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Charged-particle spectra from μ – capture on Al

Published data on the emission of charged particles following nuclear muon capture are extremely limited. In addition to its interest as a probe of the nuclear response, these data are important for the design of some current searches for lepton flavor violation. This work presents momentum spectra of protons and deuterons following μ- capture in aluminum. It is the first measurement of a muon capture process performed with a tracking spectrometer. A precision of better than 10% over the momentum range of 100–190MeV/c for protons is obtained; for deuterons of 145–250MeV/c the precision is better than 20%. The observed partial yield of protons with emission momenta above 80MeV/c (kinetic energy 3.4MeV) is 0.0322 ± 0.0007(stat) ± 0.0022(syst) per capture, and for deuterons above 130MeV/c (4.5MeV) it is 0.0122 ± 0.0009(stat) ± 0.0006(syst). Extrapolating to total yields gives 0.045 ± 0.001(stat) ± 0.003(syst) ± 0.001(extrapolation) per capture for protons and 0.018 ± 0.001(stat) ± 0.001(syst)± 0.002(extrapolation) for deuterons, which are the most precise measurements of these quantities to date.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

ProvLight: Efficient Workflow Provenance Capture on the Edge-to-Cloud Continuum

Modern scientific workflows require hybrid infrastructures combining numerous decentralized resources on the IoT/Edge interconnected to Cloud/HPC systems (aka the Computing Continuum) to enable their optimized execution. Understanding and optimizing the performance of such complex Edge-to-Cloud workflows is challenging. Capturing the provenance of key performance indicators, with their related data and processes, may assist in understanding and optimizing workflow executions. However, the capture overhead can be prohibitive, particularly in resource-constrained devices, such as the ones on the IoT/Edge.To address this challenge, based on a performance analysis of existing systems, we propose ProvLight, a tool to enable efficient provenance capture on the IoT/Edge. We leverage simplified data models, data compression and grouping, and lightweight transmission protocols to reduce overheads. We further integrate ProvLight into the E2Clab framework to enable workflow provenance capture across the Edge-to-Cloud Continuum. This integration makes E2Clab a promising platform for the performance optimization of applications through reproducible experiments.We validate ProvLight at a large scale with synthetic workloads on 64 real-life IoT/Edge devices in the FIT IoT LAB testbed. Evaluations show that ProvLight outperforms state-of-the-art systems like ProvLake and DfAnalyzer in resource-constrained devices. ProvLight is 26—37x faster to capture and transmit provenance data; uses 5—7x less CPU; 2x less memory; transmits 2x less data; and consumes 2—2.5x less energy. ProvLight [1] and E2Clab [2] are available as open-source tools.

Rosendo, Daniel↗

The Effects of Synthesis Conditions on the Carbon Capture Capacity of Polyethylenimine Impregnated Protonated Titanate Nanotubes

Capture and storage of carbon dioxide emitted from power plants, which burn fossil fuels, is one of the best ways to mitigate climate change. Polyethylenimine (PEI) impregnated protonated titanate nanotubes (PEI-PTNTs) are efficient amine-modified solid adsorbents for post combustion carbon capture. This study is to investigate the effects of synthesis conditions of titanate nanotubes on the carbon capture capacity of PEI-PTNTs. PTNTs are synthesized using hydrothermal treatment of TiO 2 anatase powder at different temperatures and in different days, followed by washing with dilute HCl solution and deionized water. PEI-PTNTs are prepared by loading PEI (M.W. = 10,000) onto PTNTs at a weight ratio of 1:1 using a wet impregnation process. PTNTs and PEI-PTNTs are characterized using transmission electron microscopy, porosity and surface area analysis, powder X-ray diffraction, and Fourier transform infrared spectroscopy. CO 2 adsorption is conducted at 75 °C using simulated flue gas, and CO 2 desorption is performed at 110 °C by purging the adsorbent with dry nitrogen gas. CO 2 adsorption experiments demonstrate that the PEI-PTNTs synthesized at 130 °C within 3 or 5 days, have the highest CO 2 capture capacity. These optimized PEI-PTNTs have a significant potential to capture CO 2 from power plants.

