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Characteristics of Post-Sorbent and High Temperature Catalytic Oxidizer Beds After Long-Term On-Orbit Use
Trace contaminants are produced on-orbit by human metabolic processes and equipment off-gassing. These potentially hazardous contaminants are removed by the Trace Contaminant Control Subassembly (TCCS) in the US segment of the International Space Station (ISS). The TCCS has been operating since February 2001. Analysis of on-orbit telemetry data indicated a slow increase in the TCCS system flow resistance over the five years of operation. Two of the packed beds within the TCCS were replaced to return the TCCS to its nominal operation conditions; the high temperature catalytic oxidizer and the post-sorbent bed. Results from the examination of the returned beds are presented along with a discussion about changes to bed service life.
Processing of SOFC Anodes for Enhanced Intermediate Temperature Catalytic Activity at High Fuel Utilization (Final Report)
The overall objective was to infiltrate anodes with nanoparticle catalysts so that anode catalytic performance can be improved as anode operation temperature is reduced from 800°C to intermediate temperatures of 700°C and 600°C and as anode fuel utilization is increased. The addition of nickel nanoparticle catalysts into the anode improves performance by providing additional triple phase boundaries (TPBs), increasing the density of electrochemical reaction sites. To achieve this goal, both liquid phase and vapor phase methods for depositing nickel nanoparticles in the anode active layer, the region of the anode near the electrolyte where the electrochemical reaction occurs. It is imperative that nanoparticles are stable against coarsening during long-term operation, so the mechanisms and kinetics of nanoparticle stability during cell operation will be investigated. Finally, priority is given to processes that are scalable and easily transferable to industry, leveraging existing Ni-YSZ cermet anode technology. Utilizing nickel nanoparticles at different temperatures has different considerations that will be addressed. At the upper end of the intermediate temperature range (800°C), it is important that performance improvement is maintained over long periods by mitigating the instability of nanoparticles. At the middle of the temperature range (700°C), it is important that performance improvement is maintained at high fuel utilizations. At the lower end of the temperature range (600°C), where the performance of cells is poor due to increased resistances, it is important to improve anode performance by significantly increasing the electrochemical reaction site density, while nanoparticle durability is less of an issue. Finally, the objective was to explore mixed ionic and electronic (MIEC) nanoparticle catalysts like GDC to see if 2-phase boundaries can be created to increase the electrochemical reactions at the anode.
Low temperature catalytic ignition of hydrogen and oxygen
Catalyst composed of 32 percent iridium metal supported on granular alumina is most active and most stable of platinum metal catalysts. Catalyst consistently induces reactions at temperatures as low as 78 K.
Low temperature catalytic conversion of CH 4 , CO 2 , and C 2 H 4 to value-added C 3 oxygenates and olefins via C 1 -C 2 coupling on Pd-Au/CeO 2
The catalytic conversion of CH 4 and CO 2 in the presence of more reactive co-reactants C 2 H 4 and O 2 on Pd-Au/CeO 2 is achieved at 200 °C and elevated pressures. Propene and acetone were produced from the catalyzed reaction of CH 4 +C 2 H 4 +O 2 ; addition of CO 2 to the reactant stream produced methyl acetate (MAc) but it significantly reduced the C-selectivities of propene and acetone. DRIFTS experiments confirmed the formation of methoxy species from CH 4 +CO 2 at 200 °C, which is an intermediate in the formation of MAc. Here, control experiments with blanks, and with CeO 2 did not show any propene, acetone, or MAc products. The complete oxidation of C 2 H 4 was avoided; the catalyst is stable, and reactant conversions and product yields were sustained for the observed 1200 min time-on-stream, indicating that there is little or no carbon deposition and sintering. This direct coupling of CH 4 and C 2 H 4 intermediates to higher carbon-number products at 200 °C is significant.
