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Lu, Dongping

Publications and source records attributed to Lu, Dongping.

At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Challenges for and Pathways Toward Solid-State Batteries

Solid-state batteries utilizing lithium metal anodes have the potential to enable batteries with a specific energy of >500 Wh/kg and an energy density of >1,500 Wh/L for thousands of cycles. When optimized they will improve the energy efficiency, operating temperature range, sustainability, and safety at a lower cost compared to projections for advanced Li-ion batteries. This improved performance is critical for the widespread adoption of electric vehicles and may enable future applications such as electric aviation. Expectations for solid-state batteries are high, there are significant materials and processing challenges that need to be overcome. Some of these challenges are well known; others are more subtle and are just becoming known. The challenges and their solutions must be clearly identified to realize high-energy solid-state Li metal batteries. In the United States, the U.S. Department of Energy (DOE) funds the majority of energy storage research and development, including solid state battery research. Web of Science publication analysis shows that worldwide DOE is second largest funder. Work on solid state batteries is distributed across different arms of DOE and is coordinated at headquarters to ensure a broad national portfolio for advanced batteries, including lithium batteries and solid-state battery devices. We note that university and national laboratory researchers in the US with a long-standing interest in solid state batteries is a small, integrated community with recognized impact for publications, patents and startup companies. The opportunity for this group to engage for research with international colleagues is growing, fostered by periodic bilateral meetings supported by DOE and by the recent joint US German research program for lithium battery interface studies. These are valuable opportunities to speed solid-state battery development. The ORNL led virtual workshop, overviewed here, confirms the community’s shared vision of the exciting advances, opportunities, and challenges. Further, we are seeing that this workshop has spawned several new informal collaborations and draft proposals. This encourages us to propose future discussion. On May 11, 2020, Oak Ridge National Laboratory (ORNL) hosted a 6-hour, on-line national workshop to discuss recent advances and most the prominent obstacles to realizing solid-state Li metal batteries. The workshop included more than 30+ experts from national laboratories, universities, and companies, all of whom have worked on solid-state batteries for multiple years. The participants shared recent advances, many not yet in print, illustrating that the community has gained significant new insights for solid-state Li battery materials over the last 5 years. In this report, the major outcomes of the workshop are organized to identify the gaps in our scientific knowledge for four core materials science areas: (1) Li metal anodes, (2) the solid electrolyte in contact with Li metal, (3) active cathode materials and solid-state composite cathodes, and (4) solid electrolytes. Illustrative examples and discussions are reported with the more comprehensive issues in the report. Discussion of additional challenges related to processing of solid-state battery materials and to the designs and architectures for mechanically robust, long-lived batteries received less attention due to time constraints. These are good themes for deeper discussion at a follow-on workshop, where a complete list of critical research topics can be identified.

25 ENERGY STORAGE↗
DOE OSTI2020

A lithium-sulfur battery with a solution-mediated pathway operating under lean electrolyte conditions

Lithium-sulfur (Li-S) battery is one of the most promising candidates for the next generation energy storage systems. However, several barriers, including polysulfide shuttle effect, the slow solid-solid surface reaction pathway in the lower discharge plateau, and corrosion of Li anode still limit its practical applications, especially under the lean electrolyte condition required for high energy density applications. Here, we propose a solution-mediated sulfur reduction pathway to improve the capacity and reversibility of the sulfur cathode and suppress dendrite growth on the Li metal anode simultaneously. With this method, a high coulombic efficiency (99%) and stable cycle life over 100 cycles were achieved under application-relevant conditions (S loading: 6.2 mg cm-2; electrolyte to sulfur ratio: 3 mLE gs-1; sulfur weigh ratio: 72 wt%). This result is enabled by a specially designed Li2S4-rich electrolyte, in which Li2S is formed through a chemical disproportionation reaction instead of electrochemical routes. A diglyme solvent was used to obtain electrolytes with the optimum range of Li2S4 concentration. Operando X-ray absorption spectroscopy confirms the solution pathway in a practical Li-S cell. This solution pathway not only introduces a new electrolyte regime for practical Li-S batteries, but also provides a new perspective for bypassing the inefficient surface pathway for other electrochemical processes.

