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Presentation at the 2022 University Turbine Systems Research (UTSR) and Advanced Turbines Program Review Meeting in San Diego, CA, September 27 - 29, 2022.
For presentation at the 2023 FECM/NETL Carbon Management Research Project Review Meeting, Pittsburgh, PA, August 28-September 1, 2023.
Accurate global measurement of carbon dioxide column with the aim of discovering and quantifying unknown sources and sinks has been a high priority for the last decade. In order to uncover the "missing sink" that is responsible for the large discrepancies in the budget the critical precision for a measurement from space needs to be on the order of 1 ppm. To better understand the CO2 budget and to evaluate its impact on global warming the National Research Council (NRC) in its recent decadal survey report (NACP) to NASA recommended a laser based total CO2 mapping mission in the near future. That's the goal of Active Sensing of CO2 Emissions over Nights, Days, and Seasons (ASCENDS) mission - to significantly enhance the understanding of the role of CO2 in the global carbon cycle. Our current goal is to develop an ultra precise, inexpensive new lidar system for column measurements of CO2 changes in the lower atmosphere that uses a Fabry-Perot interferometer based system as the detector portion of the instrument and replaces the narrow band laser commonly used in lidars with a high power broadband source. This approach reduces the number of individual lasers used in the system and considerably reduces the risk of failure. It also tremendously reduces the requirement for wavelength stability in the source putting this responsibility instead on the Fabry- Perot subsystem.
Overview presentation given at the 2024 FECM / NETL Carbon Management Research Project Review Meeting on NETL's Bipartisan Infrastructure Law-funded Smart CO2 Transport-Route Planning Tool and associated geodatabase. This machine learning informed, data-driven public resource was designed to inform regulators, industry, and researchers plan and develop safe and efficient transport routes across the country.
This final technical report describes work conducted by Membrane Technology and Research, Inc. (MTR) for the U.S. Department of Energy (DOE), National Energy Technology Lab (NETL) on the scale-up and testing of advanced Polaris™ membrane CO2 capture technology at the Technology Centre Mongstad (TCM) under award number DE-FE0031591. The work was performed from August 1, 2018 through January 31, 2023. The overall goal of this project was to design, build and operate an advanced Polaris membrane CO2 capture system at TCM. MTR was assisted in this project by Trimeric Corporation (Trimeric), an engineering design services company, the Carbon Capture Simulation for Industry Impact (CCSI2), a partnership among national laboratories, industry, and academic institutions, and the Technology Centre Mongstad (TCM), who provided the host site for the slipstream field test. This report details the work conducted to scale-up MTR’s second-generation (Gen-2) Polaris membrane and advanced planar membrane modules to a final form factor optimized for commercial use; validate their performance in an engineering-scale field test at TCM; and to show the potential of the MTR process to meet DOE CO2 capture targets from large source point emitters. Work for this project included membrane optimization and scale-up, advanced planar module design and fabrication, design and fabrication of an engineering-scale field test membrane skid, operation of the field test skid processing Residue Fluid Catalytic Cracker (RFCC) industrial flue gas at TCM, and a detailed techno-economic analysis (TEA) of the MTR membrane post-combustion process for CO2 capture. This project validated recent membrane technology advancements at the engineering-scale, moves the MTR advanced post-combustion capture technology to TRL-6, and mitigates risk in future Large Pilot or Demonstration scale-up activities.
A literature survey was conducted to assess if published data (evidence) could help inform a space suit carbon dioxide (CO2) limit. The search identified more than 120 documents about human interaction with elevated CO2. Until now, the guiding philosophy has been to drive space suit CO2 as low as reasonably achievable. NASA’s EVA Office requested an evidencebased approach to support a new generation of exploration-class extravehicular activity (EVA) space suits. Specific literature data about CO2 are not available for EVA in microgravity because EVA is an operational activity and not a research platform. However, enough data from groundbased research are available to facilitate a consensus of expert opinion on space suit CO2 limits. The compilation of data in this report can answer many but not all concerns about the consequences of hypercapnic exercise in a space suit. Inspired partial pressure of CO2 (PICO2) and not dry-gas partial pressure of CO2 (PCO2) is the appropriate metric for hypercapnic dose to establish space suit CO2 limits. The reduction of inspired gas partial pressures by saturation of the inspired gases with water vapor at 37°C is a significant factor under conditions of hypobaric space suit operation. Otherwise healthy EVA astronauts will exhibit wide variability in responses to acute hypercapnia while at rest and during exercise. What is clear from the literature is the absence of prospective (objective) accept or reject criteria for CO2 exposure in general, and no such criteria exist for operating a space suit. There is no absolute “Gold Standard” for an acceptable acute hypercapnic limit, just a gradual decrease in performance as CO2 increases. Acceptable CO2 exposure limits are occupation, situation (learned or novel tasks), and personspecific. Investigators who measured hypercapnic physiology rarely correlated those changes to neurocognitive symptoms, and those that measured hypercapnic neurocognition rarely correlated those changes with physiology. Some answers about changes in neurocognition and functional EVA performance during hypercapnic exercise in a space suit await new research.
