Mg-Ion Battery Electrode: An Organic Solid’s Herringbone Structure Squeezed upon Mg-Ion Insertion

Rodríguez-Pérez, Ismael A.; Yuan, Yifei; Bommier, Clement; Wang, Xingfeng; Ma, Lu; Leonard, Daniel P.; Lerner, Michael M.; Carter, Rich G.; Wu, Tianpin; Greaney, P. Alex; Lu, Jun; Ji, Xiulei

doi:10.1021/jacs.7b06313

Title: Mg-Ion Battery Electrode: An Organic Solid’s Herringbone Structure Squeezed upon Mg-Ion Insertion

Journal Article · Mon Aug 21 00:00:00 EDT 2017 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.7b06313· OSTI ID:1529256

Rodríguez-Pérez, Ismael A. ^[1]; Yuan, Yifei ^[2]; Bommier, Clement ^[1];

^[1]; Ma, Lu ^[2]; Leonard, Daniel P. ^[1];

^[1]; Carter, Rich G. ^[1]; Wu, Tianpin ^[2]; Greaney, P. Alex ^[3];

^[2];

^[1]

Oregon State Univ., Corvallis, OR (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Univ. of California, Riverside, CA (United States)

We report that crystalline 3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA), an organic solid, is highly amenable to host divalent metal ions, i.e., Mg²⁺ and Ca²⁺, in aqueous electrolytes, where the van der Waals structure is intrinsically superior in hosting charge-dense ions. We observe that the divalent nature of Mg²⁺ causes unique squeezing deformation of the electrode structure, where it contracts and expands in different crystallographic directions when hosting the inserted Mg-ions. This phenomenon is revealed experimentally by ex situ X-ray diffraction and transmission electron microscopy, and is investigated theoretically by first-principles calculations. Interestingly, hosting one Mg²⁺ ion requires the coordination from three PTCDA molecules in adjacent columns of stacked molecules, which rotates the columns, thus reducing the (011) spacing but increasing the (021) spacing. Here, we demonstrate that a PTCDA Mg-ion electrode delivers a reversible capacity of 125 mA h g^–1, which may include a minor contribution of hydronium storage, a good rate capability by retaining 75 mA h g^–1 at 500 mA g^–1 (or 3.7 C), and a stable cycle life. We also report Ca²⁺ storage in PTCDA, where a reversible capacity of over 80 mA h g^–1 is delivered.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); Petroleum Research Fund (PRF); USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1529256

Journal Information:: Journal of the American Chemical Society, Vol. 139, Issue 37; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 132 works

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