All Publications

  • CO2 Utilization for Water Treatment: Ion Exchange Nitrate Removal Driven by CO2 without Producing Spent Brine Regenerant ACS ES&T Water Dong, H., Chen, H., SenGupta, A. K. 2021
  • 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
  • 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
  • Tortuosity Effects in Lithium-Metal Host Anodes JOULE Chen, H., Pei, A., Wan, J., Lin, D., Vila, R., Wang, H., Mackanic, D., Steinruck, H., Huang, W., Li, Y., Yang, A., Xie, J., Wu, Y., Wang, H., Cui, Y. 2020; 4 (4): 938–52
  • Dynamic Covalent Synthesis of Crystalline Porous Graphitic Frameworks CHEM Li, X., Wang, H., Chen, H., Zheng, Q., Zhang, Q., Mao, H., Liu, Y., Cai, S., Sun, B., Dun, C., Gordon, M. P., Zheng, H., Reimer, J. A., Urban, J. J., Ciston, J., Tan, T., Chan, E. M., Zhang, J., Liu, Y. 2020; 6 (4): 933–44
  • 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
  • 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


    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

  • Electrochemical generation of liquid and solid sulfur on two-dimensional layered materials with distinct areal capacities Nature Nanotechnology Yang, A., Zhou, G., et al 2020
  • Electrochemical generation of liquid and solid sulfur on two-dimensional layered materials with distinct areal capacities. Nature nanotechnology Yang, A. n., Zhou, G. n., Kong, X. n., Vilá, R. A., Pei, A. n., Wu, Y. n., Yu, X. n., Zheng, X. n., Wu, C. L., Liu, B. n., Chen, H. n., Xu, Y. n., Chen, D. n., Li, Y. n., Fakra, S. n., Hwang, H. Y., Qin, J. n., Chu, S. n., Cui, Y. n. 2020


    It has recently been shown that sulfur, a solid material in its elementary form S8, can stay in a supercooled state as liquid sulfur in an electrochemical cell. We establish that this newly discovered state could have implications for lithium-sulfur batteries. Here, through in situ studies of electrochemical sulfur generation, we show that liquid (supercooled) and solid elementary sulfur possess very different areal capacities over the same charging period. To control the physical state of sulfur, we studied its growth on two-dimensional layered materials. We found that on the basal plane, only liquid sulfur accumulates; by contrast, at the edge sites, liquid sulfur accumulates if the thickness of the two-dimensional material is small, whereas solid sulfur nucleates if the thickness is large (tens of nanometres). Correlating the sulfur states with their respective areal capacities, as well as controlling the growth of sulfur on two-dimensional materials, could provide insights for the design of future lithium-sulfur batteries.

    View details for DOI 10.1038/s41565-019-0624-6

    View details for PubMedID 31988508

  • Uniform High Ionic Conducting Lithium Sulfide Protection Layer for Stable Lithium Metal Anode ADVANCED ENERGY MATERIALS Chen, H., Pei, A., Lin, D., Xie, J., Yang, A., Xu, J., Lin, K., Wang, J., Wang, H., Shi, F., Boyle, D., Cui, Y. 2019; 9 (22)
  • Ultrathin, flexible, solid polymer composite electrolyte enabled with aligned nanoporous host for lithium batteries. Nature nanotechnology Wan, J., Xie, J., Kong, X., Liu, Z., Liu, K., Shi, F., Pei, A., Chen, H., Chen, W., Chen, J., Zhang, X., Zong, L., Wang, J., Chen, L., Qin, J., Cui, Y. 2019


    The urgent need for safer batteries is leading research to all-solid-state lithium-based cells. To achieve energy density comparable to liquid electrolyte-based cells, ultrathin and lightweight solid electrolytes with high ionic conductivity are desired. However, solid electrolytes with comparable thicknesses to commercial polymer electrolyte separators (~10mum) used in liquid electrolytes remain challenging to make because of the increased risk of short-circuiting the battery. Here, we report on a polymer-polymer solid-state electrolyte design, demonstrated with an 8.6-mum-thick nanoporous polyimide (PI) film filled with polyethylene oxide/lithium bis(trifluoromethanesulfonyl)imide (PEO/LiTFSI) that can be used as a safe solid polymer electrolyte. The PI film is nonflammable and mechanically strong, preventing batteries from short-circuiting even after more than 1,000h of cycling, and the vertical channels enhance the ionic conductivity (2.3*10-4Scm-1 at 30°C) of the infused polymer electrolyte. All-solid-state lithium-ion batteries fabricated with PI/PEO/LiTFSI solid electrolyte show good cycling performance (200 cycles at C/2 rate) at 60°C and withstand abuse tests such as bending, cutting and nail penetration.

