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JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

High-entropy perovskite quantum dots of rare earth synergy with excellent luminescence stability via high-energy ball milling

Sibo Zhao,Hongchen Qiu,Linjing Jing,Yingtong Guo,Mingliang Li,Gang Shao,Bingbing Fan,Hailong Wang,Hongliang Xu,Hongxia Lu

The problem of low stability and high lead content limit the commercial development of halide perovskite . In this paper, the high-energy ball milling is used to rapidly and efficiently synthesize high-entropy Cs(Pb 1/5 Mn 1/5 Ni 1/5 Zn 1/5 Yb 1/5 )Cl 3 quantum dots (QDs), the introduction of high-entropy and rare earth ions reduces lead content, increases mixing entropy, and synergistically enhances the photoluminescence (PL) intensity and stability of QDs with other ions. Because the increase of entropy enhances the stability, the QDs still have 70 % PL intensity after 60 days of placement. After the QDs are exposed to the ultraviolet lamp for 8 hours, the PL intensity maintains at 67.1 % due to the loss of ligand. Ionic bonds are easily broken in water, so after soaking in water for 8 hours, the PL intensity of the QDs keeps at 32 %. The thermal stability of QDs is maintained well because of physical and chemical stability of rare earth ions. Since ethanol dissolves the ligands on the surface of the QDs, the non-radiative recombination is enhanced, so the PL intensity of QDs remains at 59 % after soaking for 8 hours. This paper provides a new way that further enhances the stability and solves high lead content of all-inorganic perovskite materials.

研究领域: 材料科学 · 光学
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Journal of Materials Chemistry C · 2024 · IF 5.7

Ultra-stable CsPbBr3-embedded polymer films for spectrally tunable X-ray nuclear batteries and flexible radiation imaging applications

Dongdong Liang,Zhiheng Xu,Dandan Yang,Zhibin Xu,Weitong Yin,Xiaobin Tang

Luminescence instability in service environments has limited the widespread use of halide perovskite materials, especially for X-ray energy conversion and detection/imaging. This work proposed a method for improving luminescence stability through polymer encapsulation, which is more convenient than compositional engineering and surface modulation. Meanwhile, the differences in the luminescence intensities of composite films synthesized by encapsulation of different polymer matrices and their luminescence stability under various harsh X-ray irradiation conditions were systematically investigated. The applications of the developed CsPbBr3-embedded polymer films with excellent luminescence performance and high service stability in X-ray radiation energy utilization and detection/imaging were discussed. The results show that CsPbBr3-embedded PS films can meet the spectral modulation requirements of radioluminescent materials for nuclear batteries and can also fulfill the needs of flexible X-ray imaging with a high spatial resolution.

研究领域: 材料科学 · 辐射物理 · 核工程 · 成像技术
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CERAMICS INTERNATIONAL · 2023 · IF 5.2

Enhanced luminescence stability of high-entropy dual-phase Cs(Pb1/5Mn1/5Ni1/5Zn1/5Cd1/5)Br3/Cs(Pb1/5Mn1/5Ni1/5Zn1/5Cd1/5)2Br5 perovskite nanocrystals coated with SiO2 and EVA

Sibo Zhao,Hengbin Mao,Weishan Ma,Mingliang Li,Shao Gang,Bingbing Fan,Hailong Wang,Hongliang Xu,Hongxia Lu

