Search NASA⌕ Search

SEARCH · Search NASA

Results for “solvent evaporation”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Why are Lead Iodide‐Based Perovskite Precursor Inks Yellow?

A challenge faced by metal halide perovskite (MHP) photovoltaics is scaling up solution deposition processes to realize rapid and inexpensive manufacturing. The challenge lies in completely understanding and controlling solution speciation, nucleation, and self-assembly of iodoplumbate complexes during solvent evaporation as the liquid transforms into gels and solids. An accurate description of solution species, at all points in the transformation, is a prerequisite to design robust and reliable processes. Here, in this study, the common assumption that initial monoplumbate solution species typically invoked (e.g., [PbI 6 ] 4− ) are certainly not the origin of optical absorbance at >400 nm wavelengths is disproved, as are many large particles of common “intermediate” iodoplumbate phases with face- or edge-sharing connectivity. Instead, a new perspective is offered, involving (partially) corner-sharing iodo(poly)plumbates (>1 Pb 2+ per complex) that experience highly dynamic chemical environments. It is outlined how the MHP field would benefit by elucidating these phenomena. Future work is required to determine the size and kinetic behavior of polyplumbate species, and contextualize these findings in relation to broader trends in materials chemistry beyond MHPs. Ultimately, a complete explanation for the solution speciation, optical absorbance signatures, and the color of MHP precursor inks remains an open challenge to the community.

14 SOLAR ENERGY↗
DOE OSTI2025

Open-air spray deposition of PCBM/BCP electron transport layer for inverted perovskite solar cells

A [6,6]-phenyl C61 butyric acid methyl ester (PCBM) and bathocuproine (BCP) electron transport layer (ETL) is spray deposited in open air directly on top of a perovskite at linear speeds of 9 m/min. The PCBM precursor ink contains a binary mixture of 1:1 chlorobenzene:chloroform, which optimizes spray wettability on the perovskite surface and allows quick solvent evaporation. A near-infrared heating module additionally provides a flash cure (<5 s) for the formation of smooth, large-area PCBM films (∼20 cm 2 ). A BCP solution in isopropanol is subsequently sprayed to form an ultrathin (<5 nm) film and characterized with a suite of high-resolution metrologies. The spray-deposition processing and near-infrared treatment do not damage the underlying perovskite. Inverted architecture devices containing the sprayed ETL achieve a champion efficiency of 20.3% and demonstrate stable performance without additional interlayers or surface treatments. Here, the technoeconomic cost of the open-air spray process is compared against traditional vacuum-based evaporation, resulting in a decrease in manufacturing costs by 26%.

14 SOLAR ENERGY↗
DOE OSTI2023

Temperature-Controlled Reversible Formation and Phase Transformation of 3D Nanocrystal Superlattices Through In Situ Small-Angle X-ray Scattering

For decades, the spontaneous organization of nanocrystals into superlattices has captivated the scientific community. However, achieving direct control over the formation of the superlattice and its phase transformations has proven to be a grand challenge, often resulting in the generation of multiple symmetries under the same experimental conditions. Here, we achieve direct control over the formation of the superlattice and its phase transformations by modulating the thermal energy of a nanocrystal dispersion without relying on solvent evaporation. In this study, we follow the temperature-dependent dynamics of the self-assembly process using synchrotron-based small-angle X-ray scattering. When cooled below –24.5 °C, lead sulfide nanocrystals form micrometer-sized three-dimensional phase-pure body-centered cubic superlattices. When cooled below –35.1 °C, these superlattices undergo a collective diffusionless phase transformation that yields denser body-centered tetragonal phases. These structural changes can be reversed by increasing the temperature of the dispersion and may lead to the direct modulation of the optical properties of these artificial solids.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Solvent Isotherms and Structural Transitions in Nanoparticle Superlattice Assembly

