Conformal Noble Metal High-Entropy Alloy Nanofilms by Atomic Layer Deposition for an Enhanced Hydrogen Evolution Reaction.

The current synthesis methods of high-entropy alloy (HEA) thin-film coatings face huge challenges in facile preparation, precise thickness control, conformal integration, and affordability. These challenges are more specific and noteworthy for noble metal-based HEA thin films where the conventional sputtering methods encounter thickness control and high-cost issues (high-purity noble metal targets required). Herein, for the first time, we report a facile and controllable synthesis process of quinary HEA coatings consisting of noble metals (Rh, Ru, Pt, Pd, and Ir), by sequential atomic layer deposition (ALD) coupled with electrical Joule heating for post-alloying. Furthermore, the resulting quinary HEA thin film with a thickness of ∼50 nm and an atomic ratio of 20:15:21:18:27 shows promising potential as a platform for catalysis, exhibiting enhanced electrocatalytic hydrogen evolution reaction (HER) performances with lower overpotentials (e.g., from 85 to 58 mV in 0.5 M H2SO4) and higher stability (by retaining more than 92% of the initial current after 20 h with a current density of 10 mA/cm2 in 0.5 M H2SO4) than other noble metal-based structure counterparts in this work. The enhanced material properties and device performances are attributed to the efficient electron transfer of HEA with the increased number of active sites. This work not only presents RhRuPtPdIr HEA thin films as promising HER catalysts but also sheds light on controllable fabrication of conformal HEA-coated complex structures toward a broad range of applications.

In Situ Observation of Shear-Induced Jamming Front Propagation during Low-Velocity Impact in Polypropylene Glycol/Fumed Silica Shear Thickening Fluids.

Shear jamming, a relatively new type of phase transition from discontinuous shear thickening into a solid-like state driven by shear in dense suspensions, has been shown to originate from frictional interactions between particles. However, not all dense suspensions shear jam. Dense fumed silica colloidal systems have wide applications in the industry of smart materials from body armor to dynamic dampers due to extremely low bulk density and high colloid stability. In this paper, we provide new evidence of shear jamming in polypropylene glycol/fumed silica suspensions using optical in situ speed recording during low-velocity impact and explain how it contributes to impact absorption. Flow rheology confirmed the presence of discontinuous shear thickening at all studied concentrations. Calculations of the flow during impact reveal that front propagation speed is 3-5 times higher than the speed of the impactor rod, which rules out jamming by densification, showing that the cause of the drastic impact absorption is the shear jamming. The main impact absorption begins when the jamming front reaches the boundary, creating a solid-like plug under the rod that confronts its movement. These results provide important insights into the impact absorption mechanism in fumed silica suspensions with a focus on shear jamming.