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At least 307 records · Page 17

High Energy Systems for Transforming CO 2 to Valuable Products (Final Report)

The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process that uses high-energy electron beams (E-Beam) to break chemical bonds. This allows the production of valuable chemicals, such as acetic acid, methanol, and carbon monoxide, at relatively low severity (pressure near one atmosphere and temperatures <150°C) from near-pure CO 2 captured from a pulverized coal-fired power plant and methane, imported as natural gas. Creating such valuable products will offset the cost of carbon capture and storage. Through this project, we have designed, constructed, and operated an E-Beam reactor to examine the feasibility of performing dry reforming reaction without a catalyst using only DEBS. We have verified the production of syngas with 1:1 H2:CO ratio and calculated that the energy cost for conversion is about 5.2 eV/molecule of product for dry reforming reaction which is similar to the energy cost for conversion using conventional thermochemical conversion but under significantly milder conditions (room temperature and atmospheric pressure). We have performed a technoeconomic analysis (TEA) to estimate the total capital requirement and the cost of production for a 99.4 MMSCFD syngas production plant via non-catalytic Direct E-Beam Synthesis (DEBS) technology utilizing a high-energy electron beam (E-Beam) accelerator. No assumption is made for syngas utilization downstream, and the incoming reactants are pure CO 2 from carbon capture (assumed to be at zero cost) and natural gas. The Total As-Spent Cost (TASC) was calculated to be $\$242.5$ million, resulting in a levelized cost of syngas (LCOS) of $\$175.84$/tonne (metric) at a natural gas price of $\$6.24$/MMBTU1. The cost of syngas is primarily determined by the price of natural gas. If the cost of the CO 2 feedstock is assumed to be non-zero, then the price of the CO 2 feed also heavily influences the levelized cost of syngas. The potential impact on the cost of electricity from syngas revenue is significant. Following DOE NETL’s guidance, a lifecycle analysis (LCA) was conducted to compare the cradle-to-gate life cycle emissions of GTI Energy’s novel Direct E-Beam Synthesis (DEBS) process that produces syngas via the reaction of methane and carbon dioxide to the emissions of a state-of-the-art Steam Methane Reforming (SMR) process that also produces syngas via the reaction of methane and steam. The DEBS process results in less GHG emissions than SMR (with CO product as the basis of comparison). openLCA was used for the LCA and the results show that the total global warming potential (GWP) of DEBS is 0.981 kg CO 2 e per kg CO product, while the SMR process has a global warming potential of 2.573 kg CO 2 e per kg CO product. The ratio of the GWP of the proposed product system to the comparison product system is 0.381. This percent change is 61.9% lower GWP than SMR.

20 FOSSIL-FUELED POWER PLANTS↗

Hybrid biophysical systems for atmospheric CO 2 capture

Negative emissions technologies will be essential for limiting anthropogenic global temperature increases to 2 °C in the later years of the 21st century. Carbonic anhydrase (CA) metalloenzymes catalyze the otherwise slow conversion of CO 2 into carbonic acid (H 2 CO 3 ), suggesting their utility in the rapid hydration and downstream capture of dissolved CO 2 in aqueous media for a variety of CO 2 capture methods, such as thermal and pH swings and mineralization. The possibility of driving the rapid capture of CO 2 by catalyzing the CO 2 hydration bottleneck carries real potential for realizing efficient direct air capture (DAC) and direct ocean capture (DOC) systems. However, scaled application of CAs will be dependent on some way of economically sourcing the enzymes at volumes relevant to scaled DAC/DOC operations. In this perspective, we consider the prospect of catalyzing CO 2 hydration using a CA that is bound to the outer membrane of a cyanobacterial host, engineered constructs we call CyCAMs. Coupling extracellular CA expression to a marine, photosynthetic cyanobacterial host results in a CO 2 hydration catalyst that is continuously refreshed during the bacterial growth cycle, without the need for enzyme purification or harvesting steps. In the case of marine cyanobacteria, sunlight and the solutes native to seawater provide the respective energy, nutrients and sources of inorganic carbon essential to maintaining the bacterial population. We consider the potential impact of CA-mediated CO 2 hydration on a variety of DAC processes, with CO 2 mineralization explored as a primary use case.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Summary Report of the Reactive CO 2 Capture: Process Integration for the New Carbon Economy Workshop, February 18-19, 2020

