In situ studies of the relationship between surface spin configurations and spin-related electrocatalytic reactions are crucial for understanding how magnetic catalysts enhance oxygen evolution reaction (OER) performance under magnetic fields. In this work, 2D Fe7Se8 nanosheets with rich surface spin configurations are synthesized via chemical vapor deposition. In situ magnetic force microscopy and Raman spectroscopy reveal that a 200 mT magnetic field eliminates spin-disordered domain walls, forming a spin-ordered single-domain structure, which lowers the OER energy barrier, as confirmed by theoretical calculations. Electrochemical tests show that under a 200 mT magnetic field, the OER overpotential of multidomain Fe7Se8 nanosheets at 10 mA cm-2 decreases from 346 mV to 259 mV, while the magnetic field has minimal effect on single-domain nanosheets. These findings highlight the critical role of spin configurations in enhancing electrocatalytic performance, offering new insights into the design of magnetic catalysts for industrial applications.

The surface spin configuration of catalysts is crucial for spin-dependent catalysis, as electrochemical reactions predominantly occur at the solid-liquid interface. This configuration influences reaction efficiency by altering the spin states of intermediates. Thus, identifying the surface spin configuration is essential for understanding the mechanisms affecting catalytic activity. This work designs multidomain and single-domain Fe7S8 nanosheets through thickness control. Under a 200 mT magnetic field, the multidomain sample transitions to a single-domain state, while the surface spin configuration of the single-domain sample remains unchanged, as observed via magnetic force microscopy. Electrochemical tests show that a saturated magnetic field of 200 mT reduces the overpotential of the multidomain sample from 306 to 240 mV at 10 mA cm-2, while the single-domain sample maintains an overpotential of 257 mV. These results demonstrate that spin disorder at magnetic domain walls limits spin selectivity during the OER, suggesting strategies for developing innovative spin-selective catalysts.

The high-frequency alternating magnetic field (AMF) is considered as a fascinating heating treatment that provides a noninvasive solution to enhance the catalytic efficiency of electrocatalyst. However, practical applications of AMF in electrochemistry are primarily concentrated on magnetic mediums. To broaden its application into nonmagnetic catalysts, herein, a practicable method is reported by modifying the working electrode substrate with magnetic Fe3O4 nanoparticles (NPs), which serves as both substrate and self-heating medium by virtue of its rapid and efficient magnetic heating effect associated with N & eacute;el relaxation triggered by external high-frequency AMF, thus boosting the catalyst performance upon it. To verify it, Pt NPs and Pt single atoms (SAs), as two representative non-magnetic catalyst, are selected for trials. The results, reveal that, when AMF is applied, Pt NPs@C/Fe3O4/C and Pt SAs@C/Fe3O4/C display remarkable enhancement of hydrogen evolution reaction magnetocurrent density respectively by approximate to 146% and approximate to 185%, whereas on unmodified bare glassy carbon there both show unnoticeable change in catalytic performance. The developed strategy opens up a vast space for exploiting the energy of a weak, non-invasive magnetic field.

Amorphous materials have been recognized as highly active electrocatalysts due to their abundant active sites stems from unsaturated chemical bonds. In addition, the application of alternating magnetic fields (AMF) to achieve magnetic heating effect has gradually become an important means to improve the performance of magnetic catalysts. Here, we have successfully realized the surfacial amorphization of confined Ni3C nanoparticles by using interfacial strain engineering. As expected, the surfacial amorphized Ni3C nanoparticles exhibit remarkable properties in electrochemical water-splitting. More importantly, magnetic measurements show that the surfacial amorphized Ni3C nanoparticles have room temperature ferromagnetism, which is consistent with our theoretical calculation results. Accordingly, under AMF stimulation, its overall water-splitting performance is further greatly improved as the result of magnetic heating effect associated with Néel relaxation. This work provides a new strategy for the development of highly efficient surfacial amorphized catalysts, and promotes the application of magnetothermal technology in amorphous catalysis.

