当前位置：
X-MOL 学术
›
J. Phys. Chem. C
›
论文详情
Our official English website, www.x-mol.net, welcomes your
feedback! (Note: you will need to create a separate account there.)
Coupled LiPF6 Decomposition and Carbonate Dehydrogenation Enhanced by Highly Covalent Metal Oxides in High-Energy Li-Ion Batteries
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2018-11-19 , DOI: 10.1021/acs.jpcc.8b07848 Yang Yu , Pinar Karayaylali , Yu Katayama 1 , Livia Giordano , Magali Gauthier , Filippo Maglia 2 , Roland Jung 2 , Isaac Lund 3 , Yang Shao-Horn
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2018-11-19 , DOI: 10.1021/acs.jpcc.8b07848 Yang Yu , Pinar Karayaylali , Yu Katayama 1 , Livia Giordano , Magali Gauthier , Filippo Maglia 2 , Roland Jung 2 , Isaac Lund 3 , Yang Shao-Horn
Affiliation
|
The (electro)chemical reactions between positive electrodes and electrolytes are not well understood. We examined the oxidation of a LiPF6-based electrolyte with ethylene carbonate (EC) with layered lithium nickel, manganese, and cobalt oxides (NMC). Density functional theory calculations showed that the driving force for EC dehydrogenation on oxides, yielding surface protic species, increased with greater Ni content in NMC. Ex situ infrared and Raman spectroscopy revealed experimental evidence for EC dehydrogenation on charged NMC surfaces. Protic species on charged NMC surfaces from EC dehydrogenation could further react with LiPF6 to generate less-coordinated F species such as PF3O-like and lithium nickel oxyfluoride species on charged NMC particles and HF and PF2O2– in the electrolyte. Larger degree of salt decomposition was coupled with increasing EC dehydrogenation on charged NMC with increasing Ni or lithium deintercalation. An oxide-mediated chemical oxidation of electrolytes was proposed, providing new insights in stabilizing high-energy positive electrodes and improving Li-ion battery cycle life.
中文翻译：
高能锂离子电池中高共价金属氧化物促进的LiPF 6分解和碳酸盐脱氢耦合
正极与电解质之间的（电化学）化学反应还不很清楚。我们研究了碳酸锂（EC）和层状锂镍，锰和钴氧化物（NMC）对LiPF 6基电解质的氧化作用。密度泛函理论计算表明，随着NMC中Ni含量的增加，EC脱氢作用于氧化物的驱动力增加，从而产生表面质子物种。异位红外和拉曼光谱显示带电NMC表面EC脱氢的实验证据。EC脱氢在带电NMC表面上的质子物种可能进一步与LiPF 6反应，生成配位较弱的F物种，例如PF 3O形状和锂镍氟氧化物物种上带电NMC颗粒和HF和PF 2 ö 2 -在电解质中。更大程度的盐分解与带电NMC上EC脱氢的增加以及Ni或锂脱嵌的增加有关。提出了一种氧化物介导的电解质化学氧化方法，为稳定高能正极和改善锂离子电池循环寿命提供了新的见解。
更新日期：2018-11-20
中文翻译：
高能锂离子电池中高共价金属氧化物促进的LiPF 6分解和碳酸盐脱氢耦合
正极与电解质之间的（电化学）化学反应还不很清楚。我们研究了碳酸锂（EC）和层状锂镍，锰和钴氧化物（NMC）对LiPF 6基电解质的氧化作用。密度泛函理论计算表明，随着NMC中Ni含量的增加，EC脱氢作用于氧化物的驱动力增加，从而产生表面质子物种。异位红外和拉曼光谱显示带电NMC表面EC脱氢的实验证据。EC脱氢在带电NMC表面上的质子物种可能进一步与LiPF 6反应，生成配位较弱的F物种，例如PF 3O形状和锂镍氟氧化物物种上带电NMC颗粒和HF和PF 2 ö 2 -在电解质中。更大程度的盐分解与带电NMC上EC脱氢的增加以及Ni或锂脱嵌的增加有关。提出了一种氧化物介导的电解质化学氧化方法，为稳定高能正极和改善锂离子电池循环寿命提供了新的见解。
京公网安备 11010802027423号