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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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Tire-derived carbon composite anodes for sodium-ion batteries
We report that hard-carbon materials are considered as one of the most promising anodes for the emerging sodium-ion batteries. Here, we report a low-cost, scalable waste tire-derived carbon as an anode for sodium-ion batteries (SIBs). The tire-derived carbons obtained by pyrolyzing the acid-treated tire at 1100 °C, 1400 °C and 1600 °C show capacities of 179, 185 and 203 mAh g -1 , respectively, after 100 cycles at a current density of 20 mA g -1 in sodium-ion batteries with good electrochemical stability. The portion of the low-voltage plateau region in the charge-discharge curves increases as the heat-treatment temperature increases. The low-voltage plateau is beneficial to enhance the energy density of the full cell. However, this plateau suffers rapid capacity fade at higher current densities. This study provides a new pathway for inexpensive, environmentally benign and value-added waste tire-derived products towards large-scale energy storage applications.
Mixed-conducting interlayer boosting the electrochemical performance of Ni-rich layered oxide cathode materials for lithium ion batteries
In this work, a unique artificial interface combing characteristics of both high ionic and electronic conductivities has been successfully constructed at the surface of Ni-rich LiNi 0·8 Co 0·1 Mn 0·1 O 2 (NCM811). The ionic conductor layer is fabricated through reacting H 3 PO 4 with the lithium residuals on the surface of NCM811 to form Li 3 PO 4 . The interface with high electronic conductivity is constructed by attaching graphene fragments to the NCM811 spherical particles. Due to the synergistic effect of the Li3PO4 coating layer and the graphene network, the modified sample (GN-LPO-NCM811) exhibits high capacity retention of 94.3% after 150 cycles at 0.5C between 3.0 and 4.3 V, while the pristine material shows a much lower retention of only 88.1%. In addition, the GN-LPO-NCM811 also presents improved cycling stability at elevated temperature of 55 °C. Even at an extremely high rate of 10C, the GN-LPO-NCM811 still remains 70% of its original capacity, while the pristine NCM811 only delivers 50% of the capacity. The stable cycling performance of GN-LPO-NCM811 is demonstrated in a full cell with graphite anode at ambient temperatures. Importantly, the thermal stability of the modified samples is also greatly enhanced. This study provides an effective method to improve the electrochemical performance of LiNi 0·8 Co 0·1 Mn 0·1 O 2 .
Optimization of Graphite–SiO blend electrodes for lithium-ion batteries: Stable cycling enabled by single-walled carbon nanotube conductive additive
Lithium-alloying materials are of great interest to improve the gravimetric and volumetric energy density of lithium-ion batteries, though their associated volume fluctuation with cycling often leads to poor cycling performance. Active-inactive alloys and blending alloys with carbon materials are common strategies to accommodate volume fluctuation. Herein we set out to optimize graphite-SiO blend electrode formulations to eliminate rapid capacity fade. Electrodes with highly stable cycling were prepared by simple planetary mixing procedures, enabled by the use of just a fraction of a weight percent of commercial SWCNTs as the only conductive additive, and by the appropriate choice of binder/stabilizing agent. In fact, the use of SWCNTs allowed for graphite-free SiO electrodes with approximately 74% higher volumetric energy density relative to traditional graphite electrodes, and superior capacity retention in coin-type full-cell testing versus NMC532 cathodes.
