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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Locally Confined Polysulfide-Reactive Electrolytes for Shuttle-Free Sodium–Sulfur Batteries

Sodium-sulfur batteries promise high-energy-density and sustainable electrochemical energy storage but suffer from uncontrolled polysulfides dissolution and high sodium reactivity. These challenges fundamentally originate from poor electrolyte-electrode compatibility. Current electrolyte research inadequately addresses the trade-off between minimal polysulfides solvation and stabilizing sodium interfaces. Here, we present a locally-confined polysulfide-reactive electrolyte strategy that mediates the polysulfide dissolution dynamics and sodium stability by leveraging an electrophilic solvating species with a localized high-concentration electrolyte. This design enables shuttle-free cell operation by synergistically restricting the global solvating power of the electrolyte through intermolecular interactions and locally scavenging sparingly dissolved polysulfides via electrolyte electrophilicity. The precisely confined surface reaction facilitates a protective cathode-electrolyte interface, realizing a quasi-solid-state sulfur conversion in our liquid ether-based electrolyte, which crucially avoids crossover-induced catastrophic sodium-metal degradation. The proposed electrolyte demonstrates long-term cycling of high-mass-loading sulfur cathodes (> 3 mg S cm −2 with commercial carbon host and 70 wt% sulfur content), which afford 710 mA h g −1 over 400 cycles in coin cells and steady pouch cell operation over 180 cycles. Furthermore, this work establishes a scalable electrolyte design protocol that regulates the reaction chemistry of highly reactive electrodes, offering a pathway toward sustainable renewable energy storage.

25 ENERGY STORAGE↗
DOE OSTI2023

Investigation of Rechargeable Calcium Metal-Selenium Batteries Enabled by Borate-Based Electrolytes

Calcium-ion batteries (CIBs) are a promising next-generation energy storage system given the low redox potential of calcium metal and high abundance of calcium compounds. For continued CIB development, the discovery of high energy density calcium ion cathodes is needed to achieve practical energy density values. Here, we report on the use of elemental Se as a promising candidate for a high-capacity cathode material for CIBs that operates via a conversion mechanism in a Ca metal battery at room temperature. The Se electrodes demonstrate a reversible specific capacity of 180 mA h g –1 with a discharge plateau near 2.0 V (vs Ca 2+ /Ca) at 100 mA g –1 using an electrolyte based on the salt calcium tetrakis(hexafluoroisopropyloxy)borate (Ca(B(hfip) 4 ) 2 ) in 1,2-dimethoxyethane (DME) and Ca metal. The reversible electrochemical reaction between calcium and selenium is investigated using operando synchrotron-based techniques and the possible reaction mechanism discussed.

25 ENERGY STORAGE↗
DOE OSTI2024

Direct Recycling of End-of-Life Cathode Material Through Redox Chemistry Mediators

Lithium-ion batteries (LIBs) are ideal for electric vehicles and electronic devices because of their high-power density and outstanding cycle life. The need for recycled LIBs material is pivotal for the sustainability of the renewable energy industry. The recycling process needs to be both economically and environmentally conscious. Direct recycling is cheaper and generates the least amount of waste compared to pyrometallurgical and hydrometallurgical processes. Direct recycling explored in this work is useful for reclaiming precious minerals from the End-of-Life (EOL) LIBs material. The EOL material has varying lithium deficiency, hence, redox mediator relithiation restores the lithium content rapidly and at low cost. The redox mechanism relithiate EOL cathode material by shuttling charges very fast between lithium metal and EOL cathode material. The redox mediator is oxidized to create lithium rich solvent and reduced to relithiate EOL cathode material. However, the process is sensitive to pH changes. The redox reaction creates acidic solvent, which may cause lithium leaching. Therefore, use of lithium hydroxide (LiOH) to remove impurities on the surface of the EOL material and as a lithium source creates a basic solution to prevent lithium leaching and relithiate EOL material. This approach will potentially pave way for fast quality cathode material recovery at a low cost.

