锂离子电池5V正极材料LiNi_（0.5）Mn_（1.5）O_4的制备及改性研究
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摘要
5V正极材料LiNi_(0.5)Mn_(1.5)O)_4具有较高容量和4.7V高电压放电平台,不仅可以满足个人电子消费品和大型电动设备对新一代电源的需求,而且可兼容工作电压较高的负极材料,从而提高电池的安全性能,使其成为下一代先进锂离子电池最受瞩目的正极材料之一。
本研究针对LiNi_(0.5)Mn_(1.5)O)_4存在循环稳定性和倍率放电性能亟待改善和提高这一关键问题,开展制备和改性研究。考察制备工艺对材料物理化学性质和电化学性能的影响,探索LiNi_(0.5)Mn_(1.5)O)_4的生长规律及材料的结构和形貌与电化学性能间的联系。通过对材料循环前后物理化学性质和电化学性能的比较,探讨了造成容量衰减的原因,并以此为依据,分别采用双掺杂、碳包覆和扩渗改性的新方法提升LiNi_(0.5)Mn_(1.5)O)_4材料的电化学性能。
锂盐的选择会导致LiNi_(0.5)Mn_(1.5)O)_4材料物理化学性质和电化学性能产生差异。乙酸锂制备的材料粒径较小,结晶度较差;氢氧化锂制备的正极材料具有较高的结晶度,进而表现出更优的电化学性能。随煅烧温度的升高或煅烧时间的延长,产物粒径尺寸呈增大趋势,结晶度提高,Mn~(3+)离子含量增多。研究发现高结晶度的材料具有优异的循环性能;小粒径材料具有更高的初始放电容量,但容量衰减严重;Mn~(3+)离子含量高的材料表现出更佳的倍率性能。研究发现过高的煅烧温度或过长的煅烧时间会导致LiNi_(0.5)Mn_(1.5)O)_4材料分解的新现象,经深入的探讨,提出了分解机制。
提出Fe~(3+)和F-离子双掺杂的方式对LiNi_(0.5)Mn_(1.5)O)_4材料进行改性。除制备了LiNi_(0.4)Mn_(1.5)Fe_(0.1)O_(3.95)F_(0.05)和LiNi_(0.475)Mn_(1.425)Fe_(0.1)O_(3.95)F_(0.05)材料,尝试了锰离子被取代(LiNi_(0.5)Mn_(1.4)Fe_(0.1)O_(3.95)F_(0.05))和引入空位(LiNi_(0.325)Mn_(1.5)Fe_(0.1)O_(3.95)F_(0.05))的改性新策略。双掺杂改性不会改变LiNi_(0.5)Mn_(1.5)O)_4材料的结构类型,能提高材料结构稳定性和产物纯度。研究发现双掺杂改性可不同程度地提升LiNi_(0.5)Mn_(1.5)O)_4正极材料的容量保持率和倍率性能。Fe~(3+)和F-离子的取代会导致材料中Mn~(3+)离子含量的改变。Mn~(3+)离子一方面可提高材料的电导率,利于提高材料的电化学反应活性;但同时也加剧材料与电解液的副反应,促进固体电解质界面(SEI)膜的形成和增厚,从而抑制电子和离子的传输。故材料电化学性能的改性效果是上述综合作用的结果。总体而言,使得材料中Mn~(3+)离子含量减少的改性方式,更利于提高容量保持率;而使材料中Mn~(3+)离子含量增多的改性方式,则更利于提高倍率性能。LiNi_(0.5)Mn_(1.4)Fe_(0.1)O_(3.95)F_(0.05)具有最佳的循环稳定性,100次循环后的容量保持率高达95.1% ; LiNi_(0.4)Mn_(1.5)_Fe_(0.1)O_(3.95)F_(0.05) 5C放电倍率下的容量为110.4mAh g~(-1) ;LiNi_(0.475)Mn_(1.425)Fe_(0.1)O_(3.95)F_(0.05)呈现出优异的综合性能,100次循环后的容量保持率为92.0%,而5C放电倍率下的容量为111.4mAh g~(-1)。研究发现空位的存在可提高锂离子在材料体相中的扩散速率和Mn~(3+)离子含量,从而该改性材料呈现出最佳的倍率性能。LiNi_(0.325)Mn_(1.5)Fe_(0.1)O_(3.95)F_(0.05) 10C放电倍率下的容量高达125mAh g~(-1), 40次循环后的容量保持率为90.7%。
采用蔗糖分解碳包覆的方法对LiNi_(0.5)Mn_(1.5)O)_4材料进行改性,系统地考察不同蔗糖使用量对材料物理化学性质和电化学性能的影响。研究发现,碳包覆改性未改变材料的结构,也不会还原Mn~(4+)离子。蔗糖使用量的增加会增多改性材料中的碳含量、增厚碳包覆层、提高电子和锂离子的传递速率以及增大颗粒的团聚程度。碳包覆改性未影响材料的放电行为,但显著提升循环和倍率性能。蔗糖使用量为1mass%的改性材料具有最佳的电化学性能,其1C倍率下的放电容量为129.8mAh g~(-1),100次循环后的容量保持率高达92.8%;5C放电倍率下的容量达114.2mAh g~(-1)。采用EIS表征分析了改性材料电化学性能提升的原因,其是由正极材料和电解液间副反应的显著抑制以及电子和锂离子动力学性质的提高所致;不同碳含量包覆改性提升电化学性能的差异是由不同的电导率和锂离子扩散能力的提高程度以及不同的颗粒团聚程度所致。
