三维纳米结构电极的制备及作为锂离子电池负极的应用
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摘要
锂离子电池具有绿色无污染、功率密度大、循环寿命长等诸多优点,已广泛应用于手机、笔记本电脑等产品中,其发展对工业、科技有重要的影响。近年来,动力型、功率型设备的大量应用对锂离子电池提出了更高的要求,从而推动了锂离子电池向具有更高的能量密度与功率密度,更长的循环寿命和更宽广的工作温度范围等方向发展。
三维纳米结构电极是近年来锂离子电池领域研究的一个热点,与传统的电极相比,它有更好的体积膨胀包容性、更强的电子与离子转移能力与更加稳定的机械结构等,因此在充放电过程中会表现出高得多的循环稳定性与倍率性能,被认为是下一代锂离子电池的理想选择之一
本文从活性材料与集流体两方面入手,设计并制造了多种三维纳米结构电极并应用于锂离子电池的负极：在活性材料的结构设计方面,通过水热法制备在Ti衬底原位合成制备得到了Sn02纳米管阵列三维电极；在集流体结构的设计方面,提出了一种简单的大规模制备Cu多孔的纳米结构三维导电网络的方法,基于这种网络,分别合成得到了Si多孔三维纳米结构电极,Ge多孔三维纳米结构电极,Sn多孔三维纳米结构电极,SiGe多孔三维纳米结构电极。此外,通过引入一种Cu纳米线阵列集流体,利用不同合成方法制备得到了Cu-Ge, Cu-Sn, Cu-Si1-xGex, Cu-Mn3O4四种核壳结构纳米线阵列三维电极。上述三维纳米结构电极均表现了较好的电化学性能。
本论文主要的创新点如下：
(1)以ZnO纳米线阵列为模板,采用一种简单的水热法,制备得到了ZnO/SnO2复合物纳米线阵列,利用HCl去除ZnO模板后,首次成功地在金属衬底片上原位合成了Sn02纳米管阵列,其作为三维电极展现了很好的电化学性能。
(2)引入一种Cu纳米线阵列集流体,通过射频溅射、直流溅射、电化学沉积等方法,分别合成得到了Cu-Ge, Cu-Sn, Cu-Si1-xGex, Cu-Mn3O4四种核壳结构纳米线阵列三维电极,这些三维纳米结构电极均表现出了很好的循环稳定性与大电流放电性能。
(3)首次提出引入Ge改善Si活性材料电化学性能,并系统研究了Ge含量对Si负极材料电化学性能的影响。
(4)通过在Cu片衬底上堆积Si02纳米颗粒模板,然后在Si02纳米颗粒的空隙间电化学沉积Cu,最后将模板去除,得到了一种新型的内部相通的三维导电网络,这种导电网络可以作为通用的锂离子电池集流体使用。
(5)基于Cu多孔三维导电网络,通过不同的合成方法制备得到了Si多孔三维纳米结构电极,Ge多孔三维纳米结构电极,Sn多孔三维纳米结构电极,SiGe多孔三维纳米结构电极,在电化学测试中,上述四种三维纳米结构电极比对应的平板电极均表现出了更加优异的性能,具有在锂离子电池应用的潜力。
Lithium-ion batteries have been widely used in portable electronic devices and greatly affect the industry, science and technology due to many advantages such as enviromentally friendly, high power density and long cycle life. Recently, higher power density, longer cycle life, and wider range of working temperature are demanded in lithium-ion batteries because of the fast development of the power type applications.
The three-dimensional (3D) nanostructured electrodes have received great interest for Lithium-ion batteries, which show significant advantages in their kinetics and electronic conduction during the charge-discharge process. Therefore,3D nanostructured electrodes are expected to show higher capacities, good cycling stability and rate capability, and thus have been considered as one of the promising choices for next generation lithium-ion batteries.
In this dissertation, we prepare several kinds of3D nanostructured electrodes for lithium-ion batteries via different ways:we propose a nanoarray template assisted method to obtain SnO2nanotube arrays; we propose a facil template-engaged approach for Cu nanoporous3D current collect, which can support Si, Ge, SiGe and Sn to form porous3D nanostructured electrode; besides, we propose a template-assisted method for Cu nanwire arrays as current collector, which can support Ge, Sn, Si1-xGex and Mn3O4to form3D electrode. Owing to the unique structure, the above-mentioned3D nanostructured electrodes exhibit improved electrochemical performance. The main innovative results are listed as follows:
(1) By using a pre-fabricated ZnO nanowire arrays as sacrificial templates, SnO2layer has been coated onto the surface of ZnO nanowires by a hydrothermal process. After HC1solution etching, SnO2nanotube arrays on titanium substrate are obtained. The as-synthesized SnO2nanotube arrays are applied as anode materials for Li-ion battery, which exhibit high capacity and good cycling performance.
(2) By employing a Cu nanwire arrays as current collector, Cu-Ge, Cu-Sn, Cu-Si1-xGex and Cu-Mn3O4core-shell nanowire arrays3D electrode have been obtained. The four kinds of3D nanostructured electrodes all exhibit good cycling stability and rate capability.
(3) We propose that alloying Ge with Si could improve the electrochemical performance of Si. The effect of Ge content on the electrochemical performance of Si-based materials has also been investigated.
(4) We demonstrate the synthesis of Cu nanoporous three-dimensional network via a simple template-assisted method. The network could be used as a universal current collector for lithium-ion batteries.
