posted on 2024-03-14, 16:08authored byWu Shu, Jiancong Li, Jin-Xun Liu, Chuwei Zhu, Tairan Wang, Li Feng, Runhai Ouyang, Wei-Xue Li
The nature of the active sites and their structure sensitivity
are the keys to rational design of efficient catalysts but have been
debated for almost one century in heterogeneous catalysis. Though
the Brønsted–Evans–Polanyi (BEP) relationship along
with linear scaling relation has long been used to study the reactivity,
explicit geometry, and composition properties are absent in this relationship,
a fact that prevents its exploration in structure sensitivity of supported
catalysts. In this work, based on interpretable multitask symbolic
regression and a comprehensive first-principles data set, we discovered
a structure descriptor, the topological under-coordinated number
mediated by number of valence electrons and the lattice constant,
to successfully address the structure sensitivity of metal catalysts.
The database used for training, testing, and transferability investigation
includes bond-breaking barriers of 20 distinct chemical bonds over
10 transition metals, two metal crystallographic phases, and 17 different
facets. The resulting 2D descriptor composing the structure term and
the reaction energy term shows great accuracy to predict the reaction
barriers and generalizability over the data set with diverse chemical
bonds in symmetry, bond order, and steric hindrance. The theory is
physical and concise, providing a constructive strategy not only
to understand the structure sensitivity but also to decipher the entangled
geometric and electronic effects of metal catalysts. The insights
revealed are valuable for the rational design of the site-specific
metal catalysts.