提出扩渗的方法对LiNi_(0.5)Mn_(1.5)O)_4材料进行改性。扩渗改性使氧化铬进入材料晶格中,并使Cr~(3+)离子富集在材料表面,形成LiNi0.5-xMn1.5-yCrx+yO4固溶体,从而增强表面结构稳定性。研究结果证实虽然氧化铬的使用量很少,但扩渗改性可显著地提升材料的循环和倍率稳定性。扩渗改性材料0.2C倍率下的放电容量为130.6mAh g~(-1),100次循环后容量保持率高达96.2%;经一系列不同倍率放电测试后,其0.2C、0.5C、1C、3C和5C倍率下的放电容量仍可达其首次对应容量的100%、99.8%、100%、99.7%和99.6%。采用EIS表征对电化学性能提升的机制进行了探讨,结果显示扩渗改性能有效地抑制SEI膜电阻,说明显著提高的电化学稳定性是由材料和电解液界面反应活性的降低所致。
5V cathode material LiNi_(0.5)Mn_(1.5)O)_4 is considered as one of the most promising cathode materials for next generation of advanced lithium ion battery due to its large capacity and high discharge plateau at 4.7V. These distinctive characters can not only meet the demands of novel power sources from individual electronic consumer products and large-scale power-driven devices, but also accommodate the anode materials with high working voltage for enhancing the safety property of batteries. The key problems which are desiderated to be solved for LiNi_(0.5)Mn_(1.5)O)_4 are to
improve the cycling stability and the rate capability. Therefore, this study is focused on preparation and modification of LiNi_(0.5)Mn_(1.5)O)_4. Through investigating the influence of preparation technologies on the physicochemical properties and electrochemical performances of the as-prepared material, the growth of LiNi_(0.5)Mn_(1.5)O)_4 and the relationship between the structure and morphology of material and its electrochemical performances are explored. By the comparisons on physicochemical properties and electrochemical performances of the materials before and after cycling, the reasons of capacity fading are discussed. Besides, the electrochemical performances of the LiNi_(0.5)Mn_(1.5)O)_4 cathode material are enhanced by the new methods of co-doping, carbon coating and diffusion modifications, respectively.