All-inorganic halide perovskite nanocrystals (NCs) have attracted much attention in many fields. However, the poor stability of NCs and the toxicity of Pb have greatly hindered their practical applications. Reducing the proportion of Pb with the concept of high-entropy and coating NCs with an outer layer have been regarded as effective strategies to solve the problems. Herein, We have successfully synthesized the all-inorganic high-entropy dual-phase Cs(Pb 1/5 Mn 1/5 Ni 1/5 Zn 1/5 Cd 1/5 )Br 3 /Cs(Pb 1/5 Mn 1/5 Ni 1/5 Zn 1/5 Cd 1/5 ) 2 Br 5 (Cs‘B’Br 3 /Cs‘B’ 2 Br 5 ) perovskite NCs with good luminescence properties by a high-energy ball milling method; On the basis of which, Cs‘B’Br 3 /Cs‘B 2 ’Br 5 NCs are coated with SiO 2 and EVA resin. Due to the amorphous SiO 2 protection, the Cs‘B’Br 3 /Cs‘B 2 ’Br 5 @SiO 2 NCs maintained 93% of their emission intensity after 90 days compared to their uncoated counterparts. The PL intensity of Cs‘B’Br 3 /Cs‘B 2 ’Br 5 NCs /EVA was significantly enhanced by a factor of 4.7 for compared to the uncoated NCs. In addition, the PL emission intensity of the Cs‘B’Br 3 /Cs‘B 2 ’Br 5 NCs /EVA remained 93.7% after 90 days, and the emission peak intensity remained approximately 63% after 8 h of placement in an enclosed environment at 80% humidity through the dense polymer chains and the hydrophobic nature of the film. Finally, the film could expand its application prospects in the field of flexible device.

研究领域: 材料科学 · 光学
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ADVANCED MATERIALS · 2025 · IF 26.8

Quantum Dot Luminescence Microspheres Enable Ultra-Efficient and Bright Micro-LEDs

Ting Gong,Tongtong Xuan,Wenhao Bai,Haorui Dong,Kai Huang,Rong-Jun Xie

Quantum dot (QD)-converted micrometer-scale light-emitting diodes (micro-LEDs) are regarded as an effective solution for achieving high-performance full-color micro-LED displays because of their narrow-band emission, simplified mass transfer, facile drive circuits, and low cost. However, these micro-LEDs suffer from significant blue light leakage and unsatisfactory electroluminescence properties due to the poor light conversion efficiency and stability of the QDs. Herein, the construction of green and red QD luminescence microspheres with the simultaneously high conversion efficiency of blue light and strong photoluminescence stability are proposed. These luminescence microspheres exhibit high external photoluminescence quantum yields exceeding 46% under 450 nm excitation, along with excellent reliability against blue light, heat, and water-oxygen degradation, owing to the waveguide and spatial confinement effects of the microspheres. The microsphere-based green and red micro-LEDs achieve world-record external quantum efficiencies of 40.8% and 22.1%, respectively, and high brightness values of 1.7 × 10 8 and 7.6 × 10 7 cd m −2 , respectively. Finally, 0.6 inch red, green, and blue monochrome micro-LED displays are demonstrated by integrating microsphere-converted micro-LED arrays with thin-film transistor backplanes, which show a pixel resolution as high as 1700 PPI and brightness exceeding 10 000 cd m −2 .

CAS / MDL: 57-09-0
研究领域: 材料科学 · 光电技术 · 显示技术
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Dielectric screening enabled ultrastable luminescence in CsPbBr3 perovskite crystal encapsulated by ferroelectric Poly(vinylidene fluoride)

Chen Huang,Yao Wang,Ziwei Cheng,Yu Wu,Jiaxin Li,Yuan Deng

Metal halide perovskites nanocrystals (NCs) are emerging as competitive alternatives for semiconductor NCs in the fields of consumer optoelectronic devices; however, boosting their long-term stability still needs extensive study. Encapsulation of perovskite NCs with polymer becomes a promising strategy, yet the dielectric screening effect on the excitons of perovskites from the polymer matrix has seldom been considered. Here, we demonstrated this effect in high-permittivity poly(vinylidene fluoride) (PVDF) encapsulated CsPbBr 3 (CPB) crystals CPB/PVDF composites films. The in situ nonuniform growth mechanism of CPB crystal with respect to its concentration in the precursor was revealed from multiscale structure observations. Comprehensive physical properties of CPB/PVDF composites with varying CPB concentrations were thoroughly investigated. Composite films made from precursors with CPB concentration increasing to saturation all showed bright luminescence, and an exceptional long fluorescence lifetime up to τ avg  = 731 ns was observed, much superior to other polymers with lower permittivity encapsulated CPB composites. The stable luminescence is understood from the strong interplay between electron-hole Coulomb interactions in CPB and its surrounding high-permittivity PVDF. Meanwhile, the interfacial interaction between CPB and PVDF greatly influenced the crystallization behavior of PVDF polymer at nanoscale, thus altered the dielectric and mechanical properties of CPB/PVDF composite films accordingly. Finally, a warm white light-emitting diode device was assembled based on green light emitting CPB/PVDF film, positively implying its potential application in high-performance optoelectronic devices.

