Defect Passivation and Enhanced Hole Extraction in Inverted Perovskite Solar Cells via CeO2@MoS2 Interfacial Engineering

Nanomaterial-based hole transport layers (HTLs) play a vital role in regulating interfacial charge extraction and recombination in perovskite solar cells (PSCs). To improve PSC efficiency, hydrothermally synthesized CeO₂@MoS₂ nanocomposites (CM NCs) were incorporated as an interfacial buffer layer into a NiO_X/MeO-2PACz HTL. The introduction of CM NCs induces strong interfacial interactions, where Mo sites in MoS₂ interact with NiO_X, modulating the Ni²⁺/Ni³⁺ ratio and reducing the interfacial trap density. Moreover, CeO₂ promotes the formation of oxygen vacancies, collectively improving the conductivity and hole transport capability of the NiO_X HTL. The MoS₂-grafted CeO₂ interlayer effectively tailors the interfacial energetics and creates an effective channel for hole transfer, thereby reducing open-circuit voltage (V_OC) loss and enhancing device performance. This interface modification efficiently enhances hole extraction, and non-radiative recombination is effectively suppressed at the NiO_X/MeO-2PACz/perovskite interface. Thereby, incorporating 2 vol% CM NCs into PSCs achieved a power conversion efficiency (PCE) of 17.93%, compared to 17.50% for a 1 vol% CM NCs-based device and 17.01% for the unmodified control device. The enhanced performance at the optimized CM NCs concentration is attributed to effective defect passivation, reduced V_OC loss, and improved interfacial band alignment, which together facilitate hole extraction and suppress non-radiative recombination. However, excessive CM NCs incorporation (4 vol%) leads to increased interfacial resistance, partial hole blocking effects associated with the n-type nature of CeO₂, and aggravated recombination, resulting in degraded device performance. These results demonstrate that precise control over CM NCs interlayer thickness and concentration is critical for maximizing device performance, providing a robust strategy for designing high-efficiency and stable NiO_X-based PSCs and advancing nanocomposite-enabled interfacial engineering for photovoltaic applications.