o k0 he 2.47 × 10–4 cm/s.'O ia ho'i, loa'a kēia electrode i nā kinetics wikiwiki loa, i kūlike me nā hualoa'a CV a me EIS ma Fig. 6a a me d a ma ka Papa S3.Eia kekahi, ua loaʻa pū ka waiwai o k0 mai ka ʻāpana Nyquist (Fig. 6d) o ka Equation S4 me ka hoʻohana ʻana i ka waiwai RCT (Table S3).Ua hōʻuluʻulu ʻia kēia mau hopena k0 mai EIS ma ka Papa S4 a hōʻike pū ʻia ʻo HWO-50% C76 e hōʻike ana i ka nui o ka hoʻololi electron kiʻekiʻe ma muli o ka hopena synergistic.ʻOiai ʻokoʻa nā koina k0 ma muli o nā kumu like ʻole o kēlā me kēia ʻano, hōʻike mau lākou i ke ʻano like o ka nui a hōʻike i ke kūlike.
No ka hoʻomaopopo piha ʻana i nā kinetics maikaʻi loa i loaʻa, he mea nui e hoʻohālikelike i nā mea electrode maikaʻi loa me nā electrodes UCC a me TCC uncoated.No ka hopena VO2 +/VO2 +, HWO-C76 ʻaʻole i hōʻike wale i ka ΔEp haʻahaʻa a ʻoi aku ka maikaʻi o ka hoʻihoʻi ʻana, akā ua hoʻopaʻa nui ʻia ka hopena chlorine evolution parasitic i hoʻohālikelike ʻia me TCC, e like me ke ana ʻana i kēia manawa ma 1.45 V pili iā SHE (Fig. 7a).Ma ke ʻano o ke kūpaʻa, ua manaʻo mākou ua paʻa kino ʻo HWO-50% C76 no ka mea ua hui pū ʻia ka catalyst me kahi PVDF binder a laila hoʻopili ʻia i nā electrodes lole kalapona.Hōʻike ka HWO-50% C76 i ka hoʻololi kiʻekiʻe o 44 mV (degradation rate 0.29 mV/cycle) ma hope o 150 cycles i hoʻohālikelike ʻia me 50 mV no UCC (Figure 7b).ʻAʻole paha kēia he ʻokoʻa nui, akā lohi loa nā kinetics o nā electrodes UCC a hoʻohaʻahaʻa me ke kaʻa kaʻa, ʻoi aku hoʻi no nā hopena hoʻohuli.ʻOiai ʻoi aku ka maikaʻi o ka hoʻohuli ʻana o TCC ma mua o ka UCC, ua ʻike ʻia ʻo TCC i kahi hoʻololi kiʻekiʻe nui o 73 mV ma hope o 150 cycles, ʻo ia paha ma muli o ka nui o ka chlorine i hana ʻia ma luna o kona ʻili.i pili pono ka catalyst i ka ili electrode.E like me ka mea i ʻike ʻia mai nā electrodes a pau i hoʻāʻo ʻia, ʻo nā electrodes me nā catalysts kākoʻo ʻole i hōʻike i nā pae like ʻole o ka hiki ʻole o ke kaʻa kaʻa, e hōʻike ana i ka hoʻololi ʻana o ka hoʻokaʻawale kiʻekiʻe i ka wā kaʻa kaʻa ma muli o ka deactivation o nā mea i hana ʻia e nā loli kemika ma mua o ka hoʻokaʻawale catalyst.Eia kekahi, inā e hoʻokaʻawale ʻia ka nui o nā ʻāpana catalyst mai ka ʻili electrode, e hopena kēia i ka piʻi nui o ka hoʻokaʻawale kiʻekiʻe (ʻaʻole wale ʻo 44 mV), no ka mea, ʻaʻohe hana o ka substrate (UCC) no ka VO2 +/VO2+ redox reaction.
Hoʻohālikelike i ka CV o ka mea electrode maikaʻi loa i hoʻohālikelike ʻia me UCC (a) a me ka paʻa o ka VO2 +/VO2+ redox reaction (b).ν = 5 mV/s no nā CV a pau i 0.1 M VOSO4/1 M H2SO4 + 1 M HCl electrolyte.
No ka hoʻonui ʻana i ka hoihoi waiwai o ka ʻenehana VRFB, ʻo ka hoʻonui ʻana a me ka hoʻomaopopo ʻana i nā kinetics o ka vanadium redox reactions he mea nui ia e hoʻokō ai i ka ikehu kiʻekiʻe.Ua hoʻomākaukau ʻia nā hui HWO-C76 a ua aʻo ʻia kā lākou hopena electrocatalytic ma ka hopena VO2 +/VO2+.Ua hōʻike ʻo HWO i ka hoʻonui kinetic liʻiliʻi i loko o nā electrolytes acidic hui pū ʻia akā ua hoʻopaʻa nui ʻia ka hoʻomohala chlorine.Ua hoʻohana ʻia nā lakio like ʻole o HWO:C76 no ka hoʻonui ʻana i nā kinetics o nā electrodes-hoʻokumu HWO.ʻO ka hoʻonui ʻana i ka C76 i ka HWO e hoʻomaikaʻi i nā kinetics hoʻoili electron o ka hopena VO2+/VO2+ ma ka electrode i hoʻololi ʻia, ʻo ia ka HWO-50% C76 ka mea maikaʻi loa no ka mea e hōʻemi ana i ka pale ʻana i ka hoʻoili kālā a hoʻopaʻa hou i ka chlorine i hoʻohālikelike ʻia me ka waihona C76 a me TCC..Ma muli o ka hopena synergistic ma waena o C=C sp2 hybridization, OH a me W-OH hui hana.ʻO ka helu hoʻohaʻahaʻa ma hope o ka holo kaʻa ʻana o HWO-50% C76 i ʻike ʻia he 0.29 mV/pōkole, ʻoiai ʻo ka helu degradation o UCC a me TCC ʻo 0.33 mV/pōkole a me 0.49 mV/pōkole, paʻa loa.i loko o nā electrolytes ʻakika hui ʻia.ʻIke maikaʻi nā hopena i hōʻike ʻia i nā mea electrode hana kiʻekiʻe no ka hopena VO2+/VO2+ me nā kinetics wikiwiki a me ke kūpaʻa kiʻekiʻe.E hoʻonui kēia i ka volta puka, e hoʻonui ai i ka pono o ka ikehu o ka VRFB, no laila e hōʻemi ana i ke kumukūʻai o kāna kūʻai ʻana i ka wā e hiki mai ana.
Loaʻa nā ʻikepili i hoʻohana ʻia a/a i ʻike ʻia i ka noiʻi o kēia manawa mai nā mea kākau ma muli o ke noi kūpono.
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