The presentation provides details on the research work done by the CCSI2 team on techno-economic modeling and optimization of an MEA solvent-based carbon capture system connected to a large scale NGCC power plant, at high CO2 capture levels above 90%. This includes an overview of the process and economic models along with the optimization results.
Carbon capture and storage has been a research area of great interest in recent years asa method for mitigation of CO2emissions, due to the effects of climate change. The development of technologies for the efficient capture of CO2are also of great interest for human spaceflight applications. One of the most promising technologies in this area is CO2 scrubbing using liquid amines, unfortunately, liquid amines with low heats of desorption tend to have slow CO2binding kinetics. One potential solution to this problem is to use the enzyme carbonic anhydrase (CA) to enhance the kinetics of CO2binding to liquid amines, allowing the overall process to be more energy efficient. Interest in using carbonic anhydrase as a biocatalyst has led to a number of efforts to improve the thermostability and solvent tolerance of several distinct carbonic anhydrase enzymes. In the work described here, we screened through a diverse set of natural carbonic anhydrases to identify candidates for protein engineering aimed at increased stability and activity in various liquid amines. We then used SCHEMA structure-guided recombination to develop a set of chimeric carbonic anhydrases with high thermostability and activity. These chimeras were used as the starting points for further protein engineering work targeting activity in liquid amine systems. Our ultimate goal is to test the engineered enzymes in a liquid amine system for cabin air revitalization on ISS or other spacecraft.
In order to better understand the budget of carbon dioxide in the Earth's atmosphere it is necessary to develop a global high precision understanding of the carbon dioxide column. In order to uncover the 'missing sink that is responsible for the large discrepancies in the budget as we presently understand it calculation has indicated that measurement accuracy on the order of 1 ppm is necessary. Because typical column average CO2 has now reached 380 ppm this represents a precision on the order of .25% for these column measurements. No species has ever been measured from space at such a precision. In recognition of the importance of understanding the CO2 budget in order to evaluate its impact on global warming the National Research Council in its decadal survey report to NASA recommended planning for a laser based total CO2 mapping mission in the near future. The extreme measurement accuracy requirements on this mission places very strong requirements on the laser system used for the measurement. This work presents an analysis of the characteristics necessary in a laser system used to make this measurement. Consideration is given to the temperature dependence, pressure broadening, and pressure shift of the CO2 lines themselves and how these impact the laser system characteristics Several systems for meeting these requirements that are under investigation at various institutions in the US as well as Europe will be discussed.
In order to better understand the budget of carbon dioxide in the Earth's atmosphere it is necessary to develop a global high precision understanding of the carbon dioxide column. In order to uncover the 'missing sink" that is responsible for the large discrepancies in the budget as we presently understand it calculation has indicated that measurement accuracy on the order of 1 ppm is necessary. Because typical column average CO2 has now reached 380 ppm this represents a precision on the order of .25% for these column measurements. No species has ever been measured from space at such a precision. In recognition of the importance of understanding the CO2 budget in order to evaluate its impact on global warming the National Research Council in its decadal survey report to NASA recommended planning for a laser based total CO2 mapping mission in the near future. The extreme measurement accuracy requirements on this mission places very strong requirements on the laser system used for the measurement. This work presents an overview of the characteristics necessary in a laser system used to make this measurement. Consideration is given to the temperature dependence, pressure broadening, and pressure shift of the CO2 lines themselves and how these impact the laser system characteristics We have been examining the possibility of making precise measurements of atmospheric carbon dioxide using broad band source of radiation. This means that many of the difficulties in wavelength control can be treated in the detector portion of the system rather than the laser source. It also greatly reduces the number of individual lasers required to make a measurement. Simplifications such as these are extremely desirable for systems designed to operate from space.
