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Li, Weihan

Publications and source records attributed to Li, Weihan.

15 records
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DOE OSTI2025

Chemical Bond Covalency in Superionic Halide Solid‐State Electrolytes

Abstract Halide solid‐state electrolytes (SSEs) are promising superionic conductors with high oxidative stability and ionic conductivity, making them attractive for all‐solid‐state lithium‐ion batteries. However, most studies have focused on ion‐stacking structures, overlooking the role of bond characteristics in ionic transport. Here, we investigate bond dynamics and the superionic transition (SIT) in bromide electrolyte, Li 3 InBr 6 , using synchrotron X‐ray techniques and ab initio molecular dynamics (AIMD) simulations. We demonstrate that the SIT in halide SSEs is driven by a thermally induced transition in bonding character (ionic to covalent) rather than a change in crystal phase. AIMD simulations further reveal enhanced Li⁺ diffusion and collective anion motion at elevated temperatures. Expanding our study to Li 3 LnBr 6 (Ln = Gd, Tb, Ho, Tm, and Lu), we confirm the widespread occurrence of SIT in this material class, with Li 3 GdBr 6 exhibiting the highest ionic conductivity (5.2 mS cm −1 at 298 K). More importantly, the ionic‐covalent transition is highly tunable through electrolyte modifications, such as cation/anion substitution and synthesis methods. Our findings provide a new perspective on ionic transport, highlighting the critical role of chemical bond characteristics in halide SSEs.

Chemistry↗
DOE OSTI2024

Superionic conducting vacancy-rich β-Li 3 N electrolyte for stable cycling of all-solid-state lithium metal batteries

The advancement of all-solid-state lithium metal batteries requires breakthroughs in solid-state electrolytes (SSEs) for the suppression of lithium dendrite growth at high current densities and high capacities (>3 mAh cm -2 ) and innovation of SSEs in terms of crystal structure, ionic conductivity and rigidness. Here we report a superionic conducting, highly lithium-compatible and air-stable vacancy-rich β-Li 3 N SSE. This vacancy-rich β-Li 3 N SSE shows a high ionic conductivity of 2.14 × 10 -3 S cm -1 at 25 °C and surpasses almost all the reported nitride-based SSEs. A Li- and N-vacancy-mediated fast lithium-ion migration mechanism is unravelled regarding vacancy-triggered reduced activation energy and increased mobile lithium-ion population. All-solid-state lithium symmetric cells using vacancy-rich β-Li 3 N achieve breakthroughs in high critical current densities up to 45 mA cm -2 and high capacities up to 7.5 mAh cm -2 , and ultra-stable lithium stripping and plating processes over 2,000 cycles. The high lithium compatibility mechanism of vacancy-rich β-Li 3 N is unveiled as intrinsic stability to lithium metal. In addition, β-Li 3 N possesses excellent air stability through the formation of protection surfaces. All-solid-state lithium metal batteries using the vacancy-rich β-Li 3 N as SSE interlayers and lithium cobalt oxide (LCO) and Ni-rich LiNi 0.83 Co 0.11 Mn 0.06 O 2 (NCM83) cathodes exhibit excellent battery performance. Extremely stable cycling performance is demonstrated with high capacity retentions of 82.05% with 95.2 mAh g -1 over 5,000 cycles at 1.0 C for LCO and 92.5% with 153.6 mAh g -1 over 3,500 cycles at 1.0 C for NCM83. Utilizing the vacancy-rich β-Li 3 N SSE and NCM83 cathodes, the all-solid-state lithium metal batteries successfully accomplished mild rapid charge and discharge rates up to 5.0 C, retaining 60.47% of the capacity. Notably, these batteries exhibited a high areal capacity, registering approximately 5.0 mAh cm -2 for the compact pellet-type cells and around 2.2 mAh cm -2 for the all-solid-state lithium metal pouch cells.