cathode material↗
DOE OSTI2014

The action mechanism of TiO{sub 2}:NaYF{sub 4}:Yb{sup 3+},Tm{sup 3+} cathode buffer layer in highly efficient inverted organic solar cells

We report the fabrication and characteristics of organic solar cells with 6.86% power conversion efficiency (PCE) by doping NaYF{sub 4}:Yb{sup 3+},Tm{sup 3+} into TiO{sub 2} cathode buffer layer. The dependence of devices performance on doping concentration of NaYF{sub 4}:Yb{sup 3+},Tm{sup 3+} is investigated. Results indicate that short-circuit current density (J{sub sc}) has an apparent improvement, leading to an enhancement of 22.7% in PCE for the optimized doping concentration of 0.05 mmol ml{sup −1} compared to the control devices. NaYF{sub 4}:Yb{sup 3+},Tm{sup 3+} nanoparticles (NPs) can play threefold roles, one is that the incident light in visible region can be scattered by NaYF{sub 4} NPs, the second is that solar irradiation in infrared region can be better utilized by Up-conversion effect of Yb{sup 3+} and Tm{sup 3+} ions, the third is that electron transport property in TiO{sub 2} thin film can be greatly improved.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Controlling Solid–Liquid Conversion Reactions for a Highly Reversible Aqueous Zinc–Iodine Battery

Aqueous rechargeable batteries are desirable for many energy storage applications due to their low cost and high safety. However, low capacity and short cycle life are the significant obstacles to their practical applications. Here, we demonstrate a highly reversible aqueous zinc-iodine battery using encapsulated iodine in microporous active carbon fibers (ACFs) as cathode materials through the rational control of solid-liquid conversion reactions. The experiments and density function theory (DFT) calculations were employed to investigate the effects of solvents and properties of carbon hosts, e.g. pore size, surface chemistries, on the adsorption of iodine species. The rational manipulation of the competition between the adsorption in carbon and solvation in electrolytes for iodine species is responsible for the high reversibility and cycling stability. The zinc-iodine batteries deliver a high capacity of 180 mAh g-1 at 1C and a stable cycle life over 3000 cycles with ~90% capacity retention as well as negligible self-discharge. We believe the principles for stabilizing the zinc-iodine system could provide new insight into conversion systems such as Li-S systems.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2017

Solar-Driven Reduction of 1 atm CO 2 to Formate at 10% Energy-Conversion Efficiency by Use of a TiO 2 -Protected III-V Tandem Photoanode in Conjunction with a Bipolar Membrane and a Pd/C Cathode Electrocatalyst

A solar-driven CO 2 -reduction (CO 2 R) cell, made up of a tandem GaAs/InGaP/TiO 2 /Ni photoanode in 1.0 M KOH(aq) (pH=13.7) to facilitate the oxygen-evolution reaction (OER), a Pd/C nanoparticle-coated Ti mesh cathode in 2.8 M KHCO 3 (aq) (pH=8.0) to perform the CO 2 R reaction, and a bipolar membrane to allow for steady-state operation of the catholyte and anolyte at different bulk pH values, was built. At the operational current density of 8.5 mA cm -2 , in 2.8 M KHCO 3 (aq), the cathode exhibited <100 mV overpotential and >94% Faradaic efficiency for the reduction of 1 atm of CO 2 (g) to formate. The anode exhibited 320 ± 7 mV overpotential for the OER in 1.0 M KOH(aq), and the bipolar membrane exhibited ~480 mV voltage loss with minimal product crossover as well as >90% and >95% selectivity for protons and hydroxide ions, respectively. The solar-driven CO 2 R cell converted sunlight to fuels at an energy-conversion efficiency of ~10%.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2026

Fe-single atom catalysts facilitate fast electron transfer with MoS 2 /SnS 2 cathodes in lithium–sulfur batteries

