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At least 397 records · Page 22
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Facet‐dependent Heterogeneous Fenton Reaction Mechanisms on Hematite Nanoparticles for (Photo)catalytic Degradation of Organic Dyes

Although heterogeneous photo‐Fenton reactions on nanoparticulate iron oxides effectively degrade organic pollutants, the underlying surface mechanisms remain debated. Here, we demonstrate how these pathways are modulated by specific hematite crystal facets. To investigate the influence of particle surface structure, methylene blue (MB) adsorption and photodegradation kinetics are examined using facet‐engineered hematite nanoparticles with distinct exposed facets. The results reveal that MB photodegradation strongly depends on both pH and facet orientation. When normalized by surface area, (116) facet shows higher photodegradation activity than those with (104) or (001) facets. This enhanced activity is attributed to favorable electronic structure and surface characteristics, including a smaller optical bandgap, faster charge transfer, and superior H 2 O 2 decomposition. In contrast, the photodegradation capacity follows (104) 〉 (116) 〉 (001), primarily due to the higher density of surface‐active sites on the (104) facet. These sites promote coupled MB adsorption and degradation, enabling removal of a greater overall quantity of MB. Additionally, under high pH conditions, hematite can degrade MB in the dark, with capacities following (001) ≫ (116) 〉 (104). These findings underscore the critical catalytic role of specific hematite surfaces and advance the understanding of facet‐dependent photoinduced redox chemistry at mineral–water interfaces.

(photo)catalytic degradation↗
DOE OSTI2023

Life-cycle analysis of sustainable aviation fuel production through catalytic hydrothermolysis

Catalytic hydrothermolysis (CH) is a sustainable aviation fuel (SAF) pathway that has been recently approved for use in aircraft fuel production. In alignment with broader sustainable aviation goals, SAF production through CH requires a quantitative assessment of carbon intensity (CI) impacts. In this study, a current-day life-cycle analysis (LCA) was performed on SAF produced via CH to determine the CI. Various oily feedstocks were considered, including vegetable oils (soybean, carinata, camelina and canola) and low-burden oils and greases (corn oil, yellow grease and brown grease). Life-cycle inventory data were collected on all processes within the CH LCA boundary: feedstock cultivation and/or collection, preprocessing, hydrothermal cleanup and CH, biocrude refining, fuel transportation and end use through combustion. Baseline results show that the CH-produced SAF can be generated with CI reductions ranging from 48 to 82% compared with conventional jet fuel. Modest improvements to CI can be achieved through incremental changes to the brown grease CH process, such as relaxing the dewatering specification and implementing renewable natural gas and electricity, which could decrease the CI from 22.9 to 7.9 g CO 2 e/MJ. Total CH fuel production potential was also assessed on the basis of current or near-future feedstock availability and CI. The total biofuel production potential of CH (SAF and renewable fuel co-products) in the US sums to approximately 3487 million gallons per year, with 97% of these volumes having a CI below 50% of that for petroleum jet fuel. The study shows that from an LCA perspective, CH offers a viable SAF pathway that is comparable with existing SAF pathways like hydroprocessed esters and fatty acids.

09 BIOMASS FUELS↗
DOE OSTI2022

Catalytic Conversion of Model Compounds of Plastic Pyrolysis Oil over ZSM-5

Mechanistic investigation of the catalytic conversion of model compounds for plastic pyrolysis oil (1-octene, octadiene, octane, and toluene) over ZSM-5 in a fixed-bed reactor was studied. 1-Octene breaks down into smaller olefins, which undergo further cracking, oligomerization, cyclization, and hydrogen transfer to eventually produce benzene, toluene, xylene (BTX), coke, and hydrogen. The effect of contact time on 1-octene conversion was further investigated and compared with thermodynamics analyses to elucidate the reaction network. Under the reaction conditions (500 oC, 1 atm), octadiene undergoes thermal coking, significantly contributing to reactor fouling. The products from octane cracking are similar to the products from 1-octene conversion whereas toluene undergoes disproportionation, dealkylation and coking. The analysis of spent catalyst showed long-chain hydrocarbons created by oligomerization reactions filled the pores and covered the surface of the catalyst. As a result, when mesoporous ZSM-5 is used instead of conventional, product selectivity is maintained for 70 hours in time-on-stream experiments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Insights into palladium poisoning of Cu/SSZ-13 selective catalytic reduction catalysts