25 ENERGY STORAGE↗
DOE OSTI2024

A family of dual-anion-based sodium superionic conductors for all-solid-state sodium-ion batteries

The sodium (Na) superionic conductor is a key component that could revolutionize the energy density and safety of conventional Na-ion batteries. However, existing Na superionic conductors are primarily based on a single-anion framework, each presenting inherent advantages and disadvantages. Here we introduce a family of amorphous Na-ion conductors (Na 2 O 2 –MCl y , M = Hf, Zr and Ta) based on the dual-anion framework of oxychloride. Benefiting from a dual-anion chemistry and with the resulting distinctive structures, Na 2 O 2 –MCl y electrolytes exhibit room-temperature ionic conductivities up to 2.0 mS cm -1 , wide electrochemical stability windows and desirable mechanical properties. All-solid-state Na-ion batteries incorporating amorphous Na 2 O 2 –HfCl 4 electrolyte and a Na 0.85 Mn 0.5 Ni 0.4 Fe 0.1 O 2 cathode exhibit a superior rate capability and long-term cycle stability, with 78% capacity retention after 700 cycles under 0.2 C (1C = 120 mA g -1 ) at room temperature. The discoveries in this work could trigger a new wave of enthusiasm for exploring new superionic conductors beyond those based on a single-anion framework.

25 ENERGY STORAGE↗
DOE OSTI2023

A Dual Anion Chemistry-Based Superionic Glass Enabling Long-Cycling All-Solid-State Sodium-Ion Batteries

Glassy Na-ion solid-state electrolytes (GNSSEs) are an important group of amorphous SSEs. However, the insufficient ionic conductivity of state-of-the-art GNSSEs at room temperature lessens their promise in the development of all-solid-state Na-ion batteries (ASSNIBs) with high energy density and improved safety. Here we report the discovery of a new sodium superionic glass, 0.5Na 2 O 2 -TaCl 5 (NTOC), based on dual-anion sublattice of oxychlorides. The unique local structures with abundant bridging and non-bridging oxygen atoms contributes to a highly disordered Na-ion distribution as well as low Na + migration barrier within NTOC, enabling an ultrahigh ionic conductivity of 4.62 mS cm −1 at 25 °C (more than 20 times higher than those of previously reported GNSSEs). Moreover, the excellent formability of glassy NTOC electrolyte and its high electrochemical oxidative stability ensure a favourable electrolyte-electrode interface, contributing to superior cycling stability of ASSNIBs for over 500 cycles at room temperature. The discovery of glassy NTOC electrolyte would reignite research enthusiasm in superionic glassy SSEs based on multi-anion chemistry.

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

Precise Tailoring of Lithium-Ion Transport for Ultralong-Cycling Dendrite-Free All-Solid-State Lithium Metal Batteries

All-solid-state lithium metal batteries can address crucial challenges regarding insufficient battery cycling life and energy density. The demonstration of long-cycling dendrite-free all-solid-state lithium metal batteries requires precise tailoring of lithium-ion transport of solid-state electrolytes (SSEs). Here, in this work, a proof of concept is reported for precise tailoring of lithium-ion transport of a halide SSE, Li 3 InCl 6 , including intragranular (within grains) but also intergranular (between grains) lithium-ion transport. Lithium-ion migration tailoring mechanism in crystals is developed by unexpected enhanced Li, In, and Cl vacancy populations and lower energy barrier for hopping. The lithium-ion transport tailoring mechanism between the grains is determined by the elimination of voids between grains and the formation of unexpected supersonic conducting grain boundaries, boosting the lithium dendrite suppression ability of SSE. Due to boosted lithium-ion conduction and dendrite-suppression ability, the all-solid-state lithium metal batteries coupled with Ni-rich LiNi 0.83 Co 0.12 Mn 0.05 O 2 cathodes and lithium metal anodes demonstrate breakthroughs in electrochemical performance by achieving extremely long cycling life at a high current density of 0.5 C (2000 cycles, 93.7% capacity retention). This concept of precise tailoring of lithium-ion transport provides a cost, time, and energy efficient solution to conquer the remaining challenges in all-solid-state lithium-metal batteries for fast developing electric vehicle markets.

