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All sourcesNASA NTRSDOE OSTI
NASA NTRS2023

Distributions of Mesoscale Periodic Structures in the Elemental and Ionic Composition of the Solar Wind

Multiple statistical and event studies based on in situ observations have shown that the solar wind contains mesoscale (∼ 100 – 10,000 Mm) periodic structures in the proton number density. Remote observations of such structures and event studies of concurrent variations in composition have demonstrated that they can form in the solar atmosphere and be preserved while advecting outwards through the heliosphere. Viall, Kepko, and Spence (J. Geophys. Res. (Space Phys.) 113, A07101, 2008; J. Geophys. Res. (Space Phys.) 114, A01201, 2009) and Kepko, Viall, and Wolfinger (J. Geophys. Res. (Space Phys.) 125(8), e28037, 2020) have reported that periodic proton density structures preferentially occur at specific radial length scales and have published their distributions from Wind measurements near L1. Here, we conduct a statistical study of 14 years (1998 – 2011) of 12-minute composition data measured by the Solar Wind Ion Composition Spectrometer instrument aboard the Advanced Composition Explorer spacecraft. We found that the elemental and ionic composition also contain statistically significant mesoscale periodic structures and, for the first time, present occurrence distributions for elemental abundance ratios with low, intermediate, and high first ionization potentials as well as for key solar wind charge states. These distributions set important constraints on solar wind formation in general and the formation of periodic mesoscale solar wind structures specifically, as the elemental and ionic composition are known to be determined at the Sun and to not evolve during advection.

Solar wind↗
DOE OSTI2024

An Overview of Mesoscale Convective Systems: Global Climatology, Satellite Observations, and Modeling Strategies

Deep convection is responsible for redistributing water as well as energy and providing vital water resources for many regions of the world. Cumulonimbus clouds aggregation into a single storm system develop mesoscale convective systems (MCS). MCSs have precipitation covering a horizontal region on the scale of 100?km or more. After more than the last seven decades, MCS has been gradually received wide attention in the scientific community as an important component of the Earth's hydrologic cycle and energy balance. MCSs differ from ordinary deep convection because of the mesoscale circulations consisting of a layer of air overturning on a scale much larger than those created by individual convective updrafts or downdrafts. Moreover, a key feature that separates MCS from ordinary deep convection is the significant portion of stratiform precipitation that results in the production and detrainment of a large number of ice particles from their organized convective cores and continues the mesoscale ascent that supports ice growth and aggregation as the crystals fall. This significant stratiform precipitation gives rise to top-heavy latent heating profiles that have substantial impacts on the upper-level global circulations, especially for those MCS that have a larger portion of stratiform rainfall. Top-heavy latent heating profiles are more frequent over the ocean than over the land. These unique features of MCS suggest that they are important for the hydrologic cycle, general circulation, and radiative balance of the climate system. In this chapter, we focus on the recent advances in the climatological perspective of MCS as well as the research tools used to better understand MCS after the advent of the satellite era. We will discuss both tropical and midlatitude MCS, the influence of modes of tropical climate variability on MCS, and the new insight from satellite observations on MCS interaction with the land surface.

Chakraborty, Sudip↗
DOE OSTI2022

Mesoscale evaluation of AMPS using AWARE radar observations of a wind and precipitation event over the Ross Island region of Antarctica

Surface, upper-air, and radar observations are used to assess the performance of the Antarctic Mesoscale Prediction System (AMPS) in simulating the mesoscale aspects of a wind and precipitation event over the Ross Island region of Antarctica that spanned January 16–20, 2016. The observations, collected during the Atmospheric Radiation Measurement (ARM) West Antarctic Radiation Experiment (AWARE), provide a unique dataset for evaluating AMPS, especially the radar observations that facilitate a three-dimensional depiction of winds and precipitation. Comparisons of AMPS forecast data with surface meteorology, balloon-sounding, and profiling radar observations at and above sites near McMurdo Station reveal a mixture of similarities and differences. A generally southerly flow is evident at low levels in both the AMPS simulations and observed Doppler radial velocities. AMPS winds are comparable to those observed at the surface and aloft in terms of magnitude, direction, and timing but the strongest simulated southerly flow is displaced eastward relative to the observations. AMPS-simulated reflectivity over the broader Ross Island region is more limited in areal extent and smaller in magnitude than observed by a scanning Doppler radar. Three episodes of surface precipitation are observed near McMurdo Station over the five-day event with peak rates of ~3 mm h -1 and a total accumulation of ~22 mm. However, AMPS produces no surface precipitation at that location over the five-day event due to a low-level dry bias in the forecasts. Herein, the results show the first observationally based three-dimensional understanding of meteorology in the Ross Island region.

