arXiv subjects

Sander Ø. Hanslin

Publications and source records attributed to Sander Ø. Hanslin.

3 recordsLinked to original sources

arXiv2024

Doping-Induced Enhancement of Hydrogen Evolution at MoS2 Electrodes

Rate theory and DFT calculations of hydrogen evolution reaction (HER) on MoS2 with Co, Ni and Pt impurities show the significance of dihydrogen (H2*) complex where both hydrogen atoms are interacting with the surface. Stabilization of such a complex affects the competing Volmer-Heyrovsky (direct H2 release) and Volmer-Tafel (H2* intermediate) pathways. The resulting evolution proceeds with a very small overpotential for all dopants ($η$ = 0.1 to 0.2 V) at 25% edge substitution, significantly reduced from the already low $η$ = 0.27 V for the undoped edge. At full edge substitution, Co-MoS2 remains highly active ($η$ = 0.18 V) while Ni- and Pt-MoS2 are deactivated ($η$ = 0.4 to 0.5 V) due to unfavorable interaction with H2*. Instead of the single S-vacancy, the site of intrinsic activity in the basal plane was found to be the undercoordinated central Mo-atom in threefold S-vacancy configurations, enabling hydrogen evolution with $η$ = 0.52 V via a H2* intermediate. The impurity atoms interact favorably with the intrinsic sulfur vacancies on the basal plane, stabilizing but simultaneously deactivating the triple vacancy configuration. The calculated shifts in overpotential are consistent with reported measurements, and the dependence on doping level may explain variations in experimental observations.

cond-mat.mtrl-sci↗

arXiv2023

Is the doped MoS2 basal plane an efficient hydrogen evolution catalyst? Calculations of voltage-dependent activation energy

Transition metal dichalcogenides are cheap and earth-abundant candidates for the replacement of precious metals as catalyst materials. Experimental measurements of the hydrogen evolution reaction (HER), for example, have demonstrated significant electrocatalytic activity of MoS2 but there is large variation depending on preparation method. In order to gain information about the mechanism and active sites for HER, we have carried out calculations of the reaction and activation energy for HER at the transition metal doped basal plane of MoS2 under electrochemical conditions, i.e. including applied electrode potential and solvent effects. The calculations are based on identifying the relevant saddle points on the energy surface obtained from density functional theory within the generalized gradient approximation, and the information on energetics is used to construct voltage-dependent volcano plots. Doping with 3d-metal atoms as well as Pt is found to enhance hydrogen adsorption onto the basal plane by introducing electronic states within the band gap, and in some cases (Co, Ni, Cu, Pt) significant local symmetry breaking. The Volmer-Heyrovsky mechanism is found to be most likely and the associated energetics show considerable dopant and voltage-dependence. While the binding free energy of hydrogen can be tuned to be seemingly favorable for HER, the calculated activation energy turns out to be significant, at least 0.7 eV at a voltage of -0.5 V vs. SHE, indicating low catalytic activity of the doped basal plane. This suggests that other sites are responsible for the experimental activity, possibly edges or basal plane defects.

cond-mat.mtrl-sci↗

arXiv2021

Light-induced Dzyaloshinskii-Moriya interactions in antiferromagnetic metals

The Dzyaloshinskii-Moriya (DM) interaction plays an essential role in novel topological spintronics, and the ability to control this chiral interaction is of key importance. Developing a general microscopic framework to compute nonequilibrium DM interactions, we theoretically show that the ac electric field component of a laser pulse induces nonequilibrium static DM interactions in an antiferromagnetic (AFM) system in the presence of relativistic spin-orbit coupling. These nonequilibrium DM interactions might even be anisotropic depending on the direction of magnetic moments and the laser pulse polarization. We further show that intense polarized laser pulses can in principle generate both classes of DM interactions, i.e., bulk-type and interfacial-type, in a magnetic system even though the crystal symmetry prohibits one of them in equilibrium. Our results reveal another aspect of rich behavior of periodically driven spin systems and the far-from-equilibrium magnetic systems.

cond-mat.mes-hall↗