Wang, Hui↗
DOE OSTI2020

Reaction heterogeneity in practical high-energy lithium–sulfur pouch cells

The lithium–sulfur (Li–S) battery is a promising next-generation energy storage technology because of its high theoretical energy and low cost. Extensive research efforts have been made on new materials and advanced characterization techniques for mechanistic studies. However, it is uncertain how discoveries made on the material level apply to realistic batteries due to limited analysis and characterization of real high-energy cells, such as pouch cells. Evaluation of pouch cells (>1 A h) (instead of coin cells) that are scalable to practical cells provides a critical understanding of current limitations which enables the proposal of strategies and solutions for further performance improvement. Herein, we design and fabricate pouch cells over 300 W h kg -1 , compare the cell parameters required for high-energy pouch cells, and investigate the reaction processes and their correlation to cell cycling behavior and failure mechanisms. Spatially resolved characterization techniques and fluid-flow simulation reveal the impacts of the liquid electrolyte diffusion within the pouch cells. We found that catastrophic failure of high-energy Li–S pouch cells results from uneven sulfur/polysulfide reactions and electrolyte depletion for the first tens of cycles, rather than sulfur dissolution as commonly reported in the literature. The uneven reaction stems from limited electrolyte diffusion through the porous channels into the central part of thick cathodes during cycling, which is amplified both across the sulfur electrodes and within the same electrode plane. A combination of strategies is suggested to increase sulfur utilization, improve nanoarchitectures for electrolyte diffusion and reduce consumption of the electrolytes and additives.

25 ENERGY STORAGE↗
DOE OSTI2019

Cathode porosity is a missing key parameter to optimize lithium-sulfur battery energy density

While high sulfur loading has been pursued as a key parameter to build realistic high-energy lithium-sulfur batteries, less attention has been paid to the cathode porosity, which is much higher in sulfur/carbon composite cathodes than in traditional lithium-ion battery electrodes. For high-energy lithium-sulfur batteries, a dense electrode with low porosity is desired to minimize electrolyte intake, parasitic weight, and cost. Here we report the profound impact on the discharge polarization, reversible capacity, and cell cycling life of lithium-sulfur batteries by decreasing cathode porosities from 70 to 40%. According to the developed mechanism-based analytical model, we demonstrate that sulfur utilization is limited by the solubility of lithium-polysulfides and further conversion from lithium-polysulfides to Li2S is limited by the electronically accessible surface area of the carbon matrix. Finally, we predict an optimized cathode porosity to maximize the cell level volumetric energy density without sacrificing the sulfur utilization.

25 ENERGY STORAGE↗
DOE OSTI2019

Superionic Conduction and Interfacial Properties of the Low Temperature Phase Li7P2S8Br0.5I0.5

Sulfide-based solid electrolytes are pursued for their application in bulk-type all-solid-state lithium batteries. Although the usefulness of Li10GeP2S12-type materials have been demonstrated in all-solid-state cathodes, a suitable material with both high ionic conductivity and good interfacial properties with common anode materials is still lacking. In this work, we explore the phase and transport properties of mechanically-milled Li7P2S8Br0.5I0.5, with emphasis on the favorable kinetics at Li metal anode. The low temperature crystalline phase Li7P2S8Br0.5I0.5 (LT-LPSBI) has exceptionally high ionic conductivity of 4.7 mS/cm at room temperature. Moreover, the LT-LPSBI supports long-term Li cycling at 0.5 mA cm-2 with low and stable interfacial resistance (5 O cm2). Transport phenomenon of Li/LT-LPSBI interface and cycling behavior of Li symmetric cells are studied and discussed in detail.

Wang, Yuxing↗
DOE OSTI2018

Enabling High-Energy-Density Cathode for Lithium-Sulfur Batteries

High-loading sulfur electrode is critical for high energy Lithium-sulfur (Li-S) batteries used for practical applications. Unfortunately, dense and high-loading sulfur electrodes usually suffer from low sulfur utilization rate and limited cycle life. In this work, effects of electrode porosity on the electrode energy density, cell cycling stability, Li anode interface, and electrolyte/sulfur ratio were systematically investigated using high loading sulfur electrodes. The reduced electrode porosity increases volumetric energy density but also hinders electrode wetting process. To solve this problem, polysulfide (Li2S6) is selected as an electrolyte additive to enhance electrolyte penetration into dense sulfur cathodes. As a result, a high energy density of 1300 Wh L-1 (at electrode level) has been obtained for a dense sulfur cathode with a sulfur loading of 4 mg cm-2 at a compressed thickness of 60 µm. Li-S batteries with dense electrodes and Li2S6 additive also demonstrate promising cycling stability (~80 % capacity retention for 200 cycles). These significant improvements are contributed by synergistic effects of the dense sulfur cathode, improved electrolyte penetration, and suppressed growth of passivation layer on Li metal anode. This study sheds light on rational sulfur cathode structure design as well as control of electrode porosity for balanced energy density and cycling life.

