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An ultrafast, continuous CO 2 capture process driven by moisture gradient and electric field with low energy consumption to capture and concentrate CO 2 from dilute sources.
In this paper, we report a novel ammonia : ammonium salt solvent based pretreatment process that can rapidly dissolve crystalline cellulose into solution and eventually produce highly amorphous cellulose under near-ambient conditions. Pre-activating the cellulose I allomorph to its ammonia–cellulose swollen complex (or cellulose III allomorph) at ambient temperatures facilitated rapid dissolution of the pre-activated cellulose in the ammonia-salt solvent ( i.e. , ammonium thiocyanate salt dissolved in liquid ammonia) at ambient pressures. For the first time in reported literature, we used time-resolved in situ neutron scattering methods to characterize the cellulose polymorphs structural modification and understand the mechanism of crystalline cellulose dissolution into a ‘molecular’ solution in real-time using ammonia-salt solvents. We also used molecular dynamics simulations to provide insight into solvent interactions that non-covalently disrupted the cellulose hydrogen-bonding network and understand how such solvents are able to rapidly and fully dissolve pre-activated cellulose III. Importantly, the regenerated amorphous cellulose recovered after pretreatment was shown to require nearly ~50-fold lesser cellulolytic enzyme usage compared to native crystalline cellulose I allomorph for achieving near-complete hydrolytic conversion into soluble sugars. Lastly, we provide proof-of-concept results to further showcase how such ammonia-salt solvents can pretreat and fractionate lignocellulosic biomass like corn stover under ambient processing conditions, while selectively co-extracting ~80–85% of total lignin, to produce a highly digestible polysaccharide-enriched feedstock for biorefinery applications. Unlike conventional ammonia-based pretreatment processes ( e.g. , Ammonia Fiber Expansion or Extractive Ammonia pretreatments), the proposed ammonia-salt process can operate at near-ambient conditions to greatly reduce the pressure/temperature severity necessary for conducting effective ammonia-based pretreatments on lignocellulose.
The relationship between ambient conditions and light-duty vehicle energy consumption has been widely researched. Relatively little effort, however, has been dedicated to understanding representative ambient conditions a light-duty vehicle may experience. As such, the framework introduced in this article provides a means of quantifying ambient conditions specific to light-duty vehicle operation by incorporating both when and where vehicles are driven. The analysis presented expands the literature beyond solely focusing on temperature; distributions for humidity, solar irradiance, and air density are also included. A procedure is presented that calculates the ambient condition distributions for each metric by relating open-source data sets describing representative vehicle utilization and representative ambient conditions. While this study explores ambient conditions related to light-duty vehicle utilization, the framework may also be applied to separate vocations. Finally, the article concludes with an example use case of the ambient condition weighting process. A binning methodology is introduced that facilitates insight into vehicle energy consumption in response to ambient conditions at the national and local levels while minimizing the number of tests or simulations required.
Climate model fidelity in representing ENSO-induced teleconnection is assessed with process-oriented diagnostics that examine a chain of processes, from equatorial Pacific precipitation to the midlatitude circulation pattern over the Pacific–North American regions. Such processes are rarely addressed during model development. Using an upper-tropospheric divergent level, local vorticity gradient of the ambient zonal flow (∂ 2 U¯/∂y 2 ) and a restoring force for Rossby waves (β * ) are estimated, the equivalent barotropic vorticity equation is solved, and an anomalous Rossby wave source (RWS') quantified. The analysis is applied to AMIP5 and AMIP6 simulations. For a realistic circulation response representation, the hypothesis that models accurately represent the strength and location of RWS', and spatial variations in β * is tested. Compared to AMIP5, in AMIP6 there are clear improvements in representing RWS' and β * . To validate the hypothesis, the analysis identifies two metrics: spatially coherent RWS' in the subtropical North Pacific, and longitudes of negative β * over the western-central North Pacific. By projecting these metrics in two and three-dimensional views, improvements or degradations in model versions are apparent. If a model’s fidelity in representing ∂ 2 U¯/∂y 2 and RWS' are compromised, then radiated Rossby waves are reflected more equatorward, resulting in zonally elongated circulation anomalies over the central North Pacific. Thus, during climate model development, applying this analysis frequently will keep a regular check on the fidelity of the modeled response to anomalous El Niño convection in conjunction with changing model ambient flow dependencies. As a result, this analysis is intended to form a process-oriented diagnostics package, a community contribution to the NOAA Model Diagnostics Task Force.
