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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 847 records · Page 47
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Performance of Lithium-Ion Batteries with 3D Printed Anodes and Compressible Carbon Structures

Carbon scaffolds have been shown to improve the performance of Li metal anodes in Li-ion batteries by acting as conductive hosts for Li metal plating and stripping. The scaffolds provide a more uniform electric field, and their 3D geometry enables smaller diffusion paths for the Li ions. In this project, several different types of carbon lattices were 3D printed, mechanically tested, and analyzed in coin cells. Planar and 3D printed graphite coatings were evaluated as the baseline, since graphite is a common anode material. The results showed that implementing a 3D graphite lattice into a coin cell improved the Li plating and stripping efficiency compared to the planar coating. However, since graphite can intercalate Li ions, other carbon materials were also explored that should act as better hosts for Li plating/stripping. To improve the compressibility of these non-graphite carbon scaffolds, five different carbon ink formulations were 3D printed in lattice configurations. SEM imaging and compression testing showed that both the final dimensions and the compressibility of the carbon lattices depended on the type of carbon precursors used. The two most suitable compositions were found to be those made with graphene oxide-resorcinol formaldehyde and graphene oxide-ammonium hydroxide. In the future, these formulations will be further refined to increase their mechanical strength, and their performance as scaffold hosts for Li metal anodes will be evaluated in coin cells.

25 ENERGY STORAGE↗
DOE OSTI2020

Controlled Reduction of Graphene Oxide Using Sulfuric Acid

Sulfuric acid under different concentrations and with the addition of SO 3 (fuming sulfuric acid) was studied as a reducing agent for the production of reduced graphene oxide (RGO). Three concentrations of sulfuric acid (1.5, 5, and 12 M), as well as 12 M with 30% SO 3 , were used. The reduction of graphene oxide increased with H 2 SO 4 concentration as observed by Fourier-transformed infrared spectroscopy and X-ray photoelectron spectroscopy. It was observed that GO lost primarily epoxide functional groups from 40.4 to 9.7% and obtaining 69.8% carbon when using 12 M H 2 SO 4 , without leaving sulfur doping. Additionally, the appearance of hexagonal domain structures observed in transmission electron microscopy and analyzed by selected area electron diffraction patterns confirmed the improvement in graphitization. Although the addition of SO 3 in H 2 SO 4 improved the GO reduction with 74% carbon, as measured by XPS, the use of SO 3 introduced sulfur doping of 1.3%. RGO produced with sulfuric acid was compared with a sample obtained via ultraviolet (UV) irradiation, a very common reduction route, by observing that the RGO produced with sulfuric acid had a higher C/O ratio than the material reduced by UV irradiation. This work showed that sulfuric acid can be used as a single-step reducing agent for RGO without sulfur contamination.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Porphene and porphite as porphyrin analogs of graphene and graphite

Two-dimensional materials have unusual properties and promise applications in nanoelectronics, spintronics, photonics, (electro)catalysis, separations, and elsewhere. Most are inorganic and their properties are difficult to tune. Here we report the preparation of Zn porphene, a member of the previously only hypothetical organic metalloporphene family. Similar to graphene, these also are fully conjugated two-dimensional polymers, but are composed of fused metalloporphyrin rings. Zn porphene is synthesized on water surface by two-dimensional oxidative polymerization of a Langmuir layer of Zn porphyrin with K 2 IrCl 6 , reminiscent of known one-dimensional polymerization of pyrroles. It is transferable to other substrates and bridges μm-sized pits. Contrary to previous theoretical predictions of metallic conductivity, it is a p-type semiconductor due to a predicted Peierls distortion of its unit cell from square to rectangular, analogous to the appearance of bond-length alternation in antiaromatic molecules. The observed reversible insertion of various metal ions, possibly carrying a fifth or sixth ligand, promises tunability and even patterning of circuits on an atomic canvas without removing any π centers from conjugation.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Impact of Anode to Cathode Crossover in Lithium‐metal Batteries With High‐Nickel Cathodes

