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DOE OSTI2025

AI‐Driven Robot Enables Synthesis‐Property Relation Prediction for Metal Halide Perovskites in Humid Atmosphere

Materials Acceleration Platforms (MAPs) – also known as self-driving laboratories– present a new paradigm for materials science and promise an order of magnitude accelerated materials discovery compared to the traditional trial-and-error approach. Metal halide perovskites (MHPs) are an emerging class of materials for optoelectronic applications but are plagued by irreproducible optoelectronic quality, particularly for films fabricated in a humid atmosphere. Here, in this work, a machine learning (ML)-guided closed-loop platform is developed with a multimodal data fusion approach to predict synthesis–property relations for the optical quality of MHP thin films in relative humidities (RHs) ranging from 5–55%. The efficiency of this approach is confirmed by the fast-dropping learning rate to 2% after experimentally sampling less than 1% of the possible 5,000+ combinations. The prediction of synthesis–property relations is done by optical and imaging characterizations. In situ photoluminescence characterization revealed the origin of thin film quality variation at different RH. These insights provide an avenue for controlling the MHP crystallization by fine-tuning the synthesis parameters and RH for a given chemistry, thus lifting the need for stringent atmosphere control. The MAP enables an accelerated screening and understanding of the synthesis design space, facilitating rational synthesis recipe choice for a wide range of materials.

AI-driven robot↗

DOE OSTI2024

Chiral-structured heterointerfaces enable durable perovskite solar cells

Mechanical failure and chemical degradation of device heterointerfaces can strongly influence the long-term stability of perovskite solar cells (PSCs) under thermal cycling and damp heat conditions. Here, we report chirality-mediated interfaces based on R-/S-methylbenzyl-ammonium between the perovskite absorber and electron-transport layer to create an elastic yet strong heterointerface with increased mechanical reliability. This interface harnesses enantiomer-controlled entropy to enhance tolerance to thermal cycling–induced fatigue and material degradation, and a heterochiral arrangement of organic cations leads to closer packing of benzene rings, which enhances chemical stability and charge transfer. The encapsulated PSCs showed retentions of 92% of power-conversion efficiency under a thermal cycling test (-40°C to 85°C; 200 cycles over 1200 hours) and 92% under a damp heat test (85% relative humidity; 85°C; 600 hours).

14 SOLAR ENERGY↗

DOE OSTI2025

Membrane Thickness Impact on Chemical Degradation Rates

Abstract A comprehensive investigation of PFSA membrane chemical degradation rates as a function of thickness (8-20 µm) is reported. The two-pronged study was conducted on bare membranes and as components of chemically-mitigated and mechanically-reinforced, state-of-the-art (SOA) membrane electrode assemblies (MEAs). The bare membranes were subjected to H2O2 vapor test and MEAs were degraded under OCV conditions, both at 90°C. Both test types employed fluoride release rates (FRR) to monitor chemical degradation rates. Vapor tests revealed that area-specific degradation rates were positively correlated with membrane thickness, but thickness normalized degradation rates were independent of thickness. Open-circuit voltage (OCV) investigations spanning the membrane thickness series of MEAs was probed via a 27-experiment 3(4-1) fractional factorial experimental design. Statistical analysis of the FRR values revealed that chemical degradation rates were dominated by the relative humidity value and that the area-specific degradation rates of MEAs were independent of membrane thickness. The OCV chemical durability insensitivity to membrane thickness is supported by on-load membrane chemical durability studies at the stack level. The results suggest that ,despite smaller ionomer inventory, SOA thin membranes and MEAs are not greatly disadvantaged relative to thicker membranes from a chemical durability perspective, provided oxidative stress levels are controlled throughout application lifetime.

