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Page 6 of 21 Chen et al. J Mater Inf 2022;2:19 https://dx.doi.org/10.20517/jmi.2022.23

Figure 3. Top and side views of (A) on-top, (B) bridge and (C) hollow-HCP surface microstructures in a 3 × 4 × 4 slab, where atoms
with different colors denote different regions. (D) Top view for adsorption configurations for different chemical species on a
representative HEA FCC (111) surface. Atoms belonging to the top surface layer are labeled with a cross. Bonds between adsorbates
and metal atoms are shown as red lines. Parameterization of the surface configurations is achieved using nearest neighbors. (E) OH*
on-top binding. Each colored zone represents a set of three parameters. Orange (1): binding site. Light green (2): surface neighbors
singly coordinated to binding site. Light gray (3): subsurface neighbors singly coordinated to binding site. (F) O* FCC hollow site
binding. Each colored zone represents a set of five parameters, except for zone 1, where the set is 35 parameters. Zones 1-3 as in (E)
and additionally dark green (4): surface neighbors doubly coordinated to binding site. Dark gray (5): subsurface neighbors doubly
coordinated to binding site. (A-C) Reproduced with permission [53] . Copyright 2021, American Chemical Society. (D) Reproduced with
permission [56] . Copyright 2021, American Chemical Society. (E) and (F) Reproduced with permission [60] . Copyright 2019, Elsevier. HCP:
hexagonal-closed packed; FCC: face-centered cubic; HEA: high-entropy alloy.

1911 configurations. Combined with data analytics and ML, the scaling relationships among the binding
energies of NH * (x = 0, 1, 2 or 3) can still be seen in FeCoNiCuMo, as in the case of monometallic
x
surfaces [57,58] . These correlations indicate that the adsorption energy of N* could be a good descriptor for
ammonia decomposition and synthesis on these HEAs.

The adsorption of OH* on Pt(111) is ~0.1 eV stronger than the optimum adsorption energy based on
[59]
Sabatier volcano plots for catalyzing the ORR . Batchelor et al. presented HT DFT calculated adsorption
[60]
energies of OH* and O* on the (111) surface of an IrPdPtRhRu HEA . As shown in Figure 3E and F, the
most stable adsorption sites of OH* and O* are the top and FCC hollow adsorption sites, respectively. A
model was established to link the local atomic arrangement around the adsorption sites to the adsorption
energy, which can predict the adsorption energy values on all possible surface sites. Our group extended this
model from the (111) surface to other Miller index surfaces, including the (100), (110), (211) and (532) of an
[61]
equimolar FCC IrPdPtRhRu HEA . A total of 12 types of coordination environments were considered for
HT DFT calculations of the adsorption energy of OH* [Figure 4A], including more than 1,000 data points.
According to these data points, we developed and trained a neural network model with high accuracy and
universality. The ligand and coordination effects on the adsorption energy were analyzed sequentially by the
feature importance based on our developed neural network model [Figure 4B]. Quantitatively, the
adsorption energy was found to have a linear relationship with the total coordination number of nearest
neighbors. More interestingly, the neural network model can be simplified to a simple linear scaling
relationship with only a slight loss of accuracy. It has been demonstrated that these recently developed