Liu Yueting, Wang Quanbo, Lei Jianping, Hao Qing, Wang Wei, Ju Huangxian
State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, PR China.
Institute of Basic Medicine Shangdong Academy of Medical Science, Jinan 250062, PR China.
Talanta. 2014 May;122:130-4. doi: 10.1016/j.talanta.2014.01.018. Epub 2014 Jan 31.
This work observed the anodic electrochemiluminescence (ECL) of C₃N₄ nanosheets (CNNS) for the first time. The ECL emission was 40 times stronger than that from bulk g-C₃N₄ in the presence of triethylamine (Et₃N) as a coreactant due to large surface-to-volume ratio, which enhanced the sensitivity for biosensing. At pH 7.0, the CNNS modified electrode prepared with 0.75 mg mL(-1) CNNS in 0.025% chitosan solution possesses good stability and acceptable reproducibility in the presence of 30 mM Et₃N. The ECL mechanism of CNNS/Et₃N system was proposed to be emitted from the excited CNNS, which was produced during the reaction between the electro-oxidation products of CNNS and coreactant Et₃N. Based on the annihilation between the oxidation product of dopamine (DA(+)) and Et₃N radical, a quenching-based method was established for sensitive and specific detection of dopamine ranging from 1.0 nM to 100 nM with a detection limit of 96 pM by using the CNNS nanosheets as an ECL emitter. The proposed method showed excellent specificity, high sensitivity and low detection limit, and could be applied in analysis of real samples.
这项工作首次观察到了C₃N₄纳米片(CNNS)的阳极电化学发光(ECL)。由于具有较大的表面积与体积比,在作为共反应剂的三乙胺(Et₃N)存在下,ECL发射比块状g-C₃N₄强40倍,这提高了生物传感的灵敏度。在pH 7.0时,用0.75 mg mL⁻¹ CNNS在0.025%壳聚糖溶液中制备的CNNS修饰电极在30 mM Et₃N存在下具有良好的稳定性和可接受的重现性。提出CNNS/Et₃N体系的ECL机理是由激发态的CNNS发射,其是在CNNS的电氧化产物与共反应剂Et₃N之间的反应过程中产生的。基于多巴胺(DA⁺)的氧化产物与Et₃N自由基之间的湮灭,建立了一种基于猝灭的方法,以CNNS纳米片作为ECL发射体,用于灵敏且特异性地检测1.0 nM至100 nM的多巴胺,检测限为96 pM。所提出的方法具有优异的特异性、高灵敏度和低检测限,可应用于实际样品的分析。