TW202102726A - Silicon ingot and manufacturing method thereof and anode material for lithium ion battery - Google Patents

Silicon ingot and manufacturing method thereof and anode material for lithium ion battery Download PDF

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TW202102726A
TW202102726A TW108123041A TW108123041A TW202102726A TW 202102726 A TW202102726 A TW 202102726A TW 108123041 A TW108123041 A TW 108123041A TW 108123041 A TW108123041 A TW 108123041A TW 202102726 A TW202102726 A TW 202102726A
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silicon
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TWI785254B (en
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余文懷
吳翰宗
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環球晶圓股份有限公司
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    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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Abstract

Provided is a silicon ingot and a manufacturing method thereof and an anode material for a lithium ion battery. The manufacturing method includes the following steps. A plurality of silicon crystal seeds are arranged in a heating device, wherein each of the silicon crystal seeds has a defect ratio of greater than or equal to 1%. A silicon raw material is placed on the silicon crystal seeds. The silicon crystal seeds and the silicon raw material are heated until the silicon raw material is melted into a silicon melt. The silicon melt is cooled to solidify the silicon melt into a silicon ingot.

Description

矽晶碇及其製造方法與鋰電池的負極材料Silicon crystal ingot, its manufacturing method and negative electrode material of lithium battery

本發明是有關於一種矽晶碇及其製造方法與鋰電池的負極材料。The invention relates to a silicon crystal ingot, a manufacturing method thereof, and a negative electrode material of a lithium battery.

目前半導體或太陽能產業所需的矽晶錠通常需要具有良好的品質（低缺陷比例），以利於半導體元件或太陽能電池的製造。矽晶錠的製造方法一般是先將矽晶種鋪設於坩鍋中，再將矽原料鋪設於矽晶種上。然後，進行加熱，以使坩鍋中的矽原料熔化而形成矽熔體（或可稱為矽熔湯）。之後，對矽熔體進行降溫，以使矽熔體自下部往上固化而形成為矽晶錠。The silicon ingots currently required by the semiconductor or solar energy industry generally need to have good quality (low defect ratio) to facilitate the manufacture of semiconductor components or solar cells. The manufacturing method of silicon ingot is generally to first lay the silicon seed crystal in a crucible, and then lay the silicon raw material on the silicon seed crystal. Then, heating is performed to melt the silicon raw material in the crucible to form a silicon melt (or can be called silicon melt soup). After that, the temperature of the silicon melt is lowered so that the silicon melt is solidified from the bottom up to form a silicon crystal ingot.

為了形成具有良好品質的矽晶錠，通常會將低缺陷比例（小於1%）的矽晶種鋪設於坩鍋中，並且使矽晶種之間的晶界（boundary）數量盡可能減少（通常使晶界數量小於4）。如此一來，後續所形成的矽晶錠即可具有相當低的缺陷比例。然而，當此種低缺陷比例的矽晶錠研磨為矽顆粒來作為鋰電池的負極材料時，由於其本身的材料特性，在充放電時會發生大幅度的體積變化，導致矽顆粒內部的應力無法釋放而導致破裂，使其喪失續電能力，因此難以作為鋰電池的負極材料。In order to form silicon ingots with good quality, silicon seeds with a low defect ratio (less than 1%) are usually laid in the crucible, and the number of boundaries between silicon seeds is minimized (usually Make the number of grain boundaries less than 4). In this way, the subsequently formed silicon crystal ingot can have a relatively low defect ratio. However, when this low defect ratio silicon ingot is ground into silicon particles as the negative electrode material of lithium batteries, due to its own material characteristics, a large volume change occurs during charging and discharging, resulting in stress inside the silicon particles. Unable to release and cause rupture, causing it to lose the ability to continue electricity, so it is difficult to be used as a negative electrode material for lithium batteries.

本發明提供一種矽晶碇的製造方法，其使用缺陷比例大於或等於1%的矽晶種。The present invention provides a method for manufacturing silicon ingots, which uses silicon seed crystals with a defect ratio greater than or equal to 1%.

