Atomic surface reduction of interfaces utilizing vapor phase approach: High energy LiNixMnyCoz oxide as a test case

Eliran Evenstein, Rosy, Shira Haber, Hadar Sclar, Lothar Houben, Kevin Leung, Michal Leskes, Malachi Noked

Research output: Contribution to journalArticlepeer-review

20 Scopus citations

Abstract

In the present work, a simple and agile methodology for atomic surface reduction of interfaces is introduced. Using a surface directed vapor phase reaction, at relatively low temperature, we show that a highly reactive and volatile molecule can be used to selectively reduce the interface, without changing the bulk of the treated material, and without the need of alternating sequence of multiple precursors, normally involved in ALD. The model system we use to demonstrate the efficacy, and potential of our approach is trimethyl aluminum, and high energy Li and Mn rich cathode (HE-NCM)as the functional material of interest. We demonstrate that with the proposed method, the particles of HE-NMC were conformally coated with ~ 3 nm amorphous layer of the reduced surface in less than 1 h (including the cooling time),as witnessed using HR-TEM. XPS and solid-state NMR, further confirmed that surface treatment was successfully achieved using the proposed method and is well explained by DFT calculations. Utilizing online electrochemical mass spectrometry (OEMS), we show in-operando that this amorphous layer helps to suppress parasitic reactions under extreme electrochemical conditions as indicated by the significant reduction in oxygen and CO2 evolution. The surface treatment further resulted in enhancement in specific capacity during the first cycle. This methodology provides a non-conventional path to achieve thin layer surface modification under facile conditions, and opens a new way to meet the requirements of surface modification strategies for improving the performance of electrode materials without utilizing expensive instrumentation and high temperature processes.

Original languageEnglish
Pages (from-to)261-269
Number of pages9
JournalEnergy Storage Materials
Volume19
DOIs
StatePublished - May 2019

Bibliographical note

Funding Information:
Rosy is thankful to the Planning and Budgeting Committee of the council of high education for awarding post-doctoral research fellowship. M.N. and M.L. are thankful to the Israeli council of high education, for Alon fellowship. S.H. would like to acknowledge the Sustainability and Energy Research Initiative (SAERI) fellowship. The project was conducted through the support of INREP, and through the support of IMOE. We thank the ISF for equipment support (MN, Grant no. 2028/17 and 2209/17 ) and funding (ML, 1580/17 ). This work was performed, in part, at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science. It was supported by Nanostructures for Electrical Energy Storage (NEES), an Energy Frontier Research Center funded by the U.S. Department of Energy , Office of Science , Office of Basic Energy Sciences under Award Number DESC0001160 . Sandia National Laboratories is a multi-mission laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International, Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA0003525.

Funding Information:
Rosy is thankful to the Planning and Budgeting Committee of the council of high education for awarding post-doctoral research fellowship. M.N. and M.L. are thankful to the Israeli council of high education, for Alon fellowship. S.H. would like to acknowledge the Sustainability and Energy Research Initiative (SAERI)fellowship. The project was conducted through the support of INREP, and through the support of IMOE. We thank the ISF for equipment support (MN, Grant no. 2028/17 and 2209/17)and funding (ML, 1580/17). This work was performed, in part, at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE)Office of Science. It was supported by Nanostructures for Electrical Energy Storage (NEES), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DESC0001160. Sandia National Laboratories is a multi-mission laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International, Inc., for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-NA0003525.

Funding Information:
Rosy is thankful to the Planning and Budgeting Committee of the council of high education for awarding post-doctoral research fellowship. M.N. and M.L. are thankful to the Israeli council of high education, for Alon fellowship. S.H. would like to acknowledge the Sustainability and Energy Research Initiative (SAERI) fellowship. The project was conducted through the support of INREP, and through the support of IMOE. We thank the ISF for equipment support (MN, Grant no. 2028/17 and 2209/17) and funding (ML, 1580/17). This work was performed, in part, at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science. It was supported by Nanostructures for Electrical Energy Storage (NEES), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DESC0001160. Sandia National Laboratories is a multi-mission laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International, Inc., for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-NA0003525.

Publisher Copyright:
© 2019 Elsevier B.V.

Keywords

  • Atomic Surface Reduction
  • electrode coatings
  • surface modification
  • volatile reactive compound

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