(5) By using this3D network as current collector, Si, Ge, SiGe and Sn porous3D nanostructured electrode have been prepared. The as-prepared four kinds of porous3D nanostructured electrodes exhibit improved cycling stability and rate capability compared to corresponding planar electrodes.
三维纳米结构电极是近年来锂离子电池领域研究的一个热点,与传统的电极相比,它有更好的体积膨胀包容性、更强的电子与离子转移能力与更加稳定的机械结构等,因此在充放电过程中会表现出高得多的循环稳定性与倍率性能,被认为是下一代锂离子电池的理想选择之一
本文从活性材料与集流体两方面入手,设计并制造了多种三维纳米结构电极并应用于锂离子电池的负极：在活性材料的结构设计方面,通过水热法制备在Ti衬底原位合成制备得到了Sn02纳米管阵列三维电极；在集流体结构的设计方面,提出了一种简单的大规模制备Cu多孔的纳米结构三维导电网络的方法,基于这种网络,分别合成得到了Si多孔三维纳米结构电极,Ge多孔三维纳米结构电极,Sn多孔三维纳米结构电极,SiGe多孔三维纳米结构电极。此外,通过引入一种Cu纳米线阵列集流体,利用不同合成方法制备得到了Cu-Ge, Cu-Sn, Cu-Si1-xGex, Cu-Mn3O4四种核壳结构纳米线阵列三维电极。上述三维纳米结构电极均表现了较好的电化学性能。
本论文主要的创新点如下：
(1)以ZnO纳米线阵列为模板,采用一种简单的水热法,制备得到了ZnO/SnO2复合物纳米线阵列,利用HCl去除ZnO模板后,首次成功地在金属衬底片上原位合成了Sn02纳米管阵列,其作为三维电极展现了很好的电化学性能。
(2)引入一种Cu纳米线阵列集流体,通过射频溅射、直流溅射、电化学沉积等方法,分别合成得到了Cu-Ge, Cu-Sn, Cu-Si1-xGex, Cu-Mn3O4四种核壳结构纳米线阵列三维电极,这些三维纳米结构电极均表现出了很好的循环稳定性与大电流放电性能。
(3)首次提出引入Ge改善Si活性材料电化学性能,并系统研究了Ge含量对Si负极材料电化学性能的影响。
(4)通过在Cu片衬底上堆积Si02纳米颗粒模板,然后在Si02纳米颗粒的空隙间电化学沉积Cu,最后将模板去除,得到了一种新型的内部相通的三维导电网络,这种导电网络可以作为通用的锂离子电池集流体使用。
(5)基于Cu多孔三维导电网络,通过不同的合成方法制备得到了Si多孔三维纳米结构电极,Ge多孔三维纳米结构电极,Sn多孔三维纳米结构电极,SiGe多孔三维纳米结构电极,在电化学测试中,上述四种三维纳米结构电极比对应的平板电极均表现出了更加优异的性能,具有在锂离子电池应用的潜力。
Lithium-ion batteries have been widely used in portable electronic devices and greatly affect the industry, science and technology due to many advantages such as enviromentally friendly, high power density and long cycle life. Recently, higher power density, longer cycle life, and wider range of working temperature are demanded in lithium-ion batteries because of the fast development of the power type applications.
The three-dimensional (3D) nanostructured electrodes have received great interest for Lithium-ion batteries, which show significant advantages in their kinetics and electronic conduction during the charge-discharge process. Therefore,3D nanostructured electrodes are expected to show higher capacities, good cycling stability and rate capability, and thus have been considered as one of the promising choices for next generation lithium-ion batteries.
In this dissertation, we prepare several kinds of3D nanostructured electrodes for lithium-ion batteries via different ways:we propose a nanoarray template assisted method to obtain SnO2nanotube arrays; we propose a facil template-engaged approach for Cu nanoporous3D current collect, which can support Si, Ge, SiGe and Sn to form porous3D nanostructured electrode; besides, we propose a template-assisted method for Cu nanwire arrays as current collector, which can support Ge, Sn, Si1-xGex and Mn3O4to form3D electrode. Owing to the unique structure, the above-mentioned3D nanostructured electrodes exhibit improved electrochemical performance. The main innovative results are listed as follows:
(1) By using a pre-fabricated ZnO nanowire arrays as sacrificial templates, SnO2layer has been coated onto the surface of ZnO nanowires by a hydrothermal process. After HC1solution etching, SnO2nanotube arrays on titanium substrate are obtained. The as-synthesized SnO2nanotube arrays are applied as anode materials for Li-ion battery, which exhibit high capacity and good cycling performance.
(2) By employing a Cu nanwire arrays as current collector, Cu-Ge, Cu-Sn, Cu-Si1-xGex and Cu-Mn3O4core-shell nanowire arrays3D electrode have been obtained. The four kinds of3D nanostructured electrodes all exhibit good cycling stability and rate capability.
(3) We propose that alloying Ge with Si could improve the electrochemical performance of Si. The effect of Ge content on the electrochemical performance of Si-based materials has also been investigated.
(4) We demonstrate the synthesis of Cu nanoporous three-dimensional network via a simple template-assisted method. The network could be used as a universal current collector for lithium-ion batteries.
(5) By using this3D network as current collector, Si, Ge, SiGe and Sn porous3D nanostructured electrode have been prepared. The as-prepared four kinds of porous3D nanostructured electrodes exhibit improved cycling stability and rate capability compared to corresponding planar electrodes.
引文
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