The selection of lithium source can give rise to the differences in physicochemical and electrochemical performances of LiNi_(0.5)Mn_(1.5)O)_4 material. The product prepared by lithium acetate has smaller particle size and lower crystallinity. In contrast, the cathode material prepared by lithium hydroxide possesses higher crystallinity and better electrochemical performance. Raising the calcination temperature or prolonging holding time results in the increasing tendency of particle size, the enhancement in crystallinity and the increment of Mn~(3+) ion. The results show that the material with high crystallinity has good cyclability, the material with small particle size delivers larger initial discharge capacity while its capacity fading is serious, and the material with higher Mn~(3+) content presents better rate capability. However, it is found that over-high calcination temperature or overlong calcination time results in the new observation of LiNi_(0.5)Mn_(1.5)O)_4 decomposition. A decomposition mechanism is proposed.
The method of Fe~(3+) and F- ions co-doping is used to modify the LiNi_(0.5)Mn_(1.5)O)_4 cathode material. Not only the LiNi_(0.4)Mn_(1.5)Fe_(0.1)O_(3.95)F_(0.05) and LiNi_(0.475)Mn_(1.425)Fe_(0.1)O_(3.95)F_(0.05) materials are prepared, but also the new modification strategies by the syntheses of the Mn-substituted LiNi0.5Mn_(1.4)Fe_(0.1)O_(3.95)F_(0.05) and deficiency-introduced LiNi_(0.325)Mn_(1.5)Fe_(0.1)O_(3.95)F_(0.05) modified materials are attempted. The co-doping modifications do not change the crystal structure type of LiNi_(0.5)Mn_(1.5)O)_4, but can improve the structural stability and the purity of products. The results show that the co-doping modifications can enhance the capacity retention and rate capability of LiNi_(0.5)Mn_(1.5)O)_4 cathode material more or less. The substitutes with Fe~(3+) and F- ions result in the changes of Mn~(3+) content. On the one hand, the Mn~(3+) ion can raise the electronic conductivity, which facilitates the enhancement in electrochemical reactivity of material. On the other hand, the Mn~(3+) ion aggravates the side reaction between the cathode material and the electrolyte, which stimulates the formation and development of the solid electrolyte interfacial (SEI) film as well as consequently hinders the electronic and ionic transfers. Therefore, the modification effect on electrochemical performance of material is attributed to the combination of above two factors. Overall, the modification pattern resulting in the decrease of Mn~(3+) ion in material facilitates the enhancement of capacity retention, and the modification pattern resulting in the increase of Mn~(3+) ion in material facilitates the enhancement of rate capability. LiNi0.5Mn_(1.4)Fe_(0.1)O_(3.95)F_(0.05) has the best cycling stability, and its capacity retention is as high as 95.1% after 100 cycles. The discharge capacity at 5C rate of LiNi0.4Mn1.5Fe0.1O_(3.95)F_(0.05) is 110.4mAh g~(-1). The LiNi0.475Mn1.425Fe0.1O_(3.95)F_(0.05) presents the outstanding combination property, its capacity retention is 92% after 100 cycles and the discharge capacity at 5C rate is 111.4mAh g~(-1). Besides, it is found that the existence of deficiency can increase the diffusion rate of lithium ion in bulk material and the Mn~(3+) ion amount, therefore the material with deficiency displays the best rate capability. LiNi_(0.325)Mn_(1.5)Fe_(0.1)O_(3.95)F_(0.05) can deliver a high discharge capacity of 125mAh g~(-1) at 10C rate with the capacity retention of 90.7% after 40 cycles.
