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All sources NASA NTRS DOE OSTI

DOE OSTI2025

Dynamic Accounting of Carbon Uptake in the Built Environment

Transforming building materials from net life-cycle CO 2 e emitters to carbon sinks is a key pathway towards decarbonizing the industrial sector. Current life-cycle assessments of materials (particularly “low-carbon” materials) often focus on cradle-to-gate emissions, which can exclude emissions and uptake (i.e., fluxes) later in the materials’ life-cycle. Further, conventional CO 2 e emission characterization disregards the dynamic effects of the timing of emissions and uptake on cumulative radiative forcing from processes like manufacturing, biomass growth, and the decadal carbon storage in long-lived building materials. This work presents a framework to analyze the cradle-to-grave CO 2 e balance of building materials using a time-dependent global warming potential calculation. We apply this framework in the dynamic accounting of carbon uptake in the built environment (D-CUBE) tool and examine two case studies: concrete and cross-laminated timber (CLT). When accounting for dynamic effects, the long storage time of biogenic carbon in CLT results in reduced warming, while the slow rate of uptake via concrete carbonation does not result in significant reductions in global warming. The D-CUBE tool allows for consistent comparisons across materials and emissions mitigation strategies at varying life-cycle stages and can be adapted to other materials or systems with different lifespans and applications. The flexibility of D-CUBE and the ability to identify CO 2 e emission hot-spot life-cycle stages will be instrumental in identifying pathways to achieving net-carbon-sequestering building materials.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1997

Electric Arc and Electrochemical Surface Texturing Technologies

Surface texturing of conductive materials can readily be accomplished by means of a moving electric arc which produces a plasma from the environmental gases as well as from the vaporized substrate and arc electrode materials. As the arc is forced to move across the substrate surface, a condensate from the plasma re-deposits an extremely rough surface which is intimately mixed and attached to the substrate material. The arc textured surfaces produce greatly enhanced thermal emittance and hold potential for use as high temperature radiator surfaces in space, as well as in systems which use radiative heat dissipation such as computer assisted tomography (CAT) scan systems. Electrochemical texturing of titanium alloys can be accomplished by using sodium chloride solutions along with ultrasonic agitation to produce a random distribution of craters on the surface. The crater size and density can be controlled to produce surface craters appropriately sized for direct bone in-growth of orthopaedic implants. Electric arc texturing and electrochemical texturing techniques, surface properties and potential applications will be presented.

Banks, Bruce A.↗

DOE OSTI2023

Probing and controlling oxygen impurity diffusion in h -BN semi-bulk crystals

Combining its unique features of ultrawide bandgap (UWBG) and two-dimensional nature, h-BN has been explored for emerging applications such as deep ultraviolet optoelectronic devices and single photon emitters. One of the unusual applications of h-BN is for solid-state neutron detectors by utilizing the property of high thermal neutron capture cross section of B-10 as well as its UWBG properties. Although a record high detection efficiency of 59% has been attained by h-BN detectors, the understanding/minimization of defects and impurities is still needed to further advance the h-BN material and detector technologies. We report metal organic chemical vapor deposition growth and oxygen (O) impurity diffusion in thick h-BN. The diffusion coefficient (D) of O impurities has been measured via the evolution of an oxygen related emission with the etching depth, providing a value of D of ∼ 2 × 10−13 cm2/s at 1450 °C and supporting the interpretation that oxygen in h-BN is a substitutional donor. A multiple-buffer-layer approach was employed to mitigate to a certain degree the issue of oxygen diffusion from sapphire substrate during growth. It was demonstrated that the performance of h-BN neutron detectors fabricated from the wafer incorporating multiple buffer layers was significantly improved, as manifested by the enhanced thermal neutron detection efficiency. The advancement of the crystal growth technology of h-BN semi-bulk crystals creates applications in optoelectronic and power electronic devices utilizing the UWBG semiconductor properties of h-BN, while high efficiency h-BN neutron detectors have the potential to supplant the traditional He-3 gas detectors in various application areas by offering the obvious advantages of UWBG semiconductor technologies.

