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电喷雾电离法合成并研究了贵金属纳米颗粒的催化反应。

Synthesis and catalytic reactions of nanoparticles formed by electrospray ionization of coinage metals.

机构信息

Department of Chemistry, Purdue University, West Lafayette, IN 47907 (USA).

出版信息

Angew Chem Int Ed Engl. 2014 Mar 17;53(12):3147-50. doi: 10.1002/anie.201309193. Epub 2014 Feb 19.

Abstract

Noble metals can be ionized by electrochemical corrosion and transported by electrospray ionization. Mass spectrometry (MS) showed solvated metal ions as the main ionic constituent of the sprayed droplets. Collection of the electrospray plume on a surface yielded noble metal nanoparticles (NPs) under ambient conditions. The NPs were characterized by several techniques. Under typical conditions, capped-nanoparticle sizes averaged 2.2 nm for gold and 6.5 nm for silver. The gold nanoparticles showed high catalytic activity in the reduction of p-nitrophenol by NaBH4 . Efficient catalysis was also observed by simply directing the spray of solvated Au(+) onto the surface of an aqueous p-nitrophenol/NaBH4 mixture. Organometallic ions were generated by spiking ligands into the spray solvent: for example, Cu(I) bipyridine cations dominated the spray during Cu electrocorrosion in acetonitrile containing bipyridine. This organometallic reagent was shown to be effective in the radical polymerization of styrene.

摘要

贵金属可通过电化学腐蚀而被电离,并通过电喷雾电离而传输。质谱(MS)表明,喷雾液滴的主要离子成分为溶剂化金属离子。在环境条件下,将电喷雾羽流收集在表面上,可得到贵金属纳米颗粒(NPs)。通过几种技术对 NPs 进行了表征。在典型条件下,金的封端纳米颗粒的平均尺寸为 2.2nm,银的为 6.5nm。金纳米颗粒在硼氢化钠还原对硝基苯酚中表现出高催化活性。通过将溶剂化 Au(+)喷雾直接引导到含有对硝基苯酚/硼氢化钠的水溶液表面上,也观察到了有效的催化作用。通过向喷雾溶剂中加入配体,可以生成有机金属离子:例如,在含有联吡啶的乙腈中,铜电化学腐蚀期间,铜(I)联吡啶阳离子主导喷雾。该有机金属试剂在苯乙烯的自由基聚合中表现出有效。

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