CAS / MDL: 7787-69-1 10031-22-8
研究领域: 材料科学 · 光学 · 电子工程
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Journal of Materials Chemistry C · 2020 ·Vol. 8 ·期 32 ·11110-11118 · IF 7.059

Core–shell metal–organic frameworks and hierarchical host–guest structures toward water-stable luminescence of lanthanide complexes in encoding beads

Dong Mo,Zhengqiang Wang,Kaiyao Sun,Xiyue Xie,Jixi Zhang,Kaiyong Cai

The photoluminescence stability of lanthanide complexes (Lnx) in biological media is of the utmost significance for the construction of optically encoded nano-on-microbeads in multiplex bioassays. Herein, we propose a new type of encoding guest consisting of MOF@MOF nanohybrids, where isomorphic ZIF-8 and ZIF-90 were employed as the core and shell domain, respectively, to separately modulate the hosting and the protection of the inner Lnx guests. Especially, the thin ZIF-90 shell epitaxially grown on the ZIF-8 core was employed as an intermediate layer to facilitate surface covalent fluorination via an aldehyde ligand. Thereby, a superhydrophobic surface was obtained, which led to strong water-resistance of the hybrid nanoparticles, stable host–guest structure, and high quantum yields (19.1%) in biological media. A coating layer of a surface active polymer (polydopamine, PDA) was utilized to conjugate the MOF nanoparticles on polystyrene microspheres for building the second-level host–guest architecture of 3D core–satellite pluralistic hybrids. Finally, single/dual-color encoded beads (EBs) were obtained by altering the ratios of the hybrid MOF guests emitting at different wavelengths. As a proof of concept, the detection of a model tumor marker (alpha-fetoprotein, AFP) was successfully performed using the encoded beads. These findings can pave the way for the rational design of core–shell MOFs and hierarchical structures with high synergy and excellent flexibility toward stable photoluminescence of lanthanide complexes in bioassays.

研究领域: 材料科学 · 生物医学工程 · 分析化学
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INORGANIC CHEMISTRY · 2019 · IF 4.85

Synthesis and Luminescence Properties of CsPbX3@Uio-67 Composites toward Stable Photoluminescence Convertors

Diwei Zhang,Jing Zhao,Quanlin Liu,Zhiguo Xia

All-inorganic halide perovskite (CsPbX3, X = Cl, Br, or I) nanocrystals (NCs) have been widely studied due to their outstanding optoelectronic properties. However, some inevitable factors like light, heat, and moisture affected the stability of CsPbX3 NCs and further limited their practical application. In this work, the stability of all-inorganic halide perovskite NCs can be improved by integrating them in the stable Zr-based metal–organic frameworks (Uio-67). Compared to pristine perovskite NCs, typical CsPbBr3@Uio-67 composites display a stable photoluminescence property that can be maintained for 30 days under ambient atmospheric conditions. Due to the proposed confinement effects of CsPbX3 NCs coordinated with the pore structures of Uio-67, the related structural model of CsPbX3@Uio-67 composites was elucidated. White LED device was further fabricated by combining CsPbBr3@Uio-67 composites and commercial K2SiF6:Mn4+ red phosphors with a blue-emitting chip, which demonstrated a wide color gamut (138% of National Television Standards Committee color space). The strategy on encapsulation of CsPbX3 NCs into Uio-67 will open up a stable platform for optoelectronic applications.