Here, we introduce a Molecular Theory for Compressible Fluids (MOLT-CF) that enables us to compute free energies and other thermodynamic functions for nanoparticle superlattices with any solvent content, including the dry limit. Quantitative agreement is observed between MOLT-CF and united-atom molecular dynamics simulations performed to assess the reliability and precision of the theory. Among other predictions, MOLT-CF shows that the amount of solvent within the superlattice decreases approximately linearly with its vapor pressure and that in the late stages of drying, solvent-filled voids form at lattice interstitials. Applied to single-component superlattices, MOLT-CF predicts fcc-to-bcc Bain transitions for decreasing vapor pressure and for increasing ligand length, both in agreement with experimental results. We explore the stability of other single-component phases and show that the C14 Frank-Kasper phase, which has been reported in experiments, is not a global free-energy minimum. Implications for precise assembly and prediction of multicomponent nanoparticle systems are discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

In-Operando Study of Shape Retention and Microstructure Development in a Hydrolyzing Sol–Gel Ink during 3D-Printing

3D printing of amorphous and crystalline ceramics is of paramount importance for the fabrication of a wide range of devices with applications across different technology fields. Printed ceramics are remarkably enabled by the sol-gel synthesis method in conjunction with continuous filament direct ink writing. During printing, multiple processes contribute to the evolution of inks including shape retention, chemical conversion, solidification, and microstructure formation. Traditionally, depending on the ink composition and printing environment, several mechanisms have been associated with the shape retention and solidification of 3D printed structures: gelation, rapid solvent evaporation, energy-driven phase transformation, and chemical-driven phase transformation. Understanding the fundamental differences between these mechanisms becomes key since they strongly influence the spatiotemporal evolution of the materials, as the out-of-equilibrium processes inherent to the extrusion, relaxation, and solidification of printed materials have significant effects on the materials properties. Herein, we investigate the shape retention mechanism and the hydrolysis-induced material conversion and microstructure formation during the 3D printing of a water reactive sol-gel ink that transforms into titanium dioxide-based ceramic. This study aims at identifying characteristic mechanisms associated with the material transformation, establishing connections between the microstructure development and the timescales associated with solidification under operando 3D-printing conditions. The investigation of this material's out-of-equilibrium pathways under processing conditions is enabled by time-resolved coherent X-ray scattering, providing simultaneous access to temporospatially resolved microstructural and dynamics information. Furthermore, we explore X-ray speckle tracking as a tool to resolve deformations of the microstructure in a printed filament associated with the deposition of consecutive filaments. Through this work, we aim at providing a fundamental understanding of the relationships behind these transformative processes in 3D printing and their timescales as the basis for achieving unprecedented control over printed materials microstructure.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Effects of Ink Formulation on Construction of Catalyst Layers for High-Performance Polymer Electrolyte Membrane Fuel Cells

Rational design of catalyst layers in a membrane electrode assembly (MEA) is crucial for achieving high-performance polymer electrolyte membrane fuel cells. Establishing a clear understanding of the property (catalyst ink)–structure (catalyst layer)–performance (MEA) relationship lays the foundation for this rational design. Here, a synergistic approach was taken to correlate the ink formulation, the microstructure of catalyst layers, and the resulting MEA performance to establish such a property–structure–performance relationship. The solvent composition (n-PA/H 2 O mixtures) demonstrated a strong influence on the performance of the MEA fabricated with an 830-EW (Aquivion) ionomer, especially polarization losses of cell activation and mass transport. The performance differences were studied in terms of how the solvent composition affects the catalyst/ionomer interface, ionomer network, and pore structure of the resulting catalyst layers. The ionomer aggregates mainly covered the surface of catalyst aggregates acting as oxygen reduction reaction active sites, and the aggregate sizes of the ionomer and catalyst (revealed by ultrasmall angle X-ray scattering and cryo-transmission electron microscopy) were dictated by tuning the solvent composition, which in turn determined the catalyst/ionomer interface (available active sites). In n-PA/H 2 O mixtures with 50~90 wt % H 2 O, the catalyst agglomerates could be effectively broken up into small aggregates, leading to enhanced kinetic activities. The boiling point of the mixed solvents determined the pore structure of ultimate catalyst layers, as evidenced by mercury porosimetry and scanning electron microscopy. For mixed solvents with a higher boiling point, the catalyst–ionomer aggregates in the ink tend to agglomerate during the solvent evaporation process and finally form larger catalyst–ionomer aggregates in the ultimate catalyst layer, resulting in more secondary pores and thus lower mass transport resistance. Both the enlarged catalyst/ionomer interface and appropriate pore structure were achieved with the catalyst layer fabricated from an n-PA/H 2 O mixture with 90 wt % H 2 O, leading to the best MEA performance.