Effect of bimetallic modification on blast furnace slag and its application in low‐temperature selective catalytic reduction
Abstract Objective In order to control NO x in low‐temperature flue gases emitted from non‐power industries and to reduce the preparation cost of denitration catalysts, this study uses inexpensive blast furnace slag as raw material to prepare denitration catalysts. Methods After cooling, drying and grinding, the blast furnace slag becomes a powder with considerable fineness and meets the requirements of activity index, which is called GGBS (ground granulated blast furnace slag). Using GGBS as denitration catalyst carrier, the active components M (M = Fe, Co, Ni, Cu and Ce) are loaded on Mn‐based GGBS catalyst using an impregnation method. Conclusions The effect of different active components on the denitration performance and sulfur resistance of Mn‐based GGBS catalysts is investigated. The results show that the Mn‐Ce/GGBS catalyst has better denitration performance and sulfur resistance. The Mn‐Ce/GGBS catalyst has a significant denitration performance when load ratio is 2:1. The active component Ce improves the denitration performance of the catalyst, reduces sulfur poisoning and extends the life of the catalyst. The SO 2 in the flue gas increases the acid sites on the catalyst surface and improves catalyst activity. The larger the ratios of Mn 4+ /Mn 3+ , Ce 4+ /Ce 3+ and O α /O β , the stronger the catalyst activity and the better the denitration performance. © 2022 Society of Chemical Industry (SCI).
Development of a Microlith® Catalytic Oxidizer for Exploration Trace Contaminant Control
The state-of-the-art in long mission duration spacecraft trace contaminant control processes rely on high-temperature catalytic oxidation for light contaminant removal. Target compounds for oxidation include metabolic methane, carbon monoxide, and low molecular weight volatile organics such as formaldehyde and methanol. Precision Combustion, Inc. and NASA Marshall Space Flight Center have been developing and testing prototype high temperature catalytic oxidizers based on PCI’s patented Microlith® technology to meet the requirements of future spaceflight exploration missions. To this end, our latest generation Microlith oxidizer, featuring an integrated heat recuperator, was subjected to endurance testing to simulate catalyst ageing over a Mars transit mission duration. Periodic reactor health testing indicates our approach results in a robust contaminant control solution for exploration missions beyond low earth orbit. Based on the demonstrated performance of this unit, a next-generation prototype was designed to meet exploration contaminant load control demands while upgrading the prototype form and fit to match flight-compatible interfaces. Prototype design considerations intended to reduce power consumption, impacting process thermal and hydraulic performance, are discussed herein.
Recent advances in hybrid metal oxide–zeolite catalysts for low-temperature selective catalytic reduction of NOx by ammonia
A hybrid catalytic system comprised of metal oxide and Cu or Fe exchanged zeolite components represents a potential advancement of state-of-the-art for selective catalytic reduction (SCR) of NOx by ammonia, including an elegant solution to the current challenge of improving the low-temperature efficiency of SCR catalysts. The idea is to enable in-situ NO oxidation over metal oxide component and concomitant fast SCR over zeolite component in the so-called “bifunctional mechanism”. This review is presented in the wake of growing interest in this innovative catalytic system. We begin this review by presenting key parameters that contribute to the synergy between metal oxide and zeolite components. Then, we discuss the materials selection for both components and their possible interactions in the system, followed by a summary of recent NH3-SCR investigations over multiple metal oxide–zeolite pairs and additional discussion on pairing techniques potentially explorable in upcoming studies. Finally, we end the review by providing the perspectives on future challenges in the development of this catalytic system.
International Space Station Alpha trace contaminant control subassembly life test report
The Environmental Control and Life Support System (ECLSS) Life Test Program (ELTP) began with Trace Contaminant Control Subassembly (TCCS) Life Testing on November 9, 1992, at 0745. The purpose of the test, as stated in the NASA document 'Requirements for Trace Contaminant Control Subassembly High Temperature Catalytic Oxidizer Life Testing (Revision A)' was to 'provide for the long duration operation of the ECLSS TCCS HTCO (High Temperature Catalytic Oxidizer) at normal operating conditions... (and thus)... to determine the useful life of ECLSS hardware for use on long duration manned space missions.' Specifically, the test was designed to demonstrate thermal stability of the HTCO catalyst. The report details TCCS stability throughout the test. Graphs are included to aid in evaluating trends and subsystem anomalies. The report summarizes activities through the final day of testing, January 17, 1995 (test day 762).