A new method for dispersing of warm fogs which impede visibility and alter schedules is described. The method uses large volume recycled water sprays to create curtains of falling drops through which the fog is processed by the ambient wind and spray-induced air flow; the fog droplets are removed by coalescence/rainout. The efficiency of this fog droplet removal process depends on the size spectra of the spray drops and optimum spray drop size is calculated as between 0.3-1.0 mm in diameter. Water spray tests were conducted in order to determine the drop size spectra and temperature response of sprays produced by commercially available fire-fighting nozzles, and nozzle array tests were utilized to study air flow patterns and the thermal properties of the overall system. The initial test data reveal that the fog-dispersal procedure is effective.
The Cryogenic Carbon Capture™ (CCC) process separates CO2 from light gases in essentially any continuous process. CCC cools the gases to the frost or desublimation point of CO2 (-100 to -135 °C), separates and pressurizes the solids, and warms all streams to produce a CO2-depleted stream at ambient pressure and a pure (99+%) pressurized liquid CO2 stream typically to about 150 bar, both at ambient temperature. The process also recovers all gas moisture and most gas impurities less volatile than CO2 (NOx, SOx, Hg, PM, UHC, CCC, etc.) in separable streams. CCC nearly eliminates refrigeration energy for sensible temperature changes through heat integration. CCC does require energy to change the CO2 phase from a mixed vapor to a pressurized fluid, which represents the minimum energy required of any process for this separation. CCC uses additional energy for turbomachinery inefficiencies, heat losses, moisture removal and overall process pressure drop. Aside from these real-world energy demands, CCC operates near the minimum energy required to perform this gas separation by minimizing stream recycling. CCC compresses CO2 as a liquid, which is one of several reasons it costs about about half as much and consumes about half as much energy as an amine process when using flue gases with about 15% CO2. The process also has several major additional advantages, including (a) it is a bolt-on retrofit technology that does not need steam or any modification of existing equipment, (b) it recovers water and nearly all pollutants in addition to CO2 from the flue gas, (c) it enables highly efficient and cost effective energy storage at grid scale and on time scales of minutes, (d) it enables NG storage if the energy storage option is used, and (d) it has a small footprint and is minimally disruptive to existing plants, requiring only electrical power and a gas source to operate. Sustainable Energy Solutions (SES) has scaled this technology through several levels, the largest of which captures nominally 1 tonne of CO2/day and is called the skid system. Skid system field tests include utility-scale power plants, cement plants, heating plants, and other utility or industrial sites that burn natural gas, biomass, coal, shredded tires, municipal waste, and combinations of these fuels. These field tests produced 95-99% CO2 capture with CO2 purities of 99+% and initial CO2 contents that range from 4 to 28%. SES currently seeks to scale the system to merchant scale (10-80 tonnes of CO2 per day). In the process of doing so, SES has demonstrated the potential for CCC to contribute to energy storage and direct air capture in innovative and cost-effective ways. This presentation discusses the overall process and highlights results from field and in-house tests. These include (a) measured CO2 capture rates and operating conditions from in-house and field tests, and (b) predicted utility-scale costs and energy demands. This discussion also includes the application of the CCC technology to energy storage and direct air capture.