Confined semiconducting CuSe quantum dots with abundant Se vacancies are synthesized by pulsed laser deposition with in situ vacuum annealing. With the presence of Se vacancies, the photogenerated charge recombination is suppressed by the self-introduced in-gap trapping states, thus enhancing the photoelectrocatalytic activity under solar illumination.

Advanced MaterialsVolume 35, Issue 32 2370227 FrontispieceFree Access Interlayer-Confined NiFe Dual Atoms within MoS2 Electrocatalyst for Ultra-Efficient Acidic Overall Water Splitting (Adv. Mater. 32/2023) Zhenzhen Jiang, Zhenzhen Jiang Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorWenda Zhou, Wenda Zhou School of Materials Science and Engineering, Anhui University, 111 Jiulong Road, Hefei, Anhui, 230601 ChinaSearch for more papers by this authorCe Hu, Ce Hu Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorXingfang Luo, Xingfang Luo Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorWei Zeng, Wei Zeng Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorXunguo Gong, Xunguo Gong Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorYong Yang, Yong Yang Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorTing Yu, Ting Yu Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorWen Lei, Wen Lei Department of Electrical, Electronic and Computer Engineering, The University of Western Australia, 35 Stirling Highway, Crawley, WA, 6009 AustraliaSearch for more papers by this authorCailei Yuan, Cailei Yuan Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this author Zhenzhen Jiang, Zhenzhen Jiang Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorWenda Zhou, Wenda Zhou School of Materials Science and Engineering, Anhui University, 111 Jiulong Road, Hefei, Anhui, 230601 ChinaSearch for more papers by this authorCe Hu, Ce Hu Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorXingfang Luo, Xingfang Luo Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorWei Zeng, Wei Zeng Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorXunguo Gong, Xunguo Gong Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorYong Yang, Yong Yang Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorTing Yu, Ting Yu Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorWen Lei, Wen Lei Department of Electrical, Electronic and Computer Engineering, The University of Western Australia, 35 Stirling Highway, Crawley, WA, 6009 AustraliaSearch for more papers by this authorCailei Yuan, Cailei Yuan Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this author First published: 10 August 2023 https://doi.org/10.1002/adma.202370227AboutPDF ToolsRequest permissionExport citationAdd to favoritesTrack citation ShareShare Give accessShare full text accessShare full-text accessPlease review our Terms and Conditions of Use and check box below to share full-text version of article.I have read and accept the Wiley Online Library Terms and Conditions of UseShareable LinkUse the link below to share a full-text version of this article with your friends and colleagues. Learn more.Copy URL Share a linkShare onEmailFacebookTwitterLinkedInRedditWechat Graphical Abstract Water Splitting In article number 2300505, Cailei Yuan and co-workers report an ingenious approach to assemble Ni and Fe dual atoms into the interlayer of MoS2. The interlayer-confined structure provides a microenvironment highly boosting the catalytic process, and meanwhile a protective “shelter” for active metal atoms away from acid corrosion, agglomeration, and detachment. The interlayer-confined strategy provides a new direction for single-atom catalysts development in the future. Volume35, Issue32August 10, 20232370227 RelatedInformation

Self-doping can not only suppress the photogenerated charge recombination of semiconducting quantum dots by self-introducing trapping states within the bandgap, but also provide high-density catalytic active sites as the consequence of abundant non-saturated bonds associated with the defects. Here, we successfully prepared semiconducting copper selenide (CuSe) confined quantum dots with abundant vacancies and systematically investigated their photoelectrochemical characteristics. Photoluminescence characterizations reveal that the presence of vacancies reduces the emission intensity dramatically, indicating a low recombination rate of photogenerated charge carriers due to the self-introduced trapping states within the bandgap. In addition, the ultra-low charge transfer resistance measured by electrochemical impedance spectroscopy implies the efficient charge transfer of CuSe semiconducting quantum dots-based photoelectrocatalysts, which is guaranteed by the high conductivity of their confined structure as revealed by room-temperature electrical transport measurements. Such high conductivity and low photogenerated charge carriers recombination rate, combined with high-density active sites and confined structure, guaranteeing the remarkable photoelectrocatalytic performance and stability as manifested by photoelectrocatalysis characterizations. This work promotes the development of semiconducting quantum dots-based photoelectrocatalysis and demonstrates CuSe semiconducting quantum confined catalysts as an advanced photoelectrocatalysts for oxygen evolution reaction.