Coms, Frank D. (ORCID:0000000249160350)↗

DOE OSTI2020

Coupled Gas-Exchange Model for C4 Leaves Comparing Stomatal Conductance Models

Plant simulation models are abstractions of plant physiological processes that are useful for investigating the responses of plants to changes in the environment. Because photosynthesis and transpiration are fundamental processes that drive plant growth and water relations, a leaf gas-exchange model that couples their interdependent relationship through stomatal control is a prerequisite for explanatory plant simulation models. Here, we present a coupled gas-exchange model for C4 leaves incorporating two widely used stomatal conductance submodels: Ball–Berry and Medlyn models. The output variables of the model includes steady-state values of CO2 assimilation rate, transpiration rate, stomatal conductance, leaf temperature, internal CO2 concentrations, and other leaf gas-exchange attributes in response to light, temperature, CO2, humidity, leaf nitrogen, and leaf water status. We test the model behavior and sensitivity, and discuss its applications and limitations. The model was implemented in Julia programming language using a novel modeling framework. Our testing and analyses indicate that the model behavior is reasonably sensitive and reliable in a wide range of environmental conditions. The behavior of the two model variants differing in stomatal conductance submodels deviated substantially from each other in low humidity conditions. The model was capable of replicating the behavior of transgenic C4 leaves under moderate temperatures as found in the literature. The coupled model, however, underestimated stomatal conductance in very high temperatures. This is likely an inherent limitation of the coupling approaches using Ball–Berry type models in which photosynthesis and stomatal conductance are recursively linked as an input of the other.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2022

Patterns and controls on island-wide aboveground biomass accumulation in second-growth forests of Puerto Rico

This dataset includes two products from Martinuzzi et al. (2022): "biomass.tif" is a 26-m resolution forest biomass (AGB) map for Puerto Rico derived from NASA G-LiHT lidar data and forest inventory data (FIA plots), in raster format. "input_multivariate_v2.shp" is a point shapefile with information on forest age, substrate, past land use, topographic wetness, slope, and precipitation, for each forest pixel. These two datasets can be used to evaluate spatial patterns of AGB in second-growth forests across transects of lidar data in humid forests of Puerto Rico, and to analyze relationship(s) between AGB and environmental variables. Additional information on these products can be found on the supporting file called "Readme.txt" included within the data archive, as well as in the original manuscript by Martinuzzi et al (2022).

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Dust pollution in China affected by different spatial and temporal types of El Niño

Dust is an important aerosol affecting air quality in China in the winter and spring seasons. Dust in China is potentially influenced by the interannual climate variability associated with El Niño. Here, the impacts of El Niño with different temporal and spatial types on dust pollution in boreal winter and spring in China and the potential mechanisms are investigated using a state-of-the-art Earth system model (E3SMv1). We find that the eastern Pacific (EP) and central Pacific (CP) El Niño both increase wintertime dust concentrations by 5–50 µg m –3 over central-eastern China. Due to a stronger wind and lower relative humidity, which favor dust emissions near sources, and a strengthened northwesterly and reduced precipitation, which are conducive to dust transport, dust concentrations during the CP El Niño are 5–20 µg m –3 higher in northern China than during the EP El Niño, although the changes are mostly insignificant. El Niño with a short duration (SD) increases boreal winter dust concentrations by 20–100 µg m –3 over northern China relative to the climatological mean, while there is a decrease of 5–50 µg m –3 during the long-duration (LD) El Niño, which is also related to the El Niño-induced changes in atmospheric circulation, precipitation, and relative humidity. In the following spring season, all types of El Niño events enhance dust over northern China, but only the increase during the LD El Niño is statistically significant, suggesting that the weaker intensity but longer duration of the LD El Niño events can significantly affect spring dust in China. Our results contribute to the current knowledge of the influence of El Niño on dust pollution, which has profound implications for air pollution control and dust storm prediction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Molecular-Level Control over Ionic Conduction and Ionic Current Direction by Designing Macrocycle-Based Ionomers

Poor ionic conductivity of the catalyst-binding, submicrometer- thick ionomer layers in energy conversion and storage devices is a huge challenge. However, ionomers are rarely designed keeping in mind the specific issues associated with nanoconfinement. Here, we designed nature-inspired ionomers (calix-2) having hollow, macrocyclic, calix[4]arene-based repeat units with precise, sub-nanometer diameter. In ≤100 nm-thick films, the in-plane proton conductivity of calix-2 was up to 8 times higher than the current benchmark ionomer Nafion at 85% relative humidity (RH), while it was 1-2 orders of magnitude higher than Nafion at 20-25% RH. Confocal laser scanning microscopy and other synthetic techniques allowed us to demonstrate the role of macrocyclic cavities in boosting the proton conductivity. The systematic self-assembly of calix-2 chains into ellipsoids in thin films was evidenced from atomic force microscopy and grazing incidence small-angle X-ray scattering measurements. Moreover, the likelihood of alignment and stacking of macrocyclic units, the presence of one-dimensional water wires across this macrocycle stacks, and thus the formation of long-range proton conduction pathways were suggested by atomistic simulations. We not only did see an unprecedented improvement in thin-film proton conductivity but also saw an improvement in proton conductivity of bulk membranes when calix-2 was added to the Nafion matrices. Nafion-calix-2 composite membranes also took advantage of the asymmetric charge distribution across calix[4]arene repeat units collectively and exhibited voltage-gating behavior. The inclusion of molecular macrocyclic cavities into the ionomer chemical structure can thus emerge as a promising design concept for highly efficient ion-conducting and ion-permselective materials for sustainable energy applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Vanderbilt Alumni Hall