Lithium–sulfur batteries (LSBs) emerge as promising next-generation energy storage systems offering cost-effectiveness, environmental friendliness, and high theoretical energy density. The practical implementation of LSBs faces significant hindrances due to the shuttle effect and sluggish redox reactions. To address these challenges, single-atom catalyst (SAC) based combination materials from d-block elements can offer increased active catalytic sites, rapid charge transfer, accelerated electron migration, and fast sulfur redox conversion kinetics of lithium polysulfides (LiPSs). In this study, we fabricated three different LSB cathodes: pure S, S@MoS 2 /SnS 2 , and S@Fe–MoS 2 /SnS 2 . These cathodes were then used to explore the cycle life, capacity, rate capability, and redox kinetic reactions of LiPSs while assessing the influence of Fe-SACs on their performance. As a result, LSBs with S@Fe–MoS 2 /SnS 2 cathodes demonstrate an extended cycle life of 1000 cycles at a C-rate of 0.2C, maintaining a capacity close to 500 mA h g −1 , the highest initial discharge capacity of 1622 mA h g −1 and 1066 mA h g −1 at 0.05C and 0.2C, and excellent rate capabilities of 708 mA h g −1 and 558 mA h g −1 at 1C and 2C, respectively. The synergistic effect of the Fe-SAC-based combination cathode (S@Fe–MoS 2 /SnS 2 ) creates plentiful adsorptive and highly active catalytic sites, resulting in substantially enhanced capacity for adsorbing soluble long-chain LiPSs. This facilitates ultra-fast redox kinetics, surpassing the performance of the S@MoS 2 /SnS 2 and pure S cathodes. In the ex situ analysis, results from powder X-ray diffraction (XRD) to observe the new phase, soft X-ray absorption spectroscopy (XAS) to investigate the electronic structure, and hard X-ray photoelectron microscopy (HAXPES) with different energies (900 eV, 2000 eV, and 6000 eV) to track the chemical-state evolution of Fe-SACs in MoS 2 /SnS 2 cathodes displayed notable electrochemical reversibility involving S 8 ⇄ LiPSs ⇄ Li 2 S conversion even after 1000 cycles. Additionally, in situ, operando Raman analysis can unveil a novel catalytic mechanism of Fe-SACs in MoS 2 /SnS 2 “facilitating rapid electron transfer” during the discharge and charge processes of LSBs involving the conversion of S 8 ⇄ long-chain LiPSs ⇄ Li 2 S 2 /Li 2 S. This study elucidates the working mechanism of Fe-SAC cathodes, offering insights into overcoming the shuttle effect and facilitating sulfur redox kinetics to advance commercial LSBs.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Micro cavity fission chamber radiation detection system

A radiation detector to monitor the neutron flux of a nuclear reactor or other high-radiation environment, that can withstand the high temperatures and radiation fields of such environment, is provided. A small dielectric substrate with a low neutron-activation cross section is provided. The substrate is coated with a neutron conversion material, such as uranium oxide or thorium oxide. One or more substrates form a micro-sized detection cavity that is filled with a detection gas. A voltage is provided across anode and cathode wires in the detection cavity. A neutron absorbed in the conversion material may release reaction products into the gas, causing ionization of the gas which then produces a current or voltage signal. The small detector volume minimizes energy deposition into the detection gas by competing particles such as gamma rays, fast electrons, and beta particles, and therefore minimizes false counts while retaining large signals from neutron interactions.