25 ENERGY STORAGE↗
DOE OSTI2020

Phase Diagram and Structure Map of Binary Nanoparticle Superlattices from a Lennard-Jones Model

A first-principles prediction of the binary nanoparticle phase diagram assembled by solvent evaporation has eluded theoretical approaches. In this paper, we show that a binary system interacting through the Lennard-Jones (LJ) potential contains all experimental phases in which nanoparticles are effectively described as quasi hard spheres. We report a phase diagram consisting of 53 equilibrium phases, whose stability is quite insensitive to the microscopic details of the potentials, thus giving rise to some type of universality. Furthermore, we show that binary lattices may be understood as consisting of certain particle clusters, i.e., motifs, that provide a generalization of the four conventional Frank–Kasper polyhedral units. Our results show that metastable phases share the very same motifs as equilibrium phases. Finally, we discuss the connection with packing models, phase diagrams with repulsive potentials, and the prediction of likely experimental superlattices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Mosaic lateral heterostructures in two-dimensional perovskite

Lateral heterostructures are important for exploring exotic physics, developing new devices and achieving device miniaturization. Endo-epitaxial growth occurring in patterned templates presents a promising strategy to realize extensive patterned areas in heterostructures, as recently demonstrated with two-dimensional (2D) covalent materials. However, the conventional lithography and etching processes used to prepare patterned templates are too aggressive for 2D lead halide perovskites, owing to their inherently soft and unstable ionic lattice. Here we create square holes of controllable size within 2D lead halide perovskites, enabling the fabrication of continuous lateral heterostructures over large areas. We demonstrate that the square holes form through spontaneous etching, a process initiated by internal strain and stabilized along the [100]/[010] crystallographic direction. Furthermore, the size of the square holes can be controlled by adjusting the etching time and temperature. Moreover, by incorporating a rapid solvent evaporation growth technique, the edges of the square holes act as templates for epitaxial growth of another type of perovskite, incorporating different halide or metal ions. Finally, we realized a series of mosaic lateral heterostructures that can emit various colours for light-emitting devices. As a result, this synthesis of diverse 2D perovskite mosaic lateral heterostructures provides valuable insights into the structural characteristics of perovskites and offers a versatile material platform for the development of complex integrated emitting devices.

Organic–inorganic nanostructures↗
DOE OSTI2021

Dynamic processes in transient phases during self-assembly of organic semiconductor thin films

Understanding and manipulating crystallization processes has been an important challenge for solution-processed organic thin films, both for fundamental studies and for fabricating thin films with near-intrinsic charge transport properties. We report an in situ X-ray scattering study of the crystallization of 2-decyl-7-phenyl-[1]benzothieno[3,2-b][1]benzothiophene (Ph-BTBT-C 10 ) during its deposition from solution. At temperatures modestly below the smectic-E/crystalline phase boundary, the crystallization goes through a transient liquid crystal state before reaching the final stable crystalline phase. Significant dynamics occur in the first few seconds of the transition, which are observed through fluctuations in the X-ray scattering intensity, and are correlated with the time interval that the transient thin film coexists with the evaporating solvent. The transition to the stable crystalline phase takes minutes or even hours under these conditions, which may be a result of the asymmetry of the molecule. Transient phases are of potential interest for applications, since they can act as a route to self-assembly of organic thin films. However, our observations show that the long-lived monolayer-stacked intermediate state does not act as a template for the bilayer-stacked crystalline phase. Rather, the grain structure is replaced through nucleation, where the nucleation free-energy barrier is related to a potential barrier that prevents molecules to flip their long axis by 180°.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Quantitative probing of the fast particle motion during the solidification of battery electrodes

Synchrotron x-ray tomography represents one of the most powerful imaging techniques that can visualize the three-dimensional microstructural complexity with a high spatial resolution. To date, however, the temporal resolution of this technique has been handicapped by the intrinsic limitations in the data acquisition speed and the lack of a suitable data processing method. The present study aims to fundamentally resolve this challenge by implementing a data analysis method that is based on differentiating discrete tomography reconstruction from a continuous scan reconstruction. With this methodological development, we capture and quantify the particle motion during the solidification of battery electrodes and reveal the statistics of the dynamically evolving motion in the drying process, which has been challenging to resolve. We discover that the particle motion exhibits a strong dependence on its geometric location within a drying electrode. Our results also imply that the final electrode quality can be controlled by balancing the solvent evaporation rate and the particle mobility in the region close to the drying surface.

