Nanoscale Li, Na, and K ion-conducting polyphosphazenes by atomic layer deposition

Nuwayhid, R. Blake; Fontecha, Daniela; Kozen, Alexander C.; Jarry, Angelique; Lee, Sang Bok; Rubloff, Gary W.; Gregorczyk, Keith E.

doi:10.1039/d1dt03736f

Title: Nanoscale Li, Na, and K ion-conducting polyphosphazenes by atomic layer deposition

Journal Article · 07 January 2022 · Dalton Transactions

DOI: https://doi.org/10.1039/d1dt03736f · OSTI ID:1978780

^[1]; Fontecha, Daniela ^[2];

^[2]; Jarry, Angelique ^[2]; Lee, Sang Bok ^[2];

^[2]; Gregorczyk, Keith E. ^[2]

University of Maryland, College Park, MD (United States); OSTI
University of Maryland, College Park, MD (United States)

A key trailblazer in the development of thin-film solid-state electrolytes has been lithium phosphorous oxynitride (LiPON), the success of which has led to recent progress in thin-film ion conductors. Here we compare the structural, electrochemical, and processing parameters between previously published LiPON and NaPON ALD processes with a novel ALD process for the K analogue potassium phosphorous oxynitride (KPON). In each ALD process, alkali tert-butoxides and diethylphosphoramidate are used as precursors. To understand the ALD surface reactions, this work proposes a reaction mechanism determined by in-operando mass spectrometry for the LiPON process as key to understanding the characteristics of the APON (A = Li, Na, K) family. As expected, NaPON and LiPON share similar reaction mechanisms as their structures are strikingly similar. KPON, however, exhibits similar ALD process parameters but the resulting film composition is quite different, showing little nitrogen incorporation and more closely resembling a phosphate glass. Due to the profound difference in structure, KPON likely undergoes an entirely different reaction mechanism. Furthermore, this paper presents a comprehensive summary of ALD ion conducting APON films as well as a perspective that highlights the versatility of ALD chemistries as a tool for the development of novel thin film ion-conductors.

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Research Organization:: University of Maryland, College Park, MD (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001160

OSTI ID:: 1978780

Journal Information:: Dalton Transactions, Journal Name: Dalton Transactions Journal Issue: 5 Vol. 51; ISSN 1477-9226

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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