Abstract

Top-performing metal halide perovskite solar cells (PSCs) with a solar-to-electric power conversion efficiency (PCE) beyond 22% often are fabricated using sequential deposition method under a controlled atmosphere in a glovebox. Meanwhile, a maximum efficiency of 13.59% was reported for CH3NH3PbI3-based PSC using a vapor-assisted solution processing method (VASP) at fully ambient air condition (in terms of both atmosphere and pressure). Herein, we introduce island-like ZnAl-layered double hydroxide (ZnAl-LDH) precursor as middle layer arrays assembling onto the TiO2 nanoparticles (NPs) of mesoporous TiO2 (mp-TiO2) texture to obtain a surged PCE up to 18.54% with a significant performance improvement of 36.4% for fully ambient VASP processed PSCs. Moreover, this enables us to fabricate hole transporting material-free PSC with a maximum efficiency of 14.45% by using ZnAl-LDH permeated mp-TiO2 as the underneath scaffold. The synergistic effect between ZnO and ZnAl2O4 semiconductors—resulting from LDH calcination—and TiO2 NPs leads to more effective electron extraction, reduces electron back transfer as a recombination barrier, and acts as an interfacial barrier between the UV-photocatalytically active TiO2 NPs and perovskite film as well.

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