The ability to rapidly detect and characterize the chemistry of trace quantities of inorganic species has multiple potential applications, including nuclear safeguards, nuclear forensics, and environmental monitoring. Some mass spectrometric methods currently exist, but they are costly and time-intensive, often destroying chemical information in the process of ionization. Ambient mass spectrometry is a relatively new analytical method in which samples are introduced to the mass spectrometer from atmospheric pressure, rather than from high vacuum. Ambient MS can operate with gentler ionization methods such as electrospray ionization (ESI) and paper-spray ionization (PSI), reducing fragmentation and preserving the chemical information of the analyte. This may be useful for determining the intended purpose of material in a sample. Strontium, part of nuclear fallout, is analyzed here to test these new analytical methods for viability. Electrospray ionization mass spectrometry functions by spraying the sample as a solution through a needle charged to a few kV. A nebulizing gas flows out along with the sample to create the spray before droplets enter a drying chamber with heated drying gas to remove the solvent molecules. From there bare analyte ions enter the mass spectrometer. This method has the advantage of relatively fast sample preparation and stable ionization. More stable ionization produces higher-quality data. Paper-spray ionization mass spectrometry operates by applying sample to a paper triangle. The paper triangle is then electrified in a metal clamp to a few kV before spray solvent is applied. The spray solvent transports analyte in the sample to the tip, where it is ionized and enters the mass spectrometer. One advantage of this method is reduced sample preparation - an analyst can even swipe a surface and cut a triangle directly from the swipe. The data analysis serves to rapidly process tens of samples all at once. The mass spectrometer outputs a file containing a few hundred spectra for each sample. The pipeline processes each one to identify peaks of interest. A full palette of data analysis metrics are generated, including plots of the raw data and plots of calculated values such as isotopic ratios. The pipeline filters the raw data to remove noise and background peaks, as well as peaks representing detector saturation. A heat map is generated to show the overall spectrum in mass-time- intensity space. Post-processing, we obtained the desired calibration curves, demonstrating that both ESI-MS and PSI-MS are viable methods for quantifying trace amounts of inorganics while retaining their chemical speciation information. ESI-MS demonstrated a linear response region of 100 ppb to 20 ppm, with a limit-of-detection of around 100 ppb. At top left is an example spectrum with the {sup 88}SrNO{sub 3} peak identified to show the retention of chemical speciation. PSI-MS showed a linear response region of around 1 ppb to 1 ppm, with a limit-of-detection of near 1 ppb. PSI-MS produced more erratic results than ESI-MS, likely due to the variability in ionization resulting from manual positioning of the paper triangle near the MS inlet. Future efforts will focus on improving the repeatability of PSI-MS as well as analyzing other species of interest such as cerium and uranium. Improvements will also be made to create more reliable data extraction and intelligent data filtering.
A new brute-force method of warm fog dispersal is described. The method uses large volume recycled water sprays to create curtains of falling drops through which the fog is processed by the ambient wind and spray induced air flow. Fog droplets are removed by coalescence/rainout. The efficiency of the technique depends upon the drop size spectra in the spray, the height to which the spray can be projected, the efficiency with which fog laden air is processed through the curtain of spray, and the rate at which new fog may be formed due to temperature differences between the air and spray water. Results of a field test program, implemented to develop the data base necessary to assess the proposed method, are presented. Analytical calculations based upon the field test results indicate that this proposed method of warm fog dispersal is feasible. Even more convincingly, the technique was successfully demonstrated in the one natural fog event which occurred during the test program. Energy requirements for this technique are an order of magnitude less than those to operate a thermokinetic system. An important side benefit is the considerable emergency fire extinguishing capability it provides along the runway.
In order to achieve a net-zero carbon footprint by 2050, the global aviation industry must reduce its dependence on fossil fuels. In this regard, there is a global challenge to produce sufficient sustainable aviation fuel (SAF) from renewable sources. Isoprene is an intermediate molecule that can be derived from multiple biomass-based or biosynthetic routes. Here, in this work, we report a green route for the catalytic conversion of isoprene to hydrocarbons that are suitable for aviation fuel. By using an Amberlyst-15 catalyst without metal loading at ambient temperature (19–23 °C), as well as 40 °C, 50 °C, and 60 °C, isoprene was converted into olefinic precursors for SAF and/or blending with conventional aviation fuels. Specifically, at ambient temperature, the process achieved approximately 70 wt % conversion of isoprene with over 50 mol % carbon selectivity toward the aviation fuel range. The resulting SAF-range hydrocarbons were composed of iso-alkenes, branched olefinic monocyclic compounds, and bicyclic compounds, covering a wide range of aviation fuel components. Our work demonstrates, for the first time, the formation of diverse hydrocarbon families for SAF and/or aviation fuel blending at ambient temperature from isoprene.