Physics↗

NASA NTRS2004

A New Process for Fabricating Random Silicon Nanotips

An improved process for the fabrication of random arrays of silicon nanotips has been demonstrated to be feasible. Relative to other such processes, this process offers advantages of low cost and simplicity. Moreover, this process can readily be combined with other processes used to fabricate integrated circuits and other monolithic silicon structures. Arrays of silicon nanotips are subjects of research and development efforts directed toward utilizing them as field emitters in flat-panel displays, vacuum microelectronics, and microwave devices. Other silicon-nanotip-fabrication processes developed thus far predominantly include lithography, etching, and/or elaborate deposition steps followed by oxide sharpening steps and are both process intensive as well as expensive. In addition to being cheaper and simpler, the present process can efficiently produce silicon nanotips that range in height from a few microns to several tens of microns and are distributed over large areas. The process mentioned here can be summarized as consisting of (1) the growth of micro-etch masks on a silicon substrate, followed by (2) etching away of the masks, along with some of the substrate, to make an array of sharp tips. In the first step of the process, a cleaned silicon substrate is subjected to reactive ion etching (RIE) in a certain mixture of oxygen and carbon tetrafluoride under radio-frequency excitation. This process step results in the growth of fluorine based compounds in the form of stumps randomly distributed on the substrate. These stumps are known in the art as polymer RIE grass. The dimensions of these stumps are of the order of hundreds of nanometers, the exact values depending on process time and gas composition. The areal density of the stumps decreases with increasing process time as they grow and merge with neighboring stumps. These stumps constitute the micro-etch masks for the next step of the process. In the second step of the process, the substrate covered with the microetch masks is subjected to deep reactive ion etching (DRIE) process, which consists of cycles of reactive ion etching alternating with passivation (the Bosch process). The gas used in the etching substeps is sulfur hexafluoride (SF6); the gas used in the passivation substeps is octafluorocyclobutane (C4F8). The portions of the substrate directly under the RIE grass stubs are etched more slowly than are the portions between the stubs. Hence, what remains at the end of the process, after the stubs and parts of the substrate have been etched away, are silicon spikes where the stubs were (see figure). In a variation of the process, one starts with a silicon or silicon-on-insulator substrate with the intent to etch through the full thickness of the substrate. That is to say, one chooses the thickness so that the DRIE step releases individual nanotips. Such individual silicon nanotips may have utility as microscopic probes in biomedical applications.

Manohara, Harish↗

DOE OSTI2019

Effects of soiling and weathering on the albedo of building envelope materials: Lessons learned from natural exposure in two European cities and tuning of a laboratory simulation practice

Chemical and physical stress, weathering, organic and inorganic matter deposition, and microbial growth over time, or “aging”, affect the optical-radiative performance of building envelope materials. Natural exposure helps to quantify these effects, but it usually requires several years. Further, the contribution of the different degradation agents cannot be isolated, and results from different campaigns cannot be easily compared because of the variability in the boundary conditions producing aging. Here in this paper we present an adaptation of the protocol implemented by ASTM as D7897-18 “Standard Practice for Laboratory Soiling and Weathering of Roofing Materials to Simulate Effects of Natural Exposure on Solar Reflectance and Thermal Emittance”. The aim is to reproduce in the laboratory the changes in albedo (solar reflectance) and thermal emittance experienced by building envelope materials in European urban areas rather than in the United States. We tuned the spraying duration and weathering cycles, and we compared the UV–vis–NIR reflectances of naturally-aged specimens (48 months in Rome and Milan) of roofing and wall finish materials to those exposed to laboratory weathering and soiling. Excluding those materials that show early physical-chemical degradation, the mean absolute deviation between natural and laboratory exposure of roofing products is equal to 0.027 in albedo. This is a lower value than the differences between two natural exposure campaigns at the same site. We clearly defined the limits of application of the protocol, providing an appraisal of the repeatability of natural aging. Moreover, we identified possible improvements in the methodology to conduct both natural and laboratory exposure.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Exploring and Embracing Heterogeneity in Atomically Thin Energy Materials

Atomically thin semiconductors offer extraordinary opportunities for the manipulation of charge carriers, many-body optical excitations, quantum light emitters, and non-charge based quantum numbers. Confinement and reduced dielectric screening in these two-dimensional (2D) materials give rise to large characteristic energies so that many-body and quantum effects are important even at room temperature. Optical excitations in extended homogeneous areas have been investigated intensely, albeit mostly focusing on a limited set of materials, particularly transition metal dichalcogenides. Much less understood are light-matter interactions for other classes of 2D semiconductors, as well as effects that arise in heterogeneous materials, either near naturally occurring defects, impurities, edges and grain boundaries, or as a result of intentional interface formation in heterostructures. Addressing such systems experimentally involves significant challenges: Understanding the atomistic growth mechanisms of 2D semiconductors, so that novel systems with designed properties, specific ‘imperfections’, or controlled interfaces can be realized; and probing of local excitations at scales that match the relevant (micrometer to nanometer) length scales in heterogeneous materials. In this research project, we addressed these challenges by harnessing quantitative in-situ microscopy to study the growth of 2D and layered semiconductors and heterostructures, combined with local spectroscopic measurements of quasiparticles excited at the nanometer scale. An integral part of the research has been the development of novel experimental approaches, both for in-situ microscopy of synthesis and for nanometer-scale spectroscopy. In particular, advanced techniques were developed for cathodoluminescence in scanning transmission electron microscopy (STEM-CL) where a nanometer-focused electron beam is used to locally excite electron-hole pairs, excitons, as well as propagating hybrid light-matter modes such as exciton-polaritons. Experiments were guided and analyzed via computations of structure, chemistry, and excitation spectra. The particular materials focus has been on group IV chalcogenides, a family of less explored 2D/layered semiconductors whose diversity in crystal structure and properties promises access to novel materials architectures and the discovery of phenomena that can support emerging technology needs.

