Highly efficient phosphor-glass composites by pressureless sintering

Zhang, Dao; **ao, Wenge; Liu, Chang; Liu, **aofeng; Ren, **jun; Xu, Beibei; Qiu, Jianrong

doi:10.1038/s41467-020-16649-z

Highly efficient phosphor-glass composites by pressureless sintering

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Published: 04 June 2020

Volume 11, article number 2805, (2020)
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Abstract

The development of high-power white light-emitting diodes demands highly efficient and stable all-inorganic color converters. In this respect, phosphor-glass/ceramic composites show great promise as they could combine the merits of high quantum efficiency of phosphors and high chemical and thermal stabilities of glass/ceramic matrices. However, strong interfacial reaction between phosphors and matrices at high temperature results in quantum efficiency loss of the embedded phosphors, and traditional solutions rely on high-pressure consolidation techniques. Here we report the intrinsic inhibition of interfacial reaction by using silica glass rather than multicomponent glasses as the matrix. The embedment of phosphors is achieved via a pressureless sintering method, rendering these color-tunable phosphor-glass composites not only accessible to three-dimensional printing technique, but also highly efficient (internal quantum efficiency >90.0%), thermally stable at 1200 °C and hydrothermally stable at 200 °C. Our results provide a facile and general strategy for develo** all-inorganic functional composites.

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Introduction

Color converters that can emit light of desired wavelengths after absorbing incident light play a key role in light-emitting^1,2,3 and -detecting⁴ devices as well as photovoltaics^5,6. However, conventional color converters with luminescent particles embedded in transparent organic polymers are notoriously easy to degrade during exposure to heat, moisture and short-wavelength radiation, leading to much shorter lifetime of the devices than expected^7,8. Recently, the so-called phosphor-converted white light-emitting diodes (pc-WLEDs) have been widely used in general lighting and display backlighting, but their extension to high-power and high-brightness lighting fields such as street lighting, automotive headlamp and large-size display, is extremely sluggish^{1,2,3,1,2,3,40}, and then YAG:Ce powders are added to obtain the final composite slurry where YAG:Ce particles can be well suspended (Fig. 1a). The slurry is then polymerized into transparent flat-plate green bodies within 30 s under high-power UV light. Green bodies with complex 3D structure can be also rapidly produced from the developed photocurable slurry with stereolithography (SLA) 3D printing (Supplementary Fig. 2), by which Kotz et al have recently fabricated various silica glass structure parts^41,42. After two-step heat treatment for debinding and densifying (Methods), the green bodies become porous and then are fully densified into transparent pure silica glass or translucent yellow YAG:Ce-PiSG (Fig. 1a,b), where for PiSG doped with 1 wt% YAG:Ce (1 wt% YAG:Ce-PiSG) the linear shrinkage is 4.7 and 27.9% after debound and densified, respectively.

As shown in Fig. 1c, pure silica glass exhibits excellent transparency with a total transmittance of 80.5% at the wavelength of 450 nm (86.2% at 600 nm), implying that full densification is achieved. With incorporating YAG:Ce into silica glass, the as-synthesized samples become translucent, accompanied by intense yellow emission upon 450 nm excitation (Fig. 1b). Transparency reduction is mainly attributed to the enhanced light scattering due to the different refractive indices of YAG:Ce (1.84) and silica glass (1.46); nevertheless, moderate light scattering is beneficial to the color uniformity and the light extraction of high-power pc-WLED, especially when laser diodes (LDs) are used as the excitation source^{Full size image}

