Unraveling the Role of Surficial Oxygen Vacancies in Stabilizing Li-Rich Layered Oxides

Wang，Kai1; Qiu，Jimin1; Hou，Fuchen2; Yang，Ming3; Nie，Kaiqi4; Wang，Jiaou4; Hou，Yichao5; Huang，Weiyuan1; Zhao，Wenguang1; Zhang，Peixin3; Lin，Junhao2; Hu，Jiangtao3; Pan，Feng1; Zhang，Mingjian6

2023-08-25

10.1002/aenm.202301216

Advanced Energy Materials   Impact Factor & Quartile

1614-6832

1614-6840

Li-rich layered oxides based on the anionic redox chemistry provide the highest practical capacity among all transition metal (TM) oxide cathodes but still struggle with poor cycling stability. Here, a certain amount of oxygen vacancies (OVs) are introduced into the ≈10 nm-thick surface region of LiNiCoMnO through a long-time medium-temperature post-annealing. These surficial enriched OVs significantly suppress the generation of O-O dimers (O, 0 < n < 4) and the associated side reactions, thus facilitating the construction of a uniform and compact cathode/electrolyte interphase (CEI) layer on the surface. The CEI layer then decreases the further side reactions and TM dissolution and protects the bulk structure upon cycling, eventually leading to enhanced cycling stability, demonstrated in both half cells and full cells. An in-depth understanding of OVs is expected to benefit the design of stable cathode materials based on anionic redox chemistry.

cathode/electrolyte interphase cycling stability Li-rich layered oxides O-O dimers oxygen vacancies

SCI

English

Others

Soft Science Research Project of Guangdong Province[2017B030301013];Basic and Applied Basic Research Foundation of Guangdong Province[2021B1515130002];National Natural Science Foundation of China[52172175];National Natural Science Foundation of China[52202269];

Chemistry ; Energy & Fuels ; Materials Science ; Physics

Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:001026333700001

WILEY-V C H VERLAG GMBH

2-s2.0-85164466901

Scopus

1.School of Advanced Materials,Peking University,Shenzhen Graduate School,Shenzhen,Guangdong,518055,China
2.Department of Physics,Southern University of Science and Technology,Shenzhen,Guangdong,518055,China
3.College of Chemistry and Environmental Engineering,Shenzhen University,Shenzhen,Guangdong,518060,China
4.Institute of High Energy Physics,Chinese Academy of Sciences,Beijing,100049,China
5.State Key Laboratory of Applied Organic Chemistry,Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province,Frontiers,Science Center for Rare Isotopes,College of Chemistry and Chemical Engineering,Lanzhou University,Lanzhou,Gansu,730000,China
6.School of Science and Engineering,The Chinese University of Hong Kong,Shenzhen,Guangdong,518172,China

Wang，Kai,Qiu，Jimin,Hou，Fuchen,et al. Unraveling the Role of Surficial Oxygen Vacancies in Stabilizing Li-Rich Layered Oxides[J]. Advanced Energy Materials,2023,13(32).

Wang，Kai.,Qiu，Jimin.,Hou，Fuchen.,Yang，Ming.,Nie，Kaiqi.,...&Zhang，Mingjian.(2023).Unraveling the Role of Surficial Oxygen Vacancies in Stabilizing Li-Rich Layered Oxides.Advanced Energy Materials,13(32).

Wang，Kai,et al."Unraveling the Role of Surficial Oxygen Vacancies in Stabilizing Li-Rich Layered Oxides".Advanced Energy Materials 13.32(2023).