Chemical and Light-Absorption Properties of Water-Soluble Organic Aerosols in Northern California and Photooxidant Production by Brown Carbon Components
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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
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A Data-Driven Framework for Predicting the Sorting and Screening Performance of an Integrated Biomass Feedstock Preprocessing System
The characteristics of mechanically sorted and screened lignocellulosic biomass, such as the mass contents of corn stover anatomical fractions (leaves, husks, stalks, cobs, etc.), can be used to calculate the intermediate feedstock quality attributes “yield” and “purity” that indicate the conversion efficiency of biocrude. No prior study has investigated the correlations from the characteristics of raw biomass and preprocessing unit operation parameters to those intermediate feedstock quality attributes. This work presents a data-driven framework for assessing and predicting the intermediate feedstock quality attributes in an integrated biomass feedstock preprocessing system. Our study used corn stover as a typical type of herbaceous biomass because of its abundance in the U.S. It began with data acquisition of moisture content, particle size distribution, and anatomical fractions of the materials after each unit operation in the system. The objective of this preprocessing system is to minimize husks and leaves and maximizing cobs and stalks by mechanically separating the materials into three streams via disc screen and air separator. Prototype neural network models were then developed to evaluate the feasibility of predicting process outcomes based on measurable parameters. It is found that incorporating physical constraints into these prediction models significantly enhances the accuracy of the predicted yield and purity against the ground truth data. The experimental data and model predictions indicate that decreasing throughput increases purity, while higher throughput results in lower purity. Finally, an optimization problem was introduced to search optimal combinations of feed material properties and preprocessing unit operation parameters, as the intermediate feedstock quality attributes – yield and purity, appeared to be competing factors. The study also suggests the continual need to improve the data-driven framework’s predictability by incorporating more accurate physical models to describe the dynamics in the preprocessing units such as the air separator.
09 - BIOMASS FUELS↗
Biomass-Derived Polymeric Binders in Silicon Anodes for Battery Energy Storage Applications
The demand for portable electronic devices has increased rapidly during the past decade, and has driven a concordant growth in battery production. Since their development as a commercial energy storage solution in the 1990s, lithium-ion batteries (LIBs) have attracted significant attention in both science and industry due to their long cycle life, high energy density, low self-discharge rate, and high working voltage. Production of LIBs requires large amounts of a polymeric binder – commonly polyvinylidene difluoride (PVDF) – for processing and performance purposes. However, since this material is petrochemically-derived, it is far from “green” or sustainable. On the other hand, polymers and their building blocks are found widely throughout nature and can be renewably sourced from biomass at low cost; therefore, replacing PVDF with biomass-derived binders is a promising approach to reduce the environmental footprint of LIBs. Additionally, polymer binders play a critical role in next-generation battery performance. For instance, silicon (Si) is a promising high-capacity anode material for LIBs because of its high theoretical capacity (4200 mA h g –1 ), low working potential, and high abundance in Earth's crust. However, its huge volume change during charge/discharge tends to result in a shortened cycle life, since conventional binders interact only weakly with silicon's native surface and cannot maintain long-term integrity of the electrode. Naturally derived polymers have found better success in this role due to their high structural advantages. In this review, we summarize recent developments in silicon anode binders derived from various biomass sources, with a focus on polymer properties and their effect on battery performance. Further, we propose various perspectives based on our own assessment of these works, and provide a brief commentary on the future outlook of the field.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
CFD-DEM Modeling of Autothermal Pyrolysis of Corn Stover with a Coupled Particle- and Reactor-Scale Framework
Autothermal operation of fast pyrolysis is an efficient process-intensification technique wherein exothermic oxidation reactions are used to overcome the heat-transfer bottleneck of conventional pyrolysis. The development of accurate, reliable modeling toolsets is imperative to generating a deeper understanding of biomass autothermal pyrolysis systems to support scale-up and industrial deployment. This modeling effort describes the development of single-particle and reactor models which incorporate detailed reaction schemes and simultaneous exothermic oxidation reactions. The particle-scale model was parameterized for corn stover feedstock with particle morphology, density, ash content, and biopolymer composition, all of which impact the emergent conversion characteristics during pyrolysis. Results were then used to parameterize a reactor-scale autothermal pyrolysis model, which was developed using a coarse-grained computational fluid dynamic-discrete element method. The simulation results compared well with experimental results, with the predicted bio-oil, light gas, and biochar yield within 3.0 wt% of the experimental yields. Further analyses were performed to test the influence of equivalence ratio, biomass injection position, and particle size distribution on autothermal pyrolysis. The analysis of the physio-chemical properties of the fluid and solid phase inside the reactor and at the reactor outlet help reveal important process interactions of autothermal pyrolysis.
