Journal of Materials Chemistry C
·
2024
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IF 5.7
Yongrun Dong,Wen Li,Tao Huang,Shuaigang Ge,Linghang Kong,Chuang Ning,Zequan Li,Wei Gao,Bingsuo Zou
Recently, lead-free double perovskites have been regarded as a promising alternative to lead halide perovskites due to their wide emission band, and environmental protection and stability properties, and are expected to become a series of rising star materials in the lighting field. However, currently, the growth of most lead-free double perovskites occurs in the strong acid environment, which not only brings high cost and environment risk, but also makes it hard to realize large-scale applications with powder products. Herein, we apply a strategy of in situ synthesis of lead-free double perovskites in a polymer matrix by using a small amount of precursors and relatively friendly DMSO solvent to obtain efficiently luminescent Sb3+/Mn2+ co-doped Cs2KInCl6/PVDF composite films in a large-area. The co-doping of Mn2+/Sb3+ into this inorganic double perovskite matrix makes microcrystals with good crystallinity and size distribution in this polymer. The as prepared co-doping composite film with Mn/Sb feeding ratio 16 : 1 shows the brightest white light emission under 320 nm excitation, with a photoluminescence quantum yield (PLQY) as high as 86.98%. The energy transfer (E-T) from the charge-transfer band to the triplet self-trapped exciton (STE) around Sb3+ and then to the ferromagnetic (FM) coupled Mn2+ pair 3d state was confirmed by the temperature-dependent PL spectra and density functional theory calculations. Finally, a single-compound white light emitting diode with chromatic coordinates of (0.31, 0.33) and fluorescent anti-counterfeiting labels could be fabricated based on this composite film with the best white emission. This work provides a new strategy for the application of lead-free double perovskites in the fields of lighting and anti-counterfeiting.
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Polymers
·
2024
·Vol. 16
·期 11
·1568
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IF 4.7
Yinbiao Shi,Xiaojia Su,Xiaoyan Wang,Mingye Ding
Inorganic CsPbX3(X = Cl, Br, I) perovskite quantum dots (PQDs) have attracted widespread attention due