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Nā te utu nui o ngā pākahiko redox rere-roto-katoa-vanadium (VRFB) ka whakawhāitihia te whakamahinga whānui. Me whakapai ake i te tere o ngā tauhohenga hiko hei whakanui ake i te mana motuhake me te whai huatanga pūngao o te VRFB, ā, ka whakaitihia te utu o te kWh o te VRFB. I roto i tēnei mahi, i whakatakotoria ngā matūriki nano o te waikura tungsten hydrated (HWO) i hangaia ki te wai wera, C76 me te C76/HWO, ki runga i ngā irahiko kakahu waro, ā, i whakamatautauria hei electrocatalysts mō te tauhohenga redox VO2+/VO2+. Ko te karu hiko matawai tukunga mara (FESEM), te ine hihi-X marara pūngao (EDX), te karu hiko tuku taumira teitei (HR-TEM), te diffraction hihi-X (XRD), te ine hihi-X photoelectron (XPS), te ine huringa Fourier infrared (FTIR) me ngā ine koki whakapā. Kua kitea ko te tāpiri o ngā fullerenes C76 ki te HWO ka taea te whakapai ake i te kaha o te hikohiko mā te whakanui ake i te kawe hiko me te whakarato i ngā rōpū mahi kua waikurahia ki runga i tōna mata, ā, mā reira ka whakatairanga i te tauhohenga redox VO2+/VO2+. Ko te hiato HWO/C76 (50 wt% C76) te mea pai rawa atu mō te tauhohenga VO2+/VO2+ me te ΔEp o te 176 mV, ko te kakahu waro kāore i rongoatia (UCC) he 365 mV. Hei tāpiri, i whakaatuhia e te hiato HWO/C76 he pānga aukati nui ki te tauhohenga whanaketanga chlorine pirinoa nā te rōpū mahi W-OH.
Nā te kaha o ngā mahi a te tangata me te tere o te hurihanga ahumahi kua hua ake te hiahia nui mō te hiko, e piki haere ana mā te 3% i ia tau1. Mō ngā tekau tau, ko te whakamahinga whānui o ngā wahie pūmua hei pūtake hiko kua hua ake ngā tukunga hau kati kōtuhi e whai wāhi ana ki te mahana o te ao, te parahanga wai me te hau, e whakawehi ana i ngā rauropi katoa. Nō reira, e matapaetia ana ka eke te urunga o te pūngao hau me te pūngao rā ma, hou, ki te 75% o te hiko katoa i te tau 20501. Heoi, ina neke atu te wāhi o te hiko mai i ngā pūtake hou ki te 20% o te whakaputanga hiko katoa, ka kore e pumau te whatunga hiko.
I roto i ngā pūnaha rokiroki pūngao katoa pērā i te pākahiko rere vanadium redox ranu2, ko te pākahiko rere vanadium redox katoa (VRFB) te mea tino tere te whanaketanga nā te maha o ngā painga, ā, e kiia ana ko te otinga pai rawa atu mō te rokiroki pūngao mō te wā roa (tata ki te 30 tau). ) Ngā kōwhiringa i te taha o te pūngao whakahou4. Nā te wehenga o te mana me te mātotoru o te pūngao, te urupare tere, te roa o te ora ratonga, me te utu iti ā-tau o te $65/kWh, ki te whakaritea ki te $93-140/kWh mō ngā pākahiko Li-ion me te waikawa-mata me te 279-420 tāra US mō ia kWh. pākahiko ia 4.
Heoi, kei te herea tonutia tā rātou hokohoko nui e ngā utu whakapaipai pūnaha teitei, ko te nuinga nā ngā puranga pūtau4,5. Nō reira, mā te whakapai ake i te mahi puranga mā te whakanui ake i te tere o ngā tauhohenga haurua-huānga e rua ka taea te whakaiti i te rahi o te puranga, ā, ka whakaiti i te utu. Nō reira, me tere te whakawhiti irahiko ki te mata o te irahiko, e whakawhirinaki ana ki te hoahoa, te hanganga me te hanganga o te irahiko, ā, me arotau āta6. Ahakoa te pumau matū me te hikohiko pai me te kawe hiko pai o ngā irahiko waro, he puhoi te tere o ā rātou mahi kāore i rongoatia nā te kore o ngā rōpū mahi hāora me te hydrophilicity7,8. Nō reira, ka whakakotahihia ngā momo electrocatalysts me ngā irahiko waro-hanga, inā koa ngā hanganga nano waro me ngā waikura whakarewa, hei whakapai ake i te tere o ngā irahiko e rua, ā, ka whakanui ake i te tere o te irahiko VRFB.