Here, the impacts of Pd poisoning to the activity, selectivity, and hydrothermal stability of Cu/SSZ-13 selective catalytic reduction (SCR) catalysts are reported. Pd lowers DeNOx efficiency of Cu/SSZ-13 via two mechanisms: (1) displacing SCR active sites in the form of isolated Pd-ions, and (2) catalyzing non-selective NH 3 oxidation in the form of PdO. The first mechanism works by the diffusion of isolated Pd-ions into chabazite cages to displace ZCu II OH SCR active species, and it occurs on Cu/SSZ-13 catalysts with and without external surface CuO clusters in similar fashion. In contrast, the second mechanism works differently with and without external surface CuO clusters. For Cu/SSZ-13 catalyst without external CuO clusters (i.e., primarily isolated Cu-ions), PdO leads to significant decrease of DeNOx efficiency at reaction temperatures above ~400°C due to its non-selective NH 3 oxidation activity at high temperatures. However, this poisoning effect becomes much less impactful on Cu/SSZ-13 catalyst containing CuO clusters. This is due to the formation of CuO-PdO solid solution via interactions between CuO and PdO, which reduces non-selective NH 3 oxidation potential. Furthermore, this solid solution formation even mitigates adverse effects caused by hydrothermal aging. Hence, the poisoning effects of Pd are closely related to Cu speciation and spatial distribution of a Cu/SSZ-13 catalyst. Finally, this study suggests a strategy in eliminating Pd poisoning, that is, the introduction of an oxide phase that effectively traps PdO but does not adversely influence SCR.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Coupling hydropyrolysis and vapor-phase catalytic hydrotreatment to produce biomethane from pine sawdust

Here, this study investigated hydropyrolysis and subsequent vapor-phase hydrotreatment over a NiAl 2 O 4 catalyst to produce biomethane (CH 4 ) from pine sawdust. The non-catalytic pressurized hydropyrolysis generated tar, CO 2 , and CO as the primary products. However, using a NiAl 2 O 4 catalyst in the second-stage reactor significantly increased the formation of CH 4 and reduced CO and CO 2 in gas products. The catalyst also fully converted tar intermediates to produce CH 4 , resulting in a maximum carbon yield of 77.7% with 97.8% selectivity. The temperature plays a crucial role in CH 4 generation, with both its yield and selectivity showing a positive correlation with the reaction temperature. Increasing the reaction pressure from 0.2 to 1.2 MPa notably inhibited the production of CH 4 , leading to a shift towards cycloalkanes due to a competitive reaction. This tandem approach shows great potential as an innovative technique for producing alternative fuels from biomass wastes.

09 BIOMASS FUELS↗
DOE OSTI2020

Epitaxial growth mechanism of heterogeneous catalytic oxidation of Mn(II) on manganite under oxic conditions

Manganese oxides are ubiquitous in soils and sediments, and their formation and transformation processes affect the migration and transformation of heavy metals and organic pollutants. Most previous work has been focused the oxidation of Mn(II) on Mn(IV) oxide surface, but it remains poorly understood how Mn(II) interacts with manganite under oxic conditions. Here, the interactions between manganite and dissolved Mn(II) within pH 5.0–9.0 under oxic conditions were systematically studied. The results indicated that adsorbed Mn(II) was directly oxidized to manganite on the surface, and the oxidation rate increased with increasing pH and oxygen partial pressure. Electrons are likely transferred in bulk manganite during the oxidation process of Mn(II). Although manganite induced Mn(II) oxidation and the epitaxial growth of bulk particles, there was no obvious change in mineral phase. Dissolved oxygen accelerated the growth of manganite in Mn(II) solution. Compared with the absence of manganite, the presence of manganite inhibited the formation of hausmannite from Mn(II) oxidation by oxygen in air. Furthermore, this study reveals the catalytic oxidation process and mechanism of Mn(II) on manganite surface, and improves the understanding of manganite crystal growth in supergene environments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2027

Hydrotreating pine-derived catalytic fast pyrolysis oil to jet fuel: Process durability and impact of operating conditions

