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Understand the Structure Evolution and Solid-Liquid Interface of Electrode Materials in Advanced Li-/Na-ion Batteries and the Effect on Battery Performance

EMSL Project ID


The overall goal of this proposal is to investigate the structure evolution and solid-liquid interface of advanced battery materials by integrated ex-situ or in-situ characterization and theoretical simulation to understand the mechanism for stable cycling or failing of batteries. Specifically, electrode materials for advanced Li-/Na-ion batteries including Si-carbon nanocomposites, Na0.44MnO2 nanorods, hard carbon nanoparticles, and Na3V2(PO4)3-graphene nanocomposites will be synthesized by well-controlled anodization or other methods; Ex-situ/in-situ characterization, electrochemical measurements, and theoretical modeling will be carried out to investigate the bulk structure/interface evolution upon cycling and the correlation between the structure/interface and battery performance. The proposed work will be focused on 1) synthesis of several model materials for advanced Li-/Na-ion batteries; 2) ex-situ and in-situ characterization of the structure/interface of electrode materials; 3) understand how the structure/interface of electrode materials evolves upon cycling and how they affect the battery performance with the help of theoretical simulation.
Achievement of these objectives will enable a detailed scientific understanding of the correlation between material structure/interface interaction and battery performance and provide guidance for new material/structure design or interface functionalization of electrode materials in advanced energy systems.
PNNL is the lead research institution, which capitalizes on our strong capabilities in materials chemistry, structure characterization, and multiscale computational modeling. The project derives considerable benefit from the in-house experimental and computational facilities at EMSL, a DOE user facility funded by OBER. The EMSL facility will be used for ex-situ TEM, SEM, XPS, XRD, NMR and AFM study and in-situ TEM and NMR characterization. The proposed work requires a close collaboration with EMSL staffs that will help efficiently digest emerging results and respond to challenges as they arise.
This proposal is directly related to the EMSL Scientific Theme Area “Energy Materials and Processes”. In particular, this proposal focuses on using advanced computational and in situ experimental tools to accelerate understanding of “material characteristics” and “solvent-mediated interfaces” to establish structure-property relationships and to enable new approaches to the design of energy materials.

