Low-Triggering-Potential Single-Color Electrochemiluminescence from Bovine Serum Albumin-Stabilized Unary Au Nanocrystals for Immunoassays

Wang, Dongyang; Liu, Xiancheng; Zeng, Ying; Zhang, Qingqing; Zhang, Bin; Zou, Guizheng

doi:10.1021/acs.analchem.2c02474

Cited by 5 publications

(6 citation statements)

References 59 publications

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“…The Ab 2(ProGRP) |CdTe conjugate also displays efficient ECL with a maximum emission potential of +0.24 V, indicating the ECL nature of CdTe NCs in the conjugates of Ab 2(ProGRP) |CdTe can be primarily preserved. This triggering potential of both CdTe NCs and Ab 2(ProGRP) |CdTe is much lower than that of the previously reported coreactant ECL from CdTe NCs, − which can be anticipated to further and effectively evade the electrochemical interference for the ECL immunoassay. The detailed coreactant-free ECL mechanism of CdTe NCs is demonstrated as follows: normalR → normalR + • + normale − .25em ( + 0.21 V ) normalR + normale − → normalR − • normalR + • + normalR − • → normalR * normalR * → normalR + h v ( R = C d T e N C s ) …”

Section: Resultsmentioning

confidence: 61%

Luminophore-Surface-Engineering-Enabled Low-Triggering-Potential and Coreactant-Free Electrochemiluminescence for Protein Determination

Gao

Ren

et al. 2023

Anal. Chem.

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Coreactant-free electrochemiluminescence (ECL) is promising for removing the exogenous effects of coreactant and simplify the operation procedures and setups of commercialized ECL bioassays. Herein, an electrosterically involved strategy for achieving a low-triggering-potential (+0.21 V vs Ag/AgCl) and coreactant-free ECL from dual-stabilizer-capped CdTe nanocrystals (NCs) is proposed with mercaptopropionic acid (MPA) and hexametaphosphate (HMP) as the capping agents of luminophores. Upon employing the CdTe NCs as the ECL tag for the immunoassay, all the tags in the bioconjugates of the CdTe NCs and the secondary antibody (Ab2|CdTe) as well as in the final achieved sandwich-type immunocomplexes can exhibit efficient coreactant-free ECL with an electrosterically involved triggering potential nature. The bioconjugates of Ab2|CdTe with Ab2 no more than 30 kDa, such as the thyroid stimulating hormone (30 kDa) and the recombinant pro-gastrin releasing peptide (ProGRP, 14 kDa), merely exhibit coreactant-free ECL around +0.24 V, while bioconjugates of Ab2|CdTe with an Ab2 beyond 30 kDa only give off coreactant-free ECL around +0.82 V. Due to the further enhanced electrosteric effect in sandwich-type immunocomplexes, only the ECL immunosensor with ProGRP as the target can give off coreactant-free ECL around +0.24 V. The electrosterically involved and coreactant-free ECL of CdTe NCs is consequently utilized to sensitively and selectively determine the molecular protein ProGRP, which demonstrates a wide linearity range from 0.1 to 2000 pg/mL and a low limit of detection at 0.05 pg/mL (S/N = 3). This low-triggering-potential and coreactant-free combined ECL platform indicates that engineering the surface of CdTe NCs with a protein can improve the performance of ECL tags in a protein-weight-involved electrosterical way.

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Section: Resultsmentioning

confidence: 61%

Luminophore-Surface-Engineering-Enabled Low-Triggering-Potential and Coreactant-Free Electrochemiluminescence for Protein Determination

Gao

Ren

et al. 2023

Anal. Chem.

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“…The effects of coreactants on ECLs of Cys-CuNCs are investigated. According to Figure A, TPrA enables Cys-CuNCs with much stronger ECLs than the other coreactants, such as 2-(dibutylamino)ethanol (DBAE), , triethylamine (TEA), triethanolamine (TEOA), hydrazine hydrate (N 2 H 4 ), , and hydrogen peroxide (H 2 O 2 ). , Cys-CuNCs/DBAE exhibits two ECL processes around +0.88 and +1.19 V (curve b), which are much weaker than those of Cys-CuNCs/TPrA, respectively (curve a). Cys-CuNCs/TEA and Cys-CuNCs/TEOA only exhibit one weak ECL process around +1.15 V (curves c and d).…”

Section: Resultsmentioning

confidence: 99%

“…Cys CuNCs e 0.85 V (3) 53,54 triethylamine (TEA), 55 triethanolamine (TEOA), 39 hydrazine hydrate (N 2 H 4 ), 35,41 and hydrogen peroxide (H 2 O 2 ). 56,57 Cys-CuNCs/DBAE exhibits two ECL processes around +0.…”