The advancement of high-energy-density lithium-metal batteries (LMBs) is hindered by the chemical instability of both lithium-metal anode and high-nickel layered oxide cathodes. While cathode-to-anode crossover is well-documented, the reverse process of anode-to-cathode crossover remains underexplored. Here, we systematically investigate such crossovers and the degradation pathway in pouch cells with a localized high-concentration electrolyte, comparing NMC622, NMC811, and NMC90 cathodes paired with lithium-metal and graphite anodes. Despite delivering higher initial capacities, LMBs exhibit faster capacity fade under long-term cycling at 45 °C. To isolate cathode-side degradation, galvanostatic electrochemical impedance spectroscopy (GEIS) measurements of cycled cathodes paired with delithiated lithium iron phosphate (LFP) counter electrodes reveal significantly higher charge-transfer resistance in cathodes cycled with lithium-metal. Surface characterization via X-ray photoelectron spectroscopy (XPS) and time-of-flight secondary ion mass spectrometry (ToF-SIMS) reveals greater electrolyte decomposition on cathodes cycled with lithium metal, leading to thicker, more organic-rich cathode–electrolyte interphases (CEIs), consistent with the elevated charge-transfer resistance observed in GEIS measurements. Notably, NMC90 shows the most pronounced CEI thickening, linking higher cathode surface reactivity to greater susceptibility to anode-to-cathode crossover. This work presents compelling evidence of crosstalk degradation originating from lithium-metal anodes and underscores the importance of cross-interface stability for the design of durable LMBs.

25 ENERGY STORAGE↗
NASA NTRS2010

Development and Testing of High Surface Area Iridium Anodes for Molten Oxide Electrolysis

Processing of lunar regolith into oxygen for habitat and propulsion is needed to support future space missions. Direct electrochemical reduction of molten regolith is an attractive method of processing, because no additional chemical reagents are needed. The electrochemical processing of molten oxides requires high surface area, inert anodes. Such electrodes need to be structurally robust at elevated temperatures (1400-1600 C), be resistant to thermal shock, have good electrical conductivity, be resistant to attack by molten oxide (silicate), be electrochemically stable and support high current density. Iridium with its high melting point, good oxidation resistance, superior high temperature strength and ductility is the most promising candidate for anodes in high temperature electrochemical processes. Several innovative concepts for manufacturing such anodes by electrodeposition of iridium from molten salt electrolyte (EL-Form process) were evaluated. Iridium electrodeposition to form of complex shape components and coating was investigated. Iridium coated graphite, porous iridium structure and solid iridium anodes were fabricated. Testing of electroformed iridium anodes shows no visible degradation. The result of development, manufacturing and testing of high surface, inert iridium anodes will be presented.

Shchetkovskiy, Anatoliy↗
NASA NTRS2010

Development and Testing of High Surface Area Iridium Anodes for Molten Oxide Electrolysis

Processing of lunar regolith into oxygen for habitat and propulsion is needed to support future space missions. Direct electrochemical reduction of molten regolith is an attractive method of processing, because no additional chemical reagents are needed. The electrochemical processing of molten oxides requires high surface area, inert anodes. Such electrodes need to be structurally robust at elevated temperatures (1400-1600?C), be resistant to thermal shock, have good electrical conductivity, be resistant to attack by molten oxide (silicate), be electrochemically stable and support high current density. Iridium with its high melting point, good oxidation resistance, superior high temperature strength and ductility is the most promising candidate for anodes in high temperature electrochemical processes. Several innovative concepts for manufacturing such anodes by electrodeposition of iridium from molten salt electrolyte (EL-Form? process) were evaluated. Iridium electrodeposition to form of complex shape components and coating was investigated. Iridium coated graphite, porous iridium structure and solid iridium anodes were fabricated. Testing of electroformed iridium anodes shows no visible degradation. The result of development, manufacturing and testing of high surface, inert iridium anodes will be presented.

Shchetkovskiy, Anatoliy↗
DOE OSTI2021

Molecularly tunable heterogeneous catalysts by edge functionalization of graphitic carbons

Disclosed are surface immobilized (electro)catalysts that may be prepared by a condensation reaction that generates an aromatic unit that is robust to acid and base and elevated temperatures. Among their many desirable characteristics, the catalysts are far less prone to the bimolecular deactivation pathways commonly observed for homogeneous catalysts, and may be used in solvents with a range of polarities and dielectric strengths. The catalysts are suitable for a wide array of thermal catalytic reactions (polymerization, oxidation, hydrogenation, cross-coupling etc.) and as anodes and/or cathodes in fuel cells, electrolyzers, and in batteries and supercapacitors.

