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Kua whakamahia whānuitia te whakakorenga hapa hei whakapai ake i te mahi a ngā pūtau hiko pūngao perovskite mata triiodide, engari kāore anō kia mārama te pānga o ngā hapa maha ki te pumau o te wāhanga-α; I konei, mā te whakamahi i te ariā mahi kiato, ka tautuhia e mātou mō te wā tuatahi te ara whakahekenga o te formamidine lead triiodide perovskite mai i te wāhanga-α ki te wāhanga-δ, ā, ka akohia te pānga o ngā hapa maha ki te arai pūngao whakawhiti wāhanga. E tohu ana ngā hua whakatauira ko ngā korenga iodine te mea pea ka puta te whakahekenga nā te mea ka tino whakaitihia e rātou te arai pūngao mō te whakawhiti wāhanga α-δ, ā, ko rātou te iti rawa o te pūngao hanganga i te mata perovskite. Ko te whakaurunga o tētahi paparanga matotoru o te oxalate mata kore-rewa ki runga i te mata perovskite ka tino aukati i te pirau o te wāhanga-α, ka ārai i te hekenga me te whakakorikori o te iodine. Hei tāpiri, ka tino whakaitihia e tēnei rautaki te whakakotahitanga kore-ira i te taha mata, ā, ka whakanuia te pai o te pūtau hiko pūngao ki te 25.39% (kua whakamanahia 24.92%). Ka taea tonu e te taputapu kāore i te tangohia he kākahu te pupuri i tōna pai o te 92% i muri i te whakamahi i te mana mōrahi mō ngā hāora 550 i raro i te whakaata i te papatipu hau 1.5 karamu.
Kua eke te pai o te hurihanga hiko (PCE) o ngā pūtau rā perovskite (PSC) ki te taumata teitei kua whakamanahia, arā, 26%. Mai i te tau 2015, kua pai ake ngā PSC hou ki te formamidine triiodide perovskite (FAPbI3) hei paparanga mimiti mārama nā te mea he pai te pumau o te wera me te āputa pai e tata ana ki te rohe Shockley-Keisser o te 2,3,4. Engari, ka pāngia ngā kiriata FAPbI3 e te whakawhiti āhua mai i te āhua α mangu ki te āhua δ kore-perovskite kōwhai i te pāmahana rūma5,6. Hei ārai i te hanganga o te āhua delta, kua whakawhanakehia ngā hanganga perovskite matatini. Ko te rautaki tino noa hei whakakore i tēnei raruraru ko te whakaranu i te FAPbI3 me te huinga o te methyl ammonium (MA+), te cesium (Cs+) me ngā bromide (Br-) ions7,8,9. Heoi, ka pāngia ngā perovskites ranu e te whānui haere o te āputa roopu me te wehenga wāhanga i puta mai i te whakaahua, ka whakararu i te mahi me te pumau o ngā PSC e puta mai ana10,11,12.
Kua whakaatuhia e ngā rangahau hou he tino pumau te FAPbI3 tioata kotahi parakore, kāore he tāpiritanga, nā te mea he tino pai te tioata me te iti o ngā hapa13,14. Nō reira, ko te whakaiti i ngā hapa mā te whakanui ake i te tioata o te FAPbI3 papatipu he rautaki nui hei whakatutuki i ngā PSC whai hua me te pumau2,15. Heoi, i te wā e whakahaerehia ana te FAPbI3 PSC, ka taea tonu te whakahekenga ki te wāhanga δ kore-perovskite hexagonal kōwhai kāore e hiahiatia16. Ko te tikanga ka tīmata te tukanga i ngā mata me ngā rohe witi e ngawari ake ana ki te wai, te wera me te mārama nā te mea he maha ngā wāhi hapa17. Nō reira, me whakangāwari te mata/witi hei whakau i te wāhanga pango o te FAPbI318. He maha ngā rautaki whakangāwari hapa, tae atu ki te whakaurunga o ngā perovskite iti-ahu, ngā ngota Lewis waikawa-pūtake, me ngā tote ammonium halide, kua tino ahu whakamua i roto i ngā formamidine PSC19,20,21,22. Tae noa ki tēnei wā, kua aro te nuinga o ngā rangahau ki te tūranga o ngā momo hapa i roto i te whakatau i ngā āhuatanga optoelectronic pērā i te whakakotahitanga o ngā kaikawe, te roa o te horapa me te hanganga roopu i roto i ngā pūtau rā22,23,24. Hei tauira, ka whakamahia te ariā mahi kiato (DFT) hei matapae i ngā kaha hanganga me ngā taumata kaha hopu o ngā momo hapa, e whakamahia whānuitia ana hei ārahi i te hoahoa passivation mahi20,25,26. I te hekenga o te maha o ngā hapa, ka pai ake te pumau o te taputapu. Heoi, i roto i ngā formamidine PSC, me tino rerekē ngā tikanga o te awe o ngā momo hapa ki te pumau o te wāhanga me ngā āhuatanga photoelectric. Ki tā mātou e mōhio ana, kāore anō kia tino mārama te māramatanga taketake mō te āhua o te whakaoho a ngā hapa i te whakawhiti wāhanga cubic ki te hexagonal (α-δ) me te tūranga o te passivation mata ki te pumau o te wāhanga o te α-FAPbI3 perovskite.
