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Title: A First-Principles Approach to Modeling Surface Site Stabilities on Multimetallic Catalysts

Journal Article · · ACS Catalysis
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2];  [3]; ORCiD logo [4]
  1. Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); SLAC
  2. Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
  3. Karlsruhe Inst. of Technology (KIT), Eggenstein-Leopoldshafen (Germany)
  4. SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

The study of multimetallic alloys and the multitude of possible surface compositions have sparked a tremendous interest in engineering low-cost materials with high activity and selectivity in heterogeneous catalysis. Multimetallic systems provide complementary functionalities and an unprecedented tunability when designing catalyst formulations. However, due to their immense structural and compositional complexity, the investigation and identification of an optimal catalyst is a tedious and time-consuming process, both experimentally and theoretically. Therefore, theoretical design principles are highly desirable to accelerate the screening of catalyst structures across the vast compositional space. In this paper, we introduce a simple and general model for predicting the site stability of multimetallic surfaces and nanoparticles, which is based on physical principles. The model requires only a small set of density functional theory (DFT) calculations of metal atom binding energies on monometallic and dilute alloy surface slabs to optimize the parameters in the simple model. The resulting model allows for the quantification of the stability of any particular atom site in any conceivable chemical environment across a wide range of morphologies, sizes, and arrangements by interpolating the derived parameters from a monometallic system to a completely diluted alloyed system. Herein, we demonstrate the robustness of the model across an extensive data set of transition metal alloy surfaces and 147-atoms cuboctahedral nanoparticles (NPs) composed of IrRhRu and PtPdRu. In conclusion, our approach yields mean absolute errors of ≈0.15 (IrRhRu), 0.20 (PtPdRu), 0.19 (IrRhRu NP), and 0.26 (PtPdRu NP) eV relative to site binding energies calculated using DFT.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); Knut and Alice Wallenberg Foundation; German Research Foundation (DFG)
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
2323492
Journal Information:
ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 2 Vol. 14; ISSN 2155-5435
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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