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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Ultrafast Metal Electrodeposition Revealed by In Situ Optical Imaging and Theoretical Modeling towards Fast–Charging Zn Battery Chemistry

Metallic Zn is a preferred anode material for rechargeable aqueous batteries towards a smart grid and renewable energy storage. Importantly, understanding how the metal nucleates and grows at the aqueous Zn anode is a critical and challenging step to achieve full reversibility of Zn battery chemistry, especially under fast-charging conditions. Here, by combining in situ optical imaging and theoretical modeling, we uncover the critical parameters governing the electrodeposition stability of the metallic Zn electrode, that is, the competition among crystallographic thermodynamics, kinetics, and Zn 2+ -ion diffusion. Moreover, steady-state Zn metal plating/ stripping with Coulombic efficiency above 99 % is achieved at 10-100 mA cm -2 in a reasonably high concentration (3 M) ZnSO 4 electrolyte. Significantly, a long-term cycling-stable Zn metal electrode is realized with a depth of discharge of 66.7% under 50 mA cm -2 in both Zn || Zn symmetrical cells and MnO 2 || Zn full cells.

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

High mass loading potassium ion stabilized manganese dioxide nanowire forests for rechargeable Zn batteries

Manganese dioxide (MnO 2 ) represents an ideal cathode material for rechargeable aqueous Zn batteries due to its high theoretical capacity (308 mAh g -1 ), suitable potential (1.4 V vs. Zn 2+ /Zn), natural abundance, and negligible toxicity. However, the capacity and rate capability of MnO 2 deteriorate significantly in thick electrodes owing to its low electrical and ionic conductivities. Herein, we report the design of high mass loading potassium ion stabilized α-MnO 2 (K 0.133 MnO 2 ) nanowire forests on carbon cloth through a seed-assisted hydrothermal method for Zn batteries. Further, the vertically aligned K 0.133 MnO 2 nanowire forests with uninterrupted charge transport afford a high area capacity of 3.54 mAh cm -2 and a capacity retention of 79.2% over 1000 cycles in aqueous electrolyte. Moreover, the high area capacity and cyclability can be readily transferred to quasi-solid-state devices.

25 ENERGY STORAGE↗
DOE OSTI2024

Suppressing metal corrosion through identification of optimal crystallographic plane for Zn batteries

Direct use of metals as battery anodes could significantly boost the energy density, but suffers from limited cycling. To make the batteries more sustainable, one strategy is mitigating the propensity for metals to form random morphology during plating through orientation regulation, e.g., hexagonal Zn platelets locked horizontally by epitaxial electrodeposition or vertically aligned through Zn/electrolyte interface modulation. Current strategies center around obtaining (002) faceted deposition due to its minimum surface energy. Here, benefiting from the capability of preparing a library of faceted monocrystalline Zn anodes and controlling the orientation of Zn platelet deposits, we challenge this conventional belief. We show that while monocrystalline (002) faceted Zn electrode with horizontal epitaxy indeed promises the highest critical current density, the (100) faceted electrode with vertically aligned deposits is the most important one in suppressing Zn metal corrosion and promising the best reversibility. Such uniqueness results from the lowest electrochemical surface area of (100) faceted electrode, which intrinsically builds upon the surface atom diffusion barrier and the orientation of the pallets. These new findings based on monocrystalline anodes advance the fundamental understanding of electrodeposition process for sustainable metal batteries and provide a paradigm to explore the processing–structure–property relationships of metal electrodes.

25 ENERGY STORAGE↗
DOE OSTI2022

Three-dimensional Zn-based alloys for dendrite-free aqueous Zn battery in dual-cation electrolytes

Aqueous zinc-ion batteries, in terms of integration with high safety, environmental benignity, and low cost, have attracted much attention for powering electronic devices and storage systems. However, the interface instability issues at the Zn anode caused by detrimental side reactions such as dendrite growth, hydrogen evolution, and metal corrosion at the solid (anode)/liquid (electrolyte) interface impede their practical applications in the fields requiring long-term performance persistence. Despite the rapid progress in suppressing the side reactions at the materials interface, the mechanism of ion storage and dendrite formation in practical aqueous zinc-ion batteries with dual-cation aqueous electrolytes is still unclear. Herein, we design an interface material consisting of forest-like three-dimensional zinc-copper alloy with engineered surfaces to explore the Zn plating/stripping mode in dual-cation electrolytes. The three-dimensional nanostructured surface of zinc-copper alloy is demonstrated to be in favor of effectively regulating the reaction kinetics of Zn plating/stripping processes. The developed interface materials suppress the dendrite growth on the anode surface towards high-performance persistent aqueous zinc-ion batteries in the aqueous electrolytes containing single and dual cations. This work remarkably enhances the fundamental understanding of dual-cation intercalation chemistry in aqueous electrochemical systems and provides a guide for exploring high-performance aqueous zinc-ion batteries and beyond.

