Engineering topics

Sun, Xiao‐Guang

Publications and source records attributed to Sun, Xiao‐Guang.

7 records

DOE OSTI2024

In Situ Cyclized Polyacrylonitrile Coating: Key to Stabilizing Porous High-Entropy Oxide Anodes for High-Performance Lithium-Ion Batteries

High-entropy oxides (HEOs) composed of multiple metal elements have attracted great attention as anode materials for lithium-ion batteries (LIBs) due to the synergistic effects of various metal species. However, the practical applications of HEOs are still plagued by poor conductivity, unstable solid electrolyte interphase (SEI) and poor cycling stability. In this work, nanosized (FeCoNiCrMn) 3 O 4 HEO (NHEO) is prepared successfully by the NaCl-assisted mechanical ball-milling strategy. Novelly, polyacrylonitrile (PAN) is used as the binder and then in situ thermochemically cyclized to construct a cyclized PAN (cPAN) outer layer onto NHEO (NHEO-cPAN). The in situ formed cPAN coating not only improves the electrical conductivity, but also reinforces the structural and interfacial stability, and thereby, the resulted NHEO-cPAN electrode exhibits significantly enhanced rate and cyclic performance. Specifically, NHEO-PAN500 electrode delivers a high reversible capacity of 560 mAh g –1 at 5 A g –1 and a high-capacity retention of 83% over 800 cycles at 3 A g –1 . Furthermore, the structural evolution and electrochemical behavior of NHEO-PAN electrode during discharge/charge is systematically investigated by operando X-ray diffraction, in situ impedance spectroscopy and ex situ high-resolution transmission electron microscopy. Therefore, this work provides new insights into the engineering of electrode and interphase for high-performance HEO electrode materials, potentially enlightening the practical applications of HEO-based LIBs.

25 ENERGY STORAGE↗

DOE OSTI2024

Multiple Functional Bonds Integrated Interphases for Long Cycle Sodium-Ion Batteries

Sodium-ion batteries (SIBs) have garnered significant interest as one of the most promising energy suppliers for power grid energy storage. However, the poor electrode/electrolyte interfacial stability leads to continual electrolyte decomposition and transition metal dissolution, resulting in rapid performance degradation of SIBs. In this work, we propose a strategy integrating multiple functional bonds to regulate electrode/electrolyte interphase by triple-coupling of succinonitrile (SN), sodium hexafluorophosphate (NaPF 6 ) and fluorinated ethylene carbonate (FEC). Theoretical calculation and experiment results show that the solvation structure of Na + and ClO 4 – is effectively reconfigured by the solvated FEC, SN and PF 6 – in PC-based carbonate electrolyte. The newly developed electrolyte demonstrates increased Na + -FEC coordination, weakened interaction of Na + -PC and participation of SN and PF 6 – anions in solvation, resulting in the formation of a conformal interfacial layer comprising of sodium oxynitrides (NaN x O y ), sodium fluoride (NaF) and phosphorus oxide compounds (NaP x O y ). Consequently, a 3 Ah pouch full cell of hard carbon//NaNi 1/3 Fe 1/3 Mn 1/3 O 2 exhibits an excellent capacity retention of 90.4 % after 1000 cycles. Detailed postmortem analysis of interface chemistry is further illustrated by multiple characterization methods. Finally, this study provides a new avenue for developing electrolyte formulations with multiple functional bonds integrated interphases to significantly improve the long-term cycling stability of SIBs.

25 ENERGY STORAGE↗

DOE OSTI2023

In Situ Ion‐Exchange Metathesis Induced Conformal LiF Surface Films on Cathode (NMC811) as a Cathode Electrolyte Interphase

High-capacity cathodes (LiNi 0.8 Mn 0.1 Co 0.1 O 2 , NMC811) are promising for vehicle electrification because of their high gravimetric energy density. However, their electrochemical performance still relies upon the stability of the cathode electrolyte interphase (CEI). A highly reactive cathode interface leads to parasitic side reactions with electrolytes, resulting in accelerated capacity fading. Well-developed LiF and LiF-like inorganic compounds are believed to be good CEI components for stabilizing such reactive electrode interfaces. However, it is challenging to form an optimal surface sub-nanolayer of LiF on the cathode surfaces because of the complexity of the electrochemical reaction during battery cycling. Herein, the formation of a conformal LiF layer on the NMC811 electrode surface via an in situ ion-exchange metathesis process is reported, demonstrating a promising electrochemical performance because of a LiF-stabilized CEI. In situ generated LiF-coated NMC811 electrodes exhibit ≈97% capacity retention up to 100 cycles at a 0.3 C rate with average coulombic efficiency of ≈99.9% and ≈80% capacity retention up to 200 cycles at a 1 C rate with average coulombic efficiency of >99.6%. This finding may pave the way for reengineering the CEI to enhance the electrochemical performances and cycling stability of the high-capacity cathodes.

