journal article·2019-08-26Open access

Novel Ordered Rocksalt-Type Lithium-Rich Li2Ru1–xNixO3−δ (0.3 ≤ x ≤ 0.5) Cathode Material with Tunable Anionic Redox Potential

Shiyao Zheng, Feng Zheng, Haodong Liu, Guiming Zhong, Jue Wu, Min Feng, Qihui Wu, Wenhua Zuo, Chaoyu Hong, Yan Chen, Ke An, Ping Liu, Shunqing Wu, Yong Yang

ACS Applied Energy Materials· Volume 2· Issue 8

Abstract

In this work, a series of ordered rocksalt (OR) type Li-rich Li2Ru1–xNixO3−δ (LRNxO, 0.3 ≤ x ≤ 0.5) are successfully synthesized and investigated for the first time. X-ray diffraction and neutron powder diffraction patterns exhibit an obvious phase transition from layered to an OR structure as the Ni content gradually increases from x = 0 to x = 0.5, which leads to different electrochemical behaviors. In the case of OR-LRN0.4O, an ∼350 mV decrease of the oxygen oxidation potential compared with Li2RuO3 (LRO) is observed from around 4.2 to 3.85 V, which is confirmed by both X-ray photelectron O 1s spectra and dQ/dV results. The role of Ni substitution on the oxygen redox reaction is studied by first-principles calculations, and it is concluded that the formation of the OR structure caused by Ni substitution is the main reason for lowering the oxygen oxidation potential. In addition, the average discharge voltage of OR-LRN0.4O is also enhanced compared with LRO. This work provides a novel innovative strategy to modulate and control the oxygen anion redox reaction for high-energy-density Li-rich materials, which shed light on the fundamental understanding and optimizing of the anion redox process in Li-rich materials.
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Research context

OpenAlex topics: Advancements in Battery Materials · Advanced Battery Materials and Technologies · Supercapacitor Materials and Fabrication

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Collaborative Innovation Center of Chemistry for Energy Materials, State Key Laboratory for Physical Chemistry of Solid Surface, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China

Department of Physics, Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Key Laboratory of Low Dimensional Condensed Matter Physics (Department of Education of Fujian Province), and Jiujiang Research Institute, Xiamen University, Xiamen 361005, China

Department of NanoEngineering, University of California San Diego, La Jolla, California 92093, United States

Xiamen Institute of Rare Earth Materials, Haixi Institutes, Chinese Academy of Sciences, Xiamen 361021, China

Department of Materials Chemistry, School of Chemical Engineering of Materials Science, Quanzhou Normal University, Quanzhou 362000, China

College of Mechanical and Energy Engineering, Jimei University, Xiamen 361021, China

Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States

School of Energy, Xiamen University, Xiamen 361005, China

Funding

Ministry of Science and Technology of the People's Republic of China · National Natural Science Foundation of China

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