Haunga ā mātou mahi o mua mō te C76, i tuatahitia e mātou te pūrongo mō te mahi hiko whakakorikori pai rawa atu o tēnei fullerene mō te VO2+/VO2+, te whakawhiti utu, ki te whakataurite ki te kakahu waro i whakamahanatia me te kore i rongoatia. Ka whakaitihia te ātete mā te 99.5% me te 97%. Ko te mahi whakakorikori o ngā rauemi waro mō te tauhohenga VO2+/VO2+ ki te whakataurite ki te C76 e whakaaturia ana i te Ripanga S1. I tētahi atu taha, he maha ngā waikura whakarewa pērā i te CeO225, ZrO226, MoO327, NiO28, SnO229, Cr2O330 me te WO331, 32, 33, 34, 35, 36, 37 kua whakamahia nā te mea he nui ake te makuku me te nui o te mahi hāora. , 38. rōpū. Ko te mahi whakakorikori o ēnei waikura whakarewa i roto i te tauhohenga VO2+/VO2+ e whakaaturia ana i te Ripanga S2. Kua whakamahia te WO3 i roto i te maha o ngā mahi nā te iti o te utu, te pumau nui i roto i ngā pāpāho waikawa, me te kaha whakaterenga teitei31,32,33,34,35,36,37,38. Heoi, kāore i te nui te whakapainga o te kinetics cathodic nā te WO3. Hei whakapai ake i te kawe hiko o te WO3, i whakamatautauria te pānga o te whakamahi i te waikura tungsten whakaitihia (W18O49) ki te mahi cathodic38. Kāore anō kia whakamatautauria te waikura tungsten hydrated (HWO) i roto i ngā tono VRFB, ahakoa he nui ake te mahi i roto i ngā tono supercapacitor nā te tere o te horapa cation ki te whakataurite ki te WOx39,40 anhydrous. Ka whakamahia e te pākahiko rere vanadium redox tuatoru o te whakatupuranga he electrolyte waikawa whakauru i hangaia mai i te HCl me te H2SO4 hei whakapai ake i te mahi pākahiko me te whakapai ake i te wairewa me te pumau o ngā katote vanadium i roto i te electrolyte. Heoi, kua noho te tauhohenga whanaketanga chlorine parasitic hei tetahi o ngā ngoikoretanga o te tuatoru o ngā whakatupuranga, nō reira ko te rapu huarahi hei aukati i te tauhohenga aromatawai chlorine kua waiho hei arotahi a ētahi rōpū rangahau.
I konei, i whakahaerehia ngā whakamātautau tauhohenga VO2+/VO2+ ki ngā hiato HWO/C76 i whakatakotoria ki runga i ngā irahiko kakahu waro hei kimi i te taurite i waenga i te kawe hiko o ngā hiato me te kinetics redox o te mata irahiko me te pehi i te whanaketanga o te chlorine pirinoa. urupare (CER). I hangaia ngā matūriki nano o te waikura tungsten hydrated (HWO) mā te tikanga hydrothermal ngāwari. I whakahaerehia ngā whakamātautau i roto i te electrolyte waikawa whakauru (H2SO4/HCl) hei whakatauira i te VRFB tuatoru o ngā whakatupuranga (G3) mō te whaihua me te tirotiro i te pānga o te HWO ki te tauhohenga whanaketanga chlorine pirinoa.
I whakamahia i roto i tēnei rangahau te vanadium(IV) sulfate hydrate (VOSO4, 99.9%, Alfa-Aeser), te waikawa whanariki (H2SO4), te waikawa hauwaiora (HCl), te dimethylformamide (DMF, Sigma-Aldrich), te polyvinylidene fluoride (PVDF, Sigma)-Aldrich), te konutai Tungsten oxide dihydrate (Na2WO4, 99%, Sigma-Aldrich) me te kakahu waro hydrophilic ELAT (Fuel Cell Store).
I whakaritea te waikura tungsten whakamakuku (HWO) mā te tauhohenga waiariki 43, i whakarewaina ai te 2 karamu o te tote Na2WO4 ki roto i te 12 ml o te H2O kia puta he wai kore tae, kātahi ka tāpirihia he 12 ml o te 2 M HCl kia puta he wairewa kōwhai mā. I whakanohoia te paraoa ki roto i te autoclave maitai kore waikura kua pania ki te Teflon, ā, i puritia ki roto i te oumu i te 180° C mō ngā hāora e 3 mō te tauhohenga waiariki. I kohia te toenga mā te tātari, i horoia kia 3 ngā wā ki te etanoru me te wai, i whakamaroketia ki roto i te oumu i te 70°C mō ngā hāora e ~3, kātahi ka whakatōtō kia puta he paura HWO kikorangi-hina.