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.

As a prototypical system for studying the Eley-Rideal (ER) mechanism at the gas-surface interface, the reaction between incident H/D atoms and pre-covered D/H atoms on Cu (111) has attracted much experimental and theoretical interest. Detailed final state-resolved experimental data have been available for about thirty-years, leading to the discovery of many interesting dynamical features. However, previous theoretical models have suffered from reduced-dimensional approximations and/or omitting energy transfer to surface phonons and electrons, or the high cost of on-the-fly ab initio molecular dynamics, preventing quantitative comparisons with experimental data. Herein, we report the first high-dimensional neural network potential (NNP) for this ER reaction based on first-principles calculations including all molecular and surface degrees of freedom. Thanks to the high efficiency of this NNP, we are able to perform extensive quasi-classical molecular dynamics simulations with the inclusion of the excitation of low-lying electron-hole pairs (EHPs), which generally yield good agreement with various experimental results. More importantly, the isotopic and/or EHP effects in total reaction cross-sections and distributions of the product energy, scattering angle, and individual ro-vibrational states have been more clearly shown and discussed. This study sheds valuable light on this important ER prototype and opens a new avenue for further investigations of ER reactions using various initial conditions, surface temperatures, and coverages in the future.

SmallVolume 19, Issue 4 2370020 Inside Front CoverFree Access Atomic Magnetic Heating Effect Enhanced Hydrogen Evolution Reaction of Gd@MoS2 Single-Atom Catalysts (Small 4/2023) Wei Zeng, Wei Zeng Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorZhenzhen Jiang, Zhenzhen Jiang Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorXunguo Gong, Xunguo Gong Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorCe Hu, Ce Hu Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorXingfang Luo, Xingfang Luo Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorWen Lei, Wen Lei Department of Electrical, Electronic and Computer Engineering, The University of Western Australia, 35 Stirling Highway, Crawley, 6009 AustraliaSearch for more papers by this authorCailei Yuan, Cailei Yuan Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this author Wei Zeng, Wei Zeng Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorZhenzhen Jiang, Zhenzhen Jiang Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorXunguo Gong, Xunguo Gong Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorCe Hu, Ce Hu Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorXingfang Luo, Xingfang Luo Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this authorWen Lei, Wen Lei Department of Electrical, Electronic and Computer Engineering, The University of Western Australia, 35 Stirling Highway, Crawley, 6009 AustraliaSearch for more papers by this authorCailei Yuan, Cailei Yuan Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, Jiangxi, 330022 ChinaSearch for more papers by this author First published: 26 January 2023 https://doi.org/10.1002/smll.202370020AboutPDF ToolsRequest permissionExport citationAdd to favoritesTrack citation ShareShare Give accessShare full text accessShare full-text accessPlease review our Terms and Conditions of Use and check box below to share full-text version of article.I have read and accept the Wiley Online Library Terms and Conditions of UseShareable LinkUse the link below to share a full-text version of this article with your friends and colleagues. Learn more.Copy URL Share a linkShare onEmailFacebookTwitterLinkedInRedditWechat Graphical Abstract Atomic-Level Magnetic Heating Effect In article number 2206155, Cailei Yuan and co-workers report a single-atom catalyst (Gd@MoS2) with long range room temperature ferromagnetic spin alignment that exhibits significant improvements in catalytic kinetics under alternating magnetic field (AMF) excitation. This increase in catalytic activity is attributed to the atomic-level magnetic heating effect resulting from the spin flip (canting) of the Gd single-atom (catalytically active centers) due to AMF action. It provides a new way to further improve the performance of single-atom catalysts. Volume19, Issue4January 25, 20232370020 RelatedInformation

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.