A new carbon-incorporated lithium phosphate solid electrolyte
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Holistic design principles for flow batteries: Cation dependent membrane resistance and active species solubility
Cation dependent resistance of a commercial cation exchange membrane, Nafion™ 212, as well as the solubility of select active materials are investigated, demonstrating practical consequences of cation choice on redox flow battery (RFB) performance. The conductivity of alkali and methyl- or -alcohol substituted ammonium cations through pretreated Nafion™ 212 reveal that cation size is the dominant factor affecting ionic transport. Among the alkali series the resistance increases with larger ionic radii and similarly, with increasing steric bulk through substitution on ammonia. The solubility of ferrocyanide, a commonly used redox flow battery posolyte (or catholyte), as well as iron, cobalt, and chromium metal-organic compounds are determined for the same series of cations. Full cells are assembled using various cation mixtures and membrane pre-treatments to demonstrate practical effects of each variable. Here, we highlight the need to carefully select the correct cations for efficient electrolyte design, since certain cations may lead to high conductivity but low solubility, or vice versa, and provide design principles for RFBs using Nafion™ 212.
Establishing substitution rules of functional groups for high-capacity organic anode materials in Na-ion batteries
Tailoring molecular structures of organic electrode materials (OEMs) can enhance their performance in Na-ion batteries, however, the substitution rules and the consequent effect on the specific capacity and working potential remain elusive. Herein, by examining three sodium carboxylates with selective N substitution or extended conjugation structure, we exploited the correlation between structure and performance to establish substitution rules for high-capacity OEMs. Our results show that substitution position and types of functional groups are essential to create active centers for uptake/removal of Na+ and thermodynamically stabilize organic structures. Furthermore, rational host design and electrolytes modulation were performed to extend the cycle life to 500 cycles. A full cell based on the optimal 2,2’-bipyridine-4,4’-dicarboxylic acid disodium salt anode and the polyaniline cathode is demonstrated to confirm the feasibility of achieving all-organic batteries. Lastly, this work provides a valuable guideline for the design principle of high-capacity and stable OEMs for sustainable energy storage.
Rechargeable metal-metal alkaline batteries: Recent advances, current issues and future research strategies
Over the past few decades, remarkable advancement has been attained in the field of rechargeable metal–metal alkaline batteries (RABs). In terms of safety, energy density, charge-discharge capacity, and long-term storage capability, metal-metal RABs (e.g., Ni–Zn, Ni–Fe, Ni–Bi, Ni–MH, Ag–Zn, Co–Zn, Cu–Zn, and Bi–Zn systems) are contemplated as the promising energy storage devices for the applications in electric vehicles (EVs), hybrid EVs, grid-scale energy storage, as well as various implantable and wearable electronic devices. Especially, Ni-MH batteries become competitive with Li-ion batteries for EVs and hybrid EVs applications due to their high tolerance against mechanical abuse, stability under wide temperature ranges, and considerable charge/discharge capacity. Meanwhile, earlier works reviewed only specific topics, so, as a rapidly growing research topic, providing a deep understanding on metal–metal RABs is timely and worthwhile. So here, in this work, we discuss the electrochemistry of all metal-metal RABs, then full cell designing with their performance will be discussed thoroughly. Further, issues associated with the existing metal–metal RABs and corresponding improvement approaches will be provided for future advances in high-performance and reliable metal-metal RABs.
Electrolyte design for Li metal-free Li batteries
Li metal, with the lowest thermodynamically achievable negative electrochemical potential and the highest specific capacity (3860 mAh g -1 ), is the ultimate anode choice for Li batteries. However, the highest reported Li plating/stripping Coulombic efficiency (CE) of 99.5% after extensive efforts is still too low for the Li metal-free (all the Li metal in cycling comes from cathode, without anode pre-lithiation) Li metal batteries. The low CE is attributed to both non-uniform Li plating/stripping on the lithiophobic Cu current collector and Li dendrite growth through lithiophilic organic–inorganic solid electrolyte interphase (SEI) formed in carbonate electrolytes. Here, we use a lithiophilic Bismuth graphite blend (Bi–Gr) substrate to replace lithiophobic Cu current collector to seed a uniform Li nucleation, and form a lithiophobic LiF-rich SEI rather than lithiophilic organic-rich SEI to suppress Li dendrite growth. Molecular dynamics simulations reveal the preferential reduction of anions in 2.0 M LiPF 6 in tetrahydrofuran/2-methyl tetrahydrofuran (2.0 M LiPF 6 –mixTHF) electrolyte to generate LiF-rich SEI on plated Li. Bi–Gr substrate and 2.0 M LiPF 6 –mixTHF electrolyte enable the Li anodes to achieve a record high CE of 99.83% at a high capacity of 1.0 mAh cm -2 and current of 0.5 mA cm -2 . The Bi particles serve as dispersed nucleation centers that promote uniform Li deposition with strong adhesion to the substrate to avoid dead Li, while the lithiophobic LiF-rich SEI promotes lateral Li growth and suppresses the vertical Li dendrite growth even at a high current density of 3.0 mA cm -2 and high areal capacities of 3.0 mAh cm -2 . The regulation of Li nucleation and growth enables the Li metal-free LiFePO 4 full cells to achieve 100 cycles at a practical areal capacity of >2.0 mAh cm -2 . This article highlights the benefits of simultaneous substrate design to improve Li nucleation and electrolyte design to promote lithiophobic SEI growth, enabling a promising and practical route Li metal-free Li metal batteries.
