TY - JOUR
T1 - The MOF-driven synthesis of supported palladium clusters with catalytic activity for carbene-mediated chemistry
AU - Fortea-Pérez, Francisco R.
AU - Mon, Marta
AU - Ferrando-Soria, Jesús
AU - Boronat, Mercedes
AU - Leyva-Pérez, Antonio
AU - Corma, Avelino
AU - Herrera, Juan Manuel
AU - Osadchii, Dmitrii
AU - Gascon Sabate, Jorge
AU - Armentano, Donatella
AU - Pardo, Emilio
N1 - Publisher Copyright:
© 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.
PY - 2017/7/1
Y1 - 2017/7/1
N2 - The development of catalysts able to assist industrially important chemical processes is a topic of high importance. In view of the catalytic capabilities of small metal clusters, research efforts are being focused on the synthesis of novel catalysts bearing such active sites. Here we report a heterogeneous catalyst consisting of Pd4 clusters with mixed-valence 0/+1 oxidation states, stabilized and homogeneously organized within the walls of a metal-organic framework (MOF). The resulting solid catalyst outperforms state-of-the-art metal catalysts in carbene-mediated reactions of diazoacetates, with high yields (>90%) and turnover numbers (up to 100,000). In addition, the MOF-supported Pd4 clusters retain their catalytic activity in repeated batch and flow reactions (>20 cycles). Our findings demonstrate how this synthetic approach may now instruct the future design of heterogeneous catalysts with advantageous reaction capabilities for other important processes.
AB - The development of catalysts able to assist industrially important chemical processes is a topic of high importance. In view of the catalytic capabilities of small metal clusters, research efforts are being focused on the synthesis of novel catalysts bearing such active sites. Here we report a heterogeneous catalyst consisting of Pd4 clusters with mixed-valence 0/+1 oxidation states, stabilized and homogeneously organized within the walls of a metal-organic framework (MOF). The resulting solid catalyst outperforms state-of-the-art metal catalysts in carbene-mediated reactions of diazoacetates, with high yields (>90%) and turnover numbers (up to 100,000). In addition, the MOF-supported Pd4 clusters retain their catalytic activity in repeated batch and flow reactions (>20 cycles). Our findings demonstrate how this synthetic approach may now instruct the future design of heterogeneous catalysts with advantageous reaction capabilities for other important processes.
UR - http://www.scopus.com/inward/record.url?scp=85021403711&partnerID=8YFLogxK
U2 - 10.1038/nmat4910
DO - 10.1038/nmat4910
M3 - Article
C2 - 28604715
AN - SCOPUS:85021403711
SN - 1476-1122
VL - 16
SP - 760
EP - 766
JO - NATURE MATERIALS
JF - NATURE MATERIALS
IS - 7
ER -