McGregor, Douglas S.↗
DOE OSTI2023

Robust highly durable solid oxide fuel cell cathodes – Improved materials compatibility & self-regulating surface chemistry

Solid oxide fuel cells (SOFCs) are electrochemical conversion devices that directly transform hydrogen or hydrocarbon fuels to electricity, with energy efficiencies as high as 90%, coupled with reduced emissions. Several factors, however, remain to be addressed when considering scale-up of SOFC technology, including the need to overcome decreased performance due to sluggish rates of the oxygen reduction reaction (ORR) at the cathode under reduced temperatures and susceptibility to degradation in performance from surface poisoning e.g. from chromia, while limiting the use of critical raw materials (lanthanides and transition metals) present in high performing mixed ionic electronic conducting electrodes like (La,Sr)CoO 3 (LSC). In this project we explored the key descriptors for determining ORR activity in SOFC electrodes and tried to recover performance degradation by applying them to SOFC electrodes. In order to do this, we first selected a model mixed ionic electronic conducting (MIEC) oxide, Pr-doped CeO 2 (Pr 0.1 Ce 0.9 O 2-δ , PCO), which is a chemically stable fluorite and free of inherent poison sources (e.g. Sr segregation in LSC) that potentially react with external impurities such as Cr-species vaporized from the interconnect. The three approaches originally planned in this project are as follows: 1) evaluation of scavenger exsolution characteristics, 2) study of scavengers gettering efficacy following Cr and Si poisoning and 3) integration of new compositions into porous electrodes. Among them, exceptional progress has been made in 2) and 3), especially understanding the role of surface infiltrants in impacting electrode performance and degradation of PCO materials. We found that the Smith acidity scale for binary oxides serves as a powerful descriptor for tuning and predicting the oxygen exchange kinetics on MIEC PCO surfaces. As a result, with infiltration with binary oxides, ranging from strongly basic (Li 2 O) to strongly acidic (SiO 2 ) onto the surface of porous PCO, it was possible to systematically vary the chemical surface exchange coefficient (k chem ) by 6 orders of magnitude! L i2 O increased k chem by nearly 1,000 times over that of pristine PCO, while SiO 2 decreased k chem by nearly the same factor. Strikingly, although the pre-exponential of k chem scales linearly with the acidity of the infiltrated binary oxide, there is nearly no change in the activation energy. With this insight, we attributed the origin of these dramatic changes in k chem values to the systematic increase and decrease in the surface electron density induced by infiltrated binary oxides. More interestingly, although both Cr 2 O 3 and SiO 2 were determined to be acidic by Smith, suggesting that this feature could likely be the primary reason that these compounds serve to poison the ORR on SOFC cathodes, the effect of poisoning could be subsequently tuned by adding multiple infiltrants and controlling their relative surface acidities. We also systematically examined the effect of serial infiltration of basic and acidic oxides. It turned out that serial infiltration of Li not only recovers approximately 20-fold degraded k chem of PCO by acidic Cr 2 O 3 but its k chem is enhanced even beyond that of the non-infiltrated PCO by more than three orders of magnitude. This was further verified with a screen-printing PCO symmetric cell in terms of the electrode performance (area-specific resistance, ASR) related to approach 3). These observations point to acidity as a key descriptor not only in tuning and predicting the ORR activity of SOFC cathodes that largely determines the overall performance of SOFC, but in mitigating and reactivating poisoned electrode performance. This work provides novel guidelines for making the electrode performance much more active and robust in SOFCs, which can further be applied to all applications requiring oxygen exchange reaction, such as electrolyzers, permeation membranes and gas sensors.

30 DIRECT ENERGY CONVERSION↗
NASA NTRS1983

Visible light to electrical energy conversion using photoelectrochemical cells

Sustained conversion of low energy visible or near i.r. light (>1.25 eV) to electrical energy has been obtained using wet photoelectrochemical cells where there are no net chemical changes in the system. Stabilization of n-type semi-conductor anodes of CdS, CdSe, CdTe, GaP, GaAs and InP to photoanodic dissolution is achieved by employing selected alkaline solutions of Na.sub.2 S, Na.sub.2 S/S, Na.sub.2 Se, Na.sub.2 Se/Se, Na.sub.2 Te and Na.sub.2 Te/Te as the electrolyte. The oxidation of (poly) sulfide, (poly)selenide or (poly)telluride species occurs at the irradiated anode, and reduction of polysulfide, polyselenide or polytelluride species occurs at the dark Pt cathode of the photoelectrochemical cell. Optical to electrical energy conversion efficiencies approaching 15% at selected frequencies have been observed in some cells. The wavelength for the onset of photocurrent corresponds to the band gap of the particular anode material used in the cell.