Hydrotreating woody biomass-derived catalytic fast pyrolysis (CFP) oil to jet fuel has the potential to enhance energy security due to the large abundance of forest and woody resources. CFP oil produced from pine over ZSM-5 was hydrotreated over sulfided NiMo/Al 2 O 3 for 410 h to study the impact of hydrotreating conditions (pressure, temperature, and weight hourly space velocity (WHSV)). The degree of deoxygenation remained high across the tested hydrotreating conditions, and the products contained < 0.01 wt% oxygen. Increasing hydrotreating pressure from 84 to 125 bar enhanced hydrogenation of aromatic rings and the formation of cycloalkanes and increasing the temperature from 385 to 400 degrees C enhanced cracking and the formation of jet-range molecules. Decreasing the weight hourly space velocity from 0.2 to 0.1 g/(g cat h) further enhanced cracking and led to higher gasoline- and lower jet fuel-range fractions. The highest jet fuel fraction (49 wt%) was obtained at 400 degrees C, 125 bar, 0.2 g/(g cat h) WHSV. CFP oils produced from pine over phosphorous-modified ZSM-5 were hydrotreated at this condition for 588 h to investigate the process durability. The hydrogenation performance of the catalyst gradually stabilized in approximately 300 h after which the product composition remained constant. Of the final hydrotreated CFP oil, 53 wt% fell in the jet fuel range with most of the tested fuel properties meeting ASTM D4054 and/or ASTM D7566 specifications. The freeze points were < -50 degrees C vs. guideline of < -40 degrees C and the viscosities at -20 degrees C were 3.8-4.1 mm 2 /s vs guideline of 8 mm 2 /s. Increasing the fraction of cycloalkanes could increase the cetane number and heating value, which did not meet the guidelines.

09 BIOMASS FUELS↗
DOE OSTI2022

Multi-pass flow-through reductive catalytic fractionation

Reductive catalytic fractionation (RCF) is a promising lignin-first biorefining strategy that selectively extracts and depolymerizes lignin from whole biomass. Flow-through (FT)-RCF enables physical separation of the biomass and catalyst, but this process configuration typically operates at high solvent-to-biomass ratios. Here, we demonstrate multi-pass FT-RCF, wherein the lignin-enriched solvent obtained after an initial FT-RCF step is recycled and used in subsequent FT-RCF without intermediate lignin recovery. Multi-pass FT-RCF reduces the solvent-to-biomass ratio from 48 to 1.9 L/kg, which is a lower solvent loading than is accessible in batch reactors, without negative impacts on delignification and monomer yield with up to 12 wt % lignin in the solvent. Overall, this work demonstrates that solvent demand in RCF processes, which is a key cost and energy driver to enable this process at scale, can be reduced by recycling lignin oil between RCF reactions.

09 BIOMASS FUELS↗
DOE OSTI2021

Compact ammonia reforming at low temperature using catalytic membrane reactors

Ammonia is a leading carrier for the storage and transport of renewable hydrogen, but its deployment requires scalable technologies for efficient decomposition and purification. In this work, we report on the efficient delivery of high purity hydrogen from ammonia decomposition using a catalytic membrane reactor (CMR). Improvements to the electroless plating process reduced the Pd membrane thickness by >35%, resulting in commensurate increases in hydrogen permeance without sacrificing selectivity. To increase throughput a commercial Ru/Al 2 O 3 catalyst was added to the lumen, and the CMR could process ammonia flowrates 10–50 times higher than an equivalent packed bed reactor while maintaining the same level of conversion. It is shown that the earth-abundant zeolite clinoptilolite could reduce ammonia impurities in the permeated H 2 to the levels required by PEM fuel cells (<25 ppb). Performance increased significantly across a >500-h durability test due to improvements in membrane permeability. Finally, the results show that CMRs are a viable technology for distributed production of hydrogen from ammonia.

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

Techno-economic and life-cycle analysis of strategies for improving operability and biomass quality in catalytic fast pyrolysis of forest residues

Many of the challenges faced by the first commercial biorefineries were associated with feedstock handling, quality, and cost. Strategies are needed to enable further expansion of biorefineries and meet the growing demand for bio-based fuels and products. Here, we examine 2 key feedstock challenges and mitigation strategies in the context of a catalytic fast pyrolysis (CFP) biorefinery: (1) the operability of the feed system, which may be improved by modifying the minimum particle size fed to the reactor, and (2) the quality of the biomass, which may be improved by employing air classification to remove undesirable material and increase fuel yields. We conduct techno-economic analysis (TEA) and life-cycle analysis for these strategies, employing a discrete event simulation model for biomass preprocessing combined with a series of correlations developed from literature data and a rigorous CFP conversion model. Our results highlight the importance of balancing increased cost and material losses from preprocessing against improved operability and fuel yields. Economics and sustainability were optimized when operating at the lowest minimum particle size, emphasizing the importance of minimizing material losses while maintaining the operability of the process. Economically, additional costs and material losses from air classification could be acceptable due to improved biomass conversion, and an optimum air classification speed was identified; however, the fuel GHG emissions were minimized when air classification was not used. Valorizing material removed during preprocessing as a coproduct could improve economics and sustainability, decreasing the burden of material losses.