This report provides a summary of feedback from the “Reactive CO 2 Capture: Process Integration for the New Carbon Economy” workshop held February 18-19, 2020. The focus of this workshop was to discuss approaches for merging carbon dioxide (CO 2 ) capture and CO 2 conversion/utilization systems into an integrated "reactive capture" strategy. By the workshop’s definition, reactive capture (RC) of CO 2 is the coupled process of capturing CO 2 from a mixed gas stream and converting it into a valuable product without going through a purified CO 2 intermediate. Participants were able to identify four key themes and associated calls to action for the reactive capture community: (1) essential role of partnerships; (2) critical challenges; (3) defining the value proposition; and (4) approach to support technological advancement.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

Multi-Scale Seismic Measurements for Site Characterization and CO2 Monitoring in an Enhanced Oil Recovery/Carbon Capture, Utilization, and Sequestration Project, Farnsworth Field, Texas

To address the challenges of climate change, significantly more geologic carbon sequestration projects are beginning. The characterization of the subsurface and the migration of the plume of supercritical carbon dioxide are two elements of carbon sequestration that can be addressed through the use of the available seismic methods in the oil and gas industry. In an enhanced oil recovery site in Farnsworth, TX, we employed three separate seismic techniques. The three-dimensional (3D) surface seismic survey required significant planning, design, and processing, but produces both a better understanding of the subsurface structure and a three-dimensional velocity model, which is essential for the second technique, a timelapse vertical seismic profile, and the third technique, cross-well seismic tomography. The timelapse 3D Vertical Seismic Profile (3D VSP) revealed both significant changes in the reservoir between the second and third surveys and geo-bodies that may represent the extent of the underground carbon dioxide. The asymmetry of the primary geo-body may indicate the preferential migration of the carbon dioxide. The third technique, cross-well seismic tomography, suggested a strong correlation between the well logs and the tomographic velocities, but did not observe changes in the injection interval.

Energy & Fuels↗

Insights from FEED studies for retrofitting existing fossil power plants with carbon capture technology

Recent United States Department of Energy (DOE) sponsored front-end engineering design (FEED) studies for retrofitting existing fossil-fueled power plants with state-of-the-art carbon capture technology contain previously overlooked real-world design considerations for near-term deployment of carbon capture. Insights from examining seven recently published FEED study reports are summarized in this paper. This includes a discussion of the design, performance, and cost implications associated with (1) location-specific considerations such as water availability, land availability, and accessibility; (2) host-plant-specific factors such as flue gas specifications, allowable degree of integration between the capture system and host plant, and operational mode; and (3) miscellaneous factors such as market conditions, permitting requirements, and business case incentives. In conclusion, this manuscript highlights (1) water availability as a key design and cost driver, with host plant steam extraction increasing capture system cooling water availability, (2) modularization and constructability impacts on the number of capture trains, (3) the impacts of host plant operational mode and capacity factor on the business case for installing capture, and (4) the merit of continued research, development, and demonstration efforts addressing steam extraction, host plant tie-in at the stack, solvent reclamation and air emissions control.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Increasing CO 2 Capture Rate in Liquid-Solvent Direct-Air Carbon Capture via Additive Manufacturing

Carbon capture is essential to meeting climate change mitigation goals. One approach currently being commercialized utilizes liquid-based solvents to capture CO 2 directly from the atmosphere but is limited by slow absorption of CO 2 into the liquid. Improved air/solvent liquid mixing increases CO 2 absorption rate, and this increased CO 2 absorption efficiency allows for smaller carbon capture systems with lower capital costs and better economic viability. In this project, we study the use of passive micromixers fabricated by metal additive manufacturing. The micromixer’s small-scale surface geometric features perturb and mix the liquid film to enhance mass transfer and CO 2 absorption. In this project, we evaluated this hypothesis through computational and experimental studies. Computational investigations focused on developing capabilities to simulate thin film (~ 100μm) fluid flow on rough surfaces. Such thin films are in a surface-tension dominated regime and simulations in this regime are prone to instabilities. Improvements to the Nalu code completed in this project resulted in a 10x timestep stability improvement for these problems.