36 MATERIALS SCIENCE↗

NASA NTRS2006

Quantum-Dot Laser for Wavelengths of 1.8 to 2.3 micron

The figure depicts a proposed semiconductor laser, based on In(As)Sb quantum dots on a (001) InP substrate, that would operate in the wavelength range between 1.8 and 2.3 m. InSb and InAsSb are the smallest-bandgap conventional III-V semiconductor materials, and the present proposal is an attempt to exploit the small bandgaps by using InSb and InAsSb nanostructures as midinfrared emitters. The most closely related prior III-V semiconductor lasers are based, variously, on strained InGaAs quantum wells and InAs quantum dots on InP substrates. The emission wavelengths of these prior devices are limited to about 2.1 m because of critical quantum-well thickness limitations for these lattice mismatched material systems. The major obstacle to realizing the proposed laser is the difficulty of fabricating InSb quantum dots in sufficient density on an InP substrate. This difficulty arises partly because of the weakness of the bond between In and Sb and partly because of the high temperature needed to crack metalorganic precursor compounds during the vapor-phase epitaxy used to grow quantum dots: The mobility of the weakly bound In at the high growth temperature is so high that In adatoms migrate easily on the growth surface, resulting in the formation of large InSb islands at a density, usually less than 5 x 10(exp 9) cm(exp -2), that is too low for laser operation. The mobility of the In adatoms could be reduced by introducing As atoms to the growth surface because the In-As bond is about 30 percent stronger than is the In-Sb bond. The fabrication of the proposed laser would include a recently demonstrated process that involves the use of alternative supplies of precursors to separate group-III and group-V species to establish local non-equilibrium process conditions, so that In(As)Sb quantum dots assemble themselves on a (001) InP substrate at a density as high as 4 x 10(exp 10) cm(exp -2). Room-temperature photoluminescence spectra of quantum dots formed by this process indicate that they emit at wavelengths from 1.7 to 2.3 microns.

Qiu, Yueming↗

DOE OSTI2024

Improving luminescence response in ZnGeN 2 /GaN superlattices: defect reduction through composition control

Abstract Color-mixed (cm) light-emitting diodes (LEDs) are theoretically the most efficient white light emitters, projected to improve white light luminous efficacy by 34% compared to incumbent phosphor converted LEDs. Since white light technology is pervasive and essential, small improvements in LED technology can result in energy savings. However, cm-LEDs are not yet realized due to poor efficacy in green and amber emitting materials, a spectral region colloquially referred to as the Green Gap. ZnGeN 2 is nearly isostructural and closely lattice-matched to GaN and can be heteroepitaxially integrated with existing GaN devices; ZnGeN 2 /GaN hybrid structures are theorized to emit green (~530 nn) light with a spontaneous emission rate 4.6–4.9 times higher than traditional InGaN LEDs when incorporated into III-N LED structures. In this report we demonstrate the molecular beam epitaxy (MBE) growth of GaN and ZnGeN 2 superlattices, an important step towards realizing multiple quantum well structures required for efficient LEDs. Elemental analysis, including atom probe tomography, shows that Ga and Ge are observed in both ZnGeN 2 and GaN layers, degrading the structural uniformity. The lack of elemental abruptness also leads to increased defect luminescence and reabsorption of band edge luminescence. The source of unintentional Ga distributed throughout the ZnGeN 2 layers was identified as excess flux escaping from around the closed MBE shutter. The source of unintentional Ge, which tended to incorporate as a single delta-doped layer in GaN, was identified as Ge riding along the cyclical metal-rich Ga adlayer used for high quality GaN, incorporating during subsequent nitrogen-rich growth step. Modifying the growth strategy results in improved structural quality, elemental abruptness, and luminescence response. This realization of structurally and elementally abrupt interfaces demonstrates the potential of heteroepitaxially integrated binary and ternary nitrides for energy-relevant devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS1999

Infalling Planetesimals in Pre-Main Sequence Stellar Systems

These are exciting times in the study of planetary system formation with a steadily expanding inventory of exo-planet detections, and imaging of dust disks around nearby young and main sequence stars. While these discoveries imply that our Solar System is far from unique, linking the data for the protoplanetary and debris disks to mature planetary systems requires a demonstration that disk evolution proceeds via planetesimal production and growth to the formation of planets. Theoretical studies of planet formation indicate that planetesimals grow, via runaway accretion, to lunar-sized (approx. = 2000 km) embryos in 10(exp 5) years. Recent gas giant planet formation studies have suggested that most of the action in planet formation occurs over 1-16 Myr, with formation of planets similar to Jupiter in t less than 10 Myr, within the time interval that infrared (IR) and optical emission line studies have demonstrated that circumstellar material remains detectable around both solar mass and intermediate mass stars. Direct imaging of exo-planetesimals is not feasible with current and foreseeable technology, since such bodies have substantially less surface area than micron-sized grains distributed in a disk, and thus are inefficient IR emitters. However, such bodies may be indirectly detectable.

