摘要
太阳能光伏发电是一种重要的绿色可再生能源,具有很好的发展前景,成为国际研究和产业的热点。近10年来,晶体硅太阳电池一直占据太阳能光伏市场的主体地位,约90%的太阳电池由晶体硅制造。因此,高效率和低成本的晶体硅太阳电池成为人们长期追求的目标,而晶体硅中杂质和缺陷以及它们对太阳电池效率的影响则是关键的科学问题。
围绕低成本高效率太阳电池用硅晶体材料,本文发明了低成本铝硅熔体法制备多晶硅技术,开发了低成本高效铸造准单晶硅晶体生长技术和低翘曲薄片太阳电池制备关键技术,同时对低成本技术制备的多晶硅原料(UMG)和铸造准单晶硅材料等进行了杂质与缺陷方面的系统研究,并对太阳电池制备技术的改进方法阐述了相关机理。本文取得了如下主要的创新结果：
(1)发明了一种利用铝硅熔体提纯多晶硅原材料的方法。利用铝硅合金较低的共熔点,实现了在较低温度下对金属硅的有效提纯；研究了杂质铝对晶体硅及太阳电池性能的影响,发现杂质铝在硅中会形成深能级缺陷,导致少子寿命的降低,从而引起电池效率的降低：同时指出,含铝的晶体硅太阳电池不存在效率的光致衰减。
(2)研究了铸造准单晶硅材料及太阳电池的性能。铸造准单晶硅氧含量较低,硼氧复合体缺陷较少,没有晶界,但有较高的位错密度(104～106cm-2)；铸造准单晶硅太阳电池效率绝对值比铸造多晶硅电池高1%左右,其中材料因素和反射率因素各占约0.3%和0.7%；同时,与普通掺硼直拉单晶硅相比,铸造准单晶电池的光致衰减要小很多,但电池效率平均低0.5%。
(3)研究了铸造准单晶硅材料中的主要杂质与缺陷行为和物理机制。研究发现,少量的分散的位错对少子寿命以及电池性能的影响不大,但这种影响随密度的增大而增大,而位错聚集体是一种危害很大的缺陷,它会大幅降低材料的机械和电学性能,严重影响电池效率,并且无法通过电池工艺消除；铸造准单晶硅底部少子寿命低主要因为铁杂质的作用,论文通过实验和模拟计算证实,铸造准单晶硅底部低少子寿命区域的形成是坩埚和氮化硅涂层中铁向硅中扩散以及初始凝固的富铁层向两侧扩散共同作用的结果；铸造准单晶硅中位错对硅中硼氧复合体缺陷具有直接影响,高密度的位错会影响硼氧复合体的形成动力学参数,但对其热力学行为不构成影响,在高密度的硅样品中,硼氧复合体形成激活能为0.57±0.02eV,形成速率常数为1.3×105s-1,比无位错硅中高两个数量级,这是因为位错在p型硅中引入带电价态,从而增加了硼氧复合体形成动力学中瞬态复合中心过程必需的空穴俘获势垒。
(4)研究了低翘曲薄片太阳电池技术。研究提出了利用金属纳米颗粒催化的新型制绒方法：通过优化银纳米颗粒的大小和制绒时间,在硅表面形成了规则排列的微孔金宇塔结构,实验和理论计算证实了这种结构在全波长段内都具有极低的反射率,但基于常规电池工艺制备的太阳电池效率反而下降,这可能是由于多孔结构造成了严重的表面复合并与扩磷过程不兼容的原因。研究还提出了一种新的铝背场技术,通过调制含硼的铝浆并降低铝浆的印刷厚度,实现了减小电池翘曲和降低碎片率的目的：由于硼在硅中固溶度较铝高,这种在硅片背面形成的掺硼铝背场在同样的烧结温度下,硼铝背场的掺杂浓度可以提高一个数量级,因此在低温烧结(≤800℃)条件下降低了硅片的背复合速率以及硅和铝接触电阻,使电池性能在铝浆厚度变化前后保持不变。
As an important renewable energy, photovoltaics (PV) have a promising future and have caught the eyes of the world. Crystalline silicon solar cell has been dominating the PV market in the past ten years. About90%of solar modules are based on crystalline silicon. As a result, low cost and high efficiency solar cells are the long-term objective and trend while scientific issues related to impurities and defects in silicon and their effects on solar cells are significant.
