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All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Directed surfaces structures and interfaces for enhanced electrocatalyst activity, selectivity, and stability for energy conversion reactions

In this project, we have employed a systematic approach to develop active, selective, and stable catalyst materials for important electrochemical reactions involving energy conversion. In particular, we have focused our attention on developing active catalyst materials for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). HER: We have synthesized and investigated several highly active and acid stable non-precious metal HER catalysts, including: [Mo 3 S 13 ] 2- nanoclusters (Nature Chemistry, 2014) and molybdenum phosphosulfide (MoP|S) (Angewandte Chemie, 2014). We have also aimed to engineer these catalyst formulations in a membrane electrode assembly (MEA) for fundamental studies of water electrolysis at high current densities, approximately 1 A/cm 2 (ChemSusChem, 2015). We furthermore investigated transition metal phosphide (TMP) catalysts for HER by a combined experimental–theoretical approach (Energy & Environmental Science, 2015). By synthesizing different TMPs and comparing experimentally determined HER activities with the hydrogen adsorption free energies, ΔG H , calculated by density functional theory, we showed that the TMPs follow a volcano relationship for the HER. Using our combined experimental–theoretical model, we predicted that the mixed metal TMP, Fe 0.5 Co 0.5 P, should have a near-optimal ΔG H . We synthesized several mixtures of Co and Fe phosphides alloys and confirmed that Fe 0.5 Co 0.5 P exhibits the highest HER activity of the investigated TMPs (Energy & Environmental Science, 2015). The understanding gained as to how to improve catalytic activity for the HER, particularly for non-precious metal materials, is important to DOE targets for sustainable H 2 production. OER: We have developed a SrIrO 3 /IrO x catalyst for acidic conditions (submitted, 2016). The SrIrO 3 /IrO x catalyst significantly outperforms rutile IrO 2 and RuO 2 , the only other OER catalysts to have reasonable stability and activity in acidic electrolyte, and in fact demonstrates the best activity for any known OER catalyst measured in either acidic or in alkaline electrolyte. For alkaline conditions we have demonstrated that the combined effect of cerium as a dopant and gold as a metal support, significantly enhances the OER activity of electrodeposited NiO x films. This NiCeO x -Au catalyst delivers high OER activity in alkaline media, and is among the most active OER electrocatalysts reported to date (Nature Energy, accepted 2016). These studies of new catalysts for the OER, both in acid and in base, are fundamental to enabling new technologies of interest for the DOE, including the production of sustainable fuels and chemicals. ORR: One method to significantly reduce the Pt loading in fuel cell devices is to increase the ORR activity of Pt based systems. To this end we have synthesized a high surface area supported meso-structured Pt x Ni alloy thin film with a double gyroid morphology that both exhibits high activity and stability for the ORR (submitted, 2016). We have furthermore developed a Ru-core, Pt-shell system that improves the per Pt site activity by more than a factor of 2 (ChemElectroChem, 2014). Further refinement, optimizing Pt-shell thickness and reducing particle sintering during processing, enabled us to obtain a mass activity that is 2 times higher than commercial Pt/C from TKK. These are important contributions to the DOE goal of reducing Pt loading since an improved understanding of how to increase mass activity and stability helps enable low Pt content fuel cells.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2014

Process Design and Economics for the Conversion of Algal Biomass to Biofuels: Algal Biomass Fractionation to Lipid-and Carbohydrate-Derived Fuel Products

The U.S. Department of Energy (DOE) promotes the production of a range of liquid fuels and fuel blendstocks from biomass feedstocks by funding fundamental and applied research that advances the state of technology in biomass production, conversion, and sustainability. As part of its involvement in this program, the National Renewable Energy Laboratory (NREL) investigates the conceptual production economics of these fuels. This includes fuel pathways from lignocellulosic (terrestrial) biomass, as well as from algal (aquatic) biomass systems.

