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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 289 records · Page 16
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Role of Solvent in the Oriented Growth of Conductive Ni‐CAT‐1 Metal‐Organic Framework at Solid–Liquid Interfaces

Abstract A controlled growth of two‐dimensional (2D) π‐conjugated metal‐organic frameworks (MOFs) on solid substrates can open exciting opportunities for the application of 2D MOFs as optoelectronic devices. Some factors like solvent composition and type of substrates are known to influence the properties of solution‐processed 2D MOF crystals; however, a mechanistic understanding of how interactions between solvent, substrate, and precursors affect heterogeneous nucleation has been limited. Here, it is reported that the structure of Ni‐catecholate (Ni‐CAT‐1) MOFs at a solid–liquid interface is controlled by solvent–substrate and solvent–MOF precursor interactions. Specifically, the structure of the MOF film can be controlled by varying the affinity of the solvent to the substrate. As a fraction of N , N ‐dimethylformamide (DMF) in a binary solvent mixture of water and DMF increases, the arrangement of Ni‐CAT‐1 crystals varies from vertically aligned nanorods to the graphite substrate to less ordered nanorods with the lower initial nucleation number density of Ni‐CAT‐1 crystals on the surface.

2D materials↗
DOE OSTI2023

Fully Inkjet‐Printed, 2D Materials‐Based Field‐Effect Transistor for Water Sensing

Abstract Despite significant progress in solution‐processing of 2D materials, it remains challenging to reliably print high‐performance semiconducting channels that can be efficiently modulated in a field‐effect transistor (FET). Herein, electrochemically exfoliated MoS 2 nanosheets are inkjet‐printed into ultrathin semiconducting channels, resulting in high on/off current ratios up to 10 3 . The reported printing strategy is reliable and general for thin film channel fabrication even in the presence of the ubiquitous coffee‐ring effect. Statistical modeling analysis on the printed pattern profiles suggests that a spaced parallel printing approach can overcome the coffee‐ring effect during inkjet printing, resulting in uniform 2D flake percolation networks. The uniformity of the printed features allows the MoS 2 channel to be hundreds of micrometers long, which easily accommodates the typical inkjet printing resolution of tens of micrometers, thereby enabling fully printed FETs. As a proof of concept, FET water sensors are demonstrated using printed MoS 2 as the FET channel, and printed graphene as the electrodes and the sensing area. After functionalization of the sensing area, the printed water sensor shows a selective response to Pb 2+ in water down to 2 ppb. This work paves the way for additive nanomanufacturing of FET‐based sensors and related devices using 2D nanomaterials.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Molecular Layer Deposited Aluminum‐Based Hybrid Resist for High‐Resolution Nanolithography and Direct Ultra‐High Aspect Ratio Pattern Transfer

Inorganic-containing hybrid photoresists are critical for next-generation extreme ultraviolet (EUV) lithography and angstrom-era semiconductor miniaturization. However, associated conventional solution processing struggles to achieve ultrathin, uniform films with high conformality and compositional control, limiting overall patterning performance. Here, this study reports the systematic lithographic patterning characterization of an Al-based hybrid resist synthesized via vapor-phase molecular layer deposition (MLD), using the trimethylaluminum (TMA) metal precursor and the hydroquinone (HQ) aromatic organic linker. The resist supports both sub-20 nm high-resolution nanolithography and virtually infinite silicon plasma etch selectivity. Lithographic performance studied using electron beam lithography (EBL) as a proxy for EUV shows that, under an optimized process adopting post-exposure bake, the resist achieves the best resolution of 15.4 nm linewidth under stringent 1:1 line-space high-density patterning—limited only by the minimum beam size of the EBL system. The resist also shows wide dose latitude and balanced performance in resolution, roughness, and sensitivity. The infinite silicon etch selectivity, stemming from spontaneous aluminum oxyfluoride passivation layer formation, enables fabrication of micrometer-tall, 40 nm-wide silicon nanofin structures using only a ≈30 nm-thick resist layer, without no hard mask. These results highlight the potential of MLD-based hybrid resists for developing next-generation resist materials for micro/nanoelectronics manufacturing.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Narrowing the Phase Distribution of Quasi-2D Perovskites for Stable Deep-Blue Electroluminescence

