Abstract:Magnetically recoverable nanoparticles provide a cheap, easy, and environmentally benign means for catalyst recovery. In an effort to move toward catalyst systems as simple to synthesize as they are to recover, we recently explored the ability to use magnetic nanoparticles directly as catalysts, without or with minimal functionalization.[1] We first studied reduced iron nanoparticles as an attractive replacement for platium series metals in the industrially important hydrogenation reaction. We established that iron-iron oxide core-shell nanoparticles (Fe CSNPs) are active in the hydrogenation of olefins in ethanol, and where resilient to the presence of water.[2] We further improved this system and showed that amphiphilic polymer-coated Fe(0) NPs could protect effectively in situ produced Fe(0) from water oxidation, while allowing a high catalytic activity in alcohol and water-rich mixtures.[3] These Fe CSNPs were also used as seed, reducing agents, and supports to generate copper/iron nanoparticles (Cu-Fe NPs) that are able to heterogeneously catalyze the Huisgen condensation. [4] Cu-Fe microparticles (Cu-Fe MPs), produced using the same principles, were shown to be powerful catalysts for the functionalization of biologically relevant molecules, while greatly limiting the copper contamination of the product. We fully characterized Cu-Fe NPs and MPs using TEM, EELS, EDAX and XPS to reveal that they consist of copper decorated nanoparticles and Cu-rich nanotubes. [5] Based on the same principles, we developped a Ru-Fe NPs catalytic system to transfer hydrogenate ketones.[6] [1] R. Hudson, Y. Feng, R.S. Varma, A. Moores, Green Chem., 2014, 16, 4493-4505 [2] R. Hudson, A. Riviere, C. M. Cirtiu, K. L. Luska, A. Moores, Chem. Commun. 2012, 48, 3360-3362. [3] R. Hudson, G. Hamasaka, T. Osako, Y. M. Yamada, C.-J. Li, Y. Uozumi, A. Moores, Green Chem. 2013, 15, 2141-2148. [4] R. Hudson, C. J. Li, A. Moores, Green Chem. 2012, 14, 622-624. [5] M. Masnadi, N. Yao, N. Braidy, A. Moores, Langmuir 2015, 31(2), 789-798. [6] R. Hudson, V. Chazelle, M. Bateman, R. Roy, C. J. Li, A. Moores, ACS Sustainable Chem. Eng. 2015, 3 (5),814–820

Reduced iron nanoparticles as magnetically retrievable catalysts for alkene hydrogenation and as galvanic reducers to access Cu and Ru-based catalysts for azide-alkyne condensation and transfer hydrogenation

251st National Meeting (2016)

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