The carbon coating method is applied to modify the LiNi_(0.5)Mn_(1.5)O)_4 cathode material through the thermal decomposition of sucrose, and the influence of sucrose amount on physicochemical property and electrochemical performance of material is systematically investigated for LiNi_(0.5)Mn_(1.5)O)_4. It is found that the carbon coating modification does not change the structure of materials and cause the reduction of Mn~(4+) ion. The increment of sucrose increases the carbon amount in modified materials, thickens the carbon layer, accelerates the transfer rate of electron and ion as well as increases the agglomeration degree of particle. The carbon coating modification can significantly enhance the cycling and rate performances of cathode material without the adverse effect on discharge behavior. The modified material by 1mass% sucrose exhibits the best electrochemical performance, the discharge capacity of 129.8mAh g~(-1) at 1C rate with high capacity retention of 92.8% after 100 cycles and the discharge capacity of 114.2mAh g~(-1) at 5C rate are obtained. Through the analysis of EIS characterization, the enhanced electrochemical performance of the modified material is caused by the remarkable suppression of side reactions between the cathode material and the electrolyte as well as the enhancements of electronic kinetics and lithium ion kinetics. The differences of electrochemical improvement originated from the carbon coating with different carbon contents are attributed to the different improvement degrees of the electronic conductivity and the lithium diffusion capacity as well as the different agglomeration degrees of particles.
The diffusion method is proposed to modify the LiNi_(0.5)Mn_(1.5)O)_4 material. It is found that the diffusion modification allows the chromium oxide to enter into the lattice of material and causes the enrichment of Cr~(3+) ion at the surface of material to form the LiNi0.5-xMn1.5-yCrx+yO4 solid solution. Therefore, the surface structural stability is enhanced. The results confirm that the diffusion modification can significantly promote the cycling and rate stabilities of material, even though the application amount of Cr2O3 is quite low. The diffusion modified material delivers a discharge capacity of 130.6mAh g~(-1) at 0.2C rate with high capacity retention of 96.2% after 100 cycles. In addition, after a series of discharge tests at different rates, this modified material can still exhibits 100%, 99.8%, 100%, 99.7% and 99.6% of its initial capacities at corresponding 0.2C, 0.5C, 1C, 3C and 5C rates, respectively. The mechanism of the enhancement in electrochemical performance is investigated through the EIS characterization. Results show that the diffusion modification effectively suppresses the SEI film resistance, indicating that the dramatically improved electrochemical stability is caused by the reduction of reactivity at the interface of active material and the electrolyte
本研究针对LiNi_(0.5)Mn_(1.5)O)_4存在循环稳定性和倍率放电性能亟待改善和提高这一关键问题,开展制备和改性研究。考察制备工艺对材料物理化学性质和电化学性能的影响,探索LiNi_(0.5)Mn_(1.5)O)_4的生长规律及材料的结构和形貌与电化学性能间的联系。通过对材料循环前后物理化学性质和电化学性能的比较,探讨了造成容量衰减的原因,并以此为依据,分别采用双掺杂、碳包覆和扩渗改性的新方法提升LiNi_(0.5)Mn_(1.5)O)_4材料的电化学性能。