研究领域: 材料科学 · 光学工程 · 纳米技术
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Graphene quantum dots via ion modification for improving photoluminescence stability in aqueous solution with heavy metal ions

Juan Yang,Pei Li,Zailing Song,Jie Li,Huan Yang,Fan Yan,Lu Li,Can Xu,Junlang Chen,Liang Chen

Graphene quantum dots (GQDs) have shown growing potential in the applications of ion detection, anti-counterfeiting ink and light-emitting devices. However, the photoluminescence (PL) properties of GQDs will be lost when they interact with some heavy metal ions. Effective strategies to improve PL stability are still limited. In this work, we prepared a new kind of GQDs modified by scandium ions (Sc 3+ ) to improve the PL of GQDs in aqueous solution containing heavy metal ions. The Sc 3+ modified GQDs (Sc@GQDs) show a slight fluorescence enhancement compared with pristine GQDs. In addition, the PL of pristine GQDs could be quenched by Fe 3+ /Cu 2+ /Cr 3+ , while the PL of Sc@GQDs was kept stable with these heavy metal ions. Meanwhile, GQDs modified by Al 3+ and Ga 3+ exhibit similar results, which further verifies the universality of this method that GQDs modified by specific metal ions to maintain the PL of GQDs with heavy metal ions. As applications, Sc@GQDs may have great potential in the fields of fluorescent flexible device and fluorescent ink.

研究领域: 材料科学 · 光学 · 环境科学
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Advanced Optical Materials · 2018 ·Vol. 7 ·期 4 ·1801323 · IF 7.43

One-Step Loading on Natural Mineral Halloysite Nanotube: An Effective Way to Enhance the Stability of Perovskite CsPbX3 (X = Cl, Br, I) Quantum Dots

Jiarui Hao,Xingyu Qu,Lei Qiu,Guogang Li,Yi Wei,Gongcheng Xing,Hongquan Wang,Chunjie Yan,Ho Seong Jang,Ziyong Cheng,Jun Lin

Currently, poor luminescence stability seriously impedes the practical application of inorganic halide perovskite (CsPbX 3 , X = Cl, Br, and I) quantum dots (QDs) in optoelectronic devices. In present work, CsPbX 3 QDs are successfully assembled on natural mineral halloysite nanotubes (HNTs) for improving the luminescence performances. Monodispersed CsPbX 3 QDs are arranged on two edges of HNTs in a highly ordered manner, which possibly originates from the electrostatic interaction between halogen ion and surface hydroxyl (Sur  OH 2 + ) on the section face of HNTs. As expected, the photoluminescence (PL) performances of CsPbX 3 @HNTs nanocomposites are obviously improved. The PL intensity still can be maintained even 80% when working at 100 °C. Almost no emission degradation is observed after storing in an open ambient condition for 28 days. Moreover, the PL intensity also maintains 82% of room temperature (RT) intensity after continuously being illuminated by 365 nm UV lamps for 144 h. Excellent white light with Commission Internationale de l'Eclairage (CIE) chromaticity coordinates (0.34, 0.32) of the white light-emitting diodes (w-LEDs) fabricated by CsPbBr 3 @HNTs, CsPbBr 1.2 Cl 1.8 @HNTs, and CsPbBr 1.2 I 1.8 @HNTs phosphors are achieved. This work opens up a new insight in achieving stable CsPbX 3 QD-based multifunctional materials by designing nanocomposites with natural clay mineral.

研究领域: 材料科学 · 光学 · 纳米技术
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Nanophotonics · 2018 ·Vol. 7 ·期 12 ·1949-1958 · IF 6.014

Stretchable and self-healable organometal halide perovskite nanocrystal-embedded polymer gels with enhanced luminescence stability

Minjie Fang,Sihui Huang,Dong Li,Chunli Jiang,Pei Tian,Hechun Lin,Chunhua Luo,Wenlei Yu,Hui Peng

Stretchable and self-healing polymer gels with luminescent property are very promising materials for next generation soft optical devices. This work presents the preparation of self-healing and luminescent polymer gels by simply blending organometal halide perovskite nanocrystals (OHP NCs) with poly(dimethylsiloxane)-urea copolymer (PDMS-urea). On the one hand, the obtained luminescent gels are not only flexible, stretchable and relatively transparent, they also exhibit excellent self-healing capability due to the reversible hydrogen bonding network in the PDMS-urea copolymer. On the other hand, the embedding of OHP NCs (MAPbBr 3 and MAPbI 3 NCs) inside the hydrophobic PDMS-urea gel greatly improved the photoluminescence stability of OHP NCs against water. Their applications as phosphors for LEDs have been demonstrated. Both the MAPbBr 3 /PDMS-urea gel and MAPbI 3 /PDMS-urea gel can fully convert the blue emission of GaN chip to green and red emissions, respectively. These gels can be used as photoluminescent materials in flexible optical devices with good self-healing capability.