25 ENERGY STORAGE↗
DOE OSTI2021

Self-organization of nanoparticles and molecules in periodic Liesegang-type structures

Chemical organization in reaction-diffusion systems offers a strategy for the generation of materials with ordered morphologies and structural hierarchy. Periodic structures are formed by either molecules or nanoparticles. On the premise of new directing factors and materials, an emerging frontier is the design of systems in which the precipitation partners are nanoparticles and molecules. We show that solvent evaporation from a suspension of cellulose nanocrystals (CNCs) and L -(+)-tartaric acid [ L -(+)-TA] causes phase separation and precipitation, which, being coupled with a reaction/diffusion, results in rhythmic alternation of CNC-rich and L -(+)-TA–rich rings. The CNC-rich regions have a cholesteric structure, while the L -(+)-TA–rich bands are formed by radially aligned elongated bundles. The moving edge of the pattern propagates with a finite constant velocity, which enables control of periodicity by varying film preparation conditions. This work expands knowledge about self-organizing reaction-diffusion systems and offers a strategy for the design of self-organizing materials.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Pore-Filled PEMs from Poly(Phenylene Sulfonic Acid)s and Electrospun Poly(Phenylene Sulfone) Fiber Mats

A novel, composite, non-PFSA-based fuel cell membrane has been fabricated using a pore filling technique. The membrane consists of a mechanically stabilizing skeleton from an electrospun poly(phenylene sulfone) (PPSU) fiber mat and a thermally crosslinkable poly(phenylene sulfonic acid) (cPPSA) proton conducting ionomer that fills the interfiber voids. cPPSA copolymer was synthesized using Ullmann coupling copolymerization of 4,4-dibromobiphenyl 3,3-disulfonic acid with 1,4-dibromobenzene-2,5-disulfonic, followed by grafting a certain fraction of backbone sulfonic acid groups with biphenyl linker. The PPSU fiber mat was electrospun from NMP/acetone solution. Pore-filling was carried out by pouring a solution of cPPSA in methanol over the mat, followed by heating at 70°C to evaporate solvent. The cPPSA was crosslinked by an additional heating step, in a vacuum oven at 210°C for 5 hours. Here the resultant membrane had excellent proton conductivity, 5 times greater than that of Nafion® 211 in the 40-90% RH range at 80°C.

25 ENERGY STORAGE↗
DOE OSTI2021

Method of making a perovskite layer at high speed

A method of making a perovskite layer includes providing a flexible substrate; providing a perovskite solution comprising an initial amount of solvent and perovskite precursor materials and a total solids concentration between 30 percent and 70 percent by weight of its saturation concentration; depositing the perovskite solution on the flexible substrate; removing a first portion of the solvent from the deposited perovskite solution and increasing the total solids concentration of the perovskite solution to at least 75 percent of its saturation concentration with a first drying step; and removing a second portion of the solvent from the deposited perovskite solution with a second drying step having a higher rate of solvent evaporation that causes saturation and a conversion reaction in the deposited perovskite solution resulting in perovskite crystal formation or formation of a perovskite intermediate phase, wherein the first drying step dwell time is at least 5 times longer than the second drying step dwell time.

