Atomic Magnetic Heating Effect Enhanced Hydrogen Evolution Reaction of Gd@MoS2 Single-Atom Catalysts.

Atomic heating on single atoms (SAs) to maximize the catalytic efficiency of each active site would be a fascinating solution to break the bottleneck for the performance improvement of single-atom catalysts (SACs) but highly challenging task. Here, based on the Gd@MoS2 SACs synthesized by a facile laser molecular beam epitaxy method, high-frequency alternating magnetic field (AMF) technology is employed to induce atomic magnetic heating on Gd SAs that is meanwhile demonstrated to be the catalytic active center. Significant improvement in catalytic kinetics under AMF excitation (3.9 mT) is achieved, yielding a remarkable enhancement of hydrogen evolution reaction magnetothermal-current by ≈924%. Through theoretical calculations and spin-related electrochemical experiments, such promotion in catalyst activity can be attributed to spin flip (or canting) in Gd SAs leading to the atomic magnetic heating effect on catalytic active center. Together with the embodied high stability, the implement of AMF to the SAs field is demonstrated in this work, and the precisely atomic magnetic heating on specific SAs offers unprecedented thinking for further improvement of SACs performance in the future.

Alternating Magnetic Field Induced Magnetic Heating in Ferromagnetic Cobalt Single-Atom Catalysts for Efficient Oxygen Evolution Reaction.

Alternating magnetic field (AMF) is a promising methodology for further improving magnetic single-atom catalyst (SAC) activity toward oxygen evolution reaction (OER). Herein, the anchoring of Co single atoms on MoS2 support (Co@MoS2), leading to the appearance of in-plane room-temperature ferromagnetic properties, is favorable for the parallel spin arrangement of oxygen atoms when a magnetic field is applied. Moreover, field-assisted electrocatalytic experiments confirmed that the spin direction of Co@MoS2 is changing with the applied magnetic field. On this basis, under AMF, the active sites in ferromagnetic Co@MoS2 were heated by exploiting the magnetic heating generated from spin polarization flip of these SACs to further expedite OER efficiency, with overpotential at 10 mA cm-2 reduced from 317 mV to 250 mV. This work introduces a feasible and efficient approach to enhance the OER performance of Co@MoS2 by AMF, shedding some light on the further development of magnetic SACs for energy conversion.

Interlayer-Confined NiFe Dual Atoms within MoS2 Electrocatalyst for Ultra-Efficient Acidic Overall Water Splitting.

Confining dual atoms (DAs) within the van der Waals gap of 2D layered materials is expected to expedite the kinetic and energetic strength in catalytic process, yet is a huge challenge in atomic-scale precise assembling DAs within two adjacent layers in the 2D limit. Here, an ingenious approach is proposed to assemble DAs of Ni and Fe into the interlayer of MoS2 . While inheriting the exceptional merits of diatomic species, this interlayer-confined structure arms itself with confinement effect, displaying the more favorable adsorption strength on the confined metal active center and higher catalytic activity towards acidic water splitting, as verified by intensive research efforts of theoretical calculations and experimental measurements. Moreover, the interlayer-confined structure also renders metal DAs a protective shelter to survive in harsh acidic environment. The findings embodied the confinement effects at the atom level, and interlayer-confined assembling of multiple species highlights a general pathway to advance interlayer-confined DAs catalysts within various 2D materials.