Section: Cys Cuncsmentioning

confidence: 99%

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Surface-Defect-Involved and Eye-Visible Electrochemiluminescence of Unary Copper Nanoclusters for Immunoassay

et al. 2023

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A single-stabilizer-capped strategy is proposed for achieving highly efficient and surface-defect-involved electrochemiluminescence (ECL) from unary copper nanoclusters (NCs) via employing L-cysteine (Cys) as a capping agent of luminophore. The Cys-capped CuNCs (Cys-CuNCs) can be electrochemically injected with valence band (VB) holes and exhibit eye-touchable ECL processes around +0.95 and +1.15 V upon employing TPrA as a coreactant. Both accumulated ECL spectra and spooling ECL spectra demonstrated that the two ECL processes are of the same single waveband and spectrally identical to each other with the same maximum emission wavelength of 640 nm. Promisingly, ECL of the Cys-CuNCs/TPrA system is obviously red-shifted for ∼150 nm to PL of Cys-CuNCs, indicating that the bandgap-engineered routes for ECLs of Cys-CuNCs are completely blocked. The oxidative-reduction ECL process of the Cys-CuNCs/TPrA system is a kind of highly efficient, eye-visible, and single-color emission in surface-defect-involved route. The capping agent of Cys can enable the CuNCs/TPrA system with a stronger ECL than other thiol capping agents, so that Cys-CuNCs are utilized as ECL tags for sensitive and selective immunoassays, which exhibit a wide linear response range from 0.05 pg/mL to 0.5 ng/ mL and a limit of detection of 0.01 pg/mL (S/N = 3) with carcinoembryonic antigen as the analyte. Moreover, both the luminophore Cys-CuNCs and conjugates Ab 2 -CuNCs can be safely stored in aqueous media without any protector, which is promising for the evolution and clinic application of metal NC ECL in the surface-defect-involved route.

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“…Additionally, the applied ECL such as Ru(bpy) 3 2+ /tripropylamine (TPrA) system is normally performed with the latter route for enhanced ECL efficiency, which requires the participation of luminophores and coreactants synchronously . Therefore, seeking matched luminophores and coreactants is a significant component for the development of ECLs . Common coreactants containing traditional TPrA, oxalate, persulfate, 2-(dibutylamino)ethanol (DBAE), and H 2 O 2 one after another have been discovered, and only a few new coreactants have been proposed for ECL. , Since Bard’s group first reported the ECL of Si nanoparticles, a variety of nanoparticles with different ECL performances such as II–VI, metals, ternary nanocrystals (NCs), and so on, have been extensively explored as ECL luminophores and utilized to develop the ECL system.…”

Section: Introductionmentioning

confidence: 99%

Electrochemiluminescence Mechanistic Insights of CuInS₂/ZnS Nanocrystals with Hydrazine Compounds as Co-reactants

Fu,

Liu,

Dong

et al. 2023

J. Phys. Chem. C

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Screening a novel electrochemiluminescence (ECL) system and reducing electrochemical interference by lowering the ECL potential are crucial to ECL evolution. Herein, an ECL system is explored with different hydrazine compounds as coreactants and ternary CuInS2/ZnS nanocrystals (CIS/ZnS NCs) as a luminophore, demonstrating that hydrazine compounds with varied structures would assuredly affect the ECL triggering potential and efficiency. Electro-oxidized hydrazine-based coreactants containing a symmetrical structure and −N–N single bonds with strong reducibility could produce an efficient electron transfer recombination path with electro-oxidized CIS/ZnS NCs, which eventually generate efficient and low-triggering-potential ECL performance; otherwise, the hydrazine compounds with a double bond, such as −CN or −CO, or strong electronegative atoms would reduce the ECL efficiency and increase the ECL triggering potential, which result from double bonds or strong electronegative atoms of hydrazine compounds hindering the protonation of coreactants and then delaying the electron–hole recombination process. The structure of hydrazine-based coreactants with a −CS double bond would competitively bond with the Cu element within CIS/ZnS NCs, contributing to the blank ECL with CIS/ZnS NCs as the luminophore. Furthermore, CIS/ZnS NCs exhibit two additional low hole injected processes under alkaline conditions through exploration of the differential pulse voltammetry (DPV) nature from CIS/ZnS NCs. The ultralow-triggering-potential of CIS/ZnS NCs around 0.11 V could be achieved by adjusting the hole injection processes of NCs and selecting pasoniazide as the coreactant, which is extremely below any previously reported ECL system. This work contributes to a deeper understanding of the ECL mechanism.

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Low-Triggering-Potential Single-Color Electrochemiluminescence from Bovine Serum Albumin-Stabilized Unary Au Nanocrystals for Immunoassays

Cited by 5 publications

References 59 publications

Luminophore-Surface-Engineering-Enabled Low-Triggering-Potential and Coreactant-Free Electrochemiluminescence for Protein Determination

Luminophore-Surface-Engineering-Enabled Low-Triggering-Potential and Coreactant-Free Electrochemiluminescence for Protein Determination

Surface-Defect-Involved and Eye-Visible Electrochemiluminescence of Unary Copper Nanoclusters for Immunoassay

Electrochemiluminescence Mechanistic Insights of CuInS₂/ZnS Nanocrystals with Hydrazine Compounds as Co-reactants

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Low-Triggering-Potential Single-Color Electrochemiluminescence from Bovine Serum Albumin-Stabilized Unary Au Nanocrystals for Immunoassays

Cited by 5 publications

References 59 publications

Luminophore-Surface-Engineering-Enabled Low-Triggering-Potential and Coreactant-Free Electrochemiluminescence for Protein Determination

Luminophore-Surface-Engineering-Enabled Low-Triggering-Potential and Coreactant-Free Electrochemiluminescence for Protein Determination

Surface-Defect-Involved and Eye-Visible Electrochemiluminescence of Unary Copper Nanoclusters for Immunoassay

Electrochemiluminescence Mechanistic Insights of CuInS2/ZnS Nanocrystals with Hydrazine Compounds as Co-reactants

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Product

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Electrochemiluminescence Mechanistic Insights of CuInS₂/ZnS Nanocrystals with Hydrazine Compounds as Co-reactants