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Updated: Jun 16, 2026

Influence of Hybrid Perovskite Fabrication Methods on Film Formation, Electronic Structure, and Solar Cell Performance
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Stoichiometry-Controlled Cobalt Sulfide-Based Hole Transport Layers for Perovskite Solar Cells.

Bonkee Koo1, Wooyeon Kim1, Young Kim1

  • 1Department of Chemical Engineering, Hanyang University, 222 Wangsimni-ro, Seongdong-gu, Seoul, 04763, Republic of Korea.

Small (Weinheim an Der Bergstrasse, Germany)
|September 19, 2025
PubMed
Summary

Dopant-free cobalt sulfide (CoxSy) hole transport layers (HTLs) improve perovskite solar cell (PSC) performance and stability. A bilayer HTL achieved a 24.41% power conversion efficiency, surpassing traditional methods.

Keywords:
cobalt sulfidehole transporting materialperovskite solar cellsp‐type nanocrystals

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Area of Science:

  • Materials Science
  • Photovoltaics
  • Inorganic Chemistry

Background:

  • Conventional hole transport layers (HTLs) in perovskite solar cells (PSCs) rely on extrinsic doping, which often leads to performance-limiting issues like structural disorder and charge trapping.
  • Developing dopant-free HTLs is crucial for enhancing PSC stability and efficiency.

Purpose of the Study:

  • To introduce and investigate cobalt sulfide (CoxSy) as a novel, dopant-free inorganic HTL for PSCs.
  • To explore the effect of controlled stoichiometry in CoxSy on band alignment and device performance.
  • To enhance hole transport and device efficiency using a CoxSy/spiro-OMeTAD bilayer HTL.

Main Methods:

  • Synthesis of phase-pure CoxSy (CoS, Co4S3, Co9S8) via a hot-injection method, controlling precursor injection temperature.
  • Fabrication of PSCs utilizing the synthesized CoxSy as HTLs.
  • Characterization of PSCs with single-layer and bilayer (CoxSy/spiro-OMeTAD) HTLs, evaluating power conversion efficiency (PCE), open-circuit voltage (Voc), and stability.

Main Results:

  • Stoichiometrically defined CoxSy HTLs exhibited distinct valence band positions, allowing tunable band alignment with perovskite layers.
  • PSCs with single-layer CoxSy HTLs achieved PCEs up to 18.65% and Voc up to 1.09 V.
  • A PSC with a Co4S3/spiro-OMeTAD bilayer HTL demonstrated a high PCE of 24.41%.
  • CoxSy-based PSCs showed improved thermal and operational stability compared to spiro-OMeTAD-only devices.

Conclusions:

  • Dopant-free CoxSy materials are effective inorganic HTLs for high-performance PSCs.
  • Controlled stoichiometry and bilayer architectures offer pathways to optimize band alignment and charge transport.
  • This strategy highlights the potential of underutilized nonstoichiometric materials for advancing photovoltaic technology.