High-performance large-area blade-coated perovskite solar cells with low ohmic loss for low lighting indoor applications

High-pe o mance la ge-a ea blade-coa ed pe o ski e sola cells wi h low ohmic loss o low ligh ing indoo applica ions Zhuoneng Bi,1,2 Xueqing Xu,1,2* Xia Chen,1 Yanqing Zhu,1 Chang Liu, 3 Hua Yu, 3* Yupeng Zheng,1,2 Pa el A. T oshin,4,5 An onio Gue e o, 6 Gang Xu1,2 1 Key Labo a o y o Renewable Ene gy, Guangdong Key Labo a o y o New and Renewable Ene gy Resea ch and De elopmen , Guangzhou Ins i u e o Ene gy Con e sion, Chinese Academy o Sciences, Guangzhou 510640, China 2 Cen e o Ma e ials Science and Op oelec onics Enginee ing, Uni e si y o Chinese Academy o Sciences, Beijing 100049, China 3 Ins i u e o Pho o ol aics, Sou hwes Pe oleum Uni e si y, Chengdu 610500, P. R. China 4 Silesian Uni e si y o Technology, Akademicka 2A, 44-100 Gliwice, Poland 5 Ins i u e o P oblems o Chemical Physics o he Russian Academy o Sciences (IPCP RAS), Academician Semeno a enue 1, Che nogolo ka, Moscow egion, 142432 Russian Fede a ion 6 Ins i u e o Ad anced Ma e ials (INAM), Uni e si a Jaume I, 12006 Cas elló, Spain * Co esponding au ho email: [email protected], [email p o ec ed]m Abs ac Eme ging hyb id o ganic-ino ganic pe o ski es wi h supe io op oelec onic p ope y demons a e p omising p ospec o pho o ol aic applica ions, in pa icula o low-ligh ing indoo applica ions e.g. wi hin in e ne o hings (IoT) ne wo ks o low- ene gy wi eless communica ion de ices. In o de o p epa e de ices wi h high powe ou pu unde low-illumina ion condi ions, scalable ab ica ion echniques a e p e e ed o la ge-a ea pe o ski e sola cells. In addi ion, one o he key pa ame e s o achie e high-e iciency la ge-a ea pe o ski e sola cells is o minimize he ohmic loss o u he boos he sola cell e iciency. He ein, a one-s ep blade-coa ing me hod assis ed by hexa luo obenzene (HFB) was de eloped o deposi la ge-a ea smoo h and de ec - ee pe o ski e ilms wi h low ohmic loss. The as- ab ica ed de ices demons a ed powe con e sion e iciency (PCE) o 20.7% (a ea o 0.2 cm2) and 16.5% (1 cm2), espec i ely, unde s anda d 1000 mW/cm2 (AM1.5G) illumina ion condi ions. Besides, he la ge-a ea (1 cm2) de ices demons a ed a ema kable PCE o ~32% unde 0.1 mW/cm2 (~285 lux) illumina ion p o ided by whi e ligh -emi ing diode (LED) lamp o indoo ligh ing which s ongly indica e ha he ab ica ed la ge-a ea de ices exhibi ed p ac ical applica ions o be used in he as majo i y o low-ligh ing indoo condi ions (≥100 lux). The analysis using a single diode model sugges s ha he high pe o mance o he la ge-a ea de ices unde low-ligh ing indoo condi ions is highly associa ed wi h he la gely educed ohmic losses o he pe o ski e ilms by a acile and scalable blade-coa ing me hod. The ohmic loss o he 1 cm2 de ice was es ima ed as low as 1.66% a ~285 lux. The p esen ed scalable app oach pa es he way o designing high-pe o mance pe o ski e sola cells o a a ie y o eme ging indoo PV applica ions. Keywo ds: pe o ski e sola cells, blade-coa ing, la ge a ea, low-ligh ing indoo applica ions, ohmic loss In oduc ion Hyb id o ganic-ino ganic pe o ski e sola cells (PSCs) ha e been demons a ed o be one o he mos p