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Abstract Monolayer two-dimensional (2D) materials possess excellent in-plane mechanical strength yet extremely low bending stiffness, making them particularly susceptible to instability, which is anticipated to have a substantial impact on their physical functionalities such as 2D-based Micro/Nanoelectromechanical systems (M/NEMS), nanochannels, and proton transport membrane. In this work, we achieve quantitatively tuning instability in suspended 2D materials including monolayer graphene and MoS2 by employing a push-to-shear strategy. We comprehensively examine the dynamic wrinkling-splitting-smoothing process and find that monolayer 2D materials experience stepwise instabilities along with different recovery processes. These stepwise instabilities are governed by the materials’ geometry, pretension, and the elastic nonlinearity. We attribute the different instability and recovery paths to the local stress redistribution in monolayer 2D materials. The tunable instability behavior of suspended monolayer 2D materials not only allows measuring their bending stiffness but also opens up new opportunities for programming the nanoscale instability pattern and even physical properties of atomically thin films.

Abstract Nanofluidics holds significant potential across diverse fields, including energy, environment, and biotechnology. Nevertheless, the fundamental driving mechanisms on the nanoscale remain elusive, underscoring the crucial importance of exploring nanoscale driving techniques. This study introduces a Laplace pressure‐driven flow method that is accurately controlled and does not interfere with interfacial dynamics. Here, we first confirmed the applicability of the Young–Laplace equation for droplet radii ranging from 1 to 10 nm. Following that, a steady‐state liquid flow within the carbon nanotube was attained in molecular dynamics simulations. This flow was driven by the Laplace pressure difference across the nanochannel, which originated from two liquid droplets of unequal sizes positioned at the channel ends, respectively. Furthermore, we employ the Sampson formula to rectify the end effect, ultimately deriving a theoretical model to quantify the flow rate, which satisfactorily describes the molecular dynamics simulation results. This research enhances our understanding on the driving mechanisms of nanoflows, providing valuable insights for further exploration in fluid dynamics on the nanoscale.

Abstract Gas permeation through nanopores is a long-standing research interest because of its importance in fundamental science and many technologies. The free molecular flow is conventionally described by Knudsen theory, under the diffuse reflection assumption. Recent experiments reported ballistic molecular transport of gases, which urges for the development of theoretical tools to address the predominant specular reflections on atomically smooth surfaces. Here we develop a generalized Knudsen theory, which is applicable to various boundary conditions covering from the extreme specular reflection to the complete diffuse reflection. Our model overcomes the limitation of Smoluchowski model, which predicts the gas flow rate diverging to infinity for specular reflection. It emphasizes that the specular reflection can reduce the dissipation flow rate. Our model is validated using molecular dynamics simulations in various scenarios. The proposed model provides insights into the gas transport under confinement and extends Knudsen theory to free molecular flow with specular reflections.

Utilizing the Marangoni effect, miniaturized machineries can be endowed with self-propulsion. Here, the authors report high-performance Marangoni hydrogel rotors with asymmetric porosity and drag reduction profile and demonstrate multiple potential functionalities.

Noncovalent interfaces play a vital role in inelastic deformation and toughening mechanisms in layered nanocomposites due to their dynamical recoverability. When interfacial engineering is applied to design layered nanocomposites, shear-lag analysis is usually implemented to evaluate the capability of interfacial loading transfer. Here, we introduce a multiscale shear-lag model that correlates macroscale mechanical properties with the molecular mechanisms to quantify the effects of interfacial configuration in graphene oxide (GO) layered nanocomposites. By investigating the mechanical responses of commensurate and incommensurate interfaces, we identify that the commensurate interface exhibits a pronounced size effect due to the nucleation and propagation of interfacial defects, whereas the incommensurate interface displays uniform deformation. Our predictions are further validated through large-scale molecular dynamics simulations for GO layered nanocomposites. This work demonstrates how size effects and interfacial configurations can be exploited to fabricate layered nanocomposites with superior mechanical properties despite relying on weak noncovalent interfaces.