25 ENERGY STORAGE↗
DOE OSTI2020

Porous FeCo Glassy Alloy as Bifunctional Support for High-Performance Zn-Air Battery

Zn-air battery (ZAB) is attracting increasing attention due to its high safety and performance. However, the practical application of ZAB relies heavily on developing durable support materials to replace conventional carbon supports which have unrecoverable corrosion issues, severely jeopardizing ZAB performance. Herein, a novel porous FeCo glassy alloy was developed as bifunctional catalytic support for ZAB. Specifically, the conducting skeleton of the porous glassy alloy was used to stabilize oxygen reduction cocatalysts, and more importantly, the FeCo served as the primary phase for oxygen evolution. To prove the concept of catalytic glassy alloy support, ultra-small Pd nanoparticles were anchored, as oxygen reduction active sites, on the porous FeCo (noted as Pd/FeCo) for ZAB. The Pd/FeCo exhibited a significantly improved electrocatalytic activity for oxygen reduction (a half-wave potential of 0.85 V) and oxygen evolution (a potential of 1.55 V to reach 10 mA cm –2 ) in the alkaline media. When used in the ZAB, the Pd/FeCo delivered an output power density of 117 mW cm –2 and outstanding cycling stability for over 200 h (400 cycles), surpassing the conventional carbon-supported Pt/C+IrO 2 catalysts. Such an integrated design of combining highly active components with porous architecture provides a new strategy to develop novel nanostructured electrocatalysts.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Quantifying and Suppressing Proton Intercalation to Enable High-Voltage Zn-Ion Batteries

Rechargeable Zn-ion batteries (ZIBs) are widely regarded as promising candidates for large-scale energy storage applications. Like most multivalent battery systems (based on Zn, Mg, Ca, etc.), further progress in ZIB development relies on the discovery and design of novel cathode hosts capable of reversible Zn 2+ (de)intercalation. This work employs VPO 4 F as a ZIB cathode and explores ensuing intercalation mechanisms along with interfacial dynamics during cycling to quantify the water dynamics in concentrated electrolytes and/or hybrid aqueous-non aqueous (HANEs) electrolyte(s). Like most oxide-based cathode materials, proton (H + ) intercalation dominates electrochemical activity during discharge of Zn x H y VPO 4 F in aqueous media due to the hydroxylated nature of the interface. Such H + electrochemistry diminishes low-rate and/or long-term electrochemical performance of ZIBs which inhibits implementation for practical applications. Thus, quantification of the water dynamics in various electrolytes is demonstrated for the first time. Detailed investigations of water mobility in various concentrated electrolytes and HANEs systems enable the design of an electrolyte that enhances aqueous anodic stability and suppresses water/proton activity during discharge. Tuning Zn 2+ /H + intercalation kinetics simultaneously allows for a high voltage (1.9 V) and long-lasting aqueous zinc-ion battery: Zn|Zn(OTf) 2 · n H 2 O-PC|Zn x H y VPO 4 F.

25 ENERGY STORAGE↗
DOE OSTI2020

Unraveling the Dissolution-Mediated Reaction Mechanism of α-MnO 2 Cathodes for Aqueous Zn-Ion Batteries

Aqueous Zn/α-MnO 2 batteries have attracted immense interest owing to their high energy density, low cost, and safety, making them desirable for future large-scale energy application. Despite these merits, the comprehensive understanding of their reaction mechanism has been elusive due to the limitations of standard bulk characterization. Here, via transmission electron microscopy, the dissolution-mediated reaction mechanism of a Zn/α-MnO 2 system is discovered and explored in full scope to involve reversible formation of Zn 4 SO 4 (OH) 6 · x H 2 O and “birnessite-like” Zn-MnO x phase upon cycling. Overall, α-MnO 2 acts primarily as a source for cell activation through dissolution and thus is not directly involved in the Zn redox chemistry. Overall, this microscopic study offers a unique knowledge on the unconventional reaction chemistry of Zn/α-MnO 2 batteries.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Stabilizing Zinc Anode Reactions by Polyethylene Oxide Polymer in Mild Aqueous Electrolytes

