DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Rapid Aqueous Spray Fabrication of Robust NiO x: A Simple and Scalable Platform for Efficient Perovskite Solar Cells

Abstract

Abstract Organometal halide perovskites have powerful intrinsic potential to drive next‐generation solar technology, but their insufficient thermomechanical reliability and unproven large‐area manufacturability limit competition with incumbent silicon photovoltaics. This work addresses these limitations by leveraging large‐area processing and robust inorganic hole transport layers (HTLs). Inverted perovskite solar cells utilizing NiO x HTLs deposited by rapid aqueous spray‐coating that outperform spin‐coated NiO x and lead to a 5× improvement in the fracture energy ( G c ), a primary metric of thermomechanical stability, are presented. The morphology, chemical composition, and optoelectronic properties of the NiO x films are characterized to understand and optimize compatibility with an archetypal double cation perovskite, Cs .17 FA .83 Pb(Br .17 I .83 ) 3 . Perovskite solar cells with sprayed NiO x show higher photovoltaic performance, exhibiting up to 82% fill factor and 17.7% power conversion efficiency (PCE)—the highest PCE reported for inverted cell with scalable charge transport layers—as well as excellent stability under full illumination and after 4000 h aging in inert conditions at room temperature. By utilizing open‐air techniques and aqueous precursors, this combination of robust materials and low‐cost processing provides a platform for scaling perovskite modules with long‐term reliability.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Stanford Univ., CA (United States)
Publication Date:
Research Org.:
Stanford Univ., CA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF)
OSTI Identifier:
1613525
Alternate Identifier(s):
OSTI ID: 1513033
Grant/Contract Number:  
EE0008559; ECCS-1542152
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 9; Journal Issue: 19; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Chemistry; energy & fuels; materials science; physics; mechanical reliability; metal oxide transport layers; perovskite solar cells; scalable deposition

Citation Formats

Scheideler, William J., Rolston, Nicholas, Zhao, Oliver, Zhang, Jinbao, and Dauskardt, Reinhold H. Rapid Aqueous Spray Fabrication of Robust NiO x: A Simple and Scalable Platform for Efficient Perovskite Solar Cells. United States: N. p., 2019. Web. doi:10.1002/aenm.201803600.
Scheideler, William J., Rolston, Nicholas, Zhao, Oliver, Zhang, Jinbao, & Dauskardt, Reinhold H. Rapid Aqueous Spray Fabrication of Robust NiO x: A Simple and Scalable Platform for Efficient Perovskite Solar Cells. United States. https://doi.org/10.1002/aenm.201803600
Scheideler, William J., Rolston, Nicholas, Zhao, Oliver, Zhang, Jinbao, and Dauskardt, Reinhold H. Wed . "Rapid Aqueous Spray Fabrication of Robust NiO x: A Simple and Scalable Platform for Efficient Perovskite Solar Cells". United States. https://doi.org/10.1002/aenm.201803600. https://www.osti.gov/servlets/purl/1613525.
@article{osti_1613525,
title = {Rapid Aqueous Spray Fabrication of Robust NiO x: A Simple and Scalable Platform for Efficient Perovskite Solar Cells},
author = {Scheideler, William J. and Rolston, Nicholas and Zhao, Oliver and Zhang, Jinbao and Dauskardt, Reinhold H.},
abstractNote = {Abstract Organometal halide perovskites have powerful intrinsic potential to drive next‐generation solar technology, but their insufficient thermomechanical reliability and unproven large‐area manufacturability limit competition with incumbent silicon photovoltaics. This work addresses these limitations by leveraging large‐area processing and robust inorganic hole transport layers (HTLs). Inverted perovskite solar cells utilizing NiO x HTLs deposited by rapid aqueous spray‐coating that outperform spin‐coated NiO x and lead to a 5× improvement in the fracture energy ( G c ), a primary metric of thermomechanical stability, are presented. The morphology, chemical composition, and optoelectronic properties of the NiO x films are characterized to understand and optimize compatibility with an archetypal double cation perovskite, Cs .17 FA .83 Pb(Br .17 I .83 ) 3 . Perovskite solar cells with sprayed NiO x show higher photovoltaic performance, exhibiting up to 82% fill factor and 17.7% power conversion efficiency (PCE)—the highest PCE reported for inverted cell with scalable charge transport layers—as well as excellent stability under full illumination and after 4000 h aging in inert conditions at room temperature. By utilizing open‐air techniques and aqueous precursors, this combination of robust materials and low‐cost processing provides a platform for scaling perovskite modules with long‐term reliability.},
doi = {10.1002/aenm.201803600},
journal = {Advanced Energy Materials},
number = 19,
volume = 9,
place = {United States},
year = {Wed Mar 27 00:00:00 EDT 2019},
month = {Wed Mar 27 00:00:00 EDT 2019}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 51 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

A Universal Deposition Protocol for Planar Heterojunction Solar Cells with High Efficiency Based on Hybrid Lead Halide Perovskite Families
journal, October 2016

