doi:10.1088/2752-5724/ac7db2

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All-solid-state thin-film batteries based on lithium phosphorus oxynitrides

doi: 10.1088/2752-5724/ac7db2

1.
Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200433, People’s Republic of China
2.
Nano Science and Technology Institute, University of Science and Technology of China, Suzhou 215123, People’s Republic of China

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Corresponding author: E-mail: zwfu@fudan.edu.cn

摘要

Abstract: Lithium phosphorus oxygen nitrogen (LiPON) as solid electrolyte discovered by Bates et al in the 1990s is an important part of all-solid-state thin-film battery (ASSTFB) due to its wide electrochemical stability window and negligible low electronic conductivity. However, the ionic conductivity of LiPON about 2 10^-6 S cm^-1 at room temperature is much lower than that of other types of solid electrolytes, which seriously limits the application of ASSTFBs. This review summarizes the research and progress in ASSTFBs based on LiPON, in the solid-state electrolyte of LiPON-derivatives with adjustable chemical compositions of the amorphous structure for the improvement of the ionic conductivity and electrochemical stability, in the critical interface issues between LiPON and electrodes, and in preparation methods for LiPON. This review is helpful for people to understand the interface characteristics and various preparation methods of LiPON in ASSTFBs. The key issues to be addressed concern how to develop solid-state electrolyte films with high conductivity and high-quality interface engineering as well as large-scale preparation technology, so as to realize the practical application of highly integrated ASSTFBs.
- LiPON /
- solid electrolyte /
- solid thin-film battery /
- interfacial property /
- preparation method
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Figure 1. Schematic of the fabrication process for all-solid-state lithium batteries based on LiPON thin-film solid electrolyte.

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Figure 2. The schematic illustration of the development of cathode thin films and solid-state electrolyte thin films in ASSTFBs.

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Figure 3. (a) Non-cytotoxic flexible batteries are integrated into intra-oral phototherapeutic devices. (b) Optica images of the micro lithium battery in the intra-oral device. Reproduced from [8]. CC BY 4.0.

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Figure 4. (a) Schematic illustration of the process for the fabrication of flexible lithium-ion batteries, and the key operation is to use sticky tapes to delaminate the battery from the mica substrate ((i) and (ii)). (b) The picture of a flexible LED system with a bendable lithium-ion battery as the power source. Reprinted with permission from [36]. Copyright (2012), American Chemical Society.

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Figure 5. Evolution of the surface capacity regarding the film thickness and the type of current collector (Pt or Cr/Pt) and SEM cross-section analysis of the 7.4 m-thick LNMO film. Reprinted from [37]. Copyright (2018), with permission from Elsevier.

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Figure 6. Illustration of the orthorhombic phase of Li_xCoO₂. The left image shows a favorable texture of LCO for the migration of lithium ions because the driving force is parallel to the intercalation planes, and the texture of LCO in the right one is unfavorable. Light blue spheres are O, red spheres are Li, and dark blue spheres are Co. Reprinted from [38]. Copyright (2017), with permission from Elsevier.

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Figure 7. (a) Typical photo and (b) cross-sectional SEM image of all-solid-state LiFeFe[CN]₆/LiPON/Li battery; (c) film battery lighting a blue LED. Reprinted with permission from [63]. Copyright (2018) American Chemical Society.

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Figure 8. (a) Schematic of simulated Li_2.94PO_3.50N_0.31 structure from AIMD. Red atoms are O, blue atoms are N, green atoms are Li, and light gray atoms are P. (b) Comparison of simulated and experimental neutron PDF data of LiPON. Reprinted with permission from [65]. Copyright (2018) American Chemical Society.

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Figure 9. The cross-sectional TEM images of the (a) pristine LCO/LiPON interface, (b) the one was cycled at 25 C, and (c) the one was cycled at 80 C. Reprinted from [99]. Copyright (2016), with permission from Elsevier.

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Figure 10. (a) XPS spectra of Co 2p, O 1s, P 2p, and the valence band at the LCO/LiPON interface with increasing LiPON coverage; (b) Change of the core levels of the LCO and the P 2p level of the LiPON layer with time. Reprinted from [104]. Copyright (2016), with permission from Elsevier.

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Figure 11. (a) Structure and composition of LCO/LiPON interface and its evolution during annealing. (b) Valence band bending, inner electric potential profile and Li-ion electrochemical potential at LCO/LiPON interface. Reprinted with permission from [105]. Copyright (2017) American Chemical Society.

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Figure 12. Complete energy band diagram of the LCO/LiPON/Li battery. Reprinted from [104]. Copyright (2016), with permission from Elsevier.

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Figure 13. Plasma plume photos of (a) radio frequency magnetron sputtering; (b) pulsed laser deposition; (c) ion beam assisted deposition.

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Figure 14. The flow chart of atomic layer deposition for LiPON. Reprinted with permission from [121]. Copyright (2015) American Chemical Society.

