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DOE OSTI2011

New Horizons for Hydrogen: Producing Hydrogen from Renewable Resources

Recent events have reminded us of the critical need to transition from crude oil, coal, and natural gas toward sustainable and domestic sources of energy. One reason is we need to strengthen our economy. In 2008 we saw the price of oil reach a record $93 per barrel. With higher oil prices, growing demand for gasoline, and increasing oil imports, an average of $235 billion per year, has left the United States economy to pay for foreign oil since 2005, or $1.2 trillion between 2005 and 2009. From a consumer perspective, this trend is seen with an average gasoline price of $2.50 per gallon since 2005, compared to an average of $1.60 between 1990 and 2004 (after adjusting for inflation). In addition to economic impacts, continued reliance on fossil fuels increases greenhouse gas emissions that may cause climate change, health impacts from air pollution, and the risk of disasters such as the Deepwater Horizon oil spill. Energy efficiency in the form of more efficient vehicles and buildings can help to reduce some of these impacts. However, over the long term we must shift from fossil resources to sustainable and renewable energy sources.

08 HYDROGEN↗
DOE OSTI2011

A Review of Barriers to and Opportunities for the Integration of Renewable Energy in the Southeast

The objectives of this study were to prepare a summary report that examines the opportunities for and obstacles to the integration of renewable energy resources in the Southeast between now and the year 2030. The report, which is based on a review of existing literature regarding renewable resources in the Southeast, includes the following renewable energy resources: wind, solar, hydro, geothermal, biomass, and tidal. The evaluation was conducted by the Oak Ridge National Laboratory for the Energy Foundation and is a subjective review with limited detailed analysis. However, the report offers a best estimate of the magnitude, time frame, and cost of deployment of renewable resources in the Southeast based upon the literature reviewed and reasonable engineering and economic estimates. For the purposes of this report, the Southeast is defined as the states of Alabama, Arkansas, Florida, Georgia, Kentucky, Louisiana, Mississippi, North Carolina, South Carolina, Tennessee, Virginia, and West Virginia. In addition, some aspects of the report (wind and geothermal) also consider the extended Southeast, which includes Maryland, Missouri, Oklahoma, and Texas. A description of the existing base of renewable electricity installations in the region is given for each technology considered. Where available, the possible barriers and other considerations regarding renewable energy resources are listed in terms of availability, investment and maintenance costs, reliability, installation requirements, policies, and energy market. As stated above, the report is a comprehensive review of renewable energy resources in the southeastern region of United States based on a literature study that included information obtained from the Southern Bio-Power wiki, sources from the Energy Foundation, sources available to ORNL, and sources found during the review. The report consists of an executive summary, this introductory chapter describing report objectives, a chapter on analysis methods and the status of renewable resources, chapters devoted to each identified renewable resource, and a brief summary chapter. Chapter 2 on analysis methods and status summarizes the benefits of integrating renewable energy resources in the Southeast. The utilization of the existing fuels, both the fossil fuels and the renewable energy resources, is evaluated. The financial rewards of renewable resources are listed, which includes the amount of fuel imported from outside the Southeast to find the net benefit of local renewable generation, and both the typical and new green job opportunities that arise from renewable generation in the Southeast. With the load growth in the Southeast, the growth of transmission and fossil fuel generation may not meet the growing demands for energy. The load growth is estimated, and the benefits of renewable resources for solving local growing energy demands are evaluated. Chapters 3-7 discuss the key renewable energy resources in the Southeast. Six resources available in this region that are discussed are (1) wind, including both onshore and offshore; (2) solar, including passive, photovoltaic, and concentrating; (3) biomass energy, including switchgrass, biomass co-firing, wood, woody biomass, wood industry by-products (harvesting residues, mill waste, etc.), agricultural byproducts, landfill gas to energy and anaerobic digester gas; (4) hydro; and (5) geothermal. Because of limited development, ocean wave and tidal were not considered to be available in significant quantity before 2030 and are not presented in the final analysis. Estimates on the location of potential megawatt generation from these renewable resources in the Southeast are made. Each chapter will describe the existing base of the renewable electricity installations in the region now and, when available, the base of the existing manufacturing capacity in the region for renewable energy resources hardware and software. The possible barriers and considerations for renewable energy resources are presented.