Ko ngā irahiko kakahu waro (CCT) i whiwhi (kāore i rongoatia) i whakamahia i roto i te oumu ngongo i te 450°C i te hau me te tere whakamahana o te 15 ºC/min mō ngā haora 10 hei whiwhi i ngā CC kua rongoatia (TCC). e ai ki te tuhinga o mua24. I tapahia te UCC me te TCC ki ngā irahiko tata ki te 1.5 cm te whānui me te 7 cm te roa. I whakaritea ngā whakatārewatanga o C76, HWO, HWO-10% C76, HWO-30% C76 me te HWO-50% C76 mā te tāpiri i te 20 mg .% (~2.22 mg) o te here PVDF ki te ~1 ml DMF, ā, i sonicated mō te haora 1 hei whakapai ake i te ōritetanga. I pania te 2 mg o ngā mea honohono C76, HWO me te HWO-C76 ki te rohe irahiko hohe UCC tata ki te 1.5 cm2. I utaina ngā whakakorikori katoa ki runga i ngā irahiko UCC, ā, i whakamahia te TCC hei whakatairite anake, i te mea i whakaatuhia e tā mātou mahi o mua kāore i hiahiatia te maimoatanga wera24. I tutuki te whakataunga o te tānga mā te paraihe i te 100 µl o te whakatārewatanga (kawenga 2 mg) kia ōrite ake te pānga. Kātahi ka whakamarokehia ngā irahiko katoa i roto i te oumu i te 60° C. i te pō. Ka inehia ngā irahiko ki mua, ki muri hoki kia tika ai te utaina o ngā taonga. Kia whai horahanga āhuahanga (~1.5 cm2) me te ārai i te pikinga o te irahiko vanadium ki te irahiko nā te pānga o te capillary, i pania he paparanga angiangi o te paraffin ki runga i te rauemi hohe.
I whakamahia te karu hiko matawai tukunga mara (FESEM, Zeiss SEM Ultra 60, 5 kV) hei tirotiro i te āhua o te mata o te HWO. I whakamahia he ine hihi-X marara pūngao kua rite ki te Feii8SEM (EDX, Zeiss Inc.) hei mahere i ngā huānga HWO-50%C76 ki runga i ngā irahiko UCC. I whakamahia he karu hiko tuku taumira teitei (HR-TEM, JOEL JEM-2100) e mahi ana i te ngaohiko tere o te 200 kV hei whakaahua i ngā matūriki HWO taumira teitei ake me ngā mowhiti diffraction. Ka whakamahia e te pūmanawa Crystallography Toolbox (CrysTBox) te mahi ringGUI hei tātari i te tauira diffraction mowhiti HWO me te whakatairite i ngā hua ki te tauira XRD. I tātarihia te hanganga me te whakakāwhata o te UCC me te TCC mā te whakamahi i te X-ray diffraction (XRD) i te tere matawai o te 2.4°/min mai i te 5° ki te 70° me te Cu Kα (λ = 1.54060 Å) mā te whakamahi i te Panalytical X-ray diffractometer (Tauira 3600). I whakaatuhia e te XRD te hanganga tioata me te āhua o te HWO. I whakamahia te pūmanawa PANalytical X'Pert HighScore hei whakataurite i ngā tihi HWO ki ngā mahere waikura tungsten e wātea ana i roto i te pātengi raraunga45. I whakaritea ngā hua HWO ki ngā hua TEM. I whakatauhia te hanganga matū me te āhua o ngā tauira HWO mā te X-ray photoelectron spectroscopy (XPS, ESCALAB 250Xi, ThermoScientific). I whakamahia te pūmanawa CASA-XPS (v 2.3.15) mō te wetewete tihi me te tātari raraunga. Hei whakatau i ngā rōpū mahi mata o HWO me HWO-50%C76, i mahia ngā inenga mā te whakamahi i te Fourier transform infrared spectroscopy (FTIR, Perkin Elmer spectrometer, mā te whakamahi i te KBr FTIR). I whakaritea ngā hua ki ngā hua XPS. I whakamahia hoki ngā inenga koki whakapā (KRUSS DSA25) hei whakaahua i te āheinga makuku o ngā irahiko.
Mō ngā inenga hikohiko katoa, i whakamahia he teihana mahi Biologic SP 300. I whakamahia te cyclic voltammetry (CV) me te electrochemical impedance spectroscopy (EIS) hei ako i te kinetics hikohiko o te tauhohenga redox VO2+/VO2+ me te pānga o te horapa reagent (VOSO4(VO2+)) ki te tere tauhohenga. I whakamahia e ngā tikanga e rua he pūtau hiko-toru me te kukū electrolyte o te 0.1 M VOSO4 (V4+) i roto i te 1 M H2SO4 + 1 M HCl (ranunga waikawa). Ko ngā raraunga hikohiko katoa i whakaaturia he mea whakatika IR. I whakamahia he hikohiko calomel kua kōtuitia (SCE) me te koiri platinum (Pt) hei hikohiko tohutoro me te hikohiko taupatupatu. Mō CV, i whakamahia ngā reiti matawai (ν) o te 5, 20, me te 50 mV/s ki te matapihi pūmanawa VO2+/VO2+ mō (0–1) V vs. SCE, kātahi ka whakatikatikaina kia tuhia e SHE (VSCE = 0.242 V vs. HSE). Hei ako i te pupuri i te ngohe o te irahiko, i whakahaerehia ngā CV hurihuri i te ν 5 mV/s mō te UCC, TCC, UCC-C76, UCC-HWO, me te UCC-HWO-50% C76. Mō ngā inenga EIS, ko te whānuitanga auau o te tauhohenga redox VO2+/VO2+ he 0.01-105 Hz, ā, ko te whakararuraru ngaohiko i te ngaohiko ara iahiko tuwhera (OCV) he 10 mV. I tuaruatia ia whakamātautau e 2-3 ngā wā hei whakarite i te ōritetanga o ngā hua. I whiwhihia ngā pūmau tere rerekē (k0) mā te tikanga Nicholson46,47.