09 BIOMASS FUELS↗
DOE OSTI2017

Final Research Performance Progress Report: Geothermal Resource Development with Zero Mass Withdrawal, Engineered Convection, and Wellbore Energy Conversion

This project is intended to demonstrate the technical and economic feasibility, and environmental and social attractiveness of a novel method of heat extraction from geothermal reservoirs. The emphasis is on assessing the potential for a heat extraction method that couples forced and free convection to maximize extraction efficiency. The heat extraction concept is enhanced by considering wellbore energy conversion, which may include only a boiler for a working fluid, or perhaps a complete boiler, turbine, and condenser cycle within the wellbore. The feasibility of this system depends on maintaining mechanical and hydraulic integrity of the wellbore, so the material properties of the casing-cement system are examined both experimentally and with well design calculations. The attractiveness depends on mitigation of seismic and subsidence risks, economic performance, environmental impact, and social impact – all of which are assessed as components of this study.

15 GEOTHERMAL ENERGY↗
DOE OSTI2017

An Overview of Natural Gas Conversion Technologies for Co-Production of Hydrogen and Value-Added Solid Carbon Products

This report was prepared in response to the U.S. Department of Energy Fuel Cell Technologies Office Congressional Appropriation language to support research on carbon-free production of hydrogen using new chemical processes that utilize natural gas to produce solid carbon and hydrogen. The U.S. produces 9-10 million tons of hydrogen annually with more than 95% of the hydrogen produced by steam-methane reforming (SMR) of natural gas. SMR is attractive because of its high hydrogen yield; but it also converts the carbon to carbon dioxide. Non-oxidative thermal decomposition of methane to carbon and hydrogen is an alternative to SMR and produces CO 2 -free hydrogen. The produced carbon can be sold as a co-product, thus providing economic credit that reduces the delivered net cost of hydrogen. The combination of producing hydrogen with potentially valuable carbon byproducts has market value in that this allows greater flexibility to match the market prices of hydrogen and carbon. That is, the higher value product can subsidize the other in pricing decisions. In this report we highlight the relevant technologies reported in the literature—primarily thermochemical and plasma conversion processes—and recent research progress and commercial activities. Longstanding technical challenges include the high energetic requirements (e.g., high temperatures and/or electricity requirements) necessary for methane activation and, for some catalytic processes, the separation of solid carbon product from the spent catalyst. We assess current and new carbon product markets that could be served given technological advances, and we discuss technical barriers and potential areas of research to address these needs. We provide preliminary economic analysis for these processes and compare to other emerging (e.g., electrolysis) and conventional (e.g., SMR) processes for hydrogen production. The overarching conclusion of this study is that the cost of hydrogen can be potentially reduced to target levels of $2/kg with the co-production and sale of a sufficiently high-value carbon product. Technological advances are required to understand the reaction conditions and design reactor systems that can achieve high yields of the select carbon products and segregate or separate the high-value carbon products, and optimize the production process for both hydrogen and carbon.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2018

