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At least 19 records

Room temperature slot-die coated perovskite layer modified with sulfonyl-γ-AApeptide for high performance perovskite solar devices

Perovskite solar cells (PSCs) exhibited remarkable progress for small aperture area cells, however, the performance of its counterpart, large aperture area cells, lags due to non-uniform and defective perovskite layers. Here, we fabricate reproducible large area homogeneous perovskite films at room temperature and without controlling humidity (up to 40 % RH) with a slot die coater on a c-TiO 2 layer deposited using a large area chemical bath. A new artificial peptide – sulfonyl-γ-AApeptide (F-GLU-S) was employed to modify the slot-die coated perovskite surface, grain boundaries and electronic defects. The multi-functional F-GLU-S with carbonyl, carboxyl, sulfonyl, benzene, and chloro groups was capable of strongly interacting with the perovskite layer and repairing the uncoordinated Pb 2+ ions and halide vacancies. As a result, both the electron and hole densities of defects were significantly suppressed; consequently, the non-radiative recombination was effectively suppressed for the modified device which can be explicitly seen in the device performance where both V oc and FF of the modified device improved considerably. Therefore, F-GLU-S modified slot-die coated MAPbI 3 – based devices demonstrated outstanding performance of 21.44 % PCE with a V oc of 1.13 V, J sc of 24.64 cm –2 , and FF 76.99 %. Furthermore, F-GLU-S passivation impeded the infiltration of moisture and oxygen due to its hydrophobic nature and defect repair potential. As a result, the modified device retained above 92 % of its original PCE after 720 h in air (room temperature and 40–60 % RH).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Catalyst layer formulations for slot-die coating of PEM fuel cell electrodes

The series of electrodes were fabricated by the scalable and manufacturable slot-die coating method for proton exchange membrane fuel cell (PEMFC) application. The inks with different amounts of solids were studied by rheological methods in order to establish a coating window with minimum manufacturing defects. The obtained electrodes were characterized by SEM, AFM, and optical microscopy, which showed that they were uniform and homogeneous with minimum defects. The electrochemical evaluation of the manufactured gas diffusion electrodes (GDE) showed that the main characteristics of the electrodes, like electrochemical surface area, proton resistivity, and double layer capacitance, were found to be close for all samples confirming the reproducibility of the slot-die process. Additionally, we studied the effects of membrane thickness on the performance of the GDE membrane electrode assemblies and determined that a decrease in membrane thickness favored the performance. Furthermore, the obtained results clearly demonstrated the applicability and feasibility of the approach for the Manufacturing of catalyst layers for the fuel cell application with potential for future mass production.

08 HYDROGEN↗

Rapid scalable fabrication of roll-to-roll slot-die coated flexible perovskite solar cells using intense pulse light annealing

Perovskite solar cells have achieved high efficiencies at the lab scale using batch processes that often may not be scalable. Processes that can be integrated into a continuous manufacturing platform, such as roll-to-roll, where several processes can be carried out sequentially are necessary to develop a new cost-competitive solar technology. In this work, intense pulsed light thermal post-processing is coupled with scalable slot-die coating and air knife evaporation in a high-speed roll-to-roll process of up to 2 m min –1 . The optimization of IPL energy parameters, web speeds, solution flow rates, and concentration of precursor inks yielded a champion power conversion efficiency of 11.24% for a 1 cm 2 roll-to-roll coated device. The overall processing time for a single layer in this process is reduced from minutes to seconds and the overall footprint of the manufacturing process is decreased. Furthermore, this demonstrates the promising capabilities for intensed pulsed light to reduce manufacturing costs and paves a roadmap for scalable and efficient PSCs on a roll-to-roll platform.