Surendranath, Yogesh↗
DOE OSTI2020

Detailed Characterization of an Annealed Reduced Graphene Oxide Catalyst for Selective Peroxide Formation Activity

Recently, electrochemical hydrogen peroxide (H 2 O 2 ) generation from oxygen molecules has been extensively studied. Thus far, the best peroxide activity under alkaline conditions has been reported at the surface of a mild reduced graphene oxide annealed at 600 °C (mrGO-600). However, the detailed material information, such as chemical functionality and structural morphology, is unknown, which results in ambiguous debates on its catalytic active sites. Therefore, to solve this problem, we intensively characterize the structure of mrGO-600 to clarify the origin of its catalytic activity. Various characterizations, including X-ray photoelectron spectroscopy, Raman spectroscopy, infrared spectroscopy, near-edge X-ray absorption fine spectroscopy, and high-resolution transmittance electron microscopy coupled with in situ infrared spectroelecrochemistry, reveal that the annealing process generates not only various hole edge defects that are related to the ring ether group but also numerous point defects that result in a small-sized disconnected graphitic carbon region. These defects are believed to form a unique atomic level configuration in mrGO-600, which enables it to facilitate high peroxide-generated activity from oxygen molecules in an alkaline electrolyte.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Examples of X-Ray Characterization Techniques in Energy Storage Research

Lithium-ion batteries have revolutionized the portable electronics and transportation sectors. Their performance is often critically dependent on the crystal structures of the anode and cathode electrode materials, which must enable the transport and reversible storage of lithium ions into and out of the lattice. Because lithium is a low-Z element, characterization of materials for lithium-ion batteries can be particularly challenging. Regardless, X-ray techniques enable analysis of material structures to better understand how battery materials perform and degrade, particularly when combined with other materials characterization and electrochemical characterization techniques. While X-ray techniques are most often used in battery research for phase identification of crystal structures, X-ray characterization techniques are also used for a wide variety of other purposes. I will discuss several examples from my research with various collaborators on several projects that highlight the impact that X-ray characterization techniques can have on battery research. The first example will focus on low-temperature microwave-assisted solvothermal synthesis of vanadium-doped LiFePO4 cathode materials for lithium-ion batteries. (1,2) Through a combination of electrochemical and materials characterization, we determined that low temperature synthesis resulted in metastable phases that enabled incorporation of higher dopant levels than resulting from high-temperature synthesis of thermodynamically stable phases. Rietveld refinement of X-ray diffraction data enabled understanding of how lattice parameters changed with doping levels and synthesis temperature. X-ray absorption near edge spectroscopy enabled understanding of the vanadium and iron oxidation states to confirm how vacancies in the structure caused by doping were charge compensated. This was important to understand because the literature suggests doping can improve LiFePO4 electrical conductivity, which improves battery charge and discharge rates. The second example will focus on understanding residual strain in lithium metal anodes. Lithium-ion batteries typically use graphite anodes, but the charge-storage capacity can be theoretically improved ~10x by using lithium metal as the anode material instead. However, lithium anodes suffer from growth of high-aspect-ratio features, such as dendrites, that can pierce nanoporous polymer separators and lead to short circuits and fires. External pressure is commonly applied to cells to enable better morphological control. We hypothesized that applied pressure may promote strain and possibly work hardening during electrochemical cycling, which motivated us to look for evidence of residual strain in lithium metal cycled under applied pressure using X-ray diffraction and sin2(..psi..) analysis. We found that lithium electrodeposited under high pressure exhibited in-plane compressive strain and that that lithium electrodeposited under low pressure did not. (3) The residual strain that accompanies electrodeposition under high pressure may lead to work hardening, which may explain how a soft metal like lithium can puncture separators and why higher pressure does not always decrease short circuits. (4-6) References: 1) Harrison, K. L.; Manthiram, A. Microwave-Assisted Solvothermal Synthesis and Characterization of Metastable LiFe1- x (VO) x PO4 Cathodes. Inorganic chemistry 2011, 50(8), 3613-3620. 2) Harrison, K. L.; Bridges, C. A.; Paranthaman, M. P.; Segre, C. U.; Katsoudas, J.; Maroni, V. A.; Idrobo, J. C.; Goodenough, J. B.; Manthiram, A. Temperature Dependence of Aliovalent-Vanadium Doping in LiFePO4 Cathodes. Chemistry of Materials 2013, 25(5), 768-781. 3) Rodriguez, M. A.; Harrison, K. L.; Goriparti, S.; Griego, J. J.; Boyce, B. L.; Perdue, B. R. Use of a Be-Dome Holder for Texture and Strain Characterization of Li Metal Thin Films via Sin2 (..psi..) Methodology. Powder Diffraction 2020, 35(2), 89-97. 4) Jungjohann, K. L.; Gannon, R. N.; Goriparti, S.; Randolph, S. J.; Merrill, L. C.; Johnson, D. C.; Zavadil, K. R.; Harris, S. J.; Harrison, K. L. Cryogenic Laser Ablation Reveals Short-Circuit Mechanism in Lithium Metal Batteries. ACS Energy Letters 2021, 6(6), 2138-2144. 5) Harrison, K. L.; Merrill, L. C.; Long, D. M.; Randolph, S. J.; Goriparti, S.; Christian, J.; Warren, B.; Roberts, S. A.; Harris, S. J.; Perry, D. L. Cryogenic Electron Microscopy Reveals That Applied Pressure Promotes Short Circuits in Li Batteries. Iscience 2021, 24(12). 6) Harrison, K. L.; Goriparti, S.; Merrill, L. C.; Long, D. M.; Warren, B.; Roberts, S. A.; Perdue, B. R.; Casias, Z.; Cuillier, P.; Boyce, B. L. Effects of Applied Interfacial Pressure on Li-Metal Cycling Performance and Morphology in 4 M LiFSI in DME. ACS Applied Materials & Interfaces 2021, 13(27), 31668-31679.

