Donor–Acceptor MOF Enabling Efficient Electrochemiluminescence Based on TSCT-TADF DOI

Jinliu Wei,

Mengru Liu,

Shujuan Lin

et al.

The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: 15(44), P. 11104 - 11111

Published: Oct. 30, 2024

Electrochemiluminescence (ECL) is an extensively studied luminescence technique recognized for its efficacy in investigating surface energy states. Effective utilization of ECL to explore and probe the charge transfer mechanisms facilitated by novel luminescent materials crucial. In this study, we demonstrate thermally activated delayed fluorescence (TADF) based on spatial through precisely controlled synthesis materials, which achieved incorporating phenyl-carbazole derivatives as donor guests within acceptor-hosted metal–organic frameworks (D-A MOFs). These hybrid structures exhibit superior intensities compared with their monomeric counterparts. Mechanistic investigation DFT calculation reveals that physically separated yet spatially closed D-A configuration induces efficient intermolecular through-spatial (TSCT), leading tuning dihedral angle guest molecules enhance π–π interactions. This study introduces a strategy precise modulation at molecular level programmable luminophores.

Language: Английский

Optically Pure Co(III) Complex Absorbed by Electrochemiluminescence-Active Covalent Organic Framework as an Enantioselective Recognition Platform to Give Opposite Responses Toward Amino Alcohol Enantiomers DOI
Lei Zhao, Wenrong Cai,

Shuyi Yuan

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(42), P. 57649 - 57658

Published: Oct. 9, 2024

Although covalent organic frameworks (COFs) accompanied by electrochemiluminescence (ECL) behavior have been introduced in recent years, they are still rarely applied for ECL-based enantioselective sensing, especially giving high recognition efficiency. In the current study, an achiral ionic COF comprised of pyridinium unit is synthesized linkage carbon–nitrogen cation bond through Zincke reaction. Interestingly, can generate clear ECL owing to presence electroactive species. Then, ECL-active employed absorb chiral Co(III) complex sensing. As a result, developed sensor displays discriminative responses toward amino alcohol enantiomers. When with (R)-configuration used, examined (S)-amino alcohols result enhancement, whereas (R)-amino lead quenching. The maximum intensity ratio between (S)- and up 47.7. addition, mechanism investigated detail. Finally, good linear relation enantiomeric composition appropriate accurate analysis purities unknown samples. short, we believe that this study constructs effective strategy combine respective advantages COFs high-efficiency

Language: Английский

Citations

2

Bimodal Oxidation Electrochemiluminescence Mechanism of Coreactant‐Embedded Covalent Organic Frameworks via Postsynthetic Modification DOI
Xiaoxiao Meng,

Lifeng Zheng,

Rengan Luo

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(17)

Published: March 5, 2024

Abstract Electrochemiluminescence (ECL) efficiency is determined by charge transfer between coreactants and emitters in coreactant systems, which are usually limited their slow intermolecular transfer. In this study, a covalent organic framework (COF) with aldehyde residue was synthesized, then were covalently integrated into the skeleton through postsynthetic modification strategy, resulting crystalline coreactant‐embedded COF nanoemitter (C–COF). Compared to pristine an equivalent external coreactant, C–COF exhibited extraordinary 1008‐fold enhancement of ECL intensity due rapid intrareticular Significantly, pH increase, shows protonation‐induced for first peaked at +1.1 V opposite trend second +1.4 V, attributed antedating oxidation self‐oxidation, respectively. The bimodal mechanism rationalized spectral characterization density functional theory calculations. nanoemitters present innovative universal avenues advancing systems.

Language: Английский

Citations

1

Electrochemiluminescence of Ultrasmall Silica Nanoparticles from Size Modulation and Multipath Surface State Adjustment for Ultrasensitive HIV-DNA Fragment Detection DOI
Jiaxin Duan,

Weiwei Cao,

Xin Zhu

et al.

Analytical Chemistry, Journal Year: 2024, Volume and Issue: 96(28), P. 11280 - 11289

Published: July 2, 2024

Here, ultrasmall SiO

Language: Английский

Citations

1

Aggregation-Induced ECL Immunosensor Using Ligand-Mediated Highly Stable Tetraphenylethene-Based Zinc Metal–Organic Frameworks for the Detection of 5-Fluorouracil DOI

Cheng Tan,

Xinyue Qian,

Kang Wu

et al.

ACS Applied Nano Materials, Journal Year: 2024, Volume and Issue: 7(14), P. 15958 - 15967

Published: July 16, 2024

Tetraphenylene (TPE) and its derivatives are highly studied materials in the field of aggregation-induced electrochemiluminescence (AIECL). We successfully synthesized a block-like metal–organic framework by employing Zn2+ TPE-based ligand H8ETTB (H8ETTB = 4′,4‴,4‴″,4‴‴′-(ethene-1,1,2,2-tetrayl) tetrakis (([1,1′-biphenyl]-3,5-dicarboxylic acid))), which demonstrates excellent ECL properties. For simplicity, we refer to this material as Zinc-based (Zn-MOF). is luminophore, increasing loading luminophore. The Zn-MOF exhibits considerable specific surface area porous structure, enables efficient reaction between luminophores coreactants, resulting ECL. emission more intense than that monomer aggregates. Due distinctive characteristics Zn-MOF, employed it an luminophore immunoassay, establishment system for extremely sensitive detection 5-fluorouracil. PdAu nanoflowers (PdAu NFs) were utilized electrodes, modified because their electrocatalytic efficiency. As result, they additionally improved performance. design immunosensor relatively straightforward, facilitating manufacture. Furthermore, was tested human serum samples, demonstrating comparable results those obtained using high-performance liquid chromatography with tandem mass spectrometry (HPLC-MS/MS). This research thus offers practical method enhance performance introduces approach identifying 5-FU clinical analysis.

Language: Английский

Citations

1

Donor–Acceptor MOF Enabling Efficient Electrochemiluminescence Based on TSCT-TADF DOI

Jinliu Wei,

Mengru Liu,

Shujuan Lin

et al.

The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: 15(44), P. 11104 - 11111

Published: Oct. 30, 2024

Electrochemiluminescence (ECL) is an extensively studied luminescence technique recognized for its efficacy in investigating surface energy states. Effective utilization of ECL to explore and probe the charge transfer mechanisms facilitated by novel luminescent materials crucial. In this study, we demonstrate thermally activated delayed fluorescence (TADF) based on spatial through precisely controlled synthesis materials, which achieved incorporating phenyl-carbazole derivatives as donor guests within acceptor-hosted metal–organic frameworks (D-A MOFs). These hybrid structures exhibit superior intensities compared with their monomeric counterparts. Mechanistic investigation DFT calculation reveals that physically separated yet spatially closed D-A configuration induces efficient intermolecular through-spatial (TSCT), leading tuning dihedral angle guest molecules enhance π–π interactions. This study introduces a strategy precise modulation at molecular level programmable luminophores.

Language: Английский

Citations

1