Abstract Neutral zinc‐air batteries (ZABs) are promising candidates for the next‐generation power devices with considerably elongated lifetime comparing to conventional alkaline ZABs. However, neutral cathodic oxygen reduction reaction (ORR) is seriously limited by the mass transfer efficiency of hydroxyl due to insufficient interfacial chemical potential‐gradient between catalytic layer and electrolyte. Herein, we highlight that electrochemical oxidation‐induced surface microenvironment optimization could realize optimal chemical potential‐gradient around catalytic sites and bring outstanding neutral ORR activity. The electrodeposited sub‐nano Pt decorated surface‐microenvironment‐optimized Co2N samples (denoted as Pt‐SMO‐Co2N NWs) possessed 92 and 338 mV higher half‐wave potential than commercial Pt/C and pristine Co2N in 0.2 M PBS. As for neutral ZABs, Pt‐SMO‐Co2N NWs cathode delivers a power density of 67.9 mW*cm−2 and displays negligible decay after nearly 80 h stability test at 20 mA*cm−2. In‐depth characterization proposes that remarkable performance improvement originates from optimized microenvironment, which increases the surface chemical potential gradient and facilitates proton coupled electron transfer during ORR. We anticipated that such synergetic optimization of microenvironment and intrinsic activity of active sites is an effective strategy which may be extended to the catalytic reactions beyond ORR. Key points We demonstrated surface microenvironment optimization via in‐situ electrochemical oxidation as an effective way to design highly active ORR catalysts. Surface microenvironment optimization realized significantly enhanced ORR and Zn‐air battery performance in neutral media. Based on ideal material platform, the key role of activating H2O and facilitating proton transfer process in ORR catalysis was revealed.

The porous characteristics of disordered carbons are critical factors to their performance on hydrogen storage and electrochemical capacitors. Even though the porous information can be estimated indirectly by gas adsorption experiments, it is still hard to directly characterize the porous morphology considering the complex 3D connectivity. To this end, we construct full-atom disordered graphene networks (DGNs) by mimicking the chlorination process of carbide-derived carbons using annealing-MD simulations, which could model the structure of disordered carbons at the atomic scale. The porous characteristics, including pore volume, pore size distribution (PSD), and specific surface area (SSA), were then computed from the coordinates of carbon atoms. From the evolution of structural features, pores grow dramatically during the formation of polyaromatic fragments and sequent disordered framework. Then structure is further graphitized while the PSD shows little change. For the obtained DGNs, the porosity, pore size, and SSA increase with decreasing density. Furthermore, SSA tends to saturate in the low-density range. The DGNs annealed at low temperatures exhibit larger SSA than high-temperature DGNs because of the abundant free edges.

Micro-ejecta, an instability growth process, occurs at metal/vacuum or metal/gas interface when compressed shock wave releases from the free surface that contains surface defects. We present molecular dynamics (MD) simulations to investigate the ejecta production from tin surface shocked by supported and unsupported waves with pressures ranging from 8.5 to 60.8 GPa. It is found that the loading waveforms have little effect on spike velocity while remarkably affect the bubble velocity. The bubble velocity of unsupported shock loading remains nonzero constant value at late time as observed in experiments. Besides, the time evolution of ejected mass in the simulations is compared with the recently developed ejecta source model, indicating the suppressed ejection of unmelted or partial melted materials. Moreover, different reference positions are chosen to characterize the amount of ejecta under different loading waveforms. Compared with supported shock case, the ejected mass of unsupported shock case saturates at lower pressure. Through the analysis on unloading path, we find that the temperature of tin sample increases quickly from tensile stress state to zero pressure state, resulting in the melting of bulk tin under decaying shock. Thus, the unsupported wave loading exhibits a lower threshold pressure causing the solid-liquid phase transition on shock release than the supported shock loading.