Grady, Carol A.↗

DOE OSTI2022

Biochemical and spectroscopic characterizations of the oligomeric antenna of the coral symbiotic Symbiodiniaceae Fugacium kawagutii

Light-harvesting antennas in photosynthesis capture light energy and transfer it to the reaction centers (RCs) where photochemistry takes place. The sustainable growth of the reef-building corals relies on a constant supply of the photosynthates produced by the endosymbiotic dinoflagellate, belonging to the family of Symbiodiniaceae. The antenna system in this group consists of the water-soluble peridinin-chlorophyll $\textit{a}$-protein (PCP) and the intrinsic membrane chlorophyll $\textit{a}$-chlorophyll $c_2$-peridinin protein complex (acpPC). In this report, a nonameric acpPC is reported in a dinoflagellate, Fugasium kawagutii (formerly Symbiodinium kawagutii sp. CS-156). We found that extensive biochemical purification altered the oligomerization states of the initially isolated nonameric acpPC. The excitation energy transfer pathways in the acpPC nonamer and its variants were studied using time-resolved fluorescence and time-resolved absorption spectroscopic techniques at 77 K. Compared to the well-characterized trimeric acpPC, the nonameric acpPC contains an 11 nm red-shifted terminal energy emitter and substantially altered excited state lifetimes of Chl $\textit{a}$. The observed energetic overlap of the fluorescence terminal energy emitters with the absorption of RCs is hypothesized to enable efficient downhill excitation energy transfer. Additionally, the shortened Chl $\textit{a}$ fluorescence decay lifetime in the oligomeric acpPC indicate a protective self-relaxation strategy. We propose that the highly-oligomerized acpPC nonamer represents an intact functional unit in the Symbiodiniaceae thylakoid membrane. They perform efficient excitation energy transfer (to RCs), and are under manageable regulations in favor of photoprotection.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2021

Probing configurational disorder in ZnGeN 2 using cluster-based Monte Carlo

ZnGeN 2 is sought as a semiconductor with comparable lattice constant to GaN and tunable band gap for integration in optoelectronic devices. Configurational disorder on the cation sublattice of ZnGeN 2 can strongly modify the electronic structure compared to the ordered material, and both ordered and disordered forms of ZnGeN 2 are candidates for light-emitting diodes and other emitters. The nonisovalent character of the disordered species (Zn 2+ and Ge 4+ ) subjects the cation ordering to strong short-range order effects. To model these effects, we use Monte Carlo (MC) simulations utilizing a cluster expansion to approximate formation enthalpy. Representative disordered configurations in 1024-atom supercells are relaxed in density functional theory calculations. From the MC structures, we extract a short-range order parameter (the N-cation coordination motif), and two long-range order parameters (Bragg-Williams and stretching parameters), and examine their correlations. We perform a thermodynamic integration to determine the mixing entropy and free energy. ZnGeN 2 exhibits a first-order phase transition with pronounced discontinuities in enthalpy and entropy, as well as in the structural order parameters. We discuss the relationship between the effective temperature used in the MC simulation and the growth temperatures in experiment in relation to the crossover from the nonequilibrium to the equilibrium growth regime. This work expands on current models of site disorder in ZnGeN 2 and provides atomic structure models with a systematic variation of the degree of cation disorder.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Role of shell composition and morphology in achieving single-emitter photostability for green-emitting “giant” quantum dots

The use of the varied chemical reactivity of precursors to drive the production of a desired nanocrystal architecture has become a common method to grow thick-shell graded alloy quantum dots (QDs) with robust optical properties. Conclusions on their behavior assume the ideal chemical gradation and uniform particle composition. In this work, advanced analytical electron microscopy (high-resolution scanning transmission electron microscopy coupled with energy dispersive spectroscopy) is used to confirm the nature and extent of compositional gradation and these data are compared with performance behavior obtained from single-nanocrystal spectroscopy to elucidate structure, chemical-composition, and optical-property correlations. In particular, the evolution of the chemical structure and single-nanocrystal luminescence was determined for a time-series of graded-alloy “CdZnSSe/ZnS” core/shell QDs prepared in a single-pot reaction. In a separate step, thick (~6 monolayers) to giant (>14 monolayers) shells of ZnS were added to the alloyed QDs via a successive ionic layer adsorption and reaction (SILAR) process, and the impact of this shell on the optical performance was also assessed. By determining the degree of alloying for each component element on a per-particle basis, we observe that the actual product from the single-pot reaction is less “graded” in Cd and more so in Se than anticipated, with Se extending throughout the structure. The latter suggests much slower Se reaction kinetics than expected or an ability of Se to diffuse away from the initially nucleated core. It was also found that the subsequent growth of thick phase-pure ZnS shells by the SILAR method was required to significantly reduce blinking and photobleaching. However, correlated single-nanocrystal optical characterization and electron microscopy further revealed that these beneficial properties are only achieved if the thick ZnS shell is complete and without large lattice discontinuities. Thus, we identify the necessary structural design features that are required for ideal light emission properties in these green-visible emitting QDs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Field-Emission Properties of Vertically Aligned Carbon Nanotube Cathodes of Varying Geometries

