Demonstration of chemistry at a point through
restructuring and catalytic activation at anchored
, Evangelos I. Papaioannou
, Wan K.W. Ramli
, David N. Miller
, Billy J. Murdoch
, Ahmed Umar
, Anders J. Barlow
, Peter J. Cumpson
, John T.S. Irvine
& Ian S. Metcalfe
Metal nanoparticles prepared by exsolution at the surface of perovskite oxides have been
recently shown to enable new dimensions in catalysis and energy conversion and storage
technologies owing to their socketed, well-anchored structure. Here we show that contrary to
general belief, exsolved particles do not necessarily re-dissolve back into the underlying
perovskite upon oxidation. Instead, they may remain pinned to their initial locations, allowing
one to subject them to further chemical transformations to alter their composition, structure
and functionality dramatically, while preserving their initial spatial arrangement. We refer to
this concept as chemistry at a point and illustrate it by tracking individual nanoparticles
throughout various chemical transformations. We demonstrate its remarkable practical utility
by preparing a nanostructured earth abundant metal catalyst which rivals platinum on a
weight basis over hundreds of hours of operation. Our concept enables the design of com-
positionally diverse conﬁned oxide particles with superior stability and catalytic reactivity.
School of Chemistry, University of St Andrews, St Andrews KY16 9ST, UK.
School of Engineering, Newcastle University, Newcastle-upon-Tyne, NE1 7RU,
School of Bioprocess Engineering, University Malaysia Perlis, 02600 Perlis, Malaysia.
National EPSRC XPS Users’ Service (NEXUS), School of
Mechanical and Systems Engineering, Newcastle University, Newcastle upon Tyne, NE1 7RU, UK.
Sasol (UK) Ltd., St Andrews KY16 9ST, UK. Dragos Neagu
and Evangelos I. Papaioannou contributed equally to this work. Correspondence and requests for materials should be addressed to
J.T.S.I. (email: firstname.lastname@example.org) or to I.S.M. (email: email@example.com)