    View details for DOI 10.1038/s41565-019-0465-3

    View details for PubMedID 31133663

  • Fast lithium growth and short circuit induced by localized-temperature hotspots in lithium batteries NATURE COMMUNICATIONS Zhu, Y., Xie, J., Pei, A., Liu, B., Wu, Y., Lin, D., Li, J., Wang, H., Chen, H., Xu, J., Yang, A., Wu, C., Wang, H., Chen, W., Cui, Y. 2019; 10
  • In Situ X-ray Absorption Spectroscopic Investigation of the Capacity Degradation Mechanism in Mg/S Batteries NANO LETTERS Xu, Y., Ye, Y., Zhao, S., Feng, J., Li, J., Chen, H., Yang, A., Shi, F., Jia, L., Wu, Y., Yu, X., Glans-Suzuki, P., Cui, Y., Guo, J., Zhang, Y. 2019; 19 (5): 2928–34
  • In Situ X-ray Absorption Spectroscopic Investigation of the Capacity Degradation Mechanism in Mg/S Batteries. Nano letters Xu, Y., Ye, Y., Zhao, S., Feng, J., Li, J., Chen, H., Yang, A., Shi, F., Jia, L., Wu, Y., Yu, X., Glans-Suzuki, P., Cui, Y., Guo, J., Zhang, Y. 2019


    The Mg/S battery is attractive because of its high theoretical energy density and the abundance of Mg and S on the earth. However, its development is hindered by the lack of understanding to the underlying electrochemical reaction mechanism of its charge-discharge processes. Here, using a unique in situ X-ray absorption spectroscopic tool, we systematically study the reaction pathways of the Mg/S cells in Mg(HMDS)2-AlCl3 electrolyte. We find that the capacity degradation is mainly due to the formation of irreversible discharge products, such as MgS and Mg3S8, through a direct electrochemical deposition or a chemical disproportionation of intermediate polysulfide. In light of the fundamental understanding, we propose to use TiS2 as a catalyst to activate the irreversible reaction of low-order MgS x and MgS, which results in an increased discharging capacity up to 900 mAh·g-1 and a longer cycling life.

    View details for PubMedID 30932498

  • An Interconnected Channel-Like Framework as Host for Lithium Metal Composite Anodes ADVANCED ENERGY MATERIALS Wang, H., Lin, D., Xie, J., Liu, Y., Chen, H., Li, Y., Xu, J., Zhou, G., Zhang, Z., Pei, A., Zhu, Y., Liu, K., Wang, K., Cui, Y. 2019; 9 (7)
  • Wrinkled Graphene Cages as Hosts for High-Capacity Li Metal Anodes Shown by Cryogenic Electron Microscopy. Nano letters Wang, H., Li, Y., Li, Y., Liu, Y., Lin, D., Zhu, C., Chen, G., Yang, A., Yan, K., Chen, H., Zhu, Y., Li, J., Xie, J., Xu, J., Zhang, Z., Vila, R., Pei, A., Wang, K., Cui, Y. 2019


    Lithium (Li) metal has long been considered the "holy grail" of battery anode chemistry but is plagued by low efficiency and poor safety due to its high chemical reactivity and large volume fluctuation, respectively. Here we introduce a new host of wrinkled graphene cage (WGC) for Li metal. Different from recently reported amorphous carbon spheres, WGC show highly improved mechanical stability, better Li ion conductivity, and excellent solid electrolyte interphase (SEI) for continuous robust Li metal protection. At low areal capacities, Li metal is preferentially deposited inside the graphene cage. Cryogenic electron microscopy characterization shows that a uniform and stable SEI forms on the WGC surface that can shield the Li metal from direct exposure to electrolyte. With increased areal capacities, Li metal is plated densely and homogeneously into the outer pore spaces between graphene cages with no dendrite growth or volume change. As a result, a high Coulombic efficiency (CE) of 98.0% was achieved under 0.5 mA/cm2 and 1-10 mAh/cm2 in commercial carbonate electrolytes, and a CE of 99.1% was realized with high-concentration electrolytes under 0.5 mA/cm2 and 3 mAh/cm2. Full cells using WGC electrodes with prestored Li paired with Li iron phosphate showed greatly improved cycle lifetime. With 10 mAh/cm2 Li metal deposition, the WGC/Li compositeanodewas able to provide a high specific capacity of 2785 mAh/g. With its roll-to-roll compatible fabrication procedure, WGC serves as a highly promising material for the practical realization of Li metal anodes in next-generation high energy density secondary batteries.

