College of Chemistry and Materials Science, Sichuan Normal University, Chengdu 610068, China.
Analyst. 2019 Nov 4;144(22):6706-6711. doi: 10.1039/c9an01480b.
Development of high-performance Pt-free non-enzymatic hydrogen peroxide (H2O2) sensors on the basis of supported metal nanoparticles (NPs) is important for industrial and biological applications. Here, we report the preparation of ultrafine, surface-clean, and well-distributed Ru NPs and concomitant formation of nitride carbon (Ru/NC) by pyrolyzing tris(2,2'-bipyridyl)ruthenium(ii) chloride (TBRC) with carbon. The use of the nitrogen (N)-containing Ru complex of TBRC as the metal precursor is essential for the preparation of ultrafine and highly dispersed Ru NPs (1.20 nm in diameter) on a NC support. The as-synthesized Ru/NC-800 displays superior analytical performance for non-enzymatic detection of H2O2 with a low detection limit of 0.468 μM, high sensitivity of 698 μA mM-1 cm-2, excellent linear detection ranging from 0.001 to 10.000 mM, good stability, and high selectivity. The control experiment results indicate that the high-performance of Ru/NC-800 must be ascribed to the ultrasmall and highly dispersed Ru NPs and N-doping, which can supply a higher density of active sites available for H2O2 detection. This study provides a facile strategy to synthesize ultrafine metal NPs and for concomitant production of NC for electrocatalytic non-enzymatic sensing.
在担载金属纳米粒子(NPs)的基础上开发高性能的无酶过氧化氢(H2O2)传感器对于工业和生物应用非常重要。在此,我们报告了通过热解三(2,2'-联吡啶)钌(ii)氯化物(TBRC)与碳来制备超细微、表面清洁且分布均匀的 Ru NPs 以及同时形成氮化物碳(Ru/NC)。使用 TBRC 作为金属前体的含氮 Ru 配合物对于在 NC 载体上制备超细微和高度分散的 Ru NPs(直径为 1.20nm)是必不可少的。所合成的 Ru/NC-800 对 H2O2 的非酶检测显示出优异的分析性能,具有低检测限 0.468 μM、高灵敏度 698 μA mM-1 cm-2、从 0.001 到 10.000 mM 的优异线性检测范围、良好的稳定性和高选择性。控制实验结果表明,Ru/NC-800 的高性能必须归因于超细微和高度分散的 Ru NPs 以及 N 掺杂,这可以提供更高密度的活性位点,可用于 H2O2 检测。本研究提供了一种简便的策略来合成超细微金属 NPs 并同时生产 NC 用于电催化非酶传感。