Yusheng Ye

All Publications

• Revealing the Multifunctions of Li3N in the Suspension Electrolyte for Lithium Metal Batteries. ACS nano Kim, M. S., Zhang, Z., Wang, J., Oyakhire, S. T., Kim, S. C., Yu, Z., Chen, Y., Boyle, D. T., Ye, Y., Huang, Z., Zhang, W., Xu, R., Sayavong, P., Bent, S. F., Qin, J., Bao, Z., Cui, Y. 2023

  Abstract

  Inorganic-rich solid-electrolyte interphases (SEIs) on Li metal anodes improve the electrochemical performance of Li metal batteries (LMBs). Therefore, a fundamental understanding of the roles played by essential inorganic compounds in SEIs is critical to realizing and developing high-performance LMBs. Among the prevalent SEI inorganic compounds observed for Li metal anodes, Li3N is often found in the SEIs of high-performance LMBs. Herein, we elucidate new features of Li3N by utilizing a suspension electrolyte design that contributes to the improved electrochemical performance of the Li metal anode. Through empirical and computational studies, we show that Li3N guides Li electrodeposition along its surface, creates a weakly solvating environment by decreasing Li+-solvent coordination, induces organic-poor SEI on the Li metal anode, and facilitates Li+ transport in the electrolyte. Importantly, recognizing specific roles of SEI inorganics for Li metal anodes can serve as one of the rational guidelines to design and optimize SEIs through electrolyte engineering for LMBs.

  View details for DOI 10.1021/acsnano.2c12470

  View details for PubMedID 36700841

• Onboard early detection and mitigation of lithium plating in fast-charging batteries. Nature communications Huang, W., Ye, Y., Chen, H., Vilá, R. A., Xiang, A., Wang, H., Liu, F., Yu, Z., Xu, J., Zhang, Z., Xu, R., Wu, Y., Chou, L. Y., Wang, H., Xu, J., Boyle, D. T., Li, Y., Cui, Y. 2022; 13 (1): 7091

  Abstract

  Fast-charging is considered as one of the most desired features needed for lithium-ion batteries to accelerate the mainstream adoption of electric vehicles. However, current battery charging protocols mainly consist of conservative rate steps to avoid potential hazardous lithium plating and its associated parasitic reactions. A highly sensitive onboard detection method could enable battery fast-charging without reaching the lithium plating regime. Here, we demonstrate a novel differential pressure sensing method to precisely detect the lithium plating event. By measuring the real-time change of cell pressure per unit of charge (dP/dQ) and comparing it with the threshold defined by the maximum of dP/dQ during lithium-ion intercalation into the negative electrode, the onset of lithium plating before its extensive growth can be detected with high precision. In addition, we show that by integrating this differential pressure sensing into the battery management system (BMS), a dynamic self-regulated charging protocol can be realized to effectively extinguish the lithium plating triggered by low temperature (0 °C) while the conventional static charging protocol leads to catastrophic lithium plating at the same condition. We propose that differential pressure sensing could serve as an early nondestructive diagnosis method to guide the development of fast-charging battery technologies.

  View details for DOI 10.1038/s41467-022-33486-4

  View details for PubMedID 36402759

• Fast-Charging of Hybrid Lithium-Ion/Lithium-Metal Anodes by Nanostructured Hard Carbon Host ACS ENERGY LETTERS Gong, H., Chen, Y., Chen, S., Xu, C., Yang, Y., Ye, Y., Huang, Z., Ning, R., Cui, Y., Bao, Z. 2022; 7 (12): 4417-4426

  View details for DOI 10.1021/acsenergylett.2c02130

  View details for Web of Science ID 000898367800001

• Integrated Three-dimensional Hydrophilicity/hydrophobicity Design for Artificial Sweating Skin (i-TRANS) Mimicking Human Body Perspiration. Advanced materials (Deerfield Beach, Fla.) Peng, Y., Zhou, J., Yang, Y., Lai, J., Ye, Y., Cui, Y. 2022: e2204168

  Abstract

  Artificial skins reproducing properties of human skin are emerging and significant for study in various areas, such as robotics, medicine, textiles, etc. Perspiration, as one of the most imperative thermoregulation functions of human skin, is gaining increasing attention, but how to realize ideal artificial skin for perspiration simulation remains challenging. Here, we propose an integrated three-dimensional hydrophilicity/hydrophobicity design for artificial sweating skin (i-TRANS). Based on normal fibrous wicking materials, the selective surface modification with gradient of Polydimethylsiloxane (PDMS) creates hydrophilicity/hydrophobicity contrast in both lateral and vertical directions. With the additional help of bottom hydrophilic Nylon 6 nanofibers, the constructed i-TRANS is able to transport "sweat" directionally without trapping undesired excess water and attain uniform "secretion" of sweat droplets on the top surface, decently mimicking human skin perspiration situation. This fairly comparable simulation not only presents new insights for replicating skin properties, but also provides proper in vitro testing platforms for perspiration-relevant research, greatly avoiding unwanted interference from the "skin" layer. In addition, the facile, fast and cost-effective fabrication approach and versatile usage of i-TRANS can further facilitate its application. This article is protected by copyright. All rights reserved.

