4.7 Article

Low-Temperature Microwave Processed TiO2 as an Electron Transport Layer for Enhanced Performance and Atmospheric Stability in Planar Perovskite Solar Cells

Journal

ACS APPLIED ENERGY MATERIALS
Volume 5, Issue 3, Pages 2679-2696

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsaem.1c02675

Keywords

perovskite solar cells; low-temperature; microwave processing; TiO2; electron transport layer; degradation; strain

Funding

  1. Department of Science and Technology (DST), India under the Clean Energy Research Initiative [DST/TMD/CERI/C140(G)]
  2. Science and Engineering Research Board (SERB), India [EMR/2015/000490, SRG/2020/001771]
  3. UKRI Global Challenge Research Fund through project SUNRISE [EP/P032591/1]

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Low-temperature solution processed planar perovskite solar cells (PSCs) using MW-TiO2 as an ETL demonstrate improved efficiency, flexibility, and stability due to the reduced defects, enhanced conductivity, and alleviated strain.
Low-temperature (similar to 150 degrees C) solution processed planar perovskite solar cells (PSCs) using TiO2 as an electron transport layer (ETL) offer promise for a simple fabrication methodology and compatibility with polymeric substrates and perovskite-based tandem devices. However, the amorphous nature and presence of trap states on the low-temperature TiO2 surface hinder the effective carrier transport. Further, perovskite crystallization on ETL develops lattice strain resulting in the creation of unwanted defect centers. Herein, a low-temperature microwave processed compact TiO2 (MW-TiO2) film is reported that possesses lower surface oxygen vacancy defects and enhanced conductivity and promotes efficient electron extraction owing to the enhanced built-in potential (V-bi) at the MW-TiO2/perovskite interface. The suppressed heterogeneous nucleation of MAPbI(3) crystals on the less defective MW-TiO2 surface relieves the interfacial strain, thereby making it a superior template for the growth of strain relaxed, high-quality perovskite films with a more n-type character having larger grains, resulting in suppressed interfacial/surface and bulk trap density. Further, MW-TiO2 mitigates the interfacial energetic disorder and Urbach energy owing to reduced strain, thereby boosting the open-circuit voltage (V-oc) by 40 mV, while improved optoelectronic properties of MW-TiO2, lower interfacial charge transfer resistance, and high-quality perovskite films simultaneously improve the short-circuit current density (k) and fill factor (FF) by 6.82 and 9.37%, respectively, over HT-TiO2 based devices. Compared to high-temperature (500 degrees C) annealed TiO2 based MAPbI(3) planar PSCs, MW-TiO2 based devices exhibited a substantial performance enhancement of 22%, leading to the best efficiency of similar to 18% and superior atmospheric stability (25 degrees C, 55% relative humidity) while maintaining 80% of its initial value after 2500 h. Experimental results are validated by device simulation studies with model accounting for trap-assisted interfacial and bulk recombination. Finally, MW processed flexible devices maintained over 80% of their initial power conversion efficiency (PCE) after 1000 bending cycles, thereby exhibiting excellent mechanical robustness. These results elucidate the critical role of MW-TiO2 in rendering improved performance, flexibility, and stability in low-temperature PSCs.

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