Wrighton, Mark S.↗
DOE OSTI2017

Mechanistic Insights Evaluating Ag, Pb, and Ni as Electrocatalysts for Furfural Reduction from First-Principles Methods

Electrochemical reduction of furfural (ECRFF) emerges as an efficient and sustainable means to obtain high-value chemicals and biofuels with the activity and product selectivity being sensitive to cathode materials. In this work, elementary steps describing furfuryl alcohol (FA) and 2-methylfuran (MF) production routes in ECRFF are studied by using periodic density functional theory on Ag, Pb, and Ni, as alternative cathode materials. The established Brønsted–Evans–Polanyi (BEP) relationship has been proven to be reliable to estimate energy barriers of C–O bond cleavage. The intrinsic characters of Ag, Pb, and Ni are then summarized in free energy diagrams to reflect the FA and MF production trends as future guidelines to evaluate ECRFF activity and selectivity on these metals. On all metal surfaces, at both terrace and stepped sites, the first C–H or O–H hydrogenation step, producing respective mh6 or mh7 intermediates, influences overall FA production. On Ag and Pb, pathways involving the mh6 intermediate are thermodynamically and kinetically favored, whereas on Ni, both mh6 and mh7 routes are competitive due to strong interactions between the furan ring and the substrate. In addition, these partially hydrogenated intermediates can also undergo C–O bond cleavage with reduced energy barriers (compared to direct C–O bond cleavage in furfural), which opens potential paths for parallel MF production. Conversion of FA into MF catalyzed by these metallic cathodes was considered as well, although the high C–O bond cleavage energy barrier is likely to hinder this process.

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

Porous and Amorphous Mn x Mo 3 S 13 Chalcogel Electrode for High-Capacity Conversion-Based Lithium-Ion Batteries

While Li-ion batteries (LIBs) are a leading energy storage technology, their energy densities are limited by the low capacity of conventional intercalation cathodes, driving interest in high energy-density Li–S batteries that make use of conversion chemistry. Achieving high capacity, reversibility, and cycle stability, and controlling volume changes in conversion batteries during the charge–discharge process, however, remains challenging. Here, in this study, we present a porous, amorphous, sulfide-based Mn x Mo 3 S 13 chalcogel, which concurrently offers high capacity and cycle stability. The solution-processable room temperature synthesized Mn x Mo 3 S 13 (x = 0.25) chalcogel exhibits a local structure that resembles the Mo 3 S 13 cluster with Mn 2+ distributed across the Mo 3 S 13 matrix, as determined by synchrotron X-ray pair distribution function (PDF) and extended X-ray absorption fine structure (EXAFS). Ab initio molecular dynamics (AIMD) simulations reveal that Mn 2+ incorporation shortens the polysulfide chain in the gel matrix compared to the Mo 3 S 13 chalcogel, while forming a coordination environment with disulfide groups, analogous to the experimental findings. A Li/Mn 0.25 Mo 3 S 13 half-cell delivers 897 mAh g –1 capacity during the first discharge and retains 571 mAh g –1 capacity after 100 cycles at a C/3 rate. Distribution of relaxation time (DRT) unveils a stable solid–electrolyte interphase (SEI) formation upon cycling that enables charge–discharge reversibility. Here, the enhanced capacity retention and cycle stability compared to those of the Li/Mo 3 S 13 cell are attributed to the reduced dissolution of active mass into the electrolyte, facilitated by the formation of shorter polysulfide chains within the Mn 0.25 Mo 3 S 13 structure and the strong affinity of Lewis-acidic Mn 2+ for polysulfide anions generated during the charge–discharge process of the Li/Mn 0.25 Mo 3 S 13 cell. Thus, this work illustrates a design principle of material for high-capacity and cycle-stable Li-metal sulfide batteries.