  View details for DOI 10.1002/adma.202204168

  View details for PubMedID 35975584

• Electrical resistance of the current collector controls lithium morphology. Nature communications Oyakhire, S. T., Zhang, W., Shin, A., Xu, R., Boyle, D. T., Yu, Z., Ye, Y., Yang, Y., Raiford, J. A., Huang, W., Schneider, J. R., Cui, Y., Bent, S. F. 2022; 13 (1): 3986

  Abstract

  The electrodeposition of low surface area lithium is critical to successful adoption of lithium metal batteries. Here, we discover the dependence of lithium metal morphology on electrical resistance of substrates, enabling us to design an alternative strategy for controlling lithium morphology and improving electrochemical performance. By modifying the current collector with atomic layer deposited conductive (ZnO, SnO2) and resistive (Al2O3) nanofilms, we show that conductive films promote the formation of high surface area lithium deposits, whereas highly resistive films promote the formation of lithium clusters of low surface area. We reveal an electrodeposition mechanism in which radial diffusion of electroactive species is promoted on resistive substrates, resulting in lateral growth of large (150m in diameter) planar lithium deposits. Using resistive substrates, similar lithium morphologies are formed in three distinct classes of electrolytes, resulting in up to ten-fold improvement in battery performance. Ultimately, we report anode-free pouch cells using the Al2O3-modified copper that maintain 60 % of their initial discharge capacity after 100 cycles, displaying the benefits of resistive substrates for controlling lithium electrodeposition.

  View details for DOI 10.1038/s41467-022-31507-w

  View details for PubMedID 35821247

• Cold-Starting All-Solid-State Batteries from Room Temperature by Thermally Modulated Current Collector in Sub-Minute. Advanced materials (Deerfield Beach, Fla.) Ye, Y., Huang, W., Xu, R., Xiao, X., Zhang, W., Chen, H., Wan, J., Liu, F., Lee, H. K., Xu, J., Zhang, Z., Peng, Y., Wang, H., Gao, X., Wu, Y., Zhou, G., Cui, Y. 2022: e2202848

  Abstract

  All-solid-state batteries (ASSBs) show great potential as high-energy and high-power energy storage devices but their attainable energy/power density at room temperature is severely reduced because of the sluggish kinetics of lithium-ion transport. Here we first reported a thermally modulated current collector (TMCC), which can rapidly cold-start ASSBs from room temperature to operating temperatures (70∼90 °C) in less than one minute, and simultaneously enhance the transient peak power density by 15-fold compared to one without heating. This TMCC is prepared by integrating a uniform, ultrathin (∼200 nm) nickel layer as a thermal modulator within an ultralight polymer-based current collector. By isolating the thermal modulator from the ion/electron pathway of ASSBs, it can provide fast, stable heat control yet does not interfere with regular battery operation. Moreover, this ultrathin (13.2 μm) TMCC effectively shortens the heat transfer pathway, minimizes heat losses, and mitigates the formation of local hot spots. The simulated heating energy consumption can be as low as ∼3.94% of total battery energy. This TMCC design with good tunability opens new frontiers towards smart energy storage devices in the future from the current collector perspective. This article is protected by copyright. All rights reserved.

  View details for DOI 10.1002/adma.202202848

  View details for PubMedID 35762033

• Heat Conductor-Insulator Transition in Electrochemically Controlled Hybrid Superlattices. Nano letters Zhou, J., Wu, Y., Kwon, H., Li, Y., Xiao, X., Ye, Y., Ma, Y., Goodson, K. E., Hwang, H. Y., Cui, Y. 2022

  Abstract

  Designing materials with ultralow thermal conductivity has broad technological impact, from thermal protection to energy harvesting. Low thermal conductivity is commonly observed in anharmonic and strongly disordered materials, yet a microscopic understanding of the correlation to atomic motion is often lacking. Here we report that molecular insertion into an existing two-dimensional layered lattice structure creates a hybrid superlattice with extremely low thermal conductivity. Vibrational characterization and ab initio molecular dynamics simulations reveal strong damping of transverse acoustic waves and significant softening of longitudinal vibrations. Together with spectral correlation analysis, we demonstrate that the molecular insertion creates liquid-like atomic motion in the existing lattice framework, causing a large suppression of heat conduction. The hybrid materials can be transformed into solution-processable coatings and used for thermal protection in wearable electronics. Our work provides a generic mechanism for the design of heat insulators and may further facilitate the engineering of heat conduction based on understanding atomic correlations.

  View details for DOI 10.1021/acs.nanolett.2c01407

  View details for PubMedID 35715219

• Scalable, Ultrathin, and High-Temperature-Resistant Solid Polymer Electrolytes for Energy-Dense Lithium Metal Batteries ADVANCED ENERGY MATERIALS Ma, Y., Wan, J., Yang, Y., Ye, Y., Xiao, X., Boyle, D. T., Burke, W., Huang, Z., Chen, H., Cui, Y., Yu, Z., Oyakhire, S. T. 2022

  View details for DOI 10.1002/aenm.202103720

  View details for Web of Science ID 000760882000001

• Capturing the swelling of solid-electrolyte interphase in lithium metal batteries. Science (New York, N.Y.) Zhang, Z., Li, Y., Xu, R., Zhou, W., Li, Y., Oyakhire, S. T., Wu, Y., Xu, J., Wang, H., Yu, Z., Boyle, D. T., Huang, W., Ye, Y., Chen, H., Wan, J., Bao, Z., Chiu, W., Cui, Y. 1800; 375 (6576): 66-70

  Abstract

  [Figure: see text].