A. CO2 - Acute: Given the history of uneven removal of CO2 from spacecraft areas, there is a history of acute illness that impacts short-term health and performance. 1) Acute CO2 symptoms occur in space flight due to a combination of CO2 scrubbing limitations, microgravity-related lack of convection, and possibly interaction with microgravity-related physiological changes. 2) Reported symptoms mainly include headaches, malaise, and lethargy. Symptoms are treatable with analgesics, rest, temporarily increasing scrubbing capability, and breathing oxygen. This does not treat the underlying pathology. 3)ld prevent occurrence of symptoms. B. CO2 - Chronic: Given prolonged exposure to elevated CO2 levels, there is a history that the long-term health of the crew is impacted. 1) Chronic CO2 exposures occur in space flight due to a combination of CO2 scrubbing limitations and microgravity-related lack of convection, with possible contribution from microgravity-related physiological changes. 2) Since acute symptoms are experienced at levels significantly lower than expected, there are unidentified long-term effects from prolonged exposure to elevated CO2 levels on orbit. There have been long term effects seen terrestrially and research needed to further elucidate long term effects on orbit. 3) Recommended disposition: Research required to further elucidate long term effects. In particular, elucidation of the role of elevated CO2 on various levels of CO2 vasodilatation of intracranial blood vessels and its potential contribution to elevation of intracranial pressure.
Estimates show that 6.2 gigatons of carbon dioxide (CO2) can be captured and utilized across three pathways, concrete, chemical, and minerals, by 2050. However, it is difficult to compare the climate benefit across these three carbon capture and utilization (CCU) pathways to determine the most effective use of captured CO2. The life cycle assessment methods to evaluate the climate benefit of CCU chemicals should additionally account for the change in material properties of concrete due to CO2 utilization. Furthermore, with most CO2 utilization technologies being in the early stages of research and development, the uncertainty and variability in process and inventory data present a significant challenge in evaluating the climate benefit. We present a stochastically determined climate return on investment (ROI) metric to rank and prioritize CO2 utilization across 20 concrete, chemical and mineral pathways based on the realized climate benefit. We show that two concrete pathways, which use CO2 during concrete mixing, and two chemical pathways, which produce formic acid through hydrogenation of CO2 and carbon monoxide through dry reforming of methane, generate the greatest climate ROI and are the only CCU pathways with a higher likelihood of generating a climate benefit than a climate burden.
Capturing and converting CO2 generated from bioethanol facilities into valuable products, leveraging renewable electricity as the primary energy input, could increase overall biorefinery carbon utilization by as much as 40% and provide a means to decarbonize fuels and chemicals production. However, significant uncertainty exists around the costs, carbon intensity, risks, and technical challenges associated with electron-driven CO2 reduction. Thus, the overarching objective of this project is to guide existing and future research and development efforts by addressing these knowledge gaps for utilizing renewable electricity and CO2 to improve biorefinery economics and carbon utilization. By September 2023, this project will develop and publish a comprehensive design report for the integration of CO2 utilization into two existing conceptual biorefinery designs, which will include conceptual process models, pioneer and nth plant economics, identification and quantification of technological risks, and projections for future cost reductions.
Hydrogen is essential in the transition to sustainable energy, and developing low-carbon production methods is a key research focus. Traditional steam methane reforming (SMR) dominates the hydrogen industry but contributes substantially to CO2 emissions. In response, Gas Switching Reforming (GSR) has emerged as a novel process that integrates carbon capture and utilizes process heat more efficiently. Unlike other reforming methods, GSR consolidates oxidation and reduction reactions within a single reactor, which minimizes external energy inputs and simplifies scaling. Like conventional steam methane reforming (SMR), GSR can be integrated with water-gas shift and pressure swing adsorption units for pure hydrogen production. This work presents a comprehensive business case analysis of GSR technology based on experimental results in Technology Readiness Level 3, Life Cycle Assessment (LCA) and Techno-Economic (TEA) evaluation incorporating ASPEN Plus process modeling considering different configurations and energy scenarios. The TEA incorporates data from kinetic experiments from various catalysts to evaluate the GSR process under various conditions. The goal of this work is to evaluate GSR’s potential to serve as a low-carbon alternative to SMR, focusing on global warming potential and additional impact categories to evaluate a wide spectrum of environmental impacts. Comparative assessments were conducted with SMR, chemical loop reforming (CLR), and proton exchange membrane (PEM) electrolysis to explore trade-offs across environmental metrics. The environmental impact assessment of this work encompasses the entire hydrogen production lifecycle from raw material extraction to plant decommissioning, using a cradle-to-gate boundary. Preliminary findings highlight that GSR, when integrated with low-carbon energy sources, could significantly reduce environmental impacts, making it a promising candidate for low-carbon hydrogen infrastructure. The insights from this business case evaluation aim to guide industry in scale-up and commercialization of this promising clean energy technology.