  • Conings, Bert; Babayigit, Aslihan; Klug, Matthew T.
  • Advanced Materials, Vol. 28, Issue 48
  • DOI: 10.1002/adma.201603747

Enhancing Photovoltaic Performance of Inverted Planar Perovskite Solar Cells by Cobalt-Doped Nickel Oxide Hole Transport Layer
journal, April 2018

  • Xie, Yulin; Lu, Kai; Duan, Jiashun
  • ACS Applied Materials & Interfaces, Vol. 10, Issue 16
  • DOI: 10.1021/acsami.8b01683

Room-Temperature-Sputtered Nanocrystalline Nickel Oxide as Hole Transport Layer for p–i–n Perovskite Solar Cells
journal, October 2018

  • Aydin, Erkan; Troughton, Joel; De Bastiani, Michele
  • ACS Applied Energy Materials, Vol. 1, Issue 11
  • DOI: 10.1021/acsaem.8b01263

Vertical recrystallization for highly efficient and stable formamidinium-based inverted-structure perovskite solar cells
journal, January 2017

  • Xie, Fengxian; Chen, Chun-Chao; Wu, Yongzhen
  • Energy & Environmental Science, Vol. 10, Issue 9
  • DOI: 10.1039/C7EE01675A

Spray-combustion synthesis: Efficient solution route to high-performance oxide transistors
journal, March 2015

  • Yu, Xinge; Smith, Jeremy; Zhou, Nanjia
  • Proceedings of the National Academy of Sciences, Vol. 112, Issue 11
  • DOI: 10.1073/pnas.1501548112

23.6%-efficient monolithic perovskite/silicon tandem solar cells with improved stability
journal, February 2017

  • Bush, Kevin A.; Palmstrom, Axel F.; Yu, Zhengshan J.
  • Nature Energy, Vol. 2, Issue 4
  • DOI: 10.1038/nenergy.2017.9

Perovskite ink with wide processing window for scalable high-efficiency solar cells
journal, March 2017


Critical Role of Interface and Crystallinity on the Performance and Photostability of Perovskite Solar Cell on Nickel Oxide
journal, December 2017

  • Nie, Wanyi; Tsai, Hsinhan; Blancon, Jean-Christophe
  • Advanced Materials, Vol. 30, Issue 5
  • DOI: 10.1002/adma.201703879

Perovskite Photovoltaics: The Path to a Printable Terawatt-Scale Technology
journal, October 2017


A solution processed nanostructured p-type NiO electrode for efficient inverted perovskite solar cells
journal, January 2016

  • Mali, Sawanta S.; Kim, Hyungjin; Shim, Sang Eun
  • Nanoscale, Vol. 8, Issue 46
  • DOI: 10.1039/C6NR06670D

Investigation of the Changes in Electronic Properties of Nickel Oxide (NiO x ) Due to UV/Ozone Treatment
journal, May 2017

  • Islam, Raisul; Chen, Gang; Ramesh, Pranav
  • ACS Applied Materials & Interfaces, Vol. 9, Issue 20
  • DOI: 10.1021/acsami.7b01629

Efficient and stable large-area perovskite solar cells with inorganic charge extraction layers
journal, October 2015


Decohesion Kinetics of PEDOT:PSS Conducting Polymer Films
journal, October 2013

  • Dupont, Stephanie R.; Novoa, Fernando; Voroshazi, Eszter
  • Advanced Functional Materials, Vol. 24, Issue 9
  • DOI: 10.1002/adfm.201302174

Efficient CH 3 NH 3 PbI 3 Perovskite Solar Cells Employing Nanostructured p-Type NiO Electrode Formed by a Pulsed Laser Deposition
journal, June 2015

  • Park, Jong Hoon; Seo, Jangwon; Park, Sangman
  • Advanced Materials, Vol. 27, Issue 27
  • DOI: 10.1002/adma.201500523

An ultra-thin, un-doped NiO hole transporting layer of highly efficient (16.4%) organic–inorganic hybrid perovskite solar cells
journal, January 2016

  • Seo, Seongrok; Park, Ik Jae; Kim, Myungjun
  • Nanoscale, Vol. 8, Issue 22
  • DOI: 10.1039/C6NR01601D

Molecular Network Reinforcement of Sol–Gel Glasses
journal, November 2007


High-Performance ZnO Transistors Processed Via an Aqueous Carbon-Free Metal Oxide Precursor Route at Temperatures Between 80-180 °C
journal, June 2013


Hexaaqua Metal Complexes for Low-Temperature Formation of Fully Metal Oxide Thin-Film Transistors
journal, August 2015


Cesium-containing triple cation perovskite solar cells: improved stability, reproducibility and high efficiency
journal, January 2016

  • Saliba, Michael; Matsui, Taisuke; Seo, Ji-Youn
  • Energy & Environmental Science, Vol. 9, Issue 6
  • DOI: 10.1039/C5EE03874J