omising candida es o he nex gene a ion pho o ol aics due o hei high powe con e sion e iciency (PCE) and low ma e ials and ab ica ion cos 1, 2. PSCs ha e e sa ile p omising applica ions in po able elec onics, such as emo e ene gy-independen senso s o he in e ne o hings ne wo ks, o low-ene gy wi eless communica ion de ices 3-5. Mos o hese de ices need o wo k con inuously unde low indoo illumina ion condi ions (100 ~ 1000 lux) 5. Low-ligh ing indoo pho o ol aics has a e y high demand in he cu en and u u e powe -supply ma ke 4. Hence, he low-ligh ing indoo pe o ski e pho o ol aics ha e ecen ly eme ged as one o he p omising and p ac ical echnology o indoo powe supply 6-11. O ganic-ino ganic pe o ski e abso be ma e ials is one o he ideal candida es o indoo pho o ol aics since hei abso p ion spec a pe ec ly ma ch he emission spec a o LED o luo escen lamps (400 - 800 nm) 12. Recen ly, Liu e al. achie ed an imp essi e PCE o 40.1% unde indoo illumina ion condi ions (824.5 lux) o he pe o ski e sola cell wi h a small ac i e a ea o 0.08 cm2 12. The e a e also mul iple o he epo s on small-a ea PSCs deli e ing PCEs o 30 – 40% unde indoo condi ions. Howe e , he small a ea de ice is no p ac ically o comme cializa ion use and he de elopmen o la ge-a ea indoo PSCs is impeded by la ge ohmic loss. Feng e al. ha e epo ed one o he highes eco ds o da e o la ge-a ea de ices (2.25 cm2) demons a ing excellen PCE o 30.6% unde indoo condi ion (1000 lux)13. Gene ally, he e a e wo popula app oaches o imp o e PCE o PSCs unde indoo illumina ion condi ions. The i s app oach equi es he de ices achie ing high shun esis ance (Rsh), which can e ec i ely minimize ohmic losses unde low-ligh condi ions 14-16. In e ace modi ica ion is a common s a egy o ob ain high shun esis ance de ices 6, 14. The o he app oach is based on supp essing he cha ge ca ie ecombina ion losses, which is mani es ed in he diode ideali y ac o s (n) close o 1 10. The ideali y ac n can be es ima ed om he dependence o he open-ci cui ol age (VOC) on he inciden ligh in ensi y 13. Achie ing good ideali y ac o s equi es supp essing ap-assis ed ecombina ion wi hin he de ice. The passi a ion o aps and de ec s in he pe o ski e ilms is an e ec i e way o educe VOC losses 12. Fo po en ial p ac ical applica ions, low-ligh ing pe o ski e sola cells should be p oduced using scalable echniques compa ible wi h he oll- o- oll p ocess. Howe e , mos o he pe o ski e ilms epo ed so a p epa ed by non-scalable me hods such as spin-coa ing. To da e, la ge-a ea deposi ion me hods emain insu icien ly in es iga ed. The i s epo s on blade-coa ing we e published in 2015, and p esen ed PSCs wi h he PCEs o 11-15% p oduced using DMF as a sol en 17, 18. Mo e ecen ly, meniscus- assis ed echnique p oduced la ge-g ain pe o ski e ilms, which boos ed he de ice e iciency up o 20% (using DMSO as a sol en ) 19. Sol en mix u es o DMSO and gamma-bu y olac one (GBL) we e p e iously used o ab ica e PSCs wi h he PCE o abou 18% 20, 21. Fu he de elopmen o he blade-coa ing echniques o PSCs ab ica ion is commonly conside ed as one o he mos p omising s eps owa ds la ge- scale comme cial applica ions o PSCs 2, 22-25. In his wo k, we p esen a one-s