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A na-eji passivation ntụpọ eme ihe nke ukwuu iji melite arụmọrụ nke lead triiodide perovskite anyanwụ sel, mana mmetụta nke ntụpọ dị iche iche na nkwụsi ike α ka edoghị anya; N'ebe a, site na iji ozizi ọrụ njupụta, anyị na-achọpụta ụzọ mmebi nke formamidine lead triiodide perovskite site na α-phase ruo δ-phase ma na-amụ mmetụta nke ntụpọ dị iche iche na mgbochi ike mgbanwe usoro. Nsonaazụ ihe atụ na-ebu amụma na oghere iodine nwere ike ibute mmebi n'ihi na ha na-ebelata ihe mgbochi ike maka mgbanwe usoro α-δ nke ukwuu ma nwee ike nhazi kacha ala na elu perovskite. Ntinye nke oyi akwa dị oke nke lead oxalate nke mmiri na-anaghị agbaze na elu perovskite na-egbochi mmebi nke α-phase nke ukwuu, na-egbochi mbugharị na mgbanwe nke iodine. Na mgbakwunye, atụmatụ a na-ebelata njikọta na-abụghị redioaktivu interface ma na-eme ka arụmọrụ sel anyanwụ dịkwuo elu ruo 25.39% (nke enwetara asambodo 24.92%). Ngwaọrụ a na-ekpuchighị akpaka ka nwere ike ịnọgide na-arụ ọrụ nke ọma ruo 92% mbụ ya mgbe ọ rụchara ọrụ na ike kachasị elu ruo awa 550 n'okpuru ọkụ ikuku 1.5 G e mere ka ọ dị ka ihe nlereanya.
Arụmọrụ mgbanwe ike (PCE) nke mkpụrụ ndụ anyanwụ perovskite (PSCs) erutela ihe ndekọ dị elu nke 26% 1. Kemgbe 2015, PSC nke oge a ahọrọla formamidine triiodide perovskite (FAPbI3) dị ka oyi akwa na-amịkọrọ ìhè n'ihi nkwụsi ike okpomọkụ ya dị mma na bandgap mmasị dị nso na oke Shockley-Keisser nke 2,3,4. N'ụzọ dị mwute, ihe nkiri FAPbI3 na-agafe mgbanwe usoro site na usoro α ojii gaa na usoro odo na-abụghị perovskite δ na okpomọkụ ụlọ 5,6. Iji gbochie nhazi nke usoro delta, emepụtala ọtụtụ ihe mejupụtara perovskite dị mgbagwoju anya. Usoro kachasị eji merie nsogbu a bụ ịgwakọta FAPbI3 na ngwakọta nke methyl ammonium (MA+), cesium (Cs+) na bromide (Br-) ions7,8,9. Agbanyeghị, perovskites ngwakọ na-ata ahụhụ site na mgbasawanye bandgap na nkewa nke usoro foto, nke na-emebi arụmọrụ na nkwụsi ike ọrụ nke PSCs10,11,12 sitere na ya.
Nnyocha ndị e mere n'oge na-adịbeghị anya egosila na otu kristal FAPbI3 dị ọcha na-enweghị ọgwụ ọ bụla nwere ezigbo nkwụsi ike n'ihi kristal ya dị mma na obere ntụpọ13,14. Ya mere, ibelata ntụpọ site n'ịbawanye kristal nke nnukwu FAPbI3 bụ atụmatụ dị mkpa iji nweta PSCs2,15 dị irè ma kwụsie ike. Agbanyeghị, n'oge ọrụ nke FAPbI3 PSC, mmebi gaa na hexagonal odo odo na-abụghị perovskite δ phase ka nwere ike ime16. Usoro a na-amalitekarị n'elu na ókèala ọka ndị na-adị mfe ịnweta mmiri, okpomọkụ na ìhè n'ihi ọnụnọ nke ọtụtụ ebe nwere ntụpọ17. Ya mere, passivation elu/ọka dị mkpa iji mee ka usoro ojii nke FAPbI318 kwụsie ike. Ọtụtụ atụmatụ passivation ntụpọ, gụnyere iwebata perovskites dị ala, molekul Lewis nke acid-base, na nnu ammonium halide, emeela nnukwu ọganihu na formamidine PSCs19,20,21,22. Ruo ugbu a, ihe fọrọ nke nta ka ọ bụrụ ọmụmụ ihe niile elekwasịla anya n'ọrụ nke ntụpọ dị iche iche na-arụ n'ịchọpụta ihe onwunwe optoelectronic dịka njikọta nke ihe na-ebu ibu, ogologo mgbasa na nhazi eriri na mkpụrụ ndụ anyanwụ22,23,24. Dịka ọmụmaatụ, a na-eji ozizi njupụta ọrụ (DFT) eburu amụma n'ụzọ ozizi ike nhazi na ijide ọkwa ike nke ntụpọ dị iche iche, nke a na-ejikarị eduzi nhazi passivation bara uru20,25,26. Ka ọnụọgụ ntụpọ na-ebelata, nkwụsi ike nke ngwaọrụ na-akawanye mma. Agbanyeghị, na formamidine PSCs, usoro nke mmetụta nke ntụpọ dị iche iche na nkwụsi ike nke usoro na ihe onwunwe fotoelectric kwesịrị ịdị iche kpamkpam. Dịka anyị maara, nghọta bụ isi nke otu ntụpọ si eme ka mgbanwe nke cubic gaa na hexagonal (α-δ) na ọrụ nke passivation elu na nkwụsi ike nke usoro nke α-FAPbI3 perovskite ka aghọtachaghị nke ọma.