Solution-processed quasi-2D perovskites contain multiple quantum wells with a broad width distribution. Inhomogeneity results in the charge funneling into the smallest bandgap components, which hinders deep-blue emission and accelerates Auger recombination. Here, a synthetic strategy applied to a range of quasi-2D perovskite systems is reported, that significantly narrows the quantum well dispersity. It is shown that the phase distribution in the perovskite film is significantly narrowed with controlled, simultaneous evaporation of solvent and antisolvent. Modulation of film formation kinetics of quasi-2D perovskite enables stable deep-blue electroluminescence with a peak emission wavelength of 466 nm and a narrow linewidth of 14 nm. Light emitting diodes using the perovskite film show a maximum luminance of 280 cd m –2 at an external quantum efficiency of 0.1%. This synthetic approach will serve in producing new materials widening the color gamut of next-generation displays.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Ultrasensitive Room Temperature Infrared Photodetection Using a Narrow Bandgap Conjugated Polymer

Abstract Photodetectors operating across the short‐, mid‐, and long‐wave infrared (SWIR–LWIR, λ = 1–14 µm) underpin modern science, technology, and society in profound ways. Narrow bandgap semiconductors that form the basis for these devices require complex manufacturing, high costs, cooling, and lack compatibility with silicon electronics, attributes that remain prohibitive for their widespread usage and the development of emerging technologies. Here, a photoconductive detector, fabricated using a solution‐processed narrow bandgap conjugated polymer is demonstrated that enables charge carrier generation in the infrared and ultrasensitive SWIR–LWIR photodetection at room temperature. Devices demonstrate an ultralow electronic noise that enables outstanding performance from a simple, monolithic device enabling a high detectivity ( D *, the figure of merit for detector sensitivity) >2.44 × 10 9 Jones (cm Hz 1/2 W −1 ) using the ultralow flux of a blackbody that mirrors the background emission of objects. These attributes, ease of fabrication, low dark current characteristics, and highly sensitive operation overcome major limitations inherent within modern narrow–bandgap semiconductors, demonstrate practical utility, and suggest that uncooled detectivities superior to many inorganic devices can be achieved at high operating temperatures.

36 MATERIALS SCIENCE↗
DOE OSTI2025

High‐Speed Slot‐Die Coating with Donor‐Priority Rapid Aggregation Kinetics for Improved Morphology and Efficiency in Ecofriendly Organic Solar Cells

Abstract Solution‐processable organic solar cells (OSCs) represent a promising renewable photovoltaic technology with significant potential for eco‐compatible production. While high power conversion efficiencies (PCEs) have been achieved in OSCs, scaling this technology for high‐throughput manufacturing remains challenging. Key reason lies in the lack of efficient control strategies for the complex and long‐duration morphology evolution during high‐speed coating process with ecofriendly solvents. Here, a donor‐priority rapid aggregation process (DP‐RAP) scheme is proposed to solve this issue by adjusting the aggregation kinetics of donor and acceptor components. DP‐RAP enables blends with a nanoscale fiber network structure and favorable crystallinity, which contributes to balanced carrier transport and reduced recombination losses. As a result, the PCE is improved from 14.3% (reference) to 17.4% (DP‐RAP) for ultra‐high speed coated PM6:BTP‐eC9 devices in atmosphere, which is one of the highest values for non‐halogenated solvent‐processed solar cells at coating speeds of 500 mm s −1 . Moreover, the DP‐RAP based devices remain a stable PCE of approximately 17.4% across a broad range of coating speeds (20–500 mm s −1 ), illustrating its tolerance to the varied manufacturing conditions. This work highlights a promising avenue for the high‐speed, ecofriendly production of efficient OSCs, pushing the boundaries of practical manufacturing in renewable energy technologies.

Chemistry↗
DOE OSTI2020

Electrical and Elastic Properties of Individual Single-Layer Nb 4 C 3 T x MXene Flakes

2D carbides and nitrides (MXenes) are widely recognized for their exceptional promise for numerous applications. However, physical property measurements of their individual monolayers remain very limited despite their importance for revealing the intrinsic physical properties of MXenes. The first mechanical and electrical measurements of individual single-layer flakes of Nb 4 C 3 T x MXene, which are prepared via an improved synthetic method are reported. Characterization of field-effect transistor devices based on individual single-layer Nb 4 C 3 T x flakes shows an electrical conductivity of 1024 ± 165 S cm -1 , which is two orders of magnitude higher than the previously reported values for bulk Nb 4 C 3 T x assemblies, and an electron mobility of 0.41 ± 0.27 cm 2 V -1 s -1 . Atomic force microscopy nanoindentation measurements of monolayer Nb 4 C 3 T x membranes yield an effective Young's modulus of 386 ± 13 GPa, assuming a membrane thickness of 1.26 nm. This is the highest value reported for nanoindentation measurements of solution-processable 2D materials, revealing the potential of Nb 4 C 3 T x as a primary component for various mechanical applications. In conclusion, the agreement between the mechanical properties of 2D Nb 4 C 3 T x MXene and cubic NbC suggests that the extensive experimental data on bulk carbides could be useful for identifying new MXenes with improved functional characteristics.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Effect of Aromatic Solvents Residuals on Electron Mobility of Organic Single Crystals

