Carbon Dioxide Conversion into Polycarbonate Diols: A Parametric Study
For presentation at the 2023 AIChE Annual Meeting, Orlando, FL, November 5-10, 2023.
Kanitkar, Swarom↗
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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
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Separation and conversion of carbon dioxide to syngas using a porous ceramic dual membrane in a thermo-electrochemical reactor
A thermo-electrochemical reactive capture apparatus includes an anode and a cathode, wherein the anode includes a first catalyst, wherein the cathode includes a second catalyst, a porous ceramic support positioned between the anode and the cathode, an electrolyte mixture in pores of the ceramic support, and a steam flow system on an outer side of the cathode. The outer side of the cathode is opposite an inner side of the cathode and the inner side of the cathode is adjacent to the ceramic support. In addition, the electrolyte mixture is configured to be molten at a temperature below about 600° C.
Campbell, Patrick↗
Molten Slag Would Boost Coal Conversion
Reactor increases residence time of uncovered char. Near-100percent carbon conversion achievable in reactor incorporating moltenslag bath. Slag maintains unconverted carbon impinging on surface at high temperatures for longer period of time, enhancing conversion.
Ferrall, J. F.↗
Low Carbon Intensity Formic Acid Chemical Synthesis from Direct Air Captured CO 2 Utilizing Chemical Plant Waste Heat - Final Technical Report
The primary objective of Low Carbon Intensity Formic Acid Chemical Synthesis from Direct Air Captured CO 2 Utilizing Chemical Plant Waste Heat (ChemFADAC) is to execute and complete a FEED study for an integrated direct air capture (DAC) and carbon conversion system (together, the DACUS system) co-located at a Nutrien nitric acid production facility in Kennewick, WA capable of capturing and converting a minimum of 5,000 MT/year net atmospheric CO 2 to low carbon intensity formic acid (FA) using industrial waste heat and renewable electricity. The goal will be achieved through the completion of four objectives using a collaborative approach with community stakeholders. Objective 1. Conduct a FEED study and Class 3 project cost estimate for the proposed DACUS system that maximizes use of thermal energy from the Nutrien KFO host site to produce low carbon intensity FA from atmospheric CO 2 . Objective 2. Perform a cradle-to-gate life-cycle analysis of the DACUS system to determine the environmental sustainability and carbon intensity (CI) of the proposed project and product from the results of the FEED study. Objective 3. Perform a business case analysis from results of the LCA, FEED study and cost estimate to justify investment to build the DACUS project at the Nutrien KFO site. Objective 4. Quantify how deployment of the proposed technology will promote and prepare a ready workforce for clean energy and manufacturing jobs and coordinate with community stakeholders to perform an environmental justice and a preliminary economic revitalization and job creation outcomes analysis.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Effect of surfactant assisted ultrasonic pretreatment on production of volatile fatty acids from mixed food waste
In this study, the potential effect of surfactant assisted ultrasonic pretreatment on mixed food waste was investigated. Surfactants, such as Rhamnolipid, Sodium dodecyl sulfate; Glucopon and Triton X 100 were evaluated in this work. Among them, the maximum solubilization of chemical oxygen demand of 45.5 % and the highest release of soluble COD of 31 g/L were observed for ultrasonication assisted by Triton X 100 at a dose of 0.01 g/g TS in 30 min. The presence of a surfactant also reduced 27.5 % of energy demand when compared to ultrasonic pretreatment alone. Compared to the non-pretreated samples after anaerobic digestion, ultrasonication assisted by Triton X 100 led to 95 % increase of volatile fatty acid titers and 83 % increase of carbon conversion efficiency. Furthermore, sonication with the addition of Triton X 100 was proven to be highly effective toward increasing digestibility of and yield of volatile fatty acid from mixed food waste.