BIOMASS FUELS,INORGANIC, ORGANIC, PHYSICAL, AND AN↗
Variation and evolution of atmospheric structure over the SEA BB season as seen from aircraft and reanalysis
The presence of absorbing aerosols and atmospheric water vapor will impact clouds both radiatively and dynamically. The atmosphere over the southeast Atlantic Ocean (SEA) experiences consistent springtime biomass burning (BB) smoke from widespread agricultural fires on the African continent. This smoke layer is initially lofted high in a continental mixed layer (~5-6km) and is then transported westward into the free troposphere where it overlies and ultimately mixes into the underlying stratocumulus-topped oceanic boundary layer. Coincident with this smoke is an elevated humidity signal which is present from the time a given airmass is over the continental source region. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) was a NASA Earth Venture Suborbital mission with the goal of measuring aerosol, cloud, and atmospheric properties over this region over three deployments in September 2016, August 2017, and October 2018. Measurements included in situ profile measurements of aerosol physical and optical properties, trace gas concentrations, and cloud properties, as well as column measurements of aerosol optical depth and trace gas concentrations from an airborne sun photometer, allowing for calculation of radiative heating at different altitudes. Here we present results from the three ORACLES deployments over the southeast Atlantic Ocean. The airborne observations capture both seasonal patterns (August through October) and spatial patterns (north/south and east/west) in the vertical smoke distribution and its correlation to atmospheric specific humidity over the SEA basin. We describe the observed variations and show that the variability in both meteorological and emissions is largely captured in the European Centre for Medium-range Weather Forecasting Copernicus Atmosphere Monitoring Service (ECMWF CAMS) reanalysis, which allows for a more systematic examination of the relative frequency of observed conditions and their radiative impact over the region. Finally, we discuss the broader radiative and dynamical implications of these results for conditions of biomass burning aerosols overlying stratocumulus clouds.
Kristina Marie Myers Pistone↗
Emerging Modification Technologies of Lignin-based Activated Carbon toward Advanced Applications
Lignin-based activated carbon (LAC) is a promising high-quality functional material due to high surface area, abundant porous structure, and various functional groups. Modification is the most important step to functionalize LAC by altering its porous and chemical properties. Here, this Review summarizes the state-of-the-art modification technologies of LAC toward advanced applications. Promising modification approaches are reviewed to display their effects on the preparation of LAC. The multiscale changes in the porosity and the surface chemistry of LAC are fully discussed. Advanced applications are then introduced to show the potential of LAC for supercapacitor electrode, catalyst support, hydrogen storage, and carbon dioxide capture. Finally, the mechanistic structure-function relationships of LAC are elaborated. These results highlight that modification technologies play a special role in altering the properties and defining the functionalities of LAC, which could be a promising porous carbon material toward industrial applications.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Airborne lidar observations of smoke haze during SCAR-B 1995
