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Total Dissolved Nitrogen and Ammonia Data for the East River Watershed, Colorado (2015-2025)

This data package contains mean values for total dissolved nitrogen (TDN) and ammonia concentrations for water samples taken from the East River Watershed in Colorado. The East River is part of the Watershed Function Scientific Focus Area (WFSFA) located in the Upper Colorado River Basin, United States. TDN was analyzed using a Shimadzu Total Nitrogen Module (TNM-1) combined with the TOC-VCSH analyzer (Shimadzu Corporation, Japan). TNM-1 is a non-specific measurement of total nitrogen (TN). All nitrogen species in samples are combusted to nitrogen monoxide and nitrogen dioxide, then reacted with ozone to form an excited state of nitrogen dioxide. Upon returning to ground state, light energy is emitted. Then, TDN is measured using a chemiluminescence detector. Ammonia was determined using a Lachat's QuikChem 8500 Series 2 Flow Injection Analysis System (LACHAT Instruments, QuckChem 8500 series 2, Automated Ion Analyzer, Loveland, Colorado). When ammonia in water samples is heated (60 degrees C) with salicylate and hypochlorite in an alkaline phosphate buffer, an emerald green color is produced which is proportional to the ammonia concentration. The color is intensified by the addition of nitroprusside. Ethylenediaminetetraacetic acid (EDTA) is added to the buffer to prevent the interference of metal ions (Ca, Mg, and Fe etc.). Ammonia-N is then determined by LACHAT flow injection and a colorimetric assay at an absorbance wavelength 660 nm. (Reference: LACHAT Instruments: QuickChem Method 90-107-06-3-A, Determination of Ammonia by Flow Injection Analysis (High Throughput, Salicylate Method/DCIC) (Multi Matrix method). Written by Lynn Egan (Application group), February 08, 2011.) All files are labeled by location and variable, and data reported are the mean values upon replicate measurements. All samples were analyzed under a rigorous quality assurance and quality control (QA/QC) process as detailed in the methods. This data package contains (1) a zip file (tdn_ammonia_data_2015-2025.zip) containing a total of 299 files: 298 data files of ammonia and TDN data from across the Lawrence Berkeley National Laboratory (LBNL) Watershed Function Scientific Focus Area (SFA) which is reported in .csv files per location and a locations.csv (1 file) with latitude and longitude for each location; (2) a file-level metadata (v7_20260901_flmd.csv) file that lists each file contained in the dataset with associated metadata; (3) a data dictionary (v7_20260901_dd.csv) file that contains terms/column_headers used throughout the files along with a definition, units, and data type; (4) PDF and docx files for the determination of Method Detection Limits (MDLs) for TDN data, which has been updated in 2026-08; and (5) PDF and docx files for the detemination of Method Detection Limits (MDLs) for Ammonia and the Interferences by LACHAT Flow Injection Analysis. Missing values within the anion data files are noted as either "-9999" or "0.0" for not detectable (N.D.) data. There are a total of 105 locations containing TDN and Ammonia-N data. Update 2020-10-07: Updated the data files to remove times from the timestamps, so that only dates remain. The data values have not changed. Update 2021-04-11: Added Determination of Method Detection Limits (MDLs) for DIC, NPOC and TDN Analyses and Determination of Method Detection Limit for Ammonia and the Interferences by LACHAT Flow Injection Analysis documents, which can be accessed as PDFs or with Microsoft Word.Update on 6/10/2022: versioned updates to this dataset was made along with these changes: (1) updated total dissolved nitrogen and ammonia data for all locations up to 2021-12-31, (2) removal of units from column headers in datafiles, (3) added row underneath headers to contain units of variables, (4) restructure of units to comply with CSV reporting format requirements, (5) added -9999 for empty numerical cells, and (6) the addition of the file-level metadata (flmd.csv) and data dictionary (dd.csv) were added to comply with the File-Level Metadata Reporting Format. Update on 2022-09-09: Updates were made to reporting format specific files (file-level metadata and data dictionary) to correct swapped file names, add additional details on metadata descriptions on both files, add a header_row column to enable parsing, and add version number and date to file names (v2_20220909_flmd.csv and v2_20220909_dd.csv). Update on 2022-12-20: Updates were made to both the data files and reporting format specific files. Units were listed incorrectly, but have been fixed to reflect correct units (ug/L). File level metadata (flmd) and data dictionary (dd) files were updated to reflect the updated versions of these files. Available data was added up until 2022-06-01. Update on 2023-08-08: Updates were made to both the data files and reporting format specific files. New available anion data was added, up until 2023-01-05. The file level metadata and data dictionary files were updated to reflect the additional data added. Update on 2024-03-11: Updates were made to both the data files and reporting format specific files. New available anion data was added, up until 2023-10-27. Further, revisions to the data files were made to remove incorrect data points (from 1970 and 2001). The reporting format specific files were updated to reflect the additional data added. Revised versions of the PDF and docx files for determination of MDLs for TDN were added to replace previous versions. Update on 2025-05-15: Updates were made to both the data files and reporting format specific files. New available TDN and Ammonia-N data was added, up until the end of WY2024 (September 30, 2024). International Generic Sample Numbers (IGSNs), when registered, were added to the data files. The reporting format specific files were updated to reflect the additional data added. Update on 2026-09-01: Updates were made to both the data files and reporting format specific files. New available TDN and Ammonia-N data was added, up until the end of WY2025 (September 30, 2025). Updated versions, as of 2026-08-10, of the PDF and docx files for determination of MDLs for TDN data were added to this dataset.