Introduction of alternating magnetic field (AMF) to electrocatalytic process has been proved an effective strategy for significantly enhancing catalytic performance of magnetic nanoparticles (NPs) electrocatalysts. Coupling AMF with currently highly promising monodispersed NPs electrocatalysts could be an interesting tactics. However, magnetic heating effect under AMF may cause agglomeration and even falloff of NPs, and how to efficiently and stably utilize AMF in monodispersed NPs electrocatalysts to enhance the catalytic performance is an urgent issue. In this work, room-temperature ferromagnetism is introduced into NiSe2_X nanoparticle by vacancy engineering, and proposes a feasible design to confine monodispersed ultra-small NiSe2_X NPs in an amorphous carbon matrix. Under AMF, the spin flips of the magnetic domains in confined NiSe2_X NPs generate magnetic heating related to Neel relaxation, which achieve rapid local heating of NiSe2_X NPs electrocatalyst and greatly improves hydrogen evolution reaction performance (a significantly increase of current density by similar to 400 %). This work provides new ideas for the preparation of ultra-small monodispersed NPs electrocatalysts that can utilize AMF to enhance catalytic performance, and has an important significance in accelerating clean energy production.

Further uprating the catalytic activities of diatomic active sites while maintaining the atomic loading and diatomic coordination by external stimulation is a promising way to break the bottleneck in the improvement of diatomic site catalysts (DASCs). Herein, the as-prepared NiFe@MoS2 DASCs treated by external high-frequency alternating magnetic field (AMF) further expedite the alkaline water electrolysis process with a superior cell voltage of 1.576 V to afford a current density of 10 mA cm−2 than that treated without AMF (1.652 V). Theoretical simulation by COMSOL Multiphysics helps visualize the increase in temperature locally around the diatomic active sites, qualitatively revealing the magnetic heating effect that originates from the anchored magnetic Ni and Fe atoms. The selective magnetic heating of bifunctional diatomic active site proposed in this work can broaden horizons and endow another dimension in the design of highly efficient catalysts toward various complicated energy-related reactions.

We examine energy dissipation of impinging molecules (CO) on Au(111) using molecular dynamics on a machine learned high-dimensional potential energy surface (PES) describing both the molecular and surface degrees of freedom. The PES was trained using a neural network method from density functional theory energies and gradients obtained with a relatively small supercell size, but it is capable of providing an accurate description of the molecule-surface interaction for larger supercells. This property allowed us to investigate the dependence of the dissipation dynamics on the supercell size. Our simulations indicated that the supercell size has essentially no effect on the direct scattered molecules, but the energy dissipation of the trapping molecules is significantly influenced by the size of the simulation cell. This observation has important implications in understanding dissipation at the gas-surface interface and their effects on various dynamics processes.

Although (oxy)hydroxides generated by electrochemical reconstruction (EC-reconstruction) of transition-metal catalysts exhibit highly catalytic activities, the amorphous nature fundamentally impedes the electrochemical kinetics due to its poor electrical conductivity. Here, EC-reconstructed NiFe/NiFeOOH core/shell nanoparticles in highly conductive carbon matrix based on the pulsed laser deposition prepared NiFe nanoparticles is successfully confined. Electrochemical characterizations and first-principles calculations demonstrate that the reconstructed NiFe/NiFeOOH core/shell nanoparticles exhibit high oxygen evolution reaction (OER) electrocatalytic activity (a low overpotential of 342.2 mV for 10 mA cm-2 ) and remarkable durability due to the efficient charge transfer in the highly conductive confined heterostructure. More importantly, benefit from the superparamagnetic nature of the reconstructed NiFe/NiFeOOH core/shell nanoparticles, a large OER improvement is achieved (an ultralow overpotential of 209.2 mV for 10 mA cm-2 ) with an alternating magnetic field stimulation. Such OER improvement can be attributed to the Néel relaxation related magnetic heating effect functionalized superparamagnetic NiFe cores, which are generally underutilized in reconstructed core/shell nanoparticles. This work demonstrates that the designed superparamagnetic core/shell nanoparticles, combined with the large improvement by magnetic heating effect, are expected to be highly efficient OER catalysts along with the confined structure guaranteed high conductivity and catalytic stability.