batteries↗
DOE OSTI2019

Insights into Boron-Based Polyanion-Tuned High-Nickel Cathodes for High-Energy-Density Lithium-Ion Batteries

Ultrahigh-Ni layered oxide cathodes (Ni content > 90%) are at the forefront for potentially enabling higher-energy density lithium-ion batteries. Unfortunately, they suffer from rapid capacity fade, poor thermal stability, and increased air sensitivity. Introduction of boron-based polyanion into layered cathodes has been found to be effective in stabilizing high-Ni cathodes, but the mechanism behind it is not yet fully understood. To develop a better understanding, we present here an extensive characterization of the ultrahigh-Ni cathode LiNi 0.94 Co 0.06 O 2 (NC) and B 2 O 3 -LiNi 0.94 Co 0.06 O 2 (B-NC). The B-NC delivers a capacity of 223 mA h g -1 with 80% capacity retention after 400 cycles in full cells with graphite anodes, superior to 61% retention for NC. In-depth interphase investigations reveal that the improved cyclability is attributed to the development of a well-passivated boron/phosphorus-rich cathode-electrolyte interphase in B-NC. Moreover, B-NC demonstrates a considerably enhanced air-exposure and thermal stability. A 30-day air-stored B-NC delivers a discharge capacity of 125 mA h g -1 at 10C rate, in sharp contrast to 65 mA h g -1 for the stored NC. Finally, this work advances the understanding of the effect boron-based polyanion insertion into layered oxides has on battery performance and offers a viable strategy for developing practically viable ultra-high-Ni cathodes with high-energy density.

25 ENERGY STORAGE↗
DOE OSTI2018

Spectroelectrochemical investigations of nickel cyclam indicate different reaction mechanisms for electrocatalytic CO 2 and H + reduction

Rising levels of atmospheric carbon dioxide continue to motivate the development of catalysts that can efficiently convert CO 2 to useful products in water without substantial amounts of H 2 formed as a byproduct. In addition to synthetic efforts, mechanistic investigations on existing catalysts are necessary to understand the molecular factors contributing to activity and selectivity, which can guide rational improvements and increase catalyst robustness. [Ni(cyclam)] 2+ (cyclam = 1,4,8,11-tetraazacyclotetradecane) is one such catalyst, known for decades to be capable of selective CO 2 reduction to CO in water, but with little mechanistic information experimentally established or catalytic intermediates characterized. To better understand the mechanisms of aqueous H + and CO 2 reduction by [Ni(cyclam)] 2+ , spectroelectrochemical investigations were performed in conjunction with activity assays. Both large surface area glassy carbon and amorphous graphite rod working electrodes were tested, with the latter found to be significantly more active and selective for CO production. Optical, resonance Raman, and EPR spectroelectrochemical experiments on [Ni(cyclam)] 2+ during catalysis under N 2 , CO 2 , and CO gases show the appearance of a single species, independent of electrode used. Identical signals are observed under oxidizing potentials. Spectroscopic and electrochemical analysis coupled with density functional theory calculations suggest that the signals observed originate from [Ni(cyclam)(H 2 PO4)] 2+ . The generation of a NiIII species under catalytic, reducing conditions suggests an ECCE mechanism for H + reduction by [Ni(cyclam)] 2+ , which differs from the proton-coupled, ECEC pathway proposed for CO 2 reduction. The divergent mechanisms seen for the two reactions may underlie the differential reactivity of [Ni(cyclam)] 2+ towards each substrate, with implications for the design of increasingly selective molecular catalysts. Finally, this observation also highlights the substantial impact of buffer and electrode choice when characterizing and benchmarking the catalytic properties of new compounds.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1989