We investigated the influence of CO2-induced geochemical reactions on the cohesive-frictional properties of host rock within the context of CO2 storage in a saline aquifer and focused on the Mt. Simon sandstone. The research objective was to model geo-mechanical changes due to host rock exposure to CO2-saturated brine while accounting for heterogeneity, double-scale porosity, and granular structure. We formulated a three-level multi-scale model for host rocks. We conducted scanning electron microscopy analyses to probe the microstructure and grid nanoindentation to measure the mechanical response. We derived new nonlinear strength upscaling solutions to correlate the effective strength characteristics and the macroscopic yield surface to the micro-structure at the nano-, micro-, and meso-scales. Specifically, our theoretical model links CO2-induced microstructural alterations to a reduction in the size of the yield surface, and a drop in the value of the friction coefficient. In turn, regarding the Illinois Basin Decatur Project, the CO2-induced drop in friction coefficient is linked to an increase in the risk of fault slip and a higher probability of induced microseismicity during and after the end of CO2 underground injection operations. The theoretical model presented is essential for the geo-mechanical modeling of CO2 underground injection operations at multiple length-scales.
Steels have a proven track record of safe operation in steam power plants for decades. Interest in developing supercritical CO2 power cycles as a more efficient and sustainable alternative to steam cycles has driven a need to understand steel performance in these new environments. In particular, the potential of the high temperature CO2 environment to influence the creep behavior of the steel must be determined. Prior research on this topic between the 1960s and 1980s found conflicting conclusions, but nevertheless raised the possibility that carburization during CO2 exposure may strongly affect the creep behavior. This raises concerns particularly for thin-sectioned components such as compact heat exchangers, where even small rates of carburization can become problematic over long operating lifetimes. To shed light on this issue, this research investigates the creep behavior of austenitic stainless steel 347H and 309H (a higher Cr alternative) at 650°C. Specimens of 0.5, 1.0, and 2.0 mm thickness were tested to further assess the effect of steel thickness. Both steels show a reduction in creep life in CO2 relative to air, with 309H showing slightly better performance than 374H. Analysis is ongoing to determine the reason for degraded creep properties.
Steels have a proven track record of safe operation in steam power plants for decades. Interest in developing supercritical CO2 power cycles as a more efficient and sustainable alternative to steam cycles has driven a need to understand steel performance in these new environments. In particular, the potential of the high temperature CO2 environment to influence the creep behavior of the steel must be determined. Prior research on this topic between the 1960s and 1980s found conflicting conclusions, but nevertheless raised the possibility that carburization during CO2 exposure may strongly affect the creep behavior. This raises concerns particularly for thin-sectioned components such as compact heat exchangers, where even small rates of carburization can become problematic over long operating lifetimes. To shed light on this issue, this research investigates the creep behavior of austenitic stainless steel 347H and 309H (a higher Cr alternative) at 650°C. Specimens of 0.5, 1.0, and 2.0 mm thickness were tested to further assess the effect of steel thickness. Both steels show a reduction in creep life in CO2 relative to air, with 309H showing slightly better performance than 374H. Analysis is ongoing to determine the reason for degraded creep properties.
Atmospheric mixing ratios of carbon dioxide (CO2) are largely controlled by anthropogenic emissions and biospheric fluxes. The processes controlling terrestrial biosphere-atmosphere carbon exchange are currently not fully understood, resulting in terrestrial biospheric models having significant differences in the quantification of biospheric CO2 fluxes. Atmospheric transport models assimilating measured (in situ or space-borne) CO2 concentrations to estimate "top-down" fluxes, generally use these biospheric CO2 fluxes as a priori information. Most of the flux inversion estimates result in substantially different spatio-temporal posteriori estimates of regional and global biospheric CO2 fluxes. The Orbiting Carbon Observatory 2 (OCO-2) satellite mission dedicated to accurately measure column CO2 (XCO2) allows for an improved understanding of global biospheric CO2 fluxes. OCO-2 provides much-needed CO2 observations in data-limited regions facilitating better global and regional estimates of "top-down" CO2 fluxes through inversion model simulations. The specific objectives of our research are to: 1) conduct GEOS-Chem 4D-Var assimilation of OCO-2 observations, using several state-of-the-science biospheric CO2 flux models as a priori information, to better constrain terrestrial CO2 fluxes, and 2) quantify the impact of different biospheric model prior fluxes on OCO-2-assimilated a posteriori CO2 flux estimates. Here we present our assessment of the importance of these a priori fluxes by conducting Observing System Simulation Experiments (OSSE) using simulated OCO-2 observations with known "true" fluxes.