Energy transfer during molecular collisions at a metal surface represents a sensitive probe of the molecule-surface interaction potential. Here, via molecular dynamics calculations on several first-principles neural network potentials, we find that the vibrational energy transfer dynamics of highly vibrationally excited NO and CO molecules scattered from Au(111) are strongly correlated with their respective potential energy landscapes in the vicinity of the dissociation barrier. Our results not only reproduce the observed significantly less vibrational relaxation of CO (v(i) = 17) than NO (v(i)= 16) scattered from Au(111) and attribute it to the different dissociation barriers in the two systems, but also show a dramatic change of dynamics due to a minor adjustment of the energy landscape near the barrier in the CO case. We find that the BEEF-vdW density functional based potential largely overestimates the vibrational relaxation of CO (v(i)= 17) even in the absence of any nonadiabatic energy loss, despite its good description for CO adsorption on Au(111). We also discuss the possibility of integrating the validated adiabatic potential with first-principles determined diabatic states towards a more complete description of the non-adiabatic energy transfer in these benchmark systems.

Among the numerous two-dimensional van der Waals (vdW) magnetic materials, Fe3GeTe2 (FGT), due to its outstanding properties such as metallicity, high Curie temperature and strong perpendicular magnetic anisotropy, has quickly emerged as a candidate with the most potential for the fabrication of all-vdW spintronic devices. Here, we fabricated a simple vertical homojunction based on two few-layer exfoliated FGT flakes. Under a certain range of external magnetic fields, the magnetization reversal can be achieved by applying a negative or positive pulse current, which can reduce the coercivity through the spin orbit torque of FGT itself in addition to the Joule heat. Moreover, the asymmetrical switching current is caused by the spin transfer torque in the homojunction. As the temperature increases, the magnetization reversal can be observed at a smaller external magnetic field. Our demonstrations of the current-assisted magnetization reversal under a magnetic field in all-vdW structures may provide support for the potential application of vdW magnetism.

Localized magnetic heating in magnetic nanoparticles caused by an alternating magnetic field (AMF) can facilitate electrocatalytic reactions, which has become an emerging strategy to further enhance overall efficiency of catalysts and frontier in an electrocatalysis field. However, the investigation of AMF-assisted electrocatalysis is still in its infancy, and how to efficiently utilize magnetic heating in magnetic nanoparticles to boost electrocatalysis reactions is in great demand. In this work, a feasible design is proposed by using Néel relaxation, efficient local heating generated in superparamagnetic CoSe2 nanoparticles confined in an amorphous carbon matrix by AMF leading to improved catalytic performance. The rapid oxygen evolution reaction enhancement of CoSe2 nanoparticles responses to switched on/off AMF, indicating that the localized magnetic heating is generated in catalysts by Néel relaxation with magnetic moments of nanoparticles rapidly flipping under AMF. Our work inspires insight to design AMF-assisted electrocatalysts and inject power into the field of electrocatalysis.

We examine energy dissipation of impinging molecules (CO) on Au(111) using molecular dynamics on a machine learned high-dimensional potential energy surface (PES) describing both the molecular and surface degrees of freedom. The PES was trained using a neural network method from density functional theory energies and gradients obtained with a relatively small supercell size, but it is capable of providing an accurate description of the molecule-surface interaction for larger supercells. This property allowed us to investigate the dependence of the dissipation dynamics on the supercell size. Our simulations indicated that the supercell size has essentially no effect on the direct scattered molecules, but the energy dissipation of the trapping molecules is significantly influenced by the size of the simulation cell. This observation has important implications in understanding dissipation at the gas-surface interface and their effects on various dynamics processes.