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
VL - 6
JO - npj Computational Materials
JF - npj Computational Materials
SN - 2057-3960
IS - 1
M1 - 144
ER -