This dataset includes processed and raw data from the Vanderbilt Alumni Hall Building (VAH) located on the University of Vanderbilt Campus in Nashville, TN. VAH is a mixed use commercial building (LEED Gold Certified) that consists of classrooms, meeting rooms, office rooms, conference rooms, an exercise room, and others. This dataset spans one year of time-series data from 2019 and includes measurements corresponding to whole building electrical power, thermal power, zone level thermal power, set-point, indoor temperature, humidity, water and air side supply and return temperatures and flow rates as CSV files. In addition to the measurements, a metadata .json file, and a .ttl file to visualize the data as per BRICK schema are also included.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2022

Idealized Simulations of the Tropical Climate and Variability in the Single Column Atmosphere Model (SCAM): Radiative-Convective Equilibrium

To explore the interactions among column processes in the Community Atmosphere Model (CAM), the single-column version of CAM (SCAM) is integrated for 1000 days in radiative-convective equilibrium (RCE) with tropical values of boundary conditions, spanning a parameter or configuration space of model physics versions (v5 vs. v6), vertical resolution (standard and 60 levels), sea surface temperature (SST), and some interpretation-driven experiments. The simulated time-mean climate is reasonable, near observations and RCE of a cyclic cloud-resolving model. Updraft detrainment in the deep convection scheme produces distinctive grid-scale structures in humidity and cloud, which also interact with radiative transfer processes. These grid artifacts average out in multi-column RCE results reported elsewhere, illustrating the nuts-and-bolts interpretability that SCAM adds to the hierarchy of model configurations. Multi-day oscillations of precipitation arise from descent of warm convection-capping layers starting near the tropopause, eventually reset by a burst of convective deepening. Experiments reveal how these oscillations depend critically on an internal parameter that controls the number of neutral buoyancy levels allowed for determining cloud top and computing dilute convective available potential energy in the deep convection scheme, and merely modified a little by disabling cloud-base radiation (heating of cloud base). This strong dependence of transient behavior in 1D on this parameter will be tested in the second part of this work, in which SCAM is coupled to a parameterized dynamics of two-dimensional, linearized gravity wave, and in the 3D simulations in future study.

Meteorology & Atmospheric Sciences↗

DOE OSTI2021

The Effect of an Equatorial Continent on the Tropical Rain Belt. Part 1: Annual Mean Changes in the ITCZ

The TRACMIP (Tropical Rain Belts with an Annual Cycle and Continent Model Intercomparison Project) ensemble includes slab-ocean aquaplanet controls and experiments with a highly idealized tropical continent, characterized by modified aquaplanet grid cells with increased evaporative resistance, increased albedo, reduced heat capacity, and no ocean heat transport (zero Q-flux). In the annual mean, an equatorial cold tongue develops west of the continent and induces dry anomalies and a split in the oceanic intertropical convergence zone (ITCZ). Ocean cooling is initiated by advection of cold, dry air from the winter portion of the continent; warm, humid anomalies in the summer portion are restricted to the continent by anomalous surface convergence. The surface energy budget suggests that ocean cooling persists and intensifies because of a positive feedback between a colder surface, drier and colder air, reduced downwelling longwave (LW) flux, and enhanced net surface LW cooling (LW feedback). A feedback between wind, evaporation, and SST (so-called WES feedback) also contributes to the establishment and maintenance of the cold tongue. Simulations with a gray-radiation model and simulations that diverge from protocol (with negligible winter cooling) confirm the importance of moist-radiative feedbacks and of rectification effects on the seasonal cycle. This mechanism coupling the continental and oceanic climate might be relevant to the double ITCZ bias. The key role of the LW feedback suggests that the study of interactions between monsoons and oceanic ITCZs requires full-physics models and a hierarchy of land models that considers evaporative processes alongside heat capacity as a defining characteristic of land.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Deliquescence of Eutectic LiCl-KCl Diluted with NaCl for Interim Waste Salt Storage

