Green energy by recoverable triple-oxide mesostructured perovskite photovoltaics

Avi Schneider; Ariel Efrati; Stav Alon; Maayan Sohmer; Lioz Etgar

doi:10.1073/pnas.2013242117

Edited by Omar M. Yaghi, University of California, Berkeley, CA, and approved October 20, 2020 (received for review June 26, 2020)

Significance

In the progress toward a more sustainable world, wind and solar energy production are the leading renewable contenders. The emerging field of perovskite solar cells has achieved remarkable efficiencies and is gaining a steady foothold among other solar technologies. However, a worldwide deployment of perovskite solar panels poses environmental and economic problems due to degradation over time. The degrading photoactive materials are usually situated between other layers, complicating or inhibiting cell recycling. Here, we investigated a structure for perovskite solar cells composed of chemically and thermally stable oxides which includes the application of the photoactive perovskite material as a final step. This structure allows for the removal and replacement of degraded perovskite, with a full restoration of photovoltaic characteristics.

Abstract

Perovskite solar cells have developed into a promising branch of renewable energy. A combination of feasible manufacturing and renewable modules can offer an attractive advancement to this field. Herein, a screen-printed three-layered all-nanoparticle network was developed as a rigid framework for a perovskite active layer. This matrix enables perovskite to percolate and form a complementary photoactive network. Two porous conductive oxide layers, separated by a porous insulator, serve as a chemically stable substrate for the cells. Cells prepared using this scaffold structure demonstrated a power conversion efficiency of 11.08% with a high open-circuit voltage of 0.988 V. Being fully oxidized, the scaffold demonstrated a striking thermal and chemical stability, allowing for the removal of the perovskite while keeping the substrate intact. The application of a new perovskite in lieu of a degraded one exhibited a full regeneration of all photovoltaic performances. Exclusive recycling of the photoactive materials from solar cells paves a path for more sustainable green energy production in the future.

Footnotes

↵¹A.S. and A.E. contributed equally to this work.
↵²To whom correspondence may be addressed. Email: lioz.etgar{at}mail.huji.ac.il.

Author contributions: A.E. and L.E. designed research; A.S., A.E., S.A., and M.S. performed research; A.S., A.E., S.A., M.S., and L.E. analyzed data; and A.S., A.E., and L.E. wrote the paper.
The authors declare no competing interest.
This article is a PNAS Direct Submission.
This article contains supporting information online at https://www.pnas.org/lookup/suppl/doi:10.1073/pnas.2013242117/-/DCSupplemental.

Data Availability.

All study data are included in the article and SI Appendix.

Published under the PNAS license.

