<p>The quest for high-efficiency and stable photoanodes remains a central challenge in dye-sensitized solar cells (DSSCs). Here, we report a hierarchical CNT-integrated lithium–zinc–aluminate (CNT–LiZn<sub>0.5</sub>Al<sub>2</sub>O<sub>4</sub>) spinel nanoarchitecture as a superior alternative to conventional CNT–ZnO and CNT–LiZn<sub>0.5</sub>O photoanodes. Using a combination of SILAR and doctor blade techniques, the nanocomposites were fabricated on FTO substrates and thoroughly characterized. X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analyses confirmed successful Li⁺ and Al<sup>3</sup>⁺ incorporation, driving a structural transition from wurtzite ZnO to a cubic spinel phase, effectively passivating defect states and tuning the electronic structure. UV–Vis Tauc analysis revealed significant bandgap narrowing from 3.04&#xa0;eV (CNT–ZnO) to 2.34&#xa0;eV (CNT–LiZn<sub>0.5</sub>Al<sub>2</sub>O<sub>4</sub>), thereby enhancing visible-light absorption. AFM and SEM studies further showed a highly textured, porous morphology, favorable for dye loading and light scattering. Combined with the CNT network’s superior charge transport, this structural and electronic synergy led to pronounced recombination suppression, as evidenced by quenched PL spectra. The resulting DSSCs exhibited stepwise performance improvement: CNT–ZnO (<i>η</i>  =  5.55%), CNT–LiZn<sub>0.5</sub>O (<i>η </i> =  7.19%), and a champion efficiency of 9.69% for CNT–LiZn<sub>0.5</sub>Al<sub>2</sub>O<sub>4</sub>, driven by a high <i>J</i><sub>sc</sub> of 19.8&#xa0;mA&#xa0;cm⁻<sup>2</sup>. This work demonstrates Li–Al co-doping within a CNT–spinel framework as an effective strategy for designing next-generation high-performance photovoltaic photoanodes.</p>

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Engineering bandgaps and charge dynamics: CNT-spinned LiZn0.5Al2O4 spinel nanoarchitectures for high-efficiency dye-sensitized solar cells

  • S. Nandhini,
  • R. Gayathri

摘要

The quest for high-efficiency and stable photoanodes remains a central challenge in dye-sensitized solar cells (DSSCs). Here, we report a hierarchical CNT-integrated lithium–zinc–aluminate (CNT–LiZn0.5Al2O4) spinel nanoarchitecture as a superior alternative to conventional CNT–ZnO and CNT–LiZn0.5O photoanodes. Using a combination of SILAR and doctor blade techniques, the nanocomposites were fabricated on FTO substrates and thoroughly characterized. X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analyses confirmed successful Li⁺ and Al3⁺ incorporation, driving a structural transition from wurtzite ZnO to a cubic spinel phase, effectively passivating defect states and tuning the electronic structure. UV–Vis Tauc analysis revealed significant bandgap narrowing from 3.04 eV (CNT–ZnO) to 2.34 eV (CNT–LiZn0.5Al2O4), thereby enhancing visible-light absorption. AFM and SEM studies further showed a highly textured, porous morphology, favorable for dye loading and light scattering. Combined with the CNT network’s superior charge transport, this structural and electronic synergy led to pronounced recombination suppression, as evidenced by quenched PL spectra. The resulting DSSCs exhibited stepwise performance improvement: CNT–ZnO (η  =  5.55%), CNT–LiZn0.5O (η  =  7.19%), and a champion efficiency of 9.69% for CNT–LiZn0.5Al2O4, driven by a high Jsc of 19.8 mA cm⁻2. This work demonstrates Li–Al co-doping within a CNT–spinel framework as an effective strategy for designing next-generation high-performance photovoltaic photoanodes.