Balanced electron and hole transport properties are essential for various organic electrical/optoelectrical applications such as organic solar cells, complementary circuits, and light-emitting transistors. However, the electron transport in organic semiconductor lags far behind the hole side, making it with vital significance to seek the factors that limit the electron mobility. Here, the authors demonstrate that the π-conjugated solvents, as essential components in the widely-used solution processing techniques, can significantly suppress the electron transport if they are not properly removed and trapped as residuals. Single crystals of typical p-type materials exhibit a transition from p-type behavior to ambipolar conductance via reducing the amount of solvent residuals, and the same effect is confirmed by varied p-type materials and solvents. The highest electron mobility reaches 0.027 cm 2 V –1 s –1 and 0.029 cm 2 V –1 s –1 for 6,13-bis(triisopropylsilylethynyl)pentacene and 5,15-bis(triisopropylsilylethynyl)tetrabenzoporphyrin, respectively. Finally, this work discloses the non-negligible existence of solvent residuals even in high quality, long-range ordered organic single crystals, and further provides efficient strategies to harvest the n-type behaviors of organic semiconductor materials.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Polymer Passivated All Inorganic Micro‐Structured CsPbI x Br y Perovskite Toward Highly Efficient Photodetectors

Abstract Solution‐processed inorganic perovskites cause chemical and structural defects unfavorable for photodetector application. Using a binary solvent, defects in CsPbI x Br y (CPIB) perovskite are passivated with poly 4‐vinylpyridine (PVP) and Poly methyl methacrylate (PMMA) polymers. X‐ray photoelectron spectroscopy and FTIR spectra reveal a Lewis base‐acid interaction between Pb 2+ and polymer, confirming the passivation of CPIB perovskite. Scanning electron microscopy analysis shows a dual‐surface morphology with microribbons and microcrystals in perovskites. After PMMA treatment, CPIB perovskite exhibits a blue shift in the bandgap (1.8 to 1.95 eV), while the PVP induced a redshift, reducing the bandgap to 1.7 eV. Blue shift in PL analysis indicates modification of grain boundaries. A higher lifetime obtained for CPIB/PVP confirms the restraint of non‐radiative recombinations. Photodetectors are fabricated with pristine CPIB, CPIB/PVP, and CPIB/PMMA perovskites. The passivated CPIB/PVP‐based photodetector exhibits a quick rise time of ≈23 ms and a decay time of ≈17 ms. It also demonstrates a remarkable photoresponsivity of 23 mA W −1 , an internal quantum efficiency of 4.9%, and a detectivity of 15.0 × 10 10 Jones at 10 mW cm −2 light intensity. This approach shows the potential for environmentally stable polymers to passivate inorganic perovskites for high photodetection performance.

Shah, Shruti↗
DOE OSTI2020

Concurrently Approaching Volumetric and Specific Capacity Limits of Lithium Battery Cathodes via Conformal Pickering Emulsion Graphene Coatings

Abstract To achieve the high energy densities demanded by emerging technologies, lithium battery electrodes need to approach the volumetric and specific capacity limits of their electrochemically active constituents, which requires minimization of the inactive components of the electrode. However, a reduction in the percentage of inactive conductive additives limits charge transport within the battery electrode, which results in compromised electrochemical performance. Here, an electrode design that achieves efficient electron and lithium‐ion transport kinetics at exceptionally low conductive additive levels and industrially relevant active material areal loadings is introduced. Using a scalable Pickering emulsion approach, Ni‐rich LiNi 0.8 Co 0.15 Al 0.05 O 2 (NCA) cathode powders are conformally coated using only 0.5 wt% of solution‐processed graphene, resulting in an electrical conductivity that is comparable to 5 wt% carbon black. Moreover, the conformal graphene coating mitigates degradation at the cathode surface, thus providing improved electrochemical cycle life. The morphology of the electrodes also facilitates rapid lithium‐ion transport kinetics, which provides superlative rate capability. Overall, this electrode design concurrently approaches theoretical volumetric and specific capacity limits without tradeoffs in cycle life, rate capability, or active material areal loading.