This work characterizes the bulk emission properties of carbon nanotube (CNT) forest cathodes fabricated with various geometries. Geometries explored include dense nanotube forests of varying height grown on 5×5 mm silicon (Si) substrates and discrete, patterned CNT pillars fabricated using UV photolithography. Dense forests heights ranged from 526 μ m to 1.41 mm, with packing fraction for dense forest calculated to be 4e10 nanotubes/cm2 based on an average nanotube separation distance of 100 nm for fixed growth dense forests. Patterned sample micro pillar heights ranged from 47 to 393 μ m with pillar widths on tested samples ranging from 250 to 270 μ m . Properties explored include emission current, turn-on field, and emission current performance over time. A parallel plate electron beam diode with a 100- μ m A-K gap and an automated test apparatus were developed to provide a configurable experiment that provides accurate and repeatable measurements for dc, dc sweep, and timed performance testing. Operating voltages for the voltage sweeps spanned from 0 to −350 V. Furthermore, testing has shown evidence of a hysteresis effect on the emission current tied to the applied field history as well as shifting of the turn-on field magnitude throughout the testing period, suggesting a conditioning effect during use. Three separate emission regions in the I–V curves during sweep testing have also been observed. In the geometric study, dense forests and patterned samples were sweep tested up to a peak applied voltage of −250 V, with the taller samples generally performing better. Currents produced in the geometric study from the dense forest emitters ranged from 36.8 to 572.34 μ A , with current densities ranging from 15 to 2.29 mA/cm2. Currents produced from the patterned micropillar emitters ranged from 39.4 to 317.51 μ A , with current densities ranging from 67 to 3 mA/cm2. DC time testing s...

36 MATERIALS SCIENCE↗

NASA NTRS2018

Modification of Radiator Pigments by Atomic Layer Deposition (ALD)

The optical and physical properties of spacecraft radiator coatings are dictated by orbital environmental conditions. For example, coatings must adequately dissipate charge buildup when orbital conditions, such as polar, geostationary or gravity neutral, result in surface charging. Current dissipation techniques include depositing a layer of ITO (indium tin oxide) on the radiator surface in a high temperature process. Other examples include the application of variable emittance coatings such as the use of VO2 to optimize radiator size, allowing for a decrease in heater power budget. The application of these enhanced coatings must be such that the properties in question are tailored to mission-specific requirements. Modification of these coatings can be accomplished during coating application preprocessing by using a deposition technique prevalent in the semiconductor micro processing industry called Atomic Layer Deposition (ALD). The preprocessing is rendered directly on the coating dry pigment before binding. ALD is a cost effective nano-manufacturing technique that allows for the conformal coating of substrates with atomic-level thickness control in a benign temperature and pressure environment. Through the introduction of paired precursor gases, thin films can be deposited on a myriad of substrates ranging from glass, polymers, aerogels, metals, powders, and other high aspect-ratio micro- and nano-structures. By providing atomic-level control, where single layers of atoms can be deposited, the fabrication of metal transparent films, precise nano-laminates, and coatings of nano-channels and pores is achievable. We have demonstrated a method for the ALD of In2O3 and ITO films on a variety of substrates from Si(100) wafers, glass slides, and on Z93P pigments (patent pending). The results indicate excellent growth of 4-22 nm thick films demonstrating an order of magnitude decrease in resistivity on the pigments.