Christensen, Scott Kenneth↗
DOE OSTI2020

Evaporation-Induced Vertical Alignment Enabling Directional Ion Transport in a 2D-Nanosheet-Based Battery Electrode

2D nanosheets have been widely explored as electrode materials owing to their extraordinarily high electrochemical activity and fast solid-state diffusion. However, the scalable electrode fabrication based on this type of material usually suffers from severe performance losses due to restricted ion-transport kinetics in a large thickness. Here, a novel strategy based on evaporation-induced assembly to enable directional ion transport via forming vertically aligned nanosheets is reported. The orientational ordering is achieved by a rapid evaporation of mixed solvents during the electrode fabrication process. Compared with conventional drop-cast electrodes, which exhibit a random arrangement of the nanosheets and obvious decrease of rate performance with increasing thickness, the electrode based on the vertically aligned nanosheets is able to retain the original high rate capability even at high mass loadings and electrode thickness. Furthermore, combined electrochemical and structural characterization reveals the electrode composed of orientation-controlled nanosheets to possess lower charge-transfer resistances, leading to more complete phase transformation in the active material.

25 ENERGY STORAGE↗
DOE OSTI2025

Cooperative Role of Mixed Solvent in the Evaporation-Induced Self-Assembly of Polypeptoid Nanocrystals

Peptoids, or polypeptoids, are biomimetic polymers that can self-assemble into nanocrystals for biomedical and biotechnological applications. Polypeptoid nanocrystals can be prepared by evaporation-induced self-assembly, but the roles of solvent components for this process have long been overlooked at the molecular level, leaving a tunable parameter for improving self-assembly protocols. This work utilized molecular dynamics simulations to study the effects of water and the commonly used tetrahydrofuran (THF) on the assembly of nanosheets from molecules of acetylated diblock polypeptoid, poly-(N-decylglycine)-b-poly-(N-2-(2-(2-methoxyethoxy)-ethoxy) ethylglycine), abbreviated as Ac-Ndc10-Nte10. To probe the stages of self-assembly, isolated molecules and preassembled nanofibers/nanosheets were simulated in pure THF, water, and their mixtures, respectively. The assembly energies show that the THF/water mixture has a greater tendency to form nanosheets than pure water. In a THF/water mixture, polypeptoids were found more uncoiled in isolated states, less compact in disordered agglomerates, and with reduced requirement for the Nte block to cover hydrophobic Ndc surfaces in the nanocrystals. Mixed solvent is vital to initiating self-assembly, as THF assists in the opening of coiled polypeptoid molecules, while water provides the thermodynamics to aggregate and ultimately form nanocrystals. To obtain wider nanosheets, it is recommended that some THF be maintained in the aqueous solvent before it becomes exhausted by evaporation. Near the nanosheet surface, the THF concentration is higher than that in bulk solution (3-4 times in 4 M THF/water). The strong adsorption of THF indicates the self-assembly in a de facto mixed solvent. These results are expected to guide the refinement of evaporation-induced self-assembly protocols for polypeptoid nanocrystals.

Luo, Xubo↗
DOE OSTI2021

A Polymer-Assisted Spinodal Decomposition Strategy toward Interconnected Porous Sodium Super Ionic Conductor-Structured Polyanion-Type Materials and Their Application as a High-Power Sodium-Ion Battery Cathode

A general polymer-assisted spinodal decomposition strategy is used to prepare hierarchically porous sodium super ionic conductor (NASICON)-structured polyanion-type materials (e.g., Na 3 V 2 (PO 4 ) 3 , Li 3 V 2 (PO 4 ) 3 , K 3 V 2 (PO 4 ) 3 , Na 4 MnV(PO 4 ) 3 , and Na 2 TiV(PO 4 ) 3 ) in a tetrahydrofuran/ethanol/H 2 O synthesis system. Depending on the boiling point of solvents, the selective evaporation of the solvents induces both macrophase separation via spinodal decomposition and mesophase separation via self-assembly of inorganic precursors and amphiphilic block copolymers, leading to the formation of hierarchically porous structures. We find that the resulting hierarchically porous Na 3 V 2 (PO 4 ) 3 possessing large specific surface area (≈77 m 2 g -1 ) and pore volume (≈0.272 cm 3 g -1 ) shows a high specific capacity of 117.6 mAh g -1 at 0.1 C achieving the theoretical value and a long cycling life with 77% capacity retention over 1000 cycles at 5 C. This method presented here can open a facile avenue to synthesize other hierarchically porous polyanion-type materials.

36 MATERIALS SCIENCE↗