Solid-state nuclear magnetic resonance (NMR) spectroscopy is a powerful tool to provide atomic structural information in material science. Figure 3d shows the ²⁷Al magic angle spinning NMR (MAS-NMR) spectra of YAG:Ce powder and YAG:Ce-PiSG. The single-peak signal at 1.5 ppm and the well-defined quadrupolar peak at 71.3 ppm can be clearly resolved, where the former represents six-coordinated Al (Al^VI) and the latter four-coordinated Al (Al^IV). The maximum peak positions, i.e. the average isotropic chemical shifts (δ_iso), as well as the peak shapes of the two aluminum species show no difference in both spectra, indicating that the local environment of these polyhedrons remains nearly the same after YAG:Ce are embedded into silica glass. The ratios of the integrated signal intensities of Al^IV and Al^VI species from YAG:Ce powder and YAG:Ce-PiSG are estimated to be 42.3:57.8 and 41.5:58.5, respectively, both of which agree well with the expected 2:3 ratio for YAG crystal. In addition, the ²⁹Si MAS-NMR spectra of pure silica glass and YAG-PiSG (Supplementary Fig. 6) are almost identical, which is consistent with the results from ²⁷Al MAS-NMR spectra. Moreover, the long-term (10 h) high-temperature stability of YAG:Ce-PiSG at 1200 °C also reflect the intrinsically inhibited interfacial reaction between YAG:Ce and silica glass. Our results unambiguously confirm that interfacial reaction between YAG:Ce and silica glass matrix is very limited even at 1250 °C for 3 h.

Versatile phosphor-silica glass composites

The extremely small diffusion rate of highly charged Si⁴⁺ and the absence of non-bridging oxygens^18,28 largely improve the activation energy (namely the required temperature) for the interfacial reaction of phosphor with silica glass, as compared with multicomponent glasses. Moreover, a reduction atmosphere is employed not only to assist the densification process, but also to preserve Ce³⁺ and Eu²⁺, two most widely used activators in phosphors, which otherwise would be oxidized into luminescence killers (Ce⁴⁺ and Eu³⁺) at high temperature. Using amorphous silica nanoparticles lower the required temperature to only 1250 °C, but, nevertheless, the structure of most phosphors including oxides and oxynitrides are thermally stable at this temperature. Therefore, the proposed strategy can generally be applied to achieve color tunable emission in silica glass based composites.

As shown in Fig. 4, not only garnet-type phosphors including Lu₃Al₅O₁₂:Ce (LuAG:Ce, blue-green), (Gd,Y)₃Al₅O₁₂:Ce (GdAG:Ce, orange) as well as YAG:Ce (yellow), but other well-known phosphors such as BaMgAl₁₀O₁₇:Eu (BAM:Eu, blue), β-SiAlON:Eu (β-Sialon:Eu, green) and Al₂O₃:Cr (far-red) were particularly incorporated into silica glass for exemplification (Fig. 4). As expected, all the as-synthesized phosphor-glass composites are highly efficient with limited IQE loss except the β-Sialon:Eu doped one (Supplementary Table 3). Unlike α-sialon, β-sialon is structurally unstable at high temperature due to N₂ evaporation⁴³, resulting in large IQE loss. Using smaller amorphous silica nanoparticles (<15 nm) or tetramethoxysilane as the precursor^43,50 could reduce the required temperature to lower than 1100 °C. It is thus anticipated that more kinds of phosphors could be incorporated into silica glass without obvious IQE loss. However, the densifying temperature of silica glasses is still too high for red nitride phosphors, and this limitation cannot be well circumvented until novel oxide or oxynitride red phosphors with high thermal stability are developed. Finally, silica glass acts as an effective buffer for the embedded phosphors against oxidation at high temperature (Supplementary Fig. 4), which will endow them with better performance as the thermographic phosphor for high-temperature (>1000 °C) thermometry³⁶.

**Fig. 4: Emission spectra of PiSG embedded with various phosphors.**

Discussion

In summary, we have developed a reduction sintering method for rapid producing highly efficient phosphor-silica glass composites. Such a pressureless consolidation technique is compatible with modern 3D printing technique, thus enabling the 3D construction of all-inorganic color converters that are thermally stable up to 1200 °C. We confirmed that interfacial reaction between phosphors and silica glass is intrinsically inhibited without adding any glass modifier cations, and the resultant composites possessing excellent luminescence properties, shows great potential for high-power and high-brightness pc-WLEDs. Our work provides a facile and general synthetic strategy to color-tunable bulk composites based on silica glass for various light-emitting and light-detecting applications, which also have strong implications for develo** innovative glass based composite materials with high-temperature stability⁵¹.