59 BASIC BIOLOGICAL SCIENCES↗
An Advanced Pretreatment/Anaerobic Digestion (APAD) Technology for Increased Conversion of Sewage Sludge to Bio-natural Gas in Small-scale Wastewater Plants of less than Five tons Sewage Sludge a Day
The problem today of energy production from sewage sludge at small-scale is that conventional Anaerobic Digestion (AD) as used today at Wastewater Treatment Facilities (WWTF) produces too little energy for warrant use of the biogas. It further leaves 50% or more of the waste behind after the treatment. To overcome this problem, we proposed a novel concept based on Advanced Wet Oxidation & Steam Explosion (AWOEx) of the recalcitrant parts of sewage sludge left behind after AD. We further suggest upgrading biogas to renewable natural gas (RNG) using gaseous fermentation of biogas with hydrogen added by a new methanogen. Overall, the DOE funded Advanced Pretreatment & Anaerobic digestion (APAD) project showed significant improvements over current practice. The project demonstrated that AWOEx followed by AD significantly enhanced the carbon conversion efficiency from 37% to 62%, an increase of 68%. This is far higher than the metric for the specific FOA of an increase of 50%. Besides, the project showed high efficiency of our biological conversion of biogas into RNG when using a new isolate of Methanothermobacter wolfeii resulting in a 100% increased production of a refined biogas with maximum 5% CO2. With both AWOEx pretreatment and biogas upgrading, the project showed a CCE of ca. 83%, far higher than any previous work on sewage sludge. Besides over 200% higher amount of energy in the form of RNG, the APAD concept will reduce disposal cost due to significant reduction in the concentration of final sludge product after APAD. The APAD technology can operate as a bolt-on to a conventional AD plant for improving conversion of the residual organics after AD as done in this DOE project. It can further be implemented as a stand-alone process with AWOEx followed by AD for WWTF’s currently operating without AD.
09 BIOMASS FUELS↗
Non-conventional pathways enable pennycress (Thlaspi arvense L.) embryos to achieve high efficiency of oil biosynthesis
Abstract Pennycress (Thlaspi arvense L.) accumulates oil up to 35% of the total seed biomass, and its overall fatty acid composition is suitable for aviation fuel. However, for this plant to become economically viable, its oil production needs to be improved. In vivo culture conditions that resemble the development of pennycress embryos in planta were developed based on the composition of the liquid endosperm. Then, substrate uptake rates and biomass accumulation were measured from cultured pennycress embryos, revealing a biosynthetic efficiency of 93%, which is one of the highest in comparison with other oilseeds to date. Additionally, the ratio of carbon in oil to CO2 indicated that non-conventional pathways are likely to be responsible for such a high carbon conversion efficiency. To identify the reactions enabling this phenomenon, parallel labeling experiments with 13C-labeled substrates were conducted in pennycress embryos. The main findings of these labeling experiments include: (i) the occurrence of the oxidative reactions of the pentose phosphate pathway in the cytosol; (ii) the reversibility of isocitrate dehydrogenase; (iii) the operation of the plastidic NADP-dependent malic enzyme; and (iv) the refixation of CO2 by Rubisco. These reactions are key providers of carbon and reductant for fatty acid synthesis and elongation.
13C-labeling↗
Innovative Polyhydroxyalkanoates (PHA) Production with Microbial Electrochemical Technology (MET)
The project “Innovative Polyhydroxyalkanoates (PHA) Production with Microbial Electrochemical Technology (MET)” addressed food waste disposal challenges by successfully converting food waste to bioplastics (known as PHAs). The novel process created by our team of researchers from universities, national labs, and industry substantially enhanced overall carbon conversion efficiency of food waste processing (> 50%), while reducing disposal costs (> 25%). The project showed economic viability potential at community scale through pilot-scale demonstration at a relevant scale (50 L reactor volume) with more than 100 hours of PHA production using realistic conditions. The project goal was to valorize food waste by shunting traditional anaerobic digestion processing and creating a value-added PHA processing route that improves the economics and sustainability of local, community-scale, wet organic waste treatment. First, the food waste undergoes microbial-based, dark fermentation to break down the food to small carbon chains known as volatile fatty acids (VFAs). Instead of microorganisms converting the VFAs into methane using normal anaerobic digestion processing, our innovative process inhibits methane production. This preserves the produced VFAs for extraction and use by a novel Haloferax mediterranei (HM) archaea, which effectively converts the VFAs to bioplastics. The project added microbial electrochemical cells (MEC) to the dark fermentation process to enhance the VFAs produced and optimize the type of bioplastics formed.