Lu, Dongping↗
DOE OSTI2018

Minimizing Polysulfide Shuttle Effect in Lithium-Ion Sulfur Batteries by Anode Surface Passivation

Lithium-ion sulfur batteries use non-metal materials as the anode to address safety concerns associated with lithium metal anode. However, polysulfide shuttle reactions still occur on the non-metal anode (such as graphite and Si), and result in limited battery efficiency. In this work, we used Al2O3 layers coated by atomic layer deposition (ALD) technique to suppress the shuttle reactions. With the optimal thickness of 2 nm Al2O3 coated on graphite anode, the Coulombic efficiency of the sulfur cathode was improved from 84% to 96% in the first cycle, and from 94% to 97% in the subsequent cycles. As a result, the discharge capacity of the sulfur cathode was increased to 550 mAh g-1 in the 100th cycle, as compared with 440 mAh g-1 when the pristine graphite anode was used. The Al2O3 passivation layer minimizes the formation of insoluble polysulfide (Li2S2, Li2S) on the surface of graphite anode and improves the efficiency and capacity retention of the graphite-sulfur batteries. The surface passivation strategy could also be used in other Li sulfur battery systems (with Li, Si, and Sn anodes), to minimize side reactions and enable high-performance and safe sulfur batteries.

Liu, Jian↗
DOE OSTI2018

Tailored Reaction Route by Micropore Confinement for Li–S Batteries Operating under Lean Electrolyte Conditions

Abstract Lithium‐sulfur (Li–S) batteries are one of the most promising alternative energy storage systems beyond Li‐ion batteries. However, the sluggish kinetics of the nucleation and growth of the solid discharge product of Li 2 S/Li 2 S 2 in the lower discharge plateau has been recently identified as a critical hurdle for attaining high specific capacity in Li–S batteries with high sulfur loadings under lean electrolyte conditions. Herein, a new strategy of breaking the charge‐transport bottleneck by successful generation of experimentally verified stable Li 2 S 2 and a reservoir of quasi‐solid lithium polysulfides within the micropores of activated carbon fiber cloth as a high‐sulfur‐loading host is proposed. The developed Li–S cell is capable of delivering a highly sustainable areal capacity of 6.0 mAh cm −2 under lower electrolyte to sulfur ratios (<3.0 mL E g S −1 ). Micropore confinement leads to generation of solid Li 2 S 2 that enables high utilization of the entire electroactive area by its inherent self‐healing capacity. This strategy opens a new avenue for rational material designs for Li–S batteries under lean electrolyte condition.

Wang, Hui↗
DOE OSTI2018

Mechanism of Formation of Li 7 P 3 S 11 Solid Electrolytes through Liquid Phase Synthesis

Crystalline Li7P3S11 is a promising solid electrolyte for all solid state lithium/lithium ion batteries. A controllable liquid phase synthesis of Li7P3S11 is more desirable compared to conventional mechanochemical synthesis, but recent attempts suffer from reduced ionic conductivities. Here we elucidate the formation mechanism of crystalline Li7P3S11 synthesized in the liquid phase (acetonitrile, or ACN). We conclude that the crystalline Li7P3S11 forms through a two-step reaction: 1) formation of solid Li3PS4∙ACN and amorphous Li2S∙P2S5 phases in the liquid phase; 2) solid-state conversion of the two phases. The implication of this two-step reaction mechanism to the morphology control and the transport properties of liquid phase synthesized Li7P3S11 is identified and discussed.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2018

Characterization of the oxidative protein folding activity of a unique plant oxidoreductase, Arabidopsis protein disulfide isomerase-11

Highlights: • AtPDI11 is a unique protein disulfide isomerase that has no ortholog in animals or yeast. • AtPDI11 has oxidoreductase activity in vitro that is much lower than hPDI. • The active site in the a' domain of AtPDI11 is critical for its oxidative folding activity. • AtPDI11 is present in four redox forms in vivo, which are determined by the active site cysteines. • AtPDI11 is required for plant growth under reducing conditions. Protein disulfide isomerases (PDIs) can catalyze disulfide bond formation in nascent secretory proteins and membrane proteins and can introduce correct disulfide bonds into substrate proteins containing mispaired disulfides. The functions of mammalian PDIs have been extensively studied; however, relative to mammalian PDIs, the systematic characterization of PDIs for their oxidoreductase activity in plants is still lacking. Arabidopsis protein disulfide isomerases-11 (AtPDI11), with the structure of a-a'-D, has no ortholog in animals or yeast. In this study, we demonstrated that AtPDI11 has oxidoreductase activity in vitro using a GSSG/GSH-mediated oxidative protein folding system. Moreover, the active site in the a' domain of AtPDI11 is critical for its oxidative folding activity. AtPDI11 is present in four redox forms in vivo, which are determined by the active site cysteines (Cys52 and Cys55 in the a domain, and Cys171 and Cys174 in the a' domain). Genetic evidence suggests that AtPDI11 is required for plant growth under reducing conditions. Our work provides an example for studying the oxidoreductase function of other plant PDIs.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2018