N'ebe a, anyị na-ekpughe ụzọ mmebi nke FAPbI3 perovskite site na α-phase ojii gaa na δ-phase odo na mmetụta nke ntụpọ dị iche iche na mgbochi ike nke mgbanwe α-site-δ-phase site na DFT. A na-atụ anya na oghere I, nke a na-emepụta ngwa ngwa n'oge mmepụta ihe nkiri na ọrụ ngwaọrụ, ga-abụ ihe kacha nwee ike ịmalite mgbanwe α-δ. Ya mere, anyị webatara oyi akwa dị oke mmiri nke lead oxalate (PbC2O4) nke na-anaghị agbaze mmiri ma kwụsie ike na kemịkalụ n'elu FAPbI3 site na mmeghachi omume in situ. Elu oxalate lead (LOS) na-egbochi nhazi nke oghere I ma na-egbochi mbugharị nke ion I mgbe ọkụ, ọkụ, na ubi eletriki kpaliri ya. LOS nke na-esi na ya apụta na-ebelata nke ukwuu njikọta na-abụghị redioative interface ma na-eme ka arụmọrụ FAPbI3 PSC ka mma ruo 25.39% (nke a kwadoro ruo 24.92%). Ngwaọrụ LOS a na-ekpuchighị ekpuchi jigidere 92% nke arụmọrụ mbụ ya mgbe ọ rụchara ọrụ na ebe kachasị ike (MPP) ruo ihe karịrị awa 550 na oke ikuku e mere ka ọ dị ka nke 1.5 G nke radieshon.
Anyị buru ụzọ mee mgbakọ ab initio iji chọta ụzọ nkewa nke FAPbI3 perovskite gaa na mgbanwe site na usoro α gaa na usoro δ. Site na usoro mgbanwe usoro zuru ezu, achọpụtara na mgbanwe site na octahedron nkekọrịta akụkụ atọ [PbI6] na usoro cubic α nke FAPbI3 gaa na octahedron nkekọrịta akụkụ otu akụkụ [PbI6] na usoro δ nke FAPbI3. gbajiri 9. Pb-I na-emepụta njikọ na nzọụkwụ mbụ (Int-1), ihe mgbochi ike ya na-erute 0.62 eV/cell, dịka egosiri na Foto 1a. Mgbe agbanwere octahedron na ntụziaka [0\(\bar{1}\)1], agbụ mkpụmkpụ hexagonal na-agbasa site na 1×1 ruo 1×3, 1×4 wee banye na usoro δ. Oke ntụzịaka nke ụzọ ahụ dum bụ (011)α//(001)δ + [100]α//[100]δ. Site na eserese nkesa ike, enwere ike ịchọpụta na mgbe nucleation nke usoro δ nke FAPbI3 gasịrị na usoro ndị a, ihe mgbochi ike dị ala karịa nke mgbanwe nke usoro α, nke pụtara na mgbanwe nke usoro ga-eme ngwa ngwa. O doro anya na nzọụkwụ mbụ nke ijikwa mgbanwe nke usoro dị oke mkpa ma ọ bụrụ na anyị chọrọ igbochi mmebi nke usoro α.
usoro mgbanwe usoro site n'aka ekpe gaa n'aka nri - usoro FAPbI3 ojii (α-phase), nke mbụ njikọ Pb-I (Int-1) na nke ọzọ njikọ Pb-I (Int-2, Int -3 na Int -4) na nke odo FAPbI3 (nke delta). b Ihe mgbochi ike na mgbanwe usoro α ruo δ nke FAPbI3 dabere na ọtụtụ ntụpọ isi dị n'ime. Ahịrị ntụpọ ahụ na-egosi ihe mgbochi ike nke kristal zuru oke (0.62 eV). c Ike nke nhazi ntụpọ isi ihe dị n'elu lead perovskite. Axis abscissa bụ ihe mgbochi ike nke mgbanwe usoro α-δ, axis ordinate bụkwa ike nke nhazi ntụpọ. Akụkụ ndị a na-acha ntụ ntụ, odo na akwụkwọ ndụ akwụkwọ ndụ bụ ụdị I (ala EB-elu FE), ụdị II (ala FE) na ụdị III (ala EB-ala FE), n'otu n'otu. d Ike nke nhazi ntụpọ VI na LOS nke FAPbI3 na njikwa. ihe mgbochi e I maka mbugharị ion na njikwa na LOS nke FAPbI3. f – ihe nnọchiteanya nke mbugharị nke ion I (ogwe oroma) na gLOS FAPbI3 (isi awọ, ndu; violet (oroma), iodine (ayodin mkpanaka)) na njikwa gf (aka ekpe: echiche elu; aka nri: ngalaba obe, aja aja); carbon; acha anụnụ anụnụ - nitrogen; ọbara ọbara - oxygen; pink pink - hydrogen). A na-enye data isi mmalite n'ụdị faịlụ data isi mmalite.
Anyị wee mụọ mmetụta nke ntụpọ isi ihe dị iche iche (gụnyere PbFA, IFA, PbI, na IPb antisite occupation; atọm interstitial Pbi na Ii; na VI, VFA, na VPb opens), nke a na-ewere dị ka ihe ndị dị mkpa. nke na-akpata mmebi nke usoro atọm na ike ka egosiri na Foto 1b na Tebụl Mgbakwunye 1. Ọ dị mma ịmara na ọ bụghị ntụpọ niile na-ebelata ihe mgbochi ike nke mgbanwe usoro α-δ (Foto 1b). Anyị kwenyere na ntụpọ ndị nwere ike nhazi dị ala na obere ihe mgbochi ike mgbanwe usoro α-δ ka a na-ewere dị ka ihe na-emerụ nkwụsi ike nke usoro. Dịka akọwara na mbụ, a na-ewere elu ndị bara ụba na lead dị ka ihe dị irè maka formamidine PSC27. Ya mere, anyị na-elekwasị anya na elu PbI2-akwụsị (100) n'okpuru ọnọdụ bara ụba na lead. Ike nhazi ntụpọ nke ntụpọ isi ihe dị n'elu dị na Foto 1c na Tebụl Mgbakwunye 1. Dabere na ihe mgbochi ike (EB) na ike nhazi usoro (FE), a na-ekewa ntụpọ ndị a n'ụdị atọ. Ụdị nke Mbụ (E nwere obere EB-FE dị elu): Ọ bụ ezie na IPb, VFA na VPb na-ebelata ihe mgbochi ike na mgbanwe nke usoro, ha nwere ike nhazi dị elu. Ya mere, anyị kwenyere na ụdị ntụpọ ndị a nwere obere mmetụta na mgbanwe nke usoro ebe ọ bụ na ha anaghị etolitekarị. Ụdị nke Abụọ (E nwere obere EB dị elu): N'ihi mmachi ike mgbanwe nke usoro nke α-δ, ntụpọ PbI, IFA na PbFA na-egbochi ebe ahụ anaghị emebi nkwụsi ike nke usoro nke α-FAPbI3 perovskite. Ụdị nke Atọ (E nwere obere EB-FE dị ala): Ntụpọ VI, Ii na Pbi nwere obere ike nhazi nwere ike ibute mmebi nke usoro ojii. Karịsịa ebe enyere FE na EB VI kacha ala, anyị kwenyere na atụmatụ kachasị dị irè bụ ibelata oghere I.