36 MATERIALS SCIENCE↗
Computationally guided synthesis of carbon coated mesoporous silica materials
Mesoporous silica materials (MSMs) are well-suited for biomedical applications due to their unique features, including a large surface area and tunable pore size. To enhance their durability, the small pores in MSMs are filled with carbon precursors and then carbonized to prevent them from interacting with unreacted silicic acid. Here, in this study, we synthesized and healed MSMs using a combination of non-reactive and reactive molecular dynamics (MD) simulations. The non-reactive MD simulation revealed that the self-assembly of Pluronic® L64 polymers in water resulted in nearly 80 % hydrogen bonds between the hydrophilic sections of the micelle and water. In the bond-boosted ReaxFF MD simulations, silicic acid precursors were condensed on the micelle surface, with over 60 % of them leading to the creation of periodic mesoporous silica within the system. Condensation of silicic acid precursors at 300 K with bond-boosting and at 1500 K without it both significantly promoted the polymerization of Si(OH) 4 , with the latter doubling the rate compared to the former. Subsequently, we healed the MSM surface by carbonizing carbon precursors inside an MSM pore. Polyethylene (PE) and high-rank lignite were identified as the most suitable precursors due to their ability to form turbostratic graphene structures. High-rank lignite exhibited the highest carbon conversion ratio to 6-membered rings, closely followed by PE, in the carbon ring formation analysis. Additionally, the production of gases, such as H 2 , increased significantly for PE at both 2200 K and 2600 K, indicating the conversion of a considerable portion of carbon into graphitic or turbostratic structures. The carbonization of PE primarily led to the formation of planar (sp 2 ) structures, while sucrose yielded the least planar structures. Finally, we studied the protective blocking of unreacted silicic acid precursor by considering a PET turbostratic graphene structure in a silica mesopore formed at 2600 K. The trajectory analysis showed that the surface of the silica was effectively coated with PET tar, preventing unreacted silicic acid from interacting with the inner silica pore surface. These findings offer valuable insights into the synthesis and carbonization-based healing processes of MSMs, enhancing their potential for various biomedical applications.
36 MATERIALS SCIENCE↗
Progress in understanding and improving oil content and quality in seeds
The world’s population is projected to increase by two billion by 2050, resulting in food and energy insecurity. Oilseed crops have been identified as key to address these challenges: they produce and store lipids in the seeds as triacylglycerols that can serve as a source of food/feed, renewable fuels, and other industrially-relevant chemicals. Therefore, improving seed oil content and composition has generated immense interest. Research efforts aiming to unravel the regulatory pathways involved in fatty acid synthesis and to identify targets for metabolic engineering have made tremendous progress. This review provides a summary of the current knowledge of oil metabolism and discusses how photochemical activity and unconventional pathways can contribute to high carbon conversion efficiency in seeds. It also highlights the importance of 13 C-metabolic flux analysis as a tool to gain insights on the pathways that regulate oil biosynthesis in seeds. Finally, a list of key genes and regulators that have been recently targeted to enhance seed oil production are reviewed and additional possible targets in the metabolic pathways are proposed to achieve desirable oil content and quality.
59 BASIC BIOLOGICAL SCIENCES↗
Characterization of Coal Seam Produced Water from the Appalachian Basin: Geochemistry, Microbiology, and Biocatalyst Development for Biological CO 2 Conversion
To enhance domestic energy repositories, it is necessary to develop carbon utilization technologies to repurpose unused carbon sources, and/or enhance the economic viability and carbon conversion efficiency of current technologies. To this end we have developed a biocatalyst, enriched from coal seam produced water, to convert gaseous and liquid C1 compounds (e.g. CO 2 , bicarbonate, formate, and/or methanol) into acetate, a C2 organic acid with a projected global market size of $\$$32.4 billion USD by 2030.