The Smoke, Clouds, Aerosol, and Radiation Brazil(SCAR-B) field campaign was conducted to study the effects that widespread and persistent biomass burning have upon radiative and chemical processes in the atmosphere. The radiative transfer characteristics of the atmosphere are altered by the introduction of particulate and gaseous materials which are the products of the combustion of vegetative material at ground level. These substances are transported and distributed horizontally and vertically by atmospheric dynamical processes which may be perturbed by the heat energy from the fires. As the pollutants disperse, their physical and chemical properties change substantially. A complete description of the effects of smoke requires that the evolution back to the natural situation be fully examined. A most important component of smoke haze investigation is finding its vertical and horizontal distribution in relation to the driving factors of dynamics and the related horizontal transport. In this presentation, we employ data from the Cloud Lidar System(CLS), carried aboard the NASA ER-2 aircraft, to provide a unique view of the particulate or aerosol loading produced by fires, especially with regard to the geometrical distribution of the aerosols in the vertical plane. The lidar has the ability to measure aerosol optical properties in a continuous fashion at quite fine vertical and horizontal resolution. The results from the lidar provide measurements that are largely independent of influences that corrupt passive instruments and thus it can serve to corroborate their results. The extended horizontal and vertical range of lidar results can also augment ground based and airborne in situ measurements which have limited horizontal and vertical scope. We present the results of our analysis of CLS observations taken during the SCAR-B field campaign. Observations of the the aerosol optical thickness from the Aerosol Robotic Network(AERONET) of solar photometers are employed in conjunction with CLS data to derive extinction to backscatter ratio values which are used to convert the lidar backscatter coefficient into extinction coefficient. The extinction coefficient is integrated vertically to find aerosol optical thickness along ER-2 flight tracks. We use images of the CLS derived extinction coefficient to depict its horizontal and vertical distribution. Multispectral photometer optical thickness is used to compute the Angstrom exponent. With these, we examine the hypothesis that the values of extinction to backscatter ratio can be related to the Anstrom coefficient since both of these would be a function of the refractive index and size distribution of the aerosols.
Hart, William D.↗
BETO 2021 Peer Review - FCIC Task 6: High Temperature Conversion
The impacts of feedstock variability on pyrolysis processes are significant but poorly defined. Current engineering designs are based on empirical guidelines, useful only over a narrow range of feedstock properties. The objectives of this project are to (1) Develop science-based knowledge of how feedstock attributes and operational parameters impact pyrolysis process reliability and product quality; and (2) Build an experimental and computational toolset that predicts these outcomes, enabling processes to optimize reliability and product quality. Biomass is a complex feedstock. Controlling for and testing the effects of individual attributes is very challenging. This project couples multiscale experimentation and modeling to accurately capture the fundamental physics and chemistry of biomass flow and conversion behavior in feeding and pyrolysis reactor operations. Our focus is on pine residue attributes – anatomical fraction (bark, needles, wood), particle morphology (size/shape distribution, density, porosity), and chemical composition (extractives, biopolymers, alkali metals) – that impact product quality for downstream catalytic upgrading. Because detailed pyrolysis product characterization is limited, cutting-edge analytical techniques are being developed to reveal impactful product attributes. The tools and knowledge developed here will enable integrated pyrolysis-based processes that are more robust, flexible, and market-responsive with respect to feedstock variability.
29 ENERGY PLANNING, POLICY, AND ECONOMY↗
Bioconversion of wastewater-derived cresols to methyl muconic acids for use in performance-advantaged bioproducts
We combine metabolic engineering and polymer chemistry to convert cresols, a main component of biomass-derived catalytic fast pyrolysis wastewater, to methyl muconic acids that have performance-advantaged properties in nylons and plasticizers.