Project Details

Project type
Large-Scale EMSL Research
Start Date
End Date


Principal Investigator

Xiaolin Li
Pacific Northwest National Laboratory


Donghai Mei
Tiangong University

Team Members

Rajankumar Patel
Pacific Northwest National Laboratory

Shaofang Fu
Washington State University

Hanlei Zhang
Pacific Northwest National Laboratory

Qiurong Shi
Washington State University

Yun Li
University of Washington

Shunli Chen
The Xinjiang Technical Institute of Physics and Chemistry, CAS

Shenyang Hu
Pacific Northwest National Laboratory

Li Fu
Environmental Molecular Sciences Laboratory

Hongfei Wang
Fudan University

Wu Xu
Pacific Northwest National Laboratory

Yuyan Shao
Pacific Northwest National Laboratory

Jun Liu
Yale University

Yuehe Lin
Washington State University

Related Publications

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Du L ,Luo L ,Feng Z ,Engelhard M H,Xie X ,Han B ,Sun J ,Zhang J ,Yin G ,Wang C ,Wang Y ,Shao Y 2017. "Nitrogen-doped graphitized carbon shell encapsulated NiFe nanoparticles: A highly durable oxygen evolution catalyst" Nano Energy 39():245-252. 10.1016/j.nanoen.2017.07.006
Fu S, C Zhu, J Song, MH Engelhard, B Xiao, D Du, and Y Lin. 2017. "Nitrogen and Fluorine-Codoped Carbon Nanowire Aerogels as Metal-Free Electrocatalysts for Oxygen Reduction Reaction." Chemistry - A European Journal 23(43):10460-10464. doi:10.1002/chem.201701969
Fu S, C Zhu, J Song, MH Engelhard, D Du, and Y Lin. 2017. "Three-dimensional Nitrogen-Doped Reduced Graphene Oxide/Carbon Nanotube Composite Catalysts for Vanadium Flow Batteries." Electroanalysis 29(5):1469-1473. doi:10.1002/elan.201600787
Fu S, C Zhu, J Song, MH Engelhard, X Li, D Du, and Y Lin. 2016. "Highly Ordered Mesoporous Bimetallic Phosphides as Efficient Oxygen Evolution Electrocatalysts." ACS Energy Letters 4(1):792-796. doi:10.1021/acsenergylett.6b00408
Fu S., C. Zhu, J. Song, M.H. Engelhard, X. Li, P. Zhang, and H. Xia, et al. 2017. "Template-Directed Synthesis of Nitrogen- and Sulfur- Codoped Carbon Nanowires Aerogels with Enhanced Electrocatalytic Performance for Oxygen Reduction." Nano Research 10, no. 6:1888-1895. PNNL-SA-123461. doi:10.1007/s12274-016-1371-8
Fu S, C Zhu, J Song, P Zhang, MH Engelhard, H Xia, D Du, and Y Lin. 2017. "Low-Pt-Content Ternary PdCuPt Nanodendrites: An Efficient Electrocatalyst for Oxygen Reduction Reaction." Nanoscale 9(3):1279-1284. doi:10.1039/c6nr06646a
Fu S, C Zhu, J Song, S Feng, D Du, MH Engelhard, D Xiao, D Li, and Y Lin. 2017. "Two-dimensional N,S-codoped carbon/Co9S8 catalysts derived from Co(OH)2 nanosheets for oxygen reduction reaction." ACS Applied Materials & Interfaces 9(42):36755-36761. doi:10.1021/acsami.7b10227
Fu S, J Song, C Zhu, GH Xu, K Amine, CJ Sun, X Li, MH Engelhard, D Du, and Y Lin. 2018. "Ultrafine and Highly Disordered Ni2Fe1 Nanofoams Enabled Highly Efficient Oxygen Evolution Reaction in Alkaline Electrolyte." Nano Energy 44:319-326. doi:10.1016/j.nanoen.2017.12.010
Jeong S., X. Li, J. Zheng, P. Yan, R. Cao, H. Jung, and C.M. Wang, et al. 2016. "Hard carbon coated nano-Si/graphite composite as a high performance anode for Li-ion batteries." Journal of Power Sources 329. PNNL-SA-116194. doi:10.1016/j.jpowsour.2016.08.089
Liu B, W Xu, P Yan, X Sun, ME Bowden, J Read, J Qian, D Mei, CM Wang, and J Zhang. 2016. "Enhanced Cycling Stability of Rechargeable Li-O2 Batteries Using High Concentration Electrolytes." Advanced Functional Materials 26(4):605-613. doi:10. 1002/adfm. 201503697
Li X, P Yan, MH Engelhard, AJ Crawford, VV Viswanathan, CM Wang, J Liu, and VL Sprenkle. 2016. "The Importance of Solid Electrolyte Interphase Formation for Long Cycle Stability Full-Cell Na-Ion Batteries." Nano Energy 27:664-672. doi:10.1016/j.nanoen.2016.07.030
Luo L, MH Engelhard, Y Shao, and C Wang. 2017. "Revealing the Dynamics of Platinum Nanoparticle Catalyst on Carbon in Oxygen and Water using Environmental TEM." ACS Catalysis 7:7658-7664. doi:10.1021/acscatal.7b02861
Pan H, J Chen, R Cao, V Murugesan, NN Rajput, KS Han, KA Persson, L Estevez, MH Engelhard, J Zhang, KT Mueller, Y Cui, Y Shao, and J Liu. 2017. "Non Encapsulation Approach for High Performance Li-S Batteries through Controlled Nucleation and Growth." Nature Energy 2:813-820. doi:10.1038/s41560-017-0005-z
