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At least 235 records · Page 13
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Engineering and characterization of carbohydrate‐binding modules for imaging cellulose fibrils biosynthesis in plant protoplasts

Abstract Carbohydrate binding modules (CBMs) are noncatalytic domains that assist tethered catalytic domains in substrate targeting. CBMs have therefore been used to visualize distinct polysaccharides present in the cell wall of plant cells and tissues. However, most previous studies provide a qualitative analysis of CBM‐polysaccharide interactions, with limited characterization of engineered tandem CBM designs for recognizing polysaccharides like cellulose and limited application of CBM‐based probes to visualize cellulose fibrils synthesis in model plant protoplasts with regenerating cell walls. Here, we examine the dynamic interactions of engineered type‐A CBMs from families 3a and 64 with crystalline cellulose‐I and phosphoric acid swollen cellulose. We generated tandem CBM designs to determine various characteristic properties including binding reversibility toward cellulose‐I using equilibrium binding assays. To compute the adsorption ( nk on ) and desorption ( k off ) rate constants of single versus tandem CBM designs toward nanocrystalline cellulose, we employed dynamic kinetic binding assays using quartz crystal microbalance with dissipation. Our results indicate that tandem CBM3a exhibited the highest adsorption rate to cellulose and displayed reversible binding to both crystalline/amorphous cellulose, unlike other CBM designs, making tandem CBM3a better suited for live plant cell wall biosynthesis imaging applications. We used several engineered CBMs to visualize Arabidopsis thaliana protoplasts with regenerated cell walls using confocal laser scanning microscopy and wide‐field fluorescence microscopy. Lastly, we also demonstrated how CBMs as probe reagents can enable in situ visualization of cellulose fibrils during cell wall regeneration in Arabidopsis protoplasts.

09 BIOMASS FUELS↗
DOE OSTI2021

A novel lung-inspired 3D-printed desiccant-coated heat exchanger for high-performance humidity management in buildings

Offering an independent humidity management method for buildings, desiccant-coated heat exchangers (DCHXs) are deemed a promising approach to improve the overall energy efficiency of air conditioning (AC) systems. State-of-the-art DCHXs, however, are bound with conventional HX topologies either providing limited desiccant-air interfacial areas or introducing excessive pressure drop penalties. In this paper a novel 3D-printed DCHX concept inspired by the bronchi arrangement of a human lung is introduced to address the shortcomings inherent in existing DCHX designs. The proposed lung-inspired DCHX utilizes two intertwined bicontinuous flow networks enabling highly efficient heat and mass transfer characteristics for augmented adsorption and regeneration processes at low pressure drop penalties. While the first network evenly distributes an incoming air stream through the entire volume of the lung-inspired DCHX, the second network volumetrically splits a cooling water stream within and through the first network. Effects of various parameters including air flow rate, outdoor air humidity ratio, and regeneration temperature on dehumidification performance and energy efficiency of the proposed lung-inspired DCHX were investigated. Experimental results indicated the proposed lung-inspired 3D-printed DCHX outperforms existing DCHX systems by demonstrating an excellent balance between a high volumetric adsorption rate and a low pressure drop penalty. The volumetric adsorption rate of the proposed lung-inspired DCHX technology is 54.8 g/m 3 -s, a more than two-fold improvement compared with state-of-the-art DCHX systems. Additionally, the lung-inspired DCHX offers high thermal energy efficiency of 56% at a low regeneration temperature of 40 °C. Therefore, the proposed lung-inspired 3D-printed DCHX offers a new solid-desiccant-based air dehumidification pathway for next-generation high-performance AC systems.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2026

A Review on Direct Air Capture of Carbon Dioxide: Sorbent Materials, Process Engineering, Industrial Scale-Up, and Future Perspectives

The relentless accumulation of anthropogenic greenhouse gases has driven atmospheric carbon dioxide concentrations to approximately 426 ppm, necessitating the aggressive deployment of negative-emission technologies to achieve net zero by 2050. Direct air capture (DAC) offers a scalable, location-independent approach to atmospheric carbon removal; however, it is fundamentally constrained by the significant thermodynamic barriers associated with capturing CO 2 from ultradilute ambient conditions, requiring minimum thermodynamic energy inputs substantially higher than those for postcombustion point sources. This comprehensive review critically examines the technological landscape of DAC, focusing on the interdependent triad of sorbent material design, contactor engineering, and regeneration thermodynamics. We evaluate the fundamental boundaries of adsorption, emphasizing that an optimal adsorption enthalpy and isosteric heat of adsorption must balance the high CO 2 uptake capacity with the energetic penalties of sorbent regeneration. A systematic, comparative analysis of state-of-the-art sorbents is presented, encompassing mesoporous silicas, zeolites, carbon-based materials (CBMs), metal−organic frameworks (MOFs), porous organic polymers (POPs), and polymeric membranes. Special attention is devoted to surface functionalization strategies, particularly amine grafting and impregnation, which transition capture mechanisms from physisorption to chemisorption to enhance selectivity under ambient moisture and low partial pressures. Furthermore, we assess the operational merits of various reactor configurations, including gas−solid, gas−liquid, and membrane contactors, alongside regeneration cycles such as temperature, vacuum, pressure, and moisture swing adsorption. Finally, the review bridges fundamental materials science with industrial application by chronicling the scale-up milestones of pioneering entities and providing a strategic roadmap for advancing DAC technology readiness levels toward global deployment.

