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Enhancing catalytic epoxide ring-opening selectivity using surface-modified Ti3C2T x MXenes
Author(s) -
Thierry K. Slot,
Varun Natu,
Enrique V. RamosFernández,
A. Sepúlveda-Escribano,
Michel W. Barsoum,
Gadi Rothenberg,
N. Raveendran Shiju
Publication year - 2021
Publication title -
2d materials
Language(s) - English
Resource type - Journals
ISSN - 2053-1583
DOI - 10.1088/2053-1583/abe951
Subject(s) - isomerization , catalysis , selectivity , mxenes , epoxide , styrene oxide , lewis acids and bases , alkylation , oxidizing agent , oxide , chemistry , nitride , materials science , photochemistry , styrene , organic chemistry , layer (electronics) , polymer , copolymer
MXenes are a new family of two-dimensional carbides and/or nitrides. Their 2D surfaces are typically terminated by O, OH and/or F atoms. Here we show that Ti 3 C 2 T x —the most studied compound of the MXene family—is a good acid catalyst, thanks to the surface acid functionalities. We demonstrate this by applying Ti 3 C 2 T x in the epoxide ring-opening reaction of styrene oxide (SO) and its isomerization in the liquid phase. Modifying the MXene surface changes the catalytic activity and selectivity. By oxidizing the surface, we succeeded in controlling the type and number of acid sites and thereby improving the yield of the mono-alkylated product to >80%. Characterisation studies show that a thin oxide layer, which forms directly on the Ti 3 C 2 T x surface, is essential for catalysing the SO ring-opening. We hypothesize that two kinds of acid sites are responsible for this catalysis: In the MXene, strong acid sites (both Lewis and Brønsted) catalyse both the ring-opening and the isomerization reactions, while in the Mxene–TiO 2 composite weaker acid sites catalyse only the ring-opening reaction, increasing the selectivity to the mono-alkylated product.

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