54 ENVIRONMENTAL SCIENCES↗

Restricting electron flow at cytochrome b6f when downstream electron acceptors are severely limited

Abstract Photosynthetic organisms frequently experience abiotic stress that restricts their growth and development. Under such circumstances, most absorbed solar energy cannot be used for CO2 fixation and can cause the photoproduction of reactive oxygen species (ROS) that can damage the photosynthetic reaction centers of PSI and PSII, resulting in a decline in primary productivity. This work describes a biological “switch” in the green alga Chlamydomonas reinhardtii that reversibly restricts photosynthetic electron transport (PET) at the cytochrome b6f (Cyt b6f) complex when the capacity for accepting electrons downstream of PSI is severely limited. We specifically show this restriction in STARCHLESS6 (sta6) mutant cells, which cannot synthesize starch when they are limited for nitrogen (growth inhibition) and subjected to a dark-to-light transition. This restriction represents a form of photosynthetic control that causes diminished electron flow to PSI and thereby prevents PSI photodamage but does not appear to rely on a ΔpH. Furthermore, when electron flow is restricted, the plastid alternative oxidase (PTOX) becomes active, functioning as an electron valve that dissipates some excitation energy absorbed by PSII and allows the formation of a proton motive force (PMF) that would drive some ATP production (potentially sustaining PSII repair and nonphotochemical quenching [NPQ]). The restriction at the Cyt b6f complex can be gradually relieved with continued illumination. This study provides insights into how PET responds to a marked reduction in availability of downstream electron acceptors and the protective mechanisms involved.

Plant Sciences↗

Local Heat Transfer Measurements in Cooler for sCO2 Power Cycles with Dilute Nitrogen and Argon Impurities

An experimental investigation of heat transfer in CO2 and CO2/N2 and CO2/argon mixtures undergoing cooling near the pseudocritical temperature has been conducted. The conditions are representative of direct sCO2 cycle coolers. Three tubing test articles were tested: conventional drawn tubing, an additively manufactured tube with a square cross section, and an additively manufactured tube with a square cross section and ribs angled 60° relative to the flow direction. The axial heat transfer coefficient distribution was determined with local wall temperature measurements. This work concludes that dilute concentrations (< 2%) of nitrogen and argon have a negligible impact on heat transfer coefficient and on friction factor.

Searle, Matthew↗

Development of High Energy Density Diaminocyclopropenium‐Phenothiazine Hybrid Catholytes for Non‐Aqueous Redox Flow Batteries

Abstract This report describes the design of diaminocyclopropenium‐phenothiazine hybrid catholytes for non‐aqueous redox flow batteries. The molecules are synthesized in a rapid and modular fashion by appending a diaminocyclopropenium (DAC) substituent to the nitrogen of the phenothiazine. Combining a versatile C‐N coupling protocol (which provides access to diverse derivatives) with computation and structure‐property analysis enabled the identification of a catholyte that displays stable two‐electron cycling at potentials of 0.64 and 1.00 V vs. Fc/Fc + as well as high solubility in all oxidation states (≥0.45 M in TBAPF 6 /MeCN). This catholyte was deployed in a high energy density two‐electron RFB, exhibiting >90 % capacity retention over 266 hours of flow cell cycling at >0.5 M electron concentration.