AMPS↗
DOE OSTI2025

Experimental Evaluation of Interfacial Bonding Strength Between 304 Stainless Steel Substrate and Electrodeposited Nickel Coating Using Mesoscale Mechanical Testing Methods

Electrodeposition is a commonly used method for depositing a metal layer on a metallic substrate, to provide a decorative finish or for functional purposes including wear and corrosion resistance. The interfacial bonding strength is a critical factor in determining the quality of electrodeposition, as it ensures the adhesion of the deposited layer to the substrate. Despite its importance, there has not previously been a suitable mechanical testing method to quantitatively characterize the bonding strength between the electrodeposited layers and the substrate, due to the high strength of the materials and to restrictions imposed by the geometry (due to the small thickness of the plating layer) to manufacture tensile bars. In this study, we introduce a novel mesoscale mechanical testing method to overcome these limitations. This technique was applied to assess the bonding strength between a 304 stainless steel (SS) substrate and electrodeposited nickel with three different plating formulae (nickel sulfamate, Watts bath, and hard nickel). The thickness of the pure nickel coatings achieved for each of the three electrolyte solutions was approximately 1 mm on each side of the substrate. Mesoscale tensile bars of 1 mm length were manufactured by a femtosecond laser, with the material interface at the center of the gauge section, and then tensile-tested with digital image correlation. Further, the results proved that the electrodeposition technique is able to produce a very high bonding strength that is close to the yield strength of both the substrate material and the electrodeposited nickel layer. Additionally, in the case of the Watts bath formula, the interfacial bonding strength between the SS 304 and electrodeposited nickel can exceed that of the nickel layer. This method is expected to be useful for quantifying the interfacial bonding strength in numerous applications.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Modeling the dynamic response of rock masses with multiple compliant fluid saturated joint sets—Part I: Mesoscale simulations

Recently a mesoscale model was developed that includes thermomechanically consistent constitutive equations with dissipation due to porous compaction, inelastic distortional deformation rate, and slipping on persistent dry joint surfaces. In this Part I of a two-part paper, we describe enhancements of the mesoscale model which include: normal compliance with hysteresis, non-persistent joints with finite area, joint sets with angular deviation, and the weakening effect of fluid pressure in the joints. Examples study the influences of these effects on average strength. These computationally expensive simulations are used to inspire functional forms in a continuum model, described in Part II, which is needed for large scale simulations of real applications.

42 ENGINEERING↗
DOE OSTI2021

Impact of a New Cloud Microphysics Parameterization on the Simulations of Mesoscale Convective Systems in E3SM

Abstract Mesoscale convective systems (MCSs) are one of the most climatically significant forms of convection because of their large role in water and energy cycles. The mesoscale features associated with MCS are difficult to represent in climate models because the relevant dynamics and physics are absent or poorly represented with coarse model resolution (∼100 km). Using a regionally refined model (RRM) with 0.25° grid spacing embedded in the Energy Exascale Earth System Model (E3SM), we explore the impact of cloud microphysics parameterizations on the simulation of precipitation, particularly MCS precipitation over the contiguous United States. The Predicted Particle Properties (P3) cloud microphysics scheme has been modified and implemented into E3SM to overcome the limitations of the default Morrison and Gettelman (MG2) scheme in which rimed precipitating ice particles (graupel/hail) are absent and frozen particles are artificially partitioned into cloud ice and snow. We show that P3 improves the simulation of precipitation statistics including frequency distribution compared with MG2 with a limited effect on the diurnal cycle. P3 predicts higher hourly rain rates, resulting in 20% more MCSs and a higher total MCS precipitation (4.4%) compared to MG2, agreeing better with observations. The improvements with P3 mainly result from improved representations of ice microphysics, which not only produces higher rain rates through melting but also leads to a stronger large‐scale ascending motion by releasing more latent heating. This study suggests that improving microphysics parameterization is important for simulating MCS precipitation as future climate model resolutions continue to increase.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Early warm-season mesoscale convective systems dominate soil moisture–precipitation feedback for summer rainfall in central United States