Kua angitu te hanga o te waikura tungsten whakamakuku (HVO) mā te tikanga hydrothermal. E whakaatu ana te ahua SEM i te pikitia 1a ko te HWO kua whakatakotoria he tautau o ngā matūriki nano me te rahi kei roto i te awhe 25-50 nm.
E whakaatu ana te tauira whakarara hihi-X o HWO i ngā tihi (001) me te (002) i te ~23.5° me te ~47.5°, ia, he āhuatanga ēnei o te WO2.63 kore-stoichiometric (W32O84) (PDF 077–0810, a = 21.4 Å, b = 17.8 Å, c = 3.8 Å, α = β = γ = 90°), e rite ana ki tō rātou tae kikorangi mārama (Pikitia 1b) 48.49. Ko ētahi atu tihi i te 20.5°, 27.1°, 28.1°, 30.8°, 35.7°, 36.7° me te 52.7° i tohaina ki (140), (620), (350), (720), (740), (560°). ) ) me (970) ngā papa whakarara e hangai ana ki te WO2.63, ia. I whakamahia te tikanga hanga kotahi e Songara et al. 43 hei tiki i tētahi hua mā, i kīia nā te aroaro o te WO3(H2O)0.333. Heoi, i roto i tēnei mahi, nā ngā āhuatanga rerekē, i whiwhihia he hua kikorangi-hina, e tohu ana ko te WO3(H2O)0.333 (PDF 087-1203, a = 7.3 Å, b = 12.5 Å, c = 7 .7 Å, α = β = γ = 90°) me te āhua whakaiti o te waikura tungsten. I whakaatuhia e te tātari haurua-taurangi mā te whakamahi i te pūmanawa X'Pert HighScore he 26% WO3(H2O)0.333:74% W32O84. I te mea ko W6+ me W4+ te wāhanga o W32O84 (1.67:1 W6+:W4+), ko te nui o te ihirangi o W6+ me W4+ e ai ki te whakatau tata ko te 72% o W6+ me te 28% o W4+. I whakaaturia ngā whakaahua SEM, ngā hihi XPS 1-hēkona i te taumata karihi, ngā whakaahua TEM, ngā hihi FTIR, me ngā hihi Raman o ngā matūriki C76 i roto i tā mātou tuhinga o mua. E ai ki a Kawada et al.,50,51 i whakaatuhia te hanganga monoclinic o te FCC i muri i te tangohanga o te toluene.
E whakaatu ana ngā whakaahua SEM i te pikitia 2a me te pikitia b i te whakatakotoranga angitu o te HWO me te HWO-50%C76 ki runga, ki waenganui hoki i ngā muka waro o te irahiko UCC. Kei te whakaatuhia ngā mahere huānga EDX o te tungsten, te waro, me te hāora i runga i ngā whakaahua SEM i te pikitia 2c i te pikitia 2d-f e tohu ana kua ōrite te ranunga o te tungsten me te waro (e whakaatu ana i te tohatoha ōrite) ki runga i te mata irahiko katoa, ā, kāore te rauemi whakakotahi i te whakatakotoranga ōrite nā te āhua o te tikanga whakatakotoranga.
Ko ngā whakaahua SEM o ngā matūriki HWO kua whakatakotoria (a) me ngā matūriki HWO-C76 (b). Ko te mahere EDX i runga i te HWO-C76 kua utaina ki runga i te UCC mā te whakamahi i te horahanga i te ahua (c) e whakaatu ana i te tohatoha o te tungsten (d), te waro (e), me te hāora (f) i roto i te tauira.
I whakamahia te HR-TEM mō te whakaahua whakanui teitei me ngā mōhiohio karaihe (Pikitia 3). E whakaatu ana te HWO i te āhua o te nanocube e whakaaturia ana i te Pikitia 3a, ā, he mārama ake i te Pikitia 3b. Mā te whakanui i te nanocube mō te diffraction o ngā wāhi kua tohua, ka taea te tiro i te hanganga kupenga me ngā papa diffraction e tutuki ana i te ture Bragg, e whakaaturia ana i te Pikitia 3c, e whakaū ana i te tioata o te rauemi. I roto i te whakaurunga ki te Pikitia 3c e whakaatu ana i te tawhiti d 3.3 Å e rite ana ki ngā papa diffraction (022) me te (620) i kitea i roto i ngā wāhanga WO3(H2O)0.333 me te W32O84, ia,43,44,49. He rite tēnei ki te tātari XRD i whakaahuahia i runga ake nei (Pikitia 1b) mai i te mea ko te tawhiti papa kupenga i kitea d (Pikitia 3c) e rite ana ki te tihi XRD kaha rawa atu i roto i te tauira HWO. E whakaaturia ana hoki ngā mowhiti tauira i te pikitia 3d, kei reira ia mowhiti e rite ana ki tētahi papa motuhake. He mā, he kikorangi hoki ngā tae o ngā papa WO3(H2O)0.333 me W32O84, ā, e whakaaturia ana hoki ō rātou tihi XRD e rite ana ki te Pikitia 1b. Ko te mowhiti tuatahi e whakaaturia ana i te hoahoa mowhiti e rite ana ki te tihi tuatahi kua tohua i roto i te tauira hihi-x o te papa diffraction (022) (620 rānei). Mai i ngā mowhiti (022) ki (402), ko ngā uara mokowā-d ko 3.30, 3.17, 2.38, 1.93, me te 1.69 Å, e rite ana ki ngā uara XRD o 3.30, 3.17, 2, 45, 1.93. me te 1.66 Å, e ōrite ana ki te 44, 45, ia.