ITO↗

DOE OSTI2022

Investigating Local Carrier Dynamics in PERC Patterned CdTe Solar Cells

Remarkable progress has been achieved in CdTe photovoltaics (PVs) to further improve cell performance while reducing manufacturing costs. Researchers optimized the front contact that leads the short-circuit current density (J sc ) over 31mA/cm 2 (e.g., (Zn, Mg)O buffer layer and/or alloying CdTe with Se). Reese et al. reported an open-circuit voltage (V oc ) over 1 V with group-V doped single crystal, showing the feasibility of increasing V oc in CdTe PV that is fixed to less than 900 mV in most cases. Recent studies suggested that the V oc improvement in polycrystalline CdTe PVs requires well-passivated back contact. One possible strategy is to use CdMgTe alloy (E g > 1.8 eV), where the band-gap offset (ΔE CB ≈ 0.2 eV) reflects minority carrier electrons, thereby decreasing surface recombination. Another strategy is to utilize a stable Al 2 O 3 layer as an electron reflector; experimental works confirmed the improved performance with a conformal Al 2 O 3 layer. In this configuration, the precise control of Al 2 O 3 (≈1 nm) over the entire CdTe layer is essential because the J sc greatly depends on the tunneling current. While promising, both CdMgTe and Al 2 O 3 passivation on CdTe introduce unfavorable valence band offset that blocks the hole transport. Kephart et al. proposed a patterned passixc vation layer (≈ 20 nm Al 2 O 3 ) with point contacts (≈ 3 μm in diameter) that extract hole carriers. This configuration is similar to the passive emitter and rear contact (PERC) design that has been extensively studied in Si PVs. While remarkably high carrier lifetime and photoluminescence (> 10 X) were measured, consistent improvement in V oc and efficiency in this CdTe PERC were not yet observed. At this time, it is unclear how the surface potential is distributed in the presence of patterned Al 2 O 3 reflectors and how this additional field impacts the PV performance for Cu-doped and group-V doped CdTe PERC devices. To tackle this challenge, we develop robust nanofabrication and characterization platform to study CdTe PERC devices consisting of a patterned Al 2 O 3 layer on CdSe( 1-x )Te x (Cu-doped, GrV-doped; x = 0 to 1; CST). First Solar supplies high-quality CST materials. The dark and light I-Vs under 1-sun illumination are extracted for a series of each set of devices. We perform quantitative and qualitative PV analysis for a series of Cu-doped and Gr-V doped PERC devices, showing notably different V oc changes for GrV-doped compared to Cu-doped PERC devices. This project attempts to produce individual contacts on single grains and grain boundaries to measure lateral transport. As a model system, we use a CdSe( 1-x )Te x film on glass prepared by a colossal grain growth (CGG) technique at National Renewable Research Laboratories (NREL). Our preliminary results confirm that intergranular transport is hindered by the electrical barrier formed near grain boundaries. The PERC fabrication and the lateral transport measurement platform developed in this project can easily be applied to other types of advanced CdSe( 1-x )Te x architectures to better understand local photocarrier transport, in turn, providing the fundamental knowledge to improve the performance of CdTe PVs.

14 SOLAR ENERGY↗

DOE OSTI2026

Integrating Carbon Capture, Utilization, & Sequestration into Chemical Pulp Mills

The U.S. pulp and paper industry presents a unique and largely untapped opportunity for large- scale carbon dioxide removal (CDR). Unlike most industrial sectors, pulp mills rely heavily on biomass, meaning that much of their carbon emissions originate from atmospheric CO₂ that was recently captured by plants. If this biogenic CO₂ can be captured and permanently stored, pulp mills can be transformed from carbon emitters into net carbon removal facilities. This project was motivated by that opportunity and aimed to develop and evaluate integrated, low-cost strategies for capturing, utilizing, and sequestering CO₂ within existing chemical pulping operations. The scope of this work focused on four complementary innovations designed to integrate seamlessly into kraft pulp mill infrastructure: (1) in situ CO₂ capture within the recovery cycle, (2) oxy-fuel retrofitting of the rotary lime kiln to produce a high-purity CO₂ stream, (3) ex situ CO₂ capture and mineralization using pulp mill residues (dregs, grits, and lime mud), and (4) beneficial reuse of these residues as mineral carbonate fertilizers. The project combined process modeling, laboratory experimentation, life cycle assessment (LCA), and field trials to evaluate the technical feasibility, economic viability, and environmental impact of these approaches. The results demonstrate that pulp mills can serve as effective platforms for carbon removal when equipped with integrated carbon capture systems. Process modeling showed that combining sodium spiking with oxy-fuel calcination significantly enhances CO₂ capture efficiency while reducing costs by up to 31% compared to conventional configurations. Experimental work further revealed that calcination behavior in high-CO₂ environments differs substantially from traditional systems, leading to the development of a new kinetic model that predicts reaction rates under these conditions. This model provides essential design guidance for next-generation decarbonized lime kilns. In parallel, the project demonstrated that alkaline mineral residues generated during pulping operations can be repurposed as a sustainable alternative to agricultural lime. Across a wide range of soils in the southeastern United States, these materials performed equivalently to commercial lime in adjusting soil pH while offering lower greenhouse gas emissions and reduced cost. Field and greenhouse studies confirmed that crop and tree growth responses were comparable, supporting their viability as a drop-in replacement. This co-product pathway provides a practical utilization strategy that offsets costs and improves overall system economics. A major contribution of this project is the first comprehensive life cycle assessment of carbon removal in pulp and paper systems across multiple system boundaries. Results show that retrofitted mills can achieve carbon removal efficiencies ranging from 12% to 92%, depending on how the system is defined. This finding highlights a critical issue in carbon accounting: reported performance is highly sensitive to methodological choices. By explicitly quantifying these differences, this work provides valuable guidance for policymakers, carbon registries, and project developers working to standardize carbon removal metrics. From a commercialization perspective, the technologies investigated in this project are well- aligned with existing industrial infrastructure, minimizing the need for entirely new facilities. 3 DE-EE0009413 Industry engagement throughout the project—including collaboration with pulp and paper companies, equipment manufacturers, and carbon removal developers—has accelerated the transition from research to deployment. Notably, a commercial developer is actively pursuing carbon capture projects at pulp mills in the southeastern United States and has cited this research as a contributing foundation. The emergence of voluntary carbon markets and long-term offtake agreements further strengthens the business case for implementation. The broader public benefits of this work are significant. By enabling large-scale carbon removal using existing industrial systems, this approach offers a near-term pathway to reduce atmospheric CO₂ concentrations while supporting domestic manufacturing and rural economies. The reuse of industrial residues as fertilizers reduces reliance on mined materials, lowers costs for farmers, and decreases environmental impacts associated with conventional lime production. In addition, the project has supported workforce development by training graduate students and researchers in carbon capture technologies, helping to build capacity in a critical area of national interest. In conclusion, this project demonstrates that integrated carbon capture, utilization, and sequestration in pulp mills is both technically feasible and economically promising. By combining process innovation, experimental validation, and systems-level analysis, the work advances the understanding of how biomass-based industries can contribute to climate mitigation. The findings provide a strong foundation for commercial deployment and offer a scalable solution for transforming a major U.S. industry into a source of durable carbon removal.