Catalytic considerations in temperature measurement.
Literature discussing catalytic activity in platinum group temperature sensors is surveyed. Methods for the determination and/or elimination of catalytic activity are reported. A particular application of the literature is discussed in which it is possible to infer that a shielded platinum total temperature probe does not experience significant catalytic activity in the wake of a supersonic hydrogen burner, while a bare iridium plus rhodium, iridium thermocouple does. It is concluded that catalytic data corrections are restricted and that it is preferable to coat the temperature sensor with a noncatalytic coating. Furthermore, the desirability of transparent coatings is discussed.
Low temperature vapor phase catalytic oxidation unit
Low temperature vapor phase catalytic oxidation unit for removing organics in urine distillation
An Evaluation of the Vapor Phase Catalytic Ammonia Removal Process for Use in a Mars Transit Vehicle
An experimental program has been developed to evaluate the potential of the Vapor Phase Catalytic Ammonia Reduction (VPCAR) technology for use as a Mars Transit Vehicle water purification system. Design modifications which will be required to ensure proper operation of the VPCAR system in reduced gravity are also evaluated. The VPCAR system is an integrated wastewater treatment technology that combines a distillation process with high temperature catalytic oxidation. The distillation portion of the system utilizes a vapor compression distillation process to provide an energy efficient phase change separation. This portion of the system removes any inorganic salts and large molecular weight, organic contaminates, i.e., non-volatile, from the product water stream and concentrates these contaminates into a byproduct stream. To oxidize the volatile organic compounds and ammonia, a vapor phase, high temperature catalytic oxidizer is used. This catalytic system converts these compounds along with the aqueous product into CO2, H2O, and N2O. A secondary catalytic bed can then be used to reduce the N2O to nitrogen and oxygen (although not evaluated in this study). This paper describes the design specification of the VPCAR process, the relative benefits of its utilization in a Mars Transit Vehicle, and the design modification which will be required to ensure its proper operation in reduced gravity. In addition, the results of an experimental evaluation of the processors is presented. This evaluation presents the processors performance based upon product water purity, water recovery rates, and power.
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.
Catalytic Ambient Temperature Dinitrogen Conversion to a Bis(silyl)amine by Mononuclear Group 4 Aryloxide Complexes
The homogeneous conversion of ambient dinitrogen to amine products via the N2 reduction reaction (N2RR) remains a prized yet challenging feat for d-block complexes and is scarcely reported for f-block complexes. New, mononuclear TiIV and ZrIV aryloxide complexes Ti(DP)2 (1Ti), Zr(DP)2 (1Zr), and DP = [2-(OC6H2-2-tBu,4-Me)2CHPh] produce up to 51 eq. and up to 7.0 eq. of HN(SiMe3)2 per Ti/Zr, from N2, K0, weak acid, and chlorotrimethylsilane. Complex 1Ti exhibits more than double the activity toward N2-silylation of any previously reported Ti N2RR catalyst and can also catalyze the formation of up to 19 eq. of NH3, a new feature in early metal N2RR chemistry. The mononuclear 1Zr is the most active Zr catalyst for N2-silylation to date. [KSm(DP)2(THF)3] (1Sm), the mononuclear analogue of our previously reported dinuclear A-Sm complex, displays only stoichiometric N2-silylation due to its vulnerability to deleterious side reactions. DFT calculations confirm the catalysis can proceed via a monomeric Ti complex with a terminally bound, activated N2, agreeing with experimental 1H DOSY NMR measurements; the N-H bond is formed first, directing the catalyst selectivity. The isolable reduction product [K3(THF)Ti(DP)(DP-)(N2)] is also an active catalyst, and an intermediate in the calculated cycle.