03 NATURAL GAS↗
DOE OSTI2011

E85 Optimized Engine through Boosting, Spray-Optimized DIG, VCR and Variable Valvetrain

The use of biofuels for internal combustion engines has several well published advantages. The biofuels, made from biological sources such as corn or sugar cane, are renewable resources that reduce the dependence on fossil fuels. Fuels from agricultural sources can therefore reduce a countries energy dependency on other nations. Biofuels also have been shown to reduce CO2 emissions into the atmosphere compared to traditional fossil based fuels. Because of these benefits several countries have set targets for the use of biofuels, especially ethanol, in their transportation fuels. Small percentages of ethanol are common place in gasoline but are typically limited to 5 to 8% by volume. Greater benefits are possible from higher concentrations and some countries such as the US and Sweden have encouraged the production of vehicles capable of operating on E85 (85% denatured ethanol and 15% gasoline). E85 capable vehicles are normally equipped to run the higher levels of ethanol by employing modified fuel delivery systems that can withstand the highly corrosive nature of the alcohol. These vehicles are not however equipped to take full advantage of ethanol's properties during the combustion process. Ethanol has a much higher blend research octane number than gasoline. This allows the use of higher engine compression ratios and spark advance which result in more efficient engine operation. Ethanol's latent heat of vaporization is also much higher that gasoline. This higher heat of vaporization cools the engine intake charge which also allows the engine compression ratio to be increased even further. An engine that is optimized for operation on high concentrations of ethanol therefore will have compression ratios that are too high to avoid spark knock (pre-ignition) if run on gasoline or a gasoline/ethanol blend that has a low percentage alcohol. An engine was developed during this project to leverage the improved evaporative cooling and high octane of E85 to improve fuel economy and offset E85's lower energy content. A 2.0 L production Direct Injection gasoline, (DIg) engine employing Dual Independent Cam Phasing, (DICP) and turbo charging was used as the base engine. Modified pistons were used to increase the geometric compression ratio from 9.2:1 to 11.85:1 by modifying the pistons and adding advanced valvetrain to proved control of displacement and effective compression ratio through valve timing control. The advanced valvetrain utilized Delphi's two step valvetrain hardware and intake cam phaser with increased phasing authority of 80 crank angle degrees. Using this hardware the engine was capable of operating knock free on all fuels tested from E0-E85 by controlling effective compression ratio using a Late Intake Valve Closing, (LIVC) strategy. The LIVC strategy results in changes in the trapped displacement such that knock limited torque for gasoline is significantly lower than E85. The use of spark retard to control knock enables higher peak torque for knock limited fuels, however a loss in efficiency results. For gasoline and E10 fuels, full effective displacement could not be reached before spark retard produced a net loss in torque. The use of an Early Intake Valve Closing, (EIVC) strategy resulted in an improvement of engine efficiency at low to mid loads for all fuels tested from E0- E85. Further the use of valve deactivation, to a single intake valve, improved combustion stability and enabled throttle-less operation down to less than 2 bar BMEP. Slight throttling to trap internal residual provided additional reductions in fuel consumption. To fully leverage the benefits of E85, or ethanol blends above E10, would require a vehicle level approach that would take advantage of the improved low end torque that is possible with E85. Operating the engine at reduced speeds and using advanced transmissions (6 speeds or higher) would provide a responsive efficient driving experience to the customer. The vehicle shift and torque converter lockup points for high ethanol blends could take advantage of the significant efficiency advantage of down-speeding and operating at higher loads to deliver the required power.

02 PETROLEUM↗
DOE OSTI2011

NGNP SITE 2 HAZARDS ASSESSMENT

The Next Generation Nuclear Plant (NGNP) Project initiated at Idaho National Laboratory (INL) by the U.S. Department of Energy pursuant to the 2005 Energy Policy Act, is based on research and development activities supported by the Generation IV Nuclear Energy Systems Initiative. The principal objective of the NGNP Project is to support commercialization of the high temperature gas-cooled reactor (HTGR) technology. The HTGR is a helium-cooled and graphite-moderated reactor that can operate at temperatures much higher than those of conventional light water reactor (LWR) technologies. Accordingly, it can be applied in many industrial applications as a substitute for burning fossil fuels, such as natural gas, to generate process heat in addition to producing electricity, which is the principal application of current LWRs. Nuclear energy in the form of LWRs has been used in the U.S. and internationally principally for the generation of electricity. However, because the HTGR operates at higher temperatures than LWRs, it can be used to displace the use of fossil fuels in many industrial applications. It also provides a carbon emission-free energy supply. For example, the energy needs for the recovery and refining of petroleum, for the petrochemical industry and for production of transportation fuels and feedstocks using coal conversion processes require process heat provided at temperatures approaching 800 C. This temperature range is readily achieved by the HTGR technology. This report summarizes a site assessment authorized by INL under the NGNP Project to determine hazards and potential challenges that site owners and HTGR designers need to be aware of when developing the HTGR design for co-location at industrial facilities, and to evaluate the site for suitability considering certain site characteristics. The objectives of the NGNP site hazard assessments are to do an initial screening of representative sites in order to identify potential challenges and restraints to be addressed in design and licensing processes; assure the HTGR technology can be deployed at variety of sites for a range of applications; evaluate potential sites for potential hazards and describe some of the actions necessary to mitigate impacts of hazards; and, provide key insights that can inform the plant design process. The report presents a summary of the process methodology and the results of an assessment of hazards typical of a class of candidate sites for the potential deployment of HTGR reactor technology. The assessment considered health and safety, and other important siting characteristics to determine the potential impact of identified hazards and potential challenges presented by the location for this technology. A four reactor module nuclear plant (2000 to 2400 MW thermal), that co-generates steam, electricity for general use in the plant, and hot gas for use in a nearby chemical processing facility, to provide the requisite performance and reliability was assumed for the assessment.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2012

