Magnetically Enhanced Oxygen Evolution Reaction in Mild Alkaline Electrolytes by Building Catalysts on Magnetic Frame.

Under large current densities, the excessive hydroxide ion (OH) consumption hampers alkaline water splitting involving the oxygen evolution reaction (OER). High OH concentration (≈30 wt.%) is often used to enhance the catalytic activity of OER, but it also leads to higher corrosion in practical systems. To achieve higher catalytic activity in low OH concentration, catalysts on magnetic frame (CMF) are built to utilize the local magnetic convection induced from the host frame's magnetic field distributions. This way, a higher reaction rate can be achieved in relatively lower OH concentrations. A CMF model system with catalytically active CoFeOx nanograins grown on the magnetic Ni foam is demonstrated. The OER current of CoFeOx@NF receives ≈90% enhancement under 400 mT (900 mA cm-2 at 1.65 V) compared to that in zero field, and exhibits remarkable durability over 120 h. As a demonstration, the water-splitting performance sees a maximum 45% magnetic enhancement under 400 mT in 1 m KOH (700 mA cm-2 at 2.4 V), equivalent to the concentration enhancement of the same electrode in a more corrosive 2 m KOH electrolyte. Therefore, the catalyst-on-magnetic-frame strategy can make efficient use of the catalysts and achieve higher catalytic activity in low OH concentration by harvesting local magnetic convection.

Predicting Complex Relaxation Processes in Metallic Glass.

Relaxation processes significantly influence the properties of glass materials. However, understanding their specific origins is difficult; even more challenging is to forecast them theoretically. In this study, using microseconds molecular dynamics simulations together with an accurate many-body interaction potential, we predict that an Al_{90}Sm_{10} metallic glass would have complex relaxation behaviors: In addition to the main (α) relaxation, the glass (i) shows a pronounced secondary (ß) relaxation at cryogenic temperatures and (ii) exhibits an anomalous relaxation process (α_{2}) accompanying α relaxation. Both of the predictions are verified by experiments. Computational simulations reveal the microscopic origins of relaxation processes: while the pronounced ß relaxation is attributed to the abundance of stringlike cooperative atomic rearrangements, the anomalous α_{2} process is found to correlate with the decoupling of the faster motions of Al with slower Sm atoms. The combination of simulations and experiments represents a first glimpse of what may become a predictive routine and integral step for glass physics.

Fundamental Link between ß Relaxation, Excess Wings, and Cage-Breaking in Metallic Glasses.

In glassy materials, the Johari-Goldstein secondary (ß) relaxation is crucial to many properties as it is directly related to local atomic motions. However, a long-standing puzzle remains elusive: why some glasses exhibit ß relaxations as pronounced peaks while others present as unobvious excess wings? Using microsecond atomistic simulation of two model metallic glasses (MGs), we demonstrate that such a difference is associated with the number of string-like collective atomic jumps. Relative to that of excess wings, we find that MGs having pronounced ß relaxations contain larger numbers of such jumps. Structurally, they are promoted by the higher tendency of cage-breaking events of their neighbors. Our results provide atomistic insights for different signatures of the ß relaxation that could be helpful for understanding the low-temperature dynamics and properties of MGs.