Compatibility of molten salts with advanced solar dynamic receiver materials

Metal-coated graphite fibers are being considered as a thermal conductivity enhancement filler material for molten salts in solar dynamic thermal energy storage systems. The successful metal coating chosen for this application must exhibit acceptable wettability and must be compatible with the molten salt environment. Contact angle values between molten lithium fluoride and several metal, metal fluoride, and metal oxide substrates have been determined at 892 C using a modification of the Wilhelmy plate technique. Reproducible contact angles with repeated exposure to the molten LiF indicated compatibility.

Jaworske, D. A.↗
DOE OSTI2022

Artificial cathode electrolyte interphase for improving high voltage cycling stability of thick electrode with Co-free 5 V spinel oxides

Spinel-type cathode LiNi 0.5 Mn 1.5 O 4 (LNMO) has intrigued the transportation industry due to its high operating voltage and total elimination of the expensive cobalt element. However, LNMO cathode with high mass loading (> 3 mAh/cm 2 in areal capacity) has suffered from excessive capacity degradation upon long cycling. Here, a robust Al 2 O 3 surface layer is introduced to the thick LNMO electrode via atomic layer deposition (ALD). The capacity retention in full cells with the graphite anode is improved from 46.3% to 75.3% after 300 cycles with cutoff voltage up to 4.85 V, while enabling average Coulombic efficiency of 99.9% during the cycling. The post-mortem analyses reveal that the Al 2 O 3 surface layer would convert to Al-O-F /Al-F species upon cycling, offering stable interphase to protect the cathode material. Furthermore, these results demonstrate the significance of surface modification enabling high voltage cathode for next-generation LIBs.

25 ENERGY STORAGE↗
DOE OSTI2015

Graphene nanocomposites for electrochemical cell electrodes

A composite composition for electrochemical cell electrode applications, the composition comprising multiple solid particles, wherein (a) a solid particle is composed of graphene platelets dispersed in or bonded by a first matrix or binder material, wherein the graphene platelets are not obtained from graphitization of the first binder or matrix material; (b) the graphene platelets have a length or width in the range of 10 nm to 10 .mu.m; (c) the multiple solid particles are bonded by a second binder material; and (d) the first or second binder material is selected from a polymer, polymeric carbon, amorphous carbon, metal, glass, ceramic, oxide, organic material, or a combination thereof. For a lithium ion battery anode application, the first binder or matrix material is preferably amorphous carbon or polymeric carbon. Such a composite composition provides a high anode capacity and good cycling response. For a supercapacitor electrode application, the solid particles preferably have meso-scale pores therein to accommodate electrolyte.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2022

Crosslinked Polyethyleneimine Gel Polymer Interface to Improve Cycling Stability of RFBs

Redox flow batteries are considered a promising technology for grid energy storage. However, capacity decay caused by crossover of active materials is a universal challenge for many flow battery systems, which are based on various chemistries. In this paper, using the vanadium redox flow battery as an example, we demonstrate a new gel polymer interface (GPI) consisting of crosslinked polyethyleneimine with a large amount of amino and carboxylic acid groups introduced between the positive electrode and the membrane. The GPI functions as a key component to prevent vanadium ions from crossing the membrane, thus supporting stable long-term cycling. Cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) measurements were conducted to investigate the effect of GPI on the electrochemical properties of graphitic carbon electrodes (GCFs) and redox reaction of catholyte. X-ray photoelectron spectroscopy (XPS) and 1 H nuclear magnetic resonance (NMR) spectra demonstrated that the crosslinked GPI is chemically stable for 100 cycles without dissolution of polymers and swelling in the strong acidic electrolytes. Results from inductively coupled plasma mass spectrometry (ICP-MS), Fourier-transform infrared (FTIR) spectroscopy, and energy-dispersive X-ray (EDX) spectroscopy proved that the GPI is effective in maintaining the concentration of vanadium species in their respective half-cells, resulting in improved cycling stability because of it prevents active species from crossing the membrane and stabilizes the oxidation states of active species.