09 - BIOMASS FUELS↗
DOE OSTI2026

Catalytic resonance theory for the kinetic signatures of multiple wavelength photocatalysis

Multi-step surface chemistry promoted with one or two wavelengths of light exhibited distinct kinetic signatures indicative of the light-adsorbate interactions and the number of photon-sensitive elementary steps. In this work, kinetic Monte Carlo simulations identified the kinetic response of general surface mechanisms to variation in the per-site photon flux of one or two wavelengths of incident light. Photocatalytic rates were described via a non-dimensional photon flux, identifying multiple kinetic regimes with unique degrees of rate control. Under photon-controlled kinetic conditions, maximum quantum yield and turnover frequency were obtained under constant illumination, while pulsing of one or more light sources was shown to exhibit slower rates and less efficient photocatalytic promotion due to the inherent dynamic nature of light, which comprises a stream of photons. Simulations provided distinct kinetic signatures in catalytic rates and Arrhenius kinetics for specific light-surface-adsorbate interactions corresponding to photocatalytic promotion of specific steps in surface chemistry.

catalytic resonance↗
DOE OSTI2021

Multiscale Catalytic Fast Pyrolysis of Grindelia Reveals Opportunities for Generating Low Oxygen Content Bio-Oils from Drought Tolerant Biomass

Grindelia squarrosa (curlycup gumweed) biomass possesses unique biochemistry, cell wall composition, and leaf architecture tailored for prolific growth in arid and semiarid climates. Most notably, this plant has developed high levels of extractable resins that have high effective H/C eff ratios ((mol H - 2 x mol O)/mol C), which is hypothesized to lead to low coke formation during catalytic fast pyrolysis (CFP) over the ZSM-5 catalyst. In microscale experiments with high ZSM-5 loadings (biomass-to-catalyst mass ratio (B/C) ~ 0.1), in situ CFP generated high yields of aromatic hydrocarbons (30% carbon yield) while ex situ CFP favored aliphatic hydrocarbons (25% carbon yield). The difference between the two configurations was attributed to the constant catalyst temperature during ex situ CFP. Deactivation leading to partially deoxygenated vapor products occurred rapidly until B/C ≤ 0.5 by the adsorption of organic species blocking access to acid sites inside the micropores of the catalyst. This was followed by more gradual deactivation leading to primary vapor breakthrough, which we attribute to coke formation on acid sites on the external surface of ZSM-5 crystallites. Noncatalytic fast pyrolysis of Grindelia in a bench scale reactor produced oils with oxygen content (18 wt % on dry basis) and carbon yield (33%) comparable to those of CFP of woody biomass. The CFP of Grindelia further reduced the oxygen content to 7 wt % for in situ CFP and 4 wt % for ex situ CFP at B/C of 2-3. The good deoxygenation was attributed to a combination of a high H/C eff ratio and overall better quality of the pyrolysis vapors that were passed over the ZSM-5 catalyst. The high inorganic content of the Grindelia likely catalyzed pyrolysis to remove oxygenated coke precursors. This integrated CFP study demonstrated that Grindelia could be an important feedstock for generating stabilized noncatalytic and CFP oils for downstream processing into fuels and/or extraction of high-value chemicals. The preprocessing of this feedstock will be required to remove inorganics, which cause an irreversible deactivation of ZSM-5.