Molten eutectic LiCl-KCl salt is a widely used electrolyte for electrorefining uranium from spent nuclear fuel. Due to the hygroscopic nature of this salt, such operations must be performed under controlled atmospheric conditions, and waste salts require careful storage to avoid deliquescence and corrosion of container materials. This study investigated a potential processing path for reducing the degree of deliquescence through dilution to varying extents with NaCl. Here, the hydration behavior of LiCl-KCl salts diluted with NaCl was evaluated in terms of mass gain due to water absorption, degree of deliquescence (including first appearances of standing water), and evidence of corrosion to stainless steel containers in a humid air environment (40°C, 20% relative humidity). In this humid air environment, pure eutectic LiCl-KCl exhibited a 50 mass % increase due to water absorption and showed evidence of standing water after 24 h. Waste salt diluted with NaCl required loadings of 89 mass % NaCl in order to prevent deliquescence and exhibited a 3 mass % increase due to water absorption. After periodic observation for 48 h, standing water was observed near all ingots with the exception of the 89 mass % NaCl samples. Dilution with 89% NaCl was also found to reduce evidence of corrosion when stored in stainless steel crucibles. While dilution with NaCl greatly decreases steady-state hydration, the storage volume is increased ~10× through this procedure.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

PHOTO‐SENSITIVE LEAF ROLLING 1 encodes a polygalacturonase that modifies cell wall structure and drought tolerance in rice

Summary The biosynthesis and modification of cell wall composition and structure are controlled by hundreds of enzymes and have a direct consequence on plant growth and development. However, the majority of these enzymes has not been functionally characterised. Rice mutants with leaf‐rolling phenotypes were screened in a field. Phenotypic analysis under controlled conditions was performed for the selected mutant and the relevant gene was identified by map‐based cloning. Cell wall composition was analysed by glycome profiling assay. We identified a photo‐sensitive leaf rolling 1 ( psl1 ) mutant with ‘napping’ (midday depression of photosynthesis) phenotype and reduced growth. The PSL1 gene encodes a cell wall‐localised polygalacturonase (PG), a pectin‐degrading enzyme. psl1 with a 260‐bp deletion in its gene displayed leaf rolling in response to high light intensity and/or low humidity. Biochemical assays revealed PG activity of recombinant PSL1 protein. Significant modifications to cell wall composition in the psl1 mutant compared with the wild‐type plants were identified. Such modifications enhanced drought tolerance of the mutant plants by reducing water loss under osmotic stress and drought conditions. Taken together, PSL1 functions as a PG that modifies cell wall biosynthesis, plant development and drought tolerance in rice.

Zhang, Guangheng↗

DOE OSTI2023

The Surface Atmosphere Integrated Field Laboratory (SAIL) Campaign

The science of mountainous hydrology spans the atmosphere through the bedrock and inherently crosses physical and disciplinary boundaries: land-atmosphere interactions in complex terrain enhance clouds and precipitation, while watersheds retain and release water over a large range of spatial and temporal scales. Limited observations in complex terrain challenge efforts to improve predictive models of the hydrology in the face of rapid changes. The Upper Colorado River exemplifies these challenges, especially with ongoing mismatches between precipitation, snowpack, and discharge. Consequently, the U.S. Department of Energy’s (DOE) Atmospheric Radiation Measurement (ARM) user facility has deployed an observatory to the East River Watershed near Crested Butte, Colorado between September 2021 and June 2023 to measure the main atmospheric drivers of water resources, including precipitation, clouds, winds, aerosols, radiation, temperature and humidity. This effort, called the Surface Atmosphere Integrated Field Laboratory (SAIL), is also working in tandem with DOE-sponsored surface and subsurface hydrologists and other federal, state, and local partners. SAIL data can be benchmarks for model development by producing a wide range of observational information on precipitation and its associated processes, including those processes that impact snowpack sublimation and redistribution, aerosol direct radiative effects in the atmosphere and in the snowpack, aerosol impacts on clouds and precipitation, and processes controlling surface fluxes of energy and mass. Preliminary data from SAIL’s first year showcase the rich information content in SAIL’s many data-streams and support testing hypotheses that will ultimately improve scientific understanding and predictability of Upper Colorado River hydrology in 2023 and beyond.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Household Materials Selection for Homemade Cloth Face Coverings and Their Filtration Efficiency Enhancement with Triboelectric Charging