A Study on the Role of Electric Field in Low-Temperature Plasma Catalytic Ammonia Synthesis via Integrated Density Functional Theory and Microkinetic Modeling
Not Available
Improving Enzyme Optimum Temperature Prediction with Resampling Strategies and Ensemble Learning
Accurate prediction of the optimal catalytic temperature ( T opt ) of enzymes is vital in biotechnology, as enzymes with high T opt values are desired for enhanced reaction rates. Recently, a machine learning method (temperature optima for microorganisms and enzymes, TOME) for predicting T opt was developed. TOME was trained on a normally distributed data set with a median T opt of 37 °C and less than 5% of T opt values above 85 °C, limiting the method’s predictive capabilities for thermostable enzymes. Due to the distribution of the training data, the mean squared error on T opt values greater than 85 °C is nearly an order of magnitude higher than the error on values between 30 and 50 °C. Here, we apply ensemble learning and resampling strategies that tackle the data imbalance to significantly decrease the error on high T opt values (>85 °C) by 60% and increase the overall R 2 value from 0.527 to 0.632. The revised method, temperature optima for enzymes with resampling (TOMER), and the resampling strategies applied in this work are freely available to other researchers as Python packages on GitHub.
In Situ Catalytic Fast Pyrolysis using Red Mud Catalyst: Impact of catalytic fast pyrolysis temperature and biomass feedstocks
Catalytic fast pyrolysis (CFP) has been considered as a very promising approach for converting lignocellulosic biomass into higher-quality bio-oils followed by hydrotreating to produce fuelrange products. A reactive, robust, and low-cost catalyst is required to drive the CFP process. Red mud, a side-product produced during the refining of bauxite to alumina, appears to be an effective catalyst for in situ CFP of biomass. In this paper, we report the impact of CFP reaction temperature on the conversion of a pinyon juniper feedstock to bio-oils using red mud as the catalyst and then to fuel-range hydrocarbons by hydrotreating of the produced bio-oil. The yield and quality of the CFP bio-oil produced and the yield and quality of hydrotreated final products were determined. When the CFP process temperature was lowered from 450 to 400ºC, the bio-oil yield increased with minimal differences in the oxygen content, hydrogen-to-carbon ratio, water content, etc. In addition, CFP bio-oils at both temperatures were processed in a single-stage continuous hydrotreater without reactor plugging during the testing period (i.e., ~100 hours on stream). The yield of CFP bio-oil produced at 400ºC was lower than the yield at 450ºC. However, the overall yield, from biomass to hydrocarbon fuel, was still higher for CFP processing at 400ºC than for processing at 450ºC. This indicates the potential for enhancing overall carbon efficiency, including CFP processing and hydrotreating, by employing red mud catalysts for biomass pyrolysis and tuning the CFP parameters. Detailed analysis of bio-oil and hydrotreated products showed a lower content of lignin-derived species in both samples. Furthermore, CFP processing of three different biomass feedstocks corroborated red mud catalyst development for producing improved quality bio-oil and, when combined with hydrotreating, for the production of fuel range hydrocarbons.
Optimizing Process Conditions during Catalytic Fast Pyrolysis of Pine with Pt/TiO 2 —Improving the Viability of a Multiple-Fixed-Bed Configuration
Catalytic fast pyrolysis (CFP) has been identified as a promising pathway for the production of renewable fuels and co-products. However, continued technology development is needed to increase process efficiency and reduce process costs. This report builds upon previous research in which a bifunctional metal–acid Pt/TiO 2 catalyst was utilized in a fixed-bed reactor operated with co-fed H 2 to improve product yield and reduce coke generation compared to conventional CFP methods. Here, we report further process optimization, in which we achieved similar CFP oil carbon efficiency (>35%) and CFP oil oxygen content (<20 wt %) to our previous report while reducing catalyst and equipment costs by increasing time-on-stream between regenerations by 40–95% and decreasing required regeneration time by more than a factor of 2. These process improvements were achieved by conducting parameter sweeps to determine optimum conditions for CFP and regeneration with key variables including pyrolysis temperature, catalytic upgrading temperature, hydrogen partial pressure, and regeneration oxygen concentration. Coupled with comprehensive oil analyses, these data provide foundational insight into the deoxygenation and coking chemistries for CFP under realistic process conditions while also advancing the technology through applied engineering.