本發明提供一種矽晶碇，其由上述的製造方法所製造。The present invention provides a silicon ingot manufactured by the above-mentioned manufacturing method.

本發明提供一種鋰電池的負極材料，其包括由上述的矽晶碇製造的矽顆粒。The present invention provides a negative electrode material for a lithium battery, which includes silicon particles made from the above-mentioned silicon ingot.

本發明的矽晶碇的製造方法包括以下步驟。於加熱裝置中排列多個矽晶種，其中每一所述矽晶種的缺陷比例大於或等於1%。於所述矽晶種上放置矽原料。對所述矽晶種與所述矽原料進行加熱，直到所述矽原料熔化為矽熔體。對所述矽熔體進行降溫，以使所述矽熔體固化為矽晶碇。The manufacturing method of the silicon ingot of the present invention includes the following steps. A plurality of silicon seed crystals are arranged in the heating device, and the defect ratio of each of the silicon seed crystals is greater than or equal to 1%. Place silicon raw material on the silicon seed crystal. The silicon seed crystal and the silicon raw material are heated until the silicon raw material is melted into a silicon melt. The temperature of the silicon melt is lowered so that the silicon melt is solidified into silicon ingots.

在本發明的矽晶碇的製造方法的一實施例中，相鄰的兩個所述矽晶種的晶向夾角大於0度且小於或等於5度。In an embodiment of the method for manufacturing a silicon ingot of the present invention, the angle between the crystal orientations of two adjacent silicon seed crystals is greater than 0 degrees and less than or equal to 5 degrees.

在本發明的矽晶碇的製造方法的一實施例中，相鄰的兩個所述矽晶種之間具有晶界，且在所述排列之後產生數量大於或等於4的晶界。In an embodiment of the method for manufacturing a silicon crystal ingot of the present invention, there are grain boundaries between two adjacent silicon seed crystals, and a number of grain boundaries greater than or equal to 4 are generated after the arrangement.

在本發明的矽晶碇的製造方法的一實施例中，每一所述矽晶種的形狀為多邊形。In an embodiment of the method for manufacturing the silicon ingot of the present invention, the shape of each silicon seed crystal is polygonal.

在本發明的矽晶碇的製造方法的一實施例中，每一所述矽晶種的形狀為四邊形。In an embodiment of the method for manufacturing a silicon crystal ingot of the present invention, the shape of each silicon seed crystal is a quadrilateral.

在本發明的矽晶碇的製造方法的一實施例中，每一所述矽晶種的每一邊長大於或等於5公分。In an embodiment of the manufacturing method of the silicon crystal ingot of the present invention, the length of each side of each silicon seed crystal is greater than or equal to 5 cm.

在本發明的矽晶碇的製造方法的一實施例中，所述矽晶種的材料包括單晶矽、多晶矽或類單晶矽。In an embodiment of the method for manufacturing a silicon ingot of the present invention, the material of the silicon seed crystal includes monocrystalline silicon, polycrystalline silicon or similar monocrystalline silicon.

本發明的矽晶碇包括由上述矽晶碇的製造方法所製造。The silicon ingot of the present invention includes those manufactured by the above-mentioned silicon ingot manufacturing method.

本發明的鋰電池的負極材料包括由上述矽晶碇製造的多個矽顆粒。The negative electrode material of the lithium battery of the present invention includes a plurality of silicon particles made of the above-mentioned silicon crystal ingot.

在本發明的鋰電池的負極材料的一實施例中，所述多個矽顆粒的缺陷比例大於或等於5%。In an embodiment of the negative electrode material of the lithium battery of the present invention, the defect ratio of the plurality of silicon particles is greater than or equal to 5%.