ep blade-coa ing assis ed by HFB app oach o deposi high-quali y de ec - ee pe o ski e ilms o indoo pe o ski e pho o ol aics. The p oposed me hod p oduces highly c ys alline pe o ski e ilms in a single s ep by using enginee ed inks based on a low inhala ion oxic sol en mix u e o DMSO, GBL and HFB. The p ehea ing o he p ecu so ink enables comple e dissolu ion o PbI2 and MAI in he mixed sol en close o he solubili y limi . I is ound ha he HFB addi i e e ec i ely smoo hs down he pe o ski e ilms and passi a e he de ec s, hus, he as- ab ica ed de ices demons a e high powe con e sion e iciency (PCE) o 20.7% on a small a ea o 0.2 cm2 and 16.5% on he a ea o 1 cm2 unde s anda d 1 sun (AM1.5G) illumina ion condi ions. Fu he mo e, he la ge-a ea (1 cm2) de ices deli e a ema kable PCE o ~32% unde 0.1 mW/cm2 (~285 lux) illumina ion p o ided by ligh - emi ing diode (LED) lamp. Resul s and discussion Figu e 1. a) Schema ic diag am o he HFB-assis ed one-s ep blade-coa ing me hod o p oduce high-quali y de ec - ee MAPbI3 ilm. b) Pho og aphs o MAPbI3 p ecu so solu ions wi h and wi hou HFB a oom empe a u e and a 70 oC. Figu e 1a shows he schema ic diag am o he blade-coa ing se up o p oduce MAPbI3 pe o ski e ilms. In he expe imen al p ocess he subs a e is ixed on a ho pla e wi h a blade se abo e he subs a e o ming he sli o a ound 100 m. The pe o ski e p ecu so ink is injec ed in o he sli and he p e-hea ing blade immedia ely mo es ho izon ally on he hea ing subs a e. Wi h he sol en e apo a ing, he black pe o ski e ilm o ms in a couple o seconds. The one-s ep blade coa ing p ocess is e y simple and adap s o di e en p ocess a ia ions. In addi ion, o u he imp o e he quali y o pe o ski e ilms on his one-s ep blade coa ing app oach he sol en may be easily modi ied. In pa icula we obse e ha he use o a co-sol en HFB in he pe o ski e p ecu so is bene icial o he ilm quali y. Fu he de ails o he one-s ep blade-coa ing p ocess a e gi en in he expe imen al sec ion. Figu e 2. a, d) AFM images o he Con ol and HFB 15% MAPbI3 ilms. b, e) Top- iew and c, ) c oss-sec ion SEM images o he Con ol HFB 15% samples. Figu e 1b shows a image o he e e ence p ecu so solu ion and he modi ied ink loaded wi h HFB addi i e. HFB is a low inhala ion oxic o ganic sol en ha is commonly used in medicine 26. HFB is immiscible wi h wa e , bu i can be miscible wi h DMSO in a ce ain p opo ion 27. A oom empe a u e, pe o ski e inks wi h HFB addi i e a e non- anspa en , which indica es incomple e ma e ial solubiliza ion bu o he p esence o a bad sol en (o an i-sol en ) such as HFB. Howe e , p ehea ing he p ecu so solu ion a 70 oC esul s in comple e solubiliza ion o PbI2 and MAI and o ma ion o anspa en solu ion wi h ma e ial concen a ions close o he solubili y limi leading o sa u a ed solu ions. Figu e S1 shows he scanning elec on mic oscopy (SEM) images o he MAPbI3 ilms p epa ed om he inks wi h di e en HFB loadings and ma ked as Con ol (co esponds o HFB 0%), HFB 5%, HFB 10%, and HFB 15%. All samples exhibi sphe uli ic g ow h and la ge gain size wi h no oids o pinholes. The Con ol and HFB 15% samples display ob ious di e ence be ween as illus a ed by he SEM images shown in Figu es 2b and 2e. The