Yan, Yichao↗

Enhancement of hard magnetism and chemical order of synthetic L 1 0 -FeNi

An ordered tetragonal L 1 0 -FeNi, also known as meteoritic mineral tetrataenite – a promising rare-earth-free hard-magnetic compound – has been synthesized starting from a mechanochemically-activated disordered cubic A1-FeNi via formation of a chemically-ordered FeNiN intermediate and its subsequent denitrogenation and further purification of the product. The nature of a process control agent employed during the mechanochemical activation of A1-FeNi and ammonia flow velocity during the synthesis of the intermediate are two of the main factors controlling the nitrogenation. Denitrogenation with hydrogen at elevated pressures and at temperatures substantially below the order-disorder L 1 0 -FeNi → A1-FeNi transition preserves the chemical order established in the intermediate nitride. Further, post-synthesis refinement of the L 1 0 -FeNi product includes the removal of residual nitrides with a dilute acid to further improve hard-magnetic properties of the material. The L 1 0 -FeNi powders synthesized using this method exhibit a coercivity as high as 2.3 kOe and a maximum energy product reaching 6 MGOe – the highest values ever reported for a synthetic tetrataenite.

36 MATERIALS SCIENCE↗

High-energy, low-jitter, narrowband ps probe laser for kHz-rate fs/ps coherent anti-Stokes Raman scattering

Hybrid fs/ps coherent anti-Stokes Raman scattering (CARS) thermometry often utilizes ps probe pulses derived from pulse shaping or spectrally filtering the primary laser source or by synchronization with a low repetition rate external laser. This results in limited energy, spectral resolution, and/or repetition rate of the ps probe. In this work, a master-oscillator power-amplifier (MOPA) laser was synchronized to the oscillator of a Ti:sapphire regenerative amplifier to achieve high-energy (600 µJ), narrowband (58 ps) probe pulses at kHz repetition rates. Furthermore, temporal filtering allows the pulse characteristics to be adjusted for each application. At 25 Torr, relevant to high-speed flows, the kHz-rate MOPA system generated signal-to-noise ratios 3× higher in nitrogen and had improved precision relative to a 10 ps probe derived from spectral filtering and the power-amplifier. The MOPA system also enabled single-shot ro-vibrational hybrid fs/ps CARS thermometry in 650 K heated air.

47 OTHER INSTRUMENTATION↗

Analysis of Lobe Power Calculator and Indication System with Physics and Cycle Based Models

The Advanced Test Reactor (ATR) at INL measures reactor power through two methods, thermal and Nitrogen-16 (N-16) activity. Water power calculator (WPC) is a thermal power system that measures flow and temperature to determine the thermal quadrant powers. The N-16 system utilizes a beta chamber detector that outputs reactivity levels to calculate lobe power through an algorithm called lobe power calculation and indication system (LPCIS). The LPCIS utilizes the N-16 system and the WPC system to determine reactor core power levels. The WPC provides accurate calculations of quadrant and total reactor thermal power. With the use of WPC measurements, thermal-to-N-16 (T2N) power ratios are produced to determine if the two indication systems agree on core power. Relative magnitude equations are used to utilize N-16 coefficients and multipliers to improve the indications of the LPCIS. This is crucial for maintaining safety limits. Currently, the LPCIS system uses linear equations and matrices to calculate lobe power through multipliers and coefficients. Advancements in technology and system upgrades have assisted system engineers at INL with the objective to reach a more dynamic system. In return the system demonstrates an increase in the accuracy of power reading while maintaining safety margins. The new proposed coefficient and multiple method implements a cycle specific, and a physics-based model intended for changing coefficients during operation. This calibration experiment focuses on power splitting, outer shim and neck shim, as well as fuel burning into the RDAS weighting factors. Results show that the Physics learning method yields a smaller error margin inside of the desired power range for the data set 166-A. This proved true for both constrained and unconstrained testing. This is most likely due to the physics data fitting approach that resulted in favorable coefficients and multipliers for 166-A. Continuing to improve the physics-based model will help improve the power accuracy of the LPCIS system.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Chemical Reactor Network Modeling of Ammonia Rich-Quench-Lean Combustion Using a Partially Stirred Reactor Approach