Iji belata VI, anyị mepụtara akwa dị oke arọ nke PbC2O4 iji melite elu FAPbI3. Ma e jiri ya tụnyere ihe ndị na-eme ka nnu halide dị na organic dị ka phenylethylammonium iodide (PEAI) na n-octylammonium iodide (OAI), PbC2O4, nke na-enweghị ion halogen na-agagharị agagharị, na-adịgide adịgide na kemịkalụ, anaghị agbaze na mmiri, ma na-agbanyụ ngwa ngwa mgbe mkpali gasịrị. Ezigbo nkwụsi ike nke mmiri dị n'elu na ubi eletriki nke perovskite. Mmiri nke PbC2O4 na mmiri bụ naanị 0.00065 g/L, nke dị ala karịa nke PbSO428. Ihe kacha mkpa bụ na enwere ike ịkwadebe akwa LOS dị oke ma dị otu na fim perovskite site na iji mmeghachi omume in situ (lee n'okpuru). Anyị mere ihe ngosi DFT nke njikọ dị n'etiti FAPbI3 na PbC2O4 dịka egosiri na Foto Mgbakwunye 1. Tebụl Mgbakwunye 2 na-egosi ike nhazi ntụpọ mgbe a gbanyere LOS. Anyị chọpụtara na LOS abụghị naanị na ọ na-eme ka ike nhazi nke ntụpọ VI dịkwuo elu site na 0.69–1.53 eV (Foto 1d), kamakwa ọ na-eme ka ike mkpali nke I dịkwuo elu na elu mbugharị na elu ọpụpụ (Foto 1e). Na ọkwa mbụ, ion I na-agagharị n'elu elu perovskite, na-ahapụ ion VI n'ọnọdụ lattice yana ihe mgbochi ike nke 0.61 eV. Mgbe ewebatara LOS, n'ihi mmetụta nke mgbochi steric, ike mkpali maka mbugharị nke ion I na-abawanye ruo. 1.28 eV. N'oge mbugharị nke ion I na-ahapụ elu perovskite, ihe mgbochi ike na VOC dịkwa elu karịa na ihe nlele njikwa (Foto 1e). E gosiri eserese atụmatụ nke ụzọ mbugharị ion I na njikwa na LOS FAPbI3 na Foto 1 f na g, n'otu n'otu. Nsonaazụ ihe nlereanya ahụ na-egosi na LOS nwere ike igbochi nhazi nke ntụpọ VI na mgbanwe nke I, si otú a gbochie mgbanwe nke α ruo δ nkebi.
A nwalere mmeghachi omume dị n'etiti oxalic acid na FAPbI3 perovskite. Mgbe agwakọtara ngwọta nke oxalic acid na FAPbI3, e mepụtara nnukwu ọnụọgụ ọcha, dịka egosiri na Foto Mgbakwunye 2. A chọpụtara ngwaahịa ntụ ntụ ahụ dị ka ihe PbC2O4 dị ọcha site na iji X-ray diffraction (XRD) (Foto Mgbakwunye 3) na Fourier transform infrared spectroscopy (FTIR) (Foto Mgbakwunye 4). Anyị chọpụtara na oxalic acid na-agbaze nke ukwuu na isopropyl alcohol (IPA) na okpomọkụ ụlọ yana mgbaze nke ihe dị ka 18 mg/mL, dịka egosiri na Foto Mgbakwunye 5. Nke a na-eme ka nhazi na-esote dị mfe ebe ọ bụ na IPA, dị ka ihe mgbaze passivation nkịtị, anaghị emebi oyi akwa perovskite karịa obere oge29. Ya mere, site n'itinye ihe nkiri perovskite n'ime mmiri oxalic acid ma ọ bụ site n'itinye ihe ngwọta oxalic acid n'ime perovskite, enwere ike nweta PbC2O4 dị gịrịgịrị ma dị oke n'elu ihe nkiri perovskite ngwa ngwa dịka usoro kemịkalụ ndị a si dị: H2C2O4 + FAPbI3 = PbC2O4 + FAI + HI. Enwere ike ịgbaze FAI na IPA ma wepụ ya n'oge esi nri. Enwere ike ijikwa ọkpụrụkpụ nke LOS site na oge mmeghachi omume na ntinye ihe tupu.