Materials Science↗

Simulations of short-term exposure to NO 2 and PM 2.5 to inform capture efficiency standards

The California building code requires all new or renovated residential dwelling units to have kitchen exhaust ventilation to manage air pollutants and moisture generated during cooking. Current performance requirements are specified as a minimum airflow and maximum sound level. This report presents an analysis to support consideration of adding a capture efficiency requirement to the code. The analysis uses a physics-based simulation model to calculate air pollutant concentrations in homes that result from cooking and the inflow of outdoor air, mediated by loss and removal process including deposition, dwelling unit ventilation, and the use of a range hood with varying levels of capture efficiency. Calculated pollutant concentrations are compared to relevant, health-based guidelines. The analysis considers the highest 1-hour concentration of nitrogen dioxide (NO 2 ), which is a product of natural gas combustion and the highest 24-hour concentrations of fine particulate matter (PM 2.5 ) which is emitted in substantial quantities from frying, broiling and grilling among other cooking activities. For NO 2 , the analysis considers cooking of a dinner for 3-4 persons consisting of pasta, meat sauce, a par-boiled vegetable, and baked garlic bread. For PM 2.5 , the analysis considers a day in which breakfast emitted particles at the 80th percentile and lunch and dinner entailed particle emissions at the 50th percentile of cooking emission events reported in the literature. Model simulations were performed to determine the level of range hood capture efficiency that will allow these cooking scenarios to occur in the vast majority (>99%) of new homes being built in California while maintaining pollutant concentrations below the health-based guidelines, if the range hood is used throughout cooking. All homes were assumed to have dwelling unit ventilation at the rate required in the building code. Simulation model input parameters were specified using a Monte Carlo approach to represent a range of housing characteristics, outdoor conditions, and indoor pollutant dynamics. Simulation results suggest that requiring a minimum capture efficiency of at least 70% is needed to avoid unacceptably high NO 2 (1-h average concentration of 100 ppb or higher) and at least 60% to avoid unacceptably high PM 2.5 (24-h average of 25 μg/m³ or higher). These results were driven by multi-family homes, which have a smaller volume of air to dilute any pollutants not captured and removed at the cooking area, resulting in higher concentrations.

54 ENVIRONMENTAL SCIENCES↗

Zeolite Membrane Reactor for Pre-Combustion Carbon Dioxide Capture

Water-gas shift (WGS) reaction followed by carbon dioxide (CO 2 ) separation is a critical step in the integrated gasification combined cycle (IGCC) process for fossil-fuel-fired electrical power generation with CO 2 capture. To intensify the IGCC process hydrogen-permselective zeolite membrane reactor offers promise to replace the conventional energy-intensive fixed-bed reactors and solvent-based CO 2 capture units. The objectives of this project were to develop a bench-scale zeolite membrane reactor (total membrane area: 932 cm 2 for a 21-tube membrane bundle) for the water-gas-shift reaction of raw syngas from an oxygen-blown coal-gasifier for H 2 production with simultaneous CO 2 separation at the capability of about 2 kilograms H 2 per day (equivalent to 2 kW IGCC power plant) and to demonstrate significant progress toward achieving overall performance goal of 90% CO 2 capture rate with 95% CO 2 purity at the cost of electricity 30% less than the baseline carbon capture approaches. This report summarizes results obtained in this project on scaling up the zeolite membrane reactor by a factor of 200 in membrane area, tests of the bench-scale zeolite membrane reactor for the water-gas-shift reaction at high temperature and high-pressure, and techno-economic analysis of the integration of the zeolite membrane reactor in IGCC power plant for the electrical generation with CO 2 capture.

20 FOSSIL-FUELED POWER PLANTS↗

Characterizing Shielded Special Nuclear Material by Neutron Capture Gamma-Ray Multiplicity Counting

We present a new neutron multiplicity counting analysis and measurement method for neutron-shielded fissile material using neutron-capture gamma rays. Neutrons absorbed in shielding produce characteristic gamma rays that preserve the otherwise lost neutron multiplicity signature. Neutron multiplicity counting provides estimates of fission parameters, such as neutron leakage multiplication, spontaneous fissioner (e.g. Pu-240) mass, and (α,n) ratio. Standard neutron multiplicity counting can incorporate the new neutron-capture gamma-ray multiplicity counting technique to characterize previously degenerate or intractable source configurations by maximizing the multiplicity signature. The new method decouples neutron source-detector interferences, such as reflection and thermalization time in the detector, that could improve measurements of the mean neutron lifetime. We also develop a detector prototype for the multiplicity counting of neutron-capture gamma rays and present detector design considerations, such as detection material and shielding, to optimize the detection of the 2.2 MeV hydrogen capture gamma ray. We simulate the prototype neutron- capture gamma-ray multiplicity counter against the BeRP ball in polyethylene shells to inform future measurements.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Demonstration and Validation of Additively Manufactured Intensified Device for Enhanced Carbon Capture