Variance Analysis of Wind and Natural Gas Generation under Different Market Structures: Some Observations

An important area of current research is whether large-scale penetration of variable renewable generation such as wind and solar power pose economic and operational burdens on the electricity system. In such scenarios, this issue has also raised considerable interest in the potential role and value of electricity storage as a method of mitigating variability in generation associated with the inherently variable nature of these forms of generation. At the same time, a number of studies have pointed to the potential benefits of renewable generation as a hedge against the volatility and potential escalation of fossil fuel prices. Prior research and this work suggest that the lack of correlation of renewable energy costs with fossil fuel prices means that adding large amounts of wind or solar generation may also reduce the volatility of system-wide electricity costs. Such variance reduction in overall system costs may be of significant value to consumers due to risk aversion. In contrast to this observation, other studies have focused on returns in restructured markets and noted that, in deregulated markets, baseload natural gas power generation may be relatively more attractive to investors because-unlike wind generation-peak power prices are often strongly correlated to natural gas prices. The analysis in this report recognizes that the potential value of risk mitigation associated with wind generation and natural gas generation may depend on whether one considers the consumer's perspective or the investor's perspective and whether the market is regulated or deregulated. We analyze the risk and return trade-offs for wind and natural gas generation for deregulated markets based on hourly prices and load over a 10-year period using historical data in the PJM Interconnection (PJM)2 from 1999 to 2008. Similar analysis is then simulated and evaluated for regulated markets under certain assumptions. Estimating the absolute value, as opposed to the relative value, of variance reduction will also depend on assumptions about risk aversion and other consumer preferences, such as loss aversion, and this is discussed.

03 NATURAL GAS↗
DOE OSTI2012

State Technologies Advancement Collaborative

The U. S. Department of Energy (DOE), National Association of State Energy Officials (NASEO), and Association of State Energy Research and Technology Transfer Institutions (ASERTTI) signed an intergovernmental agreement on November 14, 2002, that allowed states and territories and the Federal Government to better collaborate on energy research, development, demonstration and deployment (RDD&D) projects. The agreement established the State Technologies Advancement Collaborative (STAC) which allowed the states and DOE to move RDD&D forward using an innovative competitive project selection and funding process. A cooperative agreement between DOE and NASEO served as the contracting instrument for this innovative federal-state partnership obligating funds from DOE's Office of Energy Efficiency and Renewable Energy and Office of Fossil Energy to plan, fund, and implement RDD&D projects that were consistent with the common priorities of the states and DOE. DOE's Golden Field Office provided Federal oversight and guidance for the STAC cooperative agreement. The STAC program was built on the foundation of prior Federal-State efforts to collaborate on and engage in joint planning for RDD&D. Although STAC builds on existing, successful programs, it is important to note that it was not intended to replace other successful joint DOE/State initiatives such as the State Energy Program or EERE Special Projects. Overall the STAC process was used to fund, through three competitive solicitations, 35 successful multi-state research, development, deployment, and demonstration projects with an overall average non-federal cost share of 43%. Twenty-two states were awarded at least one prime contract, and organizations in all 50 states and some territories were involved as subcontractors in at least one STAC project. Projects were funded in seven program areas: (1) Building Technologies, (2) Industrial Technologies, (3) Transportation Technologies, (4) Distributed Energy Resources, (5) Hydrogen Technology Learning Centers, (6) Fossil Energy, and (7) Rebuild America.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2014

Phases 1 & 2—Coal-Based Oxy-Fuel System Evaluation and Combustor Development and Phase 2A—Recovery Act: Oxy-Fuel Turbomachinery Development for Energy Intensive Industrial Applications (Final Report, Rev.1)