锂盐的选择会导致LiNi_(0.5)Mn_(1.5)O)_4材料物理化学性质和电化学性能产生差异。乙酸锂制备的材料粒径较小,结晶度较差;氢氧化锂制备的正极材料具有较高的结晶度,进而表现出更优的电化学性能。随煅烧温度的升高或煅烧时间的延长,产物粒径尺寸呈增大趋势,结晶度提高,Mn~(3+)离子含量增多。研究发现高结晶度的材料具有优异的循环性能;小粒径材料具有更高的初始放电容量,但容量衰减严重;Mn~(3+)离子含量高的材料表现出更佳的倍率性能。研究发现过高的煅烧温度或过长的煅烧时间会导致LiNi_(0.5)Mn_(1.5)O)_4材料分解的新现象,经深入的探讨,提出了分解机制。
提出Fe~(3+)和F-离子双掺杂的方式对LiNi_(0.5)Mn_(1.5)O)_4材料进行改性。除制备了LiNi_(0.4)Mn_(1.5)Fe_(0.1)O_(3.95)F_(0.05)和LiNi_(0.475)Mn_(1.425)Fe_(0.1)O_(3.95)F_(0.05)材料,尝试了锰离子被取代(LiNi_(0.5)Mn_(1.4)Fe_(0.1)O_(3.95)F_(0.05))和引入空位(LiNi_(0.325)Mn_(1.5)Fe_(0.1)O_(3.95)F_(0.05))的改性新策略。双掺杂改性不会改变LiNi_(0.5)Mn_(1.5)O)_4材料的结构类型,能提高材料结构稳定性和产物纯度。研究发现双掺杂改性可不同程度地提升LiNi_(0.5)Mn_(1.5)O)_4正极材料的容量保持率和倍率性能。Fe~(3+)和F-离子的取代会导致材料中Mn~(3+)离子含量的改变。Mn~(3+)离子一方面可提高材料的电导率,利于提高材料的电化学反应活性;但同时也加剧材料与电解液的副反应,促进固体电解质界面(SEI)膜的形成和增厚,从而抑制电子和离子的传输。故材料电化学性能的改性效果是上述综合作用的结果。总体而言,使得材料中Mn~(3+)离子含量减少的改性方式,更利于提高容量保持率;而使材料中Mn~(3+)离子含量增多的改性方式,则更利于提高倍率性能。LiNi_(0.5)Mn_(1.4)Fe_(0.1)O_(3.95)F_(0.05)具有最佳的循环稳定性,100次循环后的容量保持率高达95.1% ; LiNi_(0.4)Mn_(1.5)_Fe_(0.1)O_(3.95)F_(0.05) 5C放电倍率下的容量为110.4mAh g~(-1) ;LiNi_(0.475)Mn_(1.425)Fe_(0.1)O_(3.95)F_(0.05)呈现出优异的综合性能,100次循环后的容量保持率为92.0%,而5C放电倍率下的容量为111.4mAh g~(-1)。研究发现空位的存在可提高锂离子在材料体相中的扩散速率和Mn~(3+)离子含量,从而该改性材料呈现出最佳的倍率性能。LiNi_(0.325)Mn_(1.5)Fe_(0.1)O_(3.95)F_(0.05) 10C放电倍率下的容量高达125mAh g~(-1), 40次循环后的容量保持率为90.7%。
采用蔗糖分解碳包覆的方法对LiNi_(0.5)Mn_(1.5)O)_4材料进行改性,系统地考察不同蔗糖使用量对材料物理化学性质和电化学性能的影响。研究发现,碳包覆改性未改变材料的结构,也不会还原Mn~(4+)离子。蔗糖使用量的增加会增多改性材料中的碳含量、增厚碳包覆层、提高电子和锂离子的传递速率以及增大颗粒的团聚程度。碳包覆改性未影响材料的放电行为,但显著提升循环和倍率性能。蔗糖使用量为1mass%的改性材料具有最佳的电化学性能,其1C倍率下的放电容量为129.8mAh g~(-1),100次循环后的容量保持率高达92.8%;5C放电倍率下的容量达114.2mAh g~(-1)。采用EIS表征分析了改性材料电化学性能提升的原因,其是由正极材料和电解液间副反应的显著抑制以及电子和锂离子动力学性质的提高所致;不同碳含量包覆改性提升电化学性能的差异是由不同的电导率和锂离子扩散能力的提高程度以及不同的颗粒团聚程度所致。
提出扩渗的方法对LiNi_(0.5)Mn_(1.5)O)_4材料进行改性。扩渗改性使氧化铬进入材料晶格中,并使Cr~(3+)离子富集在材料表面,形成LiNi0.5-xMn1.5-yCrx+yO4固溶体,从而增强表面结构稳定性。研究结果证实虽然氧化铬的使用量很少,但扩渗改性可显著地提升材料的循环和倍率稳定性。扩渗改性材料0.2C倍率下的放电容量为130.6mAh g~(-1),100次循环后容量保持率高达96.2%;经一系列不同倍率放电测试后,其0.2C、0.5C、1C、3C和5C倍率下的放电容量仍可达其首次对应容量的100%、99.8%、100%、99.7%和99.6%。采用EIS表征对电化学性能提升的机制进行了探讨,结果显示扩渗改性能有效地抑制SEI膜电阻,说明显著提高的电化学稳定性是由材料和电解液界面反应活性的降低所致。
5V cathode material LiNi_(0.5)Mn_(1.5)O)_4 is considered as one of the most promising cathode materials for next generation of advanced lithium ion battery due to its large capacity and high discharge plateau at 4.7V. These distinctive characters can not only meet the demands of novel power sources from individual electronic consumer products and large-scale power-driven devices, but also accommodate the anode materials with high working voltage for enhancing the safety property of batteries. The key problems which are desiderated to be solved for LiNi_(0.5)Mn_(1.5)O)_4 are to
improve the cycling stability and the rate capability. Therefore, this study is focused on preparation and modification of LiNi_(0.5)Mn_(1.5)O)_4. Through investigating the influence of preparation technologies on the physicochemical properties and electrochemical performances of the as-prepared material, the growth of LiNi_(0.5)Mn_(1.5)O)_4 and the relationship between the structure and morphology of material and its electrochemical performances are explored. By the comparisons on physicochemical properties and electrochemical performances of the materials before and after cycling, the reasons of capacity fading are discussed. Besides, the electrochemical performances of the LiNi_(0.5)Mn_(1.5)O)_4 cathode material are enhanced by the new methods of co-doping, carbon coating and diffusion modifications, respectively.