Understanding the flow characteristics of shale gas especially in nanopores is extremely important for the exploitation. Here, we perform molecular dynamics (MD) simulations to investigate the hydrodynamics of methane in nanometre-sized slit pores. Using equilibrium molecular dynamics (EMD), the static properties including density distribution and self-diffusion coefficient of the confined methane are firstly analyzed. For a 6 nm slit pore, it is found that methane molecules in the adsorbed layer diffuse more slowly than those in the bulk. Using nonequilibrium molecular dynamics (NEMD), the pressure-driven flow behavior of methane in nanopores is investigated. The results show that velocity profiles manifest an obvious dependence on the pore width and they translate from parabolic flow to plug flow when the width is decreased. In relatively large pores (6 – 10 nm), the parabolic flow can be described by the Navier-Stokes (NS) equation with appropriate boundary conditions because of its slip flow characteristic. Based on this equation, corresponding parameters such as viscosity and slip length are determined. Whereas, in small pores (∼ 2 nm), the velocity profile in the center exhibits a uniform tendency (plug flow) and that near the wall displays a linear increase due to the enhanced mechanism of surface diffusion. Furthermore, the profile is analyzed and fitted by a piecewise function. Under this condition, surface diffusion is found to be the root of this anomalous flow characteristic, which can be negligible in large pores. The essential tendency of our simulation results may be significant for revealing flow mechanisms at nanoscale and estimating the production accurately.

Interactions at the oil/brine/rock interfaces play a pivotal role in the mobility of crude oil within reservoir matrices. Unraveling the microscopic mechanisms of these interactions is crucial for ion-engineered water flooding in secondary and tertiary oil recovery. In this study, the occurrence and transport behavior of crude oil in kaolinite nanopores covered with thin brine films was investigated by molecular dynamics simulation. There is an apparent interface layered phenomenon for the liquid molecules in slit pores and the polar oil components primarily concentrate at the oil/brine interfacial region and form various binding connections with ions. The interfacial interactions between the polar oil components and brine ions exhibit an inhibitory effect on the transport of crude oil through nanopores. The interaction mechanism between acetic acid molecules and hydrated ions was elucidated by interaction modes and interaction intensity, which was proved to illustrate the flow difference in different brine film systems. Moreover, a strategy of exchanging the binding sites of divalent cations with acetic acid molecules by monovalent cations with a higher concentration was proposed. The cation exchange scheme was further validated, demonstrating an enhancement in the oil mobility within nanopores. These findings deepen our understanding of oil/brine/rock interfacial interactions and provide a significant molecular perspective on ion-engineered water flooding for enhanced oil recovery. [ABSTRACT FROM AUTHOR]

When water is constrained between two sheets of graphene, it becomes an intriguing monolayer solid with a square pattern due to the ultrahigh van der Waals pressure. However, the square ice phase has become a matter of debate due to the insufficient experimental interpretation and the slightly rhomboidal feature in simulated monolayer square-like structures. Here, we performed classical molecular dynamics simulations to reveal monolayer square ice in graphene nanocapillaries from the perspective of structure and dynamic characteristics. Monolayer square-like ice (instantaneous snapshot), assembled square-rhombic units with stacking faults, is a long-range ordered structure, in which the square and rhombic units are assembled in an order of alternative distribution, and the other rhombic unit forms stacking faults (polarized water chains). Spontaneous flipping of water molecules in monolayer square-like ice is intrinsic and induces transformations among different elementary units, resulting in the structural evolution of monolayer square ice in dynamics. The existence of stacking faults should be attributed to the spontaneous flipping behavior of water molecules under ambient temperature. Statistical averaging results (thermal average positions) demonstrate the inherent square characteristic of monolayer square ice. The simulated data and insight obtained here might be significant for understanding the topological structure and dynamic behavior of monolayer square ice. [ABSTRACT FROM AUTHOR]