In FY 2018 and 2019, ORNL personnel designed, prototyped, characterized, and tested the enhancement of amine-based carbon capture using additively manufactured intensified devices, i.e., devices combining multiple thermodynamic and kinetic processes into one unit operation. State of the art scrubbing technology often employs inter-stage cooling which requires multiple stages of single-purpose unit operations, leading to larger equipment size, higher capital cost, and sometimes less than optimal operating conditions for each piece of equipment. It was proposed that integrating multiple thermodynamic and kinetic operations into one unit could mitigate or negate these drawbacks. Heat and mass transfer studies demonstrated that an additively manufactured intensified device could significantly improve capture efficiency at bench scale. This project is a continuation of FEAA130 and aims at (1) demonstration and validation of enhanced CO 2 capture with 3D printed intensified devices (i.e., mass exchanger packing with internal cooling channels), for low-aqueous-solvent (LAS) based capture at the ORNL-constructed laboratory-scale (4.5-feet tall) column, namely Column A, with built-in cooling and (2) computational scoping on the conceptual design of a flexible and modular larger column, namely Column B, at ORNL for further demonstration of enhanced capture for aqueous solvent. To execute this multi-faceted project scope, an integrated project team from ORNL’s Manufacturing Science Division is tasked with applying capabilities in computational fluid dynamics (CFD), additive manufacturing, and absorber-scale demonstration/validation experiments.

42 ENGINEERING↗

Performance Criteria for Capture and/or Immobilization Technologies (Revision 1)

The capture and subsequent immobilization of regulated volatile radionuclides from the off-gas streams of a used nuclear fuel (UNF) reprocessing facility has been a topic of substantial research interest for the US Department of Energy and its international counterparts. Removal of specific radionuclides from the plant effluent streams before discharge to the environment is required to meet regulations set forth by the US Environmental Protection Agency. Upon removal, the radionuclides, as well as associated sorbents that cannot be regenerated in a cost-effective manner, are destined for conversion to a waste form. Research in separation and capture methodologies has included a wide range of technology types, and studies of waste forms are correspondingly diverse. In considering the future development and implementation of both sorbents and waste forms, it is necessary to identify benchmark measures of performance to objectively evaluate each sorbent system or waste form. Sets of performance criteria and associated metrics have been developed for sorbent and waste form evaluation. These criteria address physical, radiological, and chemical characteristics, technical practicality, technical maturity, cost, and, for sorbents, system performance. The criteria and metrics appear to be robust and should be applicable despite the eventual waste classification (as either high- or low-level waste). They are flexible enough to address both aqueous reprocessing and electrochemical reprocessing of UNF. These criteria sets can serve as tools to evaluate performance at multiple stages within the development process, and in this revision (Revision 1) they have been used to assess technologies relating to krypton/xenon separations and iodine capture from off-gas streams arising from UNF reprocessing. Assessment of krypton/xenon separations using engineered forms of two zeolite minerals (silver mordenite and hydrogen mordenite in a polyacrylonitrile-based binder [AgZ-PAN/HZ-PAN]) found that the zeolite-based separation is relatively advanced in its development, but several key issues require resolution. First, desorption processes for both krypton and xenon require refinement to provide an understanding of the product purity that can be achieved. Second, adsorption rate data is needed in order to calculate the bed depth required for effective separation. Finally, it is strongly recommended that a technical review of krypton/xenon separation by AgZ-PAN/HZ-PAN be performed to synergize available data and assess the cost savings and operational benefits that may be realized from implementation of this technology. Assessment of metal organic frameworks (MOFs) for their use in the separation of krypton/xenon found that the ideal separation would be performed using a single-column system with a MOF selective for krypton over xenon. A robust research effort should work to identify a krypton-selective MOF designed to operate at temperatures of approximately 0°C or higher, which could be preferred over cryogenic krypton/xenon capture for used fuel reprocessing off-gas streams. In the case of the CaSDB-MOF (the most well-understood xenon sorbent to date), two issues are judged of high importance. First, xenon breakthrough capacity for the CaSDB-MOF in prototypical conditions should be determined. Preliminary research indicates that breakthrough may be near immediate, presenting a substantial obstacle in separative system design. Second, development of desorption methodology should be performed to determine regeneration time, energy requirements, and the product stream composition. Silver-based sorbents (AgZ and AgAero) for use in iodine capture from the dissolver off-gas were evaluated against the established criteria. These sorbents are significantly better understood for this application as a result of research efforts over the past decade. The potential implementation of AgAero at a large scale is hindered by its physical degradation by components of the dissolver off-gas stream. Less is known about the adsorption of iodine by these sorbents from other off-gas streams in the plant. Initial experimental efforts have been closely coordinated in an effort to understand organic iodine (such as would be found in the vessel off-gas) adsorption by AgZ and AgAero. Future work should expand this experimental program, and analysis of other reprocessing facility off-gas streams such as the vitrification off-gas stream should be conducted to better understand other potential applications for iodine sorbents. A review of iodine waste form development shows that this area is diverse and that multiple promising waste forms have been identified for the immobilization of radioactive iodine. Efforts related to the direct conversion of iodine sorbents (including AgZ and AgAero) should be continued because of the advantages of direct conversion in a waste management strategy and other sorbents should continue to be advanced as merited.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Bituminous Coal and Natural Gas to Electricity: >90% Capture Cases Technical Note