Correlation between Chemical and Electronic Properties of Solution-Processed Nickel Oxide
journal, June 2018

  • Ullrich, Florian; Hillebrandt, Sabina; Hietzschold, Sebastian
  • ACS Applied Energy Materials, Vol. 1, Issue 7
  • DOI: 10.1021/acsaem.8b00284

Gas Quenching for Perovskite Thin Film Deposition
journal, July 2018


Overcoming the Limitations of Sputtered Nickel Oxide for High-Efficiency and Large-Area Perovskite Solar Cells
journal, October 2017


Mechanical integrity of solution-processed perovskite solar cells
journal, December 2016


Synthesis and use of a hyper-connecting cross-linking agent in the hole-transporting layer of perovskite solar cells
journal, January 2017

  • Watson, Brian L.; Rolston, Nicholas; Bush, Kevin A.
  • Journal of Materials Chemistry A, Vol. 5, Issue 36
  • DOI: 10.1039/C7TA05004F

Compositional Engineering for Efficient Wide Band Gap Perovskites with Improved Stability to Photoinduced Phase Segregation
journal, January 2018


A dopant-free hole-transporting material for efficient and stable perovskite solar cells
journal, January 2014

  • Liu, Jian; Wu, Yongzhen; Qin, Chuanjiang
  • Energy Environ. Sci., Vol. 7, Issue 9
  • DOI: 10.1039/C4EE01589D

Improved air stability of perovskite solar cells via solution-processed metal oxide transport layers
journal, October 2015


Engineered optical and electrical performance of rf–sputtered undoped nickel oxide thin films for inverted perovskite solar cells
journal, April 2018


The chemistry of the sol-gel process
journal, February 1989


Perovskite photovoltaics: life-cycle assessment of energy and environmental impacts
journal, January 2015

  • Gong, Jian; Darling, Seth B.; You, Fengqi
  • Energy & Environmental Science, Vol. 8, Issue 7
  • DOI: 10.1039/C5EE00615E

Overcoming ultraviolet light instability of sensitized TiO2 with meso-superstructured organometal tri-halide perovskite solar cells
journal, December 2013

  • Leijtens, Tomas; Eperon, Giles E.; Pathak, Sandeep
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms3885

Design and understanding of encapsulated perovskite solar cells to withstand temperature cycling
journal, January 2018

  • Cheacharoen, Rongrong; Rolston, Nicholas; Harwood, Duncan
  • Energy & Environmental Science, Vol. 11, Issue 1
  • DOI: 10.1039/C7EE02564E

Radiative efficiency of lead iodide based perovskite solar cells
journal, August 2014

  • Tvingstedt, Kristofer; Malinkiewicz, Olga; Baumann, Andreas
  • Scientific Reports, Vol. 4, Issue 1
  • DOI: 10.1038/srep06071

Effect of Cation Composition on the Mechanical Stability of Perovskite Solar Cells
journal, December 2017

  • Rolston, Nicholas; Printz, Adam D.; Tracy, Jared M.
  • Advanced Energy Materials, Vol. 8, Issue 9
  • DOI: 10.1002/aenm.201702116

One-step deposition by slot-die coating of mixed lead halide perovskite for photovoltaic applications
journal, January 2017


Molecule-Doped Nickel Oxide: Verified Charge Transfer and Planar Inverted Mixed Cation Perovskite Solar Cell
journal, March 2018


Highly efficient and stable planar perovskite solar cells by solution-processed tin oxide
journal, January 2016

  • Anaraki, Elham Halvani; Kermanpur, Ahmad; Steier, Ludmilla
  • Energy & Environmental Science, Vol. 9, Issue 10
  • DOI: 10.1039/C6EE02390H

Scalable fabrication of perovskite solar cells
journal, March 2018


Low-Temperature-Processed Printed Metal Oxide Transistors Based on Pure Aqueous Inks
journal, March 2017

  • Scheideler, William J.; Kumar, Rajan; Zeumault, Andre R.
  • Advanced Functional Materials, Vol. 27, Issue 14
  • DOI: 10.1002/adfm.201606062

Works referencing / citing this record:

Perovskite Solar Cells Using Surface‐Modified NiO x Nanoparticles as Hole Transport Materials in n‐i‐p Configuration
journal, May 2019


Large-area, green solvent spray deposited nickel oxide films for scalable fabrication of triple-cation perovskite solar cells
journal, January 2020

  • Kumar, Neetesh; Lee, Hock Beng; Hwang, Sunbin
  • Journal of Materials Chemistry A, Vol. 8, Issue 6
  • DOI: 10.1039/c9ta13528f

Plasma-assisted atomic layer deposition of nickel oxide as hole transport layer for hybrid perovskite solar cells
journal, January 2019

  • Koushik, Dibyashree; Jošt, Marko; Dučinskas, Algirdas
  • Journal of Materials Chemistry C, Vol. 7, Issue 40
  • DOI: 10.1039/c9tc04282b