14 SOLAR ENERGY↗

Scalable slot-die coating of phyllosilicate membranes for selective ion separations

Abstract Two-dimensional (2D) materials have recently drawn attention as candidate materials for molecular-scale membrane separations due to their tunable nanoscale interlayer properties. Phyllosilicates, a broad class of naturally abundant 2D clay minerals, offer significant advantages over synthetic 2D materials, including low cost, stability, and environmental compatibility. While these properties make phyllosilicates attractive for industrial-scale nanofiltration applications, phyllosilicate-based membranes have, to date, only been fabricated at the lab scale via vacuum filtration. Scalable fabrication methods are essential to advance the technical maturity of phyllosilicate membranes and bring these promising materials closer to large-scale adoption. Herein, we have successfully scaled up phyllosilicate (vermiculite) membrane fabrication via slot-die coating and roll-to-roll coating of an ethylenediamine–vermiculite (EDAVM) mixture onto nylon. The coated membranes are 1–2 μm $ \unicode{x03BC} \mathrm{m} $ mu m in thickness and exhibit similar structure and performance to vacuum-filtered EDAVM membranes. The membranes also show selectivity for monovalent ions over multivalent ions in binary salt mixtures. This work represents a major step toward scaling up phyllosilicate membranes for industrial ion separation applications such as resource recovery from water.

Booth, Austin [Princeton University]↗

Asymmetric side-chain engineering in semiconducting polymers: a platform for greener processing and post-functionalization of organic electronics

Organic semiconducting polymers are a powerful platform for the design of next-generation technologies due to their excellent optoelectronic properties and solution processability, allowing access to low-cost and scalable manufacturing techniques such as spin-coating, slot-die coating and roll-to-roll printing. However, their extended π-conjugation results in low solubility, requiring the use of toxic halogenated solvents to generate thin films and devices. Furthermore, accessible post-functionalization of semiconductors toward the development of multifunctional devices and sensors remains a challenge due to limited solid-state chemistry for alkyl side chains. In this work, an asymmetric side-chain engineering approach was used to introduce terminal hydroxyl moieties alongside traditional solubilizing branched alkyl chains into an isoindigo-based polymer. The hydroxyl moieties led to significantly improved processability in alcohol-based solvents without sacrificing electronic performance in thin film organic field-effect transistors. Solid state morphologies of the thin films processed from both alcohol-based and traditional halogenated solvents were further characterized using atomic force microscopy and grazing incidence wide angle X-ray scattering. Additionally, Cryo-EM was utilized in order to characterize the role of asymmetric side-chain functionality in solution state aggregation. The versatility of this design was further probed using fluorescein isothiocyanate to directly functionalize the asymmetric polymer in thin film. Furthermore, this facile solid-state post-functionalization further demonstrates asymmetric side-chain engineering to be a viable approach toward the development of sustainably manufactured multifunctional electronics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Silver Nanowire-Indium Zinc Oxide Composite Flexible Transparent Conducting Electrodes Made by Spin- coating and Photonic Curing