E gosiri onyonyo nyocha elektrọn microscopy (SEM) nke ihe nkiri njikwa na LOS perovskite na Foto 2a,b. Nsonaazụ ya na-egosi na a na-echekwa ọdịdị elu perovskite nke ọma, a na-etinyekwa ọtụtụ obere ihe dị n'elu elu ọka, nke kwesịrị ịnọchite anya oyi akwa PbC2O4 nke mmeghachi omume in-situ mepụtara. Ihe nkiri LOS perovskite nwere elu dị nro karịa (Foto mgbakwunye 6) na akụkụ kọntaktị mmiri buru ibu ma e jiri ya tụnyere ihe nkiri njikwa (Foto mgbakwunye 7). Ejiri igwe nyocha elektrọn transverse transmission dị elu (HR-TEM) chọpụta oyi akwa elu nke ngwaahịa ahụ. Ma e jiri ya tụnyere ihe nkiri njikwa (Foto 2c), a na-ahụ oyi akwa dị larịị ma dị oke arọ nke nwere ọkpụrụkpụ ihe dị ka 10 nm nke ọma n'elu LOS perovskite (Foto 2d). Site na iji igwe nyocha eletrọn gbara ọchịchịrị nke nwere akụkụ dị elu (HAADF-STEM) iji nyochaa njikọ dị n'etiti PbC2O4 na FAPbI3, enwere ike ịhụ ọnụnọ nke mpaghara kristal nke FAPbI3 na mpaghara amorphous nke PbC2O4 nke ọma (Foto mgbakwunye 8). Ejiri nha X-ray photoelectron spectroscopy (XPS) mara ihe mejupụtara elu nke perovskite mgbe ọgwụgwọ oxalic acid gasịrị, dịka egosiri na Foto 2e–g. Na Foto 2e, elu C 1s dị gburugburu 284.8 eV na 288.5 eV bụ nke akara CC na FA kpọmkwem, n'otu n'otu. Ma e jiri ya tụnyere akpụkpọ ahụ njikwa, akpụkpọ ahụ LOS gosipụtara elu ọzọ na 289.2 eV, nke a na-akpọ C2O42-. Ọkwa O1s nke LOS perovskite na-egosi oke O1s atọ dị iche na kemịkalụ na 531.7 eV, 532.5 eV, na 533.4 eV, nke kwekọrọ na COO deprotonated, C=O nke otu oxalate 30 na atọm O nke ihe mejupụtara OH (Foto 2e). )). Maka ihe nlele njikwa, naanị obere oke O1s ka a hụrụ, nke enwere ike ịkọwa na ọ bụ oxygen a na-etinye na chemisorb n'elu. Njirimara akpụkpọ ahụ njikwa nke Pb 4f7/2 na Pb 4f5/2 dị na 138.4 eV na 143.3 eV, n'otu n'otu. Anyị hụrụ na LOS perovskite na-egosipụta mgbanwe nke oke Pb nke ihe dị ka 0.15 eV gaa na ike njikọ dị elu, na-egosi mmekọrịta siri ike n'etiti atọm C2O42- na Pb (Foto 2g).
Foto SEM nke ihe nkiri njikwa na b LOS perovskite, ihe nkiri kachasị elu. c Igwe mmịpụta elektrọn nnyefe nke nwere mkpebi dị elu (HR-TEM) nke ihe nkiri njikwa na d LOS perovskite. XPS dị elu nke ihe nkiri e C 1s, f O 1s na g Pb 4f perovskite. A na-enye data isi mmalite n'ụdị faịlụ data isi mmalite.
Dịka nsonaazụ DFT si kwuo, a na-ebu amụma n'ụzọ echiche na ntụpọ VI na mbugharị I na-eme ka mgbanwe nke usoro ahụ dị mfe site na α gaa na δ. Akụkọ ndị gara aga egosila na a na-ewepụta I2 ngwa ngwa site na ihe nkiri perovskite nke PC n'oge fotomimmer mgbe ekpughere ihe nkiri ndị ahụ na nrụgide ọkụ31,32,33. Iji kwado mmetụta nke lead oxalate na α-phase nke perovskite, anyị mikpuru ihe nkiri njikwa na LOS perovskite n'ime karama iko doro anya nwere toluene, n'otu n'otu, wee jiri ìhè anyanwụ kpughee ha ruo awa 24. Anyị tụrụ nnabata nke ultraviolet na ìhè a na-ahụ anya (UV-Vis). ) toluene ngwọta, dịka egosiri na Foto 3a. Ma e jiri ya tụnyere ihe nlele njikwa, a hụrụ obere ike nnabata I2 n'ihe gbasara LOS-perovskite, na-egosi na obere LOS nwere ike igbochi ntọhapụ nke I2 na ihe nkiri perovskite n'oge mmịpụta ìhè. E gosipụtara foto nke ihe nkiri njikwa ochie na ihe nkiri LOS perovskite na ntinye nke Foto 3b na c. LOS perovskite ka bụ oji, ebe ọtụtụ ihe nkiri njikwa agbanweela odo odo. E gosiri spectra nnabata UV-a na-ahụ anya nke ihe nkiri a mikpuru na Fig. 3b, c. Anyị hụrụ na nnabata nke kwekọrọ na α dị na ihe nkiri njikwa ahụ belatara nke ọma. E mere nha X-ray iji dekọọ mmalite nke nhazi kristal ahụ. Mgbe awa 24 nke ìhè gasịrị, perovskite njikwa ahụ gosipụtara akara siri ike nke odo odo δ-phase (11.8°), ebe LOS perovskite ka nọgidere na-enwe ezigbo oge ojii (Foto 3d).
Ihe ngosiputa nke ihe ngwọta toluene a na-ahụ anya nke UV nke e tinyere ihe nkiri njikwa na ihe nkiri LOS n'okpuru otu ìhè anyanwụ ruo awa 24. Ihe ngosiputa nke ahụ na-egosi karama ebe e tinyere ihe nkiri ọ bụla n'ime olu toluene hà nhata. b Ihe ngosiputa nke ihe nkiri njikwa UV-Vis na ihe nkiri LOS tupu na mgbe awa 24 nke imikpu n'okpuru otu ìhè anyanwụ. Ihe ngosiputa nke ahụ na-egosi foto nke ihe nkiri nnwale ahụ. d Usoro mgbasa ozi X-ray nke njikwa na ihe nkiri LOS tupu na mgbe awa 24 nke ikpughe. Foto SEM nke ihe nkiri njikwa e na ihe nkiri f LOS mgbe awa 24 nke ikpughe. A na-enye data isi mmalite n'ụdị faịlụ data isi mmalite.
