Tunable covalent organic framework electrochemiluminescence from non-electroluminescent monomers

Cui, Wei‐Rong; Li, Yajie; Jiang, Qiao‐Qiao; Wu, Qiong; Liang, Ru‐Ping; Luo, Qiu-Xia; Zhang, Li; Liu, Juewen; Qiu, Jian‐Ding

doi:10.1016/j.xcrp.2021.100630

Cited by 18 publications

(16 citation statements)

References 48 publications

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“…It can be seen that the TPA-COFs with stronger electron-donating ability possess smaller band gaps and show around 1.4-fold stronger ECL intensities than TFPB-COFs (Figure B), indicating that intramolecular charge transfer can effectively activate the ECL signals of COFs. Further, a fully conjugated COF synthesized with trithiophene units shows high ECL efficiency up to 62.2% in aqueous solution, even without exogenous co-reactant …”

Section: Structural Design Of Reticular Ecl Nanoemittersmentioning

confidence: 99%

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Reticular Electrochemiluminescence Nanoemitters: Structural Design and Enhancement Mechanism

Luo

Zhu

et al. 2023

Acc. Chem. Res.

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Metrics & MoreArticle Recommendations CONSPECTUS: Electrochemiluminescence (ECL) is a powerful transduction technique, which depends critically on the formation of the excited emitter through the charge transfer between the electrochemical reaction intermediates of the emitter and the co-reactant/emitter. The exploration of ECL mechanisms for conventional nanoemitters is limited due to the uncontrollable charge transfer process. With the development of molecular nanocrystals, reticular structures such as metal−organic frameworks (MOFs) and covalent organic frameworks (COFs) have been utilized as atomically precise semiconducting materials. The long-range order in crystalline frameworks and the tunable coupling among building blocks promote the quick development of electrically conductive frameworks. Especially, the reticular charge transfer can be regulated by both interlayer electron coupling and intralayer topology-templated conjugation. By modulating intramolecular or intermolecular charge mobility, reticular structures could serve as promising candidates for enhancing ECL. Thus, reticular crystalline nanoemitters with different topologies provide a confined platform to understand ECL fundamentals for designing next-generation ECL devices.Aiming at exploring the mechanism of ECL emission, our group has developed a series of ECL nanoemitters as well as enhancement strategies of ECL emission in the past 20 years. A series of water-soluble ligandcapped quantum dots were introduced as ECL nanoemitters to create sensitive analytical methods for detecting and tracing biomarkers. The functionalized polymer dots were also designed as ECL nanoemitters for imaging of membrane proteins with signal transduction strategies of dual resonance energy transfer and dual intramolecular electron transfer. To decode the ECL fundamental and enhancement mechanisms, an electroactive MOF with accurate molecular structure was first constructed with two redox ligands as a highly crystallized ECL nanoemitter in aqueous medium. Through the mixed-ligand approach, luminophores and co-reactants were integrated into one MOF structure for self-enhanced ECL. Furthermore, several donor−acceptor COFs were developed as efficient ECL nanoemitters with tunable intrareticular charge transfer. The atomically precise structure of conductive frameworks established clear correlations between the structure and charge transport in these materials. Therefore, reticular materials as crystalline ECL nanoemitters have demonstrated both proof of concept and mechanistic innovation.In this Account, taking advantage of reticular materials with accurate molecular structure, we survey the design of the electroactive reticular materials including MOFs and COFs as crystalline ECL nanoemitters at the molecular level. The enhancement mechanisms of ECL emission of various topology frameworks are discussed via the regulation of reticular energy transfer and charge transfer and the accumulation of anion/cation radicals. Our perspective on the reticular ECL nanoemitters is ...

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Section: Structural Design Of Reticular Ecl Nanoemittersmentioning

confidence: 99%

“…Further, a fully conjugated COF synthesized with trithiophene units shows high ECL efficiency up to 62.2% in aqueous solution, even without exogenous co-reactant. 29…”

Section: Ecl Generation From Non-emitting Monomersmentioning

confidence: 99%

Reticular Electrochemiluminescence Nanoemitters: Structural Design and Enhancement Mechanism

Luo

Zhu

et al. 2023

Acc. Chem. Res.

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“…772,773 The Qiu group reported some COFs with electrochemiluminescence properties 774,775 and their application in UO 2 2+ detection. 776,777 Briefly, electrochemical sensing has the advantages of sensitive response, simple operation, and low cost, but metal-free COFs have not been widely used in electrochemical sensing due to their poor electrical conductivity. By contrast, metal nanoparticle-loaded COFs to some extent cover the shortage of low conductivity and have been developed for electrochemical sensing, but there is still room for improvement in reproducibility and stability.…”

Section: Review Articlementioning

confidence: 99%

“…772,773 The Qiu group reported some COFs with electrochemiluminescence properties 774,775 and their application in UO 2 2+ detection. 776,777…”

Section: Application Of Metalated Cofsmentioning

confidence: 99%

Metalated covalent organic frameworks: from synthetic strategies to diverse applications

2022

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“…Electrochemiluminescence (ECL) is a unique luminescent phenomenon generated by electrically stimulating substances to produce a species in an excited state and finally returning them to the ground state. − Since it integrates the characteristics of both luminescence and electricity, ECL features many advantages like high sensitivity, simple operation, low inherent background, and strong controllability. Over the past decade, ECL has acted as a powerful analytical tool in numerous fields including bioimaging, immunoassays, pharmaceutical detection, clinical diagnosis, and environment and food analysis. − In particular, ECL has advanced rapidly in recent years. For example, the intriguing concept of “aggregation-induced emission” , was introduced in the ECL field, known as “AIE-ECL”, which achieved the water-insoluble organic probes for ultrasensitive aqueous-phase detection. − Furthermore, the intensity of the AIE-ECL system gives rise to a clearly distinguishable change with the aggregation degree of the emitter.…”

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confidence: 99%

Viscosity-Responsive Electrochemiluminescence of Diphenylbenzofulvene Derivatives

Han

Chai

et al. 2023

Anal. Chem.

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The development of superior probes is highly desirable and valuable for viscosity measurement. Herein, we designed and reported a series of diphenylbenzofulvene (DPBF)-based organic luminophores according to the molecular regulation strategy. There are two free-rotating phenyl groups attached to the rigid fluorene skeleton in the DPBF, enabling its unique propeller-like noncoplanar chemical structure. Benefiting from this, DPBFs could feature outstanding PL and ECL emissions with intriguing aggregation-induced characteristics. Experimental and theoretical investigations revealed that substituent, spatial structure, and molecular orbital energy profoundly affected their luminescent behaviors. It was disclosed that fluoro-substituted DPBF(F)2 with a smaller LUMO–HOMO band gap demonstrated the strongest ECL emission and was selected as the optimal ECL emitter. Finally, DPBF(F)2 featured a linear response to the viscosity and VC content with lower limits of detection (LOD) of 5.69 μcP and 38.2 nM, respectively. This study represents the first example of the ECL probe toward viscosity and will be of great significance for both ECL application and viscosity measurement.

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Tunable covalent organic framework electrochemiluminescence from non-electroluminescent monomers

Cited by 18 publications

References 48 publications

Reticular Electrochemiluminescence Nanoemitters: Structural Design and Enhancement Mechanism

Reticular Electrochemiluminescence Nanoemitters: Structural Design and Enhancement Mechanism

Metalated covalent organic frameworks: from synthetic strategies to diverse applications

Viscosity-Responsive Electrochemiluminescence of Diphenylbenzofulvene Derivatives

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