Realizing high-throughput, low-cost perovskite solar cell (PSC) manufacturing is highly sought-after in photovoltaic (PV) research in recent years. To fully achieve roll-to-roll (R2R) manufacturing of PSCs, it is important to consider the flexible transparent electrode (TE). PET/ITO is a commonly used substrate for making flexible PSCs. When optimizing transparent conducting materials, there is a tradeoff between sheet resistance (Rsh) and optical transparency. Because commercial PET/ITO substrates are made with slow (~1 m/min) vacuum deposition processes, they tend to be expensive. Therefore, it would be advantageous to develop a high-throughput, R2R compatible, solution-deposition approach for fabricating the TE on PET substrates. While various solution-deposition processes, such as blade coating or slot-die coating, can achieve the desired web speed of > 10 m/min, there is still a need to improve the post-deposition annealing step. One promising post-deposition processing technique is intense-pulsed-light processing, also known as photonic curing. Photonic curing delivers short (0.01 – 100 ms) pulses of broadband (200 – 1500 nm) light from a xenon flash lamp to the samples. Any materials in the sample stack that absorb light will convert the impinging light pulse into heat within the sample, which drives changes in the sample (calcination, phase change, crystallization, etc.). Photonic curing has three main advantages over thermal annealing: 1. Faster processing speed (milliseconds or seconds). 2. Compatibility with plastic substrates. 3. Smaller physical footprint and less wasted energy. Since the light pulses are on for a short time, the intensity can be high while the total energy delivered to the sample is low, minimizing damages to the plastic substrates. In this work, a hybrid TE material is fabricated on PET substrates using photonic curing. The hybrid TE material contains a layer of silver nanowires (AgNWs) and a layer of metal-oxide (InOx, ITO, IZO, etc.). The AgNWs increase the light absorbed by the film during the photonic curing process, which leads to higher processing temperatures, possibly improving the conversion of the metal-oxide layer. The AgNWs also enhance the electrical conductivity of the final TE layer after photonic curing. A AgNW and metal-oxide bilayer is formed by spin coating each solution onto the PET substrate sequentially followed by a single photonic curing process. We use average optical transmittance (Tavg) from 400 to 700 nm and average Rsh to evaluate the TE performance. The following photonic curing parameters are varied to optimize Tavg (maximize) and Rsh (minimize): Pulse voltage, pulse envelope, number of micro-pulses, duty cycle, number of pulses, and pulse repetition rate. Preliminarily, we also observe a significant impact on the TE properties by the volume of AgNW deposited during the spin coating deposition step. Using dispense volumes of 80 µL and 20 µL, we achieve samples with Tavg = 73%, Rsh = 19 Ω/sq, and roughness = 9 nm, and Tavg = 83%, Rsh = 58 Ω/sq, and roughness = 5.6 nm, respectively, after photonic curing.

14 SOLAR ENERGY↗

Kinetic processes of phase separation and aggregation behaviors in slot-die processed high efficiency Y6-based organic solar cells

Morphological optimization has proved to be one crucial factor contributing to the 19% efficiency of Y6-based organic solar cells (OSCs). Although the relationship between component miscibility and film morphology has been established, it has not been clarified how the film formation processes proceed, especially for methods compatible with large-area fabrication, i.e. slot-die coating, which restricts the further optimization of the morphology. Herein, we comprehensively investigate the effect of miscibility and the film-formation kinetic process on film morphology during processing with different solvents. A highest power conversion efficiency (PCE) of 17.38% can be obtained in a D18:Y6 device processed with slot-die coating in an open-air environment. However, due to their relatively poor miscibility, incorporating a trace amount of chlorobenzene (CB) into CF can sufficiently promote Y6 aggregation, leading to increased phase separation and thus the average PCE drops to 15.16%. In contrast, a PM6:Y6 blend shows insensitive changes in the kinetic process as well as the final morphology, and thus in the comparable PCEs when cast with different solvents, which is ascribed to their relatively good miscibility. As a result, this work provides scientific guidelines for device optimization by combining the intermediate gap from miscibility to kinetic process and their impact on final morphology.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Slot-die-coating operability windows for polymer electrolyte membrane fuel cell cathode catalyst layers

Roll-to-roll (R2R) slot-die coating of polymer electrolyte membrane fuel cell (PEMFC) catalyst layers represents a scalable deposition method for producing 10–20 m 2 ·min -1 of catalyst-coated gas diffusion layers (GDLs). This high-throughput production technique will help lower the cost of PEMFC catalyst layers. The uniformity of the wet layer applied by slot die deposition is affected by process parameters such as substrate speed, vacuum pressure applied at the upstream meniscus, gap between the slot die lips and substrate, ink rheology, and other ink and substrate properties. The set of conditions for producing a defect-free coating with a dilute ink typically requires little to no upstream vacuum pressure, so suitable operating conditions can be found easily through trial and error and operator intuition. However, the higher viscosity of more concentrated inks dramatically shifts the range of settings that result in a homogeneous coating to higher vacuum levels, which are harder to find through hit or miss. A predictive model showing the range of operable conditions decreases material wastage inherent in experimentally searching for suitable parameters. In this study, the defect-free coating parameter window is explored experimentally and theoretically for two concentrations of PEFC cathode inks. Both a full capillary hydrodynamic model and a computationally cheaper viscocapillary model successfully predict the experimentally determined coating window within the experimental and model uncertainty limits for inks with 5.3 wt% and 12.0 wt% solids ink while maintaining the 0.1 mg Pt ·cm -2 Pt areal loading target. Here, this paper demonstrates a viable pathway for meeting the $30/kW net ultimate cost target of the United States Department of Energy (U.S. DOE) Hydrogen Fuel Cells Technologies Office (HFTO). The concentrated ink lowers the thermal energy and capital expenditure (CapEx) budget of the coating process by decreasing the amount of time, energy, and floorspace required for drying the coating.