  View details for DOI 10.1126/science.abi8703

  View details for PubMedID 34990230

• Coloured low-emissivity films for building envelopes for year-round energy savings NATURE SUSTAINABILITY Peng, Y., Fan, L., Jin, W., Ye, Y., Huang, Z., Zhai, S., Luo, X., Ma, Y., Tang, J., Zhou, J., Greenburg, L. C., Majumdar, A., Fan, S., Cui, Y. 2021

  View details for DOI 10.1038/s41893-021-00836-x

  View details for Web of Science ID 000734146900002

• Dynamic spatial progression of isolated lithium during battery operations. Nature Liu, F., Xu, R., Wu, Y., Boyle, D. T., Yang, A., Xu, J., Zhu, Y., Ye, Y., Yu, Z., Zhang, Z., Xiao, X., Huang, W., Wang, H., Chen, H., Cui, Y. 1800; 600 (7890): 659-663

  Abstract

  The increasing demand for next-generation energy storage systems necessitates the development of high-performance lithium batteries1-3. Unfortunately, current Li anodes exhibit rapid capacity decay and a short cycle life4-6, owing to the continuous generation of solid electrolyte interface7,8 and isolated Li (i-Li)9-11. The formation of i-Li during the nonuniform dissolution of Li dendrites12 leads to a substantial capacity loss in lithium batteries under most testing conditions13. Because i-Li loses electrical connection with the current collector, it has been considered electrochemically inactive or 'dead' in batteries14,15. Contradicting this commonly accepted presumption, here we show that i-Li is highly responsive to battery operations, owing to its dynamic polarization to the electric field in the electrolyte. Simultaneous Li deposition and dissolution occurs on two ends of the i-Li, leading to its spatial progression toward the cathode (anode) during charge (discharge). Revealed by our simulation results, the progression rate of i-Li is mainly affected by its length, orientation and the applied current density. Moreover, we successfully demonstrate the recovery of i-Li in Cu-Li cells with >100% Coulombic efficiency and realize LiNi0.5Mn0.3Co0.2O2 (NMC)-Li full cells with extended cycle life.

  View details for DOI 10.1038/s41586-021-04168-w

  View details for PubMedID 34937896

• Endoplasmic-reticulum-like catalyst coating on separator to enhance polysulfides conversion for lithium-sulfur batteries JOURNAL OF ENERGY CHEMISTRY Xu, S., Zhao, T., Wang, L., Huang, Y., Ye, Y., Zhang, N., Feng, T., Li, L., Wu, F., Chen, R. 2022; 67: 423-431

  View details for DOI 10.1016/j.jechem.2021.09.036

  View details for Web of Science ID 000725681900004

• All-Solid-State Lithium-Sulfur Batteries Enhanced by Redox Mediators. Journal of the American Chemical Society Gao, X., Zheng, X., Tsao, Y., Zhang, P., Xiao, X., Ye, Y., Li, J., Yang, Y., Xu, R., Bao, Z., Cui, Y. 2021

  Abstract

  Redox mediators (RMs) play a vital role in some liquid electrolyte-based electrochemical energy storage systems. However, the concept of redox mediator in solid-state batteries remains unexplored. Here, we selected a group of RM candidates and investigated their behaviors and roles in all-solid-state lithium-sulfur batteries (ASSLSBs). The soluble-type quinone-based RM (AQT) shows the most favorable redox potential and the best redox reversibility that functions well for lithium sulfide (Li2S) oxidation in solid polymer electrolytes. Accordingly, Li2S cathodes with AQT RMs present a significantly reduced energy barrier (average oxidation potential of 2.4 V) during initial charging at 0.1 C at 60 °C and the following discharge capacity of 1133 mAh gs-1. Using operando sulfur K-edge X-ray absorption spectroscopy, we directly tracked the sulfur speciation in ASSLSBs and proved that the solid-polysulfide-solid reaction of Li2S cathodes with RMs facilitated Li2S oxidation. In contrast, for bare Li2S cathodes, the solid-solid Li2S-sulfur direct conversion in the first charge cycle results in a high energy barrier for activation (charge to 4 V) and low sulfur utilization. The Li2S@AQT cell demonstrates superior cycling stability (average Coulombic efficiency 98.9% for 150 cycles) and rate capability owing to the effective AQT-enhanced Li-S reaction kinetics. This work reveals the evolution of sulfur species in ASSLSBs and realizes the fast Li-S reaction kinetics by designing an effective sulfur speciation pathway.

  View details for DOI 10.1021/jacs.1c07754

  View details for PubMedID 34677957

• A Morphologically Stable Li/Electrolyte Interface for All-Solid-State Batteries Enabled by 3D-Micropatterned Garnet. Advanced materials (Deerfield Beach, Fla.) Xu, R., Liu, F., Ye, Y., Chen, H., Yang, R. R., Ma, Y., Huang, W., Wan, J., Cui, Y. 2021: e2104009

  Abstract

  Morphological degradation at the Li/solid-state electrolyte (SSE) interface is a prevalent issue causing performance fading of all-solid-state batteries (ASSBs). To maintain the interfacial integrity, most ASSBs are operated under low current density with considerable stack pressure, which significantly limits their widespread usage. Herein, a novel 3D-micropatterned SSE (3D-SSE) that can stabilize the morphology of the Li/SSE interface even under relatively high current density and limited stack pressure is reported. Under the pressure of 1.0MPa, the Li symmetric cell using a garnet-type 3D-SSE fabricated by laser machining shows a high critical current density of 0.7mA cm-2 and stable cycling over 500 h under 0.5mA cm-2 . This excellent performance is attributed to the reduced local current density and amplified mechanical stress at the Li/3D-SSE interface. These two effects can benefit the flux balance between Li stripping and creep at the interface, thereby preventing interfacial degradation such as void formation and dendrite growth.

