<p>The exploration of novel Pt-free counter electrodes (CE) is a vital step in advancing the sustainability and efficiency of dye-sensitized solar cells (DSSCs). In this work, we designed a novel two-dimensional (2D) reduced graphene oxide (rGO)-decorated mixed-phase MoS<sub>2</sub>/Ni<sub><i>x</i></sub>Co<sub>1−<i>x</i></sub>S<sub>2</sub> composite as a high-performance CE via a hydrothermal method. Analysis of the crystal structure and morphology of the as-prepared MoS<sub>2</sub>/Ni<sub><i>x</i></sub>Co<sub>1−<i>x</i></sub>S<sub>2</sub>@rGO hybrids revealed the presence of MoS<sub>2</sub> nanostructures exhibiting a layered sheet and mixed-phase Ni<sub><i>x</i></sub>Co<sub>1−<i>x</i></sub>S<sub>2</sub> sphere-like morphology uniformly distributed on the 2D rGO sheets, enhancing the active surface area (131.3&#xa0;m<sup>2</sup>/g), reducing the crystallite size (41&#xa0;nm), and facilitating efficient charge transport. Ultraviolet–visible diffuse reflectance spectroscopy (UV–Vis DRS) studies revealed a significant reduction in bandgap from 2.22&#xa0;eV (MoS<sub>2</sub>/Ni<sub><i>x</i></sub>Co<sub>1−<i>x</i></sub>S<sub>2</sub>) to 1.74&#xa0;eV (MoS<sub>2</sub>/Ni<sub><i>x</i></sub>Co<sub>1−<i>x</i></sub>S<sub>2</sub>@rGO), facilitating superior visible light absorption and efficient light harvesting. Electrochemical evaluations demonstrated excellent redox kinetics, with MoS<sub>2</sub>/Ni<sub><i>x</i></sub>Co<sub>1−<i>x</i></sub>S<sub>2</sub>@20% rGO achieving low charge transfer resistance (189&#xa0;Ω cm<sup>2</sup>) and high exchange current density (3.87&#xa0;mA/cm<sup>2</sup>), surpassing both pristine MoS<sub>2</sub>/Ni<sub><i>x</i></sub>Co<sub>1−<i>x</i></sub>S<sub>2</sub> and Pt-based electrodes. The MoS<sub>2</sub>/Ni<sub><i>x</i></sub>Co<sub>1−<i>x</i></sub>S<sub>2</sub>@20%rGO CE achieved power conversion efficiency (PCE) of 5.53%, with high short-circuit current density (11.97&#xa0;mA/cm<sup>2</sup>) and excellent stability, retaining 96% efficiency over 60&#xa0;days. The enhanced performance is attributed to rGO's role in improving charge transport, reducing recombination, and providing structural stability, positioning MoS<sub>2</sub>/Ni<sub><i>x</i></sub>Co<sub>1−<i>x</i></sub>S<sub>2</sub>@20%rGO as a cost-effective alternative to Pt-based CE for practical DSSC applications.</p>

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2D rGO-Decorated Mixed-Phase MoS2/NixCo1−x S2 Composite: A High-Performance Counter Electrode for DSSC Applications

  • D. Zamrooth,
  • P. Sathish Babu,
  • T. SanthanaKrishnan,
  • G. Soorya Priya

摘要

The exploration of novel Pt-free counter electrodes (CE) is a vital step in advancing the sustainability and efficiency of dye-sensitized solar cells (DSSCs). In this work, we designed a novel two-dimensional (2D) reduced graphene oxide (rGO)-decorated mixed-phase MoS2/NixCo1−xS2 composite as a high-performance CE via a hydrothermal method. Analysis of the crystal structure and morphology of the as-prepared MoS2/NixCo1−xS2@rGO hybrids revealed the presence of MoS2 nanostructures exhibiting a layered sheet and mixed-phase NixCo1−xS2 sphere-like morphology uniformly distributed on the 2D rGO sheets, enhancing the active surface area (131.3 m2/g), reducing the crystallite size (41 nm), and facilitating efficient charge transport. Ultraviolet–visible diffuse reflectance spectroscopy (UV–Vis DRS) studies revealed a significant reduction in bandgap from 2.22 eV (MoS2/NixCo1−xS2) to 1.74 eV (MoS2/NixCo1−xS2@rGO), facilitating superior visible light absorption and efficient light harvesting. Electrochemical evaluations demonstrated excellent redox kinetics, with MoS2/NixCo1−xS2@20% rGO achieving low charge transfer resistance (189 Ω cm2) and high exchange current density (3.87 mA/cm2), surpassing both pristine MoS2/NixCo1−xS2 and Pt-based electrodes. The MoS2/NixCo1−xS2@20%rGO CE achieved power conversion efficiency (PCE) of 5.53%, with high short-circuit current density (11.97 mA/cm2) and excellent stability, retaining 96% efficiency over 60 days. The enhanced performance is attributed to rGO's role in improving charge transport, reducing recombination, and providing structural stability, positioning MoS2/NixCo1−xS2@20%rGO as a cost-effective alternative to Pt-based CE for practical DSSC applications.