25 ENERGY STORAGE↗

Manipulating Organic Semiconductor Morphology with Visible Light

A method is presented to manipulate the final morphology of roll-to-roll slot-die coated poly(3-hexylthiophene) (P3HT) by optically exciting the p-type polymer in solution while coating. These results provide a comprehensive picture of the entire knowledge chain, from demonstrating how to apply the authors’ method to a fundamental understanding of the changes in morphology and physical properties induced by exciting P3HT while coating. By combining results from density functional theory and molecular dynamics simulations with a variety of X-ray experiments, absorption spectroscopy, and THz spectroscopy, the relationship between morphology and physical properties of the thin film is demonstrated. Specifically, in P3HT films excited with light during deposition, changes in crystallinity and texture with more face-on orientation and increased out-of-plane charge mobility are observed.

36 MATERIALS SCIENCE↗

Roll-to-roll slot die coating method to create interleaving multi-layered films with chemical slurry coatings

An improved method for manufacturing a continuous self-healing barrier film is provided. The method includes slot-die coating opposing sides of a separator substrate with a curing agent slurry and a curable resin slurry using a single-sided coating line or a tandem coating line. The method also includes sequentially interleaving inner and outer protective layers via a continuous roll-to-roll process to create a multi-layered barrier film. The barrier film can optionally be formed into a barrier envelope, and an insulating core material can be inserted into the barrier envelope to define an enclosure. Evacuating and sealing the enclosure along a perimeter of the barrier envelop forms a self-healing vacuum insulation panel with excellent properties for use as a building material and in refrigeration systems, for example. The barrier film can alternatively be used in the manufacture of tires, roofing, cargo containers, food packaging, and pharmaceutical packaging, for example.

Biswas, Kaushik↗

Comprehensive evaluation of commercially scalable atomic-layer-deposited alumina coating impact on full cell battery performance across varied test conditions

Atomic Layer Deposition (ALD) has emerged as a strategic enhancement method for lithium-ion battery (LIB) materials offering potential benefits and durability benefits for industrial battery production. However, the translation from laboratory achievements to commercial-scale applications has been limited. Here, this study aims to bridge this gap by comprehensively evaluating the effects of commercially scalable Al 2 O 3 ALD coatings using full pouch cell performance as a means to assess the ALD impact. We utilized large-scale slot-die coating techniques to ensure consistent electrode quality and tested four configurations of pouch cells to analyze the individual effects of ALD coating on anode and cathode electroactive materials. Our extensive testing matrix included long-term cycling, fast discharge, fast charge, leakage current, and high voltage tests. While at lower C-rates (<~1C), the influence of Al 2 O 3 coatings on cell performance is not significant. Fast charging conditions reveal that the anode ALD coating significantly enhances performance via a passivating effect, while on the cathode, it is detrimental, potentially due to increased resistance of the thin interfacial layer formed during the ALD processing. Leakage current and high-voltage tests show that the application of ALD coatings on either anode or cathode effectively minimizes side reactions at the electrode-electrolyte interface. Additionally, ALD coatings significantly mitigate concentrated and localized lithium plating on the anodes. These insights provide a valuable understanding of the potential of ALD technologies in LIB manufacturing to tailor cell performance, paving the way for safer, more efficient, and cost-effective battery solutions.