  View details for DOI 10.1002/adma.202104009

  View details for PubMedID 34632638

• An Antipulverization and High-Continuity Lithium Metal Anode for High-Energy Lithium Batteries ADVANCED MATERIALS Ye, Y., Zhao, Y., Zhao, T., Xu, S., Xu, Z., Qian, J., Wang, L., Xing, Y., Wei, L., Li, Y., Wang, J., Li, L., Wu, F., Chen, R. 2021; 33 (49): e2105029

  Abstract

  Lithium metal is one of the most promising anode candidates for next-generation high-energy batteries. Nevertheless, lithium pulverization and associated loss of electrical contact remain significant challenges. Here, an antipulverization and high-continuity lithium metal anode comprising a small number of solid-state electrolyte (SSE) nanoparticles as conformal/sacrificial fillers and a copper (Cu) foil as the supporting current collector is reported. Guiding by the SSE, this new anode facilitates lithium nucleation, contributing to form a roundly shaped, micro-sized, and dendrite-free electrode during cycling, which effectively mitigates the lithium dendrite growth. The embedded Cu current collector in the hybrid anode not only reinforces the mechanical strength but also improves the efficient charge transfer among active lithium filaments, affording good electrode structural integrity and electrical continuity. As a result, this antipulverization and high-continuity lithium anode delivers a high average Coulombic efficiency of ≈99.6% for 300 cycles under a current density of 1 mA cm-2 . Lithium-sulfur batteries (elemental sulfur or sulfurized polyacrylonitrile cathodes) equipped with this anode show high-capacity retentions in their corresponding ether-based or carbonate-based electrolytes, respectively. This new electrode provides important insight into the design of electrodes that may experience large volume variation during operations.

  View details for DOI 10.1002/adma.202105029

  View details for Web of Science ID 000704908900001

  View details for PubMedID 34624162

• From Flower-Like to Spherical Deposition: A GCNT Aerogel Scaffold for Fast-Charging Lithium Metal Batteries ADVANCED ENERGY MATERIALS Yang, T., Li, L., Zhao, T., Ye, Y., Ye, Z., Xu, S., Wu, F., Chen, R. 2021; 11 (42)

  View details for DOI 10.1002/aenm.202102454

  View details for Web of Science ID 000705603000001

• Cation- deficient Zn-0.3(NH4)(0.3)V4O10 center dot 0.91H(2)O for rechargeable aqueous zinc battery with superior low- temperature performance ENERGY STORAGE MATERIALS He, T., Weng, S., Ye, Y., Cheng, J., Wang, X., Wang, X., Wang, B. 2021; 38: 389-396

  View details for DOI 10.1016/j.ensm.2021.03.025

  View details for Web of Science ID 000672723100011

• Sensitive, portable heavy-metal-ion detection by the sulfidation method on a superhydrophobic concentrator (SPOT) ONE EARTH Lee, H., Huang, W., Ye, Y., Xu, J., Peng, Y., Wu, T., Yang, A., Chou, L., Xiao, X., Gao, X., Liu, F., Wang, H., Liu, B., Wang, J., Cui, Y. 2021; 4 (5): 756-766

  View details for DOI 10.1016/j.oneear.2021.04.009

  View details for Web of Science ID 000655035700022

• Oxygen-deficient ammonium vanadate for flexible aqueous zinc batteries with high energy density and rate capability at-30 degrees C MATERIALS TODAY He, T., Ye, Y., Li, H., Weng, S., Zhang, Q., Li, M., Liu, T., Cheng, J., Wang, X., Lu, J., Wang, B. 2021; 43: 53-61

  View details for DOI 10.1016/j.mattod.2020.11.019

  View details for Web of Science ID 000639468500014

• Electrolyte-Resistant Dual Materials for the Synergistic Safety Enhancement of Lithium-Ion Batteries. Nano letters Chou, L., Ye, Y., Lee, H. K., Huang, W., Xu, R., Gao, X., Chen, R., Wu, F., Tsung, C., Cui, Y. 2021

  Abstract

  Safety issues associated with lithium-ion batteries are of major concern, especially with the ever-growing demand for higher-energy-density storage devices. Although flame retardants (FRs) added to electrolytes can reduce fire hazards, large amounts of FRs are required and they severely deteriorate battery performance. Here, we report a feasible method to balance flame retardancy and electrochemical performance by coating an electrolyte-insoluble FR on commercial battery separators. By integrating dual materials via a two-pronged mechanism, the quantity of FR required could be limited to an ultrathin coating layer (4 mum) that rarely influences electrochemical performance. The developed composite separator has a four-times better flame retardancy than conventional polyolefin separators in full pouch cells. Additionally, this separator can be fabricated easily on a large scale for industrial applications. High-energy-density batteries (2 Ah) were assembled to demonstrate the scaling of the composite separator and to confirm its enhanced safety through nail penetration tests.