(a) Ko te ahua HR-TEM o HWO, (b) e whakaatu ana i tētahi ahua kua whakanuia. Kei te whakaaturia ngā whakaahua o ngā papa whatu i roto i (c), ko te whakaurunga (c) e whakaatu ana i tētahi ahua kua whakanuia o ngā papa me te piko d o te 0.33 nm e rite ana ki ngā papa (002) me (620). (d) Ko te tauira mowhiti HWO e whakaatu ana i ngā papa e hono ana ki te WO3(H2O)0.333 (mā) me te W32O84 (kikorangi).
I whakahaerehia te tātaritanga XPS hei whakatau i te matū o te mata me te āhua waikura o te tungsten (Ngā Pikitia S1 me te 4). Ko te whānuitanga whānui o te matawai XPS o te HWO i hangaia ka whakaaturia i te Pikitia S1, e tohu ana i te aroaro o te tungsten. Ko ngā matawai whaiti XPS o ngā taumata matua W 4f me O 1s ka whakaaturia i ngā Pikitia 4a me b, ia. Ka wehea te matawai W 4f kia rua ngā takirua hurihuri-āmiomio e rite ana ki ngā kaha here o te āhua waikura W. me te W 4f7/2 i te 36.6 me te 34.9 eV he āhuatanga o te āhua W4+ o te 40, ia. )0.333. E whakaatu ana ngā raraunga kua taurite ko ngā ōrau ngota o W6+ me W4+ he 85% me te 15%, ia, e tata ana ki ngā uara i whakatauhia mai i ngā raraunga XRD i runga i ngā rerekētanga i waenga i ngā tikanga e rua. Ka whakaratohia e ngā tikanga e rua ngā mōhiohio tauanga me te iti o te tika, inā koa ko te XRD. Waihoki, ka tātarihia e ēnei tikanga e rua ngā wāhanga rerekē o te rauemi nā te mea he tikanga papatipu te XRD, ko te XPS ia he tikanga mata e tata ana ki ētahi nanometer anake. Kua wehea te whānuitanga O 1s kia rua ngā tihi i te 533 (22.2%) me te 530.4 eV (77.8%). Ko te tuatahi e rite ana ki te OH, ā, ko te tuarua ki ngā here hāora i roto i te whatunga i roto i te WO. Ko te noho o ngā rōpū mahi OH e rite ana ki ngā āhuatanga waikura o te HWO.
I whakahaerehia hoki he tātaritanga FTIR ki ēnei tauira e rua hei tirotiro i te aroaro o ngā rōpū mahi me ngā ngota wai taunga i roto i te hanganga HWO waikura. E whakaatu ana ngā hua he rite te āhua o te tauira HWO-50% C76 me ngā hua FT-IR HWO nā te aroaro o te HWO, engari he rerekē te kaha o ngā tihi nā te rerekētanga o te nui o te tauira i whakamahia hei whakarite mō te tātari (Pikitia 5a). E whakaatu ana te HWO-50% C76 ko ngā tihi katoa, engari ko te tihi o te waikura tungsten, e pā ana ki te fullerene 24. E whakaatuhia ana i roto i te pikitia 5a e whakaatu ana ko ngā tauira e rua e whakaatu ana i tētahi roopu whānui tino kaha i te ~710/cm e pā ana ki ngā wiri totoro OWO i roto i te hanganga whatunga HWO, me te pakihiwi kaha i te ~840/cm e pā ana ki te WO. Mō ngā wiri totoro, ko tētahi roopu koi i te 1610/cm e pā ana ki ngā wiri piko o te OH, ko tētahi roopu mimiti whānui i te 3400/cm e pā ana ki ngā wiri totoro o te OH i roto i ngā rōpū hydroxyl43. He rite tonu ēnei hua ki ngā hihi XPS i ngā Pikitia 4b, kei reira ngā rōpū mahi WO ka taea te whakarato i ngā pae hohe mō te tauhohenga VO2+/VO2+.
Tātaritanga FTIR o HWO me HWO-50% C76 (a), i tohua ngā rōpū mahi me ngā inenga koki whakapā (b, c).