Abstract The Soybean Free Air Concentration Enrichment (SoyFACE) facility is the longest running open-air carbon dioxide and ozone enrichment facility in the world. For over two decades, soybean, maize, and other crops have been exposed to the elevated carbon dioxide and ozone concentrations anticipated for late this century. The facility, located in East Central Illinois, USA, exposes crops to different atmospheric concentrations in replicated octagonal ~280 m 2 Free Air Concentration Enrichment (FACE) treatment plots. Each FACE plot is paired with an untreated control (ambient) plot. The experiment provides important ground truth data for predicting future crop productivity. Fumigation data from SoyFACE were collected every four seconds throughout each growing season for over two decades. Here, we organize, quality control, and collate 20 years of data to facilitate trend analysis and crop modeling efforts. This paper provides the rationale for and a description of the SoyFACE experiments, along with a summary of the fumigation data and collation process, weather and ambient data collection procedures, and explanations of air pollution metrics and calculations.
Enhanced geothermal systems (EGS) require cost-effective monitoring of fracture networks. We validate the capability of using borehole distributed acoustic sensing (DAS) ambient noise for fracture monitoring using core photos and core logs. The EGS Collab project has conducted 10 m scale field experiments of hydraulic fracture stimulation using 50–60 m deep experimental wells at the Sanford Underground Research Facility (SURF) in Lead, South Dakota. The first EGS Collab testbed is located at 1616.67 m (4850 ft) depth at SURF and consists of one injection well, one production well, and six monitoring wells. All wells are drilled subhorizontally from an access tunnel called a drift. The project uses a single continuous fiber-optic cable installed sequentially in the six monitoring wells to record DAS data for monitoring hydraulic fracturing during stimulation. We analyze 60 s time records of the borehole DAS ambient noise data and compute the noise root-mean-square (rms) amplitude on each channel (points along the fiber cable) to obtain DAS ambient noise rms amplitude depth profiles along the monitoring wellbore. Our noise rms amplitude profiles indicate amplitude peaks at distinct depths. We compare the DAS noise rms amplitude profiles with borehole core photos and core logs and find that the DAS noise rms amplitude peaks correspond to the locations of fractures or lithologic changes indicated in the core photos or core logs. We then compute the hourly DAS noise rms amplitude profiles in two monitoring wells during three stimulation cycles in 72 h and find that the DAS noise rms amplitude profiles vary with time, indicating the fracture opening/growth or closing during the hydraulic stimulation. Our results demonstrate that borehole DAS passive ambient noise can be used to detect fractures and monitor fracturing processes in EGS reservoirs.
Patchiness is perhaps the most salient characteristic of plankton populations in the ocean. The scale of this heterogeneity spans many orders of magnitude in its spatial extent, ranging from planetary down to microscale. It has been argued that patchiness plays a fundamental role in the functioning of marine ecosystems, insofar as the mean conditions may not reflect the environment to which organisms are adapted. Understanding the nature of this patchiness is thus one of the major challenges of oceanographic ecology. The patchiness problem is fundamentally one of physical-biological-chemical interactions. This interconnection arises from three basic sources: (1) ocean currents continually redistribute dissolved and suspended constituents by advection; (2) space-time fluctuations in the flows themselves impact biological and chemical processes, and (3) organisms are capable of directed motion through the water. This tripartite linkage poses a difficult challenge to understanding oceanic ecosystems: differentiation between the three sources of variability requires accurate assessment of property distributions in space and time, in addition to detailed knowledge of organismal repertoires and the processes by which ambient conditions control the rates of biological and chemical reactions. Various methods of observing the ocean tend to lie parallel to the axes of the space/time domain in which these physical-biological-chemical interactions take place. Given that a purely observational approach to the patchiness problem is not tractable with finite resources, the coupling of models with observations offers an alternative which provides a context for synthesis of sparse data with articulations of fundamental principles assumed to govern functionality of the system. In a sense, models can be used to fill the gaps in the space/time domain, yielding a framework for exploring the controls on spatially and temporally intermittent processes. The following discussion highlights only a few of the multitude of models which have yielded insight into the dynamics of plankton patchiness. In addition, this particular collection of examples is intended to furnish some exposure to the diversity of modeling approaches which can be brought to bear on the problem. These approaches range from abstract theoretical models intended to elucidate specific processes, to complex numerical formulations which can be used to actually simulate observed distributions in detail.