  View details for DOI 10.1021/acs.nanolett.0c04568

  View details for PubMedID 33596654

• Underpotential lithium plating on graphite anodes caused by temperature heterogeneity. Proceedings of the National Academy of Sciences of the United States of America Wang, H., Zhu, Y., Kim, S. C., Pei, A., Li, Y., Boyle, D. T., Wang, H., Zhang, Z., Ye, Y., Huang, W., Liu, Y., Xu, J., Li, J., Liu, F., Cui, Y. 2020

  Abstract

  Rechargeability and operational safety of commercial lithium (Li)-ion batteries demand further improvement. Plating of metallic Li on graphite anodes is a critical reason for Li-ion battery capacity decay and short circuit. It is generally believed that Li plating is caused by the slow kinetics of graphite intercalation, but in this paper, we demonstrate that thermodynamics also serves a crucial role. We show that a nonuniform temperature distribution within the battery can make local plating of Li above 0 V vs. Li0/Li+ (room temperature) thermodynamically favorable. This phenomenon is caused by temperature-dependent shifts of the equilibrium potential of Li0/Li+ Supported by simulation results, we confirm the likelihood of this failure mechanism during commercial Li-ion battery operation, including both slow and fast charging conditions. This work furthers the understanding of nonuniform Li plating and will inspire future studies to prolong the cycling lifetime of Li-ion batteries.

  View details for DOI 10.1073/pnas.2009221117

  View details for PubMedID 33168752

• Ultralight and fire-extinguishing current collectors for high-energy and high-safety lithium-ion batteries NATURE ENERGY Ye, Y., Chou, L., Liu, Y., Wang, H., Lee, H., Huang, W., Wan, J., Liu, K., Zhou, G., Yang, Y., Yang, A., Xiao, X., Gao, X., Boyle, D., Chen, H., Zhang, W., Kim, S., Cui, Y. 2020; 5 (10): 786–93

  View details for DOI 10.1038/s41560-020-00702-8

  View details for Web of Science ID 000578091500012

• Incorporating the nanoscale encapsulation concept from liquid electrolytes into solid-state lithium-sulfur batteries. Nano letters Gao, X., Zheng, X., Wang, J., Zhang, Z., Xiao, X., Wan, J., Ye, Y., Chou, L., Lee, H. K., Wang, J., Vila, R. A., Yang, Y., Zhang, P., Wang, L., Cui, Y. 2020

  Abstract

  Lithium-sulfur (Li-S) batteries are attractive due to their high specific energy and low-cost prospect. Most studies in the past decade are based on these batteries with liquid electrolytes, where many exciting material/structural designs are realized at the nanoscale to address problems of Li-S chemistry. Recently, there is a new promising direction to develop Li-S batteries with solid polymer electrolytes, although it is unclear whether the concepts from liquid electrolytes are applicable in the solid state to improve battery performance. Here we demonstrate that the nanoscale encapsulation concept based on Li2S-TiS2 core-shell particles, originally developed in liquid electrolytes, is very effective in solid polymer electrolytes. Using in situ optical cell measurement and sulfur K-edge X-ray absorption near edge spectroscopy, we find that polysulfides form and are well trapped inside individual particles by the nanoscale TiS2 encapsulation. This TiS2 encapsulation layer also functions to catalyze the oxidation reaction of Li2S to sulfur, even in solid-state electrolytes, proved by both experiments and density functional theory calculations. A high cell-level specific energy of 427 W∙h∙kg-1 at 60 °C (including the mass of the anode, cathode, and solid-state electrolyte, but excluding the current collector and packaging) is achieved by integrating TiS2 encapsulated Li2S cathode with ultrathin polyethylene oxide-based solid polymer electrolyte (10~20 m) and lithium metal anode. The solid-state cells show excellent stability over 150 charge/discharge cycles at 0.8 C at 80 °C. This study points to the fruitful direction of borrowing concepts from liquid electrolytes into solid-state Li-S batteries.

  View details for DOI 10.1021/acs.nanolett.0c02033

  View details for PubMedID 32515973

• Electrode Design with Integration of High Tortuosity and Sulfur-Philicity for High-Performance Lithium-Sulfur Battery MATTER Chen, H., Zhou, G., Boyle, D., Wan, J., Wang, H., Lin, D., Mackanic, D., Zhang, Z., Kim, S., Lee, H., Wang, H., Huang, W., Ye, Y., Cui, Y. 2020; 2 (6): 1605–20

  View details for DOI 10.1016/j.matt.2020.04.011

  View details for Web of Science ID 000539230500004

• Supercooled liquid sulfur maintained in three-dimensional current collector for high-performance Li-S batteries. Science advances Zhou, G., Yang, A., Gao, G., Yu, X., Xu, J., Liu, C., Ye, Y., Pei, A., Wu, Y., Peng, Y., Li, Y., Liang, Z., Liu, K., Wang, L. W., Cui, Y. 2020; 6 (21)

  Abstract

  In lithium-sulfur (Li-S) chemistry, the electrically/ionically insulating nature of sulfur and Li2S leads to sluggish electron/ion transfer kinetics for sulfur species conversion. Sulfur and Li2S are recognized as solid at room temperature, and solid-liquid phase transitions are the limiting steps in Li-S batteries. Here, we visualize the distinct sulfur growth behaviors on Al, carbon, Ni current collectors and demonstrate that (i) liquid sulfur generated on Ni provides higher reversible capacity, faster kinetics, and better cycling life compared to solid sulfur; and (ii) Ni facilitates the phase transition (e.g., Li2S decomposition). Accordingly, light-weight, 3D Ni-based current collector is designed to control the deposition and catalytic conversion of sulfur species toward high-performance Li-S batteries. This work provides insights on the critical role of the current collector in determining the physical state of sulfur and elucidates the correlation between sulfur state and battery performance, which will advance electrode designs in high-energy Li-S batteries.