Park, Kyu‐Young↗
DOE OSTI2020

Understanding the Reactivity of a Thin Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 Solid–State Electrolyte toward Metallic Lithium Anode

The thickness of solid-state electrolytes (SSEs) significantly affects the energy density and safety performance of all-solid-state lithium batteries. However, a sufficient understanding of the reactivity toward lithium metal of ultrathin SSEs (<100 μm) based on NASICON remains lacking. Herein, for the first time, a self-standing and ultrathin (70 μm) NASICON-type Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP) electrolyte via a scalable solution process is developed, and X-ray photoelectron spectroscopy reveals that changes in LAGP at the metastable Li-LAGP interface during battery operation is temperature dependent. Severe germanium reduction and decrease in LAGP particle size are detected at the Li-LAGP interface at elevated temperature. As a result, oriented plating of lithium metal on its preferred (110) face occurs during in situ X-ray diffraction cycling.

25 ENERGY STORAGE↗
DOE OSTI2021

Comprehensive Performance Calibration Guidance for Perovskites and Other Emerging Solar Cells

Emerging photovoltaic (PV) technologies (e.g., organic, perovskite, and solution processed quantum dot) have attracted remarkable attention with the rapid growth of their efficiencies, and their transition toward commercialization. Accurate and reliable efficiency measurements of these PV technologies are crucial, yet much more complicated than for conventional PV technologies due to the former's pronounced dynamic responses to changes in measurement conditions (e.g., current–voltage (I–V) scan rate and preconditioning) and their susceptibility to degradation. Adjustments to the measurement procedures are therefore necessary so that a reproducible “steady state” is reached during measurement. Furthermore, given the small size of many emerging cells, inappropriate device area definition and solar simulator setup can lead to measurement errors. Here, comprehensive efficiency calibration guidance is offered for emerging solar cells, including area measurement; spectral irradiance translation to standard test conditions; and steady-state electrical performance. The necessity of reporting steady-state efficiency is justified with a statistical performance comparison between conventional and steady-state I–V scans over hundreds of cells the group has received globally for efficiency certifications. The procedures described here do not require specialized measurement instrumentation; what matters most are changes to the measurement protocols. These described changes aim to enable better comparisons between reported efficiencies.

14 SOLAR ENERGY↗
DOE OSTI2026

Localized Heterogeneous Nucleation for Vapor‐Assisted Sequential Deposition of Metal Halide Perovskites

Vapor-assisted hybrid two-step deposition, which combines thermally evaporated inorganic layers with solution-processed organic halides to form halide perovskites, has emerged as a scalable and industry-compatible route for textured tandem photovoltaics. However, this process is often hindered by reaction-limited phase formation, particularly when compact, non-porous, and highly crystalline inorganic layers formed by thermal evaporation restrict subsequent conversion, resulting in incomplete reaction and pronounced depth-dependent heterogeneity. In this study, we introduce a strategy to regulate the inorganic precursor layer by incorporating localized heterogeneous nucleation sites. Sparsely distributed hydrophilic metal oxide species serve as effective nucleation centers during vapor deposition, enabling effective control over film morphology and crystal orientation from the early stages of growth. This tailored inorganic framework facilitates the subsequent incorporation of organic halides, alleviating reaction limitations and suppressing residual unreacted precursors. Consequently, the perovskite films exhibit improved stoichiometric uniformity and enhanced optoelectronic quality, enabling wide-bandgap perovskite solar cells with markedly improved performance and operational stability. This work provides important mechanistic insight into crystal growth engineering of vapor-deposited perovskite thin films.

nucleation↗
DOE OSTI2020

Highly Efficient and Stable Perovskite Solar Cells Enabled by Low‐Cost Industrial Organic Pigment Coating

Abstract Surface passivation of perovskite solar cells (PSCs) using a low‐cost industrial organic pigment quinacridone (QA) is presented. The procedure involves solution processing a soluble derivative of QA, N , N ‐bis(tert‐butyloxycarbonyl)‐quinacridone (TBOC‐QA), followed by thermal annealing to convert TBOC‐QA into insoluble QA. With halide perovskite thin films coated by QA, PSCs based on methylammonium lead iodide (MAPbI 3 ) showed significantly improved performance with remarkable stability. A PCE of 21.1 % was achieved, which is much higher than 18.9 % recorded for the unmodified devices. The QA coating with exceptional insolubility and hydrophobicity also led to greatly enhanced contact angle from 35.6° for the pristine MAPbI 3 thin films to 77.2° for QA coated MAPbI 3 thin films. The stability of QA passivated MAPbI 3 perovskite thin films and PSCs were significantly enhanced, retaining about 90 % of the initial efficiencies after more than 1000 hours storage under ambient conditions.