    View details for PubMedID 30676759

  • Nanostructural and Electrochemical Evolution of the Solid-Electrolyte Interphase on CuO Nanowires Revealed by Cryogenic-Electron Microscopy and Impedance Spectroscopy ACS NANO Huang, W., Boyle, D. T., Li, Y., Li, Y., Pei, A., Chen, H., Cui, Y. 2019; 13 (1): 737–44


    Battery performance is critically dependent on the nanostructure and electrochemical properties of the solid-electrolyte interphase (SEI) - a passivation film that exists on most lithium battery anodes. However, knowledge of how the SEI nanostructure forms and its impact on ionic transport remains limited due to its sensitivity to transmission electron microscopy and difficulty in accurately probing the SEI impedance. Here, we track the voltage-dependent, stepwise evolution of the nanostructure and impedance of the SEI on CuO nanowires using cryogenic-electron microscopy (cryo-EM) and electrochemical impedance spectroscopy (EIS). In carbonate electrolyte, the SEI forms at 1.0 V vs Li/Li+ as a 3 nm-thick amorphous SEI and grows to 4 nm at 0.5 V; as the potential approaches 0.0 V vs Li/Li+, the SEI on the CuO nanowires forms an 8 nm-thick inverted multilayered nanostructure in ethylene carbonate/diethyl carbonate (EC/DEC) electrolyte with 10 vol. % fluoroethylene carbonate (FEC) and a mosaic nanostructure in EC/DEC electrolyte. Upon Li deposition, the total SEI thickness grows to 16 nm and significant growth of the inner amorphous layer takes place in the inverted multilayered nanostructure, indicating electrolyte permeates the SEI. Using a refined EIS methodology, we isolate the SEI impedance on Cu and find that the SEI nanostructure directly correlates to macroscopic Li-ion transport through the SEI. The inverted layered nanostructure decreases the interfacial impedance upon formation, whereas the mosaic nanostructure continually increases the interfacial impedance during growth. These structural and electrochemical findings illustrate a more complete portrait of SEI formation and guide further improvements in engineered SEI.

    View details for DOI 10.1021/acsnano.8b08012

    View details for Web of Science ID 000456749900075

    View details for PubMedID 30589528

  • A Two-Dimensional MoS2 Catalysis Transistor by Solid-State Ion Gating Manipulation and Adjustment (SIGMA). Nano letters Wu, Y. n., Ringe, S. n., Wu, C. L., Chen, W. n., Yang, A. n., Chen, H. n., Tang, M. n., Zhou, G. n., Hwang, H. Y., Chan, K. n., Cui, Y. n. 2019


    A variety of methods including tuning chemical compositions, structures, crystallinity, defects and strain, and electrochemical intercalation have been demonstrated to enhance the catalytic activity. However, none of these tuning methods provide direct dynamical control during catalytic reactions. Here we propose a new method to tune the activity of catalysts through solid-state ion gating manipulation and adjustment (SIGMA) using a catalysis transistor. SIGMA can electrostatically dope the surface of catalysts with a high electron concentration over 5 × 1013 cm-2 and thus modulate both the chemical potential of the reaction intermediates and their electrical conductivity. The hydrogen evolution reaction (HER) on both pristine and defective MoS2 were investigated as model reactions. Our theoretical and experimental results show that the overpotential at 10 mA/cm2 and Tafel slope can be in situ, continuously, dynamically, and reversibly tuned over 100 mV and around 100 mV/dec, respectively.

    View details for DOI 10.1021/acs.nanolett.9b02888

    View details for PubMedID 31499003