Clean Energy Systems, Inc. (CES) partnered with the U.S. Department of Energy’s National Energy Technology Laboratory in 2005 to study and develop a competing technology for use in future fossil-fueled power generation facilities that could operate with near zero emissions. CES’s background in oxy-fuel (O-F) rocket technology lead to the award of Cooperative Agreement DE-FC26-05NT42645, “Coal-Based Oxy-Fuel System Evaluation and Combustor Development,” where CES was to first evaluate the potential of these O-F power cycles, then develop the detailed design of a commercial-scale O-F combustor for use in these clean burning fossil-fueled plants. Throughout the studies, CES found that in order to operate at competitive cycle efficiencies a high-temperature intermediate pressure turbine was required. This led to an extension of the Agreement for, “Oxy-Fuel Turbomachinery Development for Energy Intensive Industrial Applications” where CES was to also develop an intermediate-pressure O-F turbine (OFT) that could be deployed in O-F industrial plants that capture and sequester >99% of produced CO 2 , at competitive cycle efficiencies using diverse fuels. The following report details CES’ activities from October 2005 through March 2013, to evaluate O-F power cycles, develop and validate detailed designs of O-F combustors (main and reheat), and to design, manufacture, and test a commercial-scale OFT, under the three-phase Cooperative Agreement.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2016

Device Scale Modeling of Solvent Absorption using MFIX-TFM

Recent climate change is largely attributed to greenhouse gases (e.g., carbon dioxide, methane) and fossil fuels account for a large majority of global CO 2 emissions. That said, fossil fuels will continue to play a significant role in the generation of power for the foreseeable future. The extent to which CO 2 is emitted needs to be reduced, however, carbon capture and sequestration are also necessary actions to tackle climate change. Different approaches exist for CO 2 capture including both post-combustion and pre-combustion technologies, oxy-fuel combustion and/or chemical looping combustion. The focus of this effort is on post-combustion solvent-absorption technology. To apply CO 2 technologies at commercial scale, the availability and maturity and the potential for scalability of that technology need to be considered. Solvent absorption is a proven technology but not at the scale needed by typical power plant. The scale up and down and design of laboratory and commercial packed bed reactors depends heavily on the specific knowledge of two-phase pressure drop, liquid holdup, the wetting efficiency and mass transfer efficiency as a function of operating conditions. Simple scaling rules often fail to provide proper design. Conventional reactor design modeling approaches will generally characterize complex non-ideal flow and mixing patterns using simplified and/or mechanistic flow assumptions. While there are varying levels of complexity used within these approaches, none of these models resolve the local velocity fields. Consequently, they are unable to account for important design factors such as flow maldistribution and channeling from a fundamental perspective. Ideally design would be aided by development of predictive models based on truer representation of the physical and chemical processes that occur at different scales. Computational fluid dynamic (CFD) models are based on multidimensional flow equations with first principle foundations. CFD models can include a more accurate physical description of flow processes and be modified to include more complex behavior. Wetting performance and spatial liquid distribution inside the absorber are recognized as weak areas of knowledge requiring further investigation. CFD tools offer a possible method to investigating such topics and gaining a better understanding of their influence on reactor performance. This report focuses first on describing a hydrodynamic model for countercurrent gas-liquid flow through a packed column and then on the chemistry, heat and mass transfer specific to CO 2 absorption using monoethanolamine (MEA). The indicated model is implemented in MFIX, a CFD open source software package. The user defined functions needed to build this model are described in detail along with the keywords for the corresponding input file. A test case is outlined along with a few results. The example serves to briefly illustrate the developed CFD tool and its potential capability to investigate solvent absorption.

09 BIOMASS FUELS↗
DOE OSTI2017

Electrification and Decarbonization: Exploring U.S. Energy Use and Greenhouse Gas Emissions in Scenarios with Widespread Electrification and Power Sector Decarbonization

Electrification of end-use services in the transportation, buildings, and industrial sectors coupled with decarbonization of electricity generation has been identified as one of the key pathways to achieving a low-carbon future in the United States. By lowering the carbon intensity of the electricity generation and substituting electricity for higher-emissions fossil fuels in end-use sectors, significant reductions in carbon dioxide emissions can be achieved. This report describes a preliminary analysis that examines the potential impacts of widespread electrification on the U.S. energy sector. We develop a set of exploratory scenarios under which electrification is aggressively pursued across all end-use sectors and examine the impacts of achieving these electrification levels on electricity load patterns, total fossil energy consumption, carbon dioxide emissions, and the evolution of the U.S. power system.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2018