Pan H, KS Han, M Vijayakumar, J Xiao, R Cao, J Chen, J Zhang, KT Mueller, Y Shao, and J Liu. 2016. "Ammonium additives to dissolve lithium sulfide through hydrogen binding for high energy lithium-sulfur batteries." ACS Applied Materials & Interfaces. doi:10. 1021/acsami. 6b04158
Shi Q, C Zhu, C Bi, H Xia, MH Engelhard, D Du, and Y Lin. 2017. "Intermetallic Pd3Pb Nanowire Networks Boost Ethanol Oxidation and Oxygen Reduction Reactions with Significantly Improved Methanol Tolerance." Journal of Materials Chemistry A 5(45):23952-23959. doi:10.1039/C7TA08407B
Shi Q, C Zhu, D Du, C Bi, H Xia, S Feng, MH Engelhard, and Y Lin. 2017. "Kinetically Controlled Synthesis of AuPt Bi-metallic Aerogels and Their Enhanced Electrocatalytic Performances." Journal of Materials Chemistry A 5(37):19626-19631. doi:10.1039/c7ta06375j
Shi Q., C. Zhu, M. Tian, D. Su, M. Fu, M.H. Engelhard, and J.S. Watts, et al. 2018. "Ultrafine Pd Ensembles Anchored-Au2Cu Aerogels Boost Ethanol Electrooxidation." Nano Energy 53. PNNL-SA-135816. doi:10.1016/j.nanoen.2018.08.047
Shi Q, C Zhu, Y Li, H Xia, MH Engelhard, S Fu, D Du, and Y Lin. 2016. "A Facile Method for Synthesizing Dendritic Core-Shell Structured Ternary Metallic Aerogels and Their Enhanced Electrochemical Performances." Chemistry of Materials 28(21):7928-7934. doi:10.1021/acs.chemmater.6b03549
Song J, C Zhu, B Xu, S Fu, MH Engelhard, R Ye, D Du, SP Beckman, and Y Lin. 2017. "Bimetallic Cobalt-Based Phosphide Zeolitic Imidazolate Framework: CoPx Phase-Dependent Electrical Conductivity and Hydrogen Atom Adsorption Energy for Efficient Overall Water Splitting." Advanced Energy Materials 7(2):Article No. 1601555. doi:10.1002/aenm.201601555
Song J., K. Wang, J. Zheng, M.H. Engelhard, B. Xiao, E. Hu, and Z. Zhu, et al. 2020. "Controlling Surface Phase Transition and Chemical Reactivity of O3-Layered Metal Oxide Cathodes for High-Performance Na-ion Batteries." ACS Energy Letters 5, no. 6:1718-1725. PNNL-SA-141318. doi:10.1021/acsenergylett.0c00700
Soto FA, P Yan, MH Engelhard, A Marzouk, C Wang, J Liu, VL Sprenkle, F El-Mellouhi, PB Balbuena, and X Li. 2017. "Tuning the Solid Electrolyte Interphase for Selective Li- and Na-Ion Storage in Hard Carbon." Advanced Materials 29(18):1606860. doi:10.1002/adma.201606860
Vissers DR, Z Chen, Y Shao, MH Engelhard, U Das, PC Redfern, LA Curtiss, B Pan, J Liu, and K Amine. 2016. "An Astute Investigation Into The Role Of Manganese Deposition In The Capacity Fading Of Graphite Anode." ACS Applied Materials & Interfaces 8(22):14244–14251. doi:10. 1021/acsami. 6b02061
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Xie X., M. Song, L. Wang, N. Yang, M.H. Engelhard, L. Luo, and A. Miller, et al. 2019. "Electrocatalytic Hydrogen Evolution in Neutral pH Solutions: Dual-Phase Synergy." ACS Catalysis 9, no. 9:8712-8718. PNNL-SA-129625. doi:10.1021/acscatal.9b02609
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Zhang H, S Hwang, M Wang, Z Feng, SG Karakalos, L Luo, Z Qiao, X Xie, C Wang, D Su, Y Shao, and G Wu. 2017. "Single Atomic Iron Catalysts for Oxygen Reduction in Acidic Media: Particle Size Control and Thermal Activation." Journal of the American Chemical Society 139(40):14143-14149. doi:10.1021/jacs.7b06514
Zhou Y, CH Yen, YH Hu, C Wang, X Cheng, CM Wai, J Yang, and Y Lin. 2016. "Making Ultrafine and Highly-dispersive Multimetallic Nanoparticles in Three-dimensional Graphene With Supercritical Fluid as Excellent Electrocatalyst for Oxygen Reduction Reaction." Journal of Materials Chemistry A 4(47):18628-18638. doi:10.1039/c6ta08508c
Zhou Y, X Cheng, CH Yen, CM Wai, C Wang, J Yang, and Y Lin. 2017. "Synthesis Of An Excellent Electrocatalyst For Oxygen Reduction Reaction With Supercritical Fluid: Graphene Cellular Monolith With Ultrafine And Highly Dispersive Multimetallic Nanoparticles." Journal of Power Sources 347:69-78. doi:10.1016/j.jpowsour.2017.02.044
Zhu C., Q. Shi, S. Fu, J. Song, D. Du, D. Su, and M.H. Engelhard, et al. 2018. "Core-Shell PdPb@Pd Aerogels with Multiply-Twinned Intermetallic Nanostructures: Facile Synthesis with Accelerated Gelation Kinetics and Their Enhanced Electrocatalytic Properties." Journal of Materials Chemistry A 6, no. 17:7517-7521. PNNL-SA-126185. doi:10.1039/c7ta11233e
Zhu C, S Fu, J Song, Q Shi, D Su, MH Engelhard, X Li, D Xiao, D Li, L Estevez, D Du, and Y Lin. 2017. "Self-Assembled Fe-N-Doped Carbon Nanotube Aerogels with Single-Atom Catalysis Feature as Highly Efficient Oxygen Reduction Electrocatalysts." Small 13(15):Article No. 1603407. doi:10.1002/smll.201603407