Coiled Tube Gas Heaters For Nuclear Gas-Brayton Power Conversion

This project developed an alternative design for heat exchangers for application to heating supercritical carbon dioxide (S-CO 2 ) or air for power conversion. We have identified an annular coiled tube bundle configuration–where hot sodium enters tubes from multiple vertical inlet manifold pipes, flows in a spiral pattern radially inward and downward, and then exits into an equal number of vertical outlet manifold pipes–as a potentially attractive option. The S-CO 2 gas or air flows radially outward through the tube bundle. Coiled tube gas heaters (CTGHs) are expected to have excellent thermal shock, long-term thermal creep, in-service inspection, and reparability characteristics, compared to alternative options. CTGHs have significant commonality with modern nuclear steam generators. Extensive experience exists with the design, manufacture, operation, in-service inspection and maintenance of nuclear steam generators. The U.S. Nuclear Regulatory Commission also has extensive experience with regulatory guidance documented in NUREG 0800. CTGHs leverage this experience and manufacturing capability. The most important difference between steam generators and gas-Brayton cycles such as the S-CO 2 cycle is that the heat exchangers must operate with counter flow with high effectiveness to minimize the pinch-point temperature difference between the hot liquid coolant and the heated gas. S-CO 2 -cycle gas heaters also operate at sufficiently elevated temperatures that time dependent creep is important and allowable stresses are relatively low. Designing heat exchangers to operate in this regime requires configurations that minimize stresses and stress concentrations. The cylindrical tubes and cylindrical manifold pipes used in CTGHs are particularly effective geometries. The first major goal of this research project was to develop and experimentally validate a detailed, 3-D multi-phase (gas-solid-liquid) heat transport model for CTGHs, using methods similar to earlier UCB multi-scale models for PCHEs, which will enable optimization of CTGH designs with respect to the number of manifold pipes, S-CO 2 and sodium circulating power, and other design parameters. CTGHs are relatively novel because the tubes loaded in compression as well as the manifold pipes which form the tube sheets. The second major goal of the experimental and modeling effort was to optimize the assembly and heat treatment of the tube-to-tubesheet joints, using a novel tapered joint configuration, and to develop diffusion-bonded joints with high shear strength and creep resistance, as has been done in other applications for tapered plugs. The project would also conduct creep testing of these tubesheet joints in pressurized furnaces under prototypical conditions of stress and temperature, however this was not feasible due to numerous hinderances. Detailed microstructural investigations was conducted on the diffusion bond interface, while the bond strength was evaluated by tensile testing. The mechanical testing quantified the overall strength of the bond and measured the pull out force as well as long term behavior, which complemented the microstructural analysis and gave a complete understanding of the diffusion bond.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2018

Advanced Gasification and Novel Transformational Coal Conversion Technologies Development: Final Technical Report

This report summarizes the work carried out in furtherance of the NETL/DOE award, OTM-Enhanced Coal Syngas for Carbon Capture Power Systems and Fuel Synthesis Applications. The overall objective of the project was to further develop Oxygen Transport Membrane (OTM) technology and assess the potential for integration in coal power generation. OTM technology has the potential to enhance the quality of syngas produced by coal gasifiers, reduce the amount of cryogenic-derived oxygen required in Integrated Gasification Combined Cycle (IGCC) power plants, and allow for coal and natural gas integration. Process simulations and techno-economic analyses were carried out to estimate the cost and performance of OTM enhanced IGCC plants, IG-NGCC plants, and OTM enhanced Fischer Tropsch (FT) Liquids from coal and natural gas plants. The OTM enhanced power plants achieved higher carbon capture rates, higher efficiencies, and lower cost of electricity compared to the base cases. The most significant benefits were achieved for cases which used low rank coal as the feed. Fischer-Tropsch coal to liquids plants with iron-based catalysts and natural gas integration utilizing OTM technology showed improved carbon conversion, improved thermal efficiency and lower cost of production. With respect to OTM core technology development, significant advances have been made in several areas. The development and implementation of a third-generation membrane materials and manufacturing process has resulted in the availability of robust and reliable, high performance membranes, that can be manufactured at high yield. Progress towards the goal of higher pressure operation has been demonstrated with the development of improved metal-ceramic seals and components of the panel array module that integrate membrane-seal assemblies with primary and secondary reforming catalysts have been further developed and demonstrated. Work concluded with the successful start-up and operation of a multi-panel pilot-scale system which is the final step in technology development ahead of demonstration.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2019

Conversion of Shale Gas to Value-added Chemicals

OxEon Energy evaluated a catalytic process to directly convert methane to ethylene at high conversion and selectivity. The process uses a dual catalyst reactor where the first catalyst activates methane to produce active radicals which are combined over the second catalyst to form ethylene.