09 BIOMASS FUELS↗

DOE OSTI2021

Novel Algae Technology for CO2 Utilization

The United States, the world’s largest energy user and second largest CO2 emitter, is heavily dependent on fossil energy. In 2014, U.S. coal burning utilities emitted ~1562 million (MM) tons/year (TPY) of CO2 into the atmosphere, accounting for 76% of the total US power sector emissions1. Hence, reducing the CO2 emission footprint from coal plants is widely viewed as a key element in mitigating global warming. Despite significant interest, implementation of CO2 capture technologies has been constrained by the high capture cost which significantly increases the total cost of electricity. Not only is capturing CO2 with traditional technologies expensive, but generally the CO2 has little value and additional expense must be incurred for sequestration. This project funded by a SBIR grant from the U.S. D.O.E. to Helios-NRG in collaboration with the State University of New York at Buffalo (UB) and Membrane Technology and Research Inc. (MTR) aimed to develop a novel, algae based technology to capture CO2 from the effluent of coal-based power plants and convert it to renewable bio-fuels and higher value co-products such as animal feed and nutraceuticals with the potential to enable a substantial reduction in the net cost of carbon capture. The Phase 2 project was aimed at further demonstrating the technical feasibility of the proposed multi-stage continuous (MSC) flow CO2 capture system and the generation of high-value co-products to offset the CO2 capture cost. The project was completed and the project objectives were met and exceeded. A first-of-a-kind integrated, laboratory scale MSC process unit was fabricated and tested in a greenhouse. The tests were conducted with the preferred algae species identified in Phase I and simulated flue gas containing contaminants at levels typically present in the post flue gas desulfurization (FGD) stream, including ~12% CO2, acid gas (SOX, NOX), and a large number of heavy metals. The tests were successful and demonstrated a 25g/m2/day seasonal average algae productivity and an 80% CO2 capture efficiency. Two new algae species were identified for high-value nutraceutical production. Studies to improve growth rate and nutraceutical content of these algae species were performed and a pathway for further improvements was identified. A new dewatering technology called DeAqua was further advanced. Significant improvement in the performance index was achieved. The anti-fouling membrane was developed and fabricated into a module. The fabricated membrane module was tested with algae slurry and demonstrated improved fouling resistant properties, that can potentially reduce the cost and energy of the critical dewatering step. Test data were used to simulate operation of the overall process. The preliminary economic analysis was updated and modelled based on a 5000-acre algae farm. To the extent possible, the financial and operating assumptions used were the same as those used in the DOE’s 2022 projections for algae technology for CO2 capture and utilization. The results showed the proposed technology’s potential to significantly reduce the cost of CO2 capture compared to current options and that the high value products generated from the CO2 captured can make a step change in the cost of carbon capture. Plans to advance the technology to Phase 2B were developed and potential end-user partners were identified.

