Generative Artificial Intelligence for Designing Multi-Scale Hydrogen Fuel Cell Catalyst Layer Nanostructures.

Multiscale design of catalyst layers (CLs) is important to advancing hydrogen electrochemical conversion devices toward commercialized deployment, which has nevertheless been greatly hampered by the complex interplay among multiscale CL components, high synthesis cost and vast design space. We lack rational design and optimization techniques that can accurately reflect the nanostructure-performance relationship and cost-effectively search the design space. Here, we fill this gap with a deep generative artificial intelligence (AI) framework, GLIDER, that integrates recent generative AI, data-driven surrogate techniques and collective intelligence to efficiently search the optimal CL nanostructures driven by their electrochemical performance. GLIDER achieves realistic multiscale CL digital generation by leveraging the dimensionality-reduction ability of quantized vector-variational autoencoder. The powerful generative capability of GLIDER allows the efficient search of the optimal design parameters for the Pt-carbon-ionomer nanostructures of CLs. We also demonstrate that GLIDER is transferable to other fuel cell electrode microstructure generation, e.g., fibrous gas diffusion layers and solid oxide fuel cell anode. GLIDER is of potential as a digital tool for the design and optimization of broad electrochemical energy devices.

Effect of synthetic surfactants on the environment and the potential for substitution by biosurfactants.

The environmental impacts of the use of synthetic surfactants are discussed in this work such as their high levels of toxicity and low biodegradability. These materials destroy aquatic microbial populations, damage fish and other aquatic life, and reduce photochemical energy conversion efficiency of plants as well as adversely affecting waste-water treatment processes. With global usage of surfactants being over 15 million tonnes annually, and an estimated 60% of surfactant ending up in the aquatic environment, there is an urgent need for alternatives with lower adverse environmental effects; this review explores biosurfactants as potential alternatives. The sources and natural function of biosurfactants are presented, together with their advantages compared with their synthetic counterparts, including their low toxicity and biodegradability. Their comparable effectiveness as surfactants has been demonstrated by surface tension reduction, achieved at much lower critical micelle concentrations that those of synthetic surfactants. The limitations and challenges for the use of biosurfactants are discussed, particularly low production yields; such limitations must be addressed before wide range industrial use of biosurfactants can be achieved. Although there has been focus on achieving greater production yields, a remaining issue is the lack of research into the use of biosurfactants in a greater range of industrial and consumer applications to demonstrate their efficacy and identify candidate biosurfactants for production. This review highlights such research as deserving of further investigation, alongside the ongoing work to optimize the production process.

Effective dynamic properties of random complex media with spherical particles.

The effective dynamic bulk modulus and density are presented for random media consisting of particles in a viscous host fluid, using a core-shell, self-consistent effective medium model, under the large compressional wavelength assumption. These properties are relevant to acoustic or dynamic processes in nano- and micro-particle fluids including particle density determination, resonant acoustic mixing, and acoustic characterisation. Analytical expressions are obtained for the effective bulk modulus and mass density, incorporating the viscous nature of the fluid host into the core-shell model through wave mode conversion phenomena. The effective density is derived in terms of particle concentration, particle and host densities, particle size, and the acoustic and shear wavenumbers of the liquid host. The analytical expressions obtained agree with prior known results in the limit of both static and inviscid cases; the ratio of the effective bulk modulus to that of the fluid is found to be quasi-static. Numerical calculations demonstrate the dependence of the effective mass density on frequency, particle size (from nano- to micro-regime), and concentration. Herein it is demonstrated both theoretically and numerically that the viscosity, often neglected in the literature, indeed plays a significant role in the effective properties of nanofluids.

Modelling viscous boundary layer dissipation effects in liquid surrounding individual solid nano and micro-particles in an ultrasonic field.