基於上述，本發明使用缺陷比例大於或等於1%的矽晶種來製造矽晶碇，因此所形成的矽晶碇可具有較高的缺陷比例。此外，由於上述的矽晶碇具有較高的缺陷比例，因此適於作為鋰電池的負極材料。Based on the above, the present invention uses silicon seed crystals with a defect ratio greater than or equal to 1% to manufacture silicon ingots, so the formed silicon ingots can have a higher defect ratio. In addition, since the above-mentioned silicon ingot has a high defect ratio, it is suitable as a negative electrode material for lithium batteries.

為讓本發明的上述特徵和優點能更明顯易懂，下文特舉實施例，並配合所附圖式作詳細說明如下。In order to make the above-mentioned features and advantages of the present invention more comprehensible, the following specific embodiments are described in detail in conjunction with the accompanying drawings.

下文列舉實施例並配合所附圖式來進行詳細地說明，但所提供的實施例並非用以限制本發明所涵蓋的範圍。此外，圖式僅以說明為目的，並未依照原尺寸作圖。為了方便理解，在下述說明中相同的元件將以相同的符號標示來說明。另外，關於文中所使用「包含」、「包括」、「具有」等等用語，均為開放性的用語，也就是指「包含但不限於」。再者，文中所提到的方向性用語，例如「上」、「下」等，僅是用以參考圖式的方向，並非用來限制本發明。The following examples are listed in conjunction with the accompanying drawings for detailed description, but the provided examples are not intended to limit the scope of the present invention. In addition, the drawings are for illustrative purposes only, and are not drawn in accordance with the original dimensions. To facilitate understanding, the same elements will be described with the same symbols in the following description. In addition, the terms "include", "include", "have" and so on used in the text are all open terms, which means "including but not limited to." Furthermore, the directional terms mentioned in the text, such as "up", "down", etc., are only used to refer to the direction of the drawings, and are not used to limit the present invention.

圖1為依照本發明實施例的矽晶碇的製造方法的流程圖。在本實施例中，所提及的數量與形狀僅用以具體地說明本發明以便於了解其內容，而非用以限定本發明。FIG. 1 is a flowchart of a method for manufacturing a silicon ingot according to an embodiment of the present invention. In this embodiment, the numbers and shapes mentioned are only used to specifically illustrate the present invention so as to understand its content, but not to limit the present invention.

在本發明中，藉由於加熱裝置中鋪設缺陷比例大於或等於1%的矽晶種，可形成具有較高缺陷比例的矽晶碇。上述的矽晶碇可藉由將這些缺陷作為緩衝區域而具有可承受體積膨脹收縮特性，以適於作為鋰電池的負極材料。此外，本發明亦可進一步藉由特定的矽晶種排列方式來使得所形成的矽晶碇具有較高缺陷比例。In the present invention, by laying silicon seed crystals with a defect ratio greater than or equal to 1% in the heating device, a silicon ingot with a higher defect ratio can be formed. The above-mentioned silicon ingots can withstand volume expansion and contraction by using these defects as buffer regions, and are suitable for use as negative electrode materials for lithium batteries. In addition, the present invention can further use a specific arrangement of silicon seed crystals to make the formed silicon crystal ingots have a higher defect ratio.

首先，在步驟100中，提供具有缺陷比例大於或等於1%的矽晶種。在本實施例中，缺陷比例是指在矽晶種中具有缺陷的面積占矽晶種的總面積的比例。此外，在本實施例中，「缺陷」是指矽晶種本質上的缺陷，亦即晶格排列所造成的差排（dislocation），並非外觀上的破損、空穴等缺陷。另外，在本實施例中，矽晶種的材料可以是單晶矽、多晶矽或類單晶矽，本發明不對此作特別限定。在本實施例中，矽晶種的形狀為多邊形，例如三角形、四邊形等，本發明不對此作特別限定。First, in step 100, a silicon seed crystal with a defect ratio greater than or equal to 1% is provided. In this embodiment, the defect ratio refers to the ratio of the area with defects in the silicon seed crystal to the total area of the silicon seed crystal. In addition, in the present embodiment, "defect" refers to the intrinsic defect of the silicon seed crystal, that is, the dislocation caused by the crystal lattice arrangement, and is not the defect of appearance damage, voids, etc. In addition, in this embodiment, the material of the silicon seed crystal can be single crystal silicon, polycrystalline silicon or similar single crystal silicon, which is not particularly limited in the present invention. In this embodiment, the shape of the silicon seed crystal is a polygon, such as a triangle, a quadrilateral, etc., which is not particularly limited in the present invention.