I konei, ka whakakitea e mātou te ara whakahekenga o te perovskite FAPbI3 mai i te wāhanga-α mangu ki te wāhanga-δ kōwhai me te awe o ngā momo hapa ki te arai pūngao o te whakawhiti wāhanga-α ki te-δ mā te DFT. Ko ngā wāhi kore-I, e ngāwari ana te whakaputa i te wā hanga kiriata me te whakahaere taputapu, e matapaetia ana koia te mea tino pea hei tīmata i te whakawhiti wāhanga α-δ. Nō reira, i whakauruhia e mātou he paparanga matotoru o te oxalate mata (PbC2O4) kāore e rewa i te wai, ā, he pumau te matū ki runga i te FAPbI3 mā te tauhohenga in situ. Ka aukati te mata oxalate mata (LOS) i te hanganga o ngā wāhi kore-I, ā, ka ārai i te hekenga o ngā ion I ina whakaohokia e te wera, te mārama, me ngā mara hiko. Ko te LOS hua ka whakaiti nui i te whakakotahitanga kore-ira i te taha mata, ā, ka whakapai ake i te whai huatanga o te FAPbI3 PSC ki te 25.39% (kua whakamanahia ki te 24.92%). I puritia e te taputapu LOS kāhore he taupoki i te 92% o tōna whai huatanga taketake i muri i te whakamahinga i te pūwāhi mana mōrahi (MPP) mō ngā haora neke atu i te 550 i te papatipu hau whakaata (AM) o te 1.5 G o te irahiko.
I te tuatahi i whakahaerehia e mātou ngā tātaitanga ab initio hei kimi i te ara wetewete o te perovskite FAPbI3 ki te whakawhiti mai i te wāhanga α ki te wāhanga δ. Mā te tukanga whakawhiti wāhanga taipitopito, i kitea kua tutuki te whakawhiti mai i te octahedron tiri-kokonga-toru-ahu [PbI6] i roto i te wāhanga-α kupiko o FAPbI3 ki te octahedron tiri-taha-kotahi-ahu [PbI6] i roto i te wāhanga-δ hexagonal o FAPbI3. te pakaru 9. Ka hanga e Pb-I he hononga i te taahiraa tuatahi (Int-1), ā, ka eke tōna arai pūngao ki te 0.62 eV/pūtau, e whakaaturia ana i te Pikitia 1a. Ina nekehia te octahedron i te ahunga [0\(\bar{1}\)1], ka whānui te mekameka poto hexagonal mai i te 1×1 ki te 1×3, 1×4, ā, ka mutu ka uru ki te wāhanga δ. Ko te ōwehenga aronga o te ara katoa ko (011)α//(001)δ + [100]α//[100]δ. Mai i te tūtohi tohatoha pūngao, ka kitea i muri i te whakapūtanga o te wāhanga δ o FAPbI3 i ngā wāhanga e whai ake nei, he iti iho te arai pūngao i tērā o te whakawhiti wāhanga α, ko te tikanga ka tere ake te whakawhiti wāhanga. He mārama, he mea nui te taahiraa tuatahi o te whakahaere i te whakawhiti wāhanga mēnā e hiahia ana tātou ki te pehi i te whakahekenga wāhanga-α.
a Te tukanga whakawhiti wāhanga mai i te maui ki te matau – wāhanga mangu FAPbI3 (wāhanga-α), te wehenga hononga Pb-I tuatahi (Int-1) me te wehenga hononga Pb-I anō (Int-2, Int -3 me Int -4) me te wāhanga kōwhai FAPbI3 (wāhanga delta). b Ngā arai pūngao ki te whakawhiti wāhanga α ki δ o FAPbI3 i runga i ngā hapa pūwāhi ā-roto. E whakaatu ana te rārangi iraira i te arai pūngao o te karaihe pai (0.62 eV). c Te pūngao o te hanganga o ngā hapa pūwāhi tuatahi i runga i te mata o te perovskite mata. Ko te tuaka abscissa te arai pūngao o te whakawhiti wāhanga α-δ, ā, ko te tuaka ordinate te pūngao o te hanganga hapa. Ko ngā wāhanga kua whakamarumaruhia ki te hina, te kōwhai me te kakariki ko te momo I (EB iti-teitei FE), momo II (FE teitei) me te momo III (EB iti-iti FE), ia. d Te pūngao o te hanganga o ngā hapa VI me te LOS o FAPbI3 i roto i te mana whakahaere. e I te arai ki te hekenga katote i roto i te mana whakahaere me te LOS o FAPbI3. f – te whakaaturanga kauwhata o te hekenga o ngā iona I (ngā porowhita karaka) me te gLOS FAPbI3 (hina, mata; waiporoporo (karaka), iodine (iodine nekeneke)) i roto i te mana whakahaere gf (maui: tirohanga o runga; matau: wāhanga whakawhiti, parauri); waro; kikorangi mārama – hauota; whero – hāora; māwhero mārama – hauwai). Ka whakaratohia ngā raraunga pūtake i roto i te āhua o ngā kōnae raraunga pūtake.
Kātahi ka rangahauhia e mātou te awe o ngā momo hapa pūwāhi ā-roto (tae atu ki te PbFA, IFA, PbI, me te noho ā-paepae IPb; ngā ngota interstitial Pbi me Ii; me ngā wāhi wātea VI, VFA, me VPb), e kiia ana he mea matua. e whakaatu ana i te whakahekenga o te taumata ngota me te taumata pūngao i roto i te Pikitia 1b me te Ripanga Tāpiri 1. He mea whakamīharo, ehara i te mea ko ngā hapa katoa e whakaiti ana i te arai pūngao o te whakawhiti wāhanga α-δ (Pikitia 1b). E whakapono ana mātou ko ngā hapa he iti te kaha hanganga me ngā arai pūngao whakawhiti wāhanga α-δ iti iho e kiia ana he kino ki te pumau o te wāhanga. E ai ki te pūrongo o mua, ko ngā mata whai rawa i te mata he mea whai hua mō te formamidine PSC27. Nō reira, ka arotahi mātou ki te mata (100) kua mutu i te PbI2 i raro i ngā āhuatanga whai rawa i te mata. Ko te kaha hanganga hapa o ngā hapa pūwāhi ā-roto o te mata e whakaaturia ana i roto i te Pikitia 1c me te Ripanga Tāpiri 1. I runga i te arai pūngao (EB) me te kaha hanganga whakawhiti wāhanga (FE), ka whakarōpūtia ēnei hapa ki ngā momo e toru. Momo I (EB iti-FE teitei): Ahakoa ka whakaitihia e IPb, VFA me VPb te arai pūngao ki te whakawhiti āhua, he nui ō rātou kaha hanganga. Nō reira, e whakapono ana mātou he iti noa te pānga o ēnei momo hapa ki ngā whakawhiti āhua nā te mea he onge te hanganga. Momo II (EB teitei): Nā te pai ake o te arai pūngao whakawhiti āhua α-δ, kāore ngā hapa ā-pae PbI, IFA me PbFA e kino ki te pumau āhua o te perovskite α-FAPbI3. Momo III (EB iti-FE iti): Ka taea e ngā hapa VI, Ii me Pbi me ngā kaha hanganga iti te whakararu i te āhua pango. Ina koa i te iti rawa o te FE me te EB VI, e whakapono ana mātou ko te rautaki tino whai hua ko te whakaiti i ngā wāhi takoto kau I.