36 MATERIALS SCIENCE↗

Intensified Catalytic Conversion of CO2 into High Value Chemicals

The utilization of CO2 produced from power generation plants as a feedstock for creating new valuable products offers a strategy to reduce GHG emissions, offset carbon capture costs, and facilitate the rebalancing of the carbon cycle. After considering the thermodynamic requirement of potential products from CO2 utilization and their market size, formic acid is a desirable target that offers widespread utility in industrial chemical production and chemical energy storage as a liquid fuel. To effectively utilize CO2 from power generation plants, UK proposes an enhanced bimetallic oxide carbon utilization process (EBOCU) that enables electrochemical CO2 conversion to formic acid. The UK intensified electrocatalytic process combines three main components: 1) a novel bimetallic oxide electrocatalyst; 2) a stable electrochemical reactor using robust electrodes; and 3) a pressurized electrochemical reactor. The output from this project showed the economic viability of producing high-value formic acid from CO2 to both offset the cost associated with post-combustion CCS and reduce GHG emissions. This project developed and screened a series engineered catalysts to selectively reduce CO2 directly to formic acid. The best performing catalyst based on formic acid production, stability, and Faradaic efficiency, was immobilized on carbon electrodes, and tested inside a flow through reactor. After lab-scale testing was completed, the experimental data was used to perform a Life-Cycle Analysis (LCA) and conduct an Initial Technical and Economic Feasibility Study. The LCA showed a pathway to a net negative CO2 utilization process with the incorporation of renewable energy, while the TEA showed the potential to produce formic acid below the current commercial price. The UK EBOCU process was successfully demonstrated at the TRL3 level and has a clear pathway to further development and contribution to the nation’s ambitious decarbonization goals.

20 FOSSIL-FUELED POWER PLANTS↗

An experimental and modeling study of the application of membrane contactor reactors to methanol synthesis using pure CO 2 feeds

We describe here a post-combustion CO 2 capture and utilization (CCU) technology that converts the CO 2 into methanol (MeOH), a valuable chemical, thus providing a way to monetize the carbon captured to offset process costs. Methanol synthesis (MeS) has been discussed recently for application to CCU, but thermodynamic limitations make it difficult to convert in a single pass a large CO 2 fraction. Conventional catalysts show slow kinetics in converting CO 2 -rich syngas (or pure CO 2 ) into MeOH. Our Group developed a novel MeS process, employing a membrane contactor reactor (MCR) system that attains carbon conversions significantly higher than equilibrium. Our focus here is to process pure CO 2 streams by combining the MCR with a separate reactor, which converts the CO 2 into a syngas via the reverse water gas shift (RWGS) reaction. In this preliminary effort, the RWGS reactor (RWGSR) is assumed to reach equilibrium. Additional MeS kinetic rate data are generated validating experimentally the ability of the MeS-MCR to process as a feed the RWGSR exit stream. The performance of the combined (RWGSR/MeS-MCR) system is then simulated using a recently developed MeS-MCR model. In conclusion, the findings are encouraging, and research is currently ongoing to experimentally validate the RWGSR/MeS-MCR system performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Atmospheric Capture On Mars (and Processing)

The ultimate destination of NASA's human exploration program is Mars. In Situ Resource Utilization (ISRU) is a key technology required to enable such missions, as first proposed by Prof. Robert Ash in 1976. This presentation will review progress in the systems required to produce rocket propellant, oxygen, and other consumables on Mars using the carbon dioxide atmosphere and other potential resources. For many years, NASA, commercial companies, and academia have been developing, and demonstrating techniques to capture and purify Martian atmospheric gases for their utilization for the production of hydrocarbons, oxygen, and water in ISRU systems. Other gases will be required to be separated from Martian atmospheric gases to provide pure CO2 for processing elements. Significant progress has been demonstrated in CO2 collection via adsorption by molecular sieves, freezing, and direct compression. Early stage work in adsorption in Ionic Liquids followed by electrolysis to oxygen is also underway. In addition, other Martian gases, such as nitrogen and argon, occur in concentrations high enough to be useful as buffer gas and could be captured as well. Gas separation requirements include, but are not limited to the selective separation of: (1) methane and water from unreacted carbon oxides (CO2-CO) and hydrogen typical of a Sabatier-type process, (2) carbon oxides and water from unreacted hydrogen from a Reverse Water-Gas Shift process, and (3) carbon oxides from oxygen from a trash/waste processing reaction.

propellant production↗

Techno-economic performances and life cycle greenhouse gas emissions of various ammonia production pathways including conventional, carbon-capturing, nuclear-powered, and renewable production