This technical note provides cost and performance estimates for post combustion carbon capture (PCCC) systems designed for greater than 90 percent capture on conventional PC- and NG-fueled power plants. The cost and performance estimates provided here were developed using the National Energy Technology Laboratory’s (NETL’s) well-documented methodology for conducting technoeconomic analysis of fossil energy conversion systems and leveraging published performance and cost projections for higher capture rate systems. Included in this technical note is a brief description of the method used to adjust select 90 percent capture cases from NETL’s Cost and Performance Baselines for Fossil Energy Systems Volume 1: Bituminous Coal and Natural Gas to Electricity, hereafter referred to as the Baseline Study. This technical note is intended to serve as an interim update to NETL’s Baseline Study cases by providing cost and performance estimates for high capture PCCC technology that can be deployed in the near-term at fossil-fueled electricity generating units.

20 FOSSIL-FUELED POWER PLANTS↗

Front End Engineering Design of Linde-BASF Advanced Post-Combustion CO 2 Capture Technology at a Southern Company Natural Gas-Fired Power Plant (Final Scientific/Technical Report)

This document details the execution of Cooperative Agreement DE-FE0031847, “Front End Engineering Design of Linde-BASF Advanced Post-Combustion Carbon Dioxide (CO 2 ) Capture Technology at a Southern Company Natural Gas-Fired Power Plant” during the period of 10/1/2019 to 6/30/2022. The project was funded by the U.S. Department of Energy’s Office of Fossil Energy and Carbon Management (FECM) and managed by the National Energy Technology Laboratory (NETL). Southern Company Services, Inc. (SCS) was the prime recipient and led the project team. Other members of the project team included Linde, Inc. (Linde), Linde Engineering – Dresden (LED), and BASF. The overall goal of the project was to complete a front-end engineering design (FEED) study for installing the Linde-BASF post-combustion capture (PCC) technology at an existing domestic natural gas-fired combined cycle (NGCC) power plant within Southern Company’s portfolio of assets. The CO 2 capture plant was to be of commercial scale (at least 375 MWe) and include process units for pre-conditioning of the flue gas system, the CO 2 capture plant island, storage vessels, the CO 2 compression train, and any necessary components for integration into the NGCC plant. Mississippi Power’s Plant Daniel Unit #4 was chosen as the host site for the FEED with the target of capturing 90% of CO 2 emissions from the existing combustion turbines. The information produced by the FEED was used to develop a cost estimate of +/- 15% accuracy. Capital costs, excluding financing, are estimated at approximately $\$752$ million dollars (2021). The execution of a project based on this FEED study has an estimated duration of almost five years.