Adsorption↗
DOE OSTI2021

Effect of Fluoroethylene Carbonate Additives on the Initial Formation of the Solid Electrolyte Interphase on an Oxygen-Functionalized Graphitic Anode in Lithium-Ion Batteries

The formation of a solid electrolyte interphase (SEI) at the electrode/electrolyte interface substantially affects the stability and lifetime of lithium-ion batteries (LIBs). One of the methods to improve the lifetime of LIBs is by the inclusion of additive molecules to stabilize the SEI. To understand the effect of additive molecules on the initial stage of SEI formation, in this work we compare the decomposition and oligomerization reactions of a fluoroethylene carbonate (FEC) additive on a range of oxygen-functionalized graphitic anodes to those of an ethylene carbonate (EC) organic electrolyte. A series of density functional theory (DFT) calculations augmented by ab initio molecular dynamics (AIMD) simulations reveal that EC decomposition on an oxygen-functionalized graphitic ($11\bar{2}0$) edge facet through a nucleophilic attack on an ethylene carbon site (C E ) of an EC molecule (S2 mechanism) is spontaneous during the initial charging process of LIBs. However, decomposition of EC through a nucleophilic attack on a carbonyl carbon (C C ) site (S1 mechanism) results in alkoxide species regeneration that is responsible for continual oligomerization along the graphitic surface. In contrast, FEC prefers to decompose through an S1 pathway, which does not promote alkoxide regeneration. Including FEC as an additive is thus able to suppress alkoxide regeneration and results in a smaller and thinner SEI layer that is more flexible toward lithium intercalation during the charging/discharging process. In addition, we find that the presence of different oxygen functional groups at the surface of graphite dictates the oligomerization products and the LiF formation mechanism in the SEI.

25 ENERGY STORAGE↗
DOE OSTI2023

Dynamic Tracking of NiFe Smart Catalysts using In Situ X-Ray Absorption Spectroscopy for the Dry Methane Reforming Reaction

The exsolution of nanoparticles from perovskite precursors has been explored as a route to synthesize catalysts with sinter or coke resistance. The characteristics of these exsolved nanoparticles are highly dynamic depending on the redox nature of the environment to which they are subjected. To develop their properties for thermo- and electrocatalytic applications, it is necessary to track the states and behavior of exsolved catalysts with in situ and ex situ characterization. In this study, we conduct in situ X-ray absorption spectroscopy (XAS) along with ex situ scanning transmission electron microscopy high-angle annular dark-field (STEM-HAADF) and energy-dispersive X-ray spectroscopy analysis of the parent perovskite oxide precursor, LaFe 0.8 Ni 0.2 O 3 , as its structure forms bimetallic NiFe nanoparticles and evolves in oxidative, reductive, and dry methane reforming environments. We develop a theory that NiFe exsolution is a function of the reduction potential where LaFe 0.8 Ni 0.2 O 3 transforms to NiFe alloy supported on LaO x -LaFeO x . The Ni starts to exsolve at 268 °C, while most Fe exsolves at 700 °C. During dry methane reforming conditions, most of the Fe is oxidized by CO 2 during the reaction and re-enters the perovskite as LaFeO 3 , while Ni remains on the surface as nanoparticles in the metallic state. During the oxidative regeneration phase, most of the Fe re-enters the bulk perovskite phase, while Ni is partially regenerated with a small percentage oxidized to large NiO nanoparticles. Finally, this study sheds light on the exsolution and regeneration of bimetallic alloy nanoparticles and the influence of the reaction conditions on their catalyst performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Co(salen)-Catalyzed Oxidation of Lignin Models to Form Benzoquinones and Benzaldehydes: A Computational and Experimental Study