Maloney, James↗

DOE OSTI2025

Global Methane Budget 2000–2020

Abstract. Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. CH4 is the second most important human-influenced greenhouse gas in terms of climate forcing after carbon dioxide (CO2), and both emissions and atmospheric concentrations of CH4 have continued to increase since 2007 after a temporary pause. The relative importance of CH4 emissions compared to those of CO2 for temperature change is related to its shorter atmospheric lifetime, stronger radiative effect, and acceleration in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in quantifying the factors responsible for the observed atmospheric growth rate arise from diverse, geographically overlapping CH4 sources and from the uncertain magnitude and temporal change in the destruction of CH4 by short-lived and highly variable hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to improve, synthesise, and update the global CH4 budget regularly and to stimulate new research on the methane cycle. Following Saunois et al. (2016, 2020), we present here the third version of the living review paper dedicated to the decadal CH4 budget, integrating results of top-down CH4 emission estimates (based on in situ and Greenhouse Gases Observing SATellite (GOSAT) atmospheric observations and an ensemble of atmospheric inverse-model results) and bottom-up estimates (based on process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). We present a budget for the most recent 2010–2019 calendar decade (the latest period for which full data sets are available), for the previous decade of 2000–2009 and for the year 2020. The revision of the bottom-up budget in this 2025 edition benefits from important progress in estimating inland freshwater emissions, with better counting of emissions from lakes and ponds, reservoirs, and streams and rivers. This budget also reduces double counting across freshwater and wetland emissions and, for the first time, includes an estimate of the potential double counting that may exist (average of 23 Tg CH4 yr−1). Bottom-up approaches show that the combined wetland and inland freshwater emissions average 248 [159–369] Tg CH4 yr−1 for the 2010–2019 decade. Natural fluxes are perturbed by human activities through climate, eutrophication, and land use. In this budget, we also estimate, for the first time, this anthropogenic component contributing to wetland and inland freshwater emissions. Newly available gridded products also allowed us to derive an almost complete latitudinal and regional budget based on bottom-up approaches. For the 2010–2019 decade, global CH4 emissions are estimated by atmospheric inversions (top-down) to be 575 Tg CH4 yr−1 (range 553–586, corresponding to the minimum and maximum estimates of the model ensemble). Of this amount, 369 Tg CH4 yr−1 or ∼ 65 % is attributed to direct anthropogenic sources in the fossil, agriculture, and waste and anthropogenic biomass burning (range 350–391 Tg CH4 yr−1 or 63 %–68 %). For the 2000–2009 period, the atmospheric inversions give a slightly lower total emission than for 2010–2019, by 32 Tg CH4 yr−1 (range 9–40). The 2020 emission rate is the highest of the period and reaches 608 Tg CH4 yr−1 (range 581–627), which is 12 % higher than the average emissions in the 2000s. Since 2012, global direct anthropogenic CH4 emission trends have been tracking scenarios that assume no or minimal climate mitigation policies proposed by the Intergovernmental Panel on Climate Change (shared socio-economic pathways SSP5 and SSP3). Bottom-up methods suggest 16 % (94 Tg CH4 yr−1) larger global emissions (669 Tg CH4 yr−1, range 512–849) than top-down inversion methods for the 2010–2019 period. The discrepancy between the bottom-up and the top-down budgets has been greatly reduced compared to the previous differences (167 and 156 Tg CH4 yr−1 in Saunois et al. (2016, 2020) respectively), and for the first time uncertainties in bottom-up and top-down budgets overlap. Although differences have been reduced between inversions and bottom-up, the most important source of uncertainty in the global CH4 budget is still attributable to natural emissions, especially those from wetlands and inland freshwaters. The tropospheric loss of methane, as the main contributor to methane lifetime, has been estimated at 563 [510–663] Tg CH4 yr−1 based on chemistry–climate models. These values are slightly larger than for 2000–2009 due to the impact of the rise in atmospheric methane and remaining large uncertainty (∼ 25 %). The total sink of CH4 is estimated at 633 [507–796] Tg CH4 yr−1 by the bottom-up approaches and at 554 [550–567] Tg CH4 yr−1 by top-down approaches. However, most of the top-down models use the same OH distribution, which introduces less uncertainty to the global budget than is likely justified. For 2010–2019, agriculture and waste contributed an estimated 228 [213–242] Tg CH4 yr−1 in the top-down budget and 211 [195–231] Tg CH4 yr−1 in the bottom-up budget. Fossil fuel emissions contributed 115 [100–124] Tg CH4 yr−1 in the top-down budget and 120 [117–125] Tg CH4 yr−1 in the bottom-up budget. Biomass and biofuel burning contributed 27 [26–27] Tg CH4 yr−1 in the top-down budget and 28 [21–39] Tg CH4 yr−1 in the bottom-up budget. We identify five major priorities for improving the CH4 budget: (i) producing a global, high-resolution map of water-saturated soils and inundated areas emitting CH4 based on a robust classification of different types of emitting ecosystems; (ii) further development of process-based models for inland-water emissions; (iii) intensification of CH4 observations at local (e.g. FLUXNET-CH4 measurements, urban-scale monitoring, satellite imagery with pointing capabilities) to regional scales (surface networks and global remote sensing measurements from satellites) to constrain both bottom-up models and atmospheric inversions; (iv) improvements of transport models and the representation of photochemical sinks in top-down inversions; and (v) integration of 3D variational inversion systems using isotopic and/or co-emitted species such as ethane as well as information in the bottom-up inventories on anthropogenic super-emitters detected by remote sensing (mainly oil and gas sector but also coal, agriculture, and landfills) to improve source partitioning. The data presented here can be downloaded from https://doi.org/10.18160/GKQ9-2RHT (Martinez et al., 2024).

54 ENVIRONMENTAL SCIENCES↗