Hei whakaiti i te VI, i whakawhanakehia e mātou he paparanga matotoru o te PbC2O4 hei whakapai ake i te mata o te FAPbI3. Ki te whakatauritea ki ngā matū whakangāwari tote halide waro pērā i te phenylethylammonium iodide (PEAI) me te n-octylammonium iodide (OAI), ko te PbC2O4, kāore he iona halogen nekeneke, he pumau te matū, kāore e wairewa i roto i te wai, ā, he ngāwari te whakakore i te whakaoho. He pai te pumau o te makuku mata me te papa hiko o te perovskite. Ko te wairewatanga o te PbC2O4 i roto i te wai he 0.00065 g/L noa iho, he iti iho i te PbSO428. He mea nui ake, ka taea te whakarite mārie i ngā paparanga matotoru me te ōrite o te LOS ki runga i ngā kiriata perovskite mā te whakamahi i ngā tauhohenga in situ (tirohia i raro). I whakahaerehia e mātou ngā whakatauira DFT o te hononga ā-mata i waenga i te FAPbI3 me te PbC2O4 e whakaatuhia ana i te Pikitia Tāpiri 1. E whakaatu ana te Ripanga Tāpiri 2 i te pūngao hanganga hapa i muri i te werohanga LOS. I kitea e mātou kāore te LOS e whakanui noa i te kaha hanganga o ngā hapa VI mā te 0.69–1.53 eV (Pikitia 1d), engari ka whakanui anō hoki i te kaha whakahohe o te I i te mata hekenga me te mata putanga (Pikitia 1e). I te wāhanga tuatahi, ka heke ngā iona I i te mata perovskite, ka waiho ngā iona VI i roto i te tūranga whatunga me te ārai kaha o te 0.61 eV. Whai muri i te whakaurunga o te LOS, nā te pānga o te aukati steric, ka piki te kaha whakahohe mō te hekenga o ngā iona I ki te 1.28 eV. I te wā e heke ana ngā iona I e wehe atu ana i te mata perovskite, he teitei ake hoki te ārai kaha i roto i te VOC i te tauira mana (Pikitia 1e). Kei te Pikitia 1 f me g ngā hoahoa kauwhata o ngā ara hekenga iona I i roto i te mana me te LOS FAPbI3. E whakaatu ana ngā hua whakatauira ka taea e te LOS te aukati i te hanganga o ngā hapa VI me te whakakorikori o te I, ā, ka ārai i te nucleation o te whakawhiti wāhanga α ki δ.
I whakamātauria te tauhohenga i waenga i te waikawa oxalic me te FAPbI3 perovskite. I muri i te whakaranu i ngā otinga o te waikawa oxalic me te FAPbI3, ka puta he nui o te matū mā, e whakaaturia ana i te Pikitia Tāpiri 2. I tautuhia te hua paura hei rauemi PbC2O4 parakore mā te whakamahi i te X-ray diffraction (XRD) (Pikitia Tāpiri 3) me te Fourier transform infrared spectroscopy (FTIR) (Pikitia Tāpiri 4). I kitea e mātou he tino wairewa te waikawa oxalic i roto i te waipiro isopropyl (IPA) i te pāmahana rūma me te wairewatanga o te 18 mg/mL, e whakaaturia ana i te Pikitia Tāpiri 5. Mā tēnei ka māmā ake te tukatuka i muri mai nā te mea ko te IPA, hei whakarewa passivation noa, kāore e kino te paparanga perovskite i tua atu i te wā poto29. Nō reira, mā te tuku i te kiriata perovskite ki roto i te wairewa waikawa oxalic, mā te paninga hurihuri rānei i te wairewa waikawa oxalic ki runga i te perovskite, ka taea te tere te whiwhi i te PbC2O4 angiangi, matotoru hoki i runga i te mata o te kiriata perovskite e ai ki te whārite matū e whai ake nei: H2C2O4 + FAPbI3 = PbC2O4 + FAI +HI. Ka taea te whakarewa i te FAI ki roto i te IPA, ā, ka tangohia i te wā e tunu ana. Ka taea te whakahaere i te matotoru o te LOS mā te wā tauhohenga me te kukū o te matū mua.