Lignin is a highly abundant polyphenolic polymer that imparts mechanical strength to plant biomass. Transition-metal complexes can catalyze lignin oxidation to produce value-added products, but low catalytic efficiency has hampered their use in industry. Identifying the chemical and structural factors that govern catalytic activity is a prerequisite to rational design of catalysts with improved activity. In this study, we combine computational and experimental approaches to investigate the mechanism of Co(salen)-catalyzed oxidation of the monomeric lignin models syringyl (S), vanillyl (G), and 4-hydroxybenzyl alcohol (H) to produce benzoquinone and benzaldehyde products. Experimentally, S oxidation to form dimethoxybenzoquinone proceeded efficiently with a Co(salen) catalyst coordinated by a pyridine ligand, but G and H did not undergo oxidation. Density functional theory calculations reveal that catalyst regeneration is energetically unfavorable in the presence of H, which prevents oxidation. In contrast, S readily facilitates catalyst regeneration. Formation of methoxybenzoquinone from G was achieved experimentally by adding bulky, noncoordinating bases. These findings provide a fundamental baseline for enhancing the activity of Co-Schiff base catalysts toward lignin-like molecules by adding sterically hindered nitrogenous bases or potentially by including a cocatalyst that promotes catalyst regeneration.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Sorbent Mediated Electrocatalytic Reduction of Dilute CO 2 to Methane

Efficient CO 2 utilization is a critical component of closing the anthropogenic carbon cycle. Most studies have focused on the use of pure streams of CO 2 . However, CO 2 is generally available only in dilute streams, which requires capture by sorbents followed by energy-intensive regeneration to release concentrated CO 2 . Direct utilization of sorbed-CO 2 avoids the costly regeneration step, and the sorbent-CO 2 interaction can kinetically activate CO 2 to tune its reactivity toward products that could otherwise be inaccessible with direct CO 2 reduction. We demonstrate that an N-heterocyclic carbene, 1,3-bis(2,6-diisopropylphenyl)imidazol-2-ylidene (DPIy), quantitatively reacts with CO 2 from dilute streams (0.04 and 10%) to form the sorbent-CO 2 substrate 1,3-bis(2,6-diisopropylphenyl)imidazolium-2-carboxylate (DPICx). Electrocatalyst iron tetraphenylporphyrin chloride (Fe(TPP)Cl) typically reduces CO 2 to CO; however, with DPICx as the substrate, the eight-electron reduced product methane (CH 4 ) is produced with a high Faradaic efficiency (>85%) and regeneration of the sorbent DPIy. In addition to the overall energy and capital advantages of integrated CO 2 capture and conversion, this result illustrates how sorbents can serve a dual purpose for both CO 2 capture and chemical auxiliary purposes to access unique products. CO 2 has a spectrum of reactivity with different types of sorbents; thus, these studies demonstrate how sorbent-CO 2 interactions can be leveraged for integrated capture and utilization platforms to access a wider range of CO 2 -derived products.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

In situ electrochemical recomposition of decomposed redox-active species in aqueous organic flow batteries

Aqueous organic redox flow batteries (AORFBs) offer a safe and potentially inexpensive solution to the problem of storing massive amounts of electricity produced from intermittent renewables. However, molecular decomposition is the major barrier preventing AORFBs from being commercialized. Structural modifications can improve molecular stability at the expense of increased synthetic cost and molecular weight. Utilizing 2,6-dihydroxy-anthraquinone (DHAQ), without further structural modification, we demonstrate that electrochemical regeneration could be a viable route to achieve low-cost, long-lifetime AORFBs. In situ (online) NMR and EPR and complementary electrochemical analyses reveal that decomposition compounds i.e., 2,6-dihydroxy-anthrone (DHA) and its tautomer, 2,6-dihydroxy-anthranol (DHAL), can be converted back to DHAQ in two steps: first DHA(L) 2- are oxidized to the dimer (DHA) 2 4- at - 0.32 V vs. SHE by one-electron transfer; subsequently, the (DHA) 2 4- is oxidized to DHAQ 2- at +0.57 V vs. SHE by three-electron transfer. Electrochemical regeneration rejuvenates not only DHAQ 2- , but also the positive electrolyte – rebalancing the states of charge of both electrolytes without introducing extra ions. We demonstrate the repeated capacity recovery with DHAQ | potassium ferro-/ferricyanide flow battery in basic conditions, and show the approach is also effective for anthraquinone-2,7-disulfonate in acid. Electrochemical regeneration strategies may extend the useful lifetime of many water-soluble organic molecules with anthraquinone core structures in electrochemical cells.