03 NATURAL GAS↗

Analysis of Carbon Capture Retrofits for Cement Plants

The objective of this study is to provide an estimate of the cost to capture CO 2 in retrofit applications at cement plants. The cement plant configurations considered in this study include natural gas and solid fuel (coal and coke) cases, and both wet- and dry kiln-fed plant designs, however the base cement plants in this study were not evaluated other than characterization of their kiln off-gas stream and high-level quantification of heat integration potential at the existing plant. In each case, the base cement plant produces 1.5 M tonnes per year of finished cement, assuming 91.4 percent clinker content. This analysis includes a 10 percent retrofit cost increase for process integration and low grade heat recovery, when compared to the analogous non-heat integration case. Heat integration is considered as a potential offset to capture system heating demands (i.e., as a percentage reduction). Recovery and reuse of excess heat from the base cement plant can provide economic benefits—primarily by reducing the need to purchase supplemental natural gas for CO 2 solvent regeneration—but any process improvement must be great enough to overcome the cost increases (i.e., capital and O&M) necessary to realize those benefits. With heat integration potential of 10 percent and 30 percent, that benefit wasn’t significant enough to offset the increase in capital and operating costs, and a cost of capture increase was observed based on the assumptions in this report. Benefits of heat integration potential may be realized when natural gas prices are higher, as demonstrated in the sensitivity to natural gas price where crossover points exist between heat integration cases and their respective non-heat integration cases. Four of the base cases were further evaluated to explore the cost implications of deeper levels of gas pre-treatment to remove oxides of nitrogen (NOx) and oxides of sulfur (SOx) from the kiln off-gas stream prior to CO 2 capture, purification, and compression. The results of these additional case analyses showed a 7.4–18.8 percent increase in cost of capture over the respective base case (i.e., analogous cases without SOx/NOx removal).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Natural Gas Combined Cycle (NGCC) Power Plants with Carbon Capture and Exhaust Gas Recycle (EGR)

The purpose of this study is to determine the cost and performance of natural gas combined cycle (NGCC) power plants using state-of-the-art gas turbines with post combustion carbon capture and recycle streams designed to increase the CO 2 concentration in the inlet to the capture system. Increasing the inlet CO 2 concentration by exhaust gas recycle (EGR) is expected to improve the efficiency of the capture system and reduce its costs. Primary results indicate that adding EGR to NGCC plants with CO 2 capture results in minimal improvement to the cost of electricity. The addition of 50 percent EGR in NGCC plants with CO 2 capture reduces the LCOE by 2 percent over the LCOE of the same design without EGR as reference. Including the EGR ductwork and cooler in a greenfield plant design could still be prudent since there is some cost advantage to EGR and it would allow more flexibility for taking advantage of future improvements in the technology.

20 FOSSIL-FUELED POWER PLANTS↗

Off-Design Load Analysis of sCO2 Bottoming Cycle for a Natural Gas Combined Cycle Power Plant with Carbon Capture

As an alternative to a steam cycle, a supercritical carbon dioxide (sCO2) power cycle can be considered. Able et. al performed an analysis of an sCO2 cycle in a 2x2-1 configuration; however, this study did not include carbon capture. Previous studies assumed an H-Frame turbine and added a solvent based 95% carbon capture system and performed a levelized cost of electricity (LCOE) optimization for the plant. Their results suggest a LCOE slightly better than when using a steam cycle. In the study, steam is still generated in the heat recovery sections for the solvent regeneration in the carbon capture stripper reboiler. H-Frame gas turbines are also assumed. This work starts with the optimal design from the mentioned work to analyze the off-design performance of the power plant from 100% down to 50% load. The main operational findings and plant-efficiency for off-load conditions while maintaining the target CO2 capture rate are presented. H-Frame gas turbine off-design performance and exhaust conditions to the heat recovery section are obtained from commercial software, Thermoflow®. The CO2 turbomachinery, heat exchangers and other unit operations are sized and implemented in an Aspen Plus® model. Using the gas turbine exhaust conditions as input, the sCO2 cycle is optimized by adjusting stream split ratios, sCO2 circulation flowrate and compressor speed for maximum efficiency. This is done while keeping the target 95% CO2 capture.