Lim, Hyung-Seok↗
DOE OSTI2023

Cation-Driven Assembly of Bilayered Vanadium Oxide and Graphene Oxide Nanoflakes to Form Two-Dimensional Heterostructure Electrodes for Li-Ion Batteries

Lithium preintercalated bilayered vanadium oxide (LVO or δ-Li x V 2 O 5 ·nH 2 O) and graphene oxide (GO) nanoflakes were assembled using a concentrated lithium chloride solution and annealed under vacuum at 200 °C to form two-dimensional (2D) δ-Li x V 2 O 5 ·nH 2 O and reduced GO (rGO) heterostructures. Here we found that the Li + ions from LiCl enhanced the oxide/carbon heterointerface formation and served as stabilizing ions to improve structural and electrochemical stability. The graphitic content of the heterostructure could be easily controlled by changing the initial GO concentration prior to assembly. We found that increasing the GO content in our heterostructure composition helped inhibit the electrochemical degradation of LVO during cycling and improved the rate capability of the heterostructure. A combination of scanning electron microscopy and X-ray diffraction was used to help confirm that a 2D heterointerface formed between LVO and GO, and the final phase composition was determined using energy-dispersive X-ray spectroscopy and thermogravimetric analysis. Scanning transmission electron microscopy and electron energy-loss spectroscopy were additionally used to examine the heterostructures at high resolution, mapping the orientations of rGO and LVO layers and locally imaging their interlayer spacings. Further, electrochemical cycling of the cation-assembled LVO/rGO heterostructures in Li-ion cells with a non-aqueous electrolyte revealed that increasing the rGO content led to improved cycling stability and rate performance, despite slightly decreased charge storage capacity. The heterostructures with 0, 10, 20, and 35 wt % rGO exhibited capacities of 237, 216, 174, and 150 mAh g –1 , respectively. Moreover, the LVO/rGO-35 wt % and LVO/rGO-20 wt % heterostructures retained 75% (110 mAh g–1) and 67% (120 mAh g –1 ) of their initial capacities after increasing the specific current from 20 to 200 mA g –1 , while the LVO/rGO-10 wt % sample retained only 48% (107 mAh g –1 ) of its initial capacity under the same cycling conditions. In addition, the cation-assembled LVO/rGO electrodes exhibited enhanced electrochemical stability compared to electrodes prepared through physical mixing of LVO and GO nanoflakes in the same ratios as the heterostructure electrodes, further revealing the stabilizing effect of a 2D heterointerface. The cation-driven assembly approach, explored in this work using Li + cations, was found to induce and stabilize the formation of stacked 2D layers of rGO and exfoliated LVO. The reported assembly methodology can be applied for a variety of systems utilizing 2D materials with complementary properties for applications as electrodes in energy storage devices.

25 ENERGY STORAGE↗
DOE OSTI2017

Structure evolution and thermoelectric properties of carbonized polydopamine thin films

Carbonization of nature-inspired polydopamine can yield thin films with high electrical conductivity. Understanding of the structure of carbonized PDA (cPDA) is therefore highly desired. In this study, neutron diffraction, Raman spectroscopy, and other techniques indicate that cPDA samples are mainly amorphous with some short-range ordering and graphite-like structure that emerges with increasing heat treatment temperature. The electrical conductivity and the Seebeck coefficient show different trends with heat treatment temperature, while the thermal conductivity remains insensitive. Finally, the largest room-temperature ZT of 2 × 10 –4 was obtained on samples heat-treated at 800 °C, which is higher than that of reduced graphene oxide.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Functionalized Graphene via a One-Pot Reaction Enabling Exact Pore Sizes, Modifiable Pore Functionalization, and Precision Doping

Functionalizing graphene with exact pore size, specific functional groups, and precision doping poses many significant challenges. Current methods lack precision and produce random pore sizes, sites of attachment, and amounts of dopant, leading to compromised structural integrity and affecting graphene’s applications. In this work, we report a strategy for the synthesis of functionalized graphitic materials with modifiable nanometer-sized pores via a Pictet–Spengler polymerization reaction. This one-pot, four-step synthesis uses concepts based on covalent organic frameworks (COFs) synthesis to produce crystalline two-dimensional materials that were confirmed by PXRD, TEM measurements, and DFT studies. These new materials are structurally analogous to doped graphene and graphene oxide (GO) but, unlike GO, maintain their semiconductive properties when fully functionalized.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