Ka taea hoki e te rōpū OH te whakakorikori i te tauhohenga VO2+/VO2+, me te whakanui ake i te hydrophilicity o te irahiko, ā, ka whakatairanga i te tere o te horapa me te whakawhiti irahiko. E ai ki te whakaaturanga, e whakaatu ana te tauira HWO-50% C76 i tētahi atu tihi mō C76. Ka taea te tohu i ngā tihi i te ~2905, 2375, 1705, 1607, me te 1445 cm3 ki ngā wiri totoro CH, O=C=O, C=O, C=C, me te CO. E mōhiotia whānuitia ana ka taea e ngā rōpū mahi hāora C=O me te CO te mahi hei pokapū hohe mō ngā tauhohenga redox o te vanadium. Hei whakamātautau me te whakatairite i te makuku o ngā irahiko e rua, i tangohia ngā inenga koki whakapā e ai ki te whakaaturanga i te Pikitia 5b,c. I mimiti tonu te irahiko HWO i ngā pata wai, e tohu ana i te superhydrphilicity nā ngā rōpū mahi OH e wātea ana. He hydrophobic ake te HWO-50% C76, me te koki whakapā tata ki te 135° i muri i te 10 hēkona. Heoi, i roto i ngā inenga hikohiko, kua mākū katoa te hikohiko HWO-50%C76 i roto i te iti iho i te meneti. He rite tonu ngā inenga mākū ki ngā hua XPS me te FTIR, e tohu ana ko te nui ake o ngā rōpū OH i runga i te mata HWO ka nui ake te pai ki te wai.
I whakamatautauria ngā tauhohenga VO2+/VO2+ o ngā nanocomposites HWO me HWO-C76, ā, i whakaarohia ka pehia e te HWO te whanaketanga o te chlorine i roto i te tauhohenga VO2+/VO2+ i roto i te waikawa whakauru, ā, ka whakakorikori ake a C76 i te tauhohenga redox VO2+/VO2+ e hiahiatia ana. %, 30%, me te 50% C76 i roto i ngā whakatārewatanga HWO me te CCC i whakatakotoria ki runga i ngā irahiko me te uta katoa o te 2 mg/cm2.
E ai ki te pikitia 6, i tirohia te tere o te tauhohenga VO2+/VO2+ i runga i te mata o te irahiko mā te CV i roto i te irahiko waikawa whakauru. Ka whakaaturia ngā iahiko hei I/Ipa hei whakataurite ngāwari i te ΔEp me te Ipa/Ipc mō ngā whakakorikori rerekē i runga tonu i te kauwhata. Ka whakaaturia ngā raraunga waeine horahanga o nāianei i te Pikitia 2S. I runga i te pikitia 6a, e whakaatu ana te Pikitia 6a ka paku whakanuia e te HWO te tere whakawhiti irahiko o te tauhohenga redox VO2+/VO2+ i runga i te mata o te irahiko, ā, ka pehi i te tauhohenga o te whanaketanga o te hauota pirinoa. Heoi, ka tino whakanuia e te C76 te tere whakawhiti irahiko, ā, ka whakakorikori i te tauhohenga whanaketanga o te hauota. Nō reira, e tumanakohia ana ko te whakakotahitanga tika o te HWO me te C76 te mea pai rawa atu te mahi me te kaha nui rawa atu ki te aukati i te tauhohenga whanaketanga o te hauota. I kitea i muri i te whakanui ake i te ihirangi o te C76, ka pai ake te mahi hikohiko o ngā irahiko, e whakaatuhia ana e te hekenga o te ΔEp me te pikinga o te ōwehenga Ipa/Ipc (Ripanga S3). I whakaūtia anō hoki tēnei e ngā uara RCT i tangohia mai i te kauwhata Nyquist i te Pikitia 6d (Ripanga S3), i kitea he heke iho i te pikinga ake o te ihirangi C76. He rite anō hoki ēnei hua ki te rangahau a Li, i reira ko te tāpiri o te waro mesoporous ki te WO3 mesoporous i whakaatu i te pai ake o te nekehanga whakawhiti utu i runga i te VO2+/VO2+35. E tohu ana tēnei ko te tauhohenga tika ka whakawhirinaki pea ki te kawe hiko (here C=C) 18, 24, 35, 36, 37. Tērā pea nā te huringa o te āhua taunga i waenga i te [VO(H2O)5]2+ me te [VO2(H2O)4]+ tēnei, ka whakaitihia e te C76 te ngaohiko tauhohenga mā te whakaiti i te kaha kiko. Heoi, kāore pea tēnei e taea me ngā hiko HWO.
(a) Te whanonga ine pūngao huringa (ν = 5 mV/s) o te tauhohenga VO2+/VO2+ o ngā hiato UCC me HWO-C76 me ngā ōwehenga HWO:C76 rerekē i roto i te 0.1 M VOSO4/1 M H2SO4 + 1 M electrolyte HCl. (b) Randles-Sevchik me (c) te tikanga VO2+/VO2+ a Nicholson hei aromatawai i te whai huatanga o te horapa me te whiwhi uara k0(d).
