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Preparation and Characterization of Lead Halide Perovskites: Towards sustainable, cost-effective and upscalable solar cell manufacture
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. (Boschloo)
2018 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The perovskite solar cell (PSC) is a recent contender within the photovoltaic research field. In a matter of a few years, the power conversion efficiency (PCE) of the PSC has catapulted from 4% to above 22%, which represents one of the fastest developments in the field. The PSC band-gap tunability makes them interesting for use in tandem solar cells with other established solar cell technologies. This thesis focuses on exploring the photophysics of the perovskite material as well as the development of different perovskite preparation processes and materials for potential use in large-scale manufacture and tandem solar cell applications.

First, the photoconductivity of a perovskite film deposited on different metal oxide nanoparticle layers is investigated. The results show that the perovskite can generate free charge carriers without the presence of an electron acceptor.

Secondly, we constructed PSCs with a conducting carbon-nanotube film, as a replacement for both the hole-selective layer and the metallic back electrode, which yielded a PCE of 15.5%. Furthermore, we explored the preparation of semitransparent PSCs for tandem solar cells by using atomic-layer deposition (ALD) for depositing a thin electron-selective metal-oxide layer. We were successful using ALD directly on a perovskite layer without damage to the perovskite. Although the PSCs did not yield high PCE, the study marks a step in further development for direct ALD deposition onto the perovskite.

Finally, we developed two different methods concerning sustainable manufacture of PSCs. The first method was based on the synthesis of the mixed-ion (FAPbI3)0.87(MAPbBr3)0.17 perovskite in ambient air, which had hitherto only been possible in inert atmosphere. The best PSC was obtained by depositing the perovskite onto a 50°C warm substrate in ambient air yielding a PCE of 17.7%. In the second method, only non-hazardous solvents, water and isopropanol, were used in the synthesis of Cs0.1FA0.9Pb(I0.83Br0.17)3. It is the first publication of mixed inorganic and organic cation perovskite synthesis using a two-step preparation procedure with only non-hazardous solvents and the process yielded a PCE of 13.0%. The method allows for complete ionic control of the perovskite and further variation and improvements are therefore possible.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2018. , p. 83
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1628
Keywords [en]
perovskite solar cells, perovskite, photoconductivity, carbon nanotubes, transparent contact, ambient processing, water-based
National Category
Physical Chemistry Energy Systems Nano Technology
Research subject
Chemistry with specialization in Physical Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-340508ISBN: 978-91-513-0229-4 (print)OAI: oai:DiVA.org:uu-340508DiVA, id: diva2:1179043
Public defence
2018-03-23, Häggsalen, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 13:15 (English)
Opponent
Supervisors
Available from: 2018-02-27 Created: 2018-01-31 Last updated: 2018-04-03
List of papers
1. Probing Photocurrent Generation, Charge Transport, and Recombination Mechanisms in Mesostructured Hybrid Perovskite through Photoconductivity Measurements
Open this publication in new window or tab >>Probing Photocurrent Generation, Charge Transport, and Recombination Mechanisms in Mesostructured Hybrid Perovskite through Photoconductivity Measurements
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2015 (English)In: Journal of Physical Chemistry Letters, ISSN 1948-7185, E-ISSN 1948-7185, Vol. 6, no 21, p. 4259-4264Article in journal (Refereed) Published
Abstract [en]

Conductivity of methylammonium lead triiodide (MAPbI(3)) perovskite was measured on different mesoporous metal oxide scaffolds: TiO2, Al2O3, and ZrO2, as a function of incident light irradiation and temperature. It was found that MAPbI(3) exhibits intrinsic charge separation, and its conductivity stems from a majority of free charge carriers. The crystal morphology of the MAPbI(3) was found to significantly affect the photoconductivity, whereas in the dark the conductivity is governed by the perovskite in the pores of the mesoporous scaffold. The temperature-dependent conductivity measurements also indicate the presence of states within the band gap of the perovskite. Despite a relatively large amount of crystal defects in the measured material, the main recombination mechanism of the photogenerated charges is bimolecular (band-to-band), which suggests that the defect states are rather inactive in the recombination. This may explain the remarkable efficiencies obtained for perovskite solar cells prepared with wetchemical methods.

