High-entropy materials for electrocatalytic applications: a review of first principles modeling and simulations

High-entropy materials, for both complexity in structure and superiority in performance, have been widely confirmed to be one possible kind of advanced electrocatalyst. Significant efforts have been dedicated to modeling the atomic-level details of high-entropy catalysts to improve the viability for bottom-up design of advanced electrocatalysts. In this review, first, we survey developments in various modeling methods that are based on density functional theory. We review progress in density functional theory simulations for emulating different high-entropy electrocatalysts. Then, we review the advancements in simulations of high-entropy materials for electrocatalytic applications. Finally, we present prospects in this field. Abbreviations: HEMs: high-entropy materials; CCMs: compositionally complex materials; DFT: density functional theory; LDA: local density approximation; GGA: generalized gradient approximation; VASP: Vienna Ab initio simulation package; ECP: effective core potential; PAW: projector-augmented wave potential; VCA: virtual crystal approximation; CPA: coherent potential approximation; SQS: special quasi-random structures; SSOS: small set of ordered structures; SLAE: similar local atomic environment; HEAs: high-entropy alloys; FCC: face-centered cubic; BCC: body-centered cubic; HCP: hexagonal close-packed; ORR: oxygen reduction reaction; OER: oxide evolution reaction; HER: hydrogen evolution reaction; RDS: rate-limiting step; AEM: adsorbate evolution mechanism; LOM: lattice oxygen oxidation mechanism; HEOs: high-entropy oxides; OVs: oxygen vacancies; PDOS: projected densities of states; ADR: ammonia decomposition reaction; NRR: nitrogen reduction reaction; CO2RR: CO2 reduction reaction; TMDC: transition metal dichalcogenide; TM: transition metal; AOR: alcohol oxidation reaction; GOR: glycerol oxidation reaction; UOR: urea oxidation reaction; HEI: high-entropy intermetallic. GRAPHICAL ABSTRACT IMPACT STATEMENT This paper reviews recent developments in the field of atomistic simulations of high-entropy electrocatalysts, one of emerging state-of-the-art catalytic materials.