Stability of heterogeneous single-atom catalysts: a scaling law mapping thermodynamics to kinetics

Ya Qiong Su; Long Zhang; Yifan Wang; Jin Xun Liu; Valery Muravev; Konstantinos Alexopoulos; Ivo A.W. Filot; Dionisios G. Vlachos; Emiel J.M. Hensen

doi:10.1038/s41524-020-00411-6

Stability of heterogeneous single-atom catalysts: a scaling law mapping thermodynamics to kinetics

Ya Qiong Su, Long Zhang, Yifan Wang, Jin Xun Liu, Valery Muravev, Konstantinos Alexopoulos, Ivo A.W. Filot, Dionisios G. Vlachos (Corresponding author), Emiel J.M. Hensen

Research output: Contribution to journal › Article › Academic › peer-review

62 Citations (Scopus)

Abstract

Heterogeneous single-atom catalysts (SACs) hold the promise of combining high catalytic performance with maximum utilization of often precious metals. We extend the current thermodynamic view of SAC stability in terms of the binding energy (E_bind) of single-metal atoms on a support to a kinetic (transport) one by considering the activation barrier for metal atom diffusion. A rapid computational screening approach allows predicting diffusion barriers for metal–support pairs based on E_bind of a metal atom to the support and the cohesive energy of the bulk metal (E_c). Metal–support combinations relevant to contemporary catalysis are explored by density functional theory. Assisted by machine-learning methods, we find that the diffusion activation barrier correlates with (E_bind)²/E_c in the physical descriptor space. This diffusion scaling-law provides a simple model for screening thermodynamics to kinetics of metal adatom on a support.

Original language	English
Article number	144
Number of pages	7
Journal	npj Computational Materials
Volume	6
Issue number	1
DOIs	https://doi.org/10.1038/s41524-020-00411-6
Publication status	Published - 24 Sept 2020

Funding

The authors acknowledge financial support for the research from The Netherlands Organization for Scientific Research (NWO) through a Vici grant and Nuffic funding. Supercomputing facilities were provided by NWO. This work has received funding from the European Union’s Horizon 2020 research and innovation programme under grant No 686086 (Partial-PGMs). Y.W., K.A., and D.G.V. acknowledge support by the RAPID manufacturing institute, supported by the Department of Energy (DOE) Advanced Manufacturing Office (AMO), award number DE-EE0007888-9.5. RAPID projects at the University of Delaware are also made possible in part by funding provided by the State of Delaware. The Delaware Energy Institute gratefully acknowledges the support and partnership of the State of Delaware in furthering the essential scientific research being conducted through the RAPID projects.

Access to Document

10.1038/s41524-020-00411-6

Cite this

@article{547bceb4b5a94a919085890c3d29ffdc,

title = "Stability of heterogeneous single-atom catalysts: a scaling law mapping thermodynamics to kinetics",

abstract = "Heterogeneous single-atom catalysts (SACs) hold the promise of combining high catalytic performance with maximum utilization of often precious metals. We extend the current thermodynamic view of SAC stability in terms of the binding energy (Ebind) of single-metal atoms on a support to a kinetic (transport) one by considering the activation barrier for metal atom diffusion. A rapid computational screening approach allows predicting diffusion barriers for metal–support pairs based on Ebind of a metal atom to the support and the cohesive energy of the bulk metal (Ec). Metal–support combinations relevant to contemporary catalysis are explored by density functional theory. Assisted by machine-learning methods, we find that the diffusion activation barrier correlates with (Ebind)2/Ec in the physical descriptor space. This diffusion scaling-law provides a simple model for screening thermodynamics to kinetics of metal adatom on a support.",

author = "Su, {Ya Qiong} and Long Zhang and Yifan Wang and Liu, {Jin Xun} and Valery Muravev and Konstantinos Alexopoulos and Filot, {Ivo A.W.} and Vlachos, {Dionisios G.} and Hensen, {Emiel J.M.}",

year = "2020",

month = sep,

day = "24",

doi = "10.1038/s41524-020-00411-6",

language = "English",

volume = "6",

journal = "npj Computational Materials",

issn = "2057-3960",

publisher = "Nature Publishing Group",

number = "1",

}

TY - JOUR

T1 - Stability of heterogeneous single-atom catalysts

T2 - a scaling law mapping thermodynamics to kinetics

AU - Su, Ya Qiong

AU - Zhang, Long

AU - Wang, Yifan

AU - Liu, Jin Xun

AU - Muravev, Valery

AU - Alexopoulos, Konstantinos

AU - Filot, Ivo A.W.

AU - Vlachos, Dionisios G.

AU - Hensen, Emiel J.M.

PY - 2020/9/24

Y1 - 2020/9/24

N2 - Heterogeneous single-atom catalysts (SACs) hold the promise of combining high catalytic performance with maximum utilization of often precious metals. We extend the current thermodynamic view of SAC stability in terms of the binding energy (Ebind) of single-metal atoms on a support to a kinetic (transport) one by considering the activation barrier for metal atom diffusion. A rapid computational screening approach allows predicting diffusion barriers for metal–support pairs based on Ebind of a metal atom to the support and the cohesive energy of the bulk metal (Ec). Metal–support combinations relevant to contemporary catalysis are explored by density functional theory. Assisted by machine-learning methods, we find that the diffusion activation barrier correlates with (Ebind)2/Ec in the physical descriptor space. This diffusion scaling-law provides a simple model for screening thermodynamics to kinetics of metal adatom on a support.

AB - Heterogeneous single-atom catalysts (SACs) hold the promise of combining high catalytic performance with maximum utilization of often precious metals. We extend the current thermodynamic view of SAC stability in terms of the binding energy (Ebind) of single-metal atoms on a support to a kinetic (transport) one by considering the activation barrier for metal atom diffusion. A rapid computational screening approach allows predicting diffusion barriers for metal–support pairs based on Ebind of a metal atom to the support and the cohesive energy of the bulk metal (Ec). Metal–support combinations relevant to contemporary catalysis are explored by density functional theory. Assisted by machine-learning methods, we find that the diffusion activation barrier correlates with (Ebind)2/Ec in the physical descriptor space. This diffusion scaling-law provides a simple model for screening thermodynamics to kinetics of metal adatom on a support.

UR - http://www.scopus.com/inward/record.url?scp=85091427061&partnerID=8YFLogxK

U2 - 10.1038/s41524-020-00411-6

DO - 10.1038/s41524-020-00411-6

M3 - Article

AN - SCOPUS:85091427061

SN - 2057-3960

VL - 6

JO - npj Computational Materials

JF - npj Computational Materials

IS - 1

M1 - 144

ER -

Stability of heterogeneous single-atom catalysts: a scaling law mapping thermodynamics to kinetics

Abstract

Funding

Access to Document

Other files and links

Fingerprint

Cite this