National Category
Physical Chemistry
Identifiers
urn:nbn:se:uu:diva-268786 (URN)10.1021/acs.jpclett.5b02044 (DOI)000364435800027 ()26538041 (PubMedID)
Funder
Göran Gustafsson Foundation for promotion of scientific research at Uppala University and Royal Institute of TechnologySwedish Energy AgencySwedish Research Council
Available from: 2015-12-15 Created: 2015-12-09 Last updated: 2018-01-31Bibliographically approved
2. Carbon nanotube-based hybrid hole-transporting material and selective contact for high efficiency perovskite solar cells
Open this publication in new window or tab >>Carbon nanotube-based hybrid hole-transporting material and selective contact for high efficiency perovskite solar cells
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2016 (English)In: Energy & Environmental Science, ISSN 1754-5692, E-ISSN 1754-5706, Vol. 9, no 2, p. 461-466Article in journal (Refereed) Published
Abstract [en]

We demonstrate a high efficiency perovskite solar cell with a hybrid hole-transporting material-counter electrode based on a thin single-walled carbon nanotube (SWCNT) film and a drop-cast 2,2,7,-7-tetrakis(N, N-di-p-methoxyphenylamine)-9,90-spirobifluorene (Spiro-OMeTAD) hole-transporting material (HTM). The average efficiency of the solar cells was 13.6%, with the record cell yielding 15.5% efficiency. The efficiency of the reference solar cells with spin-coated Spiro-OMeTAD hole-transportingmaterials (HTMs) and an evaporated gold counter electrode was 17.7% (record 18.8%), that of the cells with only a SWCNT counter electrode (CE) without additional HTM was 9.1% (record 11%) and that of the cells with gold deposited directly on the perovskite layer was 5% (record 6.3%). Our results show that it is possible to manufacture high efficiency perovskite solar cells with thin film (thickness less than 1 mu m) completely carbon-based HTMCEs using industrially upscalable manufacturing methods, such as press-transferred CEs and drop-cast HTMs.

National Category
Physical Chemistry
Identifiers
urn:nbn:se:uu:diva-280914 (URN)10.1039/c5ee03394b (DOI)000369744500010 ()
Funder
Swedish Energy AgencySwedish Research CouncilKnut and Alice Wallenberg FoundationStandUpEU, FP7, Seventh Framework Programme, 604472
Available from: 2016-03-16 Created: 2016-03-16 Last updated: 2018-01-31Bibliographically approved
3. Atomic Layer Deposition of Electron Selective SnOx and ZnO Films on Mixed Halide Perovskite: Compatibility and Performance
Open this publication in new window or tab >>Atomic Layer Deposition of Electron Selective SnOx and ZnO Films on Mixed Halide Perovskite: Compatibility and Performance
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2017 (English)In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 9, no 35, p. 29707-29716Article in journal (Refereed) Published
Abstract [en]

The compatibility of atomic layer deposition directly onto the mixed halide perovskite formamidinium lead iodide:methylammonium lead bromide (CH(NH2)(2), CH3NH3)Pb(I,Br)(3) (FAPbI(3):MAPbBr(3)) perovskite films is investigated by exposing the perovskite films to the full or partial atomic layer deposition processes for the electron selective layer candidates ZnO and SnOx. Exposing the samples to the heat, the vacuum, and even the counter reactant of H2O of the atomic layer deposition processes does not appear to alter the perovskite films in terms of crystallinity, but the choice of metal precursor is found to be critical. The Zn precursor Zn(C2H5)(2) either by itself or in combination with H2O during the ZnO atomic layer deposition (ALD) process is found to enhance the decomposition of the bulk of the perovskite film into PbI2 without even forming ZnO. In contrast, the Sn precursor Sn(N(CH3)(2))(4) does not seem to degrade the bulk of the perovskite film, and conformal SnOx films can successfully be grown on top of it using atomic layer deposition. Using this SnOx film as the electron selective layer in inverted perovskite solar cells results in a lower power conversion efficiency of 3.4% than the 8.4% for the reference devices using phenyl-C-70-butyric acid methyl ester. However, the devices with SnOx show strong hysteresis and can be pushed to an efficiency of 7.8% after biasing treatments. Still, these cells lacks both open circuit voltage and fill factor compared to the references, especially when thicker SnOx films are used. Upon further investigation, a possible cause of these losses could be that the perovskite/SnOx interface is not ideal and more specifically found to be rich in Sn, O, and halides, which is probably a result of the nucleation during the SnOx growth and which might introduce barriers or alter the band alignment for the transport of charge carriers.