Land–atmosphere interactions play an important role in summer rainfall in the central United States, where mesoscale convective systems (MCSs) contribute to 30 to 70% of warm-season precipitation. Previous studies of soil moisture–precipitation feedbacks focused on the total precipitation, confounding the distinct roles of rainfall from different convective storm types. Here, we investigate the soil moisture–precipitation feedbacks associated with MCS and non-MCS rainfall and their surface hydrological footprints using a unique combination of these rainfall events in observations and land surface simulations with numerical tracers to quantify soil moisture sourced from MCS and non-MCS rainfall. Furthermore, we find that early warm-season (April to June) MCS rainfall, which is characterized by higher intensity and larger area per storm, produces coherent mesoscale spatial heterogeneity in soil moisture that is important for initiating summer (July) afternoon rainfall dominated by non-MCS events. On the other hand, soil moisture sourced from both early warm-season MCS and non-MCS rainfall contributes to lower-level atmospheric moistening favorable for upscale growth of MCSs at night. However, soil moisture sourced from MCS rainfall contributes to July MCS rainfall with a longer lead time because with higher intensity, MCS rainfall percolates into deeper soil that has a longer memory. Therefore, early warm-season MCS rainfall dominates soil moisture–precipitation feedback. This motivates future studies to examine the contribution of early warm-season MCS rainfall and associated soil moisture anomalies to predictability of summer rainfall in the major agricultural region of the central United States and other continental regions frequented by MCSs.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

The mesoscale order of nacreous pearls

A pearl’s distinguished beauty and toughness are attributable to the periodic stacking of aragonite tablets known as nacre. Nacre has naturally occurring mesoscale periodicity that remarkably arises in the absence of discrete translational symmetry. Gleaning the inspiring biomineral design of a pearl requires quantifying its structural coherence and understanding the stochastic processes that influence formation. By characterizing the entire structure of pearls (~3 mm) in a cross-section at high resolution, we show that nacre has medium-range mesoscale periodicity. Self-correcting growth mechanisms actively remedy disorder and topological defects of the tablets and act as a countervailing process to long-range disorder. Nacre has a correlation length of roughly 16 tablets (~5.5 µm) despite persistent fluctuations and topological defects. For longer distances (>25 tablets ~8.5 µm), the frequency spectrum of nacre tablets follows f –1.5 behavior, suggesting that growth is coupled to external stochastic processes—a universality found across disparate natural phenomena, which now includes pearls.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Environmental Conditions Affecting Global Mesoscale Convective System Occurrence

Abstract The ERA5 environments of mesoscale convective systems (MCSs), tracked from satellite observations, are assessed over a 20-yr period. The use of a large set of MCS tracks allows us to robustly test the sensitivity of the results to factors such as region, latitude, and diurnal cycle. We aim to provide novel information on environments of observed MCSs for assessments of global atmospheric models and to improve their ability to simulate MCSs. Statistical analysis of all tracked MCSs is performed in two complementary ways. First, we investigate the environments when an MCS has occurred at different spatial scales before and after MCS formation. Several environmental variables are found to show marked changes before MCS initiation, particularly over land. The vertically integrated moisture flux convergence shows a robust signal across different regions and when considering MCS initiation diurnal cycle. We also found spatial scale dependence of the environments between 200 and 500 km, providing new evidence of a natural length scale for use with MCS parameterization. In the second analysis, the likelihood of MCS occurrence for given environmental conditions is evaluated, by considering all environments and determining the probability of being in an MCS core or shield region. These are compared to analogous non-MCS environments, allowing discrimination between conditions suitable for MCS and non-MCS occurrence. Three environmental variables are found to be useful predictors of MCS occurrence: total column water vapor, midlevel relative humidity, and total column moisture flux convergence. Such relations could be used as trigger conditions for the parameterization of MCSs, thereby strengthening the dependence of the MCS scheme on the environment. Significance Statement Large storm systems called mesoscale convective systems form across Earth. These are collections of thunderstorms, with associated high-level clouds that produce substantial, lighter rainfall and modulate Earth’s energy balance. They produce hazardous weather conditions, such as floods and high winds, and are responsible for a high percentage of rainfall in many regions globally. We investigate the environmental conditions under which they form, so that we can understand the spatial extent of the environment which is important for their formation, and also where and when the effects of these storms might be felt. The novel information generated here should help improve the representation of these storms in weather and climate models, improving the prediction of rainfall, thunderclouds, and high-level clouds.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Evaluation of Mesoscale Convective Systems in Climate Simulations: Methodological Development and Results from MPAS-CAM over the U.S.