25 ENERGY STORAGE↗
DOE OSTI2016

Back-gated graphene anode for more efficient thermionic energy converters

Thermionic energy converters (TECs) are a direct heat-to-electricity conversion technology with great potential for high efficiency and scalability. However, space charge barrier in the inter-electrode gap and high anode work function are major obstacles toward realizing high efficiency. Here, we demonstrate for the first time a prototype TEC using a back-gated graphene anode, a barium dispenser cathode, and a controllable inter-electrode gap as small as 17 µm, which simultaneously addresses these two obstacles. This leads to an electronic conversion efficiency of 9.8% at cathode temperature of 1000 °C, the highest reported by far. We first demonstrate that electrostatic gating of graphene by a 20 nm HfO 2 dielectric layer changes the graphene anode work function by 0.63 eV, as observed from the current-voltage characteristics of the TEC. Next, we show that the efficiency increases by a factor of 30.6 by reducing the gap from 1 mm down to 17 µm, after a mono-layer of Ba is deposited on graphene by the dispenser cathode. Lastlu, we show that electrostatic gating of graphene further reduces the graphene work function from 1.85 to 1.69 eV, leading to an additional 67% enhancement in TEC efficiency. Note that the overall efficiency using the back-gated graphene anode is 6.7 times higher compared with that of a TEC with a tungsten anode and the same inter-electrode gap.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2023

Unlocking the Potential of A-Site Ca-Doped LaCo 0.2 Fe 0.8 O 3-δ : A Redox-Stable Cathode Material Enabling High Current Density in Direct CO 2 Electrolysis

Massive carbon dioxide (CO 2 ) emission from recent human industrialization has affected the global ecosystem and raised great concern for environmental sustainability. The solid oxide electrolysis cell (SOEC) is a promising energy conversion device capable of efficiently converting CO 2 into valuable chemicals using renewable energy sources. However, Sr-containing cathode materials face the challenge of Sr carbonation during CO 2 electrolysis, which greatly affects the energy conversion efficiency and long-term stability. Thus, A-site Ca-doped La1– x CaxCo 0.2 Fe 0.8 O 3-δ (0.2 ≤ x ≤ 0.6) oxides are developed for direct CO 2 conversion to carbon monoxide (CO) in an intermediate-temperature SOEC (IT-SOEC). With a polarization resistance as low as 0.18 O cm 2 in pure CO 2 atmosphere, a remarkable current density of 2.24 A cm –2 was achieved at 1.5 V with La 0.6 Ca 0.4 Co 0.2 Fe 0.8 O 3-δ (LCCF64) as the cathode in La 0.8 Sr 0.2 Ga 0.83 Mg 0.17 O 3-δ (LSGM) electrolyte (300 µm) supported electrolysis cells using La 0.6 Sr 0.4 Co 0.2 Fe 0.8 O 3-δ (LSCF) as the air electrode at 800 °C. Furthermore, symmetrical cells with LCCF64 as the electrodes also show promising electrolysis performance of 1.78 A cm –2 at 1.5 V at 800 °C. In addition, stable cell performance has been achieved on direct CO 2 electrolysis at an applied constant current of 0.5 A cm –2 at 800 °C. The easily removable carbonate intermediate produced during direct CO 2 electrolysis makes LCCF64 a promising regenerable cathode. The outstanding electrocatalytic performance of the LCCF64 cathode is ascribed to the highly active and stable metal/perovskite interfaces that resulted from the in situ exsolved Co/CoFe nanoparticles and the additional oxygen vacancies originated from the Ca 2 Fe 2 O 5 phase synergistically providing active sites for CO 2 adsorption and electrolysis. Here this study offers a novel approach to design catalysts with high performance for direct CO 2 electrolysis.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2018