HFB 15% sample exhibi s a la and uni o m c ys alline g ain su ace, whe eas he Con ol sample has wa y su ace mo phology. The su ace opog aphy o he ilms was u he s udied by a omic o ce mic oscopy (AFM) as shown in Figu e 2a and 2d. The oo -mean-squa e oughness alues o he Con ol and HFB 15% samples we e de e mined as 28.1 and 20.5 nm, espec i ely, which is consis en wi h he SEM images. The c oss-sec ion SEM images (Figu es 2c, 2 and S2) e eal he a e age hickness o pe o ski e ilms as ~415 nm and ~438 nm o Con ol and HFB 15% samples, espec i ely. I is wo h no ing ha he HFB 15% sample shows a mo e uni o m s uc u e and hickness o he pe o ski e ilm. Figu e 3. Cha ac e iza ion o he MAPbI3 ilms wi h di e en HFB loadings on he glass/FTO/SnO2-PbO/SnO2 subs a es. a) XRD di ac ion pa e ns. b) UV- is abso p ion spec a. c) S eady-s a e PL spec a. d) Time- esol ed PL (TRPL) p o iles. The e ec o he HFB addi i e on he s uc u al and op ical p ope ies o pe o ski e ilms is illus a ed in Figu e 3a and Figu e 3b, espec i ely. All samples show simila peaks on he x- ay di ac ion (XRD) pa e ns, indica ing a high phase pu i y o he pe o ski es. The di ac ion peaks a 14.12˚ 20.02˚ 28.46˚ 31.90˚ and 40.70˚ can be assigned o (110), (112), (220), (310), and (224) c ys al planes o he e agonal MAPbI3 pe o ski e la ice, espec i ely 18. The sha p and in ense (112) di ac ion peaks indica e a highly o ien ed c ys al s uc u e o he ilms. In e es ingly, he addi ion o HFB inc eases he in ensi y o (110) peaks, sugges ing imp o ed ilm c ys alliza ion. The abso p ion spec a become signi ican ly s onge wi h inc easing he HFB loading om 0% o 15%. We belie e ha he uni o m hickness o HFB-p ocessed ilms helps o a oid abso p ion losses, while in he case o Con ol samples some ligh passes h ough he oids o deep alleys in he ilms. Thus, he ob ained esul s e eal ha HFB can no only make he pe o ski e ilms mo e uni o m bu also al e he c ys al g ow h and enhance ilm abso bance. Figu es 3c and 3d show s eady-s a e pho oluminescence (PL) and ime- esol ed pho oluminescence (TRPL) spec a. The PL peaks o he HFB p ocessed sample a e ed-shi ed compa ed o ha o he Con ol sample and he magni ude o he ed-shi is p opo ional o he HFB loading wi h a ~7 nm peak shi o he HFB 15% sample. Fu he mo e, a ed-shi o he low-ene gy abso p ion onse was obse ed, which in combina ion wi h PL da a implies ha he HFB-p ocessed samples ha e a sligh ly lowe bandgap as compa ed o he Con ol, which could be a consequence o he enhanced ma e ial c ys allini y. The cha ge ca ie li e imes in he HFB-p ocessed samples we e conside ably longe han ha o he Con ol (  1= 36.0 ns and  2= 73.7 ns) sample and he li e ime inc ease was p opo ional wi h he HFB loading. In pa icula , he HFB 15% sample showed almos wice longe li e imes (  1 = 52.7 ns and  2= 122.8 ns) as compa ed o he Con ol sample, which e idences ha HFB addi i e e ec i ely supp esses ap-assis ed ca ie ecombina ion due o he o ma ion o high-quali y pe o ski e g ains wi h a low densi y o de ec s. Fab ica ion and cha ac e iza ion o pho o ol aic de ices Figu e 4. a) J-V cu es measu ed unde s anda d 100 mW cm-2 AM1.5G simula ed illumina ion condi ions. b) EQE spec a o he de