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Figure 15. (a) Schematic illustration of metal-organic chemical vapor deposition equipment. Reprinted from [123]. Copyright (2013), with permission from Elsevier. (b) Schematic diagram of the effect of metal-organic chemical vapor deposition.

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Figure 16. Reaction equation for preparing LiPON by polymer precursor method. Reprinted with permission from [71]. Copyright (2020) American Chemical Society.

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Table 1. The structural characteristic of LiPON-derivatives.

LiPON	LiBPON

LiSiPON	LiPFON

LiPSON	LiPCON

LiWPON (M = Al, Ti, W, etc)

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Table 2. The chemical formula, ionic conductivity, and activation energy of LiPON-derivatives.

Preparation method	Chemical formula	Ionic conductivity (S cm^-1 at room temperature)	Activation energy (eV)	Reference
Si-doped LiPON-derivatives
Rf magnetron sputtering	Li_2.3Si_0.2PO_1.4N_1.1	5.65 10^-6	0.500	[66]
	Li_1.9Si_0.28PO_1.1N_1.0	8.86 10^-6	0.491	[66]
	Li_2.9Si_0.35PO_1.5N_1.26	1.00 10^-5	0.487	[66]
	Li_2.9Si_0.45PO_1.6N_1.3	1.24 10^-5	0.479	[66]
Rf magnetron sputtering	Li_3.9Si_0.08PO_1.69N_1.52	5.4 10^-6	0.47	[68]
	Li_4.2Si_0.39PO_2.75N_1.76	6.6 10^-6	0.45	[68]
	Li_6.2Si_0.93PO_3.22N_2.14	9.7 10^-6	0.41	[68]
Rf magnetron sputtering	Li_0.94Si_0.30P_0.70O_2.17	1.49 10^-6	0.57	[69]
	Li_0.97Si_0.59P_0.41O_2.19	2.00 10^-7	0.56	[69]
	Li_2.40Si_0.88P_0.12O_2.28	4.09 10^-7	0.51	[69]
	Li_0.54Si_0.26P_0.74O_1.38N_0.76	1.31 10^-8	0.58	[69]
	Li_0.56Si_0.56P_0.44O_1.22N_0.72	2.81 10^-8	0.58	[69]
	Li_1.35Si_0.79P_0.21O_1.98N_0.98	2.06 10^-5	0.45	[69]
Rf magnetron sputtering	Li_0.89Ti₂Si_0.32P_3.8O_10.9N_2.52	9.2 10^-6	0.29	[74]
S-doped LiPON-derivatives
Rf magnetron sputtering	Li_0.29S_0.18O_0.53	2.6 10^-6	N/A	[75]
	Li_0.29S_0.11O_0.60	5.3 10^-6	N/A	[75]
	Li_0.29S_0.28O_0.38N_0.05	1 10^-5	N/A	[75]
	Li_0.29S_0.28O_0.35N_0.09	2 10^-5	N/A	[75]
Rf magnetron sputtering	LiBSO	2.5 10^-6	0.51	[76]
Solid-state reaction	Li₃SO₃N	10^-14	1.03	[78]
Melting reaction	Li_1.62PO_2.84S_0.11N_0.32	2.95 10^-7	0.64	[79]
Solid-state reaction	LiSPON	1.4 10^-8-6.8 10^-7	N/A	[80]
Rf magnetron sputtering	LiSPON	1.58 10^-5	N/A	[81]
Rf magnetron sputtering	LiSPON	3.23-9.75 10^-6	0.23-0.53	[83]
B-doped LiPON-derivatives
Rf magnetron sputtering	Li_0.9BO_0.66N_0.98	4.3 10^-9	N/A	[84]
	Li_3.09BO_2.53N_0.52	2.3 10^-6	N/A	[84]
	Li_3.51BO_3.03N_0.52	2.6 10^-7	N/A	[84]
Rf magnetron sputtering	LiBPON	3.5 10^-6	0.53	[89]
Rf magnetron sputtering	Li_2.65B_0.11P_0.89O_3.00N_0.15	6.88 10^-7	0.653	[90]
Other kinds of LiPON-derivatives doped with the nonmetallic element
Melting reaction	LiPFO	1.26 10^-7-6.61 10^-8	0.69-0.71	[91]
Melting reaction	LiPFON	1.95 10^-7-5.74 10^-8	0.66-0.68	[91]
Rf magnetron sputtering	Li_3.25C_0.03PO_3.87N_0.21	3.06 10^-6	0.43	[92]
Metallic element (M) doped LiPON-derivatives
Rf magnetron sputtering	Li_3.426PW_0.008O_2.091N_0.364	1.5 10^-7	0.51	[93]
Rf magnetron sputtering	Li-Al-Ti-P-O	0.34-2.46 10^-5	0.32-0.33	[94]
Rf magnetron sputtering	Li-Al-Ti-P-O-N	1.22 10^-6-1.22 10^-5	0.44-0.63	[95]
Melting reaction	Li-La-Al-P-O-N	1.47 10^-5	0.54	[96]
Rf magnetron sputtering	Li-Al-Ge-P-O-N	2.3 10^-4	0.374	[97]

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