Upon application of ultrasonic waves to a suspension of solid particles in liquid, multiple scattering occurs at the particle/liquid interfaces leading to attenuation. It was recently shown through experimental verification that multiple scattering theory must include shear wave influences at the boundary between the liquid and solid particles in a nanofluid when the concentration of the scatterers is even as low as a few percent by volume. Herein, we consider silica spheres of 50-450 nm diameter in the long-wavelength regime to elucidate the form of the shear decay fields at the liquid/solid interface for individual particles. This is important because the overlap of these fields ultimately leads to the conversion of a compressional wave to shear waves and back into the compressional wave, the effect originating due to the density contrast between the particle and the liquid. Therefore, we examine in detail the velocity, vorticity and viscous dissipation in the shear wave field and around the silica spheres using finite element modelling, giving clarity to the viscous boundary effects. We also compare the numerical modelling to semi-analytical results.

The absorption of ultrasound in emulsions: computational modelling of thermal effects.

Around liquid particles in a fluid of contrasting properties (for example, oil in water) in ultrasonic fields there are small regions where thermal waves can propagate with relatively high amplitudes. Herein, we demonstrate the existence and character of these waveforms using three-dimensional finite element modelling based on linearised Navier-Stokes equations. We investigate single particles and small clusters of particles, validating the expected thermal wavelength and the power dissipation due to viscous and thermal effects around the particle. The energy lost due to thermal and viscous dissipation is explored as a function of the average separation distance between the particles (linking to concentration) as well as the applied frequency. The determination of energy loss provides a new method for calculating the attenuation in particle systems. We demonstrate that the effective attenuation of an emulsion in which particles exist in clusters is influenced by the interparticle separation within the cluster, even at the same total particle concentration. Thus, the finite element modelling provides evidence for thermal interactions and their effect in correlated particle systems.

Multiple scattering in random dispersions of spherical scatterers: Effects of shear-acoustic interactions.

The propagation of acoustic waves through a suspension of spherical particles in a viscous liquid is investigated, through application of a multiple scattering model. The model is based on the multiple scattering formulation of Luppé, Conoir, and Norris [J. Acoust. Soc. Am. 131, 1113-1120 (2012)] which incorporated the effects of thermal and shear wave modes on propagation of the acoustic wave mode. Here, the model is simplified for the case of solid particles in a liquid, in which shear waves make a significant contribution to the effective properties. The relevant scattering coefficients and effective wavenumber are derived in analytical form. The results of calculations are presented for a system of silica particles in water, illustrating the dependence of the scattering coefficients, effective wavenumber, speed, attenuation on particle size and frequency. The results demonstrate what has already been shown experimentally; that the shear-mediated processes have a very significant effect on the effective attenuation of acoustic waves, especially as the concentration of particles increases.

Experimental verification of nanofluid shear-wave reconversion in ultrasonic fields.

Here we present the verification of shear-mediated contributions to multiple scattering of ultrasound in suspensions. Acoustic spectroscopy was carried out with suspensions of silica of differing particle sizes and concentrations in water to find the attenuation at a broad range of frequencies. As the particle sizes approach the nanoscale, commonly used multiple scattering models fail to match experimental results. We develop a new model, taking into account shear mediated contributions, and find excellent agreement with the attenuation spectra obtained using two types of spectrometer. The results determine that shear-wave phenomena must be considered in ultrasound characterisation of nanofluids at even relatively low concentrations of scatterers that are smaller than one micrometre in diameter.

Shear-mediated contributions to the effective properties of soft acoustic metamaterials including negative index.

Here we show that, for sub-wavelength particles in a fluid, viscous losses due to shear waves and their influence on neighbouring particles significantly modify the effective acoustic properties, and thereby the conditions at which negative acoustic refraction occurs. Building upon earlier single particle scattering work, we adopt a multiple scattering approach to derive the effective properties (density, bulk modulus, wavenumber). We show,through theoretical prediction, the implications for the design of "soft" (ultrasonic) metamaterials based on locally-resonant sub-wavelength porous rubber particles, through selection of particle size and concentration, and demonstrate tunability of the negative speed zones by modifying the viscosity of the suspending medium. For these lossy materials with complex effective properties, we confirm the use of phase angles to define the backward propagation condition in preference to "single-" and "double-negative" designations.