Methods

Materials

HEMA (99%), tetra(ethylene glycol) diacrylate (TTGDA), Diethylene glycol dibenzoate (DEDB, 99.5%), 2,2-dimethoxy-2-phenylacetophenone (DMPA, 99%) and Sudan red G (95%) were purchased from Aladdin, China. Tinuvin 1130 (Basf, Germany). Amorphous silica nanoparticles (a mean diameter of 40 nm, Aerosil OX50) were purchased from Evonik, Germany. Except Al₂O₃:Cr³⁺ prepared by ourselves, all other phosphors are commercially available from phosphor manufacturers (β-Sialon:Eu only from Mitsubishi Chemical, Japan).

Moulding and 3D printing of green bodies

Figure 1a shows the detailed manufacturing process of YAG:Ce-PiSG. 28.1 wt% HEMA, 14.5 wt% DEDB and 3.7 wt% TTGDA were thoroughly mixed. Then, 53.7 wt% amorphous silica nanoparticles were added to the monomer mixture in 100 times and stirred with an agitator (D500 DragonLab) after each addition to form the dispersion. Afterwards, 0.4 wt% DMPA was added into the dispersion (with respect to the amount of reactive monomer). Note that for SLA 3D printing 0.02 wt% Sudan red G was added. Finally, YAG:Ce powder (1–7 wt% with respect to the amount of silica nanoparticles) was mixed into the dispersion, which was defoamed using a vacuum ball mill for 1 h. After that, a homogeneous slurry containing silica nanoparticles and YAG:Ce powders was obtained. For disc-like plates of green bodies, the photopolymerization was performed under a high-power UV lamp (365 nm, 1000 W, 273 mW cm⁻²) for 25 s.

In the 3D printing process, a desktop LCD SLA 3D printer (L1121, isun3d, China) was used. It has a 3.5-inch LCD screen with a resolution of 2560 × 1140 DPI and an array of 405 nm LEDs as the light source. 3D models for printing were designed using SolidWorks (Dassault Systèmes, France) software and exported in the STL file format. The STL files were then imported into the 3D printing software (ChiTu Slicer, China) for slicing and printing. The printing process is automatic and the printing time of one batch depends on the height of the designed parts and the scanning speed of UV light. Finally, the printed green bodies were immersed into isopropyl alcohol for two minutes to remove the surface attachment. To demonstrate the modularization of pc-WLEDs, the size of the hemispherical dome of YAG:Ce-PiSG was designed according to mid-power (1 W) 450 nm LED chip so that the polycarbonate lens can be directly replaced by the as-prepared YAG:Ce-PiSG and sealed with heat conducting silicone (Supplementary Figs. 2 and 3).

Sintering of YAG:Ce-PiSG

The green bodies were first heat-treated at 600 °C in air for 6 h with a heating rate of 1 °C min⁻¹ using a box furnace (KSL-1100X, HF-Ke**g, China). Then, they were sintered at 1250 °C in reducing atmosphere (5%H₂ + 95%N₂) (0.1 L min⁻¹) for 3 h with a heating rate of 3 °C min⁻¹ in a high-temperature tube furnace (GSL-1400X, HF-Ke**g, China). Finally, the obtained YAG:Ce-PiSG was polished for measurements. Other phosphors embedded PiSGs were synthesized by the same procedures with YAG:Ce-PiSG.

