TY - JOUR
T1 - Interstitial modification of palladium nanoparticles with boron atoms as a green catalyst for selective hydrogenation
AU - Chan, Chun Wong Aaron
AU - Mahadi, Abdul Hanif
AU - Li, Molly Meng Jung
AU - Corbos, Elena Cristina
AU - Tang, Chiu
AU - Jones, Glenn
AU - Kuo, Winson Chun Hsin
AU - Cookson, James
AU - Brown, Christopher Michael
AU - Bishop, Peter Trenton
AU - Tsang, Shik Chi Edman
N1 - Funding Information:
We thank the EPSRC, UK and Johnson Matthey for funding this work and a DPhil studentship to ACWAC. We also thank Miss Elisabeth Wolf (Oxford Chemistry) for the assistance in the experiments of acetylene hydrogenation. E.C.C. thanks the European Commission for fellowship (PIIF-GA-2009-252242: NANOTUNE). EXAFS experiments were undertaken at the Diamond Light Source (experiment SM-6693-1). G.J. is indebted to the Royal Society for an Industrial Fellowship and a membership of the UK’s HPC Materials Chemistry Consortium (EP/F067496). We acknowledge the support from HECToR, the UK’s national high-performance computing service provided by UoE HPCx Ltd at the University of Edinburgh, Cray Inc and NAG Ltd.
Publisher Copyright:
© 2014 Macmillan Publishers Limited. All rights reserved.
Copyright:
Copyright 2017 Elsevier B.V., All rights reserved.
PY - 2014/12
Y1 - 2014/12
N2 - Lindlar catalysts comprising of palladium/calcium carbonate modified with lead acetate and quinoline are widely employed industrially for the partial hydrogenation of alkynes. However, their use is restricted, particularly for food, cosmetic and drug manufacture, due to the extremely toxic nature of lead, and the risk of its leaching from catalyst surface. In addition, the catalysts also exhibit poor selectivities in a number of cases. Here we report that a non-surface modification of palladium gives rise to the formation of an ultra-selective nanocatalyst. Boron atoms are found to take residence in palladium interstitial lattice sites with good chemical and thermal stability. This is favoured due to a strong host-guest electronic interaction when supported palladium nanoparticles are treated with a borane tetrahydrofuran solution. The adsorptive properties of palladium are modified by the subsurface boron atoms and display ultra-selectivity in a number of challenging alkyne hydrogenation reactions, which outclass the performance of Lindlar catalysts.
AB - Lindlar catalysts comprising of palladium/calcium carbonate modified with lead acetate and quinoline are widely employed industrially for the partial hydrogenation of alkynes. However, their use is restricted, particularly for food, cosmetic and drug manufacture, due to the extremely toxic nature of lead, and the risk of its leaching from catalyst surface. In addition, the catalysts also exhibit poor selectivities in a number of cases. Here we report that a non-surface modification of palladium gives rise to the formation of an ultra-selective nanocatalyst. Boron atoms are found to take residence in palladium interstitial lattice sites with good chemical and thermal stability. This is favoured due to a strong host-guest electronic interaction when supported palladium nanoparticles are treated with a borane tetrahydrofuran solution. The adsorptive properties of palladium are modified by the subsurface boron atoms and display ultra-selectivity in a number of challenging alkyne hydrogenation reactions, which outclass the performance of Lindlar catalysts.
UR - http://www.scopus.com/inward/record.url?scp=85026767077&partnerID=8YFLogxK
U2 - 10.1038/ncomms6787
DO - 10.1038/ncomms6787
M3 - Journal article
AN - SCOPUS:85026767077
SN - 2041-1723
VL - 5
JO - Nature Communications
JF - Nature Communications
M1 - 5787
ER -