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1.
Anal Chem ; 95(26): 10068-10076, 2023 Jul 04.
Artigo em Inglês | MEDLINE | ID: mdl-37339328

RESUMO

Improving the electrochemiluminescence (ECL) efficiency of luminophores has always been the goal of the ECL field. Herein, a novel crystallization-induced enhanced ECL (CIE ECL) strategy was exploited to significantly enhance the ECL efficiency of metal complex tris-(8-hydroxyquinoline)aluminum (Alq3). Alq3 monomers self-assembled and directionally grew to form Alq3 microcrystals (Alq3 MCs) in the presence of sodium dodecyl sulfate. The highly ordered crystal structure of Alq3 MCs not only constrained the intramolecular rotation of Alq3 monomers to decrease nonradiative transition but also accelerated the electron transfer between Alq3 MCs and coreactant tripropylamine to increase radiative transition, thus leading to a CIE ECL effect. Alq3 MCs exhibited brilliant anode ECL emission, which was 210-fold stronger than that of Alq3 monomers. The exceptional CIE ECL performance of Alq3 MCs coupled the efficient trans-cleavage activity of CRISPR/Cas12a assisted by rolling circle amplification and catalytic hairpin assembly to fabricate a CRISPR/Cas12a-mediated aptasensor for acetamiprid (ACE) detection. The limit of detection was as low as 0.79 fM. This work not only innovatively exploited a CIE ECL strategy to enhance the ECL efficiency of metal complexes but also integrated CRISPR/Cas12a with a dual amplification strategy for the ultrasensitive monitoring of pesticides such as ACE.

2.
J Phys Condens Matter ; 36(30)2024 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-38588675

RESUMO

Modulating interlayer coupling modes can effectively enhance the thermoelectric properties of nanomaterials or nanoscale devices. By using density functional theory combined with non-equilibrium Green's function method, we investigate the thermoelectric properties of zigzag-type black arsenic nanoscale devices with varying interlayer coupling modes. Our results show that altering the interlayer coupling mode significantly modulates the thermoelectric properties of the system. Specifically, we consider four coupling modes with different strengths, by modulating different interlayer overlap patterns. Notably, in the weaker interlayer coupling mode, the system exhibits enhanced thermoelectric properties due to increased interface phonon scattering, for example, the M4reaching a peak value of 2.23 atµ= -0.73 eV. Furthermore, we explore the temperature-dependent behavior of each coupling model. The results suggest that the thermoelectric characteristics are more sensitive to temperature variations in the weaker coupling modes. These insights provide valuable guidance for enhancing the thermoelectric performance of nanoscale devices through precise interlayer coupling modulation.

3.
Chem Commun (Camb) ; 58(60): 8428-8431, 2022 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-35796312

RESUMO

A serial oxygen vacancy (OV) on Nb2O5 is synthesised by H2 calcination, and H-300 exhibited high selectivity and activity for H2O2 (93.4%, 562.5 mmol gcat-1). A volcano relationship is identified between the OV content and performance, which provides an attractive insight into designing electrocatalysts.

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