Ammonia (NH 3 ) is conventionally produced using fossil natural gas (NG) for hydrogen production through steam reformation and synthesis in the Haber–Bosch (HB) process. The global conventional ammonia production contributes more than 420 million tons of CO 2 emissions annually. Here, in this work, we investigated the techno-economics and well-to-plant-gate (WTG) greenhouse gas (GHG) emissions of conventional NG-based, carbon-capturing, nuclear-powered, and renewable ammonia production by developing an engineering process model for each. Carbon-capturing ammonia production refers to the NG-based ammonia production while capturing CO 2 and transporting it via pipelines for storage or utilization. Nuclear-powered and renewable ammonia production represents an alternative ammonia production through water electrolysis, air separation, and the HB process using carbon-free energy sources. Nuclear and renewable energy sources are assumed to be used for nuclear-powered and renewable ammonia production, respectively. Sensitivity analyses are performed for CO 2 pipeline transport distances, potential carbon capture tax credits, and clean H 2 production cost. Carbon-capturing ammonia production reduces WTG GHG emissions by 55–70% compared to conventional NG-based ammonia production methods. Nuclear-powered and renewable ammonia production almost eliminate GHG emissions since energy supply is either zero carbon or near-zero carbon. However, when $4.16–4.83 per kg is the cost assumed for clean H 2 production using state-of-the-art electrolysis technologies, the levelized costs of nuclear-powered and renewable ammonia are calculated to be $0.92–1.06 per kg NH 3 , which are approximately four times higher than the conventional NG-based ammonia production cost. The cost of CO 2 emission avoidance is estimated in the range of $266–318 per metric ton of CO 2 for nuclear-powered and renewable ammonia production. The clean H 2 production cost is the major contributor to the levelized costs of nuclear-powered and renewable ammonia production. A lower production cost, near $1 per kg H 2 , for clean H 2 is required for nuclear-powered and renewable ammonia production to be cost-competitive with conventional NG-based ammonia production.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Method for direct conversion of carbon dioxide to dialkyl carbonates using ethylene oxide as feedstock

A method for co-production of high purity dimethyl carbonate and mono-ethylene glycol by applying a reactor, such as a membrane reactor and/or an adsorbent-catalytic reactor by capturing and reacting carbon dioxide with methanol and ethylene oxide. Carbon dioxide may be recovered from primary sources (utilities and industrial processes) by a membrane or solid adsorbent, and subsequently converted to an intermediate hydroxy-ethyl-methyl carbonate by reacting with ethylene oxide and methanol. For high-purity carbon dioxide (obtained by carbon capture technologies or from an ethanol fermentation process), the membrane reactor is replaced with a catalytic reactor for direct conversion of carbon dioxide to hydroxy-ethyl-methyl carbonate by reacting with ethylene oxide and methanol. The hydro-ethyl-methyl carbonate is further reacted with methanol for conversion to dimethyl carbonate. A combination of heterogeneous and homogeneous catalysts is implemented for an effective conversion of carbon dioxide. An integrated reactive distillation process using side reactors is used for facilitating catalytic reaction for production of high purity dimethyl carbonate.

Panchal, Chandrakant B.↗

Integrated CO 2 capture and hydrogenation in presence of Ru–Na 2 ZrO 3 : An in-situ study

Integrated CO 2 capture and conversion (ICCC) by hydrogenation is a promising strategy to utilize carbon dioxide and this work add to the effort to elucidate the catalytic hydrogenation mechanism using Ru based dual functional materials (DFM). Ru-Na 2 ZrO 3 DFMs, obtained through different wet methods, were evaluated for the first time and the relationship between Ru and support systematically investigated. The thermally stable and cyclable Ru-Na 2 ZrO 3 -a (obtained without filtration step) exhibited CO 2 conversion of 80% and a higher yield of CO at 400°C compared to previously tested DFM, while the Na depleted/Zr rich Ru-Na 2 ZrO 3 -b resulted in 90% selectivity to CH 4 with yield of 1.11 mmol/g at the same temperature. The in-situ experiments have provided conclusive evidence showing that CO 2 hydrogenation on the two Ru DFMs is fundamentally different. In Ru-Na 2 ZrO 3 -a, the monoclinic Na 2 ZrO 3 support acted as the active centre (not as promoter) for CO 2 bridging binding and hydrogenation to CH 4 at the metal-support interface through associative formate pathway with limited further reduction to methane due to lack of H 2 spillover from the small and well dispersed Ru NPs, which results in CO desorption. Conversely, abundant clusters of larger Ru NPs in Ru-Na 2 ZrO 3 -b, led to CH 4 production due to co-existent Ru on-top direct dissociation of CO 2 (preferential) and monodentate formate adsorption and further methanation. Alkali zirconates doped metals, and their synthesis method could thus play a crucial role in designing tuneable heterogeneous catalysis in C 1 chemistry, which could significantly benefit the environment by lowering CO 2 levels, encouraging cleaner industrial practices, supporting a circular economy, and converting waste CO 2 into valuable products.

