In situ monitoring of the growth of nickel, manganese, and cobalt hydroxide precursors during co-precipitation synthesis of Li-ion cathode materials

Zhange Feng, Pallab Barai, Jihyeon Gim, Ke Yuan, Yimin A. Wu, Yuanyuan Xie, Yuzi Liu, Venkat Srinivasan

Research output: Contribution to journalArticlepeer-review

25 Scopus citations

Abstract

The electrochemical performance of cathode materials for Li-ion batteries depends on the morphology of the material, which, in turn, depends on the synthesis conditions. Very few studies have focused on the impact of process conditions on the final morphology of the cathode particles and analyzed the growth during synthesis. In this paper, the evolution of nickel, manganese, and cobalt hydroxide precursor, Ni1/3Mn1/3Co1/3(OH)2, is investigated using a combination of in situ and ex situ techniques during the commonly-used coprecipitation process. These include in situ wide angle X-ray scattering, in-situ ultra-small angle X-ray scattering and ex situ particle size analysis. The growth rate of crystalline Ni1/3Mn1/3Co1/3(OH)2 primary particle is found to be almost constant, consistent with a mathematical analysis of process. The growth of the Ni1/3Mn1/3Co1/3(OH)2 secondary particle and its particle size distribution revealed different growth stages for samples prepared at different pH. These techniques are complimented with scanning electron microscopy and electrochemical testing to track the morphology and performance of the hydroxide particle and the subsequent calcined LiNi1/3Mn1/3Co1/3O2 cathode active material. This study presents insights into the synthesis process and provides a deeper understanding to aid in process optimization.

Original languageEnglish
Pages (from-to)A3077-A3083
JournalJournal of the Electrochemical Society
Volume165
Issue number13
DOIs
StatePublished - 2018
Externally publishedYes

Funding

In-situ WAXS and USAXS experiment is done at Sector 9ID in Advanced Photon Source of Argonne National Laboratory (ANL) with the help from Dr. Jan Ilavsky and Dr. Ivan Kuzmenko. The particle size analysis is conducted in the Materials Engineering Research Facility (MERF) in ANL with the help of Dr. Michael Kras. TEM images are taken at Center for Nanoscale Materials (CNM) at ANL. SEM images are taken at Electron microscopy Center at ANL. ZF and PB would acknowledge the helpful discussion with Dr. Zonghai Chen, John David Carter, Tao Li, Le Ge, Han Gao, Tongchao Liu, YoungHo Shin, Ozgenur Kahvecioglu Feridun and Albert Lipson. This work was supported by funding through the Roll-To-Roll (R2R) program under the Advanced Manufacturing Office (AMO) of US Department of Energy (US-DOE). This manuscript has been created in part by UChicago Argonne, LLC, Operator of Argonne National Laboratory (“Argonne”). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up nonexclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government. 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.

FundersFunder number
DOE Office of Science
US Department of Energy
U.S. Department of EnergyDE-AC02-06CH11357
Office of Science
Argonne National Laboratory

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