Anyị mere nyocha elektrọn mikroskopu (SEM) iji hụ mgbanwe microstructural nke ihe nkiri perovskite mgbe awa 24 nke ìhè gasịrị, dịka egosiri na Foto 3e,f. Na ihe nkiri njikwa, e bibiri nnukwu ọka ma gbanwee ha ka ha bụrụ obere agịga, nke kwekọrọ na nhazi nke ngwaahịa δ-phase FAPbI3 (Fig. 3e). Maka ihe nkiri LOS, mkpụrụ perovskite ka nọ n'ọnọdụ dị mma (Foto 3f). Nsonaazụ ahụ kwadoro na mfu nke I na-akpali mgbanwe site na oge ojii gaa na oge odo odo, ebe PbC2O4 na-eme ka oge ojii kwụsie ike, na-egbochi mfu nke I. Ebe ọ bụ na njupụta oghere dị n'elu dị elu karịa na nnukwu ọka,34 usoro a nwere ike ime na elu ọka. n'otu oge ahụ na-ewepụta iodine ma na-emepụta VI. Dịka DFT buru n'amụma, LOS nwere ike igbochi mmepụta nke ntụpọ VI ma gbochie mbugharị nke ion I gaa na elu perovskite.
Ọzọkwa, a mụrụ mmetụta nke oyi akwa PbC2O4 nwere na iguzogide mmiri nke ihe nkiri perovskite na ikuku ikuku (iru mmiri dị n'etiti 30-60%). Dịka egosiri na Foto Mgbakwunye 9, LOS perovskite ka dị oji mgbe ụbọchị iri na abụọ gachara, ebe ihe nkiri njikwa ahụ gbanwere odo odo. Na nha XRD, ihe nkiri njikwa ahụ na-egosi oke elu siri ike na 11.8° kwekọrọ na usoro δ nke FAPbI3, ebe LOS perovskite na-ejigide usoro α ojii nke ọma (Foto Mgbakwunye 10).
E jiri fotoluminescence steeti kwụsiri ike (PL) na photoluminescence edoziri oge (TRPL) mụọ mmetụta passivation nke lead oxalate na elu perovskite. Na Fig. Foto 4a na-egosi na ihe nkiri LOS amụbaala ike PL. Na onyonyo maapụ PL, ike nke ihe nkiri LOS n'ofe mpaghara niile nke 10 × 10 μm2 dị elu karịa nke ihe nkiri njikwa (Foto mgbakwunye 11), na-egosi na PbC2O4 na-eme ka ihe nkiri perovskite dịgide n'otu aka ahụ. A na-ekpebi ndụ onye na-ebu site na ime ka ire ere TRPL dị nso na otu ọrụ exponential (Foto 4b). Ndụ onye na-ebu nke ihe nkiri LOS bụ 5.2 μs, nke dị ogologo karịa ihe nkiri njikwa nwere ndụ onye na-ebu nke 0.9 μs, na-egosi mbelata njikọta elu na-abụghị redioaktivu.
PL kwụsiri ike na b-spectra nke PL nwa oge nke ihe nkiri perovskite na ihe ndị e ji iko mee. c SP curve nke ngwaọrụ ahụ (FTO/TiO2/SnO2/perovskite/spiro-OMeTAD/Au). d EQE spectrum na Jsc EQE spectrum agbakwunyere site na ngwaọrụ kachasị arụ ọrụ. d Ndabere nke ike ọkụ nke ngwaọrụ perovskite na eserese Voc. f Nyocha MKRC nkịtị site na iji ngwaọrụ oghere dị ọcha ITO/PEDOT:PSS/perovskite/PCBM/Au. VTFL bụ voltaji kachasị na-ejupụta ọnyà. Site na data ndị a, anyị gbakọrọ njupụta ọnyà (Nt). A na-enye data isi mmalite n'ụdị faịlụ data isi mmalite.
Iji mụọ mmetụta nke oyi akwa oxalate lead na arụmọrụ ngwaọrụ ahụ, ejiri usoro kọntaktị FTO/TiO2/SnO2/perovskite/spiro-OMeTAD/Au ọdịnala mee ihe. Anyị na-eji formamidine chloride (FACl) dị ka ihe mgbakwunye na precursor perovskite kama methylamine hydrochloride (MACl) iji nweta arụmọrụ ka mma nke ngwaọrụ ahụ, ebe FACl nwere ike inye mma kristal ka mma ma zere oghere band nke FAPbI335 (lee Foto Mgbakwunye 1 na 2 maka ntụnyere zuru ezu). 12-14). A họọrọ IPA dị ka ihe na-egbochi ihe mgbaze n'ihi na ọ na-enye mma kristal ka mma na ntụzịaka kachasị mma na fim perovskite ma e jiri ya tụnyere diethyl ether (DE) ma ọ bụ chlorobenzene (CB)36 (Foto Mgbakwunye 15 na 16). Ejiri nlezianya hazie ọkpụrụkpụ nke PbC2O4 iji hazie passivation ntụpọ na njem chajị site na ịhazi mkpokọta oxalic acid (Foto Mgbakwunye 17). E gosiri foto SEM nke ngwaọrụ njikwa kachasị mma na LOS na Foto Mgbakwunye 18. E gosiri usoro njupụta ugbu a (CD) maka ngwaọrụ njikwa na LOS na Foto 4c, a na-enyekwa paramita ewepụtara na Tebụl Mgbakwunye 3. Mkpụrụ ndụ njikwa kachasị arụmọrụ mgbanwe ike (PCE) 23.43% (22.94%), Jsc 25.75 mA cm-2 (25.74 mA cm-2), Voc 1.16 V (1.16 V) na nyocha azụ (n'ihu). Ihe na-ejupụta (FF) bụ 78.40% (76.69%). PCE LOS PSC kachasị bụ 25.39% (24.79%), Jsc bụ 25.77 mA cm-2, Voc bụ 1.18 V, FF bụ 83.50% (81.52%) site na azụ (Nyocha n'ihu gaa na). Ngwaọrụ LOS nwetara arụmọrụ fotovoltaic a kwadoro nke 24.92% n'ime ụlọ nyocha fotovoltaic nke ndị ọzọ a tụkwasịrị obi (Foto mgbakwunye 19). Arụmọrụ quantum mpụga (EQE) nyere Jsc agbakwunyere nke 24.90 mA cm-2 (njikwa) na 25.18 mA cm-2 (LOS PSC), n'otu n'otu, nke kwekọrọ na Jsc a tụrụ na ọkọlọtọ AM 1.5 G spectrum (Foto .4d). E gosiri nkesa ọnụọgụgụ nke PCE ndị a tụrụ maka njikwa na LOS PSCs na Foto mgbakwunye 20.