09 BIOMASS FUELS↗
Bounding the Role of Black Carbon in the Climate System: a Scientific Assessment
Black carbon aerosol plays a unique and important role in Earth's climate system. Black carbon is a type of carbonaceous material with a unique combination of physical properties. This assessment provides an evaluation of black-carbon climate forcing that is comprehensive in its inclusion of all known and relevant processes and that is quantitative in providing best estimates and uncertainties of the main forcing terms: direct solar absorption; influence on liquid, mixed phase, and ice clouds; and deposition on snow and ice. These effects are calculated with climate models, but when possible, they are evaluated with both microphysical measurements and field observations. Predominant sources are combustion related, namely, fossil fuels for transportation, solid fuels for industrial and residential uses, and open burning of biomass. Total global emissions of black carbon using bottom-up inventory methods are 7500 Gg/yr in the year 2000 with an uncertainty range of 2000 to 29000. However, global atmospheric absorption attributable to black carbon is too low in many models and should be increased by a factor of almost 3. After this scaling, the best estimate for the industrial-era (1750 to 2005) direct radiative forcing of atmospheric black carbon is +0.71 W/sq m with 90% uncertainty bounds of (+0.08, +1.27)W/sq m. Total direct forcing by all black carbon sources, without subtracting the preindustrial background, is estimated as +0.88 (+0.17, +1.48) W/sq m. Direct radiative forcing alone does not capture important rapid adjustment mechanisms. A framework is described and used for quantifying climate forcings, including rapid adjustments. The best estimate of industrial-era climate forcing of black carbon through all forcing mechanisms, including clouds and cryosphere forcing, is +1.1 W/sq m with 90% uncertainty bounds of +0.17 to +2.1 W/sq m. Thus, there is a very high probability that black carbon emissions, independent of co-emitted species, have a positive forcing and warm the climate. We estimate that black carbon, with a total climate forcing of +1.1 W/sq m, is the second most important human emission in terms of its climate forcing in the present-day atmosphere; only carbon dioxide is estimated to have a greater forcing. Sources that emit black carbon also emit other short-lived species that may either cool or warm climate. Climate forcings from co-emitted species are estimated and used in the framework described herein. When the principal effects of short-lived co-emissions, including cooling agents such as sulfur dioxide, are included in net forcing, energy-related sources (fossil fuel and biofuel) have an industrial-era climate forcing of +0.22 (0.50 to +1.08) W/sq m during the first year after emission. For a few of these sources, such as diesel engines and possibly residential biofuels, warming is strong enough that eliminating all short-lived emissions from these sources would reduce net climate forcing (i.e., produce cooling). When open burning emissions, which emit high levels of organic matter, are included in the total, the best estimate of net industrial-era climate forcing by all short-lived species from black-carbon-rich sources becomes slightly negative (0.06 W/sq m with 90% uncertainty bounds of 1.45 to +1.29 W/sq m). The uncertainties in net climate forcing from black-carbon-rich sources are substantial, largely due to lack of knowledge about cloud interactions with both black carbon and co-emitted organic carbon. In prioritizing potential black-carbon mitigation actions, non-science factors, such as technical feasibility, costs, policy design, and implementation feasibility play important roles. The major sources of black carbon are presently in different stages with regard to the feasibility for near-term mitigation. This assessment, by evaluating the large number and complexity of the associated physical and radiative processes in black-carbon climate forcing, sets a baseline from which to improve future climate forcing estimates.
black carbon↗
Integrating environmental understanding into freshwater floatovoltaic deployment using an effects hierarchy and decision trees
Abstract In an era of looming land scarcity and environmental degradation, the development of low carbon energy systems without adverse impacts on land and land-based resources is a global challenge. ‘Floatovoltaic’ energy systems—comprising floating photovoltaic (PV) panels over water—are an appealing source of low carbon energy as they spare land for other uses and attain greater electricity outputs compared to land-based systems. However, to date little is understood of the impacts of floatovoltaics on the hosting water body. Anticipating changes to water body processes, properties and services owing to floatovoltaic deployment represents a critical knowledge gap that may result in poor societal choices and water body governance. Here, we developed a theoretically-derived hierarchical effects framework for the assessment of floatovoltaic impacts on freshwater water bodies, emphasising ecological interactions. We describe how the presence of floatovoltaic systems may dramatically alter the air-water interface, with subsequent implications for surface meteorology, air-water fluxes and physical, chemical and biological properties of the recipient water body. We apply knowledge from this framework to delineate three response typologies—‘ magnitude’ , those for which the direction and magnitude of effect can be predicted; ‘ direction’ , those for which only the direction of effect can be predicted; and ‘ uncertain’ , those for which the response cannot be predicted—characterised by the relative importance of levels in the effects hierarchy. Illustrative decision trees are developed for an example water body response within each typology, specifically, evaporative water loss, cyanobacterial biomass, and phosphorus release from bed sediments, and implications for ecosystem services, including climate regulation, are discussed. Finally, the potential to use the new understanding of likely ecosystem perturbations to direct floatovoltaic design innovations and identify future research priorities is outlined, showcasing how inter-sectoral collaboration and environmental science can inform and optimise this low carbon, land-sparing renewable energy for ecosystem gains.