The growing concerns over CO 2 emissions have led to the development of various methods for CO 2 capture. CO 2 capture by amine-based sorbents has been achieved by temperature (thermal) swing adsorption (TSA) process, pressure swing adsorption (PSA) process, and temperature pressure or vacuuming swing adsorption (TPSA or TVSA) process for CO 2 capture. Amine sorbents for energy-efficient TSA, PSA, VSA, TPSA or TVSA CO 2 capture should possess a capability which allow adsorbed CO 2 to desorb and amine sorbent to be regenerated at low temperatures or low vacuums. Development of such amine sorbents would significantly decrease energy consumption and sorbent degradation during the regeneration step. The objective of this project is to develop a low vacuum swing adsorption (VSA) process for the capture of CO 2 from air. The focus is on the development of amine sorbent which allows CO 2 to adsorb in the form of weakly adsorbed CO 2 . The weakly adsorbed CO 2 species can be collected from the sorbent by applying a low vacuum at ambient temperature. Specifically, no heating (i.e., thermal energy) is needed for regeneration of amine sorbents. This novel sorbent allows VSA to be operated at ambient temperature without a significant energy demand. This process eliminates the energy-intensive heating and cooling process in temperature swing adsorption (TSA) process. Ambient temperature operation could prolong the lifetime of sorbent and minimize the maintenance cost. Extensive sorbent studies with in-situ infrared spectroscopy have revealed the modifications of conventional amine sorbents with additives can increase the fraction of weakly adsorbed CO 2 . The amine sorbents with loaded CO 2 can be regenerated in part by the following approaches: (i) mild heating to temperatures below 70 °C, (ii) flowing purging gas over modified amine sorbents at temperatures below 40 °C, (iii) vacuuming at pressure below 0.2 atm and temperatures below 40 °C. The performance of these modified amine sorbents has been tested in a 60 grams VSA unit at ambient temperatures. The results show that weakly adsorbed CO 2 which can be desorbed from modified amine sorbents with purging gas at 100 cc/min can also be evacuated at a vacuum of 1 psia at room temperature. A preliminary techno- economic analysis indicates the major cost of the VSA process with modified amine sorbents stems from the operation of vacuum pumps. Thus, developing an excellent sealing with minimum leakage for the VSA unit is the most critical task for further the development of this VSA technology.
The research program developed, validated and applies predictive computational protocols for calculating charge transfer (CT) rates in complex molecular systems, including molecular dyads and triads in liquid solution and solid-state organic semiconducting (OSC) materials. We have established a transformative computational scheme that goes beyond widely used simplifications, to achieve realistic descriptions of CT processes. The approach properly addresses the contribution of molecular environment at ambient conditions to CT processes. Our approach achieves unique insight on investigated CT processes in relevant experimental efforts. The collaborative team included three principal investigators (PIs), with complimentary expertise in classical molecular dynamics simulations and data science (Cheung), state-of-the-art electronic structure calculations (Dunietz), and cutting-edge theory and simulation techniques for modeling energy, charge and coherence transfer dynamics in molecular systems (Geva).
This report describes the MSFC space station water degradation study (WDS) and presents interim results from the first 24 months of testing. The WDS simulates the stagnant storage of water in distribution lines before the activation of the space station's water processor by storing processed water at ambient temperature in valved sections of 1-in stainless steel and titanium tube. The WDS seeks to determine whether the water quality will degrade unacceptably and whether microbial growth will proceed to an unmanageable extent during extended stagnation. During the first 24 months, significant changes have occurred. Although iodine, which is used as a biocide, was nearly depleted within the first 6 months of testing, microbial growth has been minimal. This report describes the decrease in iodine concentration and the results of microbial and biofilm analyses. Increases in total organic carbon, iodide, chloride, nickel, iron, and chromium concentrations are presented and discussed. The observed increase in conductivity and the decreases in pH and turbidity are also presented. The authors conclude that, with proper preparation, potable water can be stored under stagnant conditions without unmanageable degradation in water quality; a flushing operation and subsequent processing of the degraded water should render the water system ready for use.