Comparison of numerical and effective-medium modeling of porosity in layered media.

In this study, modeling approaches for porosity in layered media are presented and compared. First, an effective-medium model is used to account for the frequency-dependent attenuation of the elastic waves. The effective-medium model is based on a single-scattering approach, i.e., it neglects multiple-scattering effects. Then, the effective-medium model is compared in time-domain finite element simulations. The numerical model allows the study of the scattering of the elastic waves on randomly distributed spherical cavities and also accounts for multiple-scattering effects. The models are compared to investigate the validity of the effective-medium model approach. The calculated reflected laminate responses and transmission spectra from the two models show a good agreement.

Thermo-elastic multiple scattering in random dispersions of spherical scatterers.

Ultrasonic monitoring of concentrated suspensions and emulsions is limited in concentration range due to the inaccuracy of the multiple scattering models currently used to interpret measurements. This paper presents the development of a model for the additional multiple scattering caused by mode conversion to/from thermal waves. These effects are believed to cause significant deviation from established models for emulsions at high concentration, or small particle size, at low frequency. The relevant additional scattering coefficients (transition factors) are developed, in numerical and analytical form, together with the modification to the effective wavenumber. Calculations have been carried out for a bromohexadecane-in-water emulsion to demonstrate the frequency-dependence of the scattering coefficients, and the effective speed and attenuation.

Ultrasonic wave propagation in concentrated slurries--the modelling problem.

The suspended particle size distribution in slurries can, in principle, be estimated from measured ultrasonic wave attenuation across a frequency band in the 10s of MHz range. The procedure requires a computational model of wave propagation which incorporates scattering phenomena. These models fail at high particle concentrations due to hydrodynamic effects which they do not incorporate. This work seeks an effective viscosity and density for the medium surrounding the particles, which would enable the scattering model predictions to match experimental data for high solids loading. It is found that the required viscosity model has unphysical characteristics leading to the conclusion that a simple effective medium modification to the ECAH/LB is not possible. The paper confirms the successful results which can be obtained using core-shell scattering models, for smaller particles than had previously been studied, and outlines modifications to these which would permit rapid computation of sufficient stability to support fast particle sizing procedures.

Anomalous small angle x-ray scattering simulations: proof of concept for distance measurements for nanoparticle-labelled biomacromolecules in solution.

Anomalous small angle X-ray scattering can in principle be used to determine distances between metal label species on biological molecules. Previous experimental studies in the past were unable to distinguish the label-label scattering contribution from that of the molecule, because of the use of atomic labels; these labels contribute only a small proportion of the total scattering signal. However, with the development of nanocrystal labels (of 50-100 atoms) there is the possibility for a renewed attempt at applying anomalous small angle X-ray scattering for distance measurement. This is because the contribution to the scattered signal is necessarily considerably stronger than for atomic labels. Here we demonstrate through simulations, the feasibility of the technique to determine the end-to-end distances of labelled nucleic acid molecules as well as other internal distances mimicking a labelled DNA binding protein if the labels are dissimilar metal nanocrystals. Of crucial importance is the ratio of mass of the nanocrystals to that of the labelled macromolecule, as well as the level of statistical errors in the scattering intensity measurements. The mathematics behind the distance determination process is presented, along with a fitting routine than incorporates maximum entropy regularisation.

Simulation of ultrasonic array imaging of composite materials with defects.