25 ENERGY STORAGE↗

DOE OSTI2023

Ionothermally Synthesized Nanoporous Ti 0.95 W 0.05 Nb 2 O 7 : a Novel Anode Material for High-Performance Lithium-Ion Batteries

Although TiNb 2 O 7 is regarded as a fast-rechargeable lithium-ion battery (LIB) anode material, the intrinsic poor electrochemical kinetics of TiNb 2 O 7 still dramatically impedes its development. Herein, an ionothermal synthesis-assisted doping strategy is proposed for the preparation of a new W 6+ -doped TiNb 2 O 7 material (Ti 0.95 W 0.05 Nb 2 O 7 ) with nanoporous structure (denoted as NPTWNO). The improved Li + diffusion coefficient of NPTWNO suggests that the ionic-liquid-templated nanoporous architecture improves the Li+ diffusion kinetics. The density functional theory computational study reveals that the doped W 6+ successfully boosts the electronic conductivity due to the narrowed conduction-valance bandgap resulted from charge redistribution, which is reflected by the electrochemical impedance spectroscopy data. With the simultaneously enhanced Li+ diffusivity and electronic conductivity, NPTWNO achieves fast-rechargeability in LIBs. So this work indicates the potential of ionothermal synthesis-assisted doping strategy on energy storage materials and offers NPTWNO material with promising electrochemical performance.

25 ENERGY STORAGE↗

DOE OSTI2022

Conformal LiF Stabilized Interfaces via Electrochemical Fluorination on High Voltage Spinel Cathodes (≈4.9 V) for Lithium-Ion Batteries

The high voltage LiNi 0.5 Mn 1.5 O 4 (LNMO) spinel is one of the promising cathodes for the lithium-ion batteries due to its high energy densities, good rate performance. However, its high operating potential (≈4.75 V) causes extensive oxidation of conventional carbonate electrolytes, resulting an unstable and thick cathode electrolyte interphase (CEI) layer with a large irreversible capacity and low coulombic efficiency. In this work, we report the formation of thin LiF stabilized interfaces on LNMO via electrochemical fluorination that significantly improves the cycling stability and enhanced the capacity. An electrochemically induced conformal LiF layer acts as a part of a robust CEI by reducing the leakage of electrons and allowing the conduction of Li ions through it. Because of the robust LiF stabilized CEI, LNMO delivers a discharge capacity of ≈148.5 and ≈117.1 mAh g -1 at 0.1 and 1 C rate, respectively. It exhibits excellent cyclability with 80% capacity retention (CR) after 600 cycles in lithium-half cell and ≈90% CR after 200 cycles in full cell with only 0.03% and 0.05% capacity decay per cycle in conventional carbonate electrolytes without additives. Such an excellent electrochemical performance could lead to the potential development of high energy density batteries with high voltage cathodes for grid-based applications.

25 ENERGY STORAGE↗

DOE OSTI2021

Supramolecular Self-Assembled Multi-Electron-Acceptor Organic Molecule as High-Performance Cathode Material for Li-Ion Batteries

Organic electrode materials possess many advantages such as low toxicity, sustainability, and chemical/structural tunability toward high energy density. However, to compete with inorganic-based compounds, crucial aspects such as redox potential, capacity, cycling stability, and electronic conductivity need to be improved. Herein, a comprehensive strategy on the molecular design of small organic electron-acceptor-molecule—hexaazatrianthranylene (HATA) embedded quinone (HATAQ) is reported. By introducing conjugated quinone moieties into the electron-deficient hexaazatriphenylene-derivative core, HATAQ with highly extended π-conjugation can yield extra-high capacity for lithium storage, delivering a capacity of 426 mAh g -1 at 200 mA g -1 (0.4C). At an extremely high rate of 10 A g -1 (19C), a reversible capacity of 209 mAh g -1 corresponding to nearly 85% retention is obtained after 1000 cycles. A unique network of unconventional lock-and-key hydrogen bonds in the solid-state facilitates favorable supramolecular 2D layered arrangement, enhancing cycling stability. To the best of the authors’ knowledge, the capacity and rate capability of HATAQ are found to be the best ever reported for organic small-molecule-based cathodes. Finally, these results together with density functional theory studies provide proof-of-concept that the design strategy is promising for the development of organic electrodes with exceptionally high energy density, rate capability, and cycling stability.

25 ENERGY STORAGE↗

DOE OSTI2020

Ionic Liquid–Directed Nanoporous TiNb 2 O 7 Anodes with Superior Performance for Fast–Rechargeable Lithium–Ion Batteries

Nanoporous TiNb 2 O 7 (NPTNO) material is synthesized by a sol–gel method with an ionic liquid (IL) as the nanoporous structure directing template. NPTNO exhibits a high reversible capacity of 210 mAh g –1 even at the charging rate of 50 C and an excellent cyclability of half-cell capacity retention of 74% for 1000 cycles at 5 C and LiNi 0.5 Mn 1.5 O 4 -coupled full-cell capacity retentions of 81% and 87% for 1000 cycles at 1 C and 2 C, respectively. The studies of the 1000 cycled NPTNO electrode illustrate that the IL-directed mesoporous structure can enhance the cyclability of NPTNO cells due to the alleviation of repetitive mechanical stress and volume fluctuation induced by the repetitive Li + insertion-extraction processes. The measured Li + diffusion coefficients from the galvanostatic intermittent titration technique suggest that the IL-templating strategy indeed ensures the fast rechargeability of NPTNO cells based on the fast Li + diffusion kinetics. Benefitting from the nanoporous structure, NPTNO with unhindered Li + diffusion pathways achieves a superior rate capability in the titanium-based oxide materials and the best full-cell cyclability in the TNO materials. Furthermore, the templating potential of IL is demonstrated, and the superb electrochemical performance establishes the IL-directed NPTNO as a promising anode candidate for fast-rechargeable LIBs.

25 ENERGY STORAGE↗