Kei te whakaatuhia ngā whakaahua o te karu hiko matawai (SEM) o ngā kiriata perovskite mana whakahaere me ngā kiriata perovskite LOS i roto i ngā Pikitia 2a, b. E whakaatu ana ngā hua he pai te tiaki i te āhua o te mata perovskite, ā, he nui ngā matūriki angiangi kua whakatakotoria ki runga i te mata o te witi, e tohu ana i te paparanga PbC2O4 i hangaia e te tauhohenga in-situ. He maeneene ake te mata o te kiriata perovskite LOS (Pikitia Tāpiri 6) me te koki whakapā wai nui ake i te kiriata mana whakahaere (Pikitia Tāpiri 7). I whakamahia te karu hiko tuku whakawhiti teitei-taumira (HR-TEM) hei wehewehe i te paparanga mata o te hua. Ki te whakatauritea ki te kiriata mana whakahaere (Pikitia 2c), he paparanga angiangi ōrite, matotoru hoki, tata ki te 10 nm te matotoru, e kitea mārama ana i runga i te perovskite LOS (Pikitia 2d). Mā te whakamahi i te karu hiko matawai porowhita-teitei (HAADF-STEM) hei tirotiro i te hononga i waenga i te PbC2O4 me te FAPbI3, ka taea te kite mārama i te aroaro o ngā rohe tioata o te FAPbI3 me ngā rohe kore-āhua o te PbC2O4 (Pikitia Tāpiri 8). Ko te hanganga mata o te perovskite i muri i te maimoatanga waikawa oxalic i tautuhia e ngā inenga X-ray photoelectron spectroscopy (XPS), e whakaatuhia ana i roto i ngā Pikitia 2e–g. I roto i te Pikitia 2e, ko ngā tihi C 1s huri noa i te 284.8 eV me te 288.5 eV no ngā tohu CC me te FA motuhake. Ki te whakatauritea ki te membrane whakahaere, i whakaatuhia e te membrane LOS tētahi atu tihi i te 289.2 eV, e kiia ana ko te C2O42-. E toru ngā tihi O1s motuhake matū o te whānuitanga O1s o te perovskite LOS e whakaatu ana i te 531.7 eV, 532.5 eV, me te 533.4 eV, e rite ana ki te COO kua tangohia te proton, te C=O o ngā rōpū oxalate 30 me ngā ngota O o te wāhanga OH (Pikitia 2e). )). Mō te tauira whakahaere, he iti noa te tihi O1s i kitea, e taea ana te kī ko te hāora kua mimitihia ki te mata. Ko ngā āhuatanga o te membrane whakahaere o te Pb 4f7/2 me te Pb 4f5/2 kei te 138.4 eV me te 143.3 eV. I kite mātou ko te perovskite LOS e whakaatu ana i te nekehanga o te tihi Pb tata ki te 0.15 eV ki te kaha here teitei ake, e tohu ana i te taunekeneke kaha ake i waenga i ngā ngota C2O42- me te Pb (Pikitia 2g).
a Ngā whakaahua SEM o ngā kiriata perovskite mana whakahaere me te b, tirohanga o runga. c Te karu hiko whakawhiti-wāhanga teitei-taumira (HR-TEM) o ngā kiriata perovskite mana whakahaere me te d LOS. XPS teitei-taumira o e C 1s, f O 1s me g Pb 4f ngā kiriata perovskite. Ka whakaratohia ngā raraunga pūtake i roto i te ahua o ngā kōnae raraunga pūtake.
E ai ki ngā hua o te DFT, e matapaetia ana i roto i te ariā ka ngāwari te whakawhiti i te āhua mai i te α ki te δ nā ngā hapa VI me te hekenga I. Kua whakaatuhia e ngā pūrongo o mua ka tere te tukuna o te I2 mai i ngā kiriata perovskite PC i te wā e rumakina ana i muri i te whakaaturanga o ngā kiriata ki te mārama me te ahotea wera31,32,33. Hei whakaū i te pānga pumau o te oxalate mata ki te āhua-α o te perovskite, i rumakina e mātou ngā kiriata perovskite mana whakahaere me te LOS ki roto i ngā pounamu karāhe mārama kei roto te toluene, ia, kātahi ka whakamātaohia ki te hihi o te rā mō te 24 hāora. I inehia e mātou te mimiti o te otinga toluene ultraviolet me te mārama kitea (UV-Vis), e whakaaturia ana i te Pikitia 3a. Ki te whakatauritea ki te tauira mana whakahaere, he iti ake te kaha mimiti o te I2 i kitea i roto i te take o te LOS-perovskite, e tohu ana ka taea e te LOS kiato te aukati i te tukunga o te I2 mai i te kiriata perovskite i te wā e rumakina ana te mārama. Kei roto i ngā huinga o ngā Pikitia 3b me te c ngā whakaahua o ngā kiriata perovskite mana whakahaere me te LOS kua pakeke. He mangu tonu te perovskite LOS, engari kua huri te nuinga o te kiriata whakahaere hei kōwhai. Ko ngā hihi mimiti UV-kitea o te kiriata rumakina e whakaaturia ana i roto i ngā Pikitia 3b, c. I kite mātou kua heke te mimiti e rite ana ki te α i roto i te kiriata whakahaere. I mahia ngā inenga hihi-X hei tuhi i te whanaketanga o te hanganga tioata. I muri i te 24 hāora o te whakamārama, i whakaatu te perovskite whakahaere i tētahi tohu kaha o te wāhanga δ kōwhai (11.8°), i te mea kei te mau tonu te wāhanga pango pai o te perovskite LOS (Pikitia 3d).
Ngā hihi mimiti UV-kitea o ngā otinga toluene i rumakina ai te kiriata whakahaere me te kiriata LOS i raro i te rā kotahi mō ngā hāora 24. E whakaatu ana te pikitia whakauru i tētahi pounamu i rumakina ai ia kiriata ki roto i te rōrahi ōrite o te toluene. b Ngā hihi mimiti UV-Vis o te kiriata whakahaere me te kiriata LOS i mua me muri i te 24 hāora o te rumakina i raro i te rā kotahi. E whakaatu ana te pikitia whakauru i tētahi whakaahua o te kiriata whakamātautau. d Ngā tauira diffraction hihi-X o ngā kiriata whakahaere me ngā kiriata LOS i mua me muri i te 24 hāora o te whakamahanatanga. Ngā whakaahua SEM o te kiriata whakahaere e me te kiriata f LOS i muri i te 24 hāora o te whakamahanatanga. Ka whakaratohia ngā raraunga pūtake i roto i te āhua o ngā kōnae raraunga pūtake.