Fundamental Studies of Metal Centered Transformations Relevant to Catalysis

The overall objectives the research performed have been to advance the mission of the U. S. Department of Energy, with specific emphasis concerned with the conversion and use of fossil and renewable energy resources, and the synthesis of advanced chemicals. Achieving this objective requires improvements in rational catalyst design by establishing details of reaction mechanisms and their kinetics. Therefore, over the course of this award, emphasis has been directed towards obtaining detailed information concerned with fundamental transformations that occur at metal centers, with particular attention given towards reactions such as (i) hydrodesulfurization (HDS) and hydrodenitrogenation (HDN), (ii) the use of carbon dioxide as a renewable C1 feedstock, (iii) the generation of hydrogen on demand, and (iv) transformations that involve the cleavage of H–H, C–H and C–C bonds. HDS and HDN are the essential processes for removing sulfur- and nitrogen-containing impurities from crude oil in order to obtain (i) cleaner fuels that minimize environmental pollution and (ii) cleaner chemical feedstocks that are less likely to poison the catalysts that are used for subsequent transformations. The catalysts employed for HDS and HDN are typically molybdenum and tungsten sulfides and, to gain insight into these transformations at the molecular level, we have focused on developing the coordination chemistry of heterocyclic sulfur and nitrogen compounds with molybdenum and tungsten. For example, we obtained the first examples of the cleavage of thiophene C–S bonds by employing molecular molybdenum compounds. The efficient utilization of carbon dioxide as a renewable C 1 source for the synthesis of value added organic chemicals and fuels has prompted much effort towards developing catalytic reactions to functionalize CO 2 . One such approach is hydrosilylation, which can proceed in a stepwise manner to afford a series of products with different levels of reduction, namely silyl formates, silyl acetals, methoxy silanes and methane. Despite the utility of these transformations, however, most catalysts employ precious metals, which operate at elevated temperatures, and control of the level of reduction is challenging. Therefore, it is significant that we have developed zinc and magnesium systems that can achieve hydrosilylation of CO 2 and which may be modified to control the level of reduction. The growing demand for energy requires the development of alternative energy sources that are more sustainable than fossil fuels and have a reduced impact on the environment. In this regard, an attractive energy storage medium is provided by hydrogen, which can, for example, be consumed in a fuel cell with only water as a byproduct. Unfortunately, a problem with using hydrogen in this manner is that present storage and transportation techniques are inadequate. For example, not only does storing liquid hydrogen present a safety risk, considerable energy is also required to liquefy the hydrogen and maintain it in this form. Therefore, we have focused on the application of chemical methods to provide hydrogen on demand. One such method utilizes formic acid as a storage medium and we reported the first examples of molybdenum compounds that serve as catalysts for releasing H 2 from formic acid. The nature of the interaction of a C–H bond with a metal center is of pivotal importance in many transformations of organic molecules, and we have examined several systems to probe how the interaction varies according to whether the metal is molybdenum or tungsten. These studies demonstrate that tungsten exhibits a greater propensity to cleave a C–H bond. While the oxidative addition of C–H bonds to a metal center is well precedented, transformations that feature oxidative addition of C–C bonds are uncommon and so it is noteworthy that we have observed the cleavage of a strong C–C bond that is a component of an unstrained 6-membered aromatic ring. The oxidative addition of dihydrogen to a metal center, and its microscopic reverse, reductive elimination, are two of the simplest yet most important transformations in organometallic chemistry. For example, oxidative addition of dihydrogen is a key step in many transition metal-catalyzed reactions involving H 2 . However, relatively few studies have established in detail the factors that influence the thermodynamics of this transformation. Therefore, it is significant that we demonstrated experimentally that that the energetics of the oxidative addition of H 2 to the six coordinate molybdenum and tungsten halide complexes depends very strongly on the nature of both the metal and the halogen. Deuterium kinetic isotope effects (KIEs) and equilibrium isotope effects (EIEs) serve as versatile tools to infer details about reaction mechanisms. In this regard, primary deuterium isotope effects are often interpreted by using two simple guidelines: (i) the KIE for an elementary reaction is normal (k H /k D > 1) and (ii) the EIE is dictated by deuterium preferring to be located in the site corresponding to the highest frequency oscillator. We have evaluated the applicability of these rules to the interactions of H–H and C–H bonds with a transition metal center and our results question the ability to predict primary EIEs in these systems based on the simple notion that deuterium prefers to occupy the highest frequency oscillator. The key findings are that the EIEs for (i) formation of σ–complexes by coordination of H–H and C–H bonds and (ii) oxidative addition of dihydrogen exhibit unusual temperature dependencies, such that the same system may exhibit both normal (i.e. K H /K D > 1) and inverse (i.e. K H /K D < 1) values.