View Full Text

References

↵
1. P. T. Brown,
2. K. Caldeira
, Greater future global warming inferred from Earth’s recent energy budget. Nature 552, 45–50 (2017).
OpenUrl
↵
1. P. Cheng,
2. G. Li,
3. X. Zhan,
4. Y. Yang
, Next-generation organic photovoltaics based on non-fullerene acceptors. Nat. Photonics 12, 131–142 (2018).
OpenUrl CrossRef
↵
1. D. P. Fenning et al
., Precipitated iron: A limit on gettering efficacy in multicrystalline silicon. J. Appl. Phys. 113, 044521 (2013).
OpenUrl
↵
1. H. Savin et al
., Black silicon solar cells with interdigitated back-contacts achieve 22.1% efficiency. Nat. Nanotechnol. 10, 624–628 (2015).
OpenUrl
↵
1. A. Efrati et al
., Assembly of photo-bioelectrochemical cells using photosystem I-functionalized electrodes. Nat. Energy 1, 15021 (2016).
OpenUrl
↵
1. B. Dongqin et al
., Polymer-templated nucleation and crystal growth of perovskite films for solar cells with efficiency greater than 21%. Nat. Energy 1, 1–5 (2016).
OpenUrl
↵
1. A. Efrati,
2. S. Aharon,
3. M. Wierzbowska,
4. L. Etgar
, First evidence of macroscale single crystal ion exchange found in lead halide perovskites. EcoMat 2, 1–8 (2020).
OpenUrl
↵
1. Y. Zhang et al
., Bifacial stamping for high efficiency perovskite solar cells. Energy Environ. Sci. 12, 308–321 (2019).
OpenUrl
↵
1. T. Miyasaka,
2. K. Zhu,
3. N.-G. Park,
4. K. Emery,
5. M. Grätzel
, Towards stable and commercially available perovskite solar cells. Nat. Energy 1, 16152 (2016).
OpenUrl
↵
1. A. Shpatz Dayan et al
., Enhancing stability and photostability of CsPbI3 by reducing its dimensionality. Chem. Mater. 30, 8017–8024 (2018).
OpenUrl
↵
1. S. Aharon,
2. B. E. Cohen,
3. L. Etgar
, Hybrid lead halide iodide and lead halide bromide in efficient hole conductor free perovskite solar cell. J. Phys. Chem. C 118, 17160–17165 (2014).
OpenUrl
↵
1. L. Etgar
, The merit of perovskite’s dimensionality; can this replace the 3D halide perovskite? Energy Environ. Sci. 11, 234–242 (2018).
OpenUrl
↵
1. S.-H. Turren-Cruz,
2. A. Hagfeldt,
3. M. Saliba
, Methylammonium-free, high-performance, and stable perovskite solar cells on a planar architecture. Science 362, 449–453 (2018).
OpenUrl Abstract/FREE Full Text
↵
1. Z. Ku,
2. Y. Rong,
3. M. Xu,
4. T. Liu,
5. H. Han
, Full printable processed mesoscopic CH₃NH₃PbI₃/TiO₂ heterojunction solar cells with carbon counter electrode. Sci. Rep. 3, 3132 (2013).
OpenUrl CrossRef PubMed
↵
1. L. Fan,
2. J. R. Jennings,
3. S. M. Zakeeruddin,
4. M. Grätzel,
5. Q. Wang
, Redox catalysis for improved counter-electrode kinetics in dye-sensitized solar cells. ChemElectroChem 4, 1356–1361 (2017).
OpenUrl
↵
1. S. Ito et al
., Fabrication of screen-printing pastes from TiO2 powders for dye-sensitised solar cells. Prog. Photovolt. Res. Appl. 15, 603–612 (2007).
OpenUrl
↵
1. G. Liu,
2. W. Jaegermann,
3. J. He,
4. V. Sundström,
5. L. Sun
, XPS and UPS characterization of the TiO2/ZnPcGly heterointerface: Alignment of energy levels. J. Phys. Chem. B 106, 5814–5819 (2002).
OpenUrl
↵
1. A. Andersson et al
., Fluorine tin oxide as an alternative to indium tin oxide in polymer LEDs. Adv. Mater. 10, 859–863 (1998).
OpenUrl
↵
1. K. Jung et al
., Efficient composition tuning via cation exchange and improved reproducibility of photovoltaic performance in FAxMA1-xPbI3 planar heterojunction solar cells fabricated by a two-step dynamic spin-coating process. Nano Energy 54, 251–263 (2018).
OpenUrl
↵
1. J. Li,
2. S. Meng,
3. J. Niu
, Electronic structures and optical properties of monoclinic ZrO2 studied by first-principles local density approximation + U approach. J. Adv. Ceram. 6, 43–49 (2017).
OpenUrl
↵
1. W. S. Yang et al
., High-performance photovoltaic perovskite layers fabricated through intramolecular exchange. Science 348, 1234–1237 (2015).
OpenUrl Abstract/FREE Full Text
↵
1. Y. Han et al
., Degradation observations of encapsulated planar CH₃NH₃PbI₃ perovskite solar cells at high temperatures and humidity. J. Mater. Chem. A Mater. Energy Sustain. 3, 8139–8147 (2015).
OpenUrl
↵
1. F. Matteocci et al
., Encapsulation for long-term stability enhancement of perovskite solar cells. Nano Energy 30, 162–172 (2016).
OpenUrl
↵
1. A. Binek et al
., Recycling perovskite solar cells to avoid lead waste. ACS Appl. Mater. Interfaces 8, 12881–12886 (2016).
OpenUrl PubMed
↵
1. J. M. Kadro et al
., Proof-of-concept for facile perovskite solar cell recycling. Energy Environ. Sci. 9, 3172–3179 (2016).
OpenUrl
↵
1. Y. C. Kim et al
., Beneficial effects of PbI2 incorporated in organo-lead halide perovskite solar cells. Adv. Energy Mater. 6, 1502104 (2016).
OpenUrl
↵
1. M. H. Li et al
., Robust and recyclable substrate template with an ultrathin nanoporous counter electrode for organic-hole-conductor-free monolithic perovskite solar cells. ACS Appl. Mater. Interfaces 9, 41845–41854 (2017).
OpenUrl
↵
1. J. Gong,
2. S. B. Darling,
3. F. You
, Perovskite photovoltaics: Life-cycle assessment of energy and environmental impacts. Energy Environ. Sci. 8, 1953–1968 (2015).
OpenUrl
↵
1. D. Faiman et al
., “Data processing for the Negev radiation survey: Seventh year” (Ministry of National Infrastructures, Israel, 2001).
↵
1. S. D. Stranks et al
., Electron-hole diffusion lengths exceeding 1 micrometer in an organometal trihalide perovskite absorber. Science 342, 341–344 (2013).
OpenUrl Abstract/FREE Full Text
↵
1. X. Wu et al
., Trap states in lead iodide perovskites. J. Am. Chem. Soc. 137, 2089–2096 (2015).
OpenUrl CrossRef PubMed
↵
1. N. W. Duffy,
2. L. M. Peter,
3. R. M. G. Rajapakse,
4. K. G. U. Wijayantha
, A novel charge extraction method for the study of electron transport and interfacial transfer in dye sensitised nanocrystalline solar cells. Electrochem. Commun. 2, 658–662 (2000).
OpenUrl CrossRef
↵
1. E. Avigad,
2. L. Etgar
, Studying the effect of MoO3 in hole-conductor-free perovskite solar cells. ACS Energy Lett. 3, 2240–2245 (2018).
OpenUrl
↵
1. Y. Zhao,
2. A. M. Nardes,
3. K. Zhu
, Solid-state mesostructured perovskite CH3NH3PbI3 solar cells: Charge transport, recombination, and diffusion length. J. Phys. Chem. Lett. 5, 490–494 (2014).
OpenUrl
↵
1. A. Schneider,
2. S. Alon,
3. L. Etgar
, Evolution of photovoltaic performance in fully printable mesoscopic carbon based perovskite solar cells. Energy Technol. (Weinheim) 7, 1900481 (2019).
OpenUrl

