“Adv. Energy Mater.”: Aerosol-Jet-Printed Polymer Composite Electrolyte for Solid-State Lithium-Ion Batteries
Product Introduction
Equipment Parameters
I. Abstract of the Paper’s Core Research
- A process for aerosol-printed solid-state composite electrolytes has been developed.
Develop a PEO-based composite electrolyte ink tailored for aerosol printing (PEO + lithium salt + aluminum oxide nanofiller), enabling direct layer-by-layer deposition of a solid-state electrolyte onto the surface of a pre‑fabricated LFP cathode, eliminating the need for subsequent hot‑press lamination and in situ forming a seamless electrode–electrolyte interface.
- Two lithium-salt systems give rise to distinct film morphologies.
PEO/LiDFOB/Al₂O₃: The film is dense, smooth, and free of pores, with a thickness of only 40–50 μm; at 45°C, its ionic conductivity exceeds 10⁻⁵ S/cm.
PEO/LiTriflate/Al₂O₃: Forms a fluffy, porous structure with a membrane thickness of up to 200–300 μm and extremely low room-temperature conductivity.
- Excellent electrochemical performance
The optimal LiDFOB‑based half-cell delivers a capacity of 85 mAh/g at 45°C and a C/15 rate; upon heating to 75°C, the capacity exceeds 162 mAh/g, approaching the theoretical capacity of LFP at 170 mAh/g.
- Precise and controllable film thickness
Electrolyte thickness exhibits a linear relationship with the number of printed layers, with approximately 900 nm deposited per layer; a stack of 25–60 layers allows precise control of membrane thickness. A 25-layer film is too thin and prone to short circuits, whereas 35 layers (≈22 μm) enable stable charge–discharge cycling.
- The process exhibits significant industrialization potential.
Aerosol-compatible, wide-viscosity inks and maskless digital fabrication enable monolithic multi-layer printing, making it well-suited for the mass production of large-area, custom-shaped solid-state batteries.
II. Working Principle of Aerosol Spraying and Its Core Advantages Compared with Traditional Processes
(1) Principle of Aerosol Jet Deposition
- The atomization chamber ultrasonically breaks down the solid electrolyte ink into micron-sized droplets, which are then conveyed to the print nozzle by an inert carrier gas.
- A coaxial sheath gas‑compressed aerosol jet precisely deposits material in a directed manner onto the surface of the LFP cathode, with an adjustable standoff distance between the print head and the substrate.
- Layer-by-layer additive printing is employed, with the ink infiltrating the pores of the positive electrode; following vacuum drying to remove the solvent, a continuous solid-state ion-conducting membrane is formed.
- The entire process is carried out in a dry‑room environment, eliminating the need for high‑temperature lamination and any additional pre‑treatment of the separator.
(II) Five Exclusive Technological Advantages (Compared with Cast Film, Direct Writing, and Hot Pressing)
- In-situ seamless interface, eliminating voids.
Traditional cast‑film thermal lamination readily gives rise to micron‑scale gaps; aerosol droplets directly penetrate the porous positive electrode, and cross‑sectional SEM imaging confirms that the electrolyte permeates the electrode, significantly reducing interfacial contact resistance.
- Precise Preparation of Ultrathin Films
It is possible to stably fabricate dense solid electrolyte films with thicknesses of 20–50 μm, whereas conventional processes struggle to produce uniform, defect-free films thinner than 25 μm.
- The ink viscosity is compatible with an extremely wide range.
It can print both high-solid-content cathode slurries and low-viscosity polymer electrolyte precursors, whereas direct-write and FDM melt‑based printing cannot simultaneously accommodate both types of materials.
- Maskless digital fabrication, compatible with irregular substrates.
CAD‑customizable printing areas enable deposition on curved surfaces and irregular battery substrates, breaking free from template constraints.
- Continuous integrated manufacturing, streamlining the production line.
A single piece of equipment sequentially prints the positive electrode and the solid-state electrolyte, eliminating multiple process steps such as membrane separation, cutting, and hot pressing, thereby reducing both equipment and labor costs.
III. Key Technological Innovations of This Study
Innovation 1: In-situ conformal deposition, addressing high interfacial resistance at the source.
Innovation 2: Precise Control of Thin-Film Microstructure via Lithium-Salt Systems
Innovation 3: A linear film-thickness control mechanism enabling ultrathin, stable electrolytes.
