首页|Nanosponge hierarchical micro-mesoporous MFI zeolites as a high-performance catalyst for the hydroamination of methyl acrylate with aniline
Nanosponge hierarchical micro-mesoporous MFI zeolites as a high-performance catalyst for the hydroamination of methyl acrylate with aniline
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NSTL
Zeolites catalyze the hydroamination of alkenes,alkynes and dienes,yielding valuable amines,enamines and imines with high efficiency and chemoselectivity(i.e.,Markovnikov or and-Markovnikov products)thanks to the architecture of their pore system and tunable acidity.However,their micropores may impose mass-transfer constraints on reaction rates.Nevertheless,the high external surface area of hierarchical micro-mesoporous zeolites should enable them to outperform conventional zeolites.To test our hypothesis,we compared the activity of hierarchical MFI zeolites of different crystal morphologies(i.e.,nanosponge,nanosheet and micro-crystalline desilicated samples)with that of conventional medium-(MFI)and large-pore(MOR and Beta)zeolites in the hydroamination of methyl acrylate with aniline.The results showed that nanosponge MFI had the highest activity(TOF = 32.9 h"1),reaching 57% yield of the anti-Markovnikov product N-[2-(methoxycarbonyl)ethyl] aniline.Furthermore,our kinetic study revealed a pseudo-second-order rate law with respect to aniline over the most active nanosponge MFI catalyst,with an apparent activation energy of 68.9 kJ/mol.The high external surface of this catalyst(371 m~2/g)and its developed inter-crystalline mesopores(4.8 nm)suggest a kinetic-driven hydroamination reaction.Therefore,hierarchical nanosponge aluminosilicate MFI zeolites stand out as promising heterogeneous catalysts of hydroamination reactions involving bulky substrates.
NSTL