01 COAL, LIGNITE, AND PEAT↗
Midwest Regional Carbon Conversion/Utilization Procurement Grant Workshop
https://events.usea.org/events/midwest-regional-carbon-conversionutilization-procurement-grant-workshop As the U.S. economy moves toward clean energy and a lower carbon future, the U.S. Department of Energy (DOE) is seeking to partner with states, communities, and industries to support the procurement and development of carbon conversion products. These efforts have been enabled by provisions included in the Bipartisan Infrastructure Law (BIL). As part of the BIL, supporting the Administration’s goal to achieve a carbon-free power sector by 2035 and putting the United States on a path to a net-zero economy by 2050, a new initiative was established within DOE’s Office of Fossil Energy and Carbon Management through its Carbon Conversion/Utilization Program. The new initiative will establish a demonstration grant program to issue grants to eligible entities to procure commercial and industrial products derived from the conversion of anthropogenic carbon oxides and demonstrate a significant net reduction in life cycle greenhouse gas emissions compared to incumbent technologies, processes, and products. DOE-FECM will establish a demonstration grant program within the Carbon Conversion/Utilization Program to support eligible applicants that procure those commercial and industrial products derived from anthropogenic carbon oxides. Therefore, the Carbon Conversion/Utilization Program, with the assistance of the United States Energy Association (USEA), will conduct a series of workshops (both virtual and in-person) with relevant stakeholders, e.g., product manufacturers, eligible entities, or their representative national organizations (e.g., United States Conference of Mayors, etc.) to solicit input and ideas on challenges and opportunities for a potential grant program.
Larimore, Ryan↗
Production of Bioproducts from Electrochemically-Generated C1 Intermediates
The overarching objective of the project was to develop an integrated process that converts carbon dioxide (CO 2 ) into the platform chemical isopropanol (IPA) using a combination of two key technologies: CO 2 electrolysis and gas fermentation. The final goal was to demonstrate the full process at bench scale with a minimum carbon conversion efficiency of 37% and to evaluate the economics and environmental impact of scaling up the electrochemical-biochemical process.
30 DIRECT ENERGY CONVERSION↗
Overview of NETL’s Low Temperature CO2 Electrolysis Research
This keynote lecture will briefly overview diverse research areas of National Energy Technology Laboratory (NETL) to advance energy and environmental sustainability along with carbon management. Our electrochemistry efforts on carbon conversion directly support the US goal of achieving carbon-free power sector by 2035 and net zero emissions by 2050. Since CO2 electroreduction is highly structure-sensitive, NETL ongoing research has been focused on the rational design and engineering of electrocatalysts to facilitate the CO2 conversion to desirable products with good selectivity, activity, and durability. Different classes and types of electrocatalytic materials will be covered in this talk, from well-defined atomic-scale model catalysts to heterogenous, scalable powder systems at nano- and micro-scale for “real world” performance evaluation. Several spectroscopic, microscopic, and electrochemical characterization techniques along with computational findings will be additionally discussed to gain more insights into the structure-activity relation. The last part of this seminar will provide more detail on how NETL has transitioned from the most common aqueous H-type reactor for lab-scale validation to more realistic full electrolyzer cell in bench-scale prototype. The knowledge, electrocatalytic materials, and device validation achieved from NETL in-house research will be translated to industrial sector for large scale deployment and the anticipated outcome will help advance the development of low temperature CO2 electrolysis technologies.
Nguyen Phan, Thuy Duong↗
Analysis of Waste Material Feedstocks Using Laser-Induced Breakdown Spectroscopy and Machine Learning
Predicting properties such as heating value, ash fusion temperature, and mineral ash composition from Laser-Induced Breakdown Spectroscopy (LIBS) data can make gasifiers more flexible to different feedstocks. Understanding these feedstock properties in-situ improves feedstock conversion modelling methods that allow for consistent operation, higher carbon conversion, and reduced fouling and erosion rates. The purpose of this study is to demonstrate methods for model creation that take LIBS data as predictor features and estimate higher order material properties as a function of feedstock material properties. Six samples were chosen to represent a mixture of abundant and carbon rich waste materials. LIBS measurements were performed on these samples for elemental wavelengths and intensity values. Laboratory analytical results were obtained for each sample’s heating value, proximate and ultimate analysis, mineral ash composition, ash fusion temperatures, and viscosity temperatures. Thermal conductivity was measured using a HotDisk TPS 2500S. LIBS measurements were processed and used as predictor features for machine learning (ML) models to predict the sample’s material properties. Predictor feature selection algorithms, particularly minimum redundancy maximum relevance (mRMR), reduced the dimensionality of ML models. Many modelling methods such as Gaussian process regression (GPR), regression tree, neural networks (NN), and support vector machines (SVM) were demonstrated to be effective at predicting higher order properties; however, mRMR with GPR stood out as a clear winning combination.