Log in through your institution

Purchase access

You may purchase access to this article. This will require you to create an account if you don't already have one.

Article Alerts

Email Article

Citation Tools

Request Permissions

Article Classifications

Physical Sciences
Sustainability Science

Proceedings of the National Academy of Sciences: 117 (49)

Table of Contents

Submit

[1] ↵
P. T. Brown,
K. Caldeira
, Greater future global warming inferred from Earth’s recent energy budget. Nature 552, 45–50 (2017).
OpenUrl

[2] P. T. Brown,

[3] K. Caldeira

[4] ↵
P. Cheng,
G. Li,
X. Zhan,
Y. Yang
, Next-generation organic photovoltaics based on non-fullerene acceptors. Nat. Photonics 12, 131–142 (2018).
OpenUrl CrossRef

[5] P. Cheng,

[6] G. Li,

[7] X. Zhan,

[8] Y. Yang

[9] ↵
D. P. Fenning et al
., Precipitated iron: A limit on gettering efficacy in multicrystalline silicon. J. Appl. Phys. 113, 044521 (2013).
OpenUrl

[10] D. P. Fenning et al

[11] ↵
H. Savin et al
., Black silicon solar cells with interdigitated back-contacts achieve 22.1% efficiency. Nat. Nanotechnol. 10, 624–628 (2015).
OpenUrl

[12] H. Savin et al

[13] ↵
A. Efrati et al
., Assembly of photo-bioelectrochemical cells using photosystem I-functionalized electrodes. Nat. Energy 1, 15021 (2016).
OpenUrl

[14] A. Efrati et al

[15] ↵
B. Dongqin et al
., Polymer-templated nucleation and crystal growth of perovskite films for solar cells with efficiency greater than 21%. Nat. Energy 1, 1–5 (2016).
OpenUrl

[16] B. Dongqin et al

[17] ↵
A. Efrati,
S. Aharon,
M. Wierzbowska,
L. Etgar
, First evidence of macroscale single crystal ion exchange found in lead halide perovskites. EcoMat 2, 1–8 (2020).
OpenUrl

[18] A. Efrati,

[19] S. Aharon,

[20] M. Wierzbowska,

[21] L. Etgar

[22] ↵
Y. Zhang et al
., Bifacial stamping for high efficiency perovskite solar cells. Energy Environ. Sci. 12, 308–321 (2019).
OpenUrl

