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    北理工黃佳琦課題組在化學類頂級期刊Angew Chem Int Ed上發表重要研究成果

    供稿: 前沿交叉科學研究院 編輯: 朱倩云
    (2018-12-14) 閱讀次數:
    【字號  大

      近日,北京理工大學前沿交叉科學研究院黃佳琦課題組在鋰硫(Li–S)電池動力學調節方面研究取得新進展,相關研究成果以《Activating Inert Metallic Compounds for High-Rate Lithium–Sulfur Batteries Through In-Situ Etching of Extrinsic Metal》為題在線發表于化學類頂級國際期刊《Angewandte Chemie International Edition》(《德國應用化學》,影響因子12.10)。該研究利用原位刻蝕的Ni3FeN促進多硫化物的表面反應,并采用先進的表征技術揭示了原位催化轉化機理。該工作開拓了多金屬合金/化合物作為高倍率Li–S電池動力學促進劑的新思路,也提出了催化表面反應和缺陷化學作用的新見解。本文的第一作者為北京理工大學前沿交叉科學研究院/材料學院碩士研究生趙夢,共同第一作者為清華大學彭翃杰博士,通訊作者為黃佳琦特別研究員。

      因為具有較高的理論比能量,Li–S電池作為鋰離子電池最有希望的替代品受到極大的關注。其高能量密度依賴于可逆的表面電化學反應,在硫正極中引入電催化活性成分可以有效加速表面反應動力學,從而提高硫的利用率并減輕多硫化物的穿梭效應。然而,在電池工作條件下催化劑的真實活性相此前幾乎沒有被驗證過。深入挖掘表面反應機理,探明催化劑活性的來源對于指導催化劑設計具有關鍵作用。

    圖1. 多硫化物刻蝕誘導的活化機制

      類似于金屬催化劑設計的合金化策略,該團隊在單金屬化合物中引入外在金屬,活化了原來的惰性相化合物,從而促進多硫化物的表面反應動力學。以六方氮化鎳(Ni3N)作為概念驗證,其對多硫化物的催化活性較差。在引入鐵元素后,Ni3N轉變為高活性的立方鎳鐵氮化物(Ni3FeN)。在Ni3FeN中,處于立方結構頂角處的較高正電性的鐵(與鎳相比)傾向于通過多硫化物的刻蝕過程浸出,從而在鎳位點的周圍留下大量空位缺陷,極大地提高了Ni3N的催化活性。

    圖2.(a,b)循環前和(c,d)循環后Ni3FeN-G的HAADF-STEM圖像和相應的元素分布

      該團隊利用高角度環形暗場掃描透射電子顯微鏡和相應的元素映射來揭示上述機制。如圖2所示,循環前的Ni3FeN顆粒中Ni和Fe元素的分布較為均勻。而循環后的Ni3FeN顆粒顯示出異常的鐵元素的表面富集,證明在循環期間由于多硫化物的刻蝕作用發生了相遷移,從而留下大量Fe元素的空位并提高催化活性。

    圖3. Ni3FeN催化作用下Li–S電池的電化學性能

      鐵元素通過多硫化物的原位刻蝕作用而浸出,產生高活性的富空位相,從而促進了多硫化物的動力學轉化過程。這種富空位的Ni3FeN催化的Li–S電池表現出優異的倍率性能和高硫負載下的循環穩定性,并且可以極大降低電解液用量。這項工作不僅闡述了惰性單金屬化合物的外在金屬活化機制,也證明了原位相演化和空位的形成在調節催化反應中的重要作用。

      論文詳情:

      Meng Zhao, Hong-Jie Peng, Ze-Wen Zhang, Bo-Quan Li, Xiao Chen, Jin Xie, Xiang Chen, Jun-Yu Wei, Qiang Zhang, and Jia-Qi Huang*. Activating Inert Metallic Compounds for High-Rate Lithium–Sulfur Batteries Through In-Situ Etching of Extrinsic Metal, Angew Chem Int Ed , doi: 10.1002/anie.201812062.

      論文鏈接:https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.201812062

     

    作者簡介:

      黃佳琦特別研究員,九三學社社員,2012年博士畢業于清華大學化學工程系,2016年9月入職北理工前沿交叉科學研究院并組建課題組開展研究工作,在國家重點研發計劃、國家自然科學基金、北京理工大學科技創新計劃的資助下,主要開展能源存儲材料研究。黃佳琦特別研究員以第一作者/通訊作者身份,在Advanced Materials, Advanced Functional Materials, Angewandte Chemie International Edition, Energy Storage Materials, Science Bulletin等期刊發表一系列研究工作。其發表論文的總引用10000余次,h因子為56,其中30余篇為ESI高被引論文,入選2018年科睿唯安高被引科學家(材料科學)。

      黃佳琦擔任中國顆粒學會青年理事會理事,Journal of Energy Chemistry《能源化學》及Chinese Chemical Letters《中國化學快報》青年編委,任Advanced Functional Materials《先進功能材料》鋰硫電池專刊,Journal of Energy Chemistry 《能源化學》下一代電池專刊客座編輯。入選首屆中國科協青年人才托舉計劃,獲評中國化工學會侯德榜化工科技青年獎,中國顆粒學會青年顆粒學獎等。

      

     


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