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等离子体诱导无定形二硫化钼在纳米多孔金上的过度生长:具有增强电催化活性的混合纳米粒子的环境合成方法。

Plasmonic-induced overgrowth of amorphous molybdenum sulfide on nanoporous gold: An ambient synthesis method of hybrid nanoparticles with enhanced electrocatalytic activity.

机构信息

Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, 21 Nanyang Link, Singapore 637371.

出版信息

J Chem Phys. 2019 Dec 28;151(24):244709. doi: 10.1063/1.5130649.

DOI:10.1063/1.5130649
PMID:31893908
Abstract

Hybrid materials of earth abundant transition metal dichalcogenides and noble metal nanoparticles, such as molybdenum sulfide (MoS) and gold nanoparticles, exhibit synergistic effects that can enhance electrocatalytic reactions. However, most current hybrid MoS-gold synthesis requires an energy intensive heat source of >500 °C or chemical plating to achieve deposition of MoS on the gold surface. Herein, we demonstrate the direct overgrowth of MoS over colloidal nanoporous gold (NPG), conducted feasibly under ambient conditions, to form hybrid particles with enhanced electrocatalytic performance toward hydrogen evolution reaction. Our strategy exploits the localized surface plasmon resonance-mediated photothermal heating of NPG to achieve >230 °C surface temperature, which induces the decomposition of the (NH)MoS precursor and direct overgrowth of MoS over NPG. By tuning the concentration ratio between the precursor and NPG, the amount of MoS particles deposited can be systematically controlled from 0.5% to 2% of the Mo/(Au + Mo) ratio. Importantly, we find that the hybrid particles exhibit higher bridging and an apical S to terminal S atomic ratio than pure molybdenum sulfide, which gives rise to their enhanced electrocatalytic performance for hydrogen evolution reaction. We demonstrate that hybrid MoS-NPG exhibits >30 mV lower onset potential and a 1.7-fold lower Tafel slope as compared to pure MoS. Our methodology provides an energy- and cost-efficient synthesis pathway, which can be extended to the synthesis of various functional hybrid structures with unique properties for catalysis and sensing applications.

摘要

富含地球过渡金属二硫化物和贵金属纳米粒子的杂化材料,如硫化钼 (MoS) 和金纳米粒子,表现出协同效应,可以增强电催化反应。然而,大多数当前的杂化 MoS-金合成需要 >500°C 的能量密集热源或化学镀来实现 MoS 在金表面的沉积。在此,我们展示了在环境条件下可行的胶体纳米多孔金 (NPG) 上直接生长 MoS,以形成具有增强析氢反应电催化性能的杂化颗粒。我们的策略利用 NPG 的局域表面等离激元共振介导的光热加热来实现 >230°C 的表面温度,这导致 (NH)MoS 前体的分解和 MoS 在 NPG 上的直接生长。通过调整前体和 NPG 之间的浓度比,可以从 Mo/(Au + Mo) 比的 0.5%到 2%系统地控制沉积的 MoS 颗粒的量。重要的是,我们发现杂化颗粒表现出比纯钼硫化物更高的桥接和端基 S 与顶基 S 的原子比,这导致其对析氢反应的电催化性能增强。我们证明,与纯 MoS 相比,杂化 MoS-NPG 的起始电位低 30 mV 以上,塔菲尔斜率低 1.7 倍。我们的方法提供了一种节能且经济高效的合成途径,可扩展到具有独特催化和传感应用特性的各种功能杂化结构的合成。

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