In this study, a process-oriented approach is developed to evaluate warm-season mesoscale convective system (MCS) precipitation and their favorable large-scale meteorological patterns (FLSMPs) over the U.S. This approach features a novel observation-driven MCS-tracking algorithm using infrared brightness temperature and precipitation feature at 12, 25 and 50 km resolution and metrics to evaluate the model large-scale environment favorable for MCS initiation. The tracking algorithm successfully reproduces the observed MCS statistics from a reference 4-km radar MCS database. To demonstrate the utility of the new methodologies in evaluating MCS in climate simulations with mesoscale resolution, the process-oriented approach is applied to two climate simulations produced by the Variable-Resolution Model for Prediction Across Scales coupled to the Community Atmosphere Model physics, with refined horizontal grid spacing at 50 km and 25 km over North America. With the tracking algorithm applied to simulations and observations at equivalent resolutions, the simulated number of MCS and associated precipitation amount, frequency and intensity are found to be consistently underestimated in the Central U.S., particularly from May to August. The simulated MCS precipitation shows little diurnal variation and lasts too long, while MCS precipitation area is too large and intensity is too weak. The model is able to simulate four types of observed FLSMP associated with frontal systems and low-level jets (LLJ) in spring, but the frequencies are underestimated because of low-level dry bias and weaker LLJ. Precipitation simulated under different FLSMPs peak during daytime, in contrast to the observed nocturnal peak. Implications of these findings for future model development and diagnostics are discussed.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Low-Level Mesoscale and Cloud-Scale Interactions Promoting Deep Convection Initiation

Data from scanning radars, radiosondes, and vertical profilers deployed during three field campaigns are analyzed to study interactions between cloud-scale updrafts associated with initiating deep moist convection and the surrounding environment. Three cases are analyzed in which the radar networks permitted dual-Doppler wind retrievals in clear air preceding and during the onset of surface precipitation. These observations capture the evolution of (i) the mesoscale and boundary layer flow, and (ii) low-level updrafts associated with deep moist convection initiation (CI) events yielding sustained or short-lived precipitating storms. The elimination of convective inhibition did not distinguish between sustained and unsustained CI events, though the vertical distribution of convective available potential energy may have played a role. The clearest signal differentiating the initiation of sustained versus unsustained precipitating deep convection was the depth of the low-level horizontal wind convergence associated with the mesoscale flow feature triggering CI, a sharp surface wind shift boundary, or orographic upslope flow. The depth of the boundary layer relative to the height of the LFC failed to be a consistent indicator of CI potential. Widths of the earliest detectable low-level updrafts associated with sustained precipitating deep convection were ~3–5 km, larger than updrafts associated with surrounding boundary layer turbulence (~1–3 km wide). It is hypothesized that updrafts of this larger size are important for initiating cells to survive the destructive effects of buoyancy dilution via entrainment.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Shape-Selective Mesoscale Nanoarchitectures: Preparation and Photocatalytic Performance

We create ordered arrays of shape-selective gold-titania composite nanomaterials at the mesoscale (100 µm to 5 mm) by a combination of both bottom-up and top-down approaches for exquisite control of the size, shape, and arrangement of nanomaterials. Lithographic techniques along with wet chemical synthetic methods were combined to create these composite nanomaterials. The photocatalytic activity of these TiO 2, TiO 2 -Au and SiO 2 -TiO 2 -Au nano-composite mesoscale materials was monitored by the photodegradation of a model analyte, methyl orange, under UV and visible (Vis) illumination. Bare TiO 2 - and SiO 2 -TiO 2 -coated pillar arrays showed significant activity toward methyl orange in UV light with degradation rates on the order of 10 −4 –10 −3 min −1 . The photocatalytic activity of these arrays was also found to depend on the nanoparticle shape, in which particles with more edges and corners were found to be more reactive than spherical particles (i.e., the photocatalytic activity decreased as follows: diamonds > squares > triangles > spheres). SiO 2 -TiO 2 -Au nano-composite pillar arrays were tested in both UV and Vis light and showed increased activity in Vis light but decreased activity in UV light as compared to the bare semiconductor arrays. Additionally, the Au nanorod-functionalized nanoarrays exhibit a strong shape-dependence in their photocatalytic activity toward methyl orange degradation in Vis light.