特別一提的是，為了避免本實施例所使用的矽晶種與一般的碎料混淆，本實施例的矽晶種具有一定長度的邊長。舉例來說，每一個矽晶種的每一邊長例如為5公分或大於5公分。In particular, in order to avoid confusion between the silicon seed crystal used in this embodiment and general scraps, the silicon seed crystal of this embodiment has a certain side length. For example, the length of each side of each silicon seed crystal is, for example, 5 cm or more.

接著，在步驟102中，將上述矽晶種排列於加熱裝置中。加熱裝置例如是一般矽晶碇製程中所使用的坩鍋。在本實施例中，將矽晶種以陣列的方式排列於坩鍋的底部。詳細地說，如圖2所示，將四邊形（例如正方形）的矽晶種200以6×6的方式鋪設於坩鍋的底部。此外，相鄰的兩個矽晶種200之間具有晶界202，且因此圖2所示的排列方式產生了60個晶界。另外，相鄰的兩個矽晶種200的晶向夾角大於0度且小於或等於5度。Next, in step 102, the above-mentioned silicon seed crystals are arranged in a heating device. The heating device is, for example, a crucible used in a general silicon crystal ingot manufacturing process. In this embodiment, the silicon seed crystals are arranged in an array at the bottom of the crucible. In detail, as shown in FIG. 2, a quadrilateral (for example, square) silicon seed crystal 200 is laid on the bottom of the crucible in a 6×6 manner. In addition, there are grain boundaries 202 between two adjacent silicon seed crystals 200, and therefore, the arrangement shown in FIG. 2 produces 60 grain boundaries. In addition, the angle between two adjacent silicon seed crystals 200 is greater than 0 degrees and less than or equal to 5 degrees.

在上述的排列方式中，由於以相鄰的兩個矽晶種的晶向夾角大於0度且小於或等於5度的方來進行排列且產生了數量大於或等於4的晶界，因此可使得後續所形成的矽晶碇具有較高缺陷比例。詳細地說，當相鄰的兩個矽晶種的晶向夾角大於0度且小於或等於5度時，可使得所形成的矽晶碇具有因差排而造成的缺陷。此外，當在鋪設矽晶種之後產生數量大於或等於4的晶界時，可藉由晶界間的應力而使得得所形成的矽晶碇具有較高的缺陷比例。In the above arrangement, because the angle between the two adjacent silicon seed crystals is greater than 0 degrees and less than or equal to 5 degrees, and the number of grain boundaries greater than or equal to 4 is generated, it can make The subsequently formed silicon ingot has a higher defect ratio. In detail, when the angle between two adjacent silicon seed crystals is greater than 0 degrees and less than or equal to 5 degrees, the formed silicon ingots may have defects caused by misalignment. In addition, when the number of grain boundaries greater than or equal to 4 is generated after the silicon seed crystal is laid, the silicon crystal ingots formed can have a higher defect ratio due to the stress between the grain boundaries.

換句話說，在本發明中，只要所使用的矽晶種具有大於或等於1%的缺陷比例即可形成具有較高缺陷比例的矽晶碇，且在排列矽晶種時只要晶向夾角與晶界數量符合上述條件即可進一步地提高所形成的矽晶碇的缺陷比例。In other words, in the present invention, as long as the silicon seed crystal used has a defect ratio greater than or equal to 1%, a silicon ingot with a higher defect ratio can be formed, and when the silicon seed crystal is arranged, only the angle between the crystal orientation and If the number of grain boundaries meets the above conditions, the defect ratio of the formed silicon crystal ingot can be further increased.