Characterization

The transmittance spectra were measured with a UV-vis-infrared spectrometer (U-4100, Hitachi, Japan). Fluorescence microscope image was recorded on the fluorescence microscope (BX53, Olympus, Japan) in the bright-field mode. The distribution of phosphor particles within silica glass was analyzed by using a confocal laser scanning microscope (TCS SP5, Leica, Germany). The emission, excitation and temperature-dependent emission spectra were measured on FLS920P spectrometer (Edinburgh Instruments, UK), where the temperature was controlled by a high-temperature fluorescence test device (TAP-02, Orient KOJI). The IQE and Absorption were measured with a UV-NIR absolute photoluminescence quantum yield spectrometer (Quantaurus-QY Plus C13534-12, Hamamatsu Photonics, Japan), where the error is within 1%. The thermal conductivity measurement was performed by a physical performance measurement system (PPMS, Quantum Design DynaCool-9). All the high-temperature stability tests were conducted in air with a tube furnace. The chemical stability was characterized by a highly accelerated temperature and humidity stress test that the samples are immersed in distilled water and hydrothermally treated at higher than 100 °C for 10 h using a stainless-steel reactor with a Teflon lining, which is much harsher than the standard D85 test (85 °C and 85% relative humidity) as well as the normal hydrolytic resistance test for optical glass⁴⁶. The XRD patterns were obtained on a powder XRD spectrometer (D/MAX 2550/PC, Rigaku, Japan). The SEM images were taken with a scanning electron microscope (Utral-55, Carl Zeiss, Germany), and a layer of gold was sputtered to the surface of the sample to enhance the conductivity. The elementary composition (EDS and EDS map**) was analyzed by an energy-dispersive spectrometer (INCA Energy Coater, Oxford Instruments) coupled to the SEM. TEM image, SAED pattern and EDS line scanning were acquired on a JEM-2100 (JEOL, Japan) operating at 200 kV accelerating voltage. The sample was thinned using the TESCAN GAIA3 that integrates a field emission SEM with a focused ion beam (FIB). Solid-state NMR spectra were obtained on a Bruker Avance III HD 500 M spectrometer (11.7 T). ²⁷Al MAS-NMR spectra were recorded at a resonance frequency of 130.3 MHz (²⁷Al) using a 4 mm MAS-NMR probe at a spinning rate of 12 kHz. The pulse length was 0.56 μs (10°). The relaxation delay was 64 s for YAG:Ce-PiSG, and 40 s for YAG:Ce powder. The chemical shifts of ²⁷Al were referenced to an aqueous solution of 1 M Al(NO₃)₃. A resonance frequency of 99.3 MHz, a spinning rate of 8 kHz and a pulse length of 2 μs (30°) were adopted to acquire the ²⁹Si MAS NMR spectra. The relaxation delays of silica glass and YAG:Ce-PiSG were set as 350 s, and the chemical shifts were referenced to tetrakis(trimethylsilyl)silane.

LED/LD Device fabrication and measurement

High-power pc-WLED devices (Fig. 2d) were fabricated by combining 10 W 450 nm LED chips (Bridgelux, USA) with 5 wt% YAG:Ce-PiSG (0.8 mm in thickness). A power adjustable 455 nm LD (LSR455CP-FC-12W, Lasever, China) was used as the excitation source to evaluate the capability of YAG:Ce-PiSG to withstand high-density radiation. As shown in Fig. 2g, the laser was focused directly on 5 wt% YAG:Ce YAG:Ce-PiSG plate (1 cm in diameter, 0.6 mm in thickness) to form a prototype white LD device, where the beam is nearly circular and the spot size was fixed at a diameter of 1.0 mm (0.785 mm²). The optical output powers of the blue LD under different input currents were measured with a laser power meter (PM100D, Thorlabs). The optical properties of white LED/LD devices including the electroluminescence spectra, Ra, CCT, and LE were measured by an integrated test system (LHS-1000, EVERFINE) including photoelectric characteristic testing system, high accuracy array spectrophotometer (HAAS-2000), stabilized DC power supply, and an integrating sphere (SPEKTRON R98, Φ 80 cm).

Data availability

All the data supporting the findings in this study are available in the paper and Supplementary Information. Additional data related to this paper are available from the corresponding authors upon request.