Chinen, Anderson Soares↗

Bench-scale Development of a Transformational Graphene Oxide-based Membrane Process for Post-combustion CO 2 Capture

Graphene-based materials, such as graphene and graphene oxide (GO), have been considered as next-generation membrane materials. GTI Energy and The State University of New York at Buffalo (UB) have been developing a transformational GO-based membrane process (designated as GO2) that integrates a high CO 2 /N 2 selectivity membrane (GO-1) and a high CO 2 flux membrane (GO-2) for post-combustion CO 2 capture. An innovative membrane structure, consisting of GO nanochannels intercalated by single-walled carbon nanotube (SWCNT), was developed. The membrane prepared on hollow fiber substrate showed CO 2 permeance as high as 1,300 GPU with CO 2 /N 2 selectivity >200. The membranes were successfully scaled up to effective area of 50-100 cm 2 . The 50-100 cm 2 membranes showed CO 2 /N 2 selectivity ≥200 and CO 2 permeance ≥1,000 GPU for the GO-1 type, and CO 2 /N 2 selectivity ≥20 and CO 2 permeance ≥2,500 GPU for the GO-2 type. The CO 2 capture performance of the GO-based membranes was tested using a simulated flue gas. The testing results indicate that the GO-based membranes are stable in the presence of flue gas contaminants. The GO-based membranes were then further scaled up to a surface area of 1,000 cm 2 . Good stability was achieved during an integrated testing with GO-1 and GO-2 membranes using simulated flue gas. A bench-scale system was designed, constructed, and tested at the National Carbon Capture Center (NCCC). Good stability was achieved during testing of a single-stage process with >10 shutdowns/startups at NCCC. During the integrated testing, the membranes showed good stability at 50°C and 57°C. 70-90% CO 2 removal efficiencies and ≥95% CO 2 purity were validated during the steady state operation at NCCC. Techno-economic analysis indicates the GO2 membrane-based process technology provides a reduction in both the levelized cost of electricity (LCOE) and cost of capture when compared to the reference B12B case presented in the Cost and Performance Baseline for Fossil Energy Plants Volume 1: Bituminous Coal and Natural Gas to Electricity study prepared by the National Energy Technology Laboratory (NETL), before considering any system optimization or improvement opportunities. The benefits are primarily driven by a reduction in the equipment costs of the CO 2 capture process vs. the solvent-based reference process in NETL Case B12B as well as a decrease in the base plant size.

20 FOSSIL-FUELED POWER PLANTS↗

Direct Air Reactive Capture and Conversion for Utility-Scale Energy Storage (Final Report)

This final report for FEW0277 summarizes the work performed over the project performance period of October 2021 – March 2025. This project was funded under the “Reactive Capture and Conversion R&D” lab call released in FY2021. The goal of the project was to develop dual-function materials and process for capturing CO 2 from the atmosphere and converting it into CH 4 . The work was organized into four parallel tracks in 1) direct air capture materials synthesis and characterization, 2) catalysts for CO 2 conversion, 3) mechanistic investigations via ab initio simulations, and 4) process modeling, technoeconomic analysis, and lifecycle assessment. The project was split into two budget periods. The first budget period focused on development of amine-based materials, due to their known performance for CO 2 direct air capture and their potential to act synergistically with metal catalysts to enable a low-temperature methanation pathway. The second budget period focused on development of alkali-based materials and a simulated-moving-bed process for high conversion catalytic reduction of captured CO 2 to CH 4 . All project milestones were completed during the project performance period and are summarized in this report. Our work resulted in publication of eight peer-reviewed manuscripts, one patent application, and numerous presentations given at domestic and international conferences and invited academic department seminars.

03 NATURAL GAS↗

Evaluating Polymer Properties with Different Additives for Carbon Capture and Other Applications