Innovation 4: A Composite Electrolyte System with High Ionic Conductivity at Low and Medium Temperatures
Innovation 5: A fully scalable ink formulation compatible with dry‑room processes.
IV. Existing Process Challenges and Corresponding Solutions
Challenge 1: The LiTriflate‑based film is excessively thick, resulting in extremely poor room‑temperature conductivity.
Problem: After deposition, lithium trifluoromethanesulfonate ink forms a porous thick film with extremely high internal resistance, rendering normal charge–discharge performance impossible at room temperature.
✅ Breakthrough: By leveraging a LiDFOB lithium‑salt system, we have engineered a dense, ultrathin layer that significantly enhances ionic conductivity at moderate and low temperatures.
Challenge 2: Too few printing layers result in insufficient mechanical strength of the electrolyte film.
Issue: The 25-layer printed film has insufficient thickness, making it prone to lithium dendrite penetration and short circuits during battery assembly.
✅ Breakthrough: Increased to 35 printing layers, yielding a continuous, intact electrolyte membrane with a thickness of approximately 22 μm, balancing thinness with mechanical stability.
Challenge 3: Insufficient pore penetration in the positive electrode, leading to discontinuous ion transport pathways.
Issue: With too few printing layers, the electrolyte cannot fully penetrate the porous LFP structure.
✅ Breakthrough: Multi-layer stacking and stepwise deposition provide ample time for ink penetration, enabling an all‑area ion‑conductive network in the electrode.
Challenge 4: Traditional processes involve multiple steps, making continuous automated production difficult.
Issue: Cast‑film and hot‑press processes require separate equipment to fabricate electrodes and electrolytes, resulting in a complex production line and low yield.
✅ Breakthrough: Aerosol‑based integrated layer‑by‑layer printing, enabling a single device to achieve both high‑loading deposition of the positive electrode and solid‑electrolyte coating.
Challenge 5: At elevated temperatures, lithium dendrites readily penetrate the thin solid electrolyte interphase.
Issue: Ultra-thin polymer electrolytes lack physical barriers, making them prone to short circuits during long cycling.
✅ Expansion plan: In the future, it can be combined with an aerosol‑printed porous separator–composite electrolyte layer to physically suppress dendrite formation and enhance cycling stability.
V. Prospects for Future Industrial Applications
1. New-energy vehicle all-solid-state power battery
2. Large-scale Safe Energy Storage Power Station
3. Aerospace Special Energy Storage Devices
4. Flexible Wearable Energy Storage Devices
5. Miniature Medical / IoT Power Supply
Figure 1. Scanning electron microscope images of the cross-sections of solid polymer composite electrolytes fabricated by aerosol jet printing, with the following formulations: a) PEO/LiDFOB/aluminum oxide (EO:Li = 10:1); b) PEO/LiDFOB/aluminum oxide (EO:Li = 16:1); c) PEO/LiTriflate/aluminum oxide (EO:Li = 10:1); and d) PEO/LiTriflate/aluminum oxide (EO:Li = 16:1). Insets in all images show high-magnification cross-sectional views of the interface, with the scale bar set to 50 μm. The interface between the electrolyte and the cathode is indicated by arrows.
Figure 2. Temperature-dependent conductivity of aerosol-jet-printed solid polymer composite electrolytes prepared using PEO/LiDFOB/alumina (squares) and PEO/LiTriflate/alumina (circles). Solid symbols denote the 10:1 EO-to-Li ratio, while hollow symbols with a cross indicate the 16:1 ratio.
Figure 3. Discharge curves of batteries fabricated using aerosol jet printing with a PEO/LiDFOB/alumina electrolyte (with EO-to-Li ratios of a) 16:1 at 45°C and b) 10:1 at 45°C). Insets show the results measured at 75°C. In all cycles, the charging rate was C/20 (221 mA), and the discharging rate was C/15 (295 mA). Cycle numbers are indicated in the inset graphs; the second cycle is marked by a dashed line.
Figure 4. Scanning electron microscope images of the cross-sections of solid polymer composite electrolytes fabricated by aerosol jet printing, with a formulation of PEO/LiDFOB/aluminum oxide (EO:Li = 10:1), at printing counts of: a) 60, b) 35, and c) 25. The interface between the electrolyte and the cathode is indicated by arrows.
Figure 5. Linear fit between the number of printing cycles and the thickness of the printed electrolyte. Error bars indicate the uncertainty in the electrolyte thickness measurements.
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