02 PETROLEUM↗
DOE OSTI2019

Carbon Capture via Crystallization with a Guanidine Ligand

Carbon capture and storage (CCS) is an important strategy aimed at stabilizing the atmospheric CO2 concentration and thereby the global temperature. In conventional fossil fuel-fired power plants, the resulting flue gas is released into the air without any carbon dioxide scrubbing, which gradually increases the atmospheric CO 2 concentration (currently at approximately 409 ppm). Implementation of post-combustion capture (PCC) of carbon dioxide, whereby the CO 2 emitted by power plants is captured and stored into geological repositories, would enable us to continue to use relatively cheap fossil fuels such as coal, natural gas, and oil, but with significantly reduced CO 2 emissions. A recent report by the International Energy Agency indicated that by 2050 CCS could reduce the annual CO 2 emissions by almost 6 gigatones, which represents about 14% of the total carbon emission reduction necessary to limit the global temperature increase by 2 ºC by the end of the 21st century (International Energy Agency, 2016). This goal will be accomplished by developing inexpensive materials that can be used to effectively capture CO 2 and be regenerated with minimal energy penalty. This project helped address this need by introducing new materials and mechanisms for CO 2 capture. The goal of this project was to demonstrate a bench-scale CO 2 capture process based on a novel guanidinium (bi)carbonate crystallization approach, and ultimately develop an energy-efficient and cost-effective technology for CO 2 capture from flue gas. The project built on our recent discovery of a new class of aqueous guanidine sorbents that react with carbon dioxide and crystallize as carbonate or bicarbonate salts of very low aqueous solubility (Brethomé, 2018; Williams, 2019). The resulting guanidinium (bi)carbonate crystals release the CO 2 upon mild heating at 80-120 ºC, which regenerates the guanidine ligands quantitatively (Figure 1). The potential advantage of this crystallization-based approach over traditional amine scrubbing methods (i.e., using aqueous MEA) is that it allows sorbent regeneration by heating the solid crystals alone, without the bulk solution, making this process more energy-efficient.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2019

Engineering Accessible Adsorption Sites in MOFs for CO 2 Capture (Final Report)

The overall goal of this project was to synthesize metal-organic frameworks (MOFs) with improved CO 2 adsorption and selectivity properties for potential application in removing this greenhouse gas from flue gas streams during fossil fuel processing. MOFs are an important class of 2-dimensional (2D) and 3D supramolecular coordination polymer networks that are comprised of organic linkers (ligands) and metal ion-units or clusters. They generally possess very high surface area, porosity, variable thermal stability and tunable chemistry, which make them potentially candidates CO 2 adsorption. The three specific objectives of this project were as follows: 1) To synthesize MOFs with metal ions adsorption sites in more accessible locations within the structures (towards the center of the organic linkers) in order to enhance their CO 2 adsorption characteristics; 2) To investigate the CO 2 adsorption properties of new MOFs containing pyrazine- and other nitrogen containing ligands as possible improved alternatives to known amine-functionalized MOFs; and 3) To investigate the nature of the adsorption sites and mechanism(s) by conducting computational studies on CO 2 adsorption within the MOF structures and compare the results with experimental observations. The main outcomes of this research are as follows. Nitrogen-containing ligands that possesses a diaza-12-crown-4-ether moiety at the center of two phenylcarboxylic acid groups was utilized to synthesize 3D MOFs in which the added transition metal ions (i.e.CO 2 + and Mn2+) were coordinated within the crown moieties. Therefore, the structures had the metal ions in more accessible locations. The new 3D structures, being non-porous however, showed negligible adsorption capacity for CO 2 . The ligand 2,3,5,6,-pyrazinetetracarboxylic acid (PZTC) was successfully used to synthesize four new MOFs, each with one of the following metal ion; Ca2+(1D), Zn2+(2D), Mn2+ (3D) and Gd3+(3D), and with the dimensionality (D) indicated. The Ca-, Zn- and Mn- PZTC-based MOFs had no obvious accessible pores and showed no adsorption capacity for CO 2 . Gd-PZTC structure however, showed promising capacities of 1.0 mmol/g and 0.6 mmol/g at 273K and 298 K respectively. Another nitrogen-containing ligand explored was 2,2’-dinitro- trans-4,4’- stilbenedicarboxylic acid (DNSDC) and in combination with a co-ligand, 2,2’-bipyridine (2,2’-BPY). The combination of DNSDC with CO 2 + and Mn2+ yielded four new thermally stable MOFs that showed significant CO 2 absorption capacities. The experimental CO 2 adsorption capacities varied among the structures, ranging between 1.8 mmol/g at 256 K and 0.8 mmol/g at 298K. The DNSDC-based structures maintained significant stability and capacities over many adsorption cycles at 298K. With 2,2’-diamino- trans-4,4’-stillbene dicarboxylic acid (DASDC) as ligand instead of DNSDC, new 3D MOF structures were also synthesized. The structures however were less stable, and decomposed on activation (exposure to vacuum and or solvents) and therefore showed negligible CO 2 adsorption capacities. The dinitro-stilbene based MOFs showed promising CO 2 adsorption capacities, thermal stabilities and recyclability, and therefore showed potential for application in CO 2 removal from flue gas. The research accomplishments presented herein supports the Department of Energy’s (DOE) Office of Fossil Energy and the National Energy Technology Laboratory (NETL) mission in the area of research that advances the science of coal technologies, specifically carbon capture and storage. The research outcomes can guide rational design/synthesis strategies towards producing advanced materials for CO 2 capture. However, further research is needed in order to develop the materials to meet or exceed capacities and stabilities that are reported for their counterparts.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2019

