Enhanced light absorption for solid-state brown carbon from wildfires due to organic and water coatings
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54 ENVIRONMENTAL SCIENCES↗
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Evaluation of Technologies to Mitigate the Presence of Gaseous Elemental Mercury in Waste Disposal Containers
A study was conducted to evaluate sorbent technologies that can mitigate the presence of elemental mercury (Hg⁰) in waste containers for mercury-contaminated debris (MCD). Decontamination and demolition (D&D) activities at the Y-12 National Security Complex (Y-12) and other U.S. Department of Energy (DOE) Oak Ridge Reservation (ORR) facilities generate MCD requiring offsite disposal. The debris is packaged in appropriate waste containers and may be temporarily stored onsite prior to transport for treatment and/or disposal. During transportation of loads that had no visible liquid Hg at the point of origin, temperature changes can cause Hg⁰ to evaporate, condense, and form droplets on container walls. Furthermore, vibration during transportation could cause beads of Hg to be released from the debris, container walls, and ceiling, resulting in pools of liquid Hg⁰ on the container floor. Waste acceptance criteria (WAC) limitations for commercial disposal facilities, the Nevada National Security Site (NNSS), and ORR mixed low-level waste landfills prohibit the presence of any free liquids in containers identified as a solid waste form. Potential solutions to mitigate the presence of residual liquids that could be formed through vapor condensation include the use of sorbents or similar materials to capture and stabilize volatile Hg⁰ vapors and thus ensure compliance with landfill WAC requirements. This report summarizes data from small-scale laboratory experiments conducted to evaluate sorbent materials for Hg⁰ vapor suppression and sorption of liquid Hg⁰ that could form under relevant transportation and disposal conditions. A series of experiments was conducted to evaluate commercial sorbent materials and their effectiveness for Hg⁰ sorption across a temperature range from 19.4°C to 60°C. The impact of residual moisture on sorption was investigated under relevant conditions, and leaching tests were performed to assess the stability of Hg⁰ captured sorbent materials. The results provide estimates for sorbent quantities needed for a given Hg⁰ mass loading based on experimental results exposing sorbents to gaseous and liquid Hg⁰ at various mass ratios. Overall, sorbents that were most effective for Hg⁰ vapor suppression were brominated activated carbons, mackinawite-based sorbents coated on vermiculite, and sulfur-modified granular activated carbon. Elevated temperatures and moisture conditions did not result in significant increases of Hg⁰ headspace concentrations, and the materials also demonstrated high sorption capacities for the sorption of liquid Hg⁰.
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Accelerated thermal property mapping of TRISO advanced nuclear fuel
TRistructural ISOtropic (TRISO) fuel is a leading-edge nuclear fuel form representing a departure from the more traditional nuclear fuel forms utilized in the reactor fleet of today. Rather than a monolithic fuel pellet of uranium dioxide, integral fuel forms containing TRISO fuel are composed of thousands of microencapsulated uranium-bearing fuel kernels and individually coated with multiple layers of pyrolytic carbon and silicon carbide. These multilayered ceramic coatings serve as an environmental barrier to ensure radioactive and chemically reactive fission products are contained within the reactor fuel elements, but also participate in the transfer of heat generated in the nuclear fuel to the coolant – the primary purpose of a nuclear reactor. Since traditional thermal property measurement techniques, such as laser flash analysis, would be unable to resolve the thermal properties of the individual TRISO coating layers, a simplified frequency-domain thermoreflectance technique has been developed to rapidly map the thermal properties of TRISO particles. Using this technique, the thermal properties of TRISO particles have been mapped from room temperature up to 1000 °C to examine the spatial variation and temperature-dependency of the thermal properties within each layer. Additionally, spatial-domain thermoreflectance was used to examine the anisotropy of the thermal properties for each layer at different locations within a single TRISO particle, and across multiple TRISO particles to assess the intra- and inter-particle uniformity of thermal properties, respectively. To elucidate the underlying causes for the measured variations in thermal properties, scanning electron microscopy and Raman spectroscopy were used to examine variations in microstructure and chemical bonding within the different coating layers. Results from this work are then compared with previous examinations of TRISO fuel particles and microstructurally driven mechanisms for the variations in the measured thermal properties of the different carbonaceous layers are discussed.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Solvent-Free and Non-Sintered 500 Wh/kg All Solid-State Battery