Efficient and stable water adsorbents are essential for removing moisture from natural gas and olefins during their production. Industrial desiccants such as alumina and zeolites require high regeneration temperatures, while metal-organic frameworks often suffer from limited long-term stability and reusability. Here, we introduce a new type of molecular desiccants (M-PyC) that, in principle, can be reused indefinitely. These simple molecular coordination complexes undergo fully reversible phase transitions between crystalline and amorphous states through the decoordination (bond breaking) and recoordination (bond reforming) of water molecules. They exhibit high water uptake (30 wt%) and superb selectivity, excluding hydrocarbons entirely. Their effectiveness for dehydration, combined with low regeneration temperature, fast desorption kinetics, low-cost and green synthesis, easy scalability to kilogram quantities, and essentially unlimited recyclability, makes them truly competitive dehydration agents for industrial separations. The use of amorphous molecular adsorbents, where crystallinity and porosity are no longer stringent requirements, and the adsorption-desorption process entirely under ambient air, offers a conceptually different approach to adsorption-based separation science and potentially realistic solution to the long-standing challenge of sustained stability in coordinate-bonded adsorbents.
Over the past decade, metal halide perovskites (MHPs) have emerged as a promising materials platform for high-efficiency solar cells and low-cost optoelectronics. However, there are challenges that frustrate the large-scale manufacturing of MHP devices, including difficulty in controlling film composition, interface formation and their device instability under ambient conditions. Vapor processing offers an attractive path to manufacturability, while also opening the door to new opportunities in device design that could favorably impact ultrahigh efficiency tandem solar cells or overall stability. Emphasis here is on the use of an alternate processing methodology, vapor transport deposition (VTD), to deposit the MHP layer. In experimental work, we found that our deposition system had significant run-to-run variations in film thickness and composition. To understand and resolve these issues, we use COMSOL Multiphysics software to model the precursor deposition rate numerically, trying to guide the broad range of parameters in the system. The result can be matched with experimental data and provides insight into system hydrodynamics and molar transport effects. Finally, we show that chamber pressure is a key factor to scale up the VTD technique.
Washington River Protection Solutions, LLC (WRPS) contracted Pacific Northwest National Laboratory (PNNL) in support of their maturation testing and analysis to develop and deploy an ambient temperature solidification/stabilization process for low-activity waste (LAW) (referred to as “grout” in this report). The intent of this effort is to support a sample-and-send regulatory and processing strategy in the Hanford 200 West Area, specifically considering grout waste forms disposal at Hanford in the Integrated Disposal Facility (IDF). Currently the disposal of grouted LAW is not an option because the IDF is not permitted to receive this waste form. The material presented in this report is intended to help inform the U.S. Department of Energy (DOE), the site operating contractors, regulatory agencies, and stakeholders of the future implications of IDF disposal of a grouted LAW waste form, specifically for the behavior of nitrate (NO 3 - ) and nitrite (NO 2 - ) at the Hanford. The only calculation of nitrate release from a hypothetical grouted LAW inventory in the IDF showed that the overall release was slightly above the compliance limit of 45 mg/L nitrate and 3.32 mg/L nitrate after 1000 years (Asmussen et al. 2019). As such, uncertainty around the impact of nitrate and nitrite release from the IDF was identified in the recent National Academies of Sciences study of Hanford supplemental LAW by both the national laboratory team and Hanford stakeholders (Bates et al. 2023). However, these calculations (and others for the IDF involving secondary waste grout) may be conservative as no nitrate and nitrite retention in the grout waste form was assumed, nor any attenuation in the subsurface. There is evidence from the literature of processes that can attenuate nitrate migration both in the waste form and in the Hanford subsurface. If found to be technically defensible and likely to occur in the IDF and associated subsurface, then these processes should be included in modeling of the IDF to represent the behavior of nitrate and nitrite more accurately. Doing so would remove unnecessary conservatism in the modeling projections and reduce the uncertainty in assessments of facility compliance of a grouted LAW waste form in the IDF.