Molecular Engineering of Triphenylamine-Based Hydrazone Sensitizers for High-Efficiency and Stable Quasi-Solid-State Dye-Sensitized Solar Cells Achieving 32.7% Indoor Light Conversion Efficiency
摘要
Two novel triphenylamine-based hydrazone organic sensitizers, TPH-1 and TPC-1, were designed and synthesized as co-sensitizers with the benchmark N719 dye for high-performance quasi-solid-state dye-sensitized solar cells (QSSE-DSSCs). Density functional theory (DFT) and reduced density gradient analyses revealed that introducing a cyano-carboxylic dual-acceptor system in TPC-1 enhances intramolecular charge transfer and electronic coupling with TiO2. Optical and electrochemical studies confirmed the broadened visible-light absorption and favorable energy-level alignment for efficient electron injection and dye regeneration. Under simulated one-sun illumination (AM 1.5G, 100 mW·cm−2), the TPC-1/N719 device delivered a power conversion efficiency of 11.23%. Notably, under indoor illumination at 1000 lx (0.283 mW·cm−2), the QSSE-based TPC-1/N719 cell achieved an outstanding light conversion efficiency of 32.7%, which exceeds the most recently reported indoor DSSCs operating under comparable illuminance and spectral conditions. Electrochemical impedance spectroscopy revealed suppressed charge recombination and extended electron lifetimes, while thermogravimetric and long-term stability tests demonstrated excellent thermal robustness and over 97% efficiency retention after 300 h of continuous illumination. These results demonstrate that molecular engineering of hydrazone-based triphenylamine sensitizers combined with quasi-solid-state electrolytes provides an effective strategy for simultaneously achieving high efficiency, excellent stability, and state-of-the-art indoor photovoltaic performance in DSSCs.