  View details for DOI 10.1126/sciadv.aay5098

  View details for PubMedID 32937326

• Lifting the energy density of lithium ion batteries using graphite film current collectors JOURNAL OF POWER SOURCES Wu, Q., Yang, J., Zhao, Y., Song, R., Wang, Z., Huang, Z., Shi, M., Ye, Y., He, D., Mu, S. 2020; 455

  View details for DOI 10.1016/j.jpowsour.2020.227991

  View details for Web of Science ID 000523640000025

• A Fireproof, Lightweight, Polymer-Polymer Solid-State Electrolyte for Safe Lithium Batteries. Nano letters Cui, Y., Wan, J., Ye, Y., Liu, K., Chou, L., Cui, Y. 2020

  Abstract

  Safety issues in lithium-ion batteries have raised serious concerns due to their ubiquitous utilization and close contact with the human body. Replacing flammable liquid electrolytes, solid-state electrolytes (SSEs) is thought to address this issue as well as provide unmatched energy densities in Li-based batteries. However, among the most intensively studied SSEs, polymeric solid electrolyte and polymer/ceramic composites are usually flammable, leaving the safety issue unattended. Here, we report the first design of a fireproof, ultralightweight polymer-polymer SSE. The SSE is composed of a porous mechanic enforcer (polyimide, PI), a fire-retardant additive (decabromodiphenyl ethane, DBDPE), and a ionic conductivepolymer electrolyte (poly(ethylene oxide)/lithium bis(trifluoromethanesulfonyl)imide). The whole SSE is made from organic materials, with a thin, tunable thickness (10-25 mum), which endorse the energy density comparable to conventional separator/liquid electrolytes. The PI/DBDPE film is thermally stable, nonflammable, and mechanically strong, preventing Li-Li symmetrical cells from short-circuiting after more than 300 h of cycling. LiFePO4/Li half cells with our SSE show a high rate performance (131 mAh g-1 at 1 C) as well as cycling performance (300 cycles at C/2 rate) at 60 °C. Most intriguingly, pouch cells made with our polymer-polymer SSE still functioned well even under flame abuse tests.

  View details for DOI 10.1021/acs.nanolett.9b04815

  View details for PubMedID 32020809

• Highly Dispersed Cobalt Clusters in Nitrogen-Doped Porous Carbon Enable Multiple Effects for High-Performance Li-S Battery ADVANCED ENERGY MATERIALS Wang, R., Yang, J., Chen, X., Zhao, Y., Zhao, W., Qian, G., Li, S., Xiao, Y., Chen, H., Ye, Y., Zhou, G., Pan, F. 2020

  View details for DOI 10.1002/aenm.201903550

  View details for Web of Science ID 000510196200001

• Theoretical Calculation Guided Design of Single-Atom Catalysts toward Fast Kinetic and Long-Life Li-S Batteries. Nano letters Zhou, G. n., Zhao, S. n., Wang, T. n., Yang, S. Z., Johannessen, B. n., Chen, H. n., Liu, C. n., Ye, Y. n., Wu, Y. n., Peng, Y. n., Liu, C. n., Jiang, S. P., Zhang, Q. n., Cui, Y. n. 2020

  Abstract

  Lithium-sulfur (Li-S) batteries are promising next-generation energy storage technologies due to their high theoretical energy density, environmental friendliness, and low cost. However, low conductivity of sulfur species, dissolution of polysulfides, poor conversion from sulfur reduction, and lithium sulfide (Li2S) oxidation reactions during discharge-charge processes hinder their practical applications. Herein, under the guidance of density functional theory calculations, we have successfully synthesized large-scale single atom vanadium catalysts seeded on graphene to achieve high sulfur content (80 wt % sulfur), fast kinetic (a capacity of 645 mAh g-1 at 3 C rate), and long-life Li-S batteries. Both forward (sulfur reduction) and reverse reactions (Li2S oxidation) are significantly improved by the single atom catalysts. This finding is confirmed by experimental results and consistent with theoretical calculations. The ability of single metal atoms to effectively trap the dissolved lithium polysulfides (LiPSs) and catalytically convert the LiPSs/Li2S during cycling significantly improved sulfur utilization, rate capability, and cycling life. Our work demonstrates an efficient design pathway for single atom catalysts and provides solutions for the development of high energy/power density Li-S batteries.