In-situ formation of stable interface towards Li-in anode for halide solid-state electrolyte
Halide-based solid-state electrolytes (SSEs) are promising candidates for next-generation all-solid-state lithium batteries (ASSLBs) due to their high ionic conductivity and chemical stability. However, their poor interfacial compatibility with lithium metal anode and Li-In alloy significantly hinder practical application due to the requirement for a protective interlayer. In this study, a novel approach to overcome this limitation is presented by introducing iron (Fe) doping into Li 3 InCl 6 (LIC), which enables direct and stable contact with lithium-indium (Li-In) metal without a protective interlayer. Thermodynamic and computational analyses identified Fe 3+ as a suitable dopant based on its similar reduction potential to In 3+ and structural compatibility within the halide lattice. The synthesized 10 at. % Fe-doped LIC exhibits high phase purity, retained ionic conductivity, and notably improved interfacial stability. Full-cell tests using Fe-LIC achieve over 300 cycles with 80 % capacity retention. At the same time, symmetric Li-In/ Fe-LIC/ Li-In cells sustain over 500 h of operation, representing the first reported long-term cycling of LIC-based ASSLB without a protective interlayer. In conclusion, this work establishes Fe doping as an effective strategy to stabilize halide SSEs of In system against Li-In alloy, thereby simplifying cell architecture and advancing the development of safer, high-performance halide-based solid-state electrolytes.
A highly stable host for lithium metal anode enabled by Li9Al4-Li3N-AlN structure
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Wettable carbon felt framework for high loading Li-metal composite anode
Li metal anode has received extensive attention due to its high specific capacity and low potential vs. Li/Li + for lithium batteries. However, dendrite growth, volume change and "dead" Li formation during cycling hinder its practical application. Here we report an innovated cuprite-coated carbon felt as current collector, with ultralight 3D framework and significantly improved Li-metal loading through thermal infusion. The Li-metal anode has a high Li content of 90 wt.%. The cuprite coating improves the lithiophilicity of carbon felt remarkably, due to the surface affinity reaction between cuprite and Li. Moreover, the porous carbon felt provides good electronic connection and buffer space to accommodate volume change during Li stripping/plating. It leads to uniformly distributed local current density and preference of Li stripping/plating in the highly dispersed concave areas, with suppressed formation of dendrites and “dead” Li. The Li composite electrode shows excellent cycle stability with low polarization in both symmetric and full cells. Hence, this work opens a new approach for the development of high loading Li composite anodes for advanced Li metal batteries.