Towards low cost high efficiency solar grade crystalline silicon materials, aluminum-silicon melt method for solar grade poly-silicon, cast quasi-single crystalline (QSC) silicon technique and low bowing solar cell process for thin wafers were proposed in the study of this thesis. Based on the material prepared by these methods, systematic researches were carried out on the impurities and defects in silicon. Besides, detailed researches were conducted on the mechanism of solar cell process. In the following are the innovative results of this thesis.
(1) Aluminum-silicon melt purification process was invented to fabricate solar grade poly-silicon. By means of low eutectic point of aluminum and silicon, metallurgical grade silicon can be effectively purified under a comparatively low temperature. The effect of aluminum in silicon on the performance of silicon and solar cells was also investigated. Aluminum is an active impurity in silicon. It can introduce deep energy level defects in silicon, leading to the reduction of the minority carrier lifetime (MCL) and the solar cell efficiency. In addition, aluminum-containing silicon solar cells have no light-induced degradation (LID) in efficiency.
(2) The performance of QSC silicon and the corresponding solar cells were studied. It is found that QSC silicon contains fewer oxygen and thus fewer boron-oxygen complex defects. Besides, QSC silicon has better quality, i.e. few grain boundaries (GB) and dislocation density in the range of104～106cm-2. Compared to cast multicrystalline (me) silicon, The absolute efficiency of QSC silicon solar cells is1%higher, to which the material quality aspect and reflection reduction aspect contribute0.3%and0.7%, respectively. Compared to commercial boron-doped Czochralski (CZ)-silicon, QSC silicon has higher productivity but the average efficiency is0.5%lower absolutely but smaller LID in efficiency.
(3) The behaviors of main impurity and defects in QSC-silicon were studied. It is revealed that small quantities of scattered dislocations have little influence on the MCL and solar cell performance, but the adverse effect aggravates with the increase of dislocation density. The dislocation aggregates is disastrous. It can significantly degrade the mechanical and electrical performance of material, the performance of solar cells, and the recovery capacity of solar cells by fabrication process. The low MCL zone at the bottom of QSC silicon ingot is mainly ascribed to the high concentration of iron in this region. Besides, there are two iron concentration peaks from the bottom, one at the inner face of crucible bottom, and the other occurring at a height of several centimeters above the initial solid-liquid interface. It is revealed by both experiments and simulation that the diffusion of iron into the crystal from both the quartz crucible and the iron-rich layer formed at the initial stage of the whole crystallization process is responsible for the generation of two-peak characteristics. The interactions between defects in QSC silicon were studied. As example, dislocations have direct influence on the boron-oxygen complex defect. It is found that high density dislocation has influence on the kinetics but not dynamics of boron-oxygen complex generation. In the samples with high density dislocations, the activation energy of boron-oxygen complex generation is0.57±0.02eV and the pre-exponential factor is1.3×105s-1, which is two orders of magnitude higher than that of dislocation-free silicon. It is believed that the dislocation-related electronic states charged with holes can cause an energy potential barrier for the capture of single-positive holes that is required for the transformation of B-O complexes from latent centers to immediate transient centers.
(4) The low bowing solar cell processes for thin wafers were studied. By means of silver nano-particles as catalyst, surface reflection of silicon can be modulated. Both experiments and theoretical analysis have proved that a well-organized microporous structure on the pyramids can be obtained by optimizing the size of Ag nanoparticles and the texturing time, and the silicon wafer with such structures can effectively reduce the reflectivity of sunlight. However, based on the conventional cell fabrication process, the performance of silicon solar cells with such microporous structures gets degraded. It is closely associated with the strong surface recombination and the high phosphorus diffusion barrier induced by the microporous textures. A novel aluminum back surface field (BSF) process has been invented and studied. The reduction of bowing and crack of solar cells is achieved by modulating boron-containing aluminum paste and reducing the paste thickness. This approach can form boron-containing Al-BSF. Due to the higher solid solubility of boron in silicon, the dopant concentration in BSF layer can be increased by one order of magnitude. Therefore, at low firing temperature (≤800℃), the backside recombination velocity of silicon and the contact resistance between silicon and aluminum have been reduced while these is little influence on the solar cell performance.
引文
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