Dịka egosiri na Foto 4e, a gbakọrọ mmekọrịta dị n'etiti Voc na ike ọkụ iji mụọ mmetụta nke PbC2O4 na njikọta elu nke enyere aka na ọnyà. Mkpọda nke ahịrị etinyere maka ngwaọrụ LOS bụ 1.16 kBT/sq, nke dị ala karịa mkpọda nke ahịrị arụnyere maka ngwaọrụ njikwa (1.31 kBT/sq), na-akwado na LOS bara uru maka igbochi njikọta elu site na decoys. Anyị na-eji teknụzụ chaja oghere (SCLC) iji tụọ njupụta ntụpọ nke ihe nkiri perovskite n'ọtụtụ site na ịtụ njirimara IV gbara ọchịchịrị nke ngwaọrụ oghere (ITO/PEDOT:PSS/perovskite/spiro-OMeTAD/Au) dịka egosiri na eserese ahụ. 4f Gosi. A na-agbakọ njupụta ọnyà site na usoro Nt = 2ε0εVTFL/eL2, ebe ε bụ mgbanwe dielectric nke ihe nkiri perovskite, ε0 bụ mgbanwe dielectric nke ihe mkpofu, VTFL bụ voltaji na-egbochi iji mejupụta ọnyà ahụ, e bụ chajị, L bụ ọkpụrụkpụ nke ihe nkiri perovskite (650 nm). A na-agbakọ njupụta ntụpọ nke ngwaọrụ VOC ka ọ bụrụ 1.450 × 1015 cm–3, nke dị ala karịa njupụta ntụpọ nke ngwaọrụ njikwa, nke bụ 1.795 × 1015 cm–3.
A nwalere ngwaọrụ a na-ekpuchighị na ebe kachasị ike (MPP) n'okpuru nitrogen zuru oke iji lelee nkwụsi ike arụmọrụ ogologo oge ya (Foto 5a). Mgbe awa 550 gachara, ngwaọrụ LOS ka nọgidere na-enwe 92% nke arụmọrụ kachasị elu ya, ebe arụmọrụ ngwaọrụ njikwa adalatala ruo 60% nke arụmọrụ mbụ ya. A tụrụ nkesa nke ihe dị na ngwaọrụ ochie site na oge nke-efe efe ion mass spectrometry (ToF-SIMS) (Foto 5b, c). Enwere ike ịhụ nnukwu mkpokọta iodine na mpaghara njikwa ọlaedo elu. Ọnọdụ nke nchekwa gas inert anaghị ewepụ ihe ndị na-emebi gburugburu ebe obibi dị ka mmiri na oxygen, na-egosi na usoro dị n'ime (ya bụ, mbugharị ion) bụ ihe kpatara ya. Dịka nsonaazụ ToF-SIMS si kwuo, achọpụtara I- na AuI2- ions na electrode Au, na-egosi mgbasa nke I site na perovskite gaa na Au. Ike mgbaàmà nke I- na AuI2- ions na ngwaọrụ njikwa dị ihe dị ka ugboro 10 karịa nke ihe nlele VOC. Akụkọ ndị gara aga egosila na mpụta ion nwere ike ibute mbelata ngwa ngwa na njikwa oghere nke spiro-OMeTAD na ire ere kemịkalụ nke oyi akwa elektrọd dị n'elu, si otú a na-emebi njikọ interfacial dị na ngwaọrụ ahụ37,38. E wepụrụ elektrọd Au ma jiri mmiri chlorobenzene sachaa oyi akwa spiro-OMeTAD site na substrate ahụ. Anyị wee kọwaa ihe nkiri ahụ site na iji grazing incidence X-ray diffraction (GIXRD) (Foto 5d). Nsonaazụ ya na-egosi na ihe nkiri njikwa ahụ nwere oke diffraction doro anya na 11.8°, ebe ọ dịghị oke diffraction ọhụrụ pụtara na ihe nlele LOS. Nsonaazụ ya na-egosi na nnukwu mfu nke ion I na ihe nkiri njikwa na-eduga na mmepụta nke δ phase, ebe na fim LOS a na-egbochi usoro a nke ọma.
Awa 575 nke nledo MPP na-aga n'ihu nke ngwaọrụ a na-emechighị emechi n'ime ikuku nitrogen na otu anwụ na-enweghị nzacha UV. Nkesa ToF-SIM nke b I- na c AuI2- ions na ngwaọrụ njikwa LOS MPP na ngwaọrụ ịka nká. Agba odo, akwụkwọ ndụ akwụkwọ ndụ na oroma kwekọrọ na Au, Spiro-OMeTAD na perovskite. d GIXRD nke ihe nkiri perovskite mgbe ule MPP gasịrị. A na-enye data isi mmalite n'ụdị faịlụ data isi mmalite.