Navitas teamed up with UMD and ORNL to establish a reliable scientific research team. The project addressed processing limitations of state-of-the-art solid electrolytes by extending solvent-free electrode fabrication technology to the scalable production of cathode/solid electrolyte laminates. The innovation started with a solid-state sulfide electrolyte (LiPS) with Cl stabilization able to meet the keystone conductivity challenge in a film of practical thickness (μ 50 µm). The electrolyte was based on a composite of PTFE, and stabilized LiPSCl. With optimization, the ionic conductivity reached 3.3 ×10 -3 S/cm. The solid electrolyte with as low as 0.4% binder allowed long term cycling (> 500 cycles) of Li/SSE/Li cell at > 4 mA/cm 2 with the utilization of Li > 80%. The Li and SSE interfaces were successfully protected with LiF-rich SEI layer. NCM811cathode active materials were coated with a thin layer of Al 2 O 3 (5 nm). The free standing cathode film was fabricated through dry-process with Al2O3-coated NCM811, LiPSCl, active carbon, and small amount PTFE. The all-solid-state batteries were laminated with free standing surface coated NCM811 cathode film, free standing LiPSCl SSE film, and surface protected Li anode together in a single lamination step, and demonstrated high specific capacity (> 200 mAh/g) with coulombic efficiency > 99.5%. The all-solid-state batteries through solvent-free and no-sintering process are promising for large format cell with 500 Wh/Kg specific energy density.
25 ENERGY STORAGE↗
MPCVD-Grown Nanodiamond Microelectrodes with Oxygen Plasma Activation for Neurochemical Applications
Nanodiamonds (NDs) are a carbon nanomaterial that has a diamond core with heteroatoms and defects at the surface. The large surface area, defect sites, and functional groups on NDs make them a promising material for electrochemical sensing. Previously, we dip-coated ND onto carbon-fiber microelectrodes (CFMEs) and found increases in sensitivity, but the coating was sparse. Here, for this work, we directly grew thin films of ND on niobium wires using microwave plasma chemical vapor deposition (MP-CVD) to provide full surface coverage. ND microelectrodes show a reliable performance in neurotransmitter detection with good antifouling properties. To improve sensitivity, we oxygen plasma etched ND films to activate the surface and intentionally add defects and oxygen surface functional groups. For fast-scan cyclic voltammetry detection of dopamine, oxygen plasma-etching increases the sensitivity from 21 nA/μM to 90 nA/μM after treatment. Fouling was tested by repeated injections of serotonin or tyramine, and both ND and plasma oxidized nanodiamond (NDO) microelectrodes maintain their currents better compared to CFMEs and therefore are more antifouling. Furthermore, a biofouling test in brain slices shows that ND microelectrodes barely have any current drop, while the more hydrophilic NDO microelectrodes decrease more, but still not as much as CFMEs. Overall, grown ND microelectrodes are promising in neurotransmitter detection with excellent fouling resistance, whereas oxygen plasma etching slightly lowers the fouling resistance but dramatically increases sensitivity.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Carbon fiber-nanoparticle composites with electromechanical properties
A carbon fiber composite material comprising: (i) a carbon fiber having an outer surface, a thickness of at least 1 micron, and an aspect ratio of at least 1000; (ii) a sizing agent coated on the outer surface of the carbon fiber, wherein the sizing agent has a thickness of up to 200 nm; and (iii) nanoparticles having a size in at least one dimension of up to 100 nm embedded within the sizing agent, wherein the nanoparticles have a metal carbide, metal oxide, metal nitride, and/or metal boride composition. A method for producing the fiber composite material comprises: (a) continuously feeding and coating a continuous carbon fiber with a liquid containing a solvent, sizing agent, and nanoparticles in a continuous feed-through process to result in said sizing agent and nanoparticles coating the surface of the continuous carbon fiber; and (b) removing the solvent from the coated fiber.
