Understanding and Engineering Interfacial Adhesion in Solid-State Batteries with Metallic Anodes

Funding Information: The authors acknowledge funding for this work from the Engineering and Physical Sciences Research Council (EP/R002010/1, EP/R024006/1 and EP/P003532/1), Shell Global Solutions International B.V., the Spanish government (TED2021‐129254B‐C22) and Horizon Europe HORIZON‐CL5‐2021‐D2‐01 “SEATBELT” 101069726.Peer reviewedPublisher PD

Superstructure and Correlated Na+ Hopping in a Layered Mg-Substituted Sodium Manganate Battery Cathode are Driven by Local Electroneutrality

Acknowledgments ARTICLE SECTIONSJump To E.N.B. acknowledges funding from the Engineering Physical Sciences Research Council (EPSRC) via the National Productivity Interest Fund (NPIF) 2018 (EP/S515334/1). J.D.B. acknowledges funding from the Faraday Institution (EP/S003053/1, FIRG016). The authors also thank the Science and Technology Facilities Council (STFC) and ISIS Neutron and Muon source for neutron data (experiment no.: RB2010350). Additional thanks are given to the staff scientists at beamline I11 of the Diamond Light Source for synchrotron data using block allocation group time under proposal CY34243. This work also utilized the ARCHER UK National Supercomputing Service via our membership in the UK’s HEC Materials Chemistry Consortium, funded by the EPSRC (EP/L000202). The research was also carried out at the Center for Functional Nanomaterials, Brookhaven National Laboratory, through the U.S. Department of Energy, Office of Basic Energy Sciences, Contract DE-AC02-98CH10866. E.N.B. would also like to thank A. Van der Ven and M.A. Jones for illuminating discussions.Peer reviewedPublisher PD

Short-range ordering in a battery electrode, the 'cation-disordered' rocksalt Li1.25Nb0.25Mn0.5O2.

Cation order, with a local structure related to γ-LiFeO2, is observed in the nominally cation-disordered Li-excess rocksalt Li1.25Nb0.25Mn0.5O2via X-ray diffraction, neutron pair distribution function analysis, magnetic susceptibility and NMR spectroscopy. The correlation length of ordering depends on synthesis conditions and has implications for the electrochemistry of these phases.EPSRC: EP/L015978/1 Basic Energy Science, US Department of Energy: DE-SC001258

Probing Jahn-Teller Distortions and Antisite Defects in LiNiO2 with 7Li NMR Spectroscopy and Density Functional Theory

A.R.G.-S. and C.S.C. contributed equally to this work. The manuscript was written through contributions of all authors. All authors have given approval to the final version of the manuscript.Peer reviewe

Metal chalcogenide hollow polar bipyramid prisms as efficient sulfur hosts for Na-S batteries

Funding Information: We appreciate the support from the National Natural Science Foundation of China (Nos. 21773188 and 21972111), Fundamental Research Funds for the Central Universities (XDJK2019AA002), Postgraduate tutor team-building project (XYDS201911). The work at UT was supported by the Welch Foundation (F-1841) and the Texas Advanced Computing Center.Peer reviewe

Structural origins of voltage mysteresis in the Na-Ion cathode P2-Na0.67[Mg0.28Mn0.72]O2 : A combined spectroscopic and density functional theory study

Funding Information: E.N.B. acknowledges funding from the Engineering Physical Sciences Research Council (EPSRC) via the National Productivity Interest Fund (NPIF) 2018 and is also grateful for use of the ARCHER UK National Supercomputing Service via our membership in the UK’s HEC Materials Chemistry Consortium, funded by the EPSRC (EP/L000202). Research was also carried out at the Center for Functional Nanomaterials, Brookhaven National Laboratory, through the U.S. Department of Energy, Office of Basic Energy Sciences, Contract DE-AC02-98CH10866. P.J.R. thanks the Northeast Centre for Chemical Energy Storage (NECCES), an Energy Frontier Research Centre funded by the US Department of Energy, Office of Basic Energy Sciences, award DE-SC0012583. M.A.J. is grateful for the financial support of the EPSRC Centre for Doctoral Training (CDT) in Nanoscience and Nanotechnology Award EP/L015978/1. J.L. was supported by the National Research Foundation of Korea (NRF) grant funded by the Korean government (MEST) (no. 2019R1A6A1A10073437). E.N.B. also wishes to thank Dr M.F. Groh for assistance with setting up capillary XRD measurements. Publisher Copyright: ©Peer reviewedPublisher PD