NASICON-type Na 3 Fe 2 (PO 4 ) 3 as a low-cost and high-rate anode material for aqueous sodium-ion batteries
Aqueous sodium-ion batteries are attractive battery alternatives for stationary energy storage due to their inherently low cost and high safety. The development of advanced electrode materials with excellent performance and low cost is crucial for the success of aqueous Na-ion batteries. Albeit the high capacity and stable cycling of the leading anode of NaTi 2 (PO 4 ) 3 , the high price of titanium element and the low Na-insertion potential close to the hydrogen evolution reaction may plague its application. Here we introduced a NASICON-type Na 3 Fe 2 (PO 4 ) 3 as a promising anode alternative for aqueous Na-ion batteries. Synchrotron X-ray diffraction and spectroscopy confirm its phase and atomic structure. Electrochemical characterization and X-ray photoelectron spectroscopy reveal the reversible Na+ insertion in Na 3 Fe 2 (PO 4 ) 3 due to the Fe 3+ /Fe 2+ redox couple, which renders a specific capacity of ~60 mAh g -1 and excellent cycling of 1000 cycles at 10C rate. A Super high rate of 100C was also achieved for this anode with a capacity retention of 61% after 1000 cycles. In addition, the Na 3 Fe 2 (PO 4 ) 3 anode is paired with a Prussian white analogue of Na 2 Mn[Fe(CN) 6 ] into a full cell, exhibiting promising cell performance and material sustainability. Furthermore, our work underlines the importance of fabricating aqueous batteries on the basis of the Earth-abundant, cost-effective, and non-toxic elements.
Carbon-pore-sheathed cobalt nanoseeds: An exceptional and durable bifunctional catalyst for zinc-air batteries
Exceptional and durable catalysts for Zinc-air batteries are plagued by nanoparticle agglomeration. As a proof-of-concept, we designed carbon-pore-sheathed cobalt nanoseeds by loading cobalt nanoparticles into N-doped defective carbon pores. Introduced N-doping, Co-N-C bond and graphitic/graphenic carbon defects endow the catalyst with exceptional catalytic activity. Most importantly, the design of Co confined within carbon pores effectively solved the dilemma of nanomaterial stability. By balancing the high catalytic activity and stable cyclability, this unique catalyst is among the outstanding bifunctional catalysts, with a high ORR half-wave potential of 0.847 V and a low OER potential at 10 mA/cm 2 of 1.593 V. As demonstrated in the full cell, a peak power density of 135 mW/cm 2 at a current density of 200 mA/cm 2 and 450 h of stable cycling performance without fading at a current density of 30 mA/cm 2 was delivered.
The surface triple-coupling on single crystalline cathode for lithium ion batteries
Single crystalline (SC) cathode materials, which are less susceptible to micro/nano-cracks formation and offer better structure stability compared to the polycrystalline counterpart, have attained great attention. However, the parasitic side reactions at the cathode-electrolyte interface induces the loss of active species, which consequently leads to continual degradation of the electrochemical performances. Herein, a triple coupling of concentration-gradient Na+, F- co-doping and surface NaF coating are exploited for the first time on SC LiNi 0.5C o 0.2 Mn 0.3 O 2 cathode by the hydrolysis of NaPF 6 . This process regulates the external structure of materials by constructing a “sandwich” configuration from surface to bulk: rock salt - mixing zone - layered phase. The detailed interface transformation mechanism is revealed by Neutron powder diffraction (NPD), spherical aberration corrected high-resolution scanning transmission electron microscopy (HR-STEM), electron energy loss spectroscopy (EELS), and Ar+ sputtering assisted X-ray photoelectron spectroscopy (XPS). The synergistic effects endow the SC cathode with outstanding capacity retentions: 91.3% at 25 °C and 85% at 45 °C, after 500 cycles at 5 C between 3.0 and 4.5 V. In addition, a high full-cell reversible capacity of 168.9 mAh g -1 with a capacity retention of 92.4% is achieved after 300 cycles at 1 C. Multiple characterizations further indicate that these superior results are mainly ascribed to the overall structure integrity of SC material, the thin cathode electrolyte interface, high content of lithium fluoride, and the low solubility of transition metal ions. This work opens a new avenue to construct a benign interface towards high-performance lithium ion batteries.