Enhanced Cyclability of Lithium-Oxygen Batteries with Electrodes Protected by Surface Films Induced via In Situ Electrochemical Process

Although the rechargeable lithium-oxygen (Li-O2) batteries have extremely high theoretical specific energy, the practical application of these batteries is still limited by the instability of their carbon-based air-electrode, Li metal anode, and electrolytes towards reduced oxygen species. Here we demonstrate a simple one-step in-situ electrochemical pre-charging strategy to generate thin protective films on both carbon nanotubes (CNTs) air-electrode and Li metal anode simultaneously under an inert atmosphere. Li-O2 cells after such pre-treatment demonstrate significantly extended cycle life of 110 and 180 cycles under the capacity-limited protocol of 1000 mAh g-1 and 500 mAh g-1, respectively, which is far more than those without pre-treatment. The thin-films formed from decomposition of electrolyte during in-situ electrochemical pre-charging process in an inert environment can protect both CNTs air-electrode and Li metal anode prior to conventional Li-O2 discharge/charge cycling where reactive reduced oxygen species are formed. This work provides a new approach for protections of carbon-based air-electrode and Li metal anode in practical Li-O2 batteries, and may also be applied to other battery systems.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2017

Li + -Desolvation Dictating Lithium-Ion Battery’s Low-Temperature Performances

Lithium (Li) ion battery (LIB) has penetrated almost every aspects of human life, from portable electronics, vehicles to grids, and its operation stability in extreme environments becomes increasingly important. Among these, sub-zero temperature presents a kinetic challenge to the electrochemical reactions required to deliver the stored energy. In this work, we attempted to identify the rate-determining process for Li+ migration under such low temperatures, so that an optimum electrolyte formulation could be designed to maximize the energy output. Substantial increase in available capacities from graphite||LiNi0.80Co0.15Al0.05O2 chemistry down to -40°C is achieved by reducing the solvent molecule that more tightly binds to Li+ and thus constitutes high desolvation energy barrier. The fundamental understanding is applicable universally to all electrochemical devices that have to operate in similar environments.

desolvation↗
DOE OSTI2017

Electrolyte for batteries with regenerative solid electrolyte interface

An energy storage device comprising: an anode; and a solute-containing electrolyte composition wherein the solute concentration in the electrolyte composition is sufficiently high to form a regenerative solid electrolyte interface layer on a surface of the anode only during charging of the energy storage device, wherein the regenerative layer comprises at least one solute or solvated solute from the electrolyte composition.

25 ENERGY STORAGE↗
DOE OSTI2017

Thick electrodes including nanoparticles having electroactive materials and methods of making same

Electrodes having nanostructure and/or utilizing nanoparticles of active materials and having high mass loadings of the active materials can be made to be physically robust and free of cracks and pinholes. The electrodes include nanoparticles having electroactive material, which nanoparticles are aggregated with carbon into larger secondary particles. The secondary particles can be bound with a binder to form the electrode.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Lithium compensation for full cell operation

Disclosed herein are embodiments of a lithium-ion battery system comprising an anode, an anode current collector, and a layer of lithium metal in contact with the current collector, but not in contact with the anode. The lithium compensation layer dissolves into the electrolyte to compensate for the loss of lithium ions during usage of the full cell. The specific placement of the lithium compensation layer, such that there is no direct physical contact between the lithium compensation layer and the anode, provides certain advantages.

25 ENERGY STORAGE↗
DOE OSTI2015

High Energy Density Lithium-Sulfur Batteries: Challenges of Thick Sulfur Cathodes

High energy and cost-effective lithium sulfur (Li-S) battery technology has been vigorously revisited in recent years due to the urgent need of advanced energy storage technologies for transportation and large-scale energy storage applications. However, the market penetration of Li-S batteries has been plagued due to the gap in scientific knowledge between the fundamental research and the real application need. Herein, we focus on the cathode part of the Li-S system and discuss 1) the progress and issues of literature-reported sulfur cathode; 2) how to employ materials chemistry/science to address the challenges to thicken sulfur cathode; 3) the factors that affect the electrochemical performances of Li-S cells constructed at a relevant scale. This progress report attempts to tie the fundamental understanding closely to the practical application of Li-S batteries so that it may provide new insights for the research efforts of Li-S battery technology.

anodes↗