Journal of Energy Chemistry

Journal of Energy Chemistry ›› 2022, Vol. 69 ›› Issue (6): 397-405.DOI: 10.1016/j.jechem.2022.01.006

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Regulating local chemistry in ZrCo-based orthorhombic hydrides via increasing atomic interference for ultra-stable hydrogen isotopes storage

Zhaoqing Lianga,1, Zhendong Yaoa,1, Ruhong Lia, Xuezhang Xiaoa,*, Zhichao Yea, Xuancheng Wanga, Jiacheng Qia, Jiapeng Bia, Xiulin Fana, Huaqin Kouc,*, Wenhua Luoc,d, Changan Chenc,d, Lixin Chena,b,*   

  1. aState Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, Zhejiang, China;
    bKey Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Province, Hangzhou 310013, Zhejiang, China;
    cInstitute of Materials, China Academy of Engineering Physics, Mianyang 621907, Sichuan, China;
    dState Key Laboratory of Surface Physics and Chemistry, Mianyang 621907, Sichuan, China
  • Received:2021-11-15 Revised:2021-12-29 Accepted:2022-01-04 Online:2022-06-15 Published:2022-10-25
  • Contact: * E-mail addresses: xzxiao@zju.edu.cn (X. Xiao), kouhuaqin@caep.cn (H. Kou), lxchen@zju.edu.cn (L. Chen).
  • About author:1 These authors contributed equally to this work.

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Abstract: Developing a universal and reliable strategy for the modulation of composition and structure of energy storage materials with stable cycling performance is vital for hydrogen and its isotopes storage advanced system, yet still challenging. Herein, an ultra-stable lattice structure is designed and verified to increase atomic chaos and interference for effectively inhibiting disproportionation reaction and improving cycling stability in ZrCo-based hydrogen isotopes storage alloy. After screening in terms of configuration entropy calculation, we construct Zr1—xNbxCo1—2xCuxNix (x = 0.15, 0.2, 0.25) alloys with increased atomic chaos, and successfully achieve stable isostructural de-/hydrogenation during 100 cycles, whose cycling capacity retentions are above 99%, much higher than 22.4% of pristine ZrCo alloy. Both theoretical anal-ysis and experimental evidences indicate the high thermo-stability of orthorhombic lattice in Zr0.8Nb0.2Co0.6Cu0.2Ni0.2 alloy. Notably, the increased atomic chaos and interference in Zr0.8Nb0.2Co0.6Cu0.2Ni0.2 alloy causes regulation in hydrogen local chemical neighborhood, thereby con-fusing the hydrogen release order, which effectively eliminates lattice distortion and unlocks an ultra-stable lattice structure. This study provides a new and comprehensive inspiration for hydrogen atoms transport behaviors and intrinsic reason of stable orthorhombic transformation, which can contribute to paving the way for other energy storage materials modulation.

Key words: ZrCo alloy, High configuration entropy, Regulating chemical environment, Lattice stabilization, In-situ XRD, Density functional theory