  View details for DOI 10.1021/acs.nanolett.9b04719

  View details for PubMedID 31887051

• Supercooled liquid sulfur maintained in three-dimensional current collector for high-performance Li-S batteries. Science advances Zhou, G. n., Yang, A. n., Gao, G. n., Yu, X. n., Xu, J. n., Liu, C. n., Ye, Y. n., Pei, A. n., Wu, Y. n., Peng, Y. n., Li, Y. n., Liang, Z. n., Liu, K. n., Wang, L. W., Cui, Y. n. 2020; 6 (21): eaay5098

  Abstract

  In lithium-sulfur (Li-S) chemistry, the electrically/ionically insulating nature of sulfur and Li2S leads to sluggish electron/ion transfer kinetics for sulfur species conversion. Sulfur and Li2S are recognized as solid at room temperature, and solid-liquid phase transitions are the limiting steps in Li-S batteries. Here, we visualize the distinct sulfur growth behaviors on Al, carbon, Ni current collectors and demonstrate that (i) liquid sulfur generated on Ni provides higher reversible capacity, faster kinetics, and better cycling life compared to solid sulfur; and (ii) Ni facilitates the phase transition (e.g., Li2S decomposition). Accordingly, light-weight, 3D Ni-based current collector is designed to control the deposition and catalytic conversion of sulfur species toward high-performance Li-S batteries. This work provides insights on the critical role of the current collector in determining the physical state of sulfur and elucidates the correlation between sulfur state and battery performance, which will advance electrode designs in high-energy Li-S batteries.

  View details for DOI 10.1126/sciadv.aay5098

  View details for PubMedID 32494732

  View details for PubMedCentralID PMC7244266

• Development and Challenges of Functional Electrolytes for High-Performance Lithium-Sulfur Batteries ADVANCED FUNCTIONAL MATERIALS Wang, L., Ye, Y., Chen, N., Huang, Y., Li, L., Wu, F., Chen, R. 2018; 28 (38)

  View details for DOI 10.1002/adfm.201800919

  View details for Web of Science ID 000444672000016

• Flexible, conductive, and highly pressure-sensitive graphene-polyimide foam for pressure sensor application COMPOSITES SCIENCE AND TECHNOLOGY Yang, J., Ye, Y., Li, X., Lu, X., Chen, R. 2018; 164: 187–94

  View details for DOI 10.1016/j.compscitech.2018.05.044

  View details for Web of Science ID 000440121700023

• Designing Realizable and Scalable Techniques for Practical Lithium Sulfur Batteries: A Perspective JOURNAL OF PHYSICAL CHEMISTRY LETTERS Ye, Y., Wu, F., Xu, S., Qu, W., Li, L., Chen, R. 2018; 9 (6): 1398–1414

  Abstract

  To progress from the coin lithium sulfur (Li-S) cell to practical applications, it would be necessary to investigate industrially scalable methods to produce high-quality and large quantities of Li-S configurations. In this Perspective, we focused on the feasibility of scalable production of high-quality and large quantities of cathode composite, the construction of highly safe and highly stable electrolyte, and durable lithium metal anode. The results presented here suggest that the construction of highly secondary microstructures from nanoparticles is the key solution to achieve scalable cathode composite. Developing unconventional electrolyte solvent is a meaningful approach to develop high safety Li-S batteries. The high performance and high stability of lithium metal anode will enlighten the practical application of Li-S batteries. This Perspective presents outlooks for the key scalable techniques of realizable Li-S cell in the near future and provides promising strategies to accomplish long-cycle-life, high-energy-density Li-S batteries.

  View details for DOI 10.1021/acs.jpclett.7b03165

  View details for Web of Science ID 000427910200037

  View details for PubMedID 29480724

• Toward Practical High-Energy Batteries: A Modular-Assembled Oval-Like Carbon Microstructure for Thick Sulfur Electrodes ADVANCED MATERIALS Ye, Y., Wu, F., Liu, Y., Zhao, T., Qian, J., Xing, Y., Li, W., Huang, J., Li, L., Huang, Q., Bai, X., Chen, R. 2017; 29 (48)

  Abstract

  The modular assembly of microstructures from simple nanoparticles offers a powerful strategy for creating materials with new functionalities. Such microstructures have unique physicochemical properties originating from confinement effects. Here, the modular assembly of scattered ketjen black nanoparticles into an oval-like microstructure via double "Fischer esterification," which is a form of surface engineering used to fine-tune the materials surface characteristics, is presented. After carbonization, the oval-like carbon microstructure shows promise as a candidate sulfur host for the fabrication of thick sulfur electrodes. Indeed, a specific discharge capacity of 8.417 mAh cm-2 at 0.1 C with a high sulfur loading of 8.9 mg cm-2 is obtained. The large-scale production of advanced lithium-sulfur battery pouch cells with an energy density of 460.08 Wh kg-1 @18.6 Ah is also reported. This work provides a radically different approach for tuning the performance of a variety of surfaces for energy storage materials and biological applications by reconfiguring nanoparticles into desired structures.