The effects of grain boundary (GB) on the mechanical transverse wave propagation in graphene are studied via molecular dynamics simulations and frequency spectrum analysis. We reveal that GB can attenuate transverse waves at terahertz frequencies in graphene, which might be significant for manipulating terahertz noises via nanostructured modifications in graphene-based nanodevices. Two fundamental mechanisms, scattering and resonance, are found in the attenuation of terahertz waves. The scattering impairs waves slightly with a wide range of effective frequencies, whereas the resonance, occurring in the vicinity of GB, significantly reduces the amplitude responses near resonance frequencies, which displays a special frequency-selective filter-like behavior. Moreover, the strong correlation between amplitude loss and buckling height further demonstrates the effects of GB on terahertz mechanical waves in graphene with different chiralities and misorientation angles. [ABSTRACT FROM AUTHOR]

The freezing and melting of low-dimensional materials, either via a first-order phase transition or without any discontinuity in thermodynamic, still remain a matter of debate. Melting (superheating) in two-dimensional (2D) ice is fundamentally different from that in bulk counterpart. Here, we perform comprehensive molecular dynamics simulations of the superheating of monolayer ice in graphene nanocapillaries to understand the nature of melting transition in 2D water/ice. We find four different superheating (melting) scenarios can happen in the superheating of monolayer square-like ice, which are closely related to the lateral pressure and the channel width. The anomalous two-stage melting transition with arisen coexistence phase is found, which reveals the unknown extraordinary characteristics of melting in 2D water/ice. Under ultrahigh lateral pressure, the intermediate monolayer triangular amorphous ice will be formed during the superheating of monolayer square-like ice with both continuous-like and first-order phase transitions. Whereas, under low lateral pressure, the melting in monolayer square-like ice manifests typical discontinuity with notable hysteresis-loop in potential energy during the heating/cooling process. Moreover, we also find that highly puckered monolayer square-like ice can transform into bilayer AB-stacked amorphous ice with square pattern in the superheating process. The superheating behavior under high lateral pressure can be partly regarded as the compression limit of superheated monolayer water. The intrinsic phenomena in our simulated superheating of monolayer ice may be significant for understanding the melting behavior in 2D water/ice. [ABSTRACT FROM AUTHOR]

Materials containing heterogeneous nanostructures hold great promise for achieving superior mechanical properties. However, the strengthening effect due to plastically inhomogeneous deformation in heterogeneous nanostructures has not been clearly understood. Here, we investigate a prototypical heterogeneous nanostructured material of gradient nanotwinned (GNT) Cu to unravel the origin of its extra strength arising from gradient nanotwin structures relative to uniform nanotwin counterparts. We measure the back and effective stresses of GNT Cu with different nanotwin thickness gradients and compare them with those of homogeneous nanotwinned Cu with different uniform nanotwin thicknesses. We find that the extra strength of GNT Cu is caused predominantly by the extra back stress resulting from nanotwin thickness gradient, while the effective stress is almost independent of the gradient structures. The combined experiment and strain gradient plasticity modeling show that an increasing structural gradient in GNT Cu produces an increasing plastic strain gradient, thereby raising the extra back stress. The plastic strain gradient is accommodated by the accumulation of geometrically necessary dislocations inside an unusual type of heterogeneous dislocation structure in the form of bundles of concentrated dislocations. Such a heterogeneous dislocation structure produces microscale internal stresses leading to the extra back stress in GNT Cu. Altogether, this work establishes a fundamental connection between the gradient structure and extra strength in GNT Cu through the mechanistic linkages of plastic strain gradient, heterogeneous dislocation structure, microscale internal stress, and extra back stress. Broadly, this work exemplifies a general approach to unraveling the strengthening mechanisms in heterogeneous nanostructured materials. [ABSTRACT FROM AUTHOR]