36 MATERIALS SCIENCE↗
NASA NTRS2021

Do Sub-Mesoscales Inhibit Destruction of PV?

We present the first explicit form of the three components, advective, diabatic and frictional of the PV J fluxes contributed by sub-mesoscales SM. Of particular interest is the surface value of the vertical frictional PV flux which when positive, can induce destruction of PV by down-front winds. The 2005 numerical simulations of Thomas confirmed that this is indeed the case. However, since the 12 km numerical resolution could not account for sub-mesoscales SM (0.1-10) km, the effect of SM on the PV destruction process could not be quantified. The goal of this work is to provide an answer to that question asked in the title. The two SM parameterizations entering the problem, the vertical buoyancy flux and the momentum flux (Reynolds stresses), bring about a new feature, the dependence on the SM kinetic energy (represented by the dimensionless Rossby number Ro), that causes unexpected results. While in the absence of SM, there were no restrictions on where PV destruction could occur, in the presence of SM, the condition of a positive surface vertical frictional flux is restricted to SM regimes with very low Ro<1 and very high Ro>10. Since the SM kinetic energy is location dependent, so is PV destruction. The effect of SM seems to make PV destruction a much rarer occurrence than previously thought.

potential vorticity↗
DOE OSTI2020

An Adaptive-Mesh-Refinement Based Computational Tool for Simulating Catalysis at Mesoscale

In this work, we present a computational tool for mesoscale applications using open-source exascale- computing compatible adaptive-mesh-refinement (AMR) library, AMReX [2]. AMReX is software library that enables development of application solvers with block-structured Cartesian AMR. Our tool has capabilities to include realistic geometry representation, chemical species transport, reactions and thermodynamics that are critical for capturing mesoscale physics. A significant achievement is the ability of our solver to automatically import electron microscopy data in the form of a stereolithography (STL) or pixelated file format (mrc, tiff) without undergoing the tedious task of unstructured mesh generation. This feature allows for rapid simulation of catalyst particles with complex morphologies using an immersed-boundary formulation. The use of AMR allows for higher resolutions at catalyst surface interfaces, which in turn provides an accurate description of surface reactions and transport. Our solver uses a hybrid distributed and shared memory parallelism (OpenMP/GPU-based) with which strong scaling up to 10,000 processors for realistic catalyst particle simulations have been demonstrated.

BIOMASS FUELS,MATHEMATICS AND COMPUTING↗
DOE OSTI2022

Simulation of the effects of biomass burning in a mesoscale convective system in the central amazon

During the dry season of 2014, the formation of a mesoscale convective system (MCS) caused intense precipitation and strong winds in the central Amazon region. In this period, cases of MCS that occurred during the days when there were higher concentrations of CO were analyzed. Through this criterion, a case of MCS occurred on August 16th, 2014 was selected. We used the chemical-atmospheric model WRF-Chem to assess the influence of biomass burning aerosol on the intensity of precipitation, winds, vertical and horizontal transport associated with this convective system. We show that biomass burning aerosol reduces the strength of the mesoscale convective system, with less vertical and horizontal transport of carbon monoxide and ozone. Here, in the absence of biomass burning aerosol downdrafts and precipitation rate are more intense, and cloud development up to 5km is more developed, making the horizontal flow and vertical transport of ozone more intense, however, much more efficient in reducing the concentrations of other gases.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Mesoscale modeling and semi-analytical approach for the microstructure-aware effective thermal conductivity of porous polygranular materials