ices. c) S a is ics o 20 Con ol and 20 HFB 15% de ices. d) S abilized ou pu measu emen s in he maximum powe poin acking egime unde he s anda d illumina ion condi ions. Pho o ol aic de ices we e ab ica ed wi h de ice a chi ec u e o Glass/FTO/SnO2- PbO/SnO2/MAPbI3/Spi o-OMeTAD/Au. The MAPbI3 ilms we e p epa ed wi h di e en HFB loadings in he p ecu so ink, which a e ma ked as Con ol, HFB 5%, HFB 10%, and HFB 15% samples. Fu he de ails on he de ice ab ica ion can be ound in he Expe imen al sec ion. I is wo h men ioning ha he deposi ion o MAPbI3 by he de eloped one-s ep blade coa ing me hod does no equi e any addi ional s eps such as sol en annealing o an i-sol en ba h, e c. The ep esen a i e J-V cu es measu ed unde he simula ed 1 sun illumina ion condi ions a e p esen ed in Figu e 4a, whe eas he co esponding de ice pa ame e s a e summa ized in Table S1. The Con ol de ices show PCE exceeding 17%, which is in good ag eemen wi h he p e iously epo ed cha ac e is ics o he MAPbI3 de ices ab ica ed in d y box condi ions wi h a ela i e humidi y be ween 10% o 20%. Howe e , inc easing o HFB amoun in he ink imp o es he pho o ol aic pe o mance o he de ices p ocessed unde he same condi ions. Using he op imal amoun o HFB (15%), he champion cells wi h a PCE o 20.7%, open-ci cui ol age VOC o 1.13 V, sho -ci cui cu en densi y JSC o 23.4 mA/cm2, and ill ac o FF o 78.4% was achie ed. The s abilized ou pu measu emen s o he PCE and pho ocu en densi y o he champion cell deli e ed he alues o 19.8% and 21.9 mA/cm2, espec i ely (Figu e 4d). The ob ained pho ocu en densi y is in good ag eemen wi h he in eg a ed JSC ex ac ed om he EQE spec um by i s in eg a ion o e he e e ence sola AM1.5G spec um (Figu e 4b). The s a is ics o 20 de ices o each ype (Figu e 4c) show a ema kable imp o emen in a e age PCE om 16.6% o 19.1% when HFB is inco po a ed in o he p ecu so inks. Fu he mo e, i was su p ising ha HFB addi i e also imp o es he en i onmen al s abili y o he de ices as shown in Figu e S4. Thus, HFB could be conside ed as a highly p omising co-sol en o pe o ski e inks and p ocessing addi i e imp o ing simul aneously he e iciency and s abili y o PSCs. Design and cha ac e iza ion o la ge-a ea PSCs o low ligh ing indoo applica ions Figu e 5. a) J-V cu e o he ab ica ed de ice wi h an ac i e a ea o 1 cm2 measu ed unde simula ed 1 sun illumina ion condi ions. b) The linea dependences o -dV/dJ s. (JSC-J)-1 o de ices wi h di e en ac i e a ea sizes c) J-V cu es o 1 cm2 cell measu ed unde di e en illumina ion in ensi ies p o ided by whi e-ligh LED. C) J-V cu e unde 0.1 mW/cm2 (~285 lux) whi e LED. e) J-V cu es measu ed in he da k o de ices wi h di e en ac i e a ea sizes; inse shows he es ima ion o Rsh alues. ) VOC plo as a unc ion o illuminance o he calcula ion o ideali y ac o . 9. Di Giacomo, F.; Za de o, V.; Luca elli, G.; Cina, L.; Di Ca lo, A.; C ea o e, M.; B own, T. M., Mesopo ous pe o ski e sola cells and he ole o nanoscale compac laye s o ema kable all- ound high e iciency unde bo h indoo and ou doo illumina ion. Nano Ene gy 2016, 30 , 460- 469. 10. Ann, M. H.; Kim, J.; Kim, M.; Alosaimi, G.; Kim, D.; Ha, N. 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