Environmental Sciences & Ecology↗
An Overview of Potential Future Aviation Energy Carriers
Global jet fuel demand is projected to grow to 165 billion gallons by 2050 and there is growing interest in the aviation industry to understand the capabilities of alternative energy carriers. This report considers several potential energy carriers, reviewing their production potential, operational considerations, and economic implications to inform potential next steps in aeronautics research. The following energy carriers (i.e., fuels) were evaluated in this study for future use in aviation: sustainable aviation fuel (SAF) - both biomass-based and power-to-liquids (PtL) - based SAF - cryogenic hydrogen (LH 2 ) - also known as liquid hydrogen - liquefied natural gas (LNG), liquefied ethane (LE), and Jet X. The barriers and opportunities for the evaluated energy carriers vary. SAF is a commercially available drop-in fuel compatible with existing aircraft and infrastructure. SAF is limited by both higher prices and slow commercialization of multiple pathways using different feedstocks necessary to significantly grow supply. Cryogenic fuels, in contrast, have very different thermal, physical, and chemical properties than SAF and Jet A, requiring the construction of new airport storage and dispensing infrastructure and the design of new aircraft energy systems capable of mitigating heat transfer and boil-off. Cryogenic fuels offer an opportunity to diversify aviation fuel carriers from domestic energy relevant for both energy security and resilience. This means cryogenic fuels are more of a longer-term solution for aircraft but are worth exploring for potential future cost savings and emissions benefits. Jet X refers to non-drop-in liquid hydrocarbon fuels in the early stages of investigation seeking favorable properties. There are substantial barriers to non-drop-in liquid aviation fuels that are not compatible with existing aircraft and fuel infrastructure.
33 ADVANCED PROPULSION SYSTEMS↗
Single-phase catalysis for reductive etherification of diesel bioblendstocks
We developed a single-phase Pd/NbOPO 4 catalyst for reductive etherification that displays high catalytic activity, product selectivity, and regeneration stability.
Hafenstine, Glenn R.↗
Bridging particle and reactor scales in the simulation of biomass fast pyrolysis by coupling particle resolved simulation and coarse grained CFD-DEM
Efficient utilization of biomass is challenging due to the complexity of the feedstock at molecular, particle, and reactor scales. Direct coupling of particle scale model and reactor scale simulation is computationally infeasible. In this work, the results from a particle resolved simulation were used to calibrate the heat transfer and reaction kinetics of particles. A hybrid drag model was used to consider the different fluidization properties of sands and biomass particles. The computation cost was reduced using a coarse-grained Discrete Element Method (DEM). The simulated conversion rate, char yield, tar yield, and pyrolysis gas yield compare well with experiment. The residence time and axial distributions of biomass were also analyzed. This novel multi-scale method provides an efficient and accurate tool for the modeling of biomass pyrolysis reactors.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Anatomical Fraction segmentation in the biomass bales
The U.S. Department of Energy Bioenergy Technologies Office (BETO) is committed to the development of sustainable, nationwide, commercial biofuel production to displace petroleum-derived fuels, increase domestic energy production, and encourage the creation of a domestic bioenergy and bioproducts industry. Operating a commercial-scale bioenergy operation requires significant technological advancements for determining biomass feedstock quality during the preprocessing stage. Usage of non-food feedstocks- e.g., corn-stover, pine residue, and forest residue - at the biorefineries reduces strain on the food supply chain. But the non-food feedstock heterogeneity- physical size, shape, and chemical composition-poses a significant challenge during milling, conveyance, feeding, and biofuel conversion processes. 3D X-Ray imaging (CT) is capable of distinguishing material features by detecting density and compositional differences. But the inherent complexity introduced during harvesting and bailing makes the reconstruction and interpretation of baled biomass materials from x-ray data time consuming, laborious, and expensive. Feedstocks are low-density materials that produce small contrast differences in the x-ray images. This paper focuses on using the shape and texture properties, using 3D image processing techniques like 3D skeletonization, directional statistics to characterize and extract volumetric content of the different tissue samples in the biomass bales.