然後，進行一般熟知的後續製程步驟。舉例來說，在步驟104中，於矽晶種上放置所需量的矽原料。在步驟106中，對坩鍋中的矽晶種與矽原料進行加熱，直到矽原料熔化為矽熔體。在此步驟中，可控制為僅有矽原料全部熔化，或是控制為矽原料全部熔化而矽晶種部分熔化或全部熔化。在步驟108中，對矽熔體進行降溫，以使矽熔體自下部往上固化為矽晶碇。如此一來，即可形成本發明的具有較高缺陷比例的矽晶碇。此外，由於矽熔體自下部往上固化為矽晶碇，因此所形成的矽晶碇自下部往上具有增加的缺陷比例。上述步驟106與步驟108為本領域技術人員所熟知的技術手段，於此不另外進行詳細說明。Then, the well-known subsequent process steps are carried out. For example, in step 104, a required amount of silicon material is placed on the silicon seed crystal. In step 106, the silicon seed crystal and the silicon raw material in the crucible are heated until the silicon raw material melts into a silicon melt. In this step, it can be controlled that only the silicon raw material is completely melted, or it can be controlled such that the silicon raw material is completely melted and the silicon seed crystal is partially melted or completely melted. In step 108, the temperature of the silicon melt is lowered so that the silicon melt is solidified into silicon ingots from the bottom up. In this way, the silicon ingot with a higher defect ratio of the present invention can be formed. In addition, since the silicon melt solidifies into silicon ingots from the bottom to the top, the formed silicon ingots have an increased defect ratio from the bottom to the top. The above step 106 and step 108 are technical means well known to those skilled in the art, and will not be further described in detail here.

以下將以實驗例與比較例來製造矽晶碇並作說明，且相關數據呈現於表1中。In the following, experimental examples and comparative examples are used to manufacture silicon ingots and are described, and the relevant data are presented in Table 1.

實驗例1：以6×6的方式排列缺陷比例大於或等於1%的矽晶種（單晶矽，晶向為(100)，相鄰晶種的晶向夾角大於0度且小於1度，邊長為15.6公分的正方形形狀，缺陷比例為10%）。Experimental example 1: Arrange silicon seed crystals with a defect ratio greater than or equal to 1% in a 6×6 manner (single crystal silicon, crystal orientation is (100), and the angle between adjacent seed crystals is greater than 0 degree and less than 1 degree, A square shape with a side length of 15.6 cm, the defect ratio is 10%).

比較例1：採用高效多晶製程（使用邊長小於1公分的細碎料作為晶種，進行加熱製程以使晶種呈半熔狀態）。Comparative Example 1: Using a high-efficiency polycrystalline process (using fine particles with a side length of less than 1 cm as seed crystals, and performing a heating process to make the seed crystals in a semi-molten state).

比較例2：採用傳統多晶製程（使用任意邊長的矽原料，進行加熱製程以使矽原料呈全熔狀態）。Comparative Example 2: Using a traditional polycrystalline process (using silicon raw materials with any side length, heating process to make the silicon raw materials in a fully molten state).

比較例3：採用類單晶製程（使用邊長大於5公分且缺陷比例小於1%的單晶矽晶種，進行加熱製程以使晶種呈半熔狀態）。Comparative Example 3: Using a single crystal-like process (using a single crystal silicon seed crystal with a side length greater than 5 cm and a defect ratio of less than 1%, and performing a heating process to make the seed crystal in a semi-melted state).

表1   矽晶碇的晶體高度 （mm） 20 60 100 140 180 210 250 比較例1 矽晶碇的缺陷比例 （%） 1 2 3 4 7 9 11 比較例2 1 5 10 18 22 28 30 比較例3 1 3 8 22 30 35 40 實驗例1 10 16 22 30 40 45 50 Table 1 Crystal height of silicon crystal ingot (mm) 20 60 100 140 180 210 250 Comparative example 1 Defect ratio of silicon crystal ingot (%) 1 2 3 4 7 9 11 Comparative example 2 1 5 10 18 twenty two 28 30 Comparative example 3 1 3 8 twenty two 30 35 40 Experimental example 1 10 16 twenty two 30 40 45 50

