Chemical and Electrochemical Lithiation of van der Waals Tetrel-Arsenides

Mark, Justin; Hanrahan, Michael P.; Woo, Katherine E.; Lee, Shannon; Rossini, Aaron J.; Kovnir, Kirill

doi:10.1002/chem.201900339

Chemical and Electrochemical Lithiation of van der Waals Tetrel-Arsenides

Journal Article · Mon Mar 18 00:00:00 EDT 2019 · Chemistry - A European Journal

DOI:https://doi.org/10.1002/chem.201900339· OSTI ID:1526289

Mark, Justin ^[1]; Hanrahan, Michael P. ^[1]; Woo, Katherine E. ^[1]; Lee, Shannon ^[1]; Rossini, Aaron J. ^[1]; ^[1]

Ames Lab. and Iowa State Univ., Ames, IA (United States)

Lithiation of van der Waals tetrel–arsenides, GeAs and SiAs, has been researched. Electrochemical lithiation demonstrated large initial capacities of over 950 mAh g^-1 accompanied by rapid fading over successive cycling in the voltage range 0.01–2 V. Limiting the voltage range to 0.5–2 V achieved more stable cycling, which was attributed to the intercalation process with lower capacities. Ex situ powder X–ray diffraction confirmed complete amorphization of the samples after lithiation, as well as recrystallization of the binary tetrel–arsenide phases after full delithiation in the voltage range 0.5–2 V. Solid–state synthetic methods produce layered phases, in which Si–As or Ge–As layers are separated by Li cations. The first layered compounds in the corresponding ternary systems were discovered, Li_0.9Ge_2.9As_3.1 and Li₃Si₇As₈, which crystallize in the Pbam (No. 55) and P2/m (No. 10) space groups, respectively. Semiconducting layered GeAs and SiAs accommodate the extra charge from Li cations through structural rearrangement in the Si–As or Ge–As layers and eventually by replacement of the tetrel dumbbells with sets of Li atoms. Ge and Si monoarsenides reflected high structural flexibility and a mild ability for reversible lithiation.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1526289

Alternate ID(s):: OSTI ID: 1506712

Report Number(s):: IS-J--9942

Journal Information:: Chemistry - A European Journal, Journal Name: Chemistry - A European Journal Journal Issue: 25 Vol. 25; ISSN 0947-6539

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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