25 ENERGY STORAGE↗
DOE OSTI2024

Capturing carbon dioxide from air with charged-sorbents

Emissions reduction and greenhouse gas removal from the atmosphere are both necessary to achieve net-zero emissions and limit climate change. There is thus a need for improved sorbents for the capture of carbon dioxide from the atmosphere, a process known as direct air capture. In particular, low-cost materials that can be regenerated at low temperatures would overcome the limitations of current technologies. In this work, we introduce a new class of designer sorbent materials known as ‘charged-sorbents’. These materials are prepared through a battery-like charging process that accumulates ions in the pores of low-cost activated carbons, with the inserted ions then serving as sites for carbon dioxide adsorption. We use our charging process to accumulate reactive hydroxide ions in the pores of a carbon electrode, and find that the resulting sorbent material can rapidly capture carbon dioxide from ambient air by means of (bi)carbonate formation. Unlike traditional bulk carbonates, charged-sorbent regeneration can be achieved at low temperatures (90–100 °C) and the sorbent’s conductive nature permits direct Joule heating regeneration using renewable electricity. Given their highly tailorable pore environments and low cost, we anticipate that charged-sorbents will find numerous potential applications in chemical separations, catalysis and beyond.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Analysis of bipolar membranes for electrochemical CO 2 capture from air and oceanwater

Carbon dioxide (CO 2 ) must be removed from the atmosphere to mitigate the negative effects of climate change. However, the most scalable methods for removing CO 2 from the air require heat from fossil-fuel combustion to produce pure CO 2 and continuously regenerate the sorbent. Bipolar-membrane electrodialysis (BPM-ED) is a promising technology that uses renewable electricity to dissociate water into acid and base to regenerate bicarbonate-based CO 2 capture solutions, such as those used in chemical loops of direct-air-capture (DAC) processes, and in direct-ocean capture (DOC) to promote atmospheric CO 2 drawdown via decarbonization of the shallow ocean. In this study, we develop an experimentally validated 1D model for the electrochemical regeneration of CO 2 from bicarbonate-based carbon capture solutions and seawater using BPM-ED. For DAC, our experimental and computational results demonstrate that pH swings induced by BPM water dissociation drive the formation of CO 2 at the cation-exchange layer|catholyte interface with energy-intensities of less than 150 kJ mol -1 . However, high rates of bubble formation increase energy intensity at current densities >100 mA cm -2 . Correspondingly, accelerating water dissociation catalysis and enacting bubble removal could enable CO 2 recovery at energy intensities <100 kJ mol -1 and current densities >100 mA cm -2 . For DOC, mass transport limitations associated with low carbon concentrations in oceanwater suggest that DOC is best suited for clean production of acid and base usable in downstream processes. Further, these results provide design principles for industrial-scale CO 2 recovery using BPM-ED.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Sustainable forest management for carbon, wood and biodiversity must consider natural disturbance regimes

Abstract Forests provide multiple benefits that include sequestering carbon, supporting biodiversity, and providing wood products. Managing temperate forests to achieve these benefits sustainably is challenging given the legacy of past human impacts, the complexity of forest development, and increasing but unpredictable disturbances. These intricacies prompted debate about the most effective management of temperate forests to achieve climate mitigation while sustaining forest productivity, regeneration, and diversity. Most research focused on management impacts under relatively stable environmental conditions, whereas forests are facing increasingly frequent and more severe climatic and biotic disturbances. Here, we used a regionally calibrated forest growth model to simulate the effects of forest management on carbon, biodiversity, and wood production under prevalent natural disturbances in the northeastern US. We developed scenarios combining forest management and disturbance regimes based on assumptions of species-specific tree regeneration and mortality rates. We compared passive management with no cutting that prioritizes maintaining existing forest trees with two common regional harvest practices: exploitative timber harvest that prioritizes short-term wood production and regenerative timber harvest that prioritizes regenerating biodiverse native forest tree seedlings. In the absence of natural disturbance, no cutting provides 41% higher forest carbon storage and 50% higher tree structural diversity after 100 years than exploitative or regenerative practices. The presence of drought, windstorm, pest, and disease disturbances altered these outcomes. Regenerative forest management provides 25% higher forest carbon storage and 26% higher tree structural diversity after 100 years than no cutting. Our results demonstrate that wood products and their carbon storage and fossil emission avoidance are important for determining the total climate benefits of forest management under natural disturbances. Our findings highlight that natural disturbance regimes should be considered when selecting management to promote multiple forest benefits, suggesting the need for tailored as opposed to one-size-fits-all policies to sustainably manage temperate forests worldwide.