BIOMASS FUELS↗
DOE OSTI2022

Coprocessing Biomass Fast Pyrolysis and Catalytic Fast Pyrolysis Oils with Vacuum Gas Oil in Refinery Hydroprocessing

Fast pyrolysis and catalytic fast pyrolysis (CFP) have been considered to be promising approaches for converting lignocellulosic biomass into liquid bio-oils followed by upgrading to produce fuel-range hydrocarbon products. Co-processing fast pyrolysis and CFP bio-oils with petroleum feedstocks leverages the existing petroleum refining infrastructure, which reduces Capex for the overall conversion technologies for biomass to fuel and enables fast adoption of the technologies and biofuels. Here, we reported the co-processing of different woody fast pyrolysis and CFP bio-oils with petroleum vacuum gas oil (VGO) at 5-25% bio-oil blending levels over a NiMo sulfide catalyst for mild hydrocracking. The catalyst activities over ~300 hours time on stream, the product yield and properties, and the biogenic carbon content in products are provided. Co-processing of the raw fast pyrolysis bio-oil in our configuration was not successful because the instability of the bio-oil resulted in reactor plugging and bio-oil stabilization by hydrogenation enabled their stable co-processing with VGO, whereas the CFP bio-oil can be co-processed without pretreatment. Simultaneous hydrodesulfurization, hydrodeoxygenation, and hydrocracking reactions occurred during co-processing and no obvious decrease in hydrodesulfurization and hydrocracking conversion of VGO was observed, suggesting the minimal impact of co-processed bio-oils on the reaction of VGO and also the simultaneous conversion of bio-oil and VGO to produce fuel products with much-reduced S and O content. Biogenic carbon content in co-processed products calculated by yield mass balance, together with results from isotopic measurements, indicates high biogenic carbon incorporation into liquid hydrocarbon products. In conclusion, higher biogenic carbon incorporation into fuel products was observed when co-processing CFP bio-oils than the fast pyrolysis bio-oils and over 90% of carbon in CFP bio-oil was incorporated into liquid hydrocarbon products.

09 BIOMASS FUELS↗
DOE OSTI2025

Opportunity Assessment for Sustainable Aviation Fuel Production from Woody Biomass via Ex Situ Catalytic Fast Pyrolysis and Refinery Hydroprocessing

Biofuels have become a promising solution to reduce emissions in hard-to-electrify transportation sectors, such as aviation. However, several biofuel conversion pathways will likely be needed to scale sustainable aviation fuel (SAF) production to meet lower carbon intensity goals when biomass feedstock availability constraints are considered. This study evaluates the future potential of the catalytic fast pyrolysis (CFP) pathway to contribute to U.S. SAF production goals as outlined in the U.S. Department of Energy’s (DOE) SAF Grand Challenge, understanding that the CFP pathway is still under development toward maturity and scaleup. National forestland resource data from the DOE’s 2023 Billion Ton Study are integrated with recent experimental results demonstrating end-to-end woody biomass conversion to SAF via CFP and hydroprocessing in a novel bioeconomy optimization framework. U.S. refinery hydroprocessing capacity is also considered with repurposing and coprocessing strategies. Results indicate that the CFP process can contribute up to 4.6 billion gallons of SAF annually by 2040, meeting 13% of the 2050 SAF Grand Challenge target while reducing the carbon intensity (CI) of the U.S. jet fuel pool by 16%. The study further explores optimal processing strategies, suggesting that colocating CFP operations with existing petroleum refineries and repurposing some U.S. hydrocracking capacity may offer significant cost advantages and enhance the commercial viability of the CFP pathway. These results underscore the CFP pathway’s potential to support the global aviation industry’s lower carbon intensity objectives while producing other renewable fuels and products.

09 BIOMASS FUELS↗
DOE OSTI2020

Cerium(IV) Enhances the Catalytic Oxidation Activity of Single-Site Cu Active Sites in MOFs

The rates of catalytic oxidation of cyclohexane and CO are four and twenty times higher, respectively, with Cu supported on a cerium-based MOF than on the structurally analogous zirconium material. Both Ce- and Zr-based copper catalysts feature uncommon threecoordinate CuII sites bearing different nuclearities, as observed by Cu K-edge extended X-ray absorption fine structure analysis. These findings offer molecular-level understanding of the metal-support interface in MOF catalysts and establish correlations with the more established literature on zirconia and ceria-supported heterogeneous catalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Deactivation by Potassium Accumulation on a Pt/TiO 2 Bifunctional Catalyst for Biomass Catalytic Fast Pyrolysis