Pt-based alloy catalysts may promise considerable mass activity (MA) for oxygen reduction but are generally unsustainable over long-term cycles, particularly in practical proton exchange membrane fuel cells (PEMFCs). Herein, we report a series of Pt-based intermetallic compounds (Pt3Co, PtCo, and Pt3Ti) enclosed by ultrathin Pt skin with an average particle size down to about 2.3 nm, which deliver outstanding cyclic MA and durability for oxygen reduction. By breaking size limitation during ordered atomic transformation in Pt alloy systems, the MA and durability of subsize Pt-based intermetallic compounds can be simultaneously optimized. The subsize scale was also found to enhance the stability of the membrane electrode through preventing the poisoning of catalysts by ionomers in humid fuel-cell conditions. We anticipate that subsize Pt-based intermetallic compounds set a good example for the rational design of high-performance oxygen reduction electrocatalysts for PEMFCs. Furthermore, the prevention of ionomer poisoning was identified as the critical parameter for assembling robust commercial membrane electrodes in PEMFCs. [ABSTRACT FROM AUTHOR]

In this paper, we use a single nanoparticle (NP) to achieve active control of the droplet contact line. When the droplet is out of equilibrium, the resulting excess free energy provides the driving force for the depinning of the contact line and the NP. There are three ways to increase the energy barriers to be surmounted and to realize the pinning of the contact line, namely, the enhancement of the interactions between the NP and the substrate, the increase in substrate hydrophilicity, and the reduction in the NP hydrophilicity. On this basis, we obtained three styles of contact line motion including complete slipping, alternate pinning-depinning, and complete pinning and theoretically interpreted them. The basic theory presented in this paper can be applied to explain and regulate the dynamics of the contact line involved in many physical processes such as evaporation and spreading. [ABSTRACT FROM AUTHOR]

We use molecular dynamics method to study the strengthening effect of graphene-metal nanolayered composites under shock loading. The graphene interfaces have the advantages of both strong and weak interfacial features simultaneously, which solves a strengthening paradox of interfacial structures. On one hand, the weak bending stiffness of graphene leads to interlayer reflections and weakening the shock wave. On the other hand, the strong in-plane sp2-bonded structures constrain the dislocations and heal the material. The elastic recovery due to graphene interfacial constraints plays an important role in the strengthening effect, and the shock strength can be enhanced by decreasing the interlayer distance. This interface with strong/weak duality should lead to an improved fundamental understanding on the dynamic mechanism of composites with interfacial structures. [ABSTRACT FROM AUTHOR]

Using molecular dynamics (MD) simulations, we investigate the elastic–plastic mechanical performances of monolayer graphene oxide (GO) under uniaxial tension. The brittle–ductile–brittle transition and nonlinear–linear–nonlinear elastic transition is found in the uniaxial tension of GO, which displays strong correlations to the content, distribution and proportion of oxygen functional groups. In principle, the tensile behavior of graphene with epoxy groups exhibits ductile fracture features due to the unique epoxy-to-ether transformation in structural evolution. Our simulation results also reveal that wrinkling could cause a competing mechanism of strain-hardening or -softening, and in turn, the nonlinear–linear elasticity transition. Moreover, we propose a continuum mechanical model with a modified stress–strain relation to understand the unique deformation performances, which is consistent with the MD results. These findings might provide valuable insight and design guidelines for optimizing the specific mechanical properties and deformation behaviors of graphene and its derivatives. [ABSTRACT FROM AUTHOR]

The mutual transformations among the four typical divacancy defects induced by a high-energy pulse were studied via molecular dynamics simulation. Our study revealed all six possible mutual transformations and found that defects transformed by absorbing energy to overcome the energy barrier with bonding, debonding, and bond rotations. The reversibility of defect transformations was also investigated by potential energy analysis. The energy difference was found to greatly influence the transformation reversibility. The direct transformation path was irreversible if the energy difference was too large. We also studied the correlation between the transformation probability and the input energy. It was found that the transformation probability had a local maxima at an optimal input energy. The introduction of defects and their structural evolutions are important for tailoring the exceptional properties and thereby performances of graphene-based devices, such as nanoporous membranes for the filtration and desalination of water. [ABSTRACT FROM AUTHOR]