Liu, Weier (ORCID:0000000265914239)↗
DOE OSTI2024

Soil microbiome feedbacks during disturbance-driven forest ecosystem conversion

Abstract Disturbances cause rapid changes to forests, with different disturbance types and severities creating unique ecosystem trajectories that can impact the underlying soil microbiome. Pile burning—the combustion of logging residue on the forest floor—is a common fuel reduction practice that can have impacts on forest soils analogous to those following high-severity wildfire. Further, pile burning following clear-cut harvesting can create persistent openings dominated by nonwoody plants surrounded by dense regenerating conifer forest. A paired 60-year chronosequence of burn scar openings and surrounding regenerating forest after clear-cut harvesting provides a unique opportunity to assess whether belowground microbial processes mirror aboveground vegetation during disturbance-induced ecosystem shifts. Soil ectomycorrhizal fungal diversity was reduced the first decade after pile burning, which could explain poor tree seedling establishment and subsequent persistence of herbaceous species within the openings. Fine-scale changes in the soil microbiome mirrored aboveground shifts in vegetation, with short-term changes to microbial carbon cycling functions resembling a postfire microbiome (e.g. enrichment of aromatic degradation genes) and respiration in burn scars decoupled from substrate quantity and quality. Broadly, however, soil microbiome composition and function within burn scar soils converged with that of the surrounding regenerating forest six decades after the disturbances, indicating potential microbial resilience that was disconnected from aboveground vegetation shifts. This work begins to unravel the belowground microbial processes that underlie disturbance-induced ecosystem changes, which are increasing in frequency tied to climate change.

Nelson, Amelia R.↗
DOE OSTI2020

A High-Speed High-Power-Density Non-Heavy Rare-Earth Permanent Magnet Traction Motor

There has been a global push for higher torque density and lower cost traction motors. The use of non-heavy rare-earth (non-HRE) permanent magnet materials in traction motors are being investigated for the sustainability, profitability and affordability of electric vehicles and to broaden their adoption. A 20,000-rpm permanent magnet traction motor using non-HRE magnet materials is proposed. A dual three-phase winding configuration driven by a segmented dual three-phase drive is proposed to reduce the current ripple, and as a result, the DC Link capacitor, as well as to ease the voltage constraint at high speed and eliminate any risk of uncontrolled regeneration. Furthermore, the dual winding configuration enables a fault tolerant design which is useful for reliability. The paper presents comprehensive electromagnetic, thermal and mechanical designs and analyses using an integrated approach. The results have shown that the design is robust against demagnetization and confirmed its thermal and mechanical viability.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Inhibition of PTEN activity promotes IB4‐positive sensory neuronal axon growth

Abstract Traumatic nerve injuries have become a common clinical problem, and axon regeneration is a critical process in the successful functional recovery of the injured nervous system. In this study, we found that peripheral axotomy reduces PTEN expression in adult sensory neurons; however, it did not alter the expression level of PTEN in IB4‐positive sensory neurons. Additionally, our results indicate that the artificial inhibition of PTEN markedly promotes adult sensory axon regeneration, including IB4‐positive neuronal axon growth. Thus, our results provide strong evidence that PTEN is a prominent repressor of adult sensory axon regeneration, especially in IB4‐positive neurons.

Zhou, Li‐Yu↗
DOE OSTI2022

Clean Condensing Gas Furnace

Natural gas furnaces are the most common space heating equipment in the U.S. residential and commercial building markets. However, current residential natural gas condensing furnaces generate substantial acidic condensate as well as significant emissions of sulfur oxides (SOx), nitrogen oxides (NOx), carbon monoxide (CO), hydrocarbons (HC), and methane (CH 4 ) contributing to environmental degradation of air, water, and soil. This report describes a novel solution to reduce the environmental impact of natural gas condensing furnaces based on the technology of a monolithic acidic gas reduction (AGR) catalyst for SOx trapping, NOx redox to nitrogen, and oxidation of formic acid, CO, HC, and CH 4 . The AGR technology offers the following benefits: (1) a neutral furnace condensate with a pH of ~7, allowing its safe release into the sewer system thus eliminating a second drainage system; (2) trapping and removing nearly all SOx emissions; (3) NOx emissions nearly at nearly 1-2 ng/J, more than 95% lower than new emissions standards in California; (4) the use of a low-cost heat exchanger as a condensing heat exchanger (HX) since the condensate is not acidic, avoiding the need for expensive stainless steel alloys; and (5) unburnt fuel energy recovery to boost efficiency.The AGR component and AGR-enabled furnace performance were broadly tested to determine their effects on long-term reliability and durability, as well as SOx storage and regeneration activity. The AGR regeneration does not impair the performance in achieving neutral condensate and ultra-low NOx emissions, and the AGR catalyst subjected to regeneration activities continued to function well and achieved slightly better annual fuel utilization efficiency (AFUE). The 400-hour reliability and durability test of the retrofitted condensing furnace with the AGR component shows that the furnace unit still achieves a neutral furnace condensate with a pH of ~7 and enables 0~3 ng/J of NOx emissions. However, the 400-hour operation slightly degraded the AFUE because of soot particle accumulation caused by frequent incomplete combustion owing to inappropriate condensate drainage during testing. Thus, proper condensate drainage is critical for AGR-enabled furnaces. Furthermore, neutron computed tomography was employed to survey the aged AGR component and demonstrate high-resolution 2D and 3D representations for the nondestructive diagnosis of the AGR component. The tomography showed that the AGR component did not deform or suffer broken AGR channels. A new AGR catalyst with low precious metal loading was preliminarily explored to identify a pathway of optimizing AGR material loading and maximizing acidic gas reduction at low cost. The new AGR component can reduce precious metal loading by 38% and still achieve neutral condensate and ultralow NOx emissions. The furnace with the AGR component of low Pt/Rh loading enables a maximum AFUE of 97%, which is meaningfully higher than the original furnace. Long-duration testing for the furnace enabled with the low precious metal loading AGR component will be vital in future research. Although the current work demonstrates a proof of concept for the AGR-enabled furnace, the AGR assembly needs to be optimized and integrated into the design of new OEM furnace products. Furthermore, the AGR technology can be applied not only for residential gas furnaces, but also for commercial rooftop units, gas heat pumps, gas-fired water heaters, combustion boilers, and other systems.

