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Through-Space Charge Transfer Complexes Based on Terpyridine Bi-Functionalization for Efficient Solar-Driven H2O2

Manman Dai1, Ningxu Han1, Xiang Li2

  • 1State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun, Jilin, 130012, P.R. China.

Angewandte Chemie (International Ed. in English)
|December 18, 2025
PubMed
Summary
This summary is machine-generated.

Researchers developed a terpyridine functionalization strategy for precise control over donor-acceptor stacking, enhancing through-space charge transfer (TSCT) for efficient photocatalysis. This led to a new material with double the H2O2 production efficiency compared to a previous design.

Keywords:
Single crystalSupramolecular architecturesTerpyridineThrough‐space charge transfer

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Area of Science:

  • Supramolecular Chemistry
  • Materials Science
  • Photocatalysis

Background:

  • Precise control over molecular stacking is crucial for optimizing charge transfer in functional materials.
  • Terpyridine scaffolds offer versatile platforms for designing complex supramolecular architectures.
  • Donor-acceptor (D-A) interactions are key to efficient photocatalytic processes.

Purpose of the Study:

  • To develop a novel terpyridine bi-functionalization strategy for precise spatial control of D-A stacking.
  • To optimize through-space charge transfer (TSCT) for enhanced photocatalytic efficiency.
  • To investigate the structure-property relationships in Zn(II) complexes with tunable TSCT.

Main Methods:

  • Designed and synthesized two terpyridine-based ligands (L1, L2) functionalized with donor (triphenylamine) and acceptor (triphenyltriazine) units.
  • Coordinated ligands with Zn(II) to form complexes (S1, S2) with distinct D-A stacking geometries.
  • Characterized complexes using spectroscopic and electrochemical methods to evaluate TSCT, charge carrier dynamics, and photocatalytic activity.

Main Results:

  • Achieved precise molecular-level editing of D-A stacking, resulting in slip-stacked (S1) and co-facial (S2) geometries.
  • The co-facial complex (S2) exhibited significantly enhanced TSCT, leading to improved visible-light absorption and charge carrier lifetime.
  • S2 demonstrated superior charge separation efficiency and achieved a photocatalytic efficiency of 2063 µmol g⁻¹ h⁻¹ for H₂O₂ production, twice that of S1, without sacrificial agents.

Conclusions:

  • The terpyridine bi-functionalization strategy enables tunable TSCT and precise control over D-A stacking in supramolecular systems.
  • The designed Zn(II) complexes show great potential as efficient photocatalysts for H₂O₂ production.
  • This work provides valuable insights for the rational design of advanced supramolecular photocatalytic materials.