25 ENERGY STORAGE↗

Roll to Roll (R2R) Manufacturing of Electrolysis Electrodes for Low Cost Hydrogen Production: Cooperative Research and Development Final Report, CRADA Number CRD-18-00780

NREL, Argonne National Laboratory (ANL) and Oak Ridge National Laboratory (ORNL), which are also referred to collectively herein as the "Contractors" will perform electrode ink development and characterization, focusing on 1) inks with appropriate properties for R2R (gravure and slot-die) coating onto PFSA membrane and 2) catalysts suitable for electrolysis. Participant will develop acceptance criteria and characterization methods for direct coating on the membrane. The purpose of this project is to show feasibility for cost reduction of the electrode through increased throughput and improved material utilization. Successful completion of this project will result in more affordable hydrogen production via proton exchange membrane (PEM) electrolysis by substantially reducing the anode precious metal content and catalyst-coated membrane processing costs. Assists laboratory in achieving programmatic scope, adds new capability to the laboratory's core competencies. This project uses and enhances the laboratory's core competencies, and enhances U.S. competitiveness by utilizing DOE developed intellectual property and/or capabilities. This project will benefit the Fuel Cell subprogram within the EERE Fuel Cell Technologies Office (FCTO) by actively developing materials, formulations, components, and processes for PEM electrolyzer stacks for overcoming critical technical barriers to widespread hydrogen production for zero-emission transportation applications. Through this JWS, NREL, ANL and ORNL are assisting a key domestic industry partner, Proton Energy Systems, Inc., in the area of low-cost electrolyzer electrode formulation and coating technology. After completion of this project, NREL, ANL and ORNL will be able to verify whether the direct deposit coating processes investigated are suitable for producing CCMs for PEM electrolyzers, which is of great interest and benefit to the DOE EERE Fuel Cell Technologies Office (FCTO) and H2@Scale missions.

08 HYDROGEN↗

Roll-to-Roll Manufacturing of Solid Oxide Fuel Cells

The overall goal of this project is to develop a high-volume electrode electrolyte assembly (EEA) production capability to significantly increase throughput of solid oxide fuel cell (SOFC) manufacturing and reduce the cost while maintaining the same level of performance. Specifically, four approaches will be adopted: 1) optimization of the lamination process and correlation of the EEA properties and performance with the lamination conditions; 2) scale up of the lamination process and demonstration of >10 ft of EEA; 3) further increase of the EEA throughput via slot-die coating and demonstration of > 5 m/min in coating the thick anode layer; and 4) minimization of the anode thickness to reduce material cost.

30 DIRECT ENERGY CONVERSION↗

Precursor Engineering of All-Inorganic Perovskite Absorber and Rapid Photonic Annealing for Large-Area Highly Stable Perovskite Solar Modules

Currently the all-inorganic perovskites were prepared by toxic dimethylformamide (DMF) as a main solvent, and small-area PSCs were prepared by a simple spin-coating method followed by lengthy thermal annealing. All these issues limited the commercialization of these PSCs. Therefore, it is necessary to develop an eco-friendly all-inorganic perovskite ink that can be coated over large areas at low temperatures followed by rapid annealing for the scale-up manufacturing with high compatibility to the industrial scale sheet-to-sheet or roll-to-roll processes.

14 SOLAR ENERGY↗

Eco–Friendly Solvent Engineered CsPbI 2.77 Br 0.23 Ink for Large–Area and Scalable High Performance Perovskite Solar Cells

The performance of large-area perovskite solar cells (PSCs) has been assessed for typical compositions, such as methylammonium lead iodide (MAPbI 3 ), using a blade coater, slot-die coater, solution shearing, ink-jet printing, and thermal evaporation. However, the fabrication of large-area all-inorganic perovskite films is not well developed. This study develops, for the first time, an eco-friendly solvent engineered all-inorganic perovskite ink of dimethyl sulfoxide (DMSO) as a main solvent with the addition of acetonitrile (ACN), 2-methoxyethanol (2-ME), or a mixture of ACN and 2-ME to fabricate large-area CsPbI 2.77 Br 0.23 films with slot-die coater at low temperatures (40–50 °C). The perovskite phase, morphology, defect density, and optoelectrical properties of prepared with different solvent ratios are thoroughly examined and they are correlated with their respective colloidal size distribution and solar cell performance. Here, the optimized slot-die-coated CsPbI 2.77 Br 0.23 perovskite film, which is prepared from the eco-friendly binary solvents dimethyl sulfoxide:acetonitrile (0.8:0.2 v/v), demonstrates an impressive power conversion efficiency (PCE) of 19.05%. Moreover, the device maintains ≈91% of its original PCE after 1 month at 20% relative humidity in the dark. It is believed that this study will accelerate the reliable manufacturing of perovskite devices.