03 NATURAL GAS↗
DOE OSTI2022

Pilot Testing of a Highly Efficient Pre-combustion Sorbent-based Carbon Capture System

TDA developed and demonstrated a highly efficient pre-combustion carbon capture system. The overall objective of this work was to develop a new sorbent-based pre-combustion carbon capture technology for Integrated Gasification Combined Cycle (IGCC) power plants. In this project our goal was to demonstrate the techno-economic viability of the new technology by 1) demonstrating it in large-scale slipstream tests, and 2) carrying out a high fidelity engineering and cost analysis. TDA’s process used an advanced physical adsorbent that selectively removes CO 2 from coal-derived synthesis gas above the dew point of the gas at temperatures as high as 300°C. The sorbent consists of a mesoporous carbon whose surface was grafted with functional groups that remove CO 2 via a well-known acid-base interaction. As documented in bench-scale experiments and field tests with actual coal gas, the sorbent achieved a very high capacity for CO 2 at temperatures as high as 300°C. The sorbent bound CO 2 more strongly than common physical adsorbents, providing the chemical potential needed for the high temperature operation. However, because CO 2 does not form a true covalent bond with the surface sites (as is the case with chemical absorbents), the sorbent regeneration could be carried out with only a very small energy input. The heat input to regenerate our sorbent was only 4.9 kcal per mol of CO 2 , which is much lower than that for chemical absorbents (e.g., 29.9 kcal/mol CO 2 for sodium carbonate) and was similar to the requirements of physical solvents (e.g., 4 kcal/mol CO 2 for Selexol TM ). Because the sorbent operates above the dew point of the synthesis gas (unlike the Selexol TM process), a higher power cycle efficiency can be achieved. With previous DOE/NETL funding (Contract No. DE-FE-0000469), we demonstrated the techno-economic viability of the technology in bench-scale tests and slipstream demonstrations at the National Carbon Capture Center (NCCC), Wilsonville, Alabama and Wabash River IGCC plant in Terra Haute, Indiana. We demonstrated a stable working CO 2 capacity for over 11,650 cycles with simulated synthesis gas. We also evaluated its performance with actual synthesis gas in two test campaigns at the Wabash River IGCC Plant, Terre Haute, IN and the National Carbon Capture Center (NCCC), Wilsonville, AL. The slipstream tests clearly showed that the actual coal gas constituents and potential contaminants (e.g. trace metals, halides, tars) had no effect on the sorbent’s ability to remove CO 2 (the same sorbent beds were used in both field tests with no sign of deactivation for 2,000 cycles with over 26,750 SCF of gas treated). As expected, due to the high temperature CO 2 removal capability and low energy needed to regenerate the sorbent, the power cycle efficiency with our process was greater than 34% on a higher heating value (HHV) basis; in comparison, the same IGCC plant equipped with the Selexol TM solvent for carbon capture can only achieve 31.4% HHV efficiency. The capital cost for an IGCC system with TDA’s process is estimated as $2,417/kW e , which is 12% lower than that of the IGCC/ Selexol TM process. The levelized cost for electricity including the transport, storage and monitoring (TS&M) cost for CO 2 was calculated as $\$ $92.9/MWh (lowest reported to our knowledge), which is much better than the $105.2/MWh estimated for the IGCC/ Selexol TM process. In this project (DE-FE0013105), TDA Research, in collaboration with our partners Gas Technology Institute (GTI), Illinois Clean Coal Institute (ICCI), University of California, Irvine (UCI), University of Alberta (UOA), Siemens, NCCC and Sinopec advanced the technical maturity of the technology; scaling it up by a factor of 100. We optimized the reactor design using computational fluid dynamics (CFD); using adsorption modeling we improved the pressure swing adsorption (PSA) cycle sequence. We carried out two field test campaigns with a fully-equipped 0.1 MW e prototype unit (for a total of 844 hours) using actual synthesis gas to prove the viability of the new technology. A successful 30 day (707 hrs) evaluation was completed at NCCC under air blown gasification conditions. We demonstrated 97.3% carbon capture at 1,500 SLPM, 93% carbon capture at 1,800 SLPM, and 90% carbon capture at 2,100 SLPM in the NCCC tests. We also demonstrated the system for 137 hours at a Sinopec petrochemical plant under oxygen blown gasification, demonstrating 86% carbon capture at 2,660 SLPM. In collaboration with University of California, Irvine (UCI), we completed a techno-economic analysis (TEA) for TDA’s warm gas cleanup technology integrated to IGCC power plant. The net plant efficiencies (on a coal HHV basis) for the warm gas cleanup cases were estimated to be 34.0% for E-GasTM gasifier, 34.4% for GE gasifier, 33.4 for the Shell gasifier and 34.2 for the TRIG TM gasifier (Cases 2, 4, 6 and 8 in this study) with a catalytic combustor for CO 2 purification, which are significantly higher than those for the Cold Gas Case, or an increase of as much as 12% in the heat rate for Case 2, 6% for Case 4, 9% for Case 6, and 9% for Case 8. The 1st year cost of electricity with the transport, storage and monitoring (TS&M) costs for the CO 2 included was $\$ $129.2/MWh for the E-GasTM gasifier Warm Gas Cleanup Case, $\$ $131.9/MWh for the GE gasifier Warm Gas Cleanup Case, $\$ $146.8/MWh for the Shell Gasifier Warm Gas Cleanup Case, and $\$ $129.9/MWh for the TRIG TM gasifier Warm Gas Cleanup Case. For comparison, the costs for the baseline Cold Gas CO 2 removal with Selexol for the different gasifiers were: $\$ $146.6/MWh for the E-Gas TM gasifier, $\$ $142.2/MWh for the GE gasifier, $\$ $159.0/MWh for the Shell gasifier and $\$ $144.3/MWh for the TRIG TM gasifier. In summary, the costs for our system were 7 to 12% lower than the corresponding Cold Gas Cleanup cases. The results of this techno-economic analysis suggested that TDA’s high temperature PSA-based Warm Gas Clean-up Technology can make a substantial improvement in the IGCC plant thermal performance for achieving near zero CO 2 emissions for E-Gas TM , GE, Shell and TRIG TM gasifier based IGCC power plants. The capital expenses were estimated to be lower than that of Selexol’s™. Taken together, the higher net plant efficiency and lower capital and operating costs resulted in substantial reduction in the cost of carbon capture for the IGCC plant equipped with TDA’s high temperature PSA-based carbon capture system. Finally, in collaboration with Gas Technology Institute (GTI) we completed the environmental health and safety assessment for TDA’s warm gas carbon capture technology.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2024

Bench-Scale Development of a Novel Direct Air Capture Technology Using High-Capacity Structured Sorbents