[23] Y. Zhang et al

[24] ↵
T. Miyasaka,
K. Zhu,
N.-G. Park,
K. Emery,
M. Grätzel
, Towards stable and commercially available perovskite solar cells. Nat. Energy 1, 16152 (2016).
OpenUrl

[25] T. Miyasaka,

[26] K. Zhu,

[27] N.-G. Park,

[28] K. Emery,

[29] M. Grätzel

[30] ↵
A. Shpatz Dayan et al
., Enhancing stability and photostability of CsPbI3 by reducing its dimensionality. Chem. Mater. 30, 8017–8024 (2018).
OpenUrl

[31] A. Shpatz Dayan et al

[32] ↵
S. Aharon,
B. E. Cohen,
L. Etgar
, Hybrid lead halide iodide and lead halide bromide in efficient hole conductor free perovskite solar cell. J. Phys. Chem. C 118, 17160–17165 (2014).
OpenUrl

[33] S. Aharon,

[34] B. E. Cohen,

[35] L. Etgar

[36] ↵
L. Etgar
, The merit of perovskite’s dimensionality; can this replace the 3D halide perovskite? Energy Environ. Sci. 11, 234–242 (2018).
OpenUrl

[37] L. Etgar

[38] ↵
S.-H. Turren-Cruz,
A. Hagfeldt,
M. Saliba
, Methylammonium-free, high-performance, and stable perovskite solar cells on a planar architecture. Science 362, 449–453 (2018).
OpenUrl Abstract/FREE Full Text

[39] S.-H. Turren-Cruz,

[40] A. Hagfeldt,

[41] M. Saliba

[42] ↵
Z. Ku,
Y. Rong,
M. Xu,
T. Liu,
H. Han
, Full printable processed mesoscopic CH₃NH₃PbI₃/TiO₂ heterojunction solar cells with carbon counter electrode. Sci. Rep. 3, 3132 (2013).
OpenUrl CrossRef PubMed

[43] Z. Ku,

[44] Y. Rong,

[45] M. Xu,

[46] T. Liu,

[47] H. Han

[48] ↵
L. Fan,
J. R. Jennings,
S. M. Zakeeruddin,
M. Grätzel,
Q. Wang
, Redox catalysis for improved counter-electrode kinetics in dye-sensitized solar cells. ChemElectroChem 4, 1356–1361 (2017).
OpenUrl

[49] L. Fan,

[50] J. R. Jennings,

[51] S. M. Zakeeruddin,

[52] M. Grätzel,

[53] Q. Wang

[54] ↵
S. Ito et al
., Fabrication of screen-printing pastes from TiO2 powders for dye-sensitised solar cells. Prog. Photovolt. Res. Appl. 15, 603–612 (2007).
OpenUrl

[55] S. Ito et al

[56] ↵
G. Liu,
W. Jaegermann,
J. He,
V. Sundström,
L. Sun
, XPS and UPS characterization of the TiO2/ZnPcGly heterointerface: Alignment of energy levels. J. Phys. Chem. B 106, 5814–5819 (2002).
OpenUrl

[57] G. Liu,

[58] W. Jaegermann,

[59] J. He,

[60] V. Sundström,

[61] L. Sun

[62] ↵
A. Andersson et al
., Fluorine tin oxide as an alternative to indium tin oxide in polymer LEDs. Adv. Mater. 10, 859–863 (1998).
OpenUrl

[63] A. Andersson et al

[64] ↵
K. Jung et al
., Efficient composition tuning via cation exchange and improved reproducibility of photovoltaic performance in FAxMA1-xPbI3 planar heterojunction solar cells fabricated by a two-step dynamic spin-coating process. Nano Energy 54, 251–263 (2018).
OpenUrl

[65] K. Jung et al

[66] ↵
J. Li,
S. Meng,
J. Niu
, Electronic structures and optical properties of monoclinic ZrO2 studied by first-principles local density approximation + U approach. J. Adv. Ceram. 6, 43–49 (2017).
OpenUrl

[67] J. Li,

[68] S. Meng,

[69] J. Niu

[70] ↵
W. S. Yang et al
., High-performance photovoltaic perovskite layers fabricated through intramolecular exchange. Science 348, 1234–1237 (2015).
OpenUrl Abstract/FREE Full Text

[71] W. S. Yang et al

[72] ↵
Y. Han et al
., Degradation observations of encapsulated planar CH₃NH₃PbI₃ perovskite solar cells at high temperatures and humidity. J. Mater. Chem. A Mater. Energy Sustain. 3, 8139–8147 (2015).
OpenUrl