Operando Studies Reveal Structural Evolution with Electrochemical Cycling in Li–CoS 2

The desire for high energy density alternatives to Li-ion batteries has led to great interest in energy storage materials not inherently constrained by the capacity limits of standard intercalation electrode materials currently employed in commercial devices. Among the alternatives under consideration are electrode materials with theoretical capacities many times greater than intercalation electrodes, including those that store charge through so-called conversion reactions. However, the vast structural changes that enable the high theoretical capacity of conversion systems contribute to issues of poor efficiency and short cycle life. To better understand the cycling issues in conversion systems, we study the local structure evolution of the cathode active material in LiCoS 2 cells. Being metallic, and potentially being capable of redox on both the anion and cation, we would expect CoS 2 to be a promising cathode material. Through combined ex situ X-ray absorption near-edge spectroscopy and pair distribution function analysis from operando X-ray total scattering, we describe the reactions that take place over the first 1.5 cycles. In doing so, we identify the irreversible formation of a Co 9 S 8 -like local structure with significantly limited electrochemical activity as the primary source of capacity fade. The methods employed here and the insights that emerge inform the rational design of conversion systems for electrochemical energy storage.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

A long-pulse repetitive operation magnetically insulated transmission line oscillator

The improved magnetically insulated transmission line oscillator (MILO) is a gigawatt-class L-band high power microwave tube. It has allowed us to generate 3.1 GW pulse of 40 ns duration in the single-pulse operation and 500 MW pulse of 25 ns duration in the repetition rate operation. However, because of the severe impedance mismatch, the power conversion efficiency is only about 4% in the repetition rate operation. In order to eliminate the impedance mismatch and obtain repetitive long-pulse high-power microwave (HPM), a series of experiments are carried out and the recent progress is presented in this paper. In the single-pulse operation, when the diode voltage is 466 kV and current is 41.6 kA, the radiated microwave power is above 2.2 GW, the pulse duration is above 102 ns, the microwave frequency is about 1.74 GHz, and the power conversion efficiency is about 11.5%. In the repetition rate operation, under the condition of the diode voltage about 400 kV, beam current about 38 kA, the radiated microwave power is about 1.0 GW, the pulse duration is about 85 ns. Moreover, the radiated microwave power and the pulse duration decline little by little when the shot numbers increase gradually. The experimental results show that the impedance matching is a vital factor for HPM systems and one of the major technical challenges is to improve the cathode for the repetition rate operation MILO.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2017

Lithiation Mechanism of Tunnel-Structured MnO 2 Electrode Investigated by In Situ Transmission Electron Microscopy

Manganese oxide (α-MnO 2 ) has been considered as a promising energy material, including as a lithium-based battery electrode candidate, due to its environmental friendliness. Thanks to its unique 1D [2 × 2] tunnel structure, α-MnO 2 can be applied to a cathode by insertion reaction and to an anode by conversion reaction in corresponding voltage ranges, in a lithium-based battery. Numerous reports have attributed its remarkable performance to its unique tunnel structure; however, the precise electrochemical reaction mechanism remains unknown. In this study, finding of the lithiation mechanism of α-MnO 2 nanowire by in situ transmission electron microscopy (TEM) is reported. By elaborately modifying the existing in situ TEM experimental technique, rapid lithium-ion diffusion through the tunnels is verified. Furthermore, by tracing the full lithiation procedure, the evolution of the MnO intermediate phase and the development of the MnO and Li 2 O phases with preferred orientations is demonstrated, which explains how the conversion reaction occurs in α-MnO 2 material. This study provides a comprehensive understanding of the electrochemical lithiation process and mechanism of α-MnO 2 material, in addition to the introduction of an improved in situ TEM biasing technique.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