Ammonia is a promising alternative to hydrogen with high energy density and favorable storage and transport characteristics. However, low flammability and a propensity for high nitrogen oxide (NO x ) emissions make direct utilization challenging. Recently, two-stage rich-quench-lean (RQL) combustion strategies have shown promise in achieving low NO x emissions with ammonia. In this approach, the rich stage serves to oxidize a portion of the fuel while thermally decomposing as much of the remaining ammonia as possible, generating hydrogen. In the second (lean) stage, air is rapidly introduced, burning out the hydrogen and residual ammonia. Two-stage RQL combustion of ammonia has been investigated in the open literature both experimentally and numerically. In general, idealized chemical reactor network (CRN) models predict NO x concentrations below those of 2D/3D computational fluid dynamics models and experiments. The primary drivers of these discrepancies may be largely attributed to finite rate mixing nonadiabatic operation. The typical CRN model is comprised of a perfectly-stirred-reactor (PSR), followed by a plug-flow-reactor (PFR), meant to represent the flame, and postflame zones, respectively. In the two-stage RQL approach two PSR-PFR networks are arranged sequentially, corresponding to the rich and lean stages, with secondary air injection in between. In the authors' past work, this arrangement has demonstrated the significant sensitivity of exit NO x to the rich stage equivalence ratio, while the amount of secondary air injection was shown to be less critical. In this paper, the CRN model is extended to (1) include the impacts of heat loss and (2) utilize a partially-stirred-reactor (PaSR) approach to study the impacts of mixing on emissions performance. Varying amounts of heat loss are applied to the rich relaxation zone to understand emissions performance and changes to optimization of equivalence ratio and residence time. Premixed and nonpremixed configurations are considered in the rich stage PaSR, with varying degrees of mixing intensity to study the interaction between mixing, transport, and kinetic timescales. Critically, the impact of mixing between hot products and secondary air injection is studied to understand practical injector needs. Results show unburnt ammonia leaving the rich stage as a primary contributor to NO x emissions – driven both by increased heat loss and reduced mixing rates. Furthermore, heat losses have been shown to create conditions that are conducive to increased N 2 O formation in the lean stage. In conclusion, the results of this study will be considered in the context of developing optimized two-stage RQL combustors for ammonia.

Combustion↗

Development of High Energy Density Diaminocyclopropenium-Phenothiazine Hybrid Catholytes for Non-Aqueous Redox Flow Batteries

Our work describes the design of diaminocyclopropenium-phenothiazine hybrid catholytes for non-aqueous redox flow batteries. The molecules are synthesized in a rapid and modular fashion by appending a diaminocyclopropenium (DAC) substituent to the nitrogen of the phenothiazine. Combining a versatile C-N coupling protocol (which provides access to diverse derivatives) with computation and structure-property analysis enabled the identification of a catholyte that displays stable two-electron cycling at potentials of 0.64 and 1.00 V vs. Fc/Fc + as well as high solubility in all oxidation states (≥0.45 M in TBAPF 6 /MeCN). This catholyte was deployed in a high energy density two-electron RFB, exhibiting >90 % capacity retention over 266 hours of flow cell cycling at >0.5 M electron concentration.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Impurity leakage and radiative cooling in the first nitrogen and neon seeding study in the closed DIII-D SAS configuration

A comparative study of nitrogen versus neon has been carried out to analyze the impact of the two radiative species on power dissipation, SOL impurity distribution, divertor and pedestal characteristics. The experimental results show that N remains compressed in the divertor, thereby providing high radiative losses without affecting the pedestal profiles and displacing carbon as dominant radiator. Neon, instead, radiates more upstream than N thus reducing the power flux through the separatrix leading to a reduced ELM frequency and compression in the divertor. A significant amount of neon is measured in the plasma core leading to a steeper density gradient. The different behavior between the two impurities is confirmed by SOLPS-ITER modeling which for the first time at DIII-D includes multiple impurity species and a treatment of full drifts, currents and neutral–neutral collisions. The impurity transport in the SOL is studied in terms of the parallel momentum balance showing that N is mostly retained in the divertor whereas Ne leaks out consistent with its higher ionization potential and longer mean free path. This is also in agreement with the enrichment factor calculations which indicate lower divertor enrichment for neon. The strong ionization source characterizing the SAS divertor causes a reversal of the main ions and impurity flows. The flow reversal together with plasma drifts and the effect of the thermal force contribute significantly in the shift of the impurity stagnation point affecting impurity leakage. This work provides a demonstration of the impurity leakage mechanism in a closed divertor structure and the consequent impact on pedestal. Since carbon is an intrinsic radiator at DIII-D, in this paper we have also demonstrated the different role of carbon in the N vs Ne seeded cases both in the experiments and in the numerical modeling. Here, carbon contributes more when neon seeding is injected compared to when nitrogen is used. Finally, the results highlight the importance of accompanying experimental studies with numerical modeling of plasma flows, drifts and ionization profile to determine the details of the SOL impurity transport as the latter may vary with changes in divertor regime and geometry. In the cases presented here, plasma drifts and flow reversal caused by high level of closure in the slot upper divertor at DIII-D play an important role in the underlined mechanism.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Wetlands Geoprocessor (v 1.0)

