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Title: Enhancing Chemical Stability and Suppressing Ion Migration in CH3NH3PbI3 Perovskite Solar Cells via Direct Backbone Attachment of Polyesters on Grain Boundaries

Abstract

Organic–inorganic halide perovskites feature excellent optoelectronic properties but poor chemical stability. While passivating perovskite grain boundary (GB) by polymers shows prospects on long-term performance of perovskite solar cells (PSCs), its detailed impact on the ion migration phenomenon, which largely deteriorates the PSC stability, remains less probed. In this work, we introduce a new polar polymer, polycaprolactone (PCL), to passivate GBs of methylammonium lead triiodide (MAPbI3) perovskite with only 1–2 polymer monolayers via direct backbone attachment. The PSCs with passivated MAPbI3, using a classic but less stable Spiro-OMeTAD (2,2',7,7'-tetrakis[N,N-di(4-methoxyphenyl)amino]-9,9'-spirobifluorene) hole transport layer (HTL), exhibit improved power conversion efficiencies up to 20.1%, with 90% of the initial PCE being preserved after 400 h ambient storage, and 80% even after 100 h, 85 °C aging. The improved PSC stability indicates critical roles of PCL GB passivation in retarding moisture-induced decomposition and suppressing ion migration within the perovskite. Furthermore, time-of-flight secondary ion mass spectrometry reveals that I– ions can actively migrate into the electrode, HTL, and their interface in nonpassivated PSCs, even without an externally applied electric field, while such migration is significantly mitigated in PCL-passivated PSCs. This effective GB passivation by PCL suggests an important potential of polymer additives toward the development ofmore » stable high-performance PSCs.« less

Authors:
 [1];  [1];  [1]; ORCiD logo [1];  [2];  [3]; ORCiD logo [3];  [1]; ORCiD logo [1];  [1];  [4];  [4]; ORCiD logo [5];  [1]
  1. Stony Brook Univ., NY (United States)
  2. City Univ. of New York (CUNY), NY (United States)
  3. Brown Univ., Providence, RI (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Stony Brook Univ., NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); US Department of the Navy, Office of Naval Research (ONR); National Research Foundation of Korea (NRF); National Science Foundation (NSF)
OSTI Identifier:
1642408
Report Number(s):
BNL-216171-2020-JAAM
Journal ID: ISSN 0897-4756
Grant/Contract Number:  
SC0012704; NSF-1344267; 2017K1A1A2013153; OIA-1538893; N00014-17-1-2232; OIA-1929019
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 32; Journal Issue: 12; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Passivation; thin films; ions; perovskites; polymers

Citation Formats

Zhou, Yuchen, Yin, Yifan, Zuo, Xianghao, Wang, Likun, Li, Tai-De, Zhou, Yuanyuan, Padture, Nitin P., Yang, Zhenhua, Guo, Yichen, Xue, Yuan, Kisslinger, Kim, Cotlet, Mircea, Nam, Chang-Yong, and Rafailovich, Miriam H. Enhancing Chemical Stability and Suppressing Ion Migration in CH3NH3PbI3 Perovskite Solar Cells via Direct Backbone Attachment of Polyesters on Grain Boundaries. United States: N. p., 2020. Web. doi:10.1021/acs.chemmater.0c00995.
Zhou, Yuchen, Yin, Yifan, Zuo, Xianghao, Wang, Likun, Li, Tai-De, Zhou, Yuanyuan, Padture, Nitin P., Yang, Zhenhua, Guo, Yichen, Xue, Yuan, Kisslinger, Kim, Cotlet, Mircea, Nam, Chang-Yong, & Rafailovich, Miriam H. Enhancing Chemical Stability and Suppressing Ion Migration in CH3NH3PbI3 Perovskite Solar Cells via Direct Backbone Attachment of Polyesters on Grain Boundaries. United States. https://doi.org/10.1021/acs.chemmater.0c00995
Zhou, Yuchen, Yin, Yifan, Zuo, Xianghao, Wang, Likun, Li, Tai-De, Zhou, Yuanyuan, Padture, Nitin P., Yang, Zhenhua, Guo, Yichen, Xue, Yuan, Kisslinger, Kim, Cotlet, Mircea, Nam, Chang-Yong, and Rafailovich, Miriam H. Fri . "Enhancing Chemical Stability and Suppressing Ion Migration in CH3NH3PbI3 Perovskite Solar Cells via Direct Backbone Attachment of Polyesters on Grain Boundaries". United States. https://doi.org/10.1021/acs.chemmater.0c00995. https://www.osti.gov/servlets/purl/1642408.
@article{osti_1642408,
title = {Enhancing Chemical Stability and Suppressing Ion Migration in CH3NH3PbI3 Perovskite Solar Cells via Direct Backbone Attachment of Polyesters on Grain Boundaries},
author = {Zhou, Yuchen and Yin, Yifan and Zuo, Xianghao and Wang, Likun and Li, Tai-De and Zhou, Yuanyuan and Padture, Nitin P. and Yang, Zhenhua and Guo, Yichen and Xue, Yuan and Kisslinger, Kim and Cotlet, Mircea and Nam, Chang-Yong and Rafailovich, Miriam H.},
abstractNote = {Organic–inorganic halide perovskites feature excellent optoelectronic properties but poor chemical stability. While passivating perovskite grain boundary (GB) by polymers shows prospects on long-term performance of perovskite solar cells (PSCs), its detailed impact on the ion migration phenomenon, which largely deteriorates the PSC stability, remains less probed. In this work, we introduce a new polar polymer, polycaprolactone (PCL), to passivate GBs of methylammonium lead triiodide (MAPbI3) perovskite with only 1–2 polymer monolayers via direct backbone attachment. The PSCs with passivated MAPbI3, using a classic but less stable Spiro-OMeTAD (2,2',7,7'-tetrakis[N,N-di(4-methoxyphenyl)amino]-9,9'-spirobifluorene) hole transport layer (HTL), exhibit improved power conversion efficiencies up to 20.1%, with 90% of the initial PCE being preserved after 400 h ambient storage, and 80% even after 100 h, 85 °C aging. The improved PSC stability indicates critical roles of PCL GB passivation in retarding moisture-induced decomposition and suppressing ion migration within the perovskite. Furthermore, time-of-flight secondary ion mass spectrometry reveals that I– ions can actively migrate into the electrode, HTL, and their interface in nonpassivated PSCs, even without an externally applied electric field, while such migration is significantly mitigated in PCL-passivated PSCs. This effective GB passivation by PCL suggests an important potential of polymer additives toward the development of stable high-performance PSCs.},
doi = {10.1021/acs.chemmater.0c00995},
journal = {Chemistry of Materials},
number = 12,
volume = 32,
place = {United States},
year = {2020},
month = {5}
}

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