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/ 博客文章 / 電池知識 / 冬天來了,看看鋰離子電池低溫分析現象 鋰離子電池的性能很大程度上受其動力學特性的影響。 由於Li+嵌入石墨材料時需要先脫溶劑,因此需要消耗一定的能量並阻礙Li+向石墨中的擴散。 相反,當Li+從石墨材料釋放到溶液中時,首先發生溶劑化過程,並且溶劑化過程不需要能量消耗。 Li+可以快速去除石墨,導致石墨材料的充電接受能力明顯較差。 在放電可接受性方面。
在低溫下,負極石墨電極的動力學特性有所改善並變得更差。 因此,充電過程中負極的電化學極化明顯加劇,容易導致負極表面金屬鋰的析出。 德國慕尼黑工業大學Christian von Lüders的研究表明,在-2℃時,充電倍率超過C/2,金屬鋰析出量顯著增加。 例如,在C/2倍率下,相對電極表面上的鋰電鍍量大約是整個充電量。 容量的5.5%,但在9C倍率下將達到1%。 析出的金屬鋰可能進一步發展,最終成為鋰枝晶,刺穿隔膜,導致正負極短路。 因此,需要盡可能避免在低溫下為鋰離子電池充電。 當必須在低溫下對電池進行充電時,必須盡可能選擇小電流對鋰離子電池進行充電,並在充電後將鋰離子電池充分儲存,以確保負極析出的金屬鋰。可以與石墨反應並重新嵌入負極石墨電極中。
慕尼黑工業大學的Veronika Zinth等人利用中子繞射等方法研究了鋰離子電池在-20℃低溫下的析鋰行為。 中子繞射是近年來出現的一種新的探測方法。 與XRD相比,中子衍射對輕元素(Li、O、N等)更加敏感,因此非常適合鋰離子電池的無損檢測。
在實驗中,VeronikaZinth使用NMC111/石墨18650電池來研究鋰離子電池在低溫下的析鋰行為。 測試時電池依照下圖所示流程進行充放電。
下圖為C/30倍率充電第二個充電週期時不同SoC下負極的相變。 可以看出,在30.9% SoC時,負極的相主要為LiC12、Li1-XC18,以及少量的LiC6組成; SoC超過46%後,LiC12的繞射強度持續降低,而LiC6的功率持續增加。 然而,即使最終充電完成後,由於低溫下僅充電1503mAh(常溫下容量為1950mAh),負極中仍存在LiC12。 假設充電電流減小到C/100。 在這種情況下,電池在低溫下仍然可以獲得1950mAh的容量,這表明鋰離子電池在低溫下功率的下降主要是由於動力學條件的惡化。
下圖為-5℃低溫下以C/20倍率充電時負極石墨的相變。 可以看出,石墨的相變與C/30倍率充電相比有顯著差異。 從圖中可以看出,當SoC>40%時,C/12充電倍率下LiC5電池的相強度下降明顯較慢,LiC6相強度的增加也明顯弱於C/30收費率。 結果表明,在相對較高的 C/5 速率下,較少的 LiC12 繼續嵌入鋰並轉化為 LiC6。
下圖比較了負極石墨電極分別以C/30和C/5倍率充電時的相變。 此圖顯示,對於兩種不同的充電速率,貧鋰相Li1-XC18非常相似。 差異主要體現在LiC12和LiC6兩相。 從圖中可以看出,兩種充電倍率下充電初期負極內的相變趨勢較為接近。 對於LiC12階段,當充電容量達到950mAh(49%SoC)時,變化趨勢開始出現不同。 當達到1100mAh(56.4% SoC)時,兩個放大倍率下的LiC12相開始表現出明顯的差距。 以C/30低倍率充電時,LiC12相的下降很快,但在C/12倍率下LiC5相的下降要慢得多; 也就是說,低溫下鋰嵌入負極的動力學條件惡化。 ,使LiC12進一步嵌入鋰,生成LiC6相速度下降。 相應地,LiC6 相在 C/30 的低速率下增加得非常快,但在 C/5 的速率下則慢得多。 這顯示在C/5倍率下,石墨晶體結構中嵌入了更多嬌小的Li,但有趣的是,電池在C/1520.5充電倍率下的充電容量(5mAh)高於C下的充電容量(30 mAh)。 /1503.5 充電率。 電量(XNUMXmAh)較高。 未嵌入負極石墨電極中的額外Li很可能以金屬鋰的形式沉澱在石墨表面上。 充電結束後的靜置過程也從側面證明了這一點——一點點。
下圖為石墨負極充電後和放置20小時後的相結構。 充電結束時,兩種充電倍率下負極石墨電極的相有很大差異。 在C/5時,石墨負極中LiC12的比例較高,LiC6的比例較低,但靜置20小時後,兩者的差異已變得很小。
下圖為負極石墨電極在20h儲存過程中的相變。 從圖中可以看出,雖然一開始兩個相對電極的相位仍然有很大差異,但隨著儲存時間的增加,兩種充電放大倍率下的石墨陽極的相位變化非常接近。 LiC12在擱置過程中能夠繼續轉化為LiC6,顯示Li在擱置過程中會繼續嵌入石墨中。 這部分Li很可能是低溫下石墨負極表面析出的金屬鋰。 進一步分析表明,在C/30倍率充電結束時,負極石墨電極的嵌鋰率為68%。 儘管如此,擱置後嵌鋰率仍增加至71%,增加了3%。 C/5倍率充電結束時,負極石墨電極的嵌鋰率為58%,但放置20小時後,增加至70%,總共增加了12%。
上述研究表明,在低溫充電時,電池容量會因動力學條件惡化而下降。 也會因石墨嵌鋰率的降低而在負極表面析出鋰金屬。 然而,經過一段時間的儲存,這部分金屬鋰又可以重新嵌入石墨中; 在實際使用中,保存時間往往較短,並不能保證所有金屬鋰都能再次嵌入石墨中,因此可能會導致部分金屬鋰繼續存在於負極中。 鋰離子電池表面會影響鋰離子電池的容量,並可能產生鋰枝晶,危及鋰離子電池的安全。 因此,盡量避免在低溫下對鋰離子電池充電。 小電流,定型後,確保足夠的擱置時間,以消除負極石墨電極中的金屬鋰。
本文主要參考了以下文件。 本報告僅用於介紹和回顧相關科學著作、課堂教學、科學研究等。 不可用於商業用途。 如果您有任何版權問題,請隨時與我們聯繫。
1.石墨材料作為鋰離子電容器負極的倍率性能,Electrochimica Acta 55 (2010) 3330 - 3335,SRSivakkumar,JY Nerkar,AG Pandolfo
2.透過電壓弛豫和原位中子衍射研究鋰離子電池中的鋰鍍層,Journal of Power Sources 342(2017)17-23,Christian von Lüders,Veronika Zinth,Simon V.Erhard,Patrick J.Osswald, Michael Hofman , 拉爾夫吉爾斯, 安德烈亞斯喬森
3.透過原位中子繞射研究亞環境溫度下鋰離子電池中的鋰鍍層,Journal of Power Sources 271 (2014) 152-159,Veronika Zinth,Christian von Lüders,Michael Hofmann,Johannes Hattendorff,Irmgard Buchberger,Simon艾哈德、喬安娜·雷貝洛-科恩梅爾、安德烈亞斯·喬森、拉爾夫·吉爾斯