Dual-active-site strategies are widely adopted to address the intrinsic challenge of simultaneously promoting water dissociation and maintaining an optimal hydrogen adsorption free energy in alkaline hydrogen evolution. However, this paradigm implicitly presumes rapid equilibration of hydrogen intermediates (H*), thereby neglecting H* transport as a fundamental kinetic bottleneck. Here, we show that rational regulation of interfacial hydrogen-spillover pathways offers an effective kinetic lever for modulating alkaline hydrogen evolution. An atomically coupled Pt-Co₃O₄ heterostructure, featuring Pt nanoparticles anchored on Co₃O₄ nanowire arrays, is constructed as a model system. We reveal that interfacial electron transfer generates a built-in electric field, which can be effectively tuned via oxygen-vacancy-mediated modulation of the work function difference, thereby enabling controllable regulation of interfacial H* migration. This field drives a reverse hydrogen spillover process and lowers the H* migration barrier to 0.13 eV, transforming the heterointerface into a high-efficiency H* transport channel. Enabled by this field-regulated reaction pathway, the catalyst delivers an overpotential of 18.7 mV at 10 mA·cm^–2 and a Tafel slope of 27.8 mV·dec^–1 in 1.0 M KOH. The practical relevance is validated by alkaline seawater electrolysis, delivering 1.0 A·cm^–2 at 1.76 V and maintaining stable performance for over 500 h. This research clarifies the electronic origin of accelerated reverse hydrogen spillover and offers a universal design paradigm for high-performance multi-step electrocatalysis.

Non-layered two-dimensional materials (NL2DMs) have emerged as a promising complement to layered 2D materials, offering unique properties derived from their isotropic bonding and structural diversity. However, their synthesis is still facing significant challenges due to the lack of intrinsic anisotropic growth driving force. This review comprehensively outlines strategies for chemical vapor deposition (CVD)-based synthesis of NL2DMs, demonstrating how integrated thermodynamic and kinetic control enables precise thickness and morphology modulation. We also analyze the existing challenges and propose future research directions. This systematic framework paves the way for engineering NL2DMs growth with customized functionalities for next-generation optoelectronics, energy storage, and catalysis.

In supported catalysts, strong metal–support interaction (SMSI) is pivotal for modulating catalytic performance. Challenges, such as active site shielding and insufficient interfacial reactivity, have emerged as key points of attention. Here, we propose an amorphous encapsulation strategy creating permeable overlayers that preserve metal accessibility while maximizing metal–support interfaces. The engineered Pt@a-Nb₂O₅ catalyst is synthesized through a two-step process involving the heat treatment of the Nb₂O₅ support followed by wet chemical reduction. This catalyst exhibits exceptional CO oxidation performance, achieving complete CO conversion at 165 °C and demonstrating remarkable stability for over 30 h at 205 °C. The amorphous Nb₂O₅ shell, rich in oxygen vacancies, modulates the electronic structure of Pt, creating dual adsorption sites for CO and O₂ and significantly improving catalytic activity. The catalyst design, which features an amorphous-coated heterostructure, along with the amorphous encapsulation preparation method, is expected to be applicable to a wider variety of supported catalyst systems and catalytic reactions.

The heterostructure of transition metal nanocrystal on two-dimensional (2D) materials exhibits unique physical and chemical properties through various interfacial interactions. It has been established that the atomic structure and strain in the vicinity of the interface determine the band structure and phonon modes of the nanocrystal, regulating the optical and electrical properties of such heterostructures. Hence, metal–support interfacial engineering is a demonstrated approach to acquiring desired properties of the nanocrystals. However, a fundamental understanding of the interfacial structures remains elusive and precise control of the interactions has yet achieved. Herein, we explore the regulation of interface on MoS₂ supported Pt nanocrystals which were prepared by reducing ultrasonic dispersed potassium chloroplatinate. The Pt-MoS₂ heterostructure interface was systematically studied by aberration corrected transmission electron microscopy. Three types of Pt-MoS₂ interfaces with distinct atomic configurations were identified. The strain within the Pt nanocrystals is sensitive to the atomic configuration of the supporting MoS₂, which regulates the size of the Pt nanocrystals. These results provide insights on tuning of nanocrystal strain, paving the way for precise control of 2D semiconductor heterostructures.

Formic acid oxidation (FAO) is a typical anode reaction in fuel cells that can be facilitated by modulating its direct and indirect reaction pathways. Herein, PtAu bimetallic nanoparticles loaded onto Co and N co-doping carbon nanoframes (CoNC NFs) were designed to improve the selectivity of the direct reaction pathway for efficient FAO. Based on these subtle nanomaterials, the influences of elemental composition and carbon-support materials on the two pathways of FAO were investigated in detail. The results of fuel cell tests verified that the appropriate amount of Au in PtAu/CoNC can promote a direct reaction pathway for FAO, which is crucial for enhancing the oxidation efficiency of formic acid. In particular, the obtained PtAu/CoNC with an optimal Pt/Au atomic ratio of 1:1 (PtAu/CoNC-3) manifests the best catalytic performance among the analogous obtained Pt-based electrocatalysts. The FAO mass activity of the PtAu/CoNC-3 sample reached 0.88 A·mg_Pt⁻¹, which is 26.0 times higher than that of Pt/C. The results of first-principles calculation and CO stripping jointly demonstrate that the CO adsorption of PtAu/CoNC is considerably lower than that of Pt/CoNC and PtAu/C, which indicates that the synergistic effect of Pt, Au, and CoNC NFs is critical for the resistance of Pt to CO poisoning. This work is of great significance for a deeper understanding of the oxidation mechanism of formic acid and provides a feasible and promising strategy for enhancing the catalytic performance of the catalyst by improving the direct reaction pathway for FAO.