01 COAL, LIGNITE, AND PEAT↗
How is Rational Design of Electrocatalysts Crucial for Maximizing CO2 Electroreduction Performance?
The invited talk "How is Rational Design of Electrocatalysts Crucial for Maximizing CO2 Electroreduction Performance?” was presented in the symposium "Electrocatalysis for Sustainable Energy and Biomass Conversion: Fundamentals, Applications, and Perspectives”, Division of Catalysis Science and Technology, 2024 ACS Fall Meeting. The presentation briefly introduces NETL facilities and our Electrochemical Carbon Conversion portfolio to audiences. The talk primarily discusses how the geometry and surface composition of copper- and tin-based electrocatalysts would maximize the CO2 conversion to sustainable, carbon-neutral gas and liquid products in different device configurations. Ex situ and in situ characterization results are additionally discussed to correlate the structural, physico-chemical, and electronic properties with CO2 reduction activity and selectivity.
Nguyen Phan, Thuy Duong↗
Improving Carbonate-Promoted C–H Carboxylation Using Mesoporous Carbon Supports
C–H carboxylation is an attractive way to utilize CO 2 for chemical production provided that it does not consume resource-intensive reagents. Alkali carbonates dispersed into the pores of mesoporous supports display strongly basic reactivity under CO 2 , allowing them to be used as base promoters for C–H carboxylation of (hetero)arenes in the absence of other reagents or catalysts. Mesoporous oxides are convenient support materials, but only a relatively small fraction of the dispersed carbonate (ca. 10-20%) is converted to carboxylate products when metal oxide supports are used. Here we compare mesoporous oxide and carbon supports and investigate the dependence of carbonate reactivity on pore structure. We show that using mesoporous carbons supports can increase the carbonate conversion by 2–4x when compared to oxide supports. This improved carbonate reactivity is maintained across a variety of mesoporous carbons with different pore structures (ordered vs. disordered) and pore diameters, indicating that the dispersed carbonate is intrinsically more reactive on the surface of a carbon material compared to an oxide surface. Reaction of the carboxylate products with dimethyl carbonate yields isolable methyl esters as the final product and regenerates the dispersed carbonate. We show that mesoporous carbon supports are robust to at least 5 cycles of successive C–H carboxylation and methylation with dimethyl carbonate. Furthermore, understanding how the support structure affects dispersed carbonate reactivity is valuable for advancing C–H carboxylation toward practical application and utilizing these materials in other CO 2 transformations.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Proteomic approaches for advancing the understanding and application of oleaginous bacteria for bioconversion of lignin to lipid
Biological conversion of current cellulosic biorefinery lignin waste is important for complete valorization of all biomass carbons by biofuels and biochemical production. However, the deconstruction of lignin's complex polymeric framework into intermediates amenable to assimilation and subsequent lipid production for biofuels has proven challenging. Recent systems biology advances have shown promise in facilitating the bioconversion of lignin to lipids. Proteomics-guided synthetic biology approaches have proven to be effective tools for defining and designing new pathways. These pathways may help achieve optimal carbon conversion efficiency of biomass. Nevertheless, substantial challenges remain for the economic conversion of lignin to fuel. Herein, we review salient problems in the bacterial conversion of lignin to lipids with an emphasis on lignin depolymerization activities, in vivo aromatic degradation pathways, and recent advances in lipid production by oleaginous bacteria. Several mass spectrometry-based proteomics technologies and their applications to oleaginous bacteria are highlighted in this review. Together, these studies will help establish a system-level understanding of lignin bioconversion and drive efforts to build a platform for the maximal conversion of lignocellulosic biomass to economical next generation biorefinery.
Li, Xiaolu↗