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Acknowledgements

The authors thank Dr. Huajun Wu and Yongfu Liu for hel** with the measurement of LED/LD devices, and Dr. Jiajia Zhou for helpful suggestion on the manuscript. This work is financially supported by the National Key R&D Program of China (No. 2018YFB1107200), National Natural Science Foundation of China (Nos. 61775192, 51902286, 61905215 and 51772270), open funds of State Key Laboratory of Precision Spectroscopy (East China Normal University) and Wuhan Optoelectronic National Research Center (Huazhong University of Science and Technology), and the Fundamental Research Funds for the Central Universities.

Author information

These authors contributed equally: Dao Zhang, Wenge **ao, Chang Liu.

Authors and Affiliations

State Key Laboratory of Modern Optical Instrumentation, School of Optical Science and Engineering, Zhejiang University, Hangzhou, Zhejiang, 310027, China
Dao Zhang, Wenge **ao, Beibei Xu & Jianrong Qiu
School of Materials Science and Engineering, Zhejiang University, Hangzhou, Zhejiang, 310027, China
Chang Liu & **aofeng Liu
Key Laboratory of Materials for High Power Laser, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai, 201800, China
**jun Ren
CAS Center for Excellence in Ultra-intense Laser Science, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai, 201800, China
Jianrong Qiu

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Dao Zhang
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Wenge **ao
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Chang Liu
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**aofeng Liu
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**jun Ren
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Beibei Xu
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Contributions

W.X., C.L. and J.Q. conceived the idea and initiated the research. J.Q. supervised the project. W.X. and J.Q. designed the experiments. D.Z., W.X. and C.L. performed the experiments and collected the data. W.X., D.Z., C.L., X.L. and B.X. analyzed the data and discussed the results. J.R. conducted the solid-state NMR measurements and analyzed them. W.X., D.Z. and C.L. wrote the manuscript, and X.L., J.R., B.X. and J.Q. revised and commented on it.

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Correspondence to Wenge **ao or Jianrong Qiu.

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W.X., D.Z., C.L., J.Q. and X.L. are inventors on patent applications related to this work (CN110128019A, CN110272208A and PCT/CN2019/122037). All other authors declare no competing interests.

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Zhang, D., **ao, W., Liu, C. et al. Highly efficient phosphor-glass composites by pressureless sintering. Nat Commun 11, 2805 (2020). https://doi.org/10.1038/s41467-020-16649-z

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Received: 10 February 2020
Accepted: 15 May 2020
Published: 04 June 2020
DOI: https://doi.org/10.1038/s41467-020-16649-z
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Highly efficient phosphor-glass composites by pressureless sintering

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Abstract

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Rapid synthesis of phosphor-glass composites in seconds based on particle self-stabilization

Perovskite nanocrystal-embedded glasses for photonic applications

Design of mechanical-robust phosphorescence materials through covalent click reaction

Introduction

Versatile phosphor-silica glass composites

Discussion

Methods

Materials

Moulding and 3D printing of green bodies

Sintering of YAG:Ce-PiSG

Characterization

LED/LD Device fabrication and measurement

Data availability

References

Acknowledgements

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Additional information

Supplementary information

Supplementary Information

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Rapid synthesis of phosphor-glass composites in seconds based on particle self-stabilization

Carbon Nanostructure-based Glass Composites: A Review

Review on transparent polycrystalline ceramics

Patterned glass ceramic design for high-brightness high-color-quality laser-driven lightings

Unique sandwich design of high-efficiency heat-conducting phosphor-in-glass film for high-quality laser-driven white lighting

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Highly efficient phosphor-glass composites by pressureless sintering

Abstract

Similar content being viewed by others

Introduction

Versatile phosphor-silica glass composites

Discussion

Methods

Materials

Moulding and 3D printing of green bodies

Sintering of YAG:Ce-PiSG

Characterization

LED/LD Device fabrication and measurement

Data availability

References

Acknowledgements

Author information

Authors and Affiliations

Contributions

Corresponding authors

Ethics declarations

Competing interests

Additional information

Supplementary information

Rights and permissions

About this article

Cite this article

Share this article

This article is cited by

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