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<p>Interfacial tailoring is one of the main approaches for improving the efficiency and sustained device stability of dye-based sensitized solar cells. In this investigation, we propose the first-time use of a novel ionic liquid, N-(carboxymethyl)-trimethylammonium bromide<i>,</i> as a multifunctional additive integrated into the electrolyte of ZnO-based DSSCs. This ionic liquid possesses a tight-structured quaternary ammonium center with a carboxymethyl moiety, enabling effective coordination with ZnO surfaces and enhanced ionic mobility. The low steric bulk promotes intimate interfacial contact, while the carboxyl group aids passivation via electrostatic interaction and hydrogen bonding, efficiently suppressing charge recombination at the photoanode–electrolyte interface. An optimized framework integrating the novel ionic liquid, hybrid sensitization using D149 and polyamide-based dyes, and thermal annealing led to a substantial improvement in device efficiency. ZnO NPs thermally annealed at 450&#xa0;°C exhibited high crystallinity (35&#xa0;nm) with minimal defect density, facilitating more efficient dye adsorption and charge transport. In contrast, thermal annealing at 300&#xa0;°C and 600&#xa0;°C resulted in inadequate grain growth and reduced efficiency. Combined sensitization using D149 and a polyamide-based dye extended the light absorption and enhanced charge carrier injection efficiency. A cobalt-containing redox mediator reduced recombination and enhanced photovoltage. The integration of the novel ionic liquid (IL) annealed at 450&#xa0;°C, increased power conversion efficiency (PCE) to 8.2%, surpassing that of devices thermally annealed at 300&#xa0;°C (7.4%) and 600&#xa0;°C (7.7%). The optimized solar cell exhibited a V<sub>oc</sub> of 0.700&#xa0;V, a J<sub>sc</sub> of 17.8&#xa0;mA&#xa0;cm⁻<sup>2</sup>, and improved IPCE, achieving one of the highest efficiencies reported in ZnO nanoparticle-based DSSCs. This research work demonstrates a strong interfacial engineering framework targeting next-generation, high-performance DSSCs by leveraging ionic liquid technology, synergistic sensitization, and precise thermal tuning.</p>

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ZnO nanoparticle-based DSSCs via interfacial engineering using carboxymethyl-functionalized ionic liquid and thermal annealing

  • 期刊论文

  • 发表日期：

    2025年10月15日

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  • Diksha Saini,
  • Satbir Singh,
  • Gagandeep Singh,
  • Gurpreet Singh,
  • Shashi Bhushan Rana

摘要

Interfacial tailoring is one of the main approaches for improving the efficiency and sustained device stability of dye-based sensitized solar cells. In this investigation, we propose the first-time use of a novel ionic liquid, N-(carboxymethyl)-trimethylammonium bromide, as a multifunctional additive integrated into the electrolyte of ZnO-based DSSCs. This ionic liquid possesses a tight-structured quaternary ammonium center with a carboxymethyl moiety, enabling effective coordination with ZnO surfaces and enhanced ionic mobility. The low steric bulk promotes intimate interfacial contact, while the carboxyl group aids passivation via electrostatic interaction and hydrogen bonding, efficiently suppressing charge recombination at the photoanode–electrolyte interface. An optimized framework integrating the novel ionic liquid, hybrid sensitization using D149 and polyamide-based dyes, and thermal annealing led to a substantial improvement in device efficiency. ZnO NPs thermally annealed at 450 °C exhibited high crystallinity (35 nm) with minimal defect density, facilitating more efficient dye adsorption and charge transport. In contrast, thermal annealing at 300 °C and 600 °C resulted in inadequate grain growth and reduced efficiency. Combined sensitization using D149 and a polyamide-based dye extended the light absorption and enhanced charge carrier injection efficiency. A cobalt-containing redox mediator reduced recombination and enhanced photovoltage. The integration of the novel ionic liquid (IL) annealed at 450 °C, increased power conversion efficiency (PCE) to 8.2%, surpassing that of devices thermally annealed at 300 °C (7.4%) and 600 °C (7.7%). The optimized solar cell exhibited a Voc of 0.700 V, a Jsc of 17.8 mA cm⁻2, and improved IPCE, achieving one of the highest efficiencies reported in ZnO nanoparticle-based DSSCs. This research work demonstrates a strong interfacial engineering framework targeting next-generation, high-performance DSSCs by leveraging ionic liquid technology, synergistic sensitization, and precise thermal tuning.