[73] Y. Han et al

[74] ↵
F. Matteocci et al
., Encapsulation for long-term stability enhancement of perovskite solar cells. Nano Energy 30, 162–172 (2016).
OpenUrl

[75] F. Matteocci et al

[76] ↵
A. Binek et al
., Recycling perovskite solar cells to avoid lead waste. ACS Appl. Mater. Interfaces 8, 12881–12886 (2016).
OpenUrl PubMed

[77] A. Binek et al

[78] ↵
J. M. Kadro et al
., Proof-of-concept for facile perovskite solar cell recycling. Energy Environ. Sci. 9, 3172–3179 (2016).
OpenUrl

[79] J. M. Kadro et al

[80] ↵
Y. C. Kim et al
., Beneficial effects of PbI2 incorporated in organo-lead halide perovskite solar cells. Adv. Energy Mater. 6, 1502104 (2016).
OpenUrl

[81] Y. C. Kim et al

[82] ↵
M. H. Li et al
., Robust and recyclable substrate template with an ultrathin nanoporous counter electrode for organic-hole-conductor-free monolithic perovskite solar cells. ACS Appl. Mater. Interfaces 9, 41845–41854 (2017).
OpenUrl

[83] M. H. Li et al

[84] ↵
J. Gong,
S. B. Darling,
F. You
, Perovskite photovoltaics: Life-cycle assessment of energy and environmental impacts. Energy Environ. Sci. 8, 1953–1968 (2015).
OpenUrl

[85] J. Gong,

[86] S. B. Darling,

[87] F. You

[88] ↵
D. Faiman et al
., “Data processing for the Negev radiation survey: Seventh year” (Ministry of National Infrastructures, Israel, 2001).

[89] D. Faiman et al

[90] ↵
S. D. Stranks et al
., Electron-hole diffusion lengths exceeding 1 micrometer in an organometal trihalide perovskite absorber. Science 342, 341–344 (2013).
OpenUrl Abstract/FREE Full Text

[91] S. D. Stranks et al

[92] ↵
X. Wu et al
., Trap states in lead iodide perovskites. J. Am. Chem. Soc. 137, 2089–2096 (2015).
OpenUrl CrossRef PubMed

[93] X. Wu et al

[94] ↵
N. W. Duffy,
L. M. Peter,
R. M. G. Rajapakse,
K. G. U. Wijayantha
, A novel charge extraction method for the study of electron transport and interfacial transfer in dye sensitised nanocrystalline solar cells. Electrochem. Commun. 2, 658–662 (2000).
OpenUrl CrossRef

[95] N. W. Duffy,

[96] L. M. Peter,

[97] R. M. G. Rajapakse,

[98] K. G. U. Wijayantha

[99] ↵
E. Avigad,
L. Etgar
, Studying the effect of MoO3 in hole-conductor-free perovskite solar cells. ACS Energy Lett. 3, 2240–2245 (2018).
OpenUrl

[100] E. Avigad,

[101] L. Etgar

[102] ↵
Y. Zhao,
A. M. Nardes,
K. Zhu
, Solid-state mesostructured perovskite CH3NH3PbI3 solar cells: Charge transport, recombination, and diffusion length. J. Phys. Chem. Lett. 5, 490–494 (2014).
OpenUrl

[103] Y. Zhao,

[104] A. M. Nardes,

[105] K. Zhu

[106] ↵
A. Schneider,
S. Alon,
L. Etgar
, Evolution of photovoltaic performance in fully printable mesoscopic carbon based perovskite solar cells. Energy Technol. (Weinheim) 7, 1900481 (2019).
OpenUrl

[107] A. Schneider,

[108] S. Alon,

[109] L. Etgar

Main menu

User menu

Search

Green energy by recoverable triple-oxide mesostructured perovskite photovoltaics

Significance

Abstract

Footnotes

Data Availability.

References

Log in through your institution

Purchase access

Citation Manager Formats

Article Classifications

You May Also be Interested in

Similar Articles

Articles

PNAS Portals

Information

Main menu

User menu

Search

Significance

Abstract

Footnotes

Data Availability.

References

Log in using your username and password

Log in through your institution

Purchase access

Citation Manager Formats

Article Classifications

Sign up for Article Alerts

Jump to section

You May Also be Interested in

Similar Articles

Articles

PNAS Portals

Information