He, Qingquan↗
DOE OSTI2023

Direct Insertion Polymerization of Ionic Monomers: Rapid Production of Anion Exchange Membranes

Abstract The limited number of methods to directly polymerize ionic monomers currently hinders rapid diversification and production of ionic polymeric materials, namely anion exchange membranes (AEMs) which are essential components in emerging alkaline fuel cell and electrolyzer technologies. Herein, we report a direct coordination‐insertion polymerization of cationic monomers, providing the first direct synthesis of aliphatic polymers with high ion incorporations and allowing facile access to a broad range of materials. We demonstrate the utility of this method by rapidly generating a library of solution processable ionic polymers for use as AEMs. We investigate these materials to study the influence of cation identity on hydroxide conductivity and stability. We found that AEMs with piperidinium cations exhibited the highest performance, with high alkaline stability, hydroxide conductivity of 87 mS cm −1 at 80 °C, and a peak power density of 730 mW cm −2 when integrated into a fuel cell device.

Hsu, Jesse H.↗
DOE OSTI2020

Highly Efficient and Stable Perovskite Solar Cells Enabled by Low‐Cost Industrial Organic Pigment Coating

Abstract Surface passivation of perovskite solar cells (PSCs) using a low‐cost industrial organic pigment quinacridone (QA) is presented. The procedure involves solution processing a soluble derivative of QA, N , N ‐bis(tert‐butyloxycarbonyl)‐quinacridone (TBOC‐QA), followed by thermal annealing to convert TBOC‐QA into insoluble QA. With halide perovskite thin films coated by QA, PSCs based on methylammonium lead iodide (MAPbI 3 ) showed significantly improved performance with remarkable stability. A PCE of 21.1 % was achieved, which is much higher than 18.9 % recorded for the unmodified devices. The QA coating with exceptional insolubility and hydrophobicity also led to greatly enhanced contact angle from 35.6° for the pristine MAPbI 3 thin films to 77.2° for QA coated MAPbI 3 thin films. The stability of QA passivated MAPbI 3 perovskite thin films and PSCs were significantly enhanced, retaining about 90 % of the initial efficiencies after more than 1000 hours storage under ambient conditions.

He, Qingquan↗
DOE OSTI2023

Direct Insertion Polymerization of Ionic Monomers: Rapid Production of Anion Exchange Membranes

The limited number of methods to directly polymerize ionic monomers currently hinders rapid diversification and production of ionic polymeric materials, namely anion exchange membranes (AEMs) which are essential components in emerging alkaline fuel cell and electrolyzer technologies. Herein, we report a direct coordination-insertion polymerization of cationic monomers, providing the first direct synthesis of aliphatic polymers with high ion incorporations and allowing facile access to a broad range of materials. We demonstrate the utility of this method by rapidly generating a library of solution processable ionic polymers for use as AEMs. We investigate these materials to study the influence of cation identity on hydroxide conductivity and stability. Furthermore, we found that AEMs with piperidinium cations exhibited the highest performance, with high alkaline stability, hydroxide conductivity of 87 mS cm –1 at 80 °C, and a peak power density of 730 mW cm –2 when integrated into a fuel cell device.

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

Nitrogen–Rich Conjugated Macrocycles: Synthesis, Conductivity, and Application in Electrochemical CO 2 Capture

Here we report a series of nitrogen-rich conjugated macrocycles that mimic the structure and function of semiconducting 2D metal–organic and covalent organic frameworks while providing greater solution processability and surface tunability. Using a new tetraaminotriphenylene building block that is compatible with both coordination chemistry and dynamic covalent chemistry reactions, we have synthesized two distinct macrocyclic cores containing Ni–N and phenazine-based linkages, respectively. The fully conjugated macrocycle cores support strong interlayer stacking and accessible nanochannels. For the metal–organic macrocycles, good out-of-plane charge transport is preserved, with pressed pellet conductivities of 10 –3 S/cm for the nickel variants. Lastly, using electrochemically mediated CO2 capture as an example, we illustrate how colloidal phenazine-based organic macrocycles improve electrical contact and active site electrochemical accessibility relative to bulk covalent organic framework powders. Together, these results highlight how simple macrocycles can enable new synthetic directions as well as new applications by combining the properties of crystalline porous frameworks, the processability of nanomaterials, and the precision of molecular synthesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