TY - JOUR
T1 - Programmable catalysis by support polarization
T2 - elucidating and breaking scaling relations
AU - Jung, Seongjoo
AU - Pizzolitto, Cristina
AU - Biasi, Pierdomenico
AU - Dauenhauer, Paul J.
AU - Birol, Turan
N1 - Publisher Copyright:
© 2023, The Author(s).
PY - 2023/12
Y1 - 2023/12
N2 - The Sabatier principle and the scaling relations have been widely used to search for and screen new catalysts in the field of catalysis. However, these powerful tools can also serve as limitations of catalyst control and breakthrough. To overcome this challenge, this work proposes an efficient method of studying catalyst control by support polarization from first-principles. The results demonstrate that the properties of catalysts are determined by support polarization, irrespective of the magnitude of spontaneous polarization of support. The approach enables elucidating the scaling relations between binding energies at various polarization values of support. Moreover, we observe the breakdown of scaling relations for the surface controlled by support polarization. By studying the surface electronic structure and decomposing the induced charge into contributions from different atoms and orbitals, we identify the inherent structural property of the interface that leads to the breaking of the scaling relations. Specifically, the displacements of the underlying oxide support impose its symmetry on the catalyst, causing the scaling relations between different adsorption sites to break.
AB - The Sabatier principle and the scaling relations have been widely used to search for and screen new catalysts in the field of catalysis. However, these powerful tools can also serve as limitations of catalyst control and breakthrough. To overcome this challenge, this work proposes an efficient method of studying catalyst control by support polarization from first-principles. The results demonstrate that the properties of catalysts are determined by support polarization, irrespective of the magnitude of spontaneous polarization of support. The approach enables elucidating the scaling relations between binding energies at various polarization values of support. Moreover, we observe the breakdown of scaling relations for the surface controlled by support polarization. By studying the surface electronic structure and decomposing the induced charge into contributions from different atoms and orbitals, we identify the inherent structural property of the interface that leads to the breaking of the scaling relations. Specifically, the displacements of the underlying oxide support impose its symmetry on the catalyst, causing the scaling relations between different adsorption sites to break.
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U2 - 10.1038/s41467-023-43641-0
DO - 10.1038/s41467-023-43641-0
M3 - Article
C2 - 38016999
AN - SCOPUS:85178060097
SN - 2041-1723
VL - 14
JO - Nature communications
JF - Nature communications
IS - 1
M1 - 7795
ER -