Wetlands have often been described as the “Earth’s kidneys” because wetlands have the ability filter pollutants and purify water. Based upon wetland storage capacity, average daily flow, and inflow nutrient loading this model estimates potential load reductions of nitrate and orthophosphate) from a constructed surface flow wetland (CW). The model relies upon equations, coefficients, and models provided by Cheng et al. 2020 and Cheng & Basu 2017. Nitrogen (N) and phosphorus are important nutrients to ecosystems, but high concentrations can lead to water quality issues. Major sources of these nutrients come from agricultural areas where fertilizer is applied in large quantitates and/or animal waste is present. Excess nitrate and phosphorus may result in overgrowth of algae, which can decrease the dissolved oxygen in water, thereby harming and killing fish and other aquatic species. This model evaluates water purification results and estimates cost to install a surface flow constructed wetlands.

Davis, Cleve↗

Disentangling natural and anthropogenic effects on benthic macroinvertebrate assemblages in western US streams

Abstract Stream macroinvertebrate assemblages are shaped by natural and human‐related factors that operate through complex hierarchical pathways. Quantifying these relationships can provide additional insights into stream ecological assessment. We applied a structural equation modeling framework to evaluate hypothesized pathways by which watershed, riparian, and in‐stream factors affect benthic macroinvertebrate condition in the Western Mountains (WMT) and Xeric (XER) ecoregions in the United States. We developed a conceptual model grounded in theory, empirical evidence, and expert opinion to evaluate the following hypotheses: (1) macroinvertebrate assemblages are primarily driven by proximal, in‐stream factors (e.g., water quality and physical habitat); (2) anthropogenic land uses affect macroinvertebrates indirectly by altering in‐stream characteristics; and (3) riparian vegetation cover attenuates land use effects. We tested our model separately on three measures of benthic macroinvertebrate assemblage condition: ratio of observed‐to‐expected taxonomic richness (O/E); a multimetric index (MMI); and richness of Ephemeroptera, Plecoptera, and Trichoptera taxa (EPT). In the WMT, site‐level riparian cover, in‐stream physical habitat (relative bed stability), and water chemistry (total nitrogen) were the top three predictors of macroinvertebrate assemblages, each having over two times the magnitude of effect on macroinvertebrates compared with watershed‐level predictors. In the arid XER, annual precipitation and stream flow characteristics were top predictors of macroinvertebrate assemblages and had similar magnitudes of effect as in‐stream water chemistry. Path analyses revealed that land use activities in the watershed and at the stream site degraded macroinvertebrate assemblages indirectly by altering relative bed stability, water quality, and riparian cover/complexity. Increased riparian cover was associated with greater macroinvertebrate condition by reducing land use impacts on stream flow, streambed substrate, and water quality, but the pathways differed among ecoregions. In the WMT, site‐level riparian cover affected macroinvertebrate assemblages partly through indirect pathways associated with greater streambed stability and reduced total nitrogen concentrations. In contrast, in the XER, watershed‐level riparian cover affected macroinvertebrate assemblages through greater specific stream power. Identifying the relative effects of and pathways by which natural and anthropogenic factors affect macroinvertebrates can serve as a framework for prioritizing management and conservation efforts.