The selection of lithium source can give rise to the differences in physicochemical and electrochemical performances of LiNi_(0.5)Mn_(1.5)O)_4 material. The product prepared by lithium acetate has smaller particle size and lower crystallinity. In contrast, the cathode material prepared by lithium hydroxide possesses higher crystallinity and better electrochemical performance. Raising the calcination temperature or prolonging holding time results in the increasing tendency of particle size, the enhancement in crystallinity and the increment of Mn~(3+) ion. The results show that the material with high crystallinity has good cyclability, the material with small particle size delivers larger initial discharge capacity while its capacity fading is serious, and the material with higher Mn~(3+) content presents better rate capability. However, it is found that over-high calcination temperature or overlong calcination time results in the new observation of LiNi_(0.5)Mn_(1.5)O)_4 decomposition. A decomposition mechanism is proposed.
The method of Fe~(3+) and F- ions co-doping is used to modify the LiNi_(0.5)Mn_(1.5)O)_4 cathode material. Not only the LiNi_(0.4)Mn_(1.5)Fe_(0.1)O_(3.95)F_(0.05) and LiNi_(0.475)Mn_(1.425)Fe_(0.1)O_(3.95)F_(0.05) materials are prepared, but also the new modification strategies by the syntheses of the Mn-substituted LiNi0.5Mn_(1.4)Fe_(0.1)O_(3.95)F_(0.05) and deficiency-introduced LiNi_(0.325)Mn_(1.5)Fe_(0.1)O_(3.95)F_(0.05) modified materials are attempted. The co-doping modifications do not change the crystal structure type of LiNi_(0.5)Mn_(1.5)O)_4, but can improve the structural stability and the purity of products. The results show that the co-doping modifications can enhance the capacity retention and rate capability of LiNi_(0.5)Mn_(1.5)O)_4 cathode material more or less. The substitutes with Fe~(3+) and F- ions result in the changes of Mn~(3+) content. On the one hand, the Mn~(3+) ion can raise the electronic conductivity, which facilitates the enhancement in electrochemical reactivity of material. On the other hand, the Mn~(3+) ion aggravates the side reaction between the cathode material and the electrolyte, which stimulates the formation and development of the solid electrolyte interfacial (SEI) film as well as consequently hinders the electronic and ionic transfers. Therefore, the modification effect on electrochemical performance of material is attributed to the combination of above two factors. Overall, the modification pattern resulting in the decrease of Mn~(3+) ion in material facilitates the enhancement of capacity retention, and the modification pattern resulting in the increase of Mn~(3+) ion in material facilitates the enhancement of rate capability. LiNi0.5Mn_(1.4)Fe_(0.1)O_(3.95)F_(0.05) has the best cycling stability, and its capacity retention is as high as 95.1% after 100 cycles. The discharge capacity at 5C rate of LiNi0.4Mn1.5Fe0.1O_(3.95)F_(0.05) is 110.4mAh g~(-1). The LiNi0.475Mn1.425Fe0.1O_(3.95)F_(0.05) presents the outstanding combination property, its capacity retention is 92% after 100 cycles and the discharge capacity at 5C rate is 111.4mAh g~(-1). Besides, it is found that the existence of deficiency can increase the diffusion rate of lithium ion in bulk material and the Mn~(3+) ion amount, therefore the material with deficiency displays the best rate capability. LiNi_(0.325)Mn_(1.5)Fe_(0.1)O_(3.95)F_(0.05) can deliver a high discharge capacity of 125mAh g~(-1) at 10C rate with the capacity retention of 90.7% after 40 cycles.