09 BIOMASS FUELS↗
Oxidative Catalytic Fractionation of Lignocellulosic Biomass Using a Co-N-P-C Catalyst and One-Step Isolation of Aromatic Monomers via Centrifugal Partition Chromatography
Methods for catalytic fractionation of biomass provide a means to convert lignin directly into monomers while generating a high-quality cellulosic stream, contrasting conventional biomass pretreatment strategies that prioritize the cellulosic fraction. Here, a nonprecious-metal Co-N-P-C catalyst is identified for aerobic oxidative catalytic fractionation (OCF) of poplar feedstock in dimethyl carbonate that achieves significantly higher yields of aromatic monomers (24 wt %) relative to those obtained with a recently reported Co-N-C catalyst in acetone solvent (15 wt %). Mechanistic studies indicate that the acidic properties of the catalyst contribute to its improved performance by promoting extraction of lignin from insoluble polysaccharides. This OCF process is complemented by the development of a new centrifugal partition chromatography (CPC) method that supports isolation of all five major aromatic monomers (syringic acid, syringaldehyde, vanillic acid, vanillin, and para-hydroxybenzoic acid) in a single liquid–liquid extraction purification step. Furthermore, this OCF/CPC sequence has important implications for future lignin valorization efforts.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
100+ RON Gasoline Blendstock for High Efficiency, Low Emissions (CRADA 493)
The PNNL/LanzaTech alcohol-to-Jet (ATJ) patented process converts ethanol from LanzaTech’s syngas fermentation process to low aromatic jet-range isoparaffins. Compounds are generated across a wide boiling range by the process. The project goal is to improve the viability of the ATJ process by increasing the RON of the gasoline fraction and determine what types of engines and vehicles can be fueled with this gasoline. PNNL experts’ team will investigate the impact of the process conditions and catalysts formulation on the blendstock composition in relation with the fuel properties. Co-optima capabilities for fuel properties measurements will be leveraged to assess the potential engines/ vehicles applications of the produced blendstock. A techno-economic-analysis will be conducted to assess the commercial viability of the process for generating a high RON gasoline-range fuel.
09 BIOMASS FUELS↗
Cell Wall Compositions of Sorghum bicolor Leaves and Roots Remain Relatively Constant Under Drought Conditions
Renewable fuels are needed to replace fossil fuels in the immediate future. Lignocellulosic bioenergy crops provide a renewable alternative that sequesters atmospheric carbon. To prevent displacement of food crops, it would be advantageous to grow biofuel crops on marginal lands. These lands will likely face more frequent and extreme drought conditions than conventional agricultural land, so it is crucial to see how proposed bioenergy crops fare under these conditions and how that may affect lignocellulosic biomass composition and saccharification properties. We found that while drought impacts the plant cell wall of Sorghum bicolor differently according to tissue and timing of drought induction, drought-induced cell wall compositional modifications are relatively minor and produce no negative effect on biomass conversion. This contrasts with the cell wall-related transcriptome, which had a varied range of highly variable genes (HVGs) within four cell wall-related GO categories, depending on the tissues surveyed and time of drought induction. Further, many HVGs had expression changes in which putative impacts were not seen in the physical cell wall or which were in opposition to their putative impacts. Interestingly, most pre-flowering drought-induced cell wall changes occurred in the leaf, with matrix and lignin compositional changes that did not persist after recovery from drought. Most measurable physical post-flowering cell wall changes occurred in the root, affecting mainly polysaccharide composition and cross-linking. This study couples transcriptomics to cell wall chemical analyses of a C4 grass experiencing progressive and differing drought stresses in the field. As such, we can analyze the cell wall-specific response to agriculturally relevant drought stresses on the transcriptomic level and see whether those changes translate to compositional or biomass conversion differences. Our results bolster the conclusion that drought stress does not substantially affect the cell wall composition of specific aerial and subterranean biomass nor impede enzymatic hydrolysis of leaf biomass, a positive result for biorefinery processes. Coupled with previously reported results on the root microbiome and rhizosphere and whole transcriptome analyses of this study, we can formulate and test hypotheses on individual gene candidates’ function in mediating drought stress in the grass cell wall, as demonstrated in sorghum.
59 BASIC BIOLOGICAL SCIENCES↗