I whakahaerehia e mātou ngā inenga mā te karu hiko matawai (SEM) hei tirotiro i ngā huringa hanganga moroiti o te kiriata perovskite i muri i ngā haora 24 o te whakamārama, e whakaaturia ana i roto i ngā Pikitia 3e, f. I roto i te kiriata whakahaere, i whakangaromia ngā kakano nui, ā, i hurihia hei ngira iti, e rite ana ki te āhua o te hua δ-wāhanga FAPbI3 (Pikitia 3e). Mō ngā kiriata LOS, kei te pai tonu te āhua o ngā kakano perovskite (Pikitia 3f). I whakaūhia e ngā hua ko te ngaronga o te I ka tino whakaoho i te whakawhiti mai i te wāhanga pango ki te wāhanga kōwhai, ko te PbC2O4 ka whakaū i te wāhanga pango, ka ārai i te ngaronga o te I. Nā te mea he nui ake te mātotoru o te takoto kau i te mata i te nuinga o te kakano,34 he nui ake te tūponotanga o tēnei wāhanga ki te mata o te kakano. ka tukuna te iodine me te hanga VI i te wā kotahi. E ai ki te matapae a DFT, ka taea e te LOS te aukati i te hanganga o ngā hapa VI me te ārai i te hekenga o ngā iona I ki te mata perovskite.
I tua atu, i rangahauhia te pānga o te paparanga PbC2O4 ki te ātete makuku o ngā kiriata perovskite i roto i te hau āhuarangi (te haumākū whanaunga 30-60%). E ai ki te Whakaahua Tāpiri 9, i mangu tonu te perovskite LOS i muri i ngā rā 12, i te mea ka huri te kiriata whakahaere hei kōwhai. I roto i ngā inenga XRD, e whakaatu ana te kiriata whakahaere i tētahi tihi kaha i te 11.8° e rite ana ki te wāhanga δ o FAPbI3, i te mea ka mau tonu te wāhanga α pango o te perovskite LOS (Whakaahua Tāpiri 10).
I whakamahia te photoluminescence āhua-tūturu (PL) me te photoluminescence whakatau-wā (TRPL) hei ako i te pānga passivation o te mata oxalate ki te mata perovskite. I roto i te Pikitia 4a e whakaatu ana kua piki ake te kaha PL o te kiriata LOS. I roto i te whakaahua mahere PL, ko te kaha o te kiriata LOS puta noa i te rohe katoa o te 10 × 10 μm2 he teitei ake i te kiriata whakahaere (Pikitia Tāpiri 11), e tohu ana ka passivate ōrite te PbC2O4 i te kiriata perovskite. Ka whakatauhia te roanga o te oranga kawe mā te whakatata atu ki te pirau TRPL me te mahi taupū kotahi (Pikitia 4b). Ko te roanga o te oranga kawe o te kiriata LOS he 5.2 μs, he roa ake i te kiriata whakahaere me te roanga o te oranga kawe o te 0.9 μs, e tohu ana i te whakahekenga o te whakakotahitanga kore-ira o te mata.
PL āhua-pūmau me te whānuitanga-b o te PL rangitahi o ngā kiriata perovskite i runga i ngā papa karāhe. c Te pihi SP o te taputapu (FTO/TiO2/SnO2/perovskite/spiro-OMeTAD/Au). d Te whānuitanga EQE me te whānuitanga Jsc EQE kua whakauruhia mai i te taputapu tino whai hua. d Te whakawhirinakitanga o te kaha o te mārama o te taputapu perovskite ki te tūtohi Voc. f Te tātaritanga MKRC noa mā te whakamahi i te taputapu poka horoi ITO/PEDOT:PSS/perovskite/PCBM/Au. Ko te VTFL te ngaohiko whakakī mahanga mōrahi. Mai i ēnei raraunga i tatauhia e mātou te kiato mahanga (Nt). Ka whakaratohia ngā raraunga pūtake i roto i te ahua o ngā kōnae raraunga pūtake.
Hei ako i te pānga o te paparanga oxalate mata ki te mahi a te taputapu, i whakamahia he hanganga whakapā FTO/TiO2/SnO2/perovskite/spiro-OMeTAD/Au tuku iho. Ka whakamahia e mātou te formamidine chloride (FACl) hei tāpiri ki te perovskite precursor hei utu mō te methylamine hydrochloride (MACl) kia pai ake ai te mahi a te taputapu, nā te mea ka taea e te FACl te whakarato i te kounga tioata pai ake me te karo i te āputa roopu o FAPbI335 (tirohia ngā Pikitia Tāpiri 1 me te 2 mō te whakataurite taipitopito). ). 12-14). I whiriwhiria te IPA hei antisolvent nā te mea ka whakarato i te kounga tioata pai ake me te whakatakotoranga pai ake i roto i ngā kiriata perovskite ki te whakataurite ki te diethyl ether (DE) chlorobenzene (CB)36 rānei (Ngā Pikitia Tāpiri 15 me te 16). I ata arotauhia te matotoru o te PbC2O4 kia pai ai te taurite o te passivation hapa me te kawe utu mā te whakarerekē i te kukū waikawa oxalic (Pikitia Tāpiri 17). Kei te whakaatuhia ngā whakaahua SEM whakawhiti-wāhanga o ngā taputapu mana whakahaere me ngā taputapu LOS kua arotauhia i te Pikitia Tāpiri 18. Kei te whakaatuhia ngā ānau kiato iahiko (CD) mō ngā taputapu mana whakahaere me ngā taputapu LOS i te Pikitia 4c, ā, kei te Ripanga Tāpiri 3 ngā tawhā i tangohia. Ngā pūtau mana whakahaere whai huatanga tahuritanga mana mōrahi (PCE) 23.43% (22.94%), Jsc 25.75 mA cm-2 (25.74 mA cm-2), Voc 1.16 V (1.16 V) me te matawai whakamuri (whakamua). Ko te tauwehe whakakī (FF) he 78.40% (76.69%). Ko te PCE LOS PSC mōrahi he 25.39% (24.79%), Jsc he 25.77 mA cm-2, Voc he 1.18 V, FF he 83.50% (81.52%) mai i te whakamuri (matawai whakamua ki). I tutuki i te taputapu LOS te mahi photovoltaic kua whakamanahia o te 24.92% i roto i tētahi taiwhanga photovoltaic tuatoru pono (Pikitia Tāpiri 19). I homai e te whai huatanga matū ā-waho (EQE) he Jsc whakauru o te 24.90 mA cm-2 (mana) me te 25.18 mA cm-2 (LOS PSC), ia, he mea e rite ana ki te Jsc i inehia i roto i te whānuitanga AM 1.5 G paerewa (Pikitia .4d). ). Ko te tohatoha tatauranga o ngā PCE i inehia mō ngā mana whakahaere me ngā LOS PSC e whakaaturia ana i roto i te Pikitia Tāpiri 20.
