Machine-learning-accelerated screening of single metal atoms anchored on MnPS₃ monolayers as promising bifunctional oxygen electrocatalysts

Abstract

Searching for bifunctional oxygen electrocatalysts with good catalytic performance to promote the oxygen evolution/reduction reactions (OER/ORR) is of great significance to the development of sustainable and renewable clean energy. Herein,...

Theoretical Insights on the Charge State and Bifunctional OER/ORR Electrocatalyst Activity in 4d-Transition-Metal-Doped g-C3N4 Monolayers

“…For these 4d-TM N @C 54 N 71 and 4d-TM int @C 54 N 72 systems, most RDS of OER are focused on the *OH to *O (Δ G 2 OER = Δ G *O – Δ G *OH ) and *O to *OOH (Δ G 3 OER = Δ G *OOH – Δ G *O ) elemental reaction steps ,, ; most RDS of ORR is either the initial formation of *OOH species (Δ G 1 ORR = Δ G *OOH – 4.92 eV) or the final conversion of *OH species to water (Δ G 4 ORR = −Δ G *OH ). ,− Therefore, considering the obtained scaling relationship between the Δ G *OOH and Δ G *OH values (Δ G *O = 1.24Δ G *OH + 1.28) of the studied 4d-TM N @C 54 N 71 and 4d-TM int @C 54 N 72 systems (Figure a), the OER and ORR activities can be then described by the Δ G *OOH and Δ G *OH . The four free energy changes of OER (eq S14) can be modified as follows: Δ G 1 normal O E R = Δ G normal O H * Δ G 2 normal O E R = 0.24 Δ G normal O H * + 1.28 Δ G 3 normal O E R = Δ G normal O O H * − 1.24 Δ G normal O H ...…”

“…These SACs feature single transition-metal (TM) atoms dispersed on a substrate to serve as the active site. Their applications span a range of electrocatalytic processes, including the bifunctional OER/ORR electrocatalysts, nitrogen reduction reaction (NRR), hydrogen evolution reaction (HER), CO 2 reduction reaction (CO 2 RR), and so on. Especially, two-dimensional (2D) material graphitic carbon nitride (g-C 3 N 4 ) is a popular substrate of SACs for the bifunctional OER/ORR due to its abundance and low cost. − Therefore, the g-C 3 N 4 doped or loaded with metal species can serve as SACs for the bifunctional OER/ORR in acidic or alkaline electrolytes, , which has recently come to the attention of scholars.…”

Rational design of single transition-metal atoms anchored on a PtSe2 monolayer as bifunctional OER/ORR electrocatalysts: a defect chemistry and machine learning study

“…The analysis focuses on determining the optimal model use for the OER/ORR descriptor and reaction mechanism of each catalyst. 98,99 The detailed information of each descriptor is summarized in Table S15 †…”

Is Fe the Most Active Site for Fe/N-Doped Graphdiyne?

“…To probe the trending of codoping of Fe and N, we performed a machine learning analysis on the Δ G (OH*) with the Gradient Boost Regression (GBR) algorithm , because it is less likely to overfit the data . Several electronic and geometric features of the active site are included as the features, which include the p-band center (pbc), Bader charge, magnetic moment (mag), and average distance with adjacent atoms (d_ave); dd is the sum of r ab – ( r a + r b ) over all the bonds the C atom take parts in ( r ab is the bond length between atom a and b, and r a , r b are the radii of atoms a and b).…”