Ehara i te mea ko te HWO-50% C76 anake te mea i whakaatu i te mahi hiko-whakakorikori rite tonu ki a C76 mō te tauhohenga VO2+/VO2+, engari, he mea whakamīharo ake, i pehi anō hoki i te whanaketanga o te chlorine ki te C76, e whakaaturia ana i te Pikitia 6a, ā, e whakaatu ana hoki i te Hauwhā Porowhita Iti ake i te pikitia 6d (RCT raro). I whakaatu a C76 i te Ipa/Ipc kitea teitei ake i te HWO-50% C76 (Ripanga S3), ehara i te mea nā te pai ake o te whakahokinga o te tauhohenga, engari nā te taupatupatu tihi o te tauhohenga whakaiti chlorine me te SHE i te 1.2 V. Ko te mahi pai rawa atu o te HWO- Ko te 50% C76 e pā ana ki te pānga mahi tahi i waenga i te C76 tino kawe hiko kino me te kaha whakamakuku me te mahi whakaterenga W-OH i runga i te HWO. Mā te iti o te tukunga chlorine ka whakapai ake i te whai huatanga utu o te pūtau katoa, ko te pai ake o te kinetics ka whakapai ake i te whai huatanga o te ngaohiko pūtau katoa.
E ai ki te whārite S1, mō te tauhohenga āhua-hurihuri (whakawhiti irahiko puhoi) e whakahaerehia ana e te horapa, ko te iahiko tihi (IP) e whakawhirinaki ana ki te maha o ngā irahiko (n), te horahanga irahiko (A), te tauwehenga horapa (D), te tauwehenga whakawhiti irahiko (α) me te tere matawai (ν). Hei ako i te whanonga horapa o ngā rauemi kua whakamatautauria, i tuhia te whanaungatanga i waenga i te IP me te ν1/2, ā, i whakaaturia ki te Pikitia 6b. Nā te mea he whanaungatanga rārangi ngā rauemi katoa, ka whakahaerehia te tauhohenga e te horapa. Nā te mea he āhua-hurihuri te tauhohenga VO2+/VO2+, ko te pari o te rārangi e whakawhirinaki ana ki te tauwehenga horapa me te uara o te α (whārite S1). Nā te mea he pumau te tauwehenga horapa (≈ 4 × 10–6 cm2/s)52, ko te rerekētanga o te pari o te rārangi e tohu tika ana i ngā uara rerekē o te α, nō reira ko te tere whakawhiti irahiko i runga i te mata irahiko, e whakaaturia ana mō C76 me HWO -50% C76 Pari pari teitei (tere whakawhiti irahiko teitei rawa).
Ko ngā pari Warburg (W) i tatauhia mō ngā auau iti e whakaaturia ana i te Ripanga S3 (Pikitia 6d) he tata ki te 1 ngā uara mō ngā rauemi katoa, e tohu ana i te horapa tino pai o ngā momo redox me te whakaū i te whanonga raina o IP ki te whakataurite ki te ν1/2. Ka inehia te CV. Mō te HWO-50% C76, ka rerekē te pari Warburg mai i te 1 ki te 1.32, e tohu ana ehara i te mea ko te horapa mutunga kore o te matū (VO2+), engari ko te takoha pea o te whanonga paparanga angiangi ki te whanonga horapa nā te porosity o te hiko.
Hei tātari atu i te āheinga hurihuri (tere whakawhiti irahiko) o te tauhohenga redox VO2+/VO2+, i whakamahia hoki te tikanga tauhohenga hurihuri-āhua a Nicholson hei whakatau i te pūmau tere paerewa k041.42. Ka mahia tēnei mā te whakamahi i te whārite S2 hei hanga i te tawhā nekeneke kore-ahu Ψ, he mahi a ΔEp, hei mahi a ν-1/2. E whakaatu ana te Ripanga S4 i ngā uara Ψ i whiwhi mō ia rauemi irahiko. I tuhia ngā hua (Pikitia 6c) hei whiwhi k0 × 104 cm/s mai i te pari o ia kauwhata mā te whakamahi i te Whārite S3 (i tuhia ki te taha o ia rarangi, ā, kei te whakaatuhia i roto i te Ripanga S4). I kitea ko te HWO-50% C76 te pari teitei rawa (Pikitia 6c), nō reira ko te uara mōrahi o k0 he 2.47 × 10–4 cm/s. Ko te tikanga o tēnei ko tēnei irahiko te mea e tere rawa ana te nekeneke, e rite ana ki ngā hua CV me EIS i roto i te Pikitia 6a me te d me te Ripanga S3. Hei tāpiritanga, i whiwhihia hoki te uara o te k0 mai i te kauwhata Nyquist (Pikitia 6d) o te Whārite S4 mā te whakamahi i te uara RCT (Ripanga S3). Kua whakarāpopototia ēnei hua k0 mai i te EIS ki te Ripanga S4, ā, e whakaatu ana hoki ko te HWO-50% C76 te mea e whakaatu ana i te tere whakawhiti irahiko teitei rawa atu nā te pānga mahi tahi. Ahakoa he rerekē ngā uara k0 nā te rerekētanga o ngā takenga mai o ia tikanga, e whakaatu tonu ana i te raupapa ōrite o te rahi, ā, e whakaatu ana i te ōritetanga.