Biomass-derived feedstocks bring significant challenges to the longevity of the catalysts used for their conversion, and alkali metals, for example, K, in the feedstock have been widely ascribed as one of the important factors causing catalyst deactivation. To address this challenge, it is critical to understand the mechanism of catalyst deactivation caused by K accumulation to guide the improvement of catalysts and processes and the development of catalyst regeneration strategies. In this work, we report a deep understanding of the impact of K on a bifunctional Pt/TiO 2 catalyst, which is an efficient catalyst for the ex situ catalytic fast pyrolysis of biomass. We simulated the K-poisoning of Pt/TiO 2 catalysts by purposely loading different amounts of K (100-6000 ppm by weight) on the catalysts. A series of characterization approaches, including scanning transmission electron microscopy, Fourier transform infrared spectroscopy, and chemical titration, were combined with a kinetic assessment of multiple probe reactions to elucidate the mechanism of Pt/TiO 2 deactivation by K accumulation. At low K loadings (<800 ppm), K preferentially poisons the strong Lewis acid sites, leading to significantly reduced activity for acid-catalyzed alcohol dehydration. However, acetone condensation is less sensitive to the poisoning of strong Lewis acid sites. Reactions that occur on Pt sites or at the metal-support interface, including alkene hydrogenation, m-cresol hydrodeoxygenation (HDO), and CO oxidation, were not impacted. At high K loadings (>800 ppm), K starts to accumulate on the Pt-TiO 2 interfacial area, poisoning the interfacial active sites for HDO and CO oxidation reactions. We further found that the poisoning of the Pt/TiO 2 catalyst by K is reversible, and water washing can successfully remove the accumulated K and recover the activities for both alcohol dehydration and m-cresol HDO reactions.

09 BIOMASS FUELS↗
DOE OSTI2026

The Kinetic Consequences of Water on Catalytic Methane Pyrolysis

Hydrogen production from biomass and natural gas has emerged as a prominent research area in response to the growing demand for energy from alternative sources that minimize CO 2 emissions. In this study, we investigate the impact of water, which is present in and generated from biomass-derived streams, on carbon nanotube (CNT) growth and hydrogen production during methane decomposition using Ni–Mo/MgO as a catalyst. We reveal here that the role of water on CNT growth is highly complex; its effect depends on the stage of growth at which the water is incorporated. When water is introduced at the beginning of methane decomposition ( t = 0 h), methane conversion rates are negatively impacted. We hypothesize that water inhibits the significant phase changes the Ni–Mo/MgO catalyst undergoes during catalyst carburization. In contrast, the incorporation of a small percentage of water after a stabilization period ( t = 3 h) results in methane conversion rate enhancements that scale with the introduced water partial pressure as water selectively reacts with amorphous carbon deposits that lead to catalyst deactivation, thus prolonging the lifetime of some of the most active sites. Moreover, water incorporation after stabilization significantly reduces the apparent activation energy. Density Functional Theory (DFT) calculations reveal that water preferentially interacts with carbon fragments on the catalyst surface to remove carbon deposits with a barrier lower than that required for methane activation, further supporting its role in cleaning active sites on the catalyst surface. Characterization of the resulting carbon nanotubes reveals the formation of more graphitic materials produced in the presence of water, highlighting the impact of water on nanotube properties. These results provide clarity toward the many ways in which water, or cofeeding of biomass-derived materials, may impact catalytic methane pyrolysis rates.

carbon nanotubes↗
DOE OSTI2025

Catalytic Oxygen Reduction for Deep O 2 Removal from CO 2 Streams

Streams of CO 2 from various capture processes may contain several impurities of which O 2 is often overlooked as a problematic impurity. Because of its reactivity, the National Energy Technology Laboratory has recommended a stringent limit, less than 10 ppm, for the O 2 level in treated CO 2 products for safe transport, storage, and utilization. Here, in this study, a variety of catalytic oxygen reduction approaches using commercial automotive exhaust emission catalysts are evaluated for O 2 removal from CO 2 streams using different reducing agents, including H 2 , CO, CH 3 OH, and CH 4 . When the amount of reductant added into the feed is carefully controlled, H 2 , CO, or CH 3 OH can effectively remove O 2 from 1.5% to below 10 ppm with a single-reactor design (>99.93% removal efficiency), while simultaneously meeting the impurity limits for other species. With CH 4 as a reductant, it is challenging to simultaneously meet the the O 2 and CO specifications in a single-reactor design because CH 4 also reacts with CO 2 to produce high levels of CO in the stream (at several hundred ppm). A dual-reactor design is developed to enable the use of CH 4 , a readily available and low-cost reductant, for the purification of CO 2 streams to meet the specifications for O 2 and other impurities.

CO2 purification↗