Electrochemical Interfaces in Batteries

Within the framework of the Rudolf Diesel Industry Fellowship program, Peter Lamp and his team were collaborating with Moniek Tromp’s group (Inorganic Chemistry – Catalyst Characterisation, TUM)  in catalyst characterization (CCH) and with his TUM host Hubert Gasteiger’s group (Technical Electrochemistry, TUM) in technical electrochemistry (TEC) in the chemistry department of TUM on a research project focused on aging mechanisms in high-voltage cathode materials.

Project’s background The possibility of a large scale commercialization of electric and hybrid vehicles relies on the ability to improve battery characteristics such as energy, power density, safety, lifetime, and cost.

Capacity fade and impedance increase are the main phenomena that impair the long time functioning of battery cells. Both phenomena originate from a large number of simultaneous chemical processes that occur under both storage and cycling conditions. Structural and chemical changes within the bulk electrode materials generally produce capacity fade. On the other hand, phenomena involving the electrolyte-electrode interface, including transition metal dissolution from the cathode, not only contribute to capacity fade but also contribute to the rise of cell impedance. The mechanism and kinetic of the ageing reactions depend not only on a large number of physical and operating variables including temperature, voltage, charge state, C-rate, etc., but also on the specific cell chemistry and design.

Project targets This project aimed at a detailed fundamental understanding of the dissolution of transition metals for a large number of novel, high-voltage, cathode materials. At high cathode potentials, substantial capacity fading is observed. It is predominantly caused by transition metal dissolution which can lead to: i) loss of cathode active material; ii) passivation film formation on the cathode active material, causing increased cathode charge-transfer and film diffusion resistance; iii) transition metal deposition on the anode, causing increased anode charge-transfer resistance. Impurities like water and HF (produced by the decomposition of LiPF6 salt with water) may also accelerate transition metal dissolution, while electrolyte additives (e.g., TMB, FEC) may suppress it.

The project’s goals were be pursued by investigating the effect of water contamination, additive concentration, positive potential, and temperature using a combined electrochemical, chemical, and spectroscopic approach taking advantage of both ex-situ and in-situ techniques.

Doctoral Candidate:
Roland Jung, Technical Electrochemistry

Publications by the Focus Group

2024

  • Reuter, Lennart; Dickmanns, Jonas L. S.; Strehle, Benjamin; Hartmann, Louis; Maglia, Filippo; Jung, Roland; Suthar, Bharatkumar; Gasteiger, Hubert A.: Methods–Temperature-Dependent Gassing Analysis by On-Line Electrochemical Mass Spectrometry of Lithium-Ion Battery Cells with Commercial Electrolytes. Journal of The Electrochemical Society 171 (5), 2024, 050551 mehr…

2023

  • Martins, Milena; Haering, Dominik; Connell, Justin G.; Wan, Hao; Svane, Katrine L.; Genorio, Bostjan; Farinazzo Bergamo Dias Martins, Pedro; Lopes, Pietro P.; Gould, Brian; Maglia, Filippo; Jung, Roland; Stamenkovic, Vojislav; Castelli, Ivano E.; Markovic, Nenad M.; Rossmeisl, Jan; Strmcnik, Dusan: Role of Catalytic Conversions of Ethylene Carbonate, Water, and HF in Forming the Solid-Electrolyte Interphase of Li-Ion Batteries. ACS Catalysis 13 (13), 2023, 9289-9301 mehr…

2021

  • Kim, Un-Hyuck; Park, Geon-Tae; Conlin, Patrick; Ashburn, Nickolas; Cho, Kyeongjae; Yu, Young-Sang; Shapiro, David A.; Maglia, Filippo; Kim, Sung-Jin; Lamp, Peter; Yoon, Chong S.; Sun, Yang-Kook: Cation ordered Ni-rich layered cathode for ultra-long battery life. Energy & Environmental Science 14 (3), 2021, 1573-1583 mehr…
  • Yu, Yang; Karayaylali, Pinar; Sokaras, Dimosthenis; Giordano, Livia; Kou, Ronghui; Sun, Cheng-Jun; Maglia, Filippo; Jung, Roland; Gittleson, Forrest S.; Shao-Horn, Yang: Towards controlling the reversibility of anionic redox in transition metal oxides for high-energy Li-ion positive electrodes. Energy & Environmental Science 14 (4), 2021, 2322-2334 mehr…