Hei mārama rawa atu ki ngā mahi tino pai i whiwhihia, he mea nui kia whakatauritea ngā rauemi hiko tino pai ki ngā hiko UCC me ngā hiko TCC kāore i pania. Mō te tauhohenga VO2+/VO2+, kāore i te whakaatu noa a HWO-C76 i te ΔEp iti rawa me te pai ake o te whakahokinga, engari i tino pehi hoki i te tauhohenga whanaketanga haukini pirinoa ki te TCC, i inehia e te iahiko i te 1.45 V e pā ana ki te SHE (Pikitia 7a). Mō te pumau, i whakaaro mātou he pumau te HWO-50% C76 nā te mea i konatunatua te whakakorikori ki te here PVDF, kātahi ka whakamahia ki ngā hiko kakahu waro. I whakaatu a HWO-50% C76 i te nekehanga tihi o te 44 mV (tere pirau 0.29 mV/huringa) i muri i te 150 huringa ki te 50 mV mō te UCC (Pikitia 7b). Kāore pea tēnei i te rerekētanga nui, engari he tino puhoi te mahi o ngā hiko UCC, ā, ka heke i te huringa, inā koa mō ngā tauhohenga whakamuri. Ahakoa he pai ake te kaha whakahurihuri o te TCC i tō te UCC, i kitea he nui te nekehanga tihi o te TCC, arā, 73 mV i muri i te 150 huringa, tērā pea nā te nui o te chlorine i hangaia ki tōna mata. kia piri pai ai te whakakorikori ki te mata o te irahiko. E kitea ana i ngā irahiko katoa i whakamatautauria, ahakoa ngā irahiko kāore he whakakorikori tautokona i whakaatu i ngā taumata rerekē o te kore pumau o te huringa, e kī ana ko te huringa o te wehenga tihi i te wā o te huringa nā te whakakorenga o te rauemi i puta mai i ngā huringa matū kaua i te wehenga whakakorikori. Hei tāpiri, ki te wehea he nui ngā matūriki whakakorikori mai i te mata o te irahiko, ka hua ake he pikinga nui o te wehenga tihi (ehara i te 44 mV anake), nā te mea he iti te hohenga o te papa (UCC) mō te tauhohenga redox VO2+/VO2+.
Te whakataurite i te CV o te rauemi hiko pai rawa atu ki te UCC (a) me te pumau o te tauhohenga redox VO2+/VO2+ (b). ν = 5 mV/s mō ngā CV katoa i roto i te 0.1 M VOSO4/1 M H2SO4 + 1 M HCl electrolyte.
Hei whakanui ake i te ātaahua ōhanga o te hangarau VRFB, he mea nui te whakawhānui me te mārama ki te tere o ngā tauhohenga redox vanadium kia eke ki te pai o te pūngao. I whakaritea ngā matū HWO-C76, ā, i rangahauhia tō rātou pānga hiko-whakakorikori ki te tauhohenga VO2+/VO2+. He iti noa te whakanui ake o te tere o te HWO i roto i ngā electrolytes waikawa whakauru engari i tino pehi i te whanaketanga o te chlorine. I whakamahia ngā ōwehenga rerekē o te HWO:C76 hei whakapai ake i te tere o ngā electrodes e hangai ana ki te HWO. Mā te whakanui ake i te C76 ki te HWO ka whakapai ake i te tere o te whakawhiti irahiko o te tauhohenga VO2+/VO2+ i runga i te electrode kua whakarerekētia, ko te HWO-50% C76 te rauemi pai rawa atu nā te mea ka whakaitihia te ātete whakawhiti utu, ā, ka pehi anō i te chlorine ki te whakataurite ki te C76 me te putunga TCC. . Nā te pānga tahi i waenga i te whakaranu C=C sp2, ngā rōpū mahi OH me W-OH tēnei. I kitea ko te tere o te pirau i muri i te huringa auau o te HWO-50% C76 he 0.29 mV/huringa, ko te tere pirau o te UCC me te TCC he 0.33 mV/huringa me te 0.49 mV/huringa, ia, he tino pumau i roto i ngā irahiko waikawa whakauru. Nā ngā hua i whakaatuhia i angitu te tautuhi i ngā rauemi irahiko mahi teitei mō te tauhohenga VO2+/VO2+ me te tere o te nekeneke me te pumau teitei. Mā tēnei ka piki ake te ngaohiko putanga, ka piki ake te whai huatanga o te pūngao o te VRFB, ka whakaitihia te utu o tōna hokohoko ā muri ake nei.
Kei te wātea mai ngā huinga raraunga i whakamahia, i tātarihia rānei i roto i te rangahau o nāianei i ngā kaituhi e pā ana ki te tono tika.
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