研究领域: 材料科学 · 光学工程
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Advanced Optical Materials · 2023 ·Vol. 11 ·期 16 ·2300306 · IF 9

Spectrally Stable Pure Red CsPbI3 Quantum Dots Light-Emitting Diodes via Effective Low Temperature Gradient Centrifugation Separation and Surface Modification

Wei Shen,Zhan Su,Shuo Chen,Yujun Dai,Yue Qiu,Yanfeng Chen,Jiayu Jiang,Jianbin Zhang,Yun Wang,Hao Cui,Yanxing He,Kun Cao,Bo Cai,Lihui Liu,Shufen Chen

Development of high-performance and stable pure red perovskite light-emitting devices (LEDs) promotes commercialization of perovskite. Benefiting from the quantum confinement effect, pure red CsPbI 3 quantum dots (QDs) can avoid the color drift issue for mixed halide systems. Herein, a facile temperature-dependent hot-injection method combined with low temperature gradient centrifugation is employed to prepare 5.60 ± 0.05 nm pure red QDs. The QDs exhibit 642 nm photoluminescence (PL) with 37 nm full width at half maximum, and their Commission Internationale de l'Eclairage (CIE) coordinates located at (0.708, 0.292) match well with standard pure red for Rec. 2020. The PL half-lifetime for pure red QDs solution is 210 days under ambient conditions, and both the X and Y coordinates of CIE only fluctuate within (0.002, 0.002). Finally, a simple NH 4 I post-treatment to decrease ligand length further boosts the QDs conductivity, and the pure red LED exhibits 9.4% maximum external quantum efficiency. The electroluminescence spectra exhibits a sharp peak at 645 nm, and their CIE coordinates are located at (0.707, 0.290). Furthermore, the pure red LED exhibits both good working and color stability. Its half-lifetime is 25.1 min and color drifts are only (0.002, 0.002) after 30.0 min of continuous working at 60 cd m −2 with a constant current density of 3.5 mA cm −2 .

研究领域: 材料科学 · 光电技术 · 纳米科技
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Unveiling the Structure-Luminescence-Stability relationship in 5s2-Based Antimony halides toward High-Performance emitters

Lei Zhou,Lei Zhang,Yuanyuan Chang,Ming Li,Rongxing He

Emerging low-dimensional metal halides have attracted enormous research interests due to their prominent photoluminescence (PL) properties and extensive application potentials. However, the systematic discussion on the structure-luminescence-stability relationship is still lacking. Herein, a series of novel lead-free metal halides are developed to unveil the underlying relationship. The as-synthesized (C 6 H 5 NH 3 ) 6 SbCl 9 ·H 2 O single crystal is structurally unstable that would spontaneously transform into (C 6 H 5 NH 3 ) 3 ClSbCl 5 ·H 2 O in the mother liquor, due to the strong antibonding Sb-5s 2 lone pair with a spherical distribution in highly symmetrical geometry. To suppress this effect and stabilize the metastable phase, In 3+ without ns electrons is introduced into the lattice of (C 6 H 5 NH 3 ) 6 SbCl 9 ·H 2 O, as a result, the changed coordination environment, including band structure, lattice constant and intermolecular electronic interaction, not only inhibits the structure transformation, but also leads to an enhanced PL efficiency (83.37 %) at ∼ 600 nm. This work promotes the understanding of structure-luminescence-stability relationship in organic–inorganic materials, and provides a new insight for further searching for high-performance lead-free perovskite luminescent materials.

研究领域: 材料科学 · 光学
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