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Updated: Jan 15, 2026
Measurement of Ultrafast Vibrational Coherences in Polyatomic Radical Cations with Strong-Field Adiabatic Ionization
Published on: August 6, 2018
Crystalline Energy Funneling in Mixed-Ligand Zr-MOFs Drives Radical-Triggered ECL Amplification for Ultrasensitive
Ju-Zheng Wang1, Yi-Xuan Li1,2, Qiaoting Yang1
1School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, P. R. China.
Abstract:
Harnessing crystalline architectures to direct exciton migration presents a promising avenue for electrochemiluminescence (ECL) signal amplification in biosensing. Herein, we report a structurally orchestrated ECL platform based on a mixed-ligand zirconium metal-organic framework (Zr-MOF), assembled from 1,3,6,8-tetrakis(p-benzoic acid)pyrene (TBAPy) and zinc tetrakis(4-carboxyphenyl)porphyrin (ZnTCPP). The nanoscale colocalization of donor-acceptor pairs within a crystalline lattice establishes an intraframework energy funneling pathway, enabling directional resonance energy transfer (RET) from TBAPy to ZnTCPP with an efficiency of up to 76.5%. Beyond RET, radical-triggered excitation involving TBAPy•- and superoxide (O2•-) further activates ZnTCPP-centered ECL emission, resulting in a 3-fold enhancement compared to single-ligand controls. By leveraging this synergistic amplification, an aptamer-gated, signal-off ECL biosensor was constructed for femtomolar-level thrombin detection (limit of detection: 0.47 fM) with exceptional selectivity. This work exemplifies a crystalline energy-programmed approach to coupling exciton dynamics with redox-active interfaces, offering a mechanistically traceable and highly sensitive platform for advanced bioanalytical applications.
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