Polyvinyl alcohol coating induced preferred crystallographic orientation in aqueous zinc battery anodes
The development of rechargeable aqueous zinc batteries is mainly hindered by the Zn anode, which suffers from dendrite growth, corrosion, hydrogen evolution, and surface passivation. Herein, a thin polyvinyl alcohol (PVA) coating layer on Zn anode has enabled dendrite-free, long-life aqueous Zn batteries by effectively regulating the interfacial ion diffusion and inducing the homogeneous Zn nucleation and deposition of stacked plates with preferentially crystallographic orientation along (002) Zn planes. The PVA@Zn anode achieved an ultralong cycle lifespan of thousands of hours at 0.25 and 1 mA cm -2 . Outstanding durability under a deep cycling capacity (5 mA h cm -2 ), high current density (10 mA cm -2 ), and long duration conditions were achieved. The superior cyclability of PVA@Zn anode was also demonstrated in PVA@Zn//V 2 O 5 full cells. In conclusion, the insights of PVA induced Zn deposition with preferred crystal orientation and interfacial regulation shed light on the future development of stable Zn anodes.
In-situ synthesis of porous metal fluoride@carbon composite via simultaneous etching/fluorination enabled superior Li storage performance
Transition metal fluorides as Li-free conversion-type cathode materials have high theoretical specific capacities, however, their preparation strategy, sluggish electrochemical kinetic and poor cyclability have impeded their wide adoption in lithium-ion batteries. Herein, a facile in-situ synthesis of porous metal-fluoride-carbon composites is accomplished via simultaneous polytetrafluorethylene-based hard template etching and metal fluorination. This not only facilitates fast electron transfer and lithium-ion diffusion kinetics, but also buffers severe volume fluctuation during lithiation/delithation and enables the formation of a uniform and thin Li 2 CO 3 /LiF-rich cathode-electrolyte interphase. Here, as a proof of concept, the as-prepared porous FeF 3 @C (p-FeF 3 @C) indeed exhibits a high specific capacity of 230 mAh g -1 at 0.1 C together with an excellent capacity retention of 92.5% at 1 C for 200-cycles. Moreover, the practicality of the strategy is demonstrated by the superb electrochemical performance of the full-cells coupled with pre-lithiated graphite anodes. Therefore, the proposed novel synthetic strategy will enlighten the future design of high-performance metal-fluoride-carbon composites with porous structure for energy storage applications.
Stable all-solid-state sodium-sulfur batteries for low-temperature operation enabled by sodium alloy anode and confined sulfur cathode
All-solid-state sodium-sulfur (Na-S) batteries are promising for stationary energy storage devices because of their low operating temperatures (less than 100 °C), improved safety, and low-cost fabrication. Using Na alloy instead of Na metal as an anode in Na-S batteries can prevent dendrite growth and improve interfacial stability between the anode and solid electrolytes to achieve long-cycling stability. A high-sulfur content cathode possessing high sulfur utilization is also important to enable an energy-dense Na-S battery. In this work, we studied Na-Sb and Na- Sn alloy anodes and demonstrated the superiority of Na 3 Sb alloy undergoing a stable Na alloying/dealloying process at 0.04 mA cm -2 for over 500 hours. Combining the optimized Na3Sb alloy anode with sulfur-carbon composites prepared by the vapor deposition approach, the full cell shows a high sulfur specific capacity and improved rate performance. Moreover, the all-solid-state Na alloy-S battery can deliver a high initial discharge specific capacity of 1377 mAh g -1 and maintain good capacity retention of 70 % after 180 cycles at 60 °C. Further, post-cycle characterizations show that both the anode and cathode perform a reversible discharge/charge process after the 1st cycle, and the cathode undergoes significantly rearranged distributions of carbon and solid-state electrolytes after 180 cycles due to severe volume change induced by repeated sodiation/desodiation process.