Sol‐Gel Prepared Spinel HTLs for Assembling 20% Efficiency Perovskite Solar Cell in Air Without Using Anti‐Solvent and Toxic Solvent.

Low‐temperature sol‐gel prepared ZnCo2O4 spinel‐based thin films are developed as high‐performance hole transporting layer (HTL) for coating perovskite film (NA‐Psk) from the basic MAPbI3/ACN/CH3NH2 solution in air without using anti‐solvent. Inverted PSC based on 2 mole% (vs Zn) Cu2+ doped ZnCo2O4 (2%Cu@ZnCo2O4) HTL and NA‐Psk absorber exhibit the maximum power conversion efficiency (PCE) of 20.0% with no current hysteresis while the cell based on ZnCo2O4 and PEDOT:PSS HTL (using NA‐Psk absorber) achieves the PCE of 15.79% and 12.3% with a current hysteresis index of 9.8% and 32.4%, respectively. Without encapsulation, PSCs based on 2%Cu@ZnCo2O4, ZnCo2O4, and PEDOT:PSS HTLs maintain 90%, 77%, and 12%, respectively of the original efficiency by standing in ambient atmosphere (temperature: 20–25 °C, RH:30%–40%) for 1800 h. Large area (10 cm × 10 cm substrate) perovskite mini‐module (PSM) with PCE over 15% is also demonstrated by using sol‐gel prepared 2%Cu@ZnCo2O4 HTL. The poor photovoltaic performance of PEDOT:PSS HTL is due to the basic MAPbI3/ACN/CH3NH2 solution will deprotonate the acidic PEDOT:PSS to reduce its conductivity whereas ZnCo2O4 HTL are not affected by basic perovskite precursor solution. [ABSTRACT FROM AUTHOR]