36 MATERIALS SCIENCE↗

Development of a framework for sequential Bayesian design of experiments: Application to a pilot-scale solvent-based CO 2 capture process

In this paper, a methodology is developed for sequential design of experiments (SDoE) for process systems and applied to a solvent-based CO 2 capture system. In this approach, the prior knowledge of the system is used to prioritize process data collection at specific operating conditions. These data are then incorporated into a Bayesian inference methodology for updating a stochastic model by refining estimations of its underlying parameters, and the updated model is then used to generate the next set of test runs. Thus, the new knowledge obtained from the data is used to guide subsequent iterations of the experimental runs, ensuring that the overall data collection is maximally informative given that most experimental campaigns, especially at pilot or higher-scale plants, are costly, time-consuming, and resource-limited. The test run objective for this work was to minimize the maximum model prediction uncertainty for key output variables, but the methodology is generic and can be readily applied to other test run objectives. This methodology is applied to an aqueous monoethanolamine (MEA) pilot plant campaign at the National Carbon Capture Center (NCCC) in Wilsonville, Alabama, USA. The SDoE framework was utilized for two iterations, while collecting 18 sets of data representing different process conditions, and this resulted in an overall average reduction in uncertainty of approximately 50% in the prediction of CO 2 capture percentage. Moreover, 11 additional data sets were obtained with variation of absorber packing height for further model validation. This work shows the capability of the SDoE framework to maximize learning given limited resources, allowing for the reduction of model uncertainty, which is of great importance for many applications including reduction of technical risk associated with scale-up and economic analysis.

20 FOSSIL-FUELED POWER PLANTS↗

CCUS Perspectives: Assessing Historical Contexts, Current Realities, and Future Prospects

CCUS technologies are crucial solutions for mitigating climate change by reducing CO2 emissions from industrial operations and energy sectors. This review critically examines the current state of CCUS technologies, and highlights advancements, challenges, regulatory frameworks, and future directions. It comprehensively analyzes carbon capture methods, such as pre-combustion, post-combustion, and oxy-fuel combustion capture, while comparing their efficiencies and limitations. The review also explores carbon utilization techniques, such as direct and indirect utilization, emphasizing their potential applications and technological constraints. Additionally, it assesses various carbon storage methods, focusing on geological, ocean, and mineralization storage, and discusses their capacity, feasibility, and environmental implications. The study reviews the policy and regulatory frameworks, economic viability, market trends, and environmental sustainability of CCUS. By identifying research gaps and recommending future research priorities, this review aims to guide the development of more efficient/effective, and cost-effective CCUS technology, ensuring their role in a sustaining low-carbon future. This review provides a forward-looking perspective, a critical and interdisciplinary analysis that assesses the current state of CCUS technologies, and further provides a roadmap for future development.

Energy & Fuels↗

Development of a kinetic model to describe six types of symbiotic interactions in a formate utilizing microalgae-bacteria cultivation system

This study investigated an algae/formate-utilizing-bacteria system that has been developed for carbon capture. This photomixotrophic consortium consumed formate to support bacterial growth so that the resulting respiration CO 2 could be simultaneously used by algae to avoid CO 2 gas-lipid mass transfer limitation. To understand biomass growth and population interactions in this unique system, a kinetic model has been developed to describe algae and bacteria multiplication, formate and nitrogen utilizations, CO 2 mass transfer, O 2 generation and consumption, lighting condition and shading effect. The simulation indicated that this ecosystem could form six types of interactions (mutualism, commensalism, parasitism, neutralism, amensalism, and competition) depending on the light intensity and nutrient availability. Furthermore, the simulation of both batch culture and chemostat, along with parameter sensitivity tests and experimental observations, offered insights into optimal applications of algae-bacteria consortium based photobiorefinery.

59 BASIC BIOLOGICAL SCIENCES↗

FWP FEW0223: "Advanced Manufactured Carbonate Materials for Algal Biomass Production: Joint LLNL SNL Program" (Final Report)

The ability to easily and cheaply transport carbon dioxide (CO 2 ) from coal-fired power plants equipped with capture facilities to multiple, potentially distant utilization sites of widely varying scales will enable wider use of CO 2 captured from flue gas. In the case of algal biomass cultivation, delivery of CO 2 in the form of carbonate-based materials may provide a more efficient and economical method of inorganic carbon delivery than CO 2 sparging, reducing the cost of algae cultivation and increasing the value of carbon capture. Lawrence Livermore National Laboratory (LLNL) has developed advanced manufactured materials that are well-suited for carbon capture, storage, transport, and delivery. These materials consist of aqueous sodium carbonate, which captures CO 2 as sodium bicarbonate, extruded or 3D printed in a CO 2 permeable polymer to increase the surface area and improve capture kinetics. By encapsulating carbonate solutions, LLNL has demonstrated order-of-magnitude enhancements in carbon capture rates compared with liquid carbonates, enabling the use of these (otherwise kinetically-limited) inexpensive, environmentally-benign solvents for carbon capture.

20 FOSSIL-FUELED POWER PLANTS↗