binary and ternary solvent↗

Impact of Salt Chemistry and Interlayer Architecture on Solid Electrolyte Interphase Composition and Performance

Reversible lithium metal anodes require interphases that are chemically stable, mechanically robust, and compatible with scalable processing. Here, we use slot-die-coated, salt-rich PEO interlayers to design SEI nanolayers on Cu current collectors and isolate how salt anion chemistry controls interphase composition and lithium plating/stripping behavior in architectures relevant to Li plating and anode-free cells. Mesoscale modeling shows that dendrite initiation at SEI defects is governed by a tradeoff among interphase thickness, ionic conductivity, and stiffness through defect-driven current focusing, motivating controlled formation from thin precursor layers. Using UHV-transferred XPS and ToF-SIMS depth profiling after controlled Li deposition, we find that fluorinated sulfonylimide salts (LiTFSI, LiFSI) form mixed inorganic/organic interphases containing LiF and PEO-derived alkoxides, with LiFSI producing a more LiF-dominant Li-facing surface than LiTFSI under identical conditions. In contrast, LiNO 3 -containing interlayers yield a comparatively thick nitrate-derived interphase that reduces upon Li contact to an N-rich inorganic layer (Li–N/N 3− , LiN x O y ). In Cu| |Li cells, these designed interlayers reduce interfacial resistance and improve Coulombic efficiency (CE) and critical current density (CCD) relative to uncoated controls, with LiFSI- and LiNO 3 -based interlayers providing the highest CE/CCD. Overall, the results demonstrate a manufacturing-relevant approach to engineer SEI nanolayers by salt chemistry, providing pathways to improve reversible lithium metal anodes while reducing reliance on LiTFSI.

anion chemistry↗

Lithium-Ion Batteries with Safer Current Collectors

The US Department of Energy’s Oak Ridge National Laboratory and Soteria Battery Innovation Group collaborated to develop a metallized polymer film as a current collector for lithium-ion batteries and design slit patterns for electrodes to improve battery safety. The metallized polymer film serves as a fuse that will break under high temperature resulting from a short circuit. Consequently, the short circuit will be broken and the heat generated from the short circuit will be alleviated to avoid thermal runaway. The electrodes with slit patterns are expected to be broken into small segments upon mechanical impact, which can isolate the damaged electrodes from the rest. Thus, the heat generation associated with the mechanical impact will be reduced, along with the likelihood of thermal runaway. This effort aimed to improve lithium-ion battery safety by replacing traditional metal foils with metallized polymer films as current collector and introducing slit patterns to battery electrodes. The metallized polymer films were polyethylene terephthalate with a thin metal (aluminum for cathodes and copper for anodes) coating on both sides. Slit patterns with various geometries and dimensions were designed via simulation. Temperature distribution on cells with electrodes with and without slit patterns was also simulated via nemerical modeling. Electrodes on traditional metal foils and metallized polymer films were coated via a pilot-scale slot-die coater at the US Department of Energy Battery Manufacturing Facility at Oak Ridge National Laboratory. The electrodes were calendered to 35% porosity and punched out with and without slit patterns. Pouch cells were assembed with the electrodes inside a dry room for electrochemical and safety testing. Electrodes coated on metallized polymer films exhibited comparable electrochemical performance to their counterparts coated on traditional metal foils. They also showed improved safety in nail penetration and indentation tests.

25 ENERGY STORAGE↗