Scholarlink

Context <p>The rational design of metal-free organic sensitizers is critical for developing cost-effective, high-efficiency dye-sensitized solar cells (DSSCs). This study uses density functional theory (DFT) to explore how modifying the triphenylamine (TPA) donor with pyridine rings or amino groups at ortho-, meta-, and para-positions affects the optoelectronic properties of D-π-A sensitizers. Our calculations show that para-position amino substitution (dye N3) yields the most red-shifted absorption (<InlineEquation ID="IEq1"> <InlineMediaObject> <ImageObject Color="BlackWhite" FileRef="894_2025_6498_Article_IEq1.gif" Format="GIF" Height="16" Rendition="HTML" Resolution="72" Type="Linedraw" Width="36" /> </InlineMediaObject> <EquationSource Format="TEX">\({\lambda }_{max}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mi>λ</mi> <mrow> <mi mathvariant="italic">max</mi> </mrow> </msub> </math></EquationSource> </InlineEquation>=523, 50 nm beyond reference dyes), the highest theoretical open-circuit voltage (Voc = 1.77 eV, 0.3 eV higher than others), and enhanced charge transfer efficiency. These findings highlight para-position amines as a promising strategy for optimizing DSSC performance and identify N3 as a prime candidate for synthesis and experimental validation.</p> Methods <p>Ground-state geometries, vibrational frequencies, and frontier molecular orbitals were calculated using the M06 functional with the 6-31G(d) basis set, chosen for its accuracy in organic systems. UV–Vis absorption and excited-state properties were predicted via time-dependent DFT (TD-DFT) with the M06-2X functional, optimized for excited-state accuracy, and the 6-31G(d) basis set. Solvation effects in acetonitrile were modeled using the IEF-PCM polarizable continuum model. Calculations were performed with Gaussian 16.</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Rational design of triphenylamine-based sensitizers for DSSCs: a DFT comparison of pyridine and amine donor substituents

  • 期刊论文

  • 发表日期：

    2025年9月25日

查看全文
  • Damián Delgado-Montiel,
  • Norma Flores-Holguín,
  • Jesús Baldenebro-López,
  • Rody Soto-Rojo,
  • Manuel Luque-Roman,
  • Tomás Delgado-Montiel,
  • Daniel Glossman-Mitnik

摘要

Context

The rational design of metal-free organic sensitizers is critical for developing cost-effective, high-efficiency dye-sensitized solar cells (DSSCs). This study uses density functional theory (DFT) to explore how modifying the triphenylamine (TPA) donor with pyridine rings or amino groups at ortho-, meta-, and para-positions affects the optoelectronic properties of D-π-A sensitizers. Our calculations show that para-position amino substitution (dye N3) yields the most red-shifted absorption ( \({\lambda }_{max}\) λ max =523, 50 nm beyond reference dyes), the highest theoretical open-circuit voltage (Voc = 1.77 eV, 0.3 eV higher than others), and enhanced charge transfer efficiency. These findings highlight para-position amines as a promising strategy for optimizing DSSC performance and identify N3 as a prime candidate for synthesis and experimental validation.

Methods

Ground-state geometries, vibrational frequencies, and frontier molecular orbitals were calculated using the M06 functional with the 6-31G(d) basis set, chosen for its accuracy in organic systems. UV–Vis absorption and excited-state properties were predicted via time-dependent DFT (TD-DFT) with the M06-2X functional, optimized for excited-state accuracy, and the 6-31G(d) basis set. Solvation effects in acetonitrile were modeled using the IEF-PCM polarizable continuum model. Calculations were performed with Gaussian 16.