  View details for DOI 10.1002/adma.201700598

  View details for Web of Science ID 000418272000018

  View details for PubMedID 28429541

• A Praline-Like Flexible Interlayer with Highly Mounted Polysulfide Anchors for Lithium-Sulfur Batteries SMALL Zhao, T., Ye, Y., Lao, C., Divitini, G., Coxon, P. R., Peng, X., He, X., Kim, H., Xi, K., Ducati, C., Chen, R., Liu, Y., Ramakrishna, S., Kumar, R. 2017; 13 (40)

  Abstract

  The development of lithium-sulfur (Li-S) batteries is dogged by the rapid capacity decay arising from polysulfide dissolution and diffusion in organic electrolytes. To solve this critical issue, a praline-like flexible interlayer consisting of high-loading titanium oxide (TiO2 ) nanoparticles and relatively long carbon nanofibers is fabricated. TiO2 nanoparticles with a size gradient occupy both the external and internal of carbon fiber and serve as anchors that allow the chemical adsorption of polysulfides through a conductive nanoarchitecture. The porous conductive carbon backbone helps in the physical absorption of polysulfides and provides redox reaction sites to allow the polysulfides to be reused. More importantly, it offers enough mechanical strength to support a high load TiO2 nanoparticle (79 wt%) that maximizes their chemical role, and can accommodate the large volume changes. Significant enhancement in cycle stability and rate capability is achieved for a readily available sulfur/multi-walled carbon nanotube composite cathode simply by incorporating this hierarchically nanostructured interlayer. The design and synthesis of interlayers by in situ integration of metal oxides and carbon fibers via a simple route offers the potential to advance Li-S batteries for practical applications in the future.

  View details for DOI 10.1002/smll.201700357

  View details for Web of Science ID 000413416400001

  View details for PubMedID 28834268

• Sulfur Nanodots Stitched in 2D "Bubble-Like" Interconnected Carbon Fabric as Reversibility-Enhanced Cathodes for Lithium-Sulfur Batteries ACS NANO Wu, F., Ye, Y., Huang, J., Zhao, T., Qian, J., Zhao, Y., Li, L., Wei, L., Luo, R., Huang, Y., Xing, Y., Chen, R. 2017; 11 (5): 4694–4702

  Abstract

  The behavior of two-dimensional (2D) materials for energy storage systems relates to their morphology and physicochemical properties. Although various 2D materials can be found in different fields, the open access of these materials has greatly hampered their practical applications, such as in lithium-sulfur (Li-S) batteries, where the soluble intermediates should be controlled. Here, we have developed a facile approach to prepare 2D ultrathin interconnected carbon fabrics (ICFs) with "bubble-like" morphology and abundant mesopores using a "blowing bubble" method. Serving as independent meso-sized rooms, nanosulfur dots can be stitched in 2D "bubble-like" ICF, which afford a short electron-/ion-transfer path and thus is beneficial to high reversible capacity. Encapsulated with reduced graphene oxide, a binder-free/free-standing cathode was constructed for advanced Li-S batteries. In addition, the specific energy of a pouch Li-S battery with this interconnected cathode can be achieved to 1.55 Ah@315.98 Wh/kg at 0.1 C. These results suggest that the design of "bubble-like" interconnected porous carbon fabrics and their integration with reduced graphene oxide provide a facile strategy to enhance the electrochemical activity of S and have the potential to be applied to other semiconductors or insulating materials for a wide range of applications.

  View details for DOI 10.1021/acsnano.7b00596

  View details for Web of Science ID 000402498400034

  View details for PubMedID 28448119

• Gluing Carbon Black and Sulfur at Nanoscale: A Polydopamine-Based "Nano-Binder" for Double-Shelled Sulfur Cathodes ADVANCED ENERGY MATERIALS Wu, F., Ye, Y., Chen, R., Zhao, T., Qian, J., Zhang, X., Li, L., Huang, Q., Bai, X., Cui, Y. 2017; 7 (3)

  View details for DOI 10.1002/aenm.201601591

  View details for Web of Science ID 000394940100013

• Advanced Lithium-Sulfur Batteries Enabled by a Bio-Inspired Polysulfide Adsorptive Brush ADVANCED FUNCTIONAL MATERIALS Zhao, T., Ye, Y., Peng, X., Divitini, G., Kim, H., Lao, C., Coxon, P. R., Xi, K., Liu, Y., Ducati, C., Chen, R., Kumar, R. 2016; 26 (46): 8418–26

  View details for DOI 10.1002/adfm.201604069

  View details for Web of Science ID 000390117800006

• Systematic Effect for an Ultra long Cycle Lithium-Sulfur Battery NANO LETTERS Wu, F., Ye, Y., Chen, R., Qian, J., Zhao, T., Li, L., Li, W. 2015; 15 (11): 7431–39

  Abstract

  Rechargeable lithium-sulfur (Li-S) batteries are attractive candidates for energy storage devices because they have five times the theoretical energy storage of state-of-the-art Li-ion batteries. The main problems plaguing Li-S batteries are poor cycle life and limited rate capability, caused by the insulating nature of S and the shuttle effect associated with the dissolution of intermediate lithium polysulfides. Here, we report the use of biocell-inspired polydopamine (PD) as a coating agent on both the cathode and separator to address these problems (the "systematic effects"). The PD-modified cathode and separator play key roles in facilitating ion diffusion and keeping the cathode structure stable, leading to uniform lithium deposition and a solid electrolyte interphase. As a result, an ultralong cycle performance of more than 3000 cycles, with a capacity fade of only 0.018% per cycle, was achieved at 2 C. It is believed that the systematic modification of the cathode and separator for Li-S batteries is a new strategy for practical applications.

  View details for DOI 10.1021/acs.nanolett.5b02864

  View details for Web of Science ID 000364725400039

  View details for PubMedID 26502268