Bowland, Christopher C.↗
Field Testing of Self-Healing Metallic Coatings for Internal Corrosion Protection of Natural Gas Pipelines
Internal corrosion occurs in natural gas pipelines primarily due to the presence of water, carbon dioxide, and hydrogen sulfide. Internal corrosion can eventually result in leakage, cracks, and rupture of the pipeline. The objective of this work is to mitigate internal corrosion in steel pipelines transporting natural gas using cold spray coatings. The corrosion behavior of carbon steel coated with self-healing zinc chromium (ZnCr) and zinc niobium (ZnNb) cold spray coatings was investigated in a natural gas environment. For comparison purposes, hot-dip galvanized steel (HDGS) was tested under the same conditions as cold spray coatings. The field test was performed at the NW Natural gas storage facility in Mist, Oregon. The field test was conducted in a 6-inch diameter pipe transporting wet natural gas out of an underground storage well at 500 psi and 4.4 °C. The coupons were tested for 15 and 32 days under stagnant and flow conditions, respectively. Weight loss method was used to measure the corrosion rate of metallic coatings. Post-corrosion surface characterization was performed on the specimen using a scanning electron microscopy (SEM) equipped with energy dispersive X-ray spectroscopy (EDS). Crystalline phases were determined by X-ray diffraction (XRD). The field-test results confirmed that the metallic coatings provided corrosion protection of carbon steel exposed to wet natural gas under stagnant and flow conditions. The formation of the ZnCO 3 layer on top of ZnNb and ZnCr coatings led to passivation of the coatings which helps to reduce the self-corrosion. These layers form a barrier for diffusion of corrosive species to the surface.
03 NATURAL GAS↗
Superlubricious carbon films derived from natural gas
A nanocomposite coating that in turn extract self-replenishing (or -healing), superlubricious carbon film directly from natural gas or hydrocarbon gas in mechanical systems. The coating deposits on sealing and sliding surfaces reducing friction and wear. The result is a reduction in inefficiency, machine breakdown, and adverse environmental impact.
03 NATURAL GAS↗
Development of Advanced Pipeline Materials: Metallic Coatings and Composite Liners
2021 Carbon Management and Oil and Gas Research Project Review Meeting, Virtual, August 23-27, 2021
Belarbi, Zineb↗
Deciphering the PMI Surface Chemistry of Lithium-Based PFCs and its Effects on High Performance Plasmas in NSTX
The primary aims or objectives of the proposed work here focus on the dynamic measurement (Illinois PI Allain) and atomistic-based multi-scale computational atomistic simulations (UTK PI: Wirth) of: 1) lithium coatings with re-deposited hydrogenated carbon surfaces and high-Z substrates, 2) lithium coatings on boronized ATJ graphite surfaces and high-Z substrates and 3) lithium coatings on ATJ graphite and high-Z substrates with variation in temperature. Three main primary tasks are proposed to address each of the primary objectives listed above: 1) dynamic in-situ irradiation with D+, He+ species of lithium coatings with variation in interface substrate morphology (e.g. smooth vs rough, fuzz vs nanostructured); 2) validation and coupling with multi-scale computational simulations connecting the irradiated surface to the plasma edge; 3) extrapolation to long-pulse conditions (e.g. function of flux vs fluence studies). In primary objective #3, temperature-based effects will be studied to evaluate three primary mechanisms: a) D uptake and recycling, b) erosion, and c) surface melting and evaporation as a function of substrate morphology and chemistry.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Achieving high volumetric EDLC carbons via hydrothermal carbonization and cyclic activation
A novel activation method involving hydrothermal carbonization (HTC) and a pressure-induced low temperature oxidation has been demonstrated for cellulose derived HTC char by using hydrogen peroxide as an active di-oxygen source. The optimized porosity versus gravimetric capacitance results from cellulose derived HTC char synthesized at 220 °C. Almost homogeneous and small particle size micro-ellipse/sphere, relatively high surface area and narrow pore size distributions lead to a high bulk density, i.e. 0.73 g cm -3 , of coating type electrodes, which is much denser than those manufactured from steam activated carbons for supercapacitor industry, i.e., 0.52 g cm -3 . The resulting carbon prepared herein achieves a relatively high volumetric capacitance in an organic electrolyte-based supercapacitor reaching a competitive value of industrial system with the features of environment friendly, cost-effective as well as high yield, and less energy consumption.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Growth of Highly Transparent Amorphous Carbon Films Using Beam Plasma Source