Engineering Accessible Adsorption Sites in MOFs for CO 2 Capture

The overall goal of this project was to synthesize metal-organic frameworks (MOFs) with improved CO 2 adsorption and selectivity properties for potential application in removing this greenhouse gas from flue gas streams during fossil fuel processing. MOFs are an important class of 2-dimensional (2D) and 3D supramolecular coordination polymer networks that are comprised of organic linkers (ligands) and metal ion-units or clusters. They generally possess very high surface area, porosity, variable thermal stability and tunable chemistry, which make them potential candidates for CO 2 adsorption. The three specific objectives of this project were as follows: 1) To synthesize MOFs with metal ion adsorption sites in more accessible locations within the structures (towards the center of the organic linkers) in order to enhance their CO 2 adsorption characteristics; 2) To investigate the CO 2 adsorption properties of new MOFs containing pyrazine- and other nitrogen containing ligands as possible improved alternatives to known amine-functionalized MOFs; and 3) To investigate the nature of the adsorption sites and mechanism(s) by conducting computational studies on CO 2 adsorption within the MOF structures and compare the results with experimental observations. The main outcomes of this research are as follows: Nitrogen-containing ligands that possess a diaza-12-crown-4-ether moiety at the center of two phenylcarboxylic acid groups were utilized to synthesize 3D MOFs in which the added transition metal ions (i.e. Co 2+ and Mn 2+ ) were coordinated within the crown moieties. Therefore, the structures had the metal ions in more accessible locations. The new 3D structures, being non-porous however, showed negligible adsorption capacity for CO 2 . The ligand 2,3,5,6,-pyrazinetetracarboxylic acid (PZTC) was successfully used to synthesize four new MOFs, each with one of the following metal ions; Ca 2+ (1D), Zn 2+ (2D), Mn 2+ (3D) and Gd 3+ (3D), and with the dimensionality (D) indicated. The Ca-, Zn- and Mn- PZTC-based MOFs had no obvious accessible pores and showed no adsorption capacity for CO 2 . Gd-PZTC structure however, showed promising capacities of 1.0 mmol/g and 0.6 mmol/g at 273K and 298 K respectively. Another nitrogen-containing ligand explored was 2,2’-dinitro- trans-4,4’- stilbenedicarboxylic acid (DNSDC) and in combination with a co-ligand, 2,2’-bipyridine (2,2’-BPY). The combination of DNSDC with Co 2+ and Mn 2+ yielded four new thermally stable MOFs that showed significant CO 2 absorption capacities. The experimental CO 2 adsorption capacities varied among the structures, ranging between 1.8 mmol/g at 256 K and 0.8 mmol/g at 298K. The DNSDC-based structures maintained significant stability and capacities over many adsorption cycles at 298K. With 2,2’-diamino- trans-4,4’-stillbene dicarboxylic acid (DASDC) as ligand instead of DNSDC, new 3D MOF structures were also synthesized. The structures, however, were less stable, and decomposed on activation (exposure to vacuum and or solvents) and therefore showed negligible CO 2 adsorption capacities. The dinitro-stilbene based MOFs showed promising CO 2 adsorption capacities, thermal stabilities and recyclability, and therefore showed potential for application in CO 2 removal from flue gas. The research accomplishments presented herein support the Department of Energy’s (DOE) Office of Fossil Energy and the National Energy Technology Laboratory (NETL) mission in the area of research that advances the science of coal technologies, specifically carbon capture and storage. The research outcomes can guide rational design/synthesis strategies towards producing advanced materials for CO 2 capture. However, further research is needed in order to develop the materials to meet or exceed capacities and stabilities that are reported for their counterparts.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2020