25 ENERGY STORAGE↗
DOE OSTI2023

Lithium-compatible and air-stable vacancy-rich Li 9 N 2 Cl 3 for high–areal capacity, long-cycling all–solid-state lithium metal batteries

Attaining substantial areal capacity (>3 mAh/cm 2 ) and extended cycle longevity in all–solid-state lithium metal batteries necessitates the implementation of solid-state electrolytes (SSEs) capable of withstanding elevated critical current densities and capacities. In this study, we report a high-performing vacancy-rich Li 9 N 2 Cl 3 SSE demonstrating excellent lithium compatibility and atmospheric stability and enabling high–areal capacity, long-lasting all–solid-state lithium metal batteries. The Li 9 N 2 Cl 3 facilitates efficient lithium-ion transport due to its disordered lattice structure and presence of vacancies. Notably, it resists dendrite formation at 10 mA/cm 2 and 10 mAh/cm 2 due to its intrinsic lithium metal stability. Furthermore, it exhibits robust dry-air stability. Incorporating this SSE in Ni-rich LiNi 0.83 Co 0.11 Mn 0.06 O 2 cathode-based all–solid-state batteries, we achieve substantial cycling stability (90.35% capacity retention over 1500 cycles at 0.5 C) and high areal capacity (4.8 mAh/cm 2 in pouch cells). These findings pave the way for lithium metal batteries to meet electric vehicle performance demands.

25 ENERGY STORAGE↗
DOE OSTI2022

Forecasting battery capacity and power degradation with multi-task learning

Lithium-ion batteries degrade due to usage and exposure to environmental conditions, which affects their capability to store energy and supply power. Accurately predicting the capacity and power fade of lithium-ion battery cells is challenging due to intrinsic manufacturing variances and coupled nonlinear ageing mechanisms. In this paper, we propose a data-driven prognostics framework to predict both capacity and power fade simultaneously with multi-task learning. The model is able to predict the degradation trajectory of both capacity and internal resistance together with knee-points and end-of-life points accurately at early-life stage. The validation shows an average percentage error of 2.37% and 1.24% for the prediction of capacity fade and resistance rise, respectively. The model's ability to accurately predict the degradation, facing capacity and resistance estimation errors, further demonstrates the model's robustness and generalizability. Compared with single-task learning models for forecasting capacity and power degradation, the model shows a significant prediction accuracy improvement and computational cost reduction. This work presents the highlights of multi-task learning in the degradation prognostics for lithium-ion batteries.

25 ENERGY STORAGE↗
DOE OSTI2021

A general strategy for preparing pyrrolic-N 4 type single-atom catalysts via pre-located isolated atoms

Single-atom catalysts (SACs) have been applied in many fields due to their superior catalytic performance. Because of the unique properties of the single-atom-site, using the single atoms as catalysts to synthesize SACs is promising. In this work, we have successfully achieved Co 1 SAC using Pt 1 atoms as catalysts. More importantly, this synthesis strategy can be extended to achieve Fe and Ni SACs as well. X-ray absorption spectroscopy (XAS) results demonstrate that the achieved Fe, Co, and Ni SACs are in a M1-pyrrolic N 4 (M= Fe, Co, and Ni) structure. Density functional theory (DFT) studies show that the Co(Cp) 2 dissociation is enhanced by Pt 1 atoms, thus leading to the formation of Co 1 atoms instead of nanoparticles. These SACs are also evaluated under hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), and the nature of active sites under HER are unveiled by the operando XAS studies. These new findings extend the application fields of SACs to catalytic fabrication methodology, which is promising for the rational design of advanced SACs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

A Minimal Information Set To Enable Verifiable Theoretical Battery Research

Batteries are an enabling technology for addressing sustainability through the electrification of various forms of transportation (1) and grid storage. (2) Batteries are truly multi-scale, multi-physics devices, and accordingly various theoretical descriptions exist to understand their behavior (3-5) ranging from atomistic details to techno-economic trends. As we explore advanced battery chemistries (6,7) or previously inaccessible aspects of existing ones, (8-10) new theories are required to drive decisions. (11-13) The decisions are influenced by the limitations of the underlying theory. Advanced theories used to understand battery phenomena are complicated and require substantial effort to reproduce. However, such constraints should not limit the insights from these theories. We can strive to make the theoretical research verifiable such that any battery stakeholder can assess the veracity of new theories, sophisticated simulations or elaborate analyses. We distinguish verifiability, which amounts to “Can I trust the results, conclusions and insights and identify the context where they are relevant?”, from reproducibility, which ensures “Would I get the same results if I followed the same steps?” With this motivation, we propose a checklist to guide future reports of theoretical battery research in Table 1. We hereafter discuss our thoughts leading to this and how it helps to consistently document necessary details while allowing complete freedom for creativity of individual researchers. Given the differences between experimental and theoretical studies, the proposed checklist differs from its experimental counterparts. (14,15) This checklist covers all flavors of theoretical battery research, ranging from atomic/molecular calculations (16-19) to mesoscale (20,21) and continuum-scale interactions, (9,22) and techno-economic analysis. (23,24) Finally, as more and more experimental studies analyze raw data, (25) we feel this checklist would be broadly relevant.