Environmental Sciences & Ecology↗

Visualization of bulk and edge photocurrent flow in anisotropic Weyl semimetals

Materials that rectify light into current in their bulk are desired for optoelectronic applications. In Weyl semimetals that break inversion symmetry, bulk photocurrents may arise due to nonlinear optical processes that are enhanced near the Weyl nodes. However, the photoresponse of these materials is commonly studied by scanning photocurrent microscopy, which convolves the effects of photocurrent generation and collection. Here we directly image the photocurrent flow inside the type-II Weyl semimetals WTe 2 and TaIrTe 4 using high-sensitivity quantum magnetometry with nitrogen-vacancy centre spins. We elucidate a mechanism for bulk photocurrent generation, which we call the anisotropic photothermoelectric effect, where unequal thermopowers along different crystal axes drive intricate circulations of photocurrent around the photoexcitation. Using overlapping scanning photocurrent microscopy and magnetic imaging at the interior and edges of the sample, we visualize how the anisotropic photothermoelectric effect stimulates the long-range photocurrent collected in our WTe 2 and TaIrTe 4 devices through the Shockley–Ramo mechanism. Furthermore, our results highlight a widely relevant source of current flow and will inspire photodetectors that utilize bulk materials with thermoelectric anisotropy.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Combined Nitrogen and Phosphorous Recovery via Electrochemical Technology Integration into Municipal Wastewater Treatment Plants

This project developed electroN-P, an electrochemical technology for recovering nitrogen and phosphorus as a fertilizer product from anaerobic digester centrate, targeting an advancement from TRL 4 to 6. The reactor was scaled 220× from a 250 mL batch cell to a continuous 4-channel system treating 55 L of wastewater, recovering >80% of phosphorus. Energy consumption under constant-voltage operation was lower than the embedded energy of conventional fertilizers, while constant-current operation produced a cost-competitive product with a smaller reactor footprint. TEA and LCA outcomes were highly sensitive to the magnesium source; alternative magnesium salt configurations projected reduced costs and embedded energy compared to sacrificial rods, but at the expense of significantly longer operation times. The recovered fertilizer performed comparably to diammonium phosphate and triple superphosphate in soil and plant trials. Integrating the technology into a whole-plant model reduced aeration energy by nearly 50%, lowering the levelized cost of water treatment from $0.668/m 3 to $0.648/m 3 . Results support targeting commercialization at smaller (≤1 MGD) facilities with high-strength digester streams. Further investigation into the transport and corrosion kinetics governing sacrificial anode wear is recommended to support continuous, longer-term operation.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Near-Surface Imaging of the Multicomponent Gas Phase above a Silver Catalyst during Partial Oxidation of Methanol

Fundamental chemistry in heterogeneous catalysis is increasingly explored using operando techniques in order to address the pressure gap between ultrahigh vacuum studies and practical operating pressures. Because most operando experiments focus on the surface and surface-bound species, there is a knowledge gap of the near-surface gas phase and the fundamental information the properties of this region convey about catalytic mechanisms. In this work, we demonstrate in situ visualization and measurement of gas-phase species and temperature distributions in operando catalysis experiments using complementary near-surface optical and mass spectrometry techniques. The partial oxidation of methanol over a silver catalyst demonstrates the value of these diagnostic techniques at 600 Torr (800 mbar) pressure and temperatures from 150 to 410 °C. Planar laser-induced fluorescence provides two-dimensional images of the formaldehyde product distribution that show the development of the boundary layer above the catalyst under different flow conditions. Raman scattering imaging provides measurements of a wide range of major species, such as methanol, oxygen, nitrogen, formaldehyde, and water vapor. Near-surface molecular beam mass spectrometry enables simultaneous detection of all species using a gas sampling probe. Detection of gas-phase free radicals, such as CH 3 and CH 3 O, and of minor products, such as acetaldehyde, dimethyl ether, and methyl formate, provides insights into catalytic mechanisms of the partial oxidation of methanol. The combination of these techniques provides a detailed picture of the coupling between the gas phase and surface in heterogeneous catalysis and enables parametric studies under different operating conditions, which will enhance our ability to constrain microkinetic models of heterogeneous catalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Catalytic Removal of Oxygen and Pollutants in Exhaust Gases from Pressurized Oxy-Combustors