The COVID-19 pandemic is currently causing a severe disruption and shortage in the global supply chain of necessary personal protective equipment (e.g., N95 respirators). The U.S. CDC has recommended use of household cloth by the general public to make cloth face coverings as a method of source control. We evaluated the filtration properties of natural and synthetic materials using a modified procedure for N95 respirator approval. Common fabrics of cotton, polyester, nylon, and silk had filtration efficiency of 5–25%, polypropylene spunbond had filtration efficiency 6–10%, and paper-based products had filtration efficiency of 10–20%. An advantage of polypropylene spunbond is that it can be simply triboelectrically charged to enhance the filtration efficiency (from 6 to >10%) without any increase in pressure (stable overnight and in humid environments). Using the filtration quality factor, fabric microstructure, and charging ability, we are able to provide an assessment of suggested fabric materials for homemade facial coverings.

36 MATERIALS SCIENCE↗

DOE OSTI2025

A novel methodology for assessing the hygroscopicity of aerosol filter samples

Abstract. Due to US regulations, concentrations of hygroscopic inorganic sulfate and nitrate have declined in recent years, leading to an increased importance of the hygroscopic nature of organic matter (OM). The hygroscopicity of OM is poorly characterized because only a fraction of the multitude of organic compounds in the atmosphere is readily measured, and there is limited information on their hygroscopic behaviors. Hygroscopicity of aerosol is traditionally measured using a humidified tandem differential mobility analyzer (HTDMA) or electrodynamic balance (EDB). EDB measures water uptake by a single particle. For ambient and chamber studies, HTDMA measurements provide water uptake and particle size information but not chemical composition. To fill this information gap, we developed a novel methodology to assess the water uptake by particles collected on Teflon filters. This method uses the same filter sample for both hygroscopicity measurements and chemical characterization, thereby providing an opportunity to link the measured hygroscopicity with ambient particle composition. To test the method, hygroscopic measurements were conducted in the laboratory for ammonium sulfate, sodium chloride, glucose, and malonic acid, which were collected on 25 mm Teflon filters using an aerosol generator and sampler. Constant-humidity solutions (CHSs), including potassium chloride, barium chloride dihydrate, and potassium sulfate, were employed in a saturated form to maintain the relative humidity (RH) at approximately 84 %, 90 %, and 97 % in small chambers. Our preliminary experiments revealed that, without the pouch, water uptake measurements were not feasible due to rapid water loss during weighing. Additionally, we observed some absorption by the aluminum pouch itself. To account for this, concurrent measurements were conducted for both the loaded and the blank filters at each RH level. Thus, the dry loaded and blank Teflon filters were placed in aluminum pouches with one side open and in RH-controlled chambers for more than 24 h. The wet loaded samples and wet blanks were then weighed using an ultramicrobalance to determine the water uptake by the respective compound and the blank Teflon filter. The net amount of water absorbed by each compound was calculated by subtracting the water uptake of the blank filter from that of the wet loaded filter. Hygroscopic parameters, including the water-to-solute (W / S) ratio, molality, mass fraction solute (mfs), and growth factors (GFs), were calculated from the measurements. The results obtained are consistent with those reported by the Extended Aerosol Inorganics Model (E-AIM) and previous studies utilizing HTDMA and EDB for these compounds, highlighting the accuracy of this new methodology. This new approach enables the hygroscopicity and chemical composition of individual filter samples to be assessed so that in complex mixtures, such as chamber and ambient samples, the total water uptake can be parsed between the inorganic and organic components of the aerosol.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Will Anthropogenic Warming Increase Evapotranspiration? Examining Irrigation Water Demand Implications of Climate Change in California