E ai ki te Whakaahua 4e, i tatauhia te whanaungatanga i waenga i te Voc me te kaha o te mārama hei ako i te pānga o te PbC2O4 ki te whakakotahitanga mata i āwhinahia e te mahanga. Ko te pari o te raina kua whakauruhia mō te taputapu LOS he 1.16 kBT/sq, he iti iho i te pari o te raina kua whakauruhia mō te taputapu whakahaere (1.31 kBT/sq), e whakaū ana he whai hua te LOS mō te aukati i te whakakotahitanga mata e ngā maminga. Ka whakamahia e mātou te hangarau whakawhāiti iahiko ātea (SCLC) hei ine i te kiato hapa o te kiriata perovskite mā te ine i te āhuatanga IV pōuri o te taputapu poka (ITO/PEDOT:PSS/perovskite/spiro-OMeTAD/Au) e ai ki te whakaaturanga i te whakaahua. Whakaaturanga 4f. Ka tatauhia te mātotoru o te mahanga mā te tātai Nt = 2ε0εVTFL/eL2, ko ε te pūmau dielectric whanaunga o te kiriata perovskite, ko ε0 te pūmau dielectric o te korehau, ko VTFL te ngaohiko whakawhāiti mō te whakakī i te mahanga, ko e te utu, ko L te matotoru o te kiriata perovskite (650 nm). Ka tatauhia te mātotoru hapa o te taputapu VOC kia 1.450 × 1015 cm–3, he iti iho i te mātotoru hapa o te taputapu whakahaere, arā, 1.795 × 1015 cm–3.
I whakamātauria te taputapu kāhore he mea i whakakīia ki te pūwāhi mana mōrahi (MPP) i raro i te awatea katoa i raro i te hauota hei tirotiro i tōna pumau mahi mō te wā roa (Pikitia 5a). I muri i ngā hāora 550, i mau tonu te taputapu LOS i te 92% o tōna pai mōrahi, i te mea kua heke te mahi a te taputapu whakahaere ki te 60% o tōna mahi taketake. I inehia te tohatoha o ngā huānga i roto i te taputapu tawhito mā te ine ira papatipu katote tuarua wā-o-te-rere (ToF-SIMS) (Pikitia 5b, c). Ka kitea he nui te kohi o te iodine i te rohe whakahaere koura o runga. Ko ngā tikanga o te tiaki hau kore mahi ka kore e whakauru i ngā āhuatanga whakaiti taiao pēnei i te makuku me te hāora, e kī ana ko ngā tikanga ā-roto (arā, te hekenga katote) te take. E ai ki ngā hua o te ToF-SIMS, i kitea ngā katote I- me AuI2- i roto i te hiko Au, e tohu ana i te horapa o te I mai i te perovskite ki te Au. Ko te kaha tohu o ngā katote I- me AuI2- i roto i te taputapu whakahaere he tata ki te 10 ngā wā teitei ake i te tauira VOC. Kua whakaatuhia e ngā pūrongo o mua ka taea e te urunga o te katote te arahi ki te hekenga tere o te kawe pū o te spiro-OMeTAD me te waikura matū o te paparanga hiko o runga, ā, ka kino te hononga ā-mata i roto i te taputapu37,38. I tangohia te hiko Au, ā, i horoia te paparanga spiro-OMeTAD mai i te papa ki te otinga chlorobenzene. Kātahi ka tautuhia e mātou te kiriata mā te whakamahi i te grazing incidence X-ray diffraction (GIXRD) (Pikitia 5d). E whakaatu ana ngā hua he mārama te tihi diffraction o te kiriata whakahaere i te 11.8°, engari kāore he tihi diffraction hou e puta ana i roto i te tauira LOS. E whakaatu ana ngā hua ko ngā ngaronga nui o ngā katote I i roto i te kiriata whakahaere ka arahi ki te whakaputanga o te wāhanga δ, i roto i te kiriata LOS kua mārama te aukati i tēnei tukanga.
575 hāora o te aroturuki MPP tonu o tētahi taputapu kāore i hiritia i roto i te hauota hauota me te 1 rā, kāore he tātari UV. Te tohatoha ToF-SIMS o ngā iona b I- me c AuI2- i roto i te taputapu whakahaere LOS MPP me te taputapu tawhito. Ko ngā atarangi o te kōwhai, te kakariki me te karaka e rite ana ki te Au, Spiro-OMeTAD me te perovskite. d GIXRD o te kiriata perovskite i muri i te whakamātautau MPP. Ka whakaratohia ngā raraunga pūtake i roto i te ahua o ngā kōnae raraunga pūtake.
I inehia te kawe hiko e pā ana ki te pāmahana hei whakaū i te kaha o te PbC2O4 ki te aukati i te hekenga o te katote (Pikitia Tāpiri 21). Ka whakatauhia te kaha whakahohenga (Ea) o te hekenga o te katote mā te ine i te huringa o te kawe hiko (σ) o te kiriata FAPbI3 i ngā pāmahana rerekē (T) me te whakamahi i te whanaungatanga Nernst-Einstein: σT = σ0exp(−Ea/kBT), ko σ0 he pūmau, ko kB te pūmau Boltzmann. Ka whiwhi mātou i te uara o Ea mai i te pari o ln(σT) ki te 1/T, arā, 0.283 eV mō te mana whakahaere me te 0.419 eV mō te taputapu LOS.