In this work, we studied the effect of the curvature ratio, which is defined as the ratio of the local substrate radii to droplet radii, on the spontaneous directed movement and stagnation of a droplet on a conical substrate. The stagnation phenomenon emerged when the ratio exceeded a critical value. We found that the moving process of the droplet from the tip to the base of the conical substrate can be divided into three stages based on the critical curvature ratio. In order, these comprise: the fast-moving stage (S1) where the droplet obtains large driving force and resistance force, which are resulted from large contact line and contact angle difference between the two opposite sides of the droplet, respectively; the short transition stage (S2) where the droplet morphology tends to be symmetry, both driving force and resistance force decrease rapidly to a low level; and the stagnation stage (S3) where the curvature ratio is much larger than the critical value. Both driving force and resistance force approach zero, the droplet stagnates at the local substrate instead of moving forward. The curvature ratio based theoretical analyses of free energy, driving force and resistance force are in good consistence with simulation results, and can well describe the moving process and the stagnation phenomenon of the droplet on the conical substrate. [ABSTRACT FROM AUTHOR]

We theoretically and numerically investigate the growth of buckling-driven wrinkles in graphene monolayers. It is found that the growth of buckling-driven wrinkles in a graphene monolayer is remarkably chirality- and size-dependent. In small sizes, the flexural response of a graphene sheet cannot be accurately described by the classical Euler regime, and the non-continuum effect leads to zigzag-along-preferred buckling. With the increase of size, the width/length ratio α of the compressed region plays an important role in the growth of buckling-driven wrinkles. When α < 0.5, the oblique buckling happens in armchair-along compression; when 0.5 < α < 1.0, the effect of edge warp leads to zigzag-along-preferred buckling. When 1.0 < α < 3.0, the potential energy density difference due to chiral bending stiffness leads to armchair-along-preferred buckling. When α > 3.0, the non-continuum effect and chiral bending stiffness can both be neglected, and the buckling in a graphene monolayer is isotropic. The chirality-along-preferred transition of compressed buckling in a graphene monolayer leads to an improved fundamental understanding of the dynamics mechanism of graphene-based nanodevices, especially for the nanodevices with high frequency response. [ABSTRACT FROM AUTHOR]

Atomistic simulations were utilized to develop fundamental insights regarding the elongation process starting from ultranarrow graphene nanoribbons (GNRs) and resulting in monatomic carbon chains (MACCs). There are three key findings. First, we demonstrate that complete, elongated, and stable MACCs with fracture strains exceeding 100% can be formed from both ultranarrow armchair and zigzag GNRs. Second, we demonstrate that the deformation processes leading to the MACCs have strong chirality dependence. Specifically, armchair GNRs first form DNA-like chains, then develop into monatomic chains by passing through an intermediate configuration in which monatomic chain sections are separated by two-atom attachments. In contrast, zigzag GNRs form rope-ladder-like chains through a process in which the carbon hexagons are first elongated into rectangles; these rectangles eventually coalesce into monatomic chains through a novel triangle-pentagon deformation structure under further tensile deformation. Finally, we show that the width of GNRs plays an important role in the formation of MACCs, and that the ultranarrow GNRs facilitate the formation of full MACCs. The present work should be of considerable interest due to the experimentally demonstrated feasibility of using narrow GNRs to fabricate novel nanoelectronic components based upon monatomic chains of carbon atoms. [ABSTRACT FROM AUTHOR]

We investigate the underlying mechanism of capillary force balance at the contact line. In particular, we offer a novel approach to describe and quantify the capillary force on the liquid in coexistence with its vapor phase, which is crucial in wetting and spreading dynamics. Its relation with the interface tension is elucidated. The proposed model is verified by our molecular dynamics simulations over a wide contact angle range. Differences in capillary forces are observed in evaporating droplets on homogeneous and decorated surfaces. Our findings not only provide a theoretical insight into capillary forces at the contact line, but also validate Young's equation based on a mechanical interpretation. [ABSTRACT FROM AUTHOR]