25 ENERGY STORAGE↗
DOE OSTI2021

New Insights into the High‐Performance Black Phosphorus Anode for Lithium‐Ion Batteries

Abstract Black phosphorus (BP) is a promising anode material in lithium‐ion batteries (LIBs) owing to its high electrical conductivity and capacity. However, the huge volume change of BP during cycling induces rapid capacity fading. In addition, the unclear electrochemical mechanism of BP hinders the development of rational designs and preparation of high‐performance BP‐based anodes. Here, a high‐performance nanostructured BP–graphite–carbon nanotubes composite (BP/G/CNTs) synthesized using ball‐milling method is reported. The BP/G/CNTs anode delivers a high initial capacity of 1375 mA h g −1 at 0.15 A g −1 and maintains 1031.7 mA h g −1 after 450 cycles. Excellent high‐rate performance is demonstrated with a capacity of 508.1 mA h g −1 after 3000 cycles at 2 A g −1 . Moreover, for the first time, direct evidence is provided experimentally to present the electrochemical mechanism of BP anodes with three‐step lithiation and delithiation using ex situ X‐ray diffraction (XRD), ex situ X‐ray absorption spectroscopy (XAS), ex situ X‐ray emission spectroscopy, operando XRD, and operando XAS, which reveal the formation of Li 3 P 7 , LiP, and Li 3 P. Furthermore, the study indicates an open‐circuit relaxation effect of the electrode with ex situ and operando XAS analyses.

Li, Minsi↗
DOE OSTI2021

ENPOLITE: Comparing Lithium-Ion Cells across Energy, Power, Lifetime, and Temperature

Due to their impressive energy density, power density, lifetime, and cost, lithium-ion batteries have become the most important electrochemical storage system, with applications including consumer electronics, electric vehicles, and stationary energy storage. However, each application has unique, often conflicting product specifications, requiring a balanced overall assessment. The Ragone plot is a commonly-used plot to compare energy and power of lithium-ion battery chemistries. Important parameters including cost, lifetime, and temperature sensitivity are not considered. Overall, a standardized and balanced reporting and visualization of specifications would greatly help an informed cell selection process.

25 ENERGY STORAGE↗
DOE OSTI2020

Stabilizing and understanding the interface between nickel-rich cathode and PEO-based electrolyte by lithium niobium oxide coating for high-performance all-solid-state batteries

The pursuit of high energy density and safe lithium ion batteries (LIBs) is the urgent goal for the development of next-generation electric vehicles (EVs). All-solid-state batteries (ASSBs) with the combination of poly(ethylene oxide) (PEO)-based solid polymer electrolyte (SPE) and Ni-rich lithium nickel manganese cobalt oxide LiNi0.8Mn0.1Co0.1O2 (NMC811) cathode are promising candidates for EVs due to their improved energy density and safety. However, the low electrochemical oxidation window of PEO-based SPE and the instability of NMC811 at the charge/discharge process seriously restrict the battery performance. Herein, a high voltage stable solid-state electrolyte layer lithium niobium oxide (LNO) is coated on the NMC811 electrode surface by atomic layer deposition for stabilizing NMC811-PEO solid polymer batteries. Electrochemical tests show that LNO coating can stabilize the NMC811 active materials and mitigate the decomposition of SPE upon the cycling process, rendering a good performance of NMC811-PEO solid polymer battery. Mechanism studies by SEM, STEM, XAS, and XPS disclose that the uncoated NMC811 suffers from chemomechanical degradations along with oxygen release triggering the decomposition of SPE, which results in unstable cathodic electrolyte interphase. With LNO coating, chemomechanical degradations and oxygen release are inhibited and the decomposition of SPE is mitigated. This paper renders a stable and high-performance high-energy-density SSB for high voltage application, which paves the way toward next-generation solid-state LIBs.

25 ENERGY STORAGE↗