Non-equilibrium reducing flame aerosol process to create supported high-entropy alloy nanoparticles

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Abstract
High-entropy alloy (HEA) nanomaterials provide opportunities and property combinations for energy and electronic applications, but their practical synthesis faces challenges of elemental immiscibility, metal reducibility, and particle aggregation during their synthesis. Herein, we report a broadly applicable non-equilibrium, scalable, and in-situ reducing flame aerosol process for synthesis of supported HEA nanoparticles. This versatile process can directly load a high concentration of 2 ~ 4 nm HEA nanoparticles on various 1- to 3-dimensional supports. Notably, simultaneous formation of HEA nanoparticles and a mesoporous silica support was successfully realized in a single step. Exploration of this process demonstrates the role of kinetics and entropy on decreasing alloy particle size and altering the reducibility of elements. We propose an entropy-induced reduction mechanism to incorporate oxidizable elements into HEAs, which extends the compositional space of HEA nanoparticles. As a representative catalytic application, we present a RuPdOsIrPt/graphene electrocatalyst with high activity and stability for hydrogen oxidation reaction. Our findings open horizons for high-performance HEA design and applications in diverse fields such as catalysis, electrochemistry, and sensing.
Funding Information
  • Building Technologies Office (DEEE-0008675)
  • National Energy Technology Laboratory (DE-FE0032209)
  • Division of Chemical, Bioengineering, Environmental and Transport Systems (CBET-1804996)
  • Basic Energy Sciences (DE-AC52-07NA27344)
  • Basic Energy Sciences (DE-SC0012704)
  • Basic Energy Sciences (DE-AC02-05CH11231)
  • Division of Materials Research (DMR-2427094)

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