Here we established a comprehensive modeling approach for investigating the microstructure-aware effective thermal conductivity ($κ_{eff}$) for porous microstructures containing solid particles and gaseous pores. Our approach combines the mesoscale computational modeling framework and the semi-analytical method, allowing for efficient prediction of $κ_{eff}$ for realistic porous microstructures, while considering complicated microstructural thermal conduction pathways effectively in the prediction. We used the diffuse-interface mesoscale computational model to generate extensive simulated $κ_{eff}$ data for realistic digital representations of microstructures with wide ranges of porosity ($f_p$), thermal conductivity of the gas phase ($κ_g$), and thermal conductivity of the solid phase ($κ_s$). From the simulated data, we identified two property variation regimes for $κ_{eff}$: (1) a slow $κ_{eff}$ increase for $κ_s ~ κ_g$; and (2) a faster $κ_{eff}$ increase for $κ_s \gg κ_g$. To capture the key features of the relationship between the microstructure and $κ_{eff}$, we derived a semi-analytical model by introducing structure and intensification factors. The two new factors incorporate the calibrated effective contribution of the solid volume with $κ_s$ and additional interfacial effects into the prediction of $κ_{eff}$, respectively, allowing for consideration of parallel, serial, and interfacial conduction mechanisms effectively. Using the selected simulation data, we quantified key model parameters within the semi-analytical model and verified that the parameterized model exhibits excellent agreement with simulated $κ_{eff}$ for the entire range of the parameter space.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Anion-dependent phase behavior of methylimidazolium-based ionic liquids mixed with water: Correlation between local molecular structure and mesoscale behaviors

The mesoscopic phase behavior of decylmethylimidazolium (C 10 mim) ionic liquids (ILs) bearing three monovalent anions—thiocyanate (SCN − ), nitrate (NO 3 − ), and chloride (Cl − )—mixed with water at relatively high IL contents (50–95 wt%) was investigated. Small-angle and wide-angle X-ray scattering (SAXS/WAXS) were employed to follow the evolution of both local and mesoscale structures across this composition range. In the absence of water, C 10 mimSCN and C 10 mimCl behaved as disordered liquids, whereas C 10 mimNO 3 spontaneously formed a hexagonally ordered cylindrical mesophase and displayed a sticky-solid macroscopic appearance. Upon addition of water, C 10 mimSCN remained a viscous liquid and only weakly ordered lamellar domains were observed. This limited ordering is attributed to the lack of hydrogen bonding and weak interaction energy between SCN − anions and C 10 mim + cations. In contrast, the trigonal-planar NO 3 − and point-like Cl − anions promoted the formation of well-defined hexagonal mesophases up to 35–45 wt% water. The formation of hydrogen bonding of the two anions with imidazolium ring protons likely enabled the creation of compact ion clusters that effectively exclude water molecules from the immediate vicinity of the IL aggregates. These findings demonstrate that the interaction energy between ion pairs dictate IL-water interactions and therefore control the transition from disordered liquids to ordered mesophases in IL/water mixtures with high IL contents. In conclusion, the combined SAXS/WAXS analysis reveals a correlation between local intermolecular structure and the emergence of mesoscopic order, providing a systematic framework for tailoring mesoscale structures in alkylimidazolium-based IL/water systems.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Carbonation of Alkaline Earth Metal Hydroxides: Structure across Nano- to Mesoscales

The conversion of gaseous CO 2 into a solid constitution through mineralization is an active area of carbon capture, and alkaline earth metal hydroxides (M(OH) 2 , M = Ca 2+ , Mg 2+ ) are frontrunners in this area. As model systems, nanolime samples are excellent templates for the study of this reaction. Here, we have examined these under ambient pressure conditions with controlled humidity and CO 2 . Utilizing a broad range of analytical methods, we first established the purity and structures of the selected materials. We then examined the structural changes due to carbonation, using infrared spectroscopy, X-ray scattering, and neutron scattering. The resulting structural changes are resolved from nanoscale to mesoscale and from early-stage to late-stage carbonation. Ca(OH) 2 and Mg(OH) 2 are found to behave quite differently. As expected from prior work, the carbonation of Ca(OH) 2 is kinetically favored. Further, our structure studies suggest this is due to a facile reaction at the fractal interface of the particles. From early- to late-stage carbonation, there is a consistent increase in the fractal roughness. This is in contrast to Mg(OH) 2 where the same surface evolves into a smooth conformal coating. For this material the major reacting component is at the mesoscale, suggesting globular particle growth or evolving macro-porosity. Because neutron scattering is sensitive to hydrogen content, we expected a significant change as M(OH) 2 evolves to MCO 3 . Such a change is found for Ca(OH) 2 but not for Mg(OH) 2 , providing evidence for the formation of hydrated carbonates for the later material. The formation of a conformal layer along with water-rich carbonate formation is an impediment to the use of Mg(OH) 2 for carbon capture. For energy-efficient carbon capture, it would be desirable to enhance carbonation rates for Mg(OH) 2 , and one possible route would be the use of anhydrous fluids.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