A high-performance solid-state synthesized LiVOPO4 for lithium-ion batteries

Funding Information: This research was funded by U.S. Department of Energy , Office of Energy Efficiency and Renewable Energy (EERE) program under BMR award no. DE-EE0006852 . The structural characterization using NMR and PDF techniques was supported by the NorthEast Center for Chemical Energy Storage (NECCES), an Energy Frontier Research Center supported by the U.S. Department of Energy , Office of Science, Office of Basic Energy Sciences under award no. DE-SC0012583 . This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. We thank Dr. Fengxia Xin for help with TG-MS data acquisition, and Drs. Jatinkumar Rana and Jia Ding, for many helpful discussions. Funding Information: This research was funded by U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE) program under BMR award no. DE-EE0006852. The structural characterization using NMR and PDF techniques was supported by the NorthEast Center for Chemical Energy Storage (NECCES), an Energy Frontier Research Center supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under award no. DE-SC0012583. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. We thank Dr. Fengxia Xin for help with TG-MS data acquisition, and Drs. Jatinkumar Rana and Jia Ding, for many helpful discussions. Publisher Copyright: © 2019 The AuthorsPeer reviewe

Synergistic Degradation Mechanism in Single Crystal Ni-Rich NMC//Graphite Cells

Acknowledgments We acknowledge Diamond Light Source for time on beamline I09 under Proposals SI30201-1 and SI30201-2. This work is supported by the Faraday Institution under Grants FIRG044, FIRG024, and FIRG060.Peer reviewedPublisher PD

Operando characterization and theoretical modelling of metal|electrolyte interphase growth kinetics in solid-state-batteries - Part II: Modelling

Understanding the interfacial dynamics of batteries is crucial to control degradation and increase electrochemical performance and cycling life. If the chemical potential of a negative electrode material lies outside of the stability window of an electrolyte (either solid or liquid), a decomposition layer (interphase) will form at the interface. To better understand and control degradation at interfaces in batteries, theoretical models describing the rate of formation of these interphases are required. This study focuses on the growth kinetics of the interphase forming between solid electrolytes and metallic negative electrodes in solid-state batteries. More specifically, we demonstrate that the rate of interphase formation and metal plating during charge can be accurately described by adapting the theory of coupled ion-electron transfer (CIET). The model is validated by fitting experimental data presented in the first part of this study. The data was collected operando as a Na metal layer was plated on top of a NaSICON solid electrolyte (Na3.4Zr2Si2.4P0.6O12 or NZSP) inside a XPS chamber. This study highlights the depth of information which can be extracted from this single operando experiment, and is widely applicable to other solid-state electrolyte systems

17O NMR Spectroscopy in Lithium-Ion Battery Cathode Materials: Challenges and Interpretation.

Modern studies of lithium-ion battery (LIB) cathode materials employ a large range of experimental and theoretical techniques to understand the changes in bulk and local chemical and electronic structures during electrochemical cycling (charge and discharge). Despite its being rich in useful chemical information, few studies to date have used 17O NMR spectroscopy. Many LIB cathode materials contain paramagnetic ions, and their NMR spectra are dominated by hyperfine and quadrupolar interactions, giving rise to broad resonances with extensive spinning sideband manifolds. In principle, careful analysis of these spectra can reveal information about local structural distortions, magnetic exchange interactions, structural inhomogeneities (Li+ concentration gradients), and even the presence of redox-active O anions. In this Perspective, we examine the primary interactions governing 17O NMR spectroscopy of LIB cathodes and outline how 17O NMR may be used to elucidate the structure of pristine cathodes and their structural evolution on cycling, providing insight into the challenges in obtaining and interpreting the spectra. We also discuss the use of 17O NMR in the context of anionic redox and the role this technique may play in understanding the charge compensation mechanisms in high-capacity cathodes, and we provide suggestions for employing 17O NMR in future avenues of research.E.N.B. acknowledges funding from the Engineering Physical Sciences Research Council (EPSRC) via the National Productivity Interest Fund (NPIF) 2018. E.N.B. would also like to thank K.R. Bassey for assistance with figure preparation and invaluable advice and discussions