A single beam plasma source was used to deposit hydrogenated amorphous carbon (a-C:H) coatings at room temperature. Using methane source gas, a-C:H coatings were deposited at different radio frequency (RF) power to fabricate transparent and durable coatings. The film deposition rate was almost linearly proportional to the ion source power. Hydrogenated amorphous carbon films of ~100 nm thickness appeared to be highly transparent from UV to the infrared range with a transmittance of ~90% and optical bandgap of ~3.7 eV. The coatings also possess desirable mechanical properties with Young’s modulus of ~78 GPa and density of ~1.9 g/cm3. The combined material properties of high transmittance and high durability make the ion-source-deposited a-C:H coatings attractive for many applications.
36 MATERIALS SCIENCE↗
Improved representation of black carbon mixing structures suggests stronger direct radiative heating
Black carbon significantly influences the Earth system because of its strong solar radiation absorption. However, its direct radiative effect remains poorly understood in current climate models, partly because current climate models oversimplify the diverse structures formed when black carbon mixes with other atmospheric components. Here we show that incorporating more realistic, multi-mixing-structure representations of black carbon increases the direct radiative effect. We find that aged black carbon particles, with thicker coatings and higher embedded fractions, enhance the direct radiative effect more efficiently. Using machine learning alongside the Community Earth System Model, we show that the direct radiative effect at the top of the atmosphere in regions with heavy black carbon pollution is 31.6% greater when multi-mixing structures are considered. These findings highlight the importance of modeling complex mixing structures of particle-resolved black carbon to accurately capture their warming impacts on global atmosphere, particularly in highly polluted regions.
54 ENVIRONMENTAL SCIENCES↗
Facile synthesis of co-doped Carbon nanofibers for supercapacitor applications
Here, in this study, the synthesis and electrochemical performance of carbon nanofibers (CNFs) co-doped with aluminum (Al) and nitrogen (N) and decorated with zinc oxide (ZnO) nanoparticles are investigated. After electrospinning polyacrylonitrile (PAN) nanofibers, the nanofiber mats are coated with Al and ZnO precursors by the dip coating method and converted into carbon nanofibers by thermal treatments at 850 °C. Co-doping and nanoparticle decoration affect the efficacy of carbon nanofibers as supercapacitors. With a maximal specific capacitance of 206.28 Fg -1 , it is believed that our produced carbon nanofibers, which can effectively store the renewable energy resources required to meet the rising energy demand, offer superior electrochemical properties compared to traditional supercapacitor materials. The effective incorporation of Al, N, and ZnO into the CNF structure, in conjunction with enhanced electrochemical performance, represents a significant advancement in the development of functional carbon nanofibers.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Ion and Hydrodynamic Translucency in 1D van der Waals Heterostructured Boron-Nitride Single-Walled Carbon Nanotubes
An unresolved challenge in nanofluidics is tuning ion selectivity and hydrodynamic transport in pores, particularly for those with diameters larger than a nanometer. In contrast to conventional strategies that focus on changing surface functionalization or confinement degree by varying the radial dimension of the pores, we explore a unique approach for manipulating ion selectivity and hydrodynamic flow enhancement by externally coating single-walled carbon nanotubes (SWCNTs) with a few layers of hexagonal boron nitride (h-BN). Here, for van der Waals heterostructured BN-SWCNTs, we observed a 9-fold increase in cation selectivity for K + versus Cl – compared to pristine SWCNTs of the same 2.2 nm diameter, while hydrodynamic slip lengths decreased by more than an order of magnitude. These results suggest that the single-layer graphene inner surface may be translucent to charge-regulation and hydrodynamic-slip effects arising from h-BN on the outside of the SWCNT. Such 1D heterostructures could serve as synthetic platforms with tunable properties for exploring distinct nanofluidic phenomena and their potential applications.