A tụrụ njikwa dabere na okpomọkụ iji gosi na PbC2O4 nwere ike igbochi mbugharị ion (Foto mgbakwunye 21). A na-ekpebi ike mkpali (Ea) nke mbugharị ion site na ịtụ mgbanwe na njikwa (σ) nke ihe nkiri FAPbI3 na okpomọkụ dị iche iche (T) na iji mmekọrịta Nernst-Einstein: σT = σ0exp(−Ea/kBT), ebe σ0 bụ mgbanwe, kB bụ mgbanwe Boltzmann. Anyị na-enweta uru nke Ea site na mkpọda nke ln(σT) megide 1/T, nke bụ 0.283 eV maka njikwa na 0.419 eV maka ngwaọrụ LOS.
Na nchịkọta, anyị na-enye usoro echiche iji chọpụta ụzọ mmebi nke FAPbI3 perovskite na mmetụta nke ntụpọ dị iche iche na ihe mgbochi ike nke mgbanwe usoro α-δ. N'ime ntụpọ ndị a, a na-atụ anya na ntụpọ VI ga-eme ka mgbanwe usoro dị mfe site na α gaa na δ. A na-ewebata oyi akwa dị oke mmiri nke PbC2O4 nke na-anaghị agbaze mmiri ma kwụsie ike nke kemịkalụ iji mee ka α-phase nke FAPbI3 guzosie ike site na igbochi nhazi nke oghere I na mbugharị nke ions I. Usoro a na-ebelata njikọta interfacial na-abụghị radiative nke ukwuu, na-eme ka arụmọrụ nke mkpụrụ ndụ anyanwụ dịkwuo elu ruo 25.39%, ma na-eme ka nkwụsi ike ọrụ ka mma. Nsonaazụ anyị na-enye nduzi maka iru PSC formamidine dị irè ma kwụsie ike site na igbochi mgbanwe usoro α gaa na δ nke ntụpọ kpatara.
A zụtara titanium(IV) isopropoxide (TTIP, 99.999%) site na Sigma-Aldrich. A zụtara Hydrochloric acid (HCl, 35.0–37.0%) na ethanol (anhydrous) site na Guangzhou Chemical Industry. A zụtara SnO2 (15 wt% tin(IV) oxide colloidal dispersion) site na Alfa Aesar. A zụtara Lead(II) iodide (PbI2, 99.99%) site na TCI Shanghai (China). A zụtara Formamidine iodide (FAI, ≥99.5%), formamidine chloride (FACl, ≥99.5%), methylamine hydrochloride (MACl, ≥99.5%), 2,2′,7,7′-tetrakis-(N, N-di-p) )-methoxyaniline)-9,9′-spirobifluorene (Spiro-OMeTAD, ≥99.5%), lithium bis(trifluoromethane)sulfonylamide (Li-TFSI, 99.95%), 4-tert-butylpyridine (tBP, 96%) site na Xi'an Polymer Light Technology Company (China). N,N-dimethylformamide (DMF, 99.8%), dimethyl sulfoxide (DMSO, 99.9%), isopropyl alcohol (IPA, 99.8%), chlorobenzene (CB, 99.8%), acetonitrile (ACN). A zụtara ya na Sigma-Aldrich. A zụtara Oxalic acid (H2C2O4, 99.9%) na Macklin. E jiri kemịkalụ niile dịka e si nweta ha na-enweghị mgbanwe ọ bụla ọzọ.
E jiri ihe nhicha, acetone, na ethanol hichaa ihe ndị dị n'ime ITO ma ọ bụ FTO (1.5 × 1.5 cm2) n'ụzọ ultrasonic, wee kpọọ nkụ n'okpuru iyi nitrogen. E tinyere ihe mkpuchi TiO2 dị oke njọ n'elu ihe mkpuchi FTO site na iji ihe ngwọta titanium diisopropoxybis (acetylacetonate) na ethanol (1/25, v/v) nke e tinyere na 500 °C maka nkeji iri isii. E jiri mmiri deionized gbasaa SnO2 colloidal na oke olu nke 1:5. N'elu ihe dị ọcha e ji UV ozone gwọọ maka nkeji iri abụọ, e tinyere ihe mkpuchi SnO2 na 4000 rpm maka sekọnd iri atọ wee kpoo ọkụ na 150 °C maka nkeji iri atọ. Maka ihe ngwọta perovskite precursor, a gbazere 275.2 mg FAI, 737.6 mg PbI2 na FACl (20 mol%) na ihe mgbaze agwakọtara DMF/DMSO (15/1). A kwadebere oyi akwa perovskite site n'itinye 40 μL nke ihe ngwọta perovskite precursor n'elu oyi akwa SnO2 nke UV-ozone gwọchara na 5000 rpm n'ime ikuku gburugburu maka sekọnd 25. Sekọnd 5 mgbe oge ikpeazụ gasịrị, a tụbara 50 μL nke ihe ngwọta MACl IPA (4 mg/mL) ngwa ngwa n'elu ihe mkpuchi ahụ dị ka ihe na-egbochi ihe mgbaze. Mgbe ahụ, a na-ewepụ ihe nkiri ndị a kwadebere ọhụrụ na 150°C maka nkeji 20 wee na 100°C maka nkeji 10. Mgbe emechara ka ihe nkiri perovskite dị jụụ ruo okpomọkụ ụlọ, a na-etinye ihe ngwọta H2C2O4 (1, 2, 4 mg agbazere na 1 mL IPA) na 4000 rpm maka sekọnd 30 iji mee ka elu perovskite dịgide. A na-eji ngwakọta spiro-OMeTAD nke e ji agwakọta spiro-OMeTAD 72.3 mg, CB 1 ml, 27 µl tBP na 17.5 µl Li-TFSI (520 mg na 1 ml acetonitrile) kpuchie ihe nkiri ahụ na 4000 rpm n'ime s30. N'ikpeazụ, a kpọnwụrụ oyi akwa Au dị 100 nm n'ime oghere ikuku na ọnụego nke 0.05 nm/s (0~1 nm), 0.1 nm/s (2~15 nm) na 0.5 nm/s (16~100 nm).