Two-dimensional (2D) MoS₂ with appealing physical properties is a promising candidate for next-generation electronic and optoelectronic devices, where the ultrathin MoS₂ is usually laid on or gated by a dielectric oxide layer. The oxide/MoS₂ interfaces widely existing in these devices have significant impacts on the carrier transport of the MoS₂ channel by diverse interface interactions. Artificial design of the oxide/MoS₂ interfaces would provide an effective way to break through the performance limit of the 2D devices but has yet been well explored. Here, we report a high-performance MoS₂-based phototransistor with an enhanced photoresponse by interfacing few-layer MoS₂ with an ultrathin TiO₂ layer. The TiO₂ is deposited on MoS₂ through the oxidation of an e-beam-evaporated ultrathin Ti layer. Upon a visible-light illumination, the fabricated TiO₂/MoS₂ phototransistor exhibits a responsivity of up to 2,199 A/W at a gate voltage of 60 V and a detectivity of up to 1.67 × 10¹³ Jones at a zero-gate voltage under a power density of 23.2 μW/mm². These values are 4.0 and 4.2 times those of the pure MoS₂ phototransistor. The significantly enhanced photoresponse of TiO₂/MoS₂ device can be attributed to both interface charge transfer and photogating effects. Our results not only provide valuable insights into the interactions at TiO₂/MoS₂ interface, but also may inspire new approach to develop other novel optoelectronic devices based on 2D layered materials.

Surface engineering is known as an effective strategy to enhance the catalytic properties of Pt-based nanomaterials. Herein, we report on surface engineering Ni-Pt nanoalloys with a facile method by varying the Ni doping concentration and oleylamine/oleic- acid surfactant-mix. The alloy-composition, exposed facet condition, and surface lattice strain are, thereby manipulated to optimize the catalytic efficiency of such nanoalloys for methanol oxidation reaction (MOR). Exemplary nanoalloys including Ni_0.69Pt_0.31 truncated octahedrons, Ni_0.45Pt_0.55 nanomultipods and Ni_0.20Pt_0.80 nanoflowers are thoroughly characterized, with a commercial Pt/C catalyst as a common benchmark. Their variations in MOR catalytic efficiency are significant: 2.2 A/mg_Pt for Ni_0.20Pt_0.80 nanoflowers, 1.2 A/mg_Pt for Ni_0.45Pt_0.55 nanomultipods, 0.7 A/mg_Pt for Ni_0.69Pt_0.31 truncated octahedrons, and 0.6 A/mg_Pt for the commercial Pt/C catalysts. Assisted by density functional theory calculations, we correlate these observed catalysis-variations particularly to the intriguing presence of surface interplanar-strains, such as {111} facets with an interplanar-tensile-strain of 2.6% and {200} facets with an interplanar-tensile-strain of 3.5%, on the Ni_0.20Pt_0.80 nanoflowers.

The morphology and structural stability of metal/2D semiconductor interfaces strongly affect the performance of 2D electronic devices and synergistic catalysis. However, the structural evolution at the interfaces has not been well explored particularly at atomic resolution. In this work, we study the structural evolution of Au nanoparticles (NPs) on few-layer MoS₂ by high resolution transmission electron microscopy (HRTEM) and quantitative high-angle annular dark field scanning TEM. It is found that in the transition of Au from nanoparticles to dendrites, a dynamically epitaxial alignment between Au and MoS₂ lattices is formed, and Moiré patterns can be directly observed in HRTEM images due to the mismatch between Au and MoS₂ lattices. This epitaxial alignment can occur in ambient conditions, and can also be accelerated by the irradiation of high-energy electron beam. In situ observation clearly reveals the rotation of Au NPs, the atom migration inside Au NPs, and the transfer of Au atoms between neighboring Au NPs, finally leading to the formation of epitaxially aligned Au dendrites on MoS₂. The structural evolution of metal/2D semiconductor interfaces at atomic scale can provide valuable information for the design and fabrication of the metal/2D semiconductor nano-devices with desired physical and chemical performances.

A simple yet general one-step solvothermal method is applied to synthesize sub-7 nm monodispersed single-crystal NiPt₂ nanoparticles (NPs) with the morphology of truncated octahedrons in the alloying state of disordered atomic arrangements. The effective magnetic moments of these NPs exhibit an anomalous temperature dependency, increasing from approximately 0.9 μ_B/atom at 15 K to 1.9 μ_B/atom at 300 K. This is an increase by a factor of more than three compared with bulk Ni. On the basis of experiments involving X-ray absorption near-edge spectroscopy of the L3 edge for Pt and density functional theory calculations, the observed novel magnetism enhancement and its anomalous temperature dependence are attributed to the electron transfer arising from the thermal-activation effects.