Ultrasonic transducer arrays are extensively used for the nondestructive evaluation of materials for aerospace and other applications. However, their use with composites requires some technique development because of reflections at the layer boundaries and the effects of attenuation. When used in full matrix capture mode, algorithms such as the total focusing method (TFM) must be applied to obtain the image. In composite materials, improvement to the algorithm is required to include the effects of material anisotropy (affecting wave speed) and optimum aperture limits to optimize the signal-to-noise ratio and location detection for a defect in the material. This paper presents simulations of the ultrasonic array signals in multilayer anisotropic materials with and without a simulated defect. A kernel model for plane wave propagation in the material is combined with an angular spectrum decomposition (for finite transducer elements) and transducer frequency response, to model the full array signals. Inclusion of the defect is through its far-field scattering response. The model facilitates the study of imaging algorithm development by identification of the effects of anisotropy, signal-to-noise ratio, and aperture limit. An analytical method for the calculation of the effective group velocity in the composite at low frequency is demonstrated, permitting rapid calculation of time delay laws in practice.

Simulation of incoherent and coherent backscattered wave fields from cavities in a solid matrix.

This paper reports a study of the backscattered ultrasonic signal from a solid layer containing spherical cavities, to determine the conditions in which an effective medium model is a valid description of the response. The work is motivated by the need to model the response of porous composite materials for ultrasonic non-destructive evaluation (NDE) techniques. The numerical simulation predicts the response of a layer containing cavities at a single set of random locations, and compares it to the predicted response from a homogeneous layer with ensemble-averaged material properties (effective medium model). The study investigates the conditions in which the coherent (ensemble-averaged) response is obtained even from a single configuration of scatterers. Simulations are carried out for a range of cavity sizes and volume fractions. The deviation of the response from effective medium behavior is modeled, along with the trends as a function of cavity radius, volume fraction, and frequency, in order to establish an acceptability criterion for application of an effective medium model.

A comparison of stochastic and effective medium approaches to the backscattered signal from a porous layer in a solid matrix.

This paper reports a study of the backscattering behavior of a solid layer containing randomly spaced spherical cavities in the long wavelength limit. The motivation for the work arises from a need to model the responses of porous composite materials in ultrasonic NDE procedures. A comparison is made between models based on a summation over discrete scatterers, which show interesting emergent properties, and an integral formulation based on an ensemble average, and with a simple slab effective medium approximation. The similarities and differences between these three models are demonstrated. A simple quantitative criterion is established which sets the maximum frequency at which ensemble average or equivalent homogeneous medium models can represent echo signal generation in a porous layer for given interpore spacing, or equivalently, given pore size and concentration.

Acoustic scattering by a spherical obstacle: modification to the analytical long-wavelength solution for the zero-order coefficient.

Classical long wavelength approximate solutions to the scattering of acoustic waves by a spherical liquid particle suspended in a liquid (an emulsion) show small but significant differences from full solutions at very low k(c)a (typically k(c)a < 0.01) and above at k(c)a > 0.1, where k(c) is the compressional wavenumber and a the particle radius. These differences may be significant in the context of dispersed particle size estimates based on compression wave attenuation measurements. This paper gives an explanation of how these differences arise from approximations based on the significance of terms in the modulus of the complex zero-order partial wave coefficient, A(0). It is proposed that a more accurate approximation results from considering the terms in the real and imaginary parts of the coefficient, separately.

Acoustic scattering in dispersions: improvements in the calculation of single particle scattering coefficients.

Measurements of ultrasound speed and attenuation can be related to the properties of dispersed systems by applying a scattering model. Rayleigh's method for scattering of sound by a spherical object, and its subsequent developments to include viscous, thermal, and other effects (known as the ECAH model) has been widely adopted. The ECAH method has difficulties, including numerical ill-conditioning, calculation of Bessel functions at large arguments, and inclusion of thermal effects in all cases. The present work develops techniques for improving the ECAH calculations to allow its use in instrumentation. It is shown that thermal terms can be neglected in some boundary equations up to approximately 100 GHz in water, and several simplified solutions result. An analytical solution for the zero-order coefficient is presented, with separate nonthermal and thermal parts, allowing estimation of the thermal contribution. Higher orders have been simplified by estimating the small shear contribution as the inertial limit is approached. The condition of the matrix solutions have been greatly improved by these techniques and by including appropriate scaling factors. A method is presented for calculating the required Bessel functions when the argument is large (high frequency or large particle size). The required number of partial wave orders is also considered.