A tụrụ arụmọrụ SC nke mkpụrụ ndụ anyanwụ perovskite site na iji Keithley 2400 mita n'okpuru ọkụ simulator anyanwụ (SS-X50) na ike ọkụ nke 100 mW/cm2 ma nyochaa ya site na iji mkpụrụ ndụ anyanwụ silicon ọkọlọtọ a na-ahazi. Ọ gwụla ma e kwuru ihe ọzọ, a tụrụ usoro SP n'ime igbe uwe aka jupụtara na nitrogen na okpomọkụ ụlọ (~25°C) na ụdị nyocha ihu na azụ (nzọụkwụ voltaji 20 mV, oge igbu oge 10 ms). E jiri ihe mkpuchi onyinyo chọpụta mpaghara dị irè nke 0.067 cm2 maka PSC a tụrụ. E mere nha EQE na ikuku gburugburu site na iji sistemụ PVE300-IVT210 (Industrial Vision Technology(s) Pte Ltd) yana ìhè monochromatic lekwasịrị anya na ngwaọrụ ahụ. Maka nkwụsi ike ngwaọrụ, e mere nnwale nke mkpụrụ ndụ anyanwụ na-abụghị nke e ji ihe kpuchie na igbe uwe nitrogen na nrụgide 100 mW/cm2 na-enweghị nzacha UV. A na-eji SIMS oge PHI nanoTOFII tụọ ToF-SIMS. E ji egbe ion Ar nke dị kV 4 kV nke nwere mpaghara 400 × 400 µm nweta nyocha omimi nke profaịlụ.
E mere nha fotoelectron spectroscopy (XPS) na sistemụ Thermo-VG Scientific (ESCALAB 250) site na iji monochromatized Al Kα (maka ụdị XPS) na nrụgide nke 5.0 × 10–7 Pa. E mere nyocha elektrọn microscopy (SEM) na sistemụ JEOL-JSM-6330F. E jiri atomik force microscopy (AFM) (Bruker Dimension FastScan) tụọ ọdịdị elu na ịdị njọ nke ihe nkiri perovskite. A na-ejide STEM na HAADF-STEM na FEI Titan Themis STEM. E jiri UV-3600Plus (Shimadzu Corporation) tụọ spectra absorption UV-Vis. E dekọrọ ugbu a na-egbochi chaja oghere (SCLC) na mita Keithley 2400. E jiri FLS 1000 photoluminescence spectroscopy tụọ stady-state photoluminescence (PL) na oge edoziri photoluminescence (TRPL) nke ire ere ndụ onye na-ebu ibu. E jiri usoro Horiba LabRam Raman HR Evolution tụọ onyonyo nke eserese PL. E jiri usoro Thermo-Fisher Nicolet NXR 9650 mee Fourier transform infrared spectroscopy (FTIR).
N'ọrụ a, anyị na-eji usoro nlele ụzọ SSW iji mụọ ụzọ mgbanwe nke usoro site na α-phase gaa na δ-phase. Na usoro SSW, a na-ekpebi mmegharị nke elu ike nwere ike site na ntụziaka nke ọnọdụ dị nro na-enweghị usoro (nke abụọ mepụtara), nke na-enye ohere ka a mụọ ihe zuru ezu na nke ebumnuche nke elu ike nwere ike. N'ọrụ a, a na-eme nlele ụzọ na supercell 72-atom, a na-anakọtakwa ihe karịrị ụzọ mbụ/ikpeazụ 100 (IS/FS) na ọkwa DFT. Dabere na ntọala data IS/FS, enwere ike ịchọpụta ụzọ jikọtara nhazi mbụ na nhazi ikpeazụ site na mmekorita dị n'etiti atọm, wee jiri mmegharị ụzọ abụọ n'elu elu nkeji mgbanwe chọpụta usoro ọnọdụ mgbanwe nke ọma. (VK-DESV). Mgbe ịchọchara ọnọdụ mgbanwe, enwere ike ikpebi ụzọ nwere ihe mgbochi kachasị ala site na ịhazi ihe mgbochi ike.
E ji VASP (ụdị 5.3.5) mee mgbakọ DFT niile, ebe a na-egosi mmekọrịta elektrọn-ion nke atọm C, N, H, Pb, na I site na atụmatụ ebili mmiri amplified (PAW). A kọwara ọrụ njikọ mgbanwe site na ihe dị ka gradient zuru oke na parametrization Perdue-Burke-Ernzerhoff. E debere oke ike maka ebili mmiri ụgbọelu na 400 eV. Grid k-point Monkhorst-Pack nwere nha (2 × 2 × 1). Maka nhazi niile, e mere ka ọnọdụ lattice na atọm ka mma ruo mgbe akụkụ nrụgide kachasị dị n'okpuru 0.1 GPa na akụkụ ike kachasị dị n'okpuru 0.02 eV/Å. Na ụdị elu, elu nke FAPbI3 nwere akwa 4, akwa ala nwere atọm edoziri edozi nke na-eme ka ahụ FAPbI3 dị ka ahụ, akwa atọ kachasị elu nwekwara ike ịkwaga n'enweghị nsogbu n'oge usoro nhazi. Oyi akwa PbC2O4 dị 1 ML n'ọkpụrụkpụ ma dị n'elu I-terminal nke FAPbI3, ebe Pb na-ejikọta na 1 I na 4 O.
Maka ozi ndị ọzọ gbasara nhazi ọmụmụ ihe a, lee Nchịkọta Akụkọ Nchịkọta Ihe Okike nke metụtara akụkọ a.
A na-etinye data niile e nwetara ma ọ bụ nyochaa n'oge ọmụmụ ihe a n'isiokwu ebipụtara, yana n'ime ozi nkwado na faịlụ data raw. Data raw ewepụtara n'ọmụmụ ihe a dị na https://doi.org/10.6084/m9.figshare.2410016440. E nyere data isi mmalite maka edemede a.
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