Hei whakarāpopototanga, ka whakaratohia e mātou he anga ariā hei tautuhi i te ara whakahekenga o te perovskite FAPbI3 me te awe o ngā momo hapa ki te arai pūngao o te whakawhiti wāhanga α-δ. I roto i ēnei hapa, e matapaetia ana e ngā hapa VI ka ngāwari te whakaputa i te whakawhiti wāhanga mai i te α ki te δ. Ka whakaurua he paparanga matotoru kore-wairewa, ā, he pumau te matū o te PbC2O4 hei whakau i te wāhanga-α o te FAPbI3 mā te aukati i te hanganga o ngā wāhi kore I me te hekenga o ngā iona I. Ka whakaitihia e tēnei rautaki te whakakotahitanga kore-ira-a-roto, ka whakanui ake i te whai huatanga o te pūtau rā ki te 25.39%, ā, ka whakapai ake i te pumau o te mahi. Ka whakaratohia e ā mātou hua he aratohu mō te whakatutuki i ngā PSC formamidine whai hua me te pumau mā te aukati i te whakawhiti wāhanga α ki te δ i puta mai i te hapa.
I hokona te Titanium(IV) isopropoxide (TTIP, 99.999%) mai i Sigma-Aldrich. I hokona te waikawa hauwaiora (HCl, 35.0–37.0%) me te etanoru (korewai) mai i Guangzhou Chemical Industry. I hokona te SnO2 (15 wt% tin(IV) oxide colloidal dispersion) mai i Alfa Aesar. I hokona te Lead(II) iodide (PbI2, 99.99%) mai i TCI Shanghai (Haina). I hokona mai i te Kamupene Hangarau Mārama Poramiti o Xi'an (Haina) te Formamidine iodide (FAI, ≥99.5%), te formamidine chloride (FACl, ≥99.5%), te methylamine hydrochloride (MACl, ≥99.5%), te 2,2′,7,7′-tetrakis-(N , N-di-p) )-methoxyaniline)-9,9′-spirobifluorene (Spiro-OMeTAD, ≥99.5%), te lithium bis(trifluoromethane)sulfonylimide (Li-TFSI, 99.95%), te 4-tert -butylpyridine (tBP, 96%). N,N-dimethylformamide (DMF, 99.8%), dimethyl sulfoxide (DMSO, 99.9%), isopropyl alcohol (IPA, 99.8%), chlorobenzene (CB, 99.8%), acetonitrile (ACN). I hokona mai i Sigma-Aldrich. I hokona mai te waikawa oxalic (H2C2O4, 99.9%) i Macklin. I whakamahia ngā matū katoa i te wā i riro mai ai, kāore he whakarerekētanga kē atu.
I horoia ngā papa ITO, FTO rānei (1.5 × 1.5 cm2) mā te whakamahi i te hopi horoi, te acetone, me te etanoru mō te 10 meneti, ia, kātahi ka whakamaroketia i raro i te awa hauota. I whakatakotoria he paparanga ārai TiO2 matotoru ki runga i te papa FTO mā te whakamahi i te otinga o te titanium diisopropoxybis (acetylacetonate) i roto i te etanoru (1/25, v/v) i whakatakotoria ki te 500 °C mō te 60 meneti. I whakaranua te marara colloidal SnO2 ki te wai deionized i roto i te ōwehenga rōrahi o te 1:5. I runga i te papa ma i rongoatia ki te ozone UV mō te 20 meneti, i whakatakotoria he kiriata angiangi o ngā nanoparticles SnO2 i te 4000 rpm mō te 30 hēkona, kātahi ka whakamahanahia ki te 150 °C mō te 30 meneti. Mō te otinga perovskite precursor, i whakarewaina te 275.2 mg FAI, 737.6 mg PbI2 me te FACl (20 mol%) ki roto i te whakarewa whakauru DMF/DMSO (15/1). I whakaritea te paparanga perovskite mā te centrifuge i te 40 μL o te wairewa perovskite i runga i te paparanga SnO2 i tukatukahia ki te UV-ozone i te 5000 rpm i roto i te hau taiao mō te 25 hēkona. 5 hēkona i muri i te wā whakamutunga, i maturuturu teretia te 50 μL o te wairewa MACl3 IPA (4 mg/mL) ki runga i te papa hei ārai-whakarewa. Kātahi, ka whakamahanahia ngā kiriata hou i whakaritea i te 150°C mō te 20 meneti, kātahi ka whakamahanahia ki te 100°C mō te 10 meneti. I muri i te whakamatao i te kiriata perovskite ki te pāmahana rūma, ka centrifugehia te wairewa H2C2O4 (1, 2, 4 mg i rewa i roto i te 1 mL IPA) i te 4000 rpm mō te 30 hēkona hei whakakore i te mata perovskite. I pania ki runga i te kiriata he otinga spiro-OMeTAD i whakaritea mā te whakaranu i te 72.3 mg spiro-OMeTAD, 1 ml CB, 27 µl tBP me te 17.5 µl Li-TFSI (520 mg i roto i te 1 ml acetonitrile) i hurihia ki te 4000 rpm i roto i te 30 hēkona. Hei whakamutunga, i mimitihia he paparanga Au matotoru 100 nm i roto i te korehau i te tere o te 0.05 nm/s (0~1 nm), 0.1 nm/s (2~15 nm) me te 0.5 nm/s (16~100 nm).