Anthropogenic climate change is one of this generation’s most pressing concerns, with the potential to completely alter the delicate balance we’ve struck with nature. Already, global temperatures have risen 1.29°C, leading to disrupted weather systems, extinctions, increased risks of wildfires, and sea level rise, to name a few effects. Carbon dioxide emission from the combustion of fossil fuels and other industrial activity is a large driver of this phenomenon, as it absorbs heat before it can be radiated away from Earth, trapping it. Carbon dioxide has reached unprecedented levels in our atmosphere, showing a 50% increase from preindustrial averages to a whopping 430 ppm. Thus, reducing the amount of carbon dioxide via carbon capture technology is an important endeavor that serves to benefit everyone. The Microencapsulated CO 2 Sorbent (MECS) team at Lawrence Livermore National Laboratory (LLNL) has turned to microencapsulation to approach this endeavor. Microcapsules provide an attractive approach to carbon capture, combining large surface areas for more efficient mass transfer, regenerative abilities, reduced solvent loss, and improved handling. Additionally, while existing carbon capture technology relies on industrial plants, capsules could present a modular approach to carbon capture, reducing the need for extensive physical infrastructure. The MECS team’s design consists of a polymer membrane that contains a liquid carbon sequestering sorbent, aqueous sodium carbonate. The carbon capturing reaction occurs in three distinct steps, the first of which is the dissolution of carbon dioxide into the sorbent solution and its conversion into carbonic acid (H 2 CO 3 ), shown in equations 1 and 2 respectively. Because this step hinges upon the ability of carbon dioxide to reach the solution inside the capsule, it is necessary that the microcapsule shell is permeable to carbon dioxide gas. The MECS team produces these microcapsules using the in-air droplet encapsulation apparatus (IDEA) shown in figure 1, which can produce uniform micron-scale droplets at speeds much faster than traditional single-dispersal microfluidic-based techniques. The IDEA Is 100 times faster than these current techniques and can reach up to 1000 times their speed when incorporating a multi-nozzle design. Additionally, because droplets are produced in-air via vibration, IDEA can decrease post-processing times and material waste by 99% and can fabricate microgels that are 10 to 100 times more viscous than can be produced via traditional microfluidics. While this design represents a breakthrough in the throughput, efficiency, and tunability of microcapsule production, it imposes a major constraint on the microcapsule curing process. Because microcapsule shells are crosslinked with UV light while falling 30 cm through the air, this gives them a reaction window of approximately 0.2 seconds. Thus, the system and shell formulations must be optimized such that the shells can be fully crosslinked within this very narrow window, prompting investigations into curing behavior.

36 MATERIALS SCIENCE↗

Advances in Carbon Capture and Use (CCU) Technologies: A Comprehensive Review and CO2 Mitigation Potential Analysis

One of society’s major current challenges is carbon dioxide emissions and their consequences. In this context, new technologies for carbon dioxide (CO2) capture have attracted much attention. One of these is carbon capture and utilization (CCU). This work focuses on the latest trends in a holistic approach to carbon dioxide capture and utilization. Absorption, adsorption, membranes, and chemical looping are considered for CO2 capture. Each CO2 capture technology is described, and its benefits and drawbacks are discussed. For the use of carbon dioxide, various possible applications of CCU are described, starting with the utilization of carbon dioxide in agriculture and proceeding to the conversion of CO2 into fuels (catalytic processes), chemicals (photocatalytic processes), polymers, and building supplies. For decades, carbon dioxide has been used in industrial processes, such as CO2-enhanced oil recovery, the food industry, organic compound production (such as urea), water treatment, and, therefore, the production of flame retardants and coolants. There also are several new CO2-utilization technologies at various stages of development and exploitation, such as electrochemical conversion to fuels, CO2-enhanced oil recovery, and supercritical CO2. At the end of this review, future opportunities are discussed regarding machine learning (ML) and life cycle assessment (LCA).

Peres, Christiano B.↗

Current Developments of Carbon Capture Storage and/or Utilization–Looking for Net-Zero Emissions Defined in the Paris Agreement

An essential line of worldwide research towards a sustainable energy future is the materials and processes for carbon dioxide capture and storage. Energy from fossil fuels combustion always generates carbon dioxide, leading to a considerable environmental concern with the values of CO2 produced in the world. The increase in emissions leads to a significant challenge in reducing the quantity of this gas in the atmosphere. Many research areas are involved solving this problem, such as process engineering, materials science, chemistry, waste management, and politics and public engagement. To decrease this problem, green and efficient solutions have been extensively studied, such as Carbon Capture Utilization and Storage (CCUS) processes. In 2015, the Paris Agreement was established, wherein the global temperature increase limit of 1.5 °C above pre-industrial levels was defined as maximum. To achieve this goal, a global balance between anthropogenic emissions and capture of greenhouse gases in the second half of the 21st century is imperative, i.e., net-zero emissions. Several projects and strategies have been implemented in the existing systems and facilities for greenhouse gas reduction, and new processes have been studied. This review starts with the current data of CO2 emissions to understand the need for drastic reduction. After that, the study reviews the recent progress of CCUS facilities and the implementation of climate-positive solutions, such as Bioenergy with Carbon Capture and Storage and Direct Air Capture. Future changes in industrial processes are also discussed.

Regufe, Maria João (ORCID:0000000327748302)↗