由表1可以看出，相較於以一般方式製造的矽晶碇（比較例1、比較例2、比較例3），以本發明的製造方法所形成的矽晶碇（實驗例1）在不同的高度區域中皆具有明顯較高的缺陷比例。It can be seen from Table 1 that compared with the conventionally manufactured silicon ingots (Comparative Example 1, Comparative Example 2, and Comparative Example 3), the silicon ingot formed by the manufacturing method of the present invention (Experimental Example 1) is There are obviously higher defect ratios in different height areas.

本發明使用缺陷比例大於或等於1%的矽晶種來製造矽晶碇，因此所形成的矽晶碇可具有較高的缺陷比例。由於矽晶碇中的這些缺陷可作為緩衝區域而使得矽晶碇在膨脹收縮時不會損壞甚至破裂，因此可應用於需要具有可承受體積膨脹收縮特性的材料的元件中，例如作為鋰電池的負極材料。The present invention uses silicon seed crystals with a defect ratio greater than or equal to 1% to manufacture silicon ingots, so the formed silicon ingots can have a higher defect ratio. Since these defects in the silicon ingot can be used as a buffer area so that the silicon ingot will not be damaged or even broken during expansion and contraction, it can be applied to components that require materials that can withstand volume expansion and contraction, such as lithium batteries. Anode material.

此外，對於一般因缺陷比例過高而報廢的矽晶種或矽晶碇來說，本發明可以回收使用這些報廢材料，以達到降低成本以及解決庫存堆積的效果。In addition, for silicon seed crystals or silicon ingots that are generally scrapped due to an excessively high defect ratio, the present invention can recycle these scrapped materials to achieve the effect of reducing costs and solving inventory accumulation.

另外，作為鋰電池的負極材料，通常須採用具有可承受體積膨脹收縮特性的材料，以避免鋰電池的負極在充放電的過程中因體積膨脹收縮而損壞。因此，本發明的矽晶碇適於作為鋰電池的負極材料。In addition, as the negative electrode material of a lithium battery, a material that can withstand volume expansion and contraction is usually used to avoid damage to the negative electrode of the lithium battery due to volume expansion and contraction during the charging and discharging process. Therefore, the silicon ingot of the present invention is suitable as a negative electrode material for lithium batteries.

在形成本發明的矽晶碇之後，將矽晶碇研磨為粒徑界於0.1 μm至50 μm的矽顆粒。由於矽顆粒的缺陷比例與矽晶碇的缺陷比例呈正比，因此這些矽顆粒的缺陷比例可大於或等於5%。之後，將這些矽顆粒應用於鋰電池的負極材料並採用一般的鋰電池負極製程，以形成具有高可靠度的鋰電池負極。After the silicon ingot of the present invention is formed, the silicon ingot is ground into silicon particles with a particle size between 0.1 μm and 50 μm. Since the defect ratio of silicon particles is proportional to the defect ratio of silicon ingots, the defect ratio of these silicon particles can be greater than or equal to 5%. After that, these silicon particles are applied to the negative electrode material of the lithium battery and the general lithium battery negative electrode manufacturing process is adopted to form a lithium battery negative electrode with high reliability.

雖然本發明已以實施例揭露如上，然其並非用以限定本發明，任何所屬技術領域中具有通常知識者，在不脫離本發明的精神和範圍內，當可作些許的更動與潤飾，故本發明的保護範圍當視後附的申請專利範圍所界定者為準。Although the present invention has been disclosed in the above embodiments, it is not intended to limit the present invention. Anyone with ordinary knowledge in the relevant technical field can make some changes and modifications without departing from the spirit and scope of the present invention. The scope of protection of the present invention shall be determined by the scope of the attached patent application.