I inehia te mahi SC o ngā pūtau rā perovskite mā te whakamahi i te mita Keithley 2400 i raro i te whakamārama o te pūwhakamārama rā (SS-X50) i te kaha o te mārama o te 100 mW/cm2, ā, i manatokohia mā te whakamahi i ngā pūtau rā silicon paerewa kua whakatikatikaina. Ki te kore e kīia tētahi atu mea, i inehia ngā pihi SP i roto i te pouaka karapu kī tonu i te hauota i te pāmahana rūma (~25°C) i roto i ngā aratau matawai whakamua me te whakamuri (taahiraa ngaohiko 20 mV, wā whakaroa 10 ms). I whakamahia he kopare atarangi hei whakatau i te horahanga whai hua o te 0.067 cm2 mō te PSC i inehia. I mahia ngā inenga EQE i roto i te hau taiao mā te whakamahi i te pūnaha PVE300-IVT210 (Industrial Vision Technology(s) Pte Ltd) me te mārama kotahi-tae e arotahi ana ki te taputapu. Mō te pumau o te taputapu, i mahia te whakamātautau o ngā pūtau rā kāore i te kapihia i roto i te pouaka karapu hauota i te pēhanga 100 mW/cm2 me te kore he tātari UV. Ka inehia te ToF-SIMS mā te whakamahi i te PHI nanoTOFII time-of-flight SIMS. I whiwhihia te tātaritanga hohonu mā te whakamahi i tētahi pū ion Ar 4 kV me te horahanga 400×400 µm.
I whakahaerehia ngā inenga mō te ine irahiko whakaahua-X (XPS) i runga i tētahi pūnaha Thermo-VG Scientific (ESCALAB 250) mā te whakamahi i te Al Kα kotahi-ira (mō te aratau XPS) i te pēhanga o te 5.0 × 10–7 Pa. I whakahaerehia te irahiko matawai (SEM) i runga i tētahi pūnaha JEOL-JSM-6330F. I inehia te āhua o te mata me te taratara o ngā kiriata perovskite mā te whakamahi i te irahiko kaha ngota (AFM) (Bruker Dimension FastScan). Kei te FEI Titan Themis STEM te STEM me te HAADF-STEM. I inehia ngā ira mimiti UV–Vis mā te whakamahi i te UV-3600Plus (Shimadzu Corporation). I tuhia te iahiko whakawhāiti utu ātea (SCLC) ki runga i tētahi mita Keithley 2400. I inehia te irahiko whakaahua pumau (PL) me te irahiko whakaahua whakatau-wā (TRPL) o te pirau oranga kawe mā te whakamahi i te irahiko whakaahua FLS 1000. I inehia ngā whakaahua mahere PL mā te whakamahi i te pūnaha Horiba LabRam Raman HR Evolution. I whakahaerehia te tirotiro infrared Fourier transform (FTIR) mā te whakamahi i te pūnaha Thermo-Fisher Nicolet NXR 9650.
I tēnei mahi, ka whakamahia e mātou te tikanga tauira ara SSW hei ako i te ara whakawhiti ā-wāhanga mai i te ā-α ki te ā-δ. I roto i te tikanga SSW, ka whakatauhia te nekehanga o te mata pūngao pūmanawa e te ahunga o te aratau ngohengohe matapōkere (te tuarua o ngā taupatupatu), e āhei ai te ako taipitopito me te whāinga o te mata pūngao pūmanawa. I roto i tēnei mahi, ka mahia te tauira ara ki runga i te pūtau nui 72-ngota, ā, neke atu i te 100 ngā takirua āhua tīmatanga/whakamutunga (IS/FS) ka kohia i te taumata DFT. I runga i te huinga raraunga takirua IS/FS, ka taea te whakatau i te ara e hono ana i te hanganga tīmatanga me te hanganga whakamutunga me te ōritetanga i waenga i ngā ngota, kātahi ka whakamahia te nekehanga rua-ara i te mata wae rerekē hei whakatau maeneene i te tikanga āhua whakawhiti. (VK-DESV). Whai muri i te rapu i te āhua whakawhiti, ka taea te whakatau i te ara me te ārai iti rawa mā te whakarārangi i ngā ārai pūngao.
I whakahaerehia ngā tātaitanga DFT katoa mā te whakamahi i te VASP (putanga 5.3.5), kei reira ngā taunekeneke irahiko-katote o ngā ngota C, N, H, Pb, me te I e tohuhia ana e te kaupapa ngaru whakakaha kua whakamaheretia (PAW). Ka whakaahuahia te mahi hononga whakawhiti e te whakatata whānui o te rōnaki i roto i te tawhā Perdue-Burke-Ernzerhoff. I whakatakotoria te rohe pūngao mō ngā ngaru papa ki te 400 eV. Ko te rahi o te whatunga k-ira Monkhorst–Pack ko (2 × 2 × 1). Mō ngā hanganga katoa, i tino arotauhia ngā tūranga whatunga me te ngota tae noa ki te iti iho o te wāhanga ahotea mōrahi i te 0.1 GPa, ā, i raro iho i te 0.02 eV/Å te wāhanga kaha mōrahi. I roto i te tauira mata, e 4 ngā paparanga o te mata o FAPbI3, kei te paparanga o raro ngā ngota pumau e whakaata ana i te tinana o FAPbI3, ā, ka taea e ngā paparanga e toru o runga te neke noa i te wā o te tukanga arotau. He 1 ML te matotoru o te paparanga PbC2O4, ā, kei runga i te mata I-terminal o FAPbI3, te wāhi e herea ai te Pb ki te 1 I me te 4 O.
Mō ētahi atu kōrero e pā ana ki te hoahoa o te rangahau, tirohia te Whakarāpopototanga o te Pūrongo Pūkete Taiao e pā ana ki tēnei tuhinga.
Kei roto i te tuhinga kua whakaputaina ngā raraunga katoa i kohia, i tātarihia rānei i tēnei rangahau, tae atu ki ngā mōhiohio tautoko me ngā kōnae raraunga mata. Kei te wātea ngā raraunga mata i whakaaturia i roto i tēnei rangahau i https://doi.org/10.6084/m9.figshare.2410016440. Kua whakaratohia ngā raraunga pūtake mō tēnei tuhinga.
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