04 OIL SHALES AND TAR SANDS↗
DOE OSTI2018

One-pot catalytic conversion of biomass and alkanes: Kinetically coupling deoxygenation and dehydrogenation pathways

The stoichiometric hydrogen deficiency of carbohydrate feedstock implies that all conversion processes must remove oxygen and concurrently increase hydrogen content to form liquid hydrocarbon products. With support from the DOE Early Career program (DE-SC0008418) we have investigated the use of transition metal carbides for hydrodeoxygenation (HDO) chemistries using CH 4 and H 2 as co-reactants. We report that concurrently processing CH 4 and C 1 -C 3 oxygenates (oxygenate/CH 4 = 0.01-0.1) at 950 K on molybdenum carbide clusters encapsulated in zeolite micropores results in a staged bed with upstream CH 4 reforming and downstream CH 4 dehydroaromatization. Forward rates of CH 4 pyrolysis limited by CH 4 activation are unperturbed by the introduction of oxygenates with a (C/H) eff <0.25 after rigorously accounting for the thermodynamic reversibility caused by the H 2 produced in oxygenate reforming reactions and the fraction of the active catalyst bed deemed unavailable for CH 4 dehydroaromatization. A binomial distribution of 12 C/ 13 C isotopologues of CO is observed upon introduction of CH 3 13 COOH/CH 4 reactants suggesting that the introduction of oxygenates with a (C/H) eff <0.25 results in complete fragmentation of the oxygenate at these temperatures which in turn results in the invariance of forward rates of CH 4 pyrolysis when using CO 2 , HCOOH, or CH 3 COOH co-feeds. The stoichiometric loss of oxygen as CO when co-processing C 1 -C 3 oxygenates and CH 4 at these temperatures demonstrates that (C/H) eff =(C-O)/H is a single valued descriptor for oxygen removal on Mo/HZSM-5 catalysts. Separately, we have demonstrated the utility of transition metal carbides for vapor phase catalytic hydrodeoxygenation using molecular hydrogen with high selectivity for C-O cleavage and near absence of sequential hydrogenation reactions at atmospheric hydrogen pressure and illustrated that the faculty of transition metal carbides for selective hydrodeoxygenation arises due to oxygen-modification of the catalyst in situ. The oxophilic characteristics of these materials engender both the observed acid-metal catalytic bifunctionality and selectivity for hydrodeoxygenation. The evolution of catalyst surface composition and catalytic function under oxidative reaction environments proffers unique challenges in structural characterization of these materials and in this context, we developed and demonstrated the use of chemical titration and chemical transient studies to assess catalytic site identity and densities.

09 BIOMASS FUELS↗
DOE OSTI2020

Spatial Atomic Layer Deposition to Scale Manufacturing of Robust Catalysts for Biomass Conversion Applications: Cooperative Research and Development Final Report, CRADA Number CRD-17-715

This CRADA will facilitate technology maturation for NREL-developed ALD-coated catalyst materials that are tailored for durability during harsh biomass conversion chemistries. This project will address optimizing process parameters for scale-up of Al2O3 ALD-coated catalysts, demonstrating ALD-coated catalyst performance for muconic acid hydrogenation, and validating economic models that project significant cost benefits for ALD-enhanced catalytic processes. This work will strengthen private-public partnerships in the area of advanced catalyst manufacturing for energy-related technology. Critical information will be collected to elevate the Technology Readiness Level and increase our competitiveness for cooperative R&D agreements and licensing. Success of this work will be crosscutting as it can facilitate advanced catalyst development for both renewable and conventional processes.

09 BIOMASS FUELS↗
DOE OSTI2020

Integration of a Microturbine Power Conversion Unit in MAGNET

The Microreactor Agile Non-nuclear Experimental Testbed (MAGNET) facility is being constructed at Idaho National Laboratory’s (INL’s) Energy Systems Laboratory to assist with the development, demonstration, and validation of microreactor components and systems. MAGNET will accommodate various types of test articles representative of different microreactor designs. A power conversion unit (PCU) simulator loop was proposed to use the rejected heat from the test article and mimic the thermal hydraulic conditions (e.g., temperature, pressure and flow rate) that would be experienced if an actual Brayton cycle PCU was attached. However, due to the high-estimated cost of the PCU simulator and the availability of a turbogenerator used for previous testing at Sandia National Laboratories, the PCU simulator design was abandoned in favor of integrating an actual PCU into MAGNET. A commercial Capstone C30 was modified by Sandia to use external electrical heating, rather than combustion heating, to provide a power output from 1 to ~30 kWe. The C30 has a single-stage centrifugal combustor, a static radial heat exchanger, and a radial inflow turbine arranged on a single shaft with a high-speed alternator. Since the operating temperature and energy transfer per unit working fluid mass are comparable, the MAGNET PCU will provide researchers with the ability to evaluate the test article heat transfer under representative operating conditions with the transient system behavior associated with a closed Brayton cycle PCU. This report examines the integration of a modified commercial Capstone C30 turbogenerator into MAGNET, outlines a proposed set of tests, and describes future work.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2023