Keywords
perovskite solar cell, atomic layer deposition, interfaces, electron selective layers, precursor chemistry
National Category
Materials Chemistry Engineering and Technology
Identifiers
urn:nbn:se:uu:diva-335852 (URN)10.1021/acsami.7b07627 (DOI)000410597500034 ()28792724 (PubMedID)
Available from: 2018-01-25 Created: 2018-01-25 Last updated: 2018-02-12Bibliographically approved
4. Ambient air-processed mixed-ion perovskites for high-efficiency solar cells
Open this publication in new window or tab >>Ambient air-processed mixed-ion perovskites for high-efficiency solar cells
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2016 (English)In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 4, no 42, p. 16536-16545Article in journal (Refereed) Published
Abstract [en]

Mixed-ion (FAPbI(3))(1-x)(MAPbBr(3))(x) perovskite solar cells have achieved power conversion efficiencies surpassing 20%. However, in order to obtain these high efficiencies the preparation is performed in a controlled inert atmosphere. Here, we report a procedure for manufacturing highly efficient solar cells with a mixed-ion perovskite in ambient atmosphere. By including a heating step at moderate temperatures of the mesoporous titanium dioxide substrates, and spin-coating the perovskite solution on the warm substrates in ambient air, a red intermediate phase is obtained. Annealing the red phase at 100 degrees C results in a uniform and crystalline perovskite film, whose thickness is dependent on the substrate temperature prior to spin-coating. The temperature was optimized between 20 and 100 degrees C and it was observed that 50 degrees C substrate temperature yielded the best solar cell performances. The average efficiency of the best device was 17.6%, accounting for current-voltage (I-V) measurement hysteresis, with 18.8% performance in the backward scan direction and 16.4% in the forward scan direction. Our results show that it is possible to manufacture high-efficiency mixed-ion perovskite solar cells under ambient conditions, which is relevant for large-scale and low-cost device manufacturing processing.

National Category
Physical Chemistry
Identifiers
urn:nbn:se:uu:diva-310043 (URN)10.1039/c6ta06912f (DOI)000387166900031 ()
Funder
Göran Gustafsson Foundation for promotion of scientific research at Uppala University and Royal Institute of TechnologySwedish Energy AgencyÅForsk (Ångpanneföreningen's Foundation for Research and Development)Swedish Research Council FormasSwedish Research Council
Available from: 2016-12-09 Created: 2016-12-09 Last updated: 2018-01-31Bibliographically approved
5. Preparation of mixed-ion and inorganic perovskite films using water and isopropanol as solvents for solar cell applications
Open this publication in new window or tab >>Preparation of mixed-ion and inorganic perovskite films using water and isopropanol as solvents for solar cell applications
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2018 (English)In: Sustainable Energy & Fuels, E-ISSN 2398-4902, Vol. 2, no 3, p. 606-615Article in journal (Refereed) Published
Abstract [en]

Presently, the most efficient lead halide perovskite solar cells are manufactured by using high-boiling point organic solvents to dissolve the perovskite precursor materials prior to the perovskite formation. Previously, efforts have been made to exchange the said solvents for water with some success. Herein, we build on that work to develop a procedure for synthesising perovskite absorbers using only water and isopropanol as solvents. Our technique can be utilised for fabricating many different perovskite compositions, organic and inorganic. The technique is based on the high solubility of metal nitrates, such as lead(ii) nitrate and caesium(i) nitrate, in water and, respectively, their poor solubilities in isopropanol. The inclusion of CsNO3 to Pb(NO3)2 films does not result in a phase separation of the perovskite material as one would expect when using lead(ii) halide precursor films. Using the perovskite composition Cs0.1FA0.9Pb(I0.83Br0.17)3 we were able to reach an average solar cell power conversion efficiency of 13.0%. Furthermore, the technique can be applied to many different perovskite compositions making it appealing for large-scale manufacturing of perovskite solar cells.

Place, publisher, year, edition, pages
The Royal Society of Chemistry, 2018
National Category
Physical Chemistry
Identifiers
urn:nbn:se:uu:diva-340427 (URN)10.1039/C7SE00538E (DOI)000426712600011 ()
Funder
Göran Gustafsson Foundation for Research in Natural Sciences and MedicineSwedish Energy AgencyÅForsk (Ångpanneföreningen's Foundation for Research and Development)Swedish Research Council FormasSwedish Foundation for Strategic Research Swedish Research Council
Available from: 2018-01-30 Created: 2018-01-30 Last updated: 2018-05-23Bibliographically approved

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