Abstract Climate modeling studies and observations do not fully agree on the implications of anthropogenic warming for evapotranspiration (ET), a major component of the water cycle and driver of irrigation water demand. Here, we use California as a testbed to assess the ET impacts of changing atmospheric conditions induced by climate change on irrigated systems. Our analysis of irrigated agricultural and urban regions shows that warmer atmospheric temperatures have minimal implications for ET rates and irrigation water demands—about one percent change per degree Celsius warming (∼1% °C −1 ). By explicitly modeling irrigation, we control for the confounding effect of climate‐driven soil moisture changes and directly estimate water demand implications. Our attribution analysis of the drivers of ET response to global anthropogenic warming shows that as the atmospheric temperature and vapor pressure deficit depart from the ideal conditions for transpiration, regulation of stomata resistance by stressed vegetation almost completely offsets the expected increase in ET rates that would otherwise result from abiotic processes alone. We further show that anthropogenic warming of the atmosphere has minimal implications for mean relative humidity (<1.7% °C −1 ) and the surface available energy (<0.2% °C −1 ), which are critical drivers of ET. This study corroborates the growing evidence that plant physiological changes moderate the degree to which changes in potential ET are realized as actual ET.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Science Area 1: Standard Award: Model-Data Fusion to Examine Multiscale Dynamical Controls on Snow Cover and Critical Zone Moisture Inputs (Final Report)

In many mountain watersheds of the world, seasonal snowpacks play an important role as natural reservoirs of water. Seasonal snowpacks accumulate water during cold, wet winter months that subsequently melts. Downstream communities depend on water from melting seasonal snowpacks to support agricultural, industrial, and municipal water needs. Rapidly melting snowpacks can also present a flooding hazard, particularly if snowpacks melt at rates faster than anticipated and where adequate reservoir capacity is unavailable to buffer river flows associated with melt. The spatial and temporal dynamics of snow accumulation and melt also play an important role in supporting upland ecosystems in mountain landscapes. Snowmelt provides soil moisture that enable terrestrial ecosystem productivity and exert control on soil microorganisms that play important roles in global carbon cycles. Climate warming is gradually decreasing the amount of precipitation in mountain watersheds arriving as snow, presenting potentially profound disruptions to mountain ecosystems, as well as downstream delivery of water. The overarching goal of this project was to understand how interactions between the near-surface atmosphere and surface topography control the input, accumulation, retention, and release of water from mountain snowpacks. Over a 5-year period, this project pursued an approach combining high-resolution regional climate modeling, satellite and airborne remote sensing data, and ground-based observations to develop and analyze benchmark datasets to address overarching science questions and hypotheses. Key products include a continuous, long-term, high spatiotemporal resolution (1 km/1 hr) dataset characterizing key climate variables in the Upper Colorado River Basin. The dataset included historical estimates of precipitation, temperature, humidity, solar and longwave radiation, and wind speeds. Additionally, the project developed a 20+ year long, 30 m spatial, daily temporal multi-sensor dataset characterizing snow presence/absence in the East/Taylor River watersheds in the Central Rocky Mountains of Colorado. The project supported training of 1 postdoctoral scholar, 1 Ph.D. student, and 1 M.S. student.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

CO 2 Uptake and Stability Enhancement in Vinyltrimethoxysilane‐Treated SBA‐15 Solid Amine‐Based Sorbents

Abstract Silica‐supported amine absorbents, including materials produced by tethering aminosilanes or infusion of poly(ethyleneimine), represent a promising class of materials for CO 2 capture applications, including direct air and point source capture. Various silica surface treatments and functionalization strategies are explored to enhance stability and CO 2 uptake in amine‐based solid sorbent systems. Here, the synthesis and characterization of novel vinyltrimethoxysilane‐treated Santa Barbara Amorphous‐15 (SBA‐15) supports and the corresponding enhancement in CO 2 uptake compared to various SBA‐15‐based control supports are presented. The relationship between CO 2 diffusion and amine efficiency in these systems is explored using a previously reported kinetic model. The synthesized materials are characterized with CO 2 and H 2 O isotherms, diffuse reflectance infrared Fourier transform spectroscopy, 1 H T 1 – T 2 relaxation correlation NMR, and rapid thermal cycling experiments. The novel support materials are shown to enable high amine efficiencies, approaching a fourfold improvement over standard SBA‐15‐supported amines, while simultaneously exhibiting excellent stability when cycled rapidly under humid conditions. As the poly(ethyleneimine) loadings are held constant across the various samples, enhancements in CO 2 uptake are attributed to differences in the way the poly(ethyleneimine) interacts with the support surface.

Vallace, Anthony↗