Effect of changes of physical properties on CO2 capture solvents on its absorption rate

Concern over greenhouse gas emissions, such as CO2 from fossil fuel combustion, is leading to new regulations on fossil-fuel fired power generation facilities. Using amine-based solutions for CO2 capture in power plants is the most common method utilized industrially and studied in the laboratory environment. However, a limited number of amines are available for carbon capture research after balancing the capital cost and energy penalty. In the carbon capture process, physical properties such as viscosity, surface tension, wettability, etc. are found to play important roles in solvent performance. In this context, we are exploring an approach to enhance the CO2 capture of amine solvents by tuning the physical properties of the amine solvents by the addition of additives. These additives in the amine solution utilize controlled bubble generation to increase liquid-gas contact surface area. This method can increase mass transfer in the absorber column, specifically at the bottom where the mass transfer is limited. These additives can enhance the CO2 capture efficiency by changing the physical property of the solvent which in turn can lower the capital cost associated with the system. This work can be applied to all common aqueous amine solvent and would be of great interest to those in the CCS community.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2021

An Overview of Policies Influencing Air Pollution from the Electricity Sector in South Asia

The electricity sector is a substantial source of air pollution and associated health problems in South Asia and elsewhere. Fossil-fueled power plants emit a wide variety of harmful pollutants. Those with the greatest health impacts are particulate matter and ozone. Once released into the atmosphere, there is no practical way to remove air pollutants, which means that policies designed to improve air quality have to limit the pollutants before release. However, tackling such pollution is challenging because developing economies also need to provide electricity as a basic necessity for their citizens and as an engine of economic growth. This report provides examples of policies impacting air pollution from the fossil-fuel electricity sector in the South Asian countries of Afghanistan, Bangladesh, Bhutan, India, the Maldives, Nepal, Pakistan, and Sri Lanka. Some of this information was difficult to locate, so this is not a comprehensive study, but rather an overview or "scan" of the sector that includes examples of (1) policies that directly regulate air quality by limiting emissions from specific point sources (by restricting operating hours, for instance), and (2) indirect policies that incentivize or disincentivize polluting activities, such as policies to encourage fuel switching, for example. The report shows (1) the great variation among the policy instruments used in each country, (2) that many countries, especially those that have a mismatch between seasonal demand and resource availability, could improve energy security and reduce air pollution through increased cross-border electricity trade, and (3) some countries have contradictory policies (promoting both coal and renewables, for instance).

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2021

Energy Storage and Power Plant Decommissioning

The report examines three fossil-fuel power plant decommissioning strategies to assess the role of energy storage in enabling an equitable clean energy transition future. The analysis showed how storage could enable reduction of fossil-fuel sources from the grid while enabling increased renewable energy integration into the electric grid. The report offers recommendations for future work, including the need to further develop the non-energy benefit attributes of energy storage systems with a focus on the benefits accrued to local communities to understand past decisions and inform future decision-making tools that account for environmental, economic, and social impacts, particularly those on disadvantaged communities.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2022

Phase I: Natural Gas-Based Energy Storage at Abbott Power Plant

Compressed Natural Gas Energy Storage (CNGES), uses the potential energy of compressed natural gas within an integrated energy storage system. Specifically, an inventory of high-pressure natural gas is stored during off-peak hours in a first stage by controlling the balance of gas entering a pipeline from the transmission system, and in a second stage by using new compressors to fill vessels onsite. The natural gas storage medium is then discharged through an expander-generator to use the potential energy from the gas to generate electricity without combustion. The excess chemical energy stored in the natural gas is integrated with an existing fossil-based asset to provide power generation during peak hours and increase the reliability of the associated fossil generating facility.

03 NATURAL GAS↗
DOE OSTI2023

Cost and Performance Projections for Coal- and Natural Gas-Fired Power Plants

This report provides quantitative estimates of future cost and performance improvements for fossil-fueled power plants equipped with carbon capture developed through the adaption/modification of relevant Aspen Plus ® case study models from published NETL techno-economic analyses. The cost and performance estimates in this report are meant to represent prospective improvements that may be realized for low-carbon-emitting PC and NGCC power plants through robust commercial deployment (e.g., learning by doing) of high TRL technologies as well as additional investments in targeted RD&D activities. The methodology used to develop the estimates in this report is intended to allow direct comparison of the technology improvements with the SOA baseline published in NETL’s Fossil Energy Baseline (Rev 4a) Report.

20 FOSSIL-FUELED POWER PLANTS↗