Computationally aided, entropy-driven synthesis of highly efficient and durable multi-elemental alloy catalysts

Abstract

Multi-elemental alloy nanoparticles (MEA-NPs) hold great promise for catalyst discovery in a virtually unlimited compositional space. However, rational and controllable synthesize of these intrinsically complex structures remains a challenge. Here, we report the computationally aided, entropy-driven design and synthesis of highly efficient and durable catalyst MEA-NPs. The computational strategy includes prescreening of millions of compositions, prediction of alloy formation by density functional theory calculations, and examination of structural stability by a hybrid Monte Carlo and molecular dynamics method. Selected compositions can be efficiently and rapidly synthesized at high temperature (e.g., 1500 K, 0.5 s) with excellent thermal stability. We applied these MEA-NPs for catalytic NH 3 decomposition and observed outstanding performance due to the synergistic effect of multielemental mixing, their small size, and the alloy phase. We anticipate that the computationally aided rational design and rapid synthesis of MEA-NPs are broadly applicable for various catalytic reactions and will accelerate material discovery. Computationally aided, entropy-driven synthesis of highly efficient and durable multi-elemental alloy catalysts.(11), eaaz0510. 6 Sci Adv ARTICLE TOOLS

On the electronic structure and hydrogen evolution reaction activity of platinum group metal-based high-entropy-alloy nanoparticles

“…11 Löffler et al found that Cr-Mn-Fe-Co-Ni complex solid solution showed at least comparable catalytic activity to Pt in oxygen reduction reaction (ORR), in despite that none of its constituents had good ORR activity. 12 In addition to HEA, other alternative denominations have also been discussed elsewhere, such as complex solid solutions, [12][13][14] multiprincipal element alloys, 15 polyelemental particles, 16,17 multi-elemental alloy, 18 and multimetallic clusters/particles. 19 These kinds of alloys may present a class of promising ideal catalysts having desired activity, stability and selectivity and thus make a paradigm shi in catalysis research.…”

“…19 These kinds of alloys may present a class of promising ideal catalysts having desired activity, stability and selectivity and thus make a paradigm shi in catalysis research. 20 These alloy catalysts with appealing performances have been reported recently, [10][11][12][17][18][19][21][22][23][24] yet, the interpretation on their properties is still challenging. Quite recently, Rossmeisl and co-authors have made a great step in theoretically predicting ORR 25 and CO 2 and CO reduction 26 properties on HEAs by combing density functional theory calculations and supervised machine learning.…”

“…To date, the reports on HEA NPs are still scarce compared to HEA bulk, and almost all the syntheses require special techniques such as carbothermal shock, 10,18,19,21 spark ablation, 27 sputtering, 12 and mechanical ball milling. 28 Here, we show the chemical synthesis of single-phase HEA NPs consisting of Ru, Rh, Pd, Ir, and Pt in a nearly equal molar ratio by a simple onepot polyol method.…”

Nano High‐Entropy Materials: Synthesis Strategies and Catalytic Applications

“…Quite recently, they applied theoretical computation to facilitate the rational design of HEA-NPs. [81] Prescreening millions of compositions was performed before practical synthesis of HEA-NPs via CTS method, density functional theory (DFT) calculations were carried out to predict their formation energies, while a hybrid Monte Carlo and molecular dynamics (MC-MD) approach was implemented to stimulate their formation process both thermodynamically and kinetically. This computational strategy provides rational guidance for HEA-NPs design and saves substantial time and laboratory work from experimentally exploring an actually unlimited compositional space.…”

Engineering sub-2 nm ultrasmall high-entropy alloy nanoparticles with extremely superior performance for hydrogen evolution catalysis

“…High-entropy alloys (HEAs) have demonstrated significant potential applications in many fields due to their unique and fascinating properties [16][17][18][19][20] . Thus, HEAs have recently garnered increased attentions and become one of the hottest materials.…”