100、102、104、106、108:步驟 200:矽晶種 202:晶界100, 102, 104, 106, 108: steps 200: silicon seed crystal 202: Grain Boundary

圖1為依照本發明實施例的矽晶碇的製造方法的流程圖。 圖2為鋪設於坩鍋底部的矽晶種的上是示意圖。FIG. 1 is a flowchart of a method for manufacturing a silicon ingot according to an embodiment of the present invention. Figure 2 is a schematic view of the top of the silicon seed crystals laid on the bottom of the crucible.

200:矽晶種 200: silicon seed crystal

202:晶界 202: Grain Boundary

Claims (10)

一種矽晶碇的製造方法，包括： 於加熱裝置中排列多個矽晶種，其中每一所述矽晶種的缺陷比例大於或等於1%； 於所述矽晶種上放置矽原料； 對所述矽晶種與所述矽原料進行加熱，直到所述矽原料熔化為矽熔體； 對所述矽熔體進行降溫，以使所述矽熔體固化為矽晶碇。A method for manufacturing silicon crystal ingots, including: Arranging a plurality of silicon seed crystals in the heating device, wherein the defect ratio of each of the silicon seed crystals is greater than or equal to 1%; Placing silicon material on the silicon seed crystal; Heating the silicon seed crystal and the silicon raw material until the silicon raw material melts into a silicon melt; The temperature of the silicon melt is lowered so that the silicon melt is solidified into silicon ingots. 如申請專利範圍第1項所述的矽晶碇的製造方法，其中相鄰的兩個所述矽晶種的晶向夾角大於0度且小於或等於5度。According to the method for manufacturing silicon crystal ingots as described in the first item of the scope of patent application, the angle between the crystal orientations of the two adjacent silicon seed crystals is greater than 0 degrees and less than or equal to 5 degrees. 如申請專利範圍第1項所述的矽晶碇的製造方法，其中相鄰的兩個所述矽晶種之間具有晶界，且在所述排列之後產生數量大於或等於4的晶界。According to the manufacturing method of the silicon crystal ingot described in the first item of the scope of patent application, there are grain boundaries between two adjacent silicon seed crystals, and a number of grain boundaries greater than or equal to 4 are generated after the arrangement. 如申請專利範圍第1項所述的矽晶碇的製造方法，其中每一所述矽晶種的形狀為多邊形。According to the method for manufacturing the silicon crystal ingot described in the first item of the scope of patent application, the shape of each silicon crystal crystal is polygonal. 如申請專利範圍第4項所述的矽晶碇的製造方法，其中每一所述矽晶種的形狀為四邊形。According to the method for manufacturing the silicon crystal ingot described in item 4 of the scope of patent application, the shape of each silicon crystal crystal is a quadrilateral. 如申請專利範圍第4項所述的矽晶碇的製造方法，其中每一所述矽晶種的每一邊長大於或等於5公分。According to the method for manufacturing the silicon crystal ingot described in item 4 of the scope of patent application, the length of each side of each silicon seed crystal is greater than or equal to 5 cm. 如申請專利範圍第1項所述的矽晶碇的製造方法，其中所述矽晶種的材料包括單晶矽、多晶矽或類單晶矽。According to the method for manufacturing the silicon crystal ingot described in the first item of the scope of patent application, the material of the silicon seed crystal includes single crystal silicon, polycrystalline silicon or similar single crystal silicon. 一種矽晶碇，由如申請專利範圍第1項至第7項中任一項所述的矽晶碇的製造方法所製造。A silicon ingot manufactured by the method for manufacturing a silicon ingot as described in any one of items 1 to 7 of the scope of patent application. 一種鋰電池的負極材料，包括由如申請專利範圍第8項所述的矽晶碇製造的多個矽顆粒。A negative electrode material for a lithium battery includes a plurality of silicon particles made of the silicon ingot as described in item 8 of the scope of patent application. 如申請專利範圍第9項所述的鋰電池的負極材料，其中所述多個矽顆粒的缺陷比例大於或等於5%。The negative electrode material of the lithium battery as described in item 9 of the scope of patent application, wherein the defect ratio of the plurality of silicon particles is greater than or equal to 5%.
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