The work performed under this project has resulted into development of a DAC technology utilizing a structured sorbent to capture CO 2 from ambient air with a key innovation of direct Joule heating of the sorbent for CO 2 desorption. A working SMA, fully integrated with an electrically resistive heating layer, high surface area support, and high CO 2 capacity sorbent coated onto a commercial ceramic monolithic substrate, was successfully developed and demonstrated over >200 adsorption-desorption cycles in a high-fidelity bench test unit directly using ambient air. A cordierite-based monolith was selected as a substrate owing to its high surface area, low bulk density, low heat capacity, and commercial availability. Reaction kinetics study conducted during this project led to development of a promoter for the base Na 2 CO 3 sorbent that could be incorporated into the sorbent to enhance to achieve higher CO 2 adsorption/desorption rates, greater working capacity, and reduced regeneration temperature. An accelerated aging study was conducted in a TGA to determine sorbent stability and no degradation in the sorbent performance was observed even after 250 adsorption-desorption cycles. An electrically resistive heating layer was developed with tunable electrical properties. The heating layer was coated onto the selected cordierite substrate. Aging studies performed showed the electrical properties and heating performance was stable after 500 heating and cooling cycles. The collective findings on the selected cordierite substrate, robust heating layer, promoter and sorbent selection were used to synthesize a full, 6”x6” SMA for bench-scale testing. The bench-scale DAC system was constructed to test full size SMAs using real ambient air for adsorption and joule heating for regeneration. After completing shakedown and commissioning of the 1 kg/day of CO 2 capacity DAC bench unit, an extended operation was performed to complete over 230 cycles with the full size SMA. This testing showed no observable degradation in sorbent performance. A detailed process model, TEA and LCA were developed for a conceptual 100,000 TPY CO 2 removal DAC facility. The LCA results show the net CO 2 e emissions from the DAC system are highly dependent on the electricity source. All other factors, including SMA manufacturing, materials for facility enclosure, etc., are minor cost contributors compared to the energy consumption required for CO 2 removal. With the successful development and validation of the SMA for the sustained performance for CO 2 removal from ambient air with joule heated regeneration in this project, a fully integrated 1 TPY bench-scale DAC system is currently in development with the support of DOE/FECM (DE-FE0032243). The project objective is to demonstrate the engineering design of the DAC system to produce a continuous, high purity CO 2 stream from ambient air. This project will address and validate key engineering features of the DAC system including the gas sealing mechanism and panels, enclosure and air contactor design, and automation sequence to achieve continuous CO 2 production.

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DOE OSTI2024

Core-Shell Oxidative Aromatization Catalysts for Single Step Liquefaction of Distributed Shale Gas (Final Technical Report)

The objective of this project was to design and demonstrate a core-shell structured multifunctional catalyst to convert the light (dry) components of shale gas into liquid aromatic compounds (primarily benzene and toluene) in a single step. Operated in a modular oxidative aromatization system (OAS) under a cyclic redox scheme, the novel catalyst and process can significantly improve the value and transportability of distributed shale gas. Since the project started, each quarter addressed a different set of tasks related to the completion of the milestone detailed in the project award. The yearly summaries of these tasks are summarized below: Q1-Q4: • Conducted project planning and literature search. • Investigated a number of SHC redox catalysts using thermogravimetric analysis and fixed-bed reactor experiments. • Initiated process modeling towards generating two process models for the methane DHA base case and OAS process. • Developed DHA catalysts capable of producing >500 g/kg-cat-hr aromatics at 80% or greater aromatics selectivity at 700°C. Q5-Q8: • Developed alternative approaches with sequential bed configurations to enhance the aromatic yields based on OCM+DHA • Improved the zeolite synthesis efficiency by using the microwave-assisted technique and investigated the synthesis conditions on the zeolite yield, crystalline structure and morphology • Constructed a set of Aspen Plus process models with significant energy savings for OAS as compared to the base case non-oxidative DHA. • Adapted conventional hydrothermal method to be applicable to the microwave synthesizer unit for more efficient catalyst synthesis. • Studied the structure of the OCM catalyst and the dispersion of the carbonate in the redox reactions and in methane flow with Raman Spectroscopy. Q9-Q12: • Scaled up the catalyst synthesis with the microwave synthesis method. Based on its performance, procedural characterizations and catalytic performance testing were further conducted for the new microwave synthesized catalysts with the newly-developed product analysis procedure. • Developed the reaction system setup for the C2-DHA or OCM+DHA reaction product and achieved a better product collection-analysis method for the aromatic products with an improved carbon balance. The product from the OCM reaction exhibited complicated effects on the DHA catalyst. • Conducted additional OCM catalyst characterization using Near Ambient Pressure X-ray Photoelectron Spectroscopy and in situ Raman characterization • Validated the significant energy savings for OAS as compared to the base case non-oxidative DHA. Successfully set up the simulation model for the OCM+DHA+SHC reaction system based on the updated experimental results from NCSU. Q13-End of project: • Synthesized new zeolite catalysts by the microwave method, conducted characterizations (XRD, SEM, and TEM) and catalytic behavior testing. • Explored the “wet” C 2 H 6 and C 2 H 4 DHA reactions with using steam co-feed. A subsequent reduction as the regeneration step can regenerate the DHA catalyst and recover 99% activity of the fresh performance. • Achieved a 15.3% single-pass aromatic yield from methane by rationally combining the OCM and DHA at different temperatures. • Conducted a 105-hour stability test with an improved regeneration procedure, with an average aromatic yield of 13.8%. • Developed new catalyst and achieved a record-high 23.2% yield.

03 NATURAL GAS↗