Intensified Catalytic Conversion of CO2 into High Value Chemicals

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

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2023

Accelerating Additive Manufacturing Process Design for Energy Conversion Materials using In-situ Sensing and Machine Learning

One promising candidate for manufacturing of the bismuth Telluride thermoelectric legs is laser powder bed fusion (LPBF) additive Manufacturing (AM). AM processing parameters highly influence the material properties, however current processing parameter development methods in AM are costly and time consuming. In-situ sensors allow for the capture of physically relevant process information on a layer-by-layer basis and will be used to aide process development. To optimize the AM process for the best thermoelectric performance, process variables, in-situ process sensor data and ex-situ material characterization data are collected. Several different interpretable machine learning (ML) approaches are used, and the performance of each method are assessed. Significant input process variables include laser focus, hatch spacing and laser power. The best performing models are used to determine the manufacturing parameters that maximize the power factor. AM of bismuth telluride material provides the ability to create complex geometries enabling more efficient energy conversion.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2023

High-Efficiency Electrochemical Conversion of CO 2 to Ethylene

During the past century, our civilization’s technological advances have been driven by the conversion of carbon-rich fossil fuels into electricity, heat, polymers, fertilizers, and other carbon-based products that are the foundation of modern society. It is now clear, however, that this carbon economy is no longer sustainable for humanity or our ecosystem. A study by the National Academies showed that to avoid catastrophic climate change, we not only need to dramatically and rapidly reduce global emissions of CO 2 , but we will need to remove billions of tons of CO 2 from the earth’s atmosphere and oceans by mid-century. This presents a massive, unprecedented challenge to our species, but if managed well it also represents a historic opportunity: capture and utilization of CO 2 is arguably the largest economic opportunity of the next hundred years, also known as “industry of the future”.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Harnessing photoautotroph-methanotroph interactions for biogas conversion to fuels and chemicals using binary consortia (Project Final Technical Report)

Industrial, municipal, and agricultural waste streams containing stranded organic carbon represent a significant and underutilized feedstock to produce fuels and chemicals. With anaerobic digestion deployed at large scales to capture organic waste streams, over 6 million tons of biogas are available today. However, the utilization of biogas represents a significant challenge due to its low pressure and presence of contaminants such as H 2 S, ammonia, and volatile organic carbon compounds. To tap into this immense potential, effective biotechnologies that co-utilize both CO 2 and CH 4 are needed. Recent studies demonstrated that, in nature, microbial communities have developed a highly efficient way to recover energy and capture carbon from both CH 4 and CO 2 through metabolic coupling of methane oxidation to oxygenic photosynthesis. Using two synthetic methanotroph – photoautotroph (M-P) co-cultures that exhibit stable growth under a broad range of cultivation conditions, in this project we proposed to harness the interspecies interactions within these cocultures for biogas conversion to fuels and chemicals. To facilitate this overarching objective, we aim to develop experimental and computational tools to gain qualitative and quantitative understandings on the interactions and dynamics of the coculture at both systems and molecular levels, and to validate our findings through experiments and mutant development. The fundamental understanding on the interactions and dynamics of the photoautotroph-methanotroph will lay the foundation for the design and optimization of synthetic binary consortia for production of fuels and chemicals from biogas. We expect the knowledge gained from this project may be generally applicable to other cross-feeding binary consortium, and the tools developed can be adapted to study the interactions and dynamics of other multi-organism platforms.