2020

  • Castelli, Ivano E.; Zorko, Milena; Østergaard, Thomas M.; Martins, Pedro F. B. D.; Lopes, Pietro P.; Antonopoulos, Byron K.; Maglia, Filippo; Markovic, Nenad M.; Strmcnik, Dusan; Rossmeisl, Jan: The role of an interface in stabilizing reaction intermediates for hydrogen evolution in aprotic electrolytes. Chemical Science 11 (15), 2020, 3914-3922 mehr…
  • Ryu, Hoon-Hee; Park, Nam-Yung; Noh, Tae-Chong; Kang, Gyeong-Cheol; Maglia, Filippo; Kim, Sung-Jin; Yoon, Chong S.; Sun, Yang-Kook: Microstrain Alleviation in High-Energy Ni-Rich NCMA Cathode for Long Battery Life. ACS Energy Letters 6 (1), 2020, 216-223 mehr…
  • Zhang, Yirui; Katayama, Yu; Tatara, Ryoichi; Giordano, Livia; Yu, Yang; Fraggedakis, Dimitrios; Sun, Jame Guangwen; Maglia, Filippo; Jung, Roland; Bazant, Martin Z.; Shao-Horn, Yang: Revealing electrolyte oxidation via carbonate dehydrogenation on Ni-based oxides in Li-ion batteries by in situ Fourier transform infrared spectroscopy. Energy & Environmental Science 13 (1), 2020, 183-199 mehr…

2019

  • Jung, Roland; Linsenmann, Fabian; Thomas, Rowena; Wandt, Johannes; Solchenbach, Sophie; Maglia, Filippo; Stinner, Christoph; Tromp, Moniek; Gasteiger, Hubert A.: Nickel, Manganese, and Cobalt Dissolution from Ni-Rich NMC and Their Effects on NMC622-Graphite Cells. Journal of The Electrochemical Society 166 (2), 2019, A378-A389 mehr…
  • Park, Kang-Joon; Hwang, Jang-Yeon; Ryu, Hoon-Hee; Maglia, Filippo; Kim, Sung-Jin; Lamp, Peter; Yoon, Chong S.; Sun, Yang-Kook: Degradation Mechanism of Ni-Enriched NCA Cathode for Lithium Batteries: Are Microcracks Really Critical? ACS Energy Letters 4 (6), 2019, 1394-1400 mehr…

2018

  • Strmcnik, Dusan; Castelli, Ivano E.; Connell, Justin G.; Haering, Dominik; Zorko, Milena; Martins, Pedro; Lopes, Pietro P.; Genorio, Bostjan; Østergaard, Thomas; Gasteiger, Hubert A.; Maglia, Filippo; Antonopoulos, Byron K.; Stamenkovic, Vojislav R.; Rossmeisl, Jan; Markovic, Nenad M.: Electrocatalytic transformation of HF impurity to H2 and LiF in lithium-ion batteries. Nature Catalysis 1 (4), 2018, 255-262 mehr…

2017

  • Jung, Roland; Metzger, Michael; Maglia, Filippo; Stinner, Christoph; Gasteiger, Hubert A.: Chemical versus Electrochemical Electrolyte Oxidation on NMC111, NMC622, NMC811, LNMO, and Conductive Carbon. The Journal of Physical Chemistry Letters 8 (19), 2017, 4820-4825 mehr…
  • Jung, Roland; Metzger, Michael; Maglia, Filippo; Stinner, Christoph; Gasteiger, Hubert A.: Oxygen Release and Its Effect on the Cycling Stability of LiNixMnyCozO2(NMC) Cathode Materials for Li-Ion Batteries. Journal of The Electrochemical Society 164 (7), 2017, A1361-A1377 mehr…