The carbon coating method is applied to modify the LiNi_(0.5)Mn_(1.5)O)_4 cathode material through the thermal decomposition of sucrose, and the influence of sucrose amount on physicochemical property and electrochemical performance of material is systematically investigated for LiNi_(0.5)Mn_(1.5)O)_4. It is found that the carbon coating modification does not change the structure of materials and cause the reduction of Mn~(4+) ion. The increment of sucrose increases the carbon amount in modified materials, thickens the carbon layer, accelerates the transfer rate of electron and ion as well as increases the agglomeration degree of particle. The carbon coating modification can significantly enhance the cycling and rate performances of cathode material without the adverse effect on discharge behavior. The modified material by 1mass% sucrose exhibits the best electrochemical performance, the discharge capacity of 129.8mAh g~(-1) at 1C rate with high capacity retention of 92.8% after 100 cycles and the discharge capacity of 114.2mAh g~(-1) at 5C rate are obtained. Through the analysis of EIS characterization, the enhanced electrochemical performance of the modified material is caused by the remarkable suppression of side reactions between the cathode material and the electrolyte as well as the enhancements of electronic kinetics and lithium ion kinetics. The differences of electrochemical improvement originated from the carbon coating with different carbon contents are attributed to the different improvement degrees of the electronic conductivity and the lithium diffusion capacity as well as the different agglomeration degrees of particles.
The diffusion method is proposed to modify the LiNi_(0.5)Mn_(1.5)O)_4 material. It is found that the diffusion modification allows the chromium oxide to enter into the lattice of material and causes the enrichment of Cr~(3+) ion at the surface of material to form the LiNi0.5-xMn1.5-yCrx+yO4 solid solution. Therefore, the surface structural stability is enhanced. The results confirm that the diffusion modification can significantly promote the cycling and rate stabilities of material, even though the application amount of Cr2O3 is quite low. The diffusion modified material delivers a discharge capacity of 130.6mAh g~(-1) at 0.2C rate with high capacity retention of 96.2% after 100 cycles. In addition, after a series of discharge tests at different rates, this modified material can still exhibits 100%, 99.8%, 100%, 99.7% and 99.6% of its initial capacities at corresponding 0.2C, 0.5C, 1C, 3C and 5C rates, respectively. The mechanism of the enhancement in electrochemical performance is investigated through the EIS characterization. Results show that the diffusion modification effectively suppresses the SEI film resistance, indicating that the dramatically improved electrochemical stability is caused by the reduction of reactivity at the interface of active material and the electrolyte
引文
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