09 BIOMASS FUELS↗
DOE OSTI2025

Development of a scalable, robust electrocatalytic technology for conversion of CO 2 to formic acid via microstructured materials

This project was funded by the Bioenergy Engineering for Product Synthesis (BEEPS) program under the Funding Opportunity Announcement (FOA) DE-FOA-0001916 Topic Area 5 “Rewiring Carbon Utilization”. This FOA sought projects that would electrocatalytically reduce CO 2 to a carbon intermediate and then upconvert to a multi-carbon product or fuel via non-photosynthetic biological system engineering. The project sought to combine the expertise of OCO Chem, whose chief scientist had previously developed an efficient electrocatalytic reactor for conversion of CO 2 to formate with potential to scale, Montana State University investigators who had recently patented a method for laterally grading membranes with the potential of improving reactant distribution and more uniform efficiency across membrane-based reactors, and University of South Florida which had recently discovered a novel C-C bond forming reaction not known to naturally occur in biological systems and which uses C1 substrates and circumvents the central microbial metabolism.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Comprehensive Life Cycle Analysis of Methanol Production and Methanol-to-Diesel Conversion

Methanol is a strategic chemical and intermediate in the manufacture of synthetic diesel, due to its versatility, diesel’s compatibility with existing infrastructure, and their role in industrial and transport applications. Conventional production methods for methanol, primarily steam methane reforming (SMR), rely on natural gas and are subject to the price variability due to market conditions and geopolitical events. They are also associated with greenhouse gas (GHG) emissions. Methanol and synthetic diesel production could be integrated with nuclear energy to stabilize fuel prices and insulate pricing from outside geopolitical events due to the relative stability of nuclear fuel as compared to natural gas. This could lead to increased transportation fuel security, reliability and resilience. An added benefit is the abatement of emissions when substituting nuclear energy for conventional energy from natural gas. This report presents a comprehensive life cycle analysis(LCA) framework which was developed to evaluate the GHG emissions reduction potential associated with nuclear integrated methanol production, methanol-to-diesel upgrading, and end-use combustion. Gate-to-gate methanol production and cradle-to-grave emissions were evaluated in, starting with a business-as-usual (BAU) SMR-based methanol plant, and then considering stepwise nuclear integration. Methanol-to-diesel (MTD) conversion was evaluated accounting for nuclear energy integration and hydrogen production via high-temperature steam electrolysis (HTSE) using electricity either from the grid or from a dedicated nuclear power system. This multi-step process diverts stable and reliable nuclear energy into the transportation sector by upgrading low energy dense natural gas into liquid fuels fully compatible with existing infrastructure.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2025

Thermochemical conversion of waste plastics with coal and biomass to generate value-added products

Co-gasification of waste plastic and waste coal/biomass in steam was investigated to evaluate the effects of operating conditions and low-cost catalyst compositions of coal ash on syngas production and tar mitigation. The results demonstrate the benefits of waste plastic conversion with coal or biomass. A better understanding of these processes will facilitate the development of more accurate kinetic models for industrial-scale chemical recycling.

co-gasification↗
DOE OSTI2026

Photo-Reactive Amine-Based Direct Air Capture and Conversion of CO2

This study presents a novel photochemical approach to direct air capture (DAC) and CO2 conversion, utilizing a ruthenium-modified mesoporous TiO2 composite infused with linear polyethyleneimine (L-PEI) and enhanced by light absorbing and earth abundant titanium nitride (TiN). This light-activated system operates at ambient pressure and addresses long-standing challenges in conventional amine-based thermal reactive carbon capture (RCC), including amine degradation and CO2 slip. Our findings demonstrate that L-PEI effectively stabilizes CO2 adsorption and facilitates high-yield methanation over 50 cycles with a non-flammable forming gas mixture (approximately 5% H2). Comparatively, composites incorporating small-molecule amines exhibited poor stability under illumination, while highly mobilie branched PEI (B-PEI) formulations suffered from significant catalyst deactivation. A technoeconomic analysis suggests that methane synthesis via this platform could be achieved at costs below $5/kg under current electrocatalytic hydrogen pricing. These findings highlight the potential of this approach to enhance energy security by enabling decentralized, scalable fuel production from atmospheric CO2.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