The primary goal of this project was to develop and validate advanced catalytic materials and systems for purifying the flue gas generated from pressurized oxy-combustors in an effort to achieve the purity specifications of carbon dioxide (CO 2 ) streams required by the U.S. Department of Energy (USDOE) for application in enhanced oil recovery. The technology has shown great potential for improving energy efficiency, simplifying process complexity, and lowering costs compared with current state-of-the-art oxy-combustion flue gas purification technologies. Laboratory studies were conducted for the development, characterization, and screening of metal catalysts for residual oxygen (O 2 ) reduction with methane (CH 4 ) and multifunctional carbon catalysts for combined nitrogen oxides (NO x ), sulfur oxides (SO x ), and mercury (Hg) removal. A bench-scale reverse-flow fixed-bed (RFFB) reactor and a trickle-bed direct-contact cooler (DCC) reactor capable of treating 15 standard liters per min of pressurized oxy-combustion flue gas were fabricated and tested with both a simulated flue gas in the laboratory and a slipstream of actual flue gas at a 100 kW th Staged, Pressurized Oxy-Combustion (SPOC) pilot facility. Process simulation and techno-economic studies were performed to evaluate the energy efficiency and cost of the developed catalytic flue gas purification process integrated into a conceptual 550-MWe SPOC power plant. The goal and objectives of the project have been successfully accomplished. A cobalt-manganese (CoMn) oxide catalyst was developed and demonstrated in the bench-scale RFFB reactor in either a reverse-flow or one-direction flow mode of operation that met the success criterion of performance for residual O 2 reduction. A carbon catalyst was developed and demonstrated in the bench-scale DCC reactor that met the success criterion of performance for combined NO x /SO x /Hg removal. Slipstream testing of the integrated DCC-RFFB system at the SPOC pilot facility demonstrated stable operation and verified the superior performance obtained in the laboratory. The techno-economic analysis showed that a 550-MWe SPOC plant integrated with the catalytic flue gas purification process would result in costs of electricity of $\$$96.94/MWh and $\$$80.27/MWh in two assessed cases compared with $\$$91.07/MWh reported for the USDOE’s Current Technology Case, which generated only a partially pure CO 2 stream. On the basis of the results and findings from this project, scale-up studies of materials production and system demonstration and optimization studies of reactors and processes are recommended at the next stage of technology development.

20 FOSSIL-FUELED POWER PLANTS↗

Facile and Scalable Synthesis of Metal- and Nitrogen-Doped Carbon Nanotubes for Efficient Electrochemical CO 2 Reduction

Metal- and nitrogen-doped carbon (M–N–C) is a promising material to catalyze electrochemical CO 2 reduction reaction (CO 2 RR). However, most M–N–C catalysts in the literature require complicated synthesis procedures and produce small quantities per batch, limiting the commercialization potential. In this work, we developed a simple and scalable synthesis method to convert metal-impurity-containing commercial carbon nanotubes (CNTs) and nitrogen-containing organic precursors into M–N–C via one-step moderate-temperature (650 °C) pyrolysis without any other treatment nor the need to add metal precursors. Batches of catalysts in varied mass up to 10 g (150 mL in volume) per batch were synthesized, and repeatable catalytic performances were demonstrated. To the best of our knowledge, the 10 g batch is one of the largest batches of CO2RR catalysts synthesized in the literature while requiring minimal synthesis steps. The catalyst possessed single-atomic iron–nitrogen (Fe–N) sites, enabling a high performance of >95% CO product selectivity at a high current density of 400 mA/cm 2 and high stability for 45 h at 100 mA/cm 2 in a flow cell testing. The catalyst outperformed a benchmark noble-metal nanoparticle catalyst and achieved longer stability than many other reported M–N–C catalysts in the literature. The scalable and cost-effective synthesis developed in this work paves a pathway toward practical CO 2 RR applications. The direct utilization of metal impurities from raw CNTs for efficient catalyst synthesis with minimal treatment is a green and sustainable engineering approach.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Coherent fluctuations in a partially magnetized small magnetron discharge operating on molecular nitrogen

We report experimental data on rotating plasma disturbances in a quasi-steady direct-current magnetron discharge operating with molecular nitrogen at pressures of 27, 40, 67, and 133 Pa. Experiments with a segmented anode measuring the local current flow reveal up to 12 coherent structures (“spokes”) propagating in the +E×B and −E×B azimuthal directions. The current–voltage characteristics are studied and found to follow a negative resistance profile at the lower discharge currents. The existence of coherent structures and the number of spokes observed depend on the discharge current and operating pressure. Lower pressures are more favorable to the retrograde −E×B spoke rotation, which is observed in the 27, 40, and 67 Pa discharges. The results are interpreted with a gradient-driven drift wave model, and using the dispersion relation, we show that the propagation direction depends on the orientation of the local electric field within the plasma. Using an electron fluid model, we show how experimental conditions can lead to field reversals that generate −E×B spoke rotation in the lower pressure discharges.

Physics↗