The oxygen evolution reaction (OER) is the bottleneck that limits the energy efficiency of water-splitting. The process involves four electrons' transfer and the generation of triplet state O
from ...singlet state species (OH
or H
O). Recently, explicit spin selection was described as a possible way to promote OER in alkaline conditions, but the specific spin-polarized kinetics remains unclear. Here, we report that by using ferromagnetic ordered catalysts as the spin polarizer for spin selection under a constant magnetic field, the OER can be enhanced. However, it does not applicable to non-ferromagnetic catalysts. We found that the spin polarization occurs at the first electron transfer step in OER, where coherent spin exchange happens between the ferromagnetic catalyst and the adsorbed oxygen species with fast kinetics, under the principle of spin angular momentum conservation. In the next three electron transfer steps, as the adsorbed O species adopt fixed spin direction, the OER electrons need to follow the Hund rule and Pauling exclusion principle, thus to carry out spin polarization spontaneously and finally lead to the generation of triplet state O
. Here, we showcase spin-polarized kinetics of oxygen evolution reaction, which gives references in the understanding and design of spin-dependent catalysts.
Abstract
Producing hydrogen by water electrolysis suffers from the kinetic barriers in the oxygen evolution reaction (OER) that limits the overall efficiency. With spin-dependent kinetics in OER, to ...manipulate the spin ordering of ferromagnetic OER catalysts (e.g., by magnetization) can reduce the kinetic barrier. However, most active OER catalysts are not ferromagnetic, which makes the spin manipulation challenging. In this work, we report a strategy with spin pinning effect to make the spins in paramagnetic oxyhydroxides more aligned for higher intrinsic OER activity. The spin pinning effect is established in oxide
FM
/oxyhydroxide interface which is realized by a controlled surface reconstruction of ferromagnetic oxides. Under spin pinning, simple magnetization further increases the spin alignment and thus the OER activity, which validates the spin effect in rate-limiting OER step. The spin polarization in OER highly relies on oxyl radicals (O∙) created by 1
st
dehydrogenation to reduce the barrier for subsequent O-O coupling.
Abstract
The kagome lattice Co
3
Sn
2
S
2
exhibits the quintessential topological phenomena of a magnetic Weyl semimetal such as the chiral anomaly and Fermi-arc surface states. Probing its magnetic ...properties is crucial for understanding this correlated topological state. Here, using spin-polarized scanning tunneling microscopy/spectroscopy (STM/S) and non-contact atomic force microscopy (nc-AFM) combined with first-principle calculations, we report the discovery of localized spin-orbit polarons (SOPs) with three-fold rotation symmetry nucleated around single S-vacancies in Co
3
Sn
2
S
2.
The SOPs carry a magnetic moment and a large diamagnetic orbital magnetization of a possible topological origin associated relating to the diamagnetic circulating current around the S-vacancy. Appreciable magneto-elastic coupling of the SOP is detected by nc-AFM and STM. Our findings suggest that the SOPs can enhance magnetism and more robust time-reversal-symmetry-breaking topological phenomena. Controlled engineering of the SOPs may pave the way toward practical applications in functional quantum devices.
Braiding Majorana zero modes is essential for fault-tolerant topological quantum computing. Iron-based superconductors with nontrivial band topology have recently emerged as a surprisingly promising ...platform for creating distinct Majorana zero modes in magnetic vortices in a single material and at relatively high temperatures. The magnetic field-induced Abrikosov vortex lattice makes it difficult to braid a set of Majorana zero modes or to study the coupling of a Majorana doublet due to overlapping wave functions. Here we report the observation of the proposed quantum anomalous vortex with integer quantized vortex core states and the Majorana zero mode induced by magnetic Fe adatoms deposited on the surface. We observe its hybridization with a nearby field-induced Majorana vortex in iron-based superconductor FeTe
Se
. We also observe vortex-free Yu-Shiba-Rusinov bound states at the Fe adatoms with a weaker coupling to the substrate, and discover a reversible transition between Yu-Shiba-Rusinov states and Majorana zero mode by manipulating the exchange coupling strength. The dual origin of the Majorana zero modes, from magnetic adatoms and external magnetic field, provides a new single-material platform for studying their interactions and braiding in superconductors bearing topological band structures.
In Weyl semimetals, charge density wave (CDW) order can spontaneously break the chiral symmetry, gap out the Weyl nodes, and drive the material into the axion insulating phase. Investigations have ...however been limited since CDWs are rarely seen in Weyl semimetals. Here, using scanning tunneling microscopy/spectroscopy (STM/S), we report the discovery of a novel unidirectional CDW order on the (001) surface of chiral crystal CoSi - a unique Weyl semimetal with unconventional chiral fermions. The CDW is incommensurate with both lattice momentum and crystalline symmetry directions, and exhibits an intra unit cell π phase shift in the layer stacking direction. The tunneling spectrum shows a particle-hole asymmetric V-shaped energy gap around the Fermi level that modulates spatially with the CDW wave vector. Combined with first-principle calculations, we identify that the CDW is locked to the crystal chirality and is related by a mirror reflection between the two enantiomers of the chiral crystal. Our findings reveal a novel correlated topological quantum state in chiral CoSi crystals and raise the potential for exploring the unprecedented physical behaviors of unconventional chiral fermions.
Superhydrophobic and superhydrophilic properties of chemically-modified graphene have been achieved in larger-area vertically aligned few-layer graphene nanosheets (FLGs), prepared on Si (111) ...substrate by microwave plasma chemical vapor deposition (MPCVD). Furthermore, in order to enhance wettability, silicon wafers with microstructures were fabricated, on which graphene nanosheets were grown and modified by a chemical method to form hydrophilic and hydrophobic structures. A superhydrophilic graphene surface (contact angle 0°) and a superhydrophobic graphene surface (contact angle 152.0°) were obtained. The results indicate that the microstructured silicon enhances the hydrophilic and hydrophobic wettabilities significantly.
To synthesize monodisperse palladium nanoparticles dispersed on reduced graphene oxide (RGO) sheets, we have developed an easy and scalable solvothermal reduction method from an organic solution ...system. The RGO-supported palladium nanoparticles with a diameter of 3.8 nm are synthesized in N-methyl-2-pyrrolidone (NMP) and in the presence of oleylamine and trioctylphosphine, which facilitates simultaneous reduction of graphene oxide and formation of Pd nanocrystals. So-produced Pd/RGO was tested for potential use as electrocatalyst for the electro-oxidation of formic acid. Pd/RGO catalyzes formic acid oxidation very well compared to Pd/Vulcan XC-72 catalyst. This synthesis method is a new way to prepare excellent electrocatalysts, which is of great significance in energy-related catalysis.
We report a systematic study of the etching of MoSs crystals by using XeF2 as a gaseous reactant. By controlling the etching process, monolayer MoS2 with uniform morphology can be obtained. The Raman ...and photoluminescence spectra of the resulting material were similar to those of exfoliated MoS2. Utilizing this strategy, different patterns such as a Hall bar structure and a hexagonal array can be realized. Furthermore, the etching mechanism was studied by introducing graphene as an etching mask. We believe our technique opens an easy and controllable way of etching MoS2, which can be used to fabricate complex nanostructures, such as nanoribbons, quantum dots, and transistor structures. This etching process using XeF2 can also be extended to other interesting two-dimensional crystals.
PDF