Abstract Zn dendrites growth and poor cycling stability are significant challenges for rechargeable aqueous Zn batteries. Zn metal deposition‐dissolution in aqueous electrolytes is typically determined by Zn anode–electrolyte interfaces. In this work, the role of a long‐chain polyethylene oxide (PEO) polymer as a multifunctional electrolyte additive in stabilizing Zn metal anodes is reported. PEO molecules suppress Zn 2+ ion transfer kinetics and regulate Zn 2+ ion concentration in the vicinity of Zn anodes through interactions between ether groups of PEO and Zn 2+ ions. The suppressed Zn 2+ ion transfer kinetics and homogeneous Zn 2+ ion distribution at the interface promotes dendrite‐free homogeneous Zn deposition. In addition, electrochemically inert PEO molecules adsorbed onto Zn anodes can protect the anode surfaces from H 2 generation and, thereby, enhance their electrochemical stability. Stable cycling over 3000 h and high reversibility (Coulombic efficiency > 99.5%) of Zn anodes is demonstrated in 1 m ZnSO 4 electrolyte with 0.5 wt% PEO. This finding provides helpful insights into the mechanism of Zn metal anodes stabilization by low‐cost multifunctional polymer electrolyte additives that stabilize interfacial reactions.

Jin, Yan↗
DOE OSTI2022

Structural, Dynamic, and Chemical Complexities in Zinc Anode of an Operating Aqueous Zn-Ion Battery

Aqueous Zn-ion battery is a promising technology for electrochemical energy storage. The formation of Zn dendrites, however, can jeopardize the cell cycle life and thus, hinders the industrial adoption of this technology. A fundamental understanding of the kinetic mechanisms is crucial for improving the Zn-ion battery. Here, in situ and operando X-ray microscopy methods are utilized to visualize the Zn plating and stripping behaviors under different electrochemical conditions. It is demonstrated that the substrate curvature, local morphology, electrochemical protocols, and the surface chemistry can collectively affect the Zn plating behavior. Furthermore, these results provide new insights for developing the next-generation dendrite-free and long-span aqueous Zn-ion battery.

25 ENERGY STORAGE↗
DOE OSTI2022

High-Performance InZn Alloy Anodes toward Practical Aqueous Zinc Batteries

Aqueous Zn batteries have high safety, low-cost and potential of delivering comparable energy density to alkali-ion batteries. However, its practical application is largely hampered by the limited cycle life associated with Zn anodes under conditions of high depth of discharge and high plating current densities. In this work, we report on electrodeposited indium-zinc alloy anodes that have well-dispersed zinc-domains surrounding indium domains that form a porous structure after dealloying which greatly improves tolerance to Zn dendrite formation. The InZn anodes exhibit low polarization of ~5 to 25 mV and demonstrate 700 cycles at a current density of ~10 mA cm -2 with a capacity of 5 mAh cm-2 capacity (45% depth-of-discharge). Full cells with an InZn anode, dibenzo[b,i]thianthrene-5,7,12,14-tetraone (DTT) cathode, in 2M ZnSO 4 deliver a capacity of ~ 110 mAh g -1 and good stability over 40 cycles. Finally, the work reveals a rational design of Zn-based anodes towards practical battery applications and opens the curtain for future development of aqueous Zn batteries.

25 ENERGY STORAGE↗
DOE OSTI2020

Potentiodynamics of the Zinc and Proton Storage in Disordered Sodium Vanadate for Aqueous Zn-Ion Batteries

A rechargeable Zn-ion battery is a promising aqueous system, where coinsertion of Zn 2+ and H + could address the obstacles of the sluggish ionic transport in cathode materials imposed by multivalent battery chemistry. However, there is a lack of fundamental understanding of this dual-ion transport, especially the potentiodynamics of the storage process. Here, a quantitative analysis of Zn 2+ and H + transport in a disordered sodium vanadate (NaV 3 O 8 ) cathode material has been reported. Collectively, synchrotron X-ray analysis shows that both Zn 2+ and H + storages follow an intercalation storage mechanism in NaV 3 O 8 and proceed in a sequential manner, where intercalations of 0.26 Zn 2+ followed by 0.24 H + per vanadium atom occur during discharging, while reverse dynamics happens during charging. We find that such a unique and synergistic dual-ion sequential storage favors a high capacity (265 mA h g –1 ) and an energy density (221 W h kg –1 ) based on the NaV 3 O 8 cathode and a great cycling life (a capacity retention of 78% after 2000 cycles) in Zn/NaV 3 O 8 full cells.

36 MATERIALS SCIENCE↗