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Title: The Molybdenum Oxide Interface Limits the High-Temperature Operational Stability of Unencapsulated Perovskite Solar Cells

Abstract

Here, we report on the improved operational stability of unencapsulated perovskite solar cells (PSCs) aged in an ambient atmosphere at elevated temperatures (70 °C) for >1000 h under constant illumination and bias at 30–50% relative humidity. We identify a previously unseen interfacial degradation mechanism concerning the use of a MoOx interlayer, which was originally added to increase operational stability. Specifically, the hole-transport layer/MoOx interface buckles under illumination at 70 °C, which leads to delamination and rapid losses of short-circuit current density corresponding to an average $$t_{80}$$ of ~55 h. By judiciously evaluating various hole-transport layers, interlayers, and contacts, we find that replacing the MoOx with a VOx interlayer, regardless of the other components in the solar cell, alleviates this buckling issue due to its higher activation barrier toward crystallization, leading to significant gains in PSC operational stability. Unencapsulated devices aged in an ambient atmosphere with a VOx interlayer retain 71% of their initial PCE on average after constant illumination and bias at 70 °C for 1100 h ($$t_{80}$$ ~ 645 h). Currently, this is the highest temperature reported for the operational stability of unencapsulated n-i-p PSCs aged in air. Identification of a new facet of the complex degradation mechanisms in PSCs will allow for targeted acceleration testing to speed the deployment of low-cost, long-lasting electricity generation under realistic operating temperatures.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [4];  [4]; ORCiD logo [4];  [4]; ORCiD logo [5];  [4];  [4];  [5]; ORCiD logo [5]; ORCiD logo [4]; ORCiD logo [4]; ORCiD logo [2];  [4]; ORCiD logo [4]; ORCiD logo [4]
  1. Colorado School of Mines, Golden, CO (United States); Harvard Univ., Cambridge, MA (United States)
  2. Stanford Univ., CA (United States)
  3. Colorado School of Mines, Golden, CO (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)
  4. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  5. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States); Stanford Univ., CA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office; National Science Foundation (NSF)
OSTI Identifier:
1660219
Alternate Identifier(s):
OSTI ID: 1671819
Report Number(s):
NREL/JA-5900-75917
Journal ID: ISSN 2380-8195; MainId:6669;UUID:9c929e68-283e-ea11-9c2f-ac162d87dfe5;MainAdminID:16308
Grant/Contract Number:  
AC36-08GO28308; EE0008174; EE0008167; ECCS-1542152
Resource Type:
Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 5; Journal Issue: 7; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; degradation; perovskite solar cells; stability

Citation Formats

Schloemer, Tracy H., Raiford, James A., Gehan, Timothy S., Moot, Taylor, Nanayakkara, Sanjini, Harvey, Steven P., Bramante, Rosemary C., Dunfield, Sean, Louks, Amy E., Maughan, Annalise E., Bliss, Lyle, McGehee, Michael D., van Hest, Maikel F. A. M., Reese, Matthew O., Bent, Stacey F., Berry, Joseph J., Luther, Joseph M., and Sellinger, Alan. The Molybdenum Oxide Interface Limits the High-Temperature Operational Stability of Unencapsulated Perovskite Solar Cells. United States: N. p., 2020. Web. doi:10.1021/acsenergylett.0c01023.
Schloemer, Tracy H., Raiford, James A., Gehan, Timothy S., Moot, Taylor, Nanayakkara, Sanjini, Harvey, Steven P., Bramante, Rosemary C., Dunfield, Sean, Louks, Amy E., Maughan, Annalise E., Bliss, Lyle, McGehee, Michael D., van Hest, Maikel F. A. M., Reese, Matthew O., Bent, Stacey F., Berry, Joseph J., Luther, Joseph M., & Sellinger, Alan. The Molybdenum Oxide Interface Limits the High-Temperature Operational Stability of Unencapsulated Perovskite Solar Cells. United States. https://doi.org/10.1021/acsenergylett.0c01023
Schloemer, Tracy H., Raiford, James A., Gehan, Timothy S., Moot, Taylor, Nanayakkara, Sanjini, Harvey, Steven P., Bramante, Rosemary C., Dunfield, Sean, Louks, Amy E., Maughan, Annalise E., Bliss, Lyle, McGehee, Michael D., van Hest, Maikel F. A. M., Reese, Matthew O., Bent, Stacey F., Berry, Joseph J., Luther, Joseph M., and Sellinger, Alan. Mon . "The Molybdenum Oxide Interface Limits the High-Temperature Operational Stability of Unencapsulated Perovskite Solar Cells". United States. https://doi.org/10.1021/acsenergylett.0c01023. https://www.osti.gov/servlets/purl/1660219.
@article{osti_1660219,
title = {The Molybdenum Oxide Interface Limits the High-Temperature Operational Stability of Unencapsulated Perovskite Solar Cells},
author = {Schloemer, Tracy H. and Raiford, James A. and Gehan, Timothy S. and Moot, Taylor and Nanayakkara, Sanjini and Harvey, Steven P. and Bramante, Rosemary C. and Dunfield, Sean and Louks, Amy E. and Maughan, Annalise E. and Bliss, Lyle and McGehee, Michael D. and van Hest, Maikel F. A. M. and Reese, Matthew O. and Bent, Stacey F. and Berry, Joseph J. and Luther, Joseph M. and Sellinger, Alan},
abstractNote = {Here, we report on the improved operational stability of unencapsulated perovskite solar cells (PSCs) aged in an ambient atmosphere at elevated temperatures (70 °C) for >1000 h under constant illumination and bias at 30–50% relative humidity. We identify a previously unseen interfacial degradation mechanism concerning the use of a MoOx interlayer, which was originally added to increase operational stability. Specifically, the hole-transport layer/MoOx interface buckles under illumination at 70 °C, which leads to delamination and rapid losses of short-circuit current density corresponding to an average $t_{80}$ of ~55 h. By judiciously evaluating various hole-transport layers, interlayers, and contacts, we find that replacing the MoOx with a VOx interlayer, regardless of the other components in the solar cell, alleviates this buckling issue due to its higher activation barrier toward crystallization, leading to significant gains in PSC operational stability. Unencapsulated devices aged in an ambient atmosphere with a VOx interlayer retain 71% of their initial PCE on average after constant illumination and bias at 70 °C for 1100 h ($t_{80}$ ~ 645 h). Currently, this is the highest temperature reported for the operational stability of unencapsulated n-i-p PSCs aged in air. Identification of a new facet of the complex degradation mechanisms in PSCs will allow for targeted acceleration testing to speed the deployment of low-cost, long-lasting electricity generation under realistic operating temperatures.},
doi = {10.1021/acsenergylett.0c01023},
journal = {ACS Energy Letters},
number = 7,
volume = 5,
place = {United States},
year = {Mon Jun 15 00:00:00 EDT 2020},
month = {Mon Jun 15 00:00:00 EDT 2020}
}

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