36 MATERIALS SCIENCE↗
Heat Transfer of Supercritical Carbon Dioxide in 3D-Printed Tubes with Internal Ribs and Yttria Stabilized Zirconia Coating
This technical report describes measurements performed in NETL’s Heat Exchanger Experimental Test (HEET) facility using supercritical carbon dioxide as the working fluid. 3D printed tubes with internal ribs and yttria stabilized zirconia (YSZ) exterior coatings were employed in the heat exchanger. Heat transfer and friction factor enhancements from the internal ribs were characterized over a range of flow conditions. Additionally, the thermal resistance from the YSZ coating was characterized for both a freshly applied coating and a coating subjected to thermal aging.
36 MATERIALS SCIENCE↗
Bioinspired synthesis of thermally stable and mechanically strong nanocomposite coatings
Abstract An innovative biomimetic method has been developed to synthesize layered nanocomposite coatings using silica and sugar-derived carbon to mimic the formation of a natural seashell structure. The layered nanocomposites are fabricated through alternate coatings of condensed silica and sugar. Sugar-derived carbon is a cost-effective material as well as environmentally friendly. Pyrolysis of sugar will form polycyclic aromatic carbon sheets, i.e., carbon black. The resulting final nanocomposite coatings can survive temperatures of more than 1150 °C and potentially up to 1650 °C. These coatings have strong mechanical properties, with hardness of more than 11 GPa and elastic modulus of 120 GPa, which are 80% greater than those of pure silica. The layered coatings have many applications, such as shielding in the form of mechanical barriers, body armor, and space debris shields. Graphical abstract
36 MATERIALS SCIENCE↗
Influence of Coating Method on the Performance of Roll-to-Roll Coated PEM Fuel Cell Catalyst Layers
As production of fuel cell vehicles and power systems increases there is a need to understand the process science of fuel cell manufacturing. Industrial production of polymer electrolyte membrane fuel cell (PEMFC) electrodes will rely on continuous roll-to-roll (R2R) coating methods to meet the rates needed for mass production. There are a variety of coating methods that could be used to coat catalyst layers. The different physics of each method may result in different morphologies and performance. Here we present the results of a study comparing fuel cell catalyst layers coated using two R2R coating methods: slot-die and gravure. These two methods were selected because the physics of applying the liquid to the substrate is very different between the two cases. Pt/C catalysts layers were coated directly onto carbon-fiber gas diffusion media to create gas diffusion electrodes (GDEs), without the use of a decal transfer process. These GDEs were assembled into membrane electrode assemblies (MEAs) by hot pressing to Nafion membranes. In situ performance and other electrochemical diagnostics were used to determine the influence of coating method on catalyst layer electrochemical properties. Electron microscopy was utilized to understand the influence of coating method on electrode morphology and its influence on electrochemical properties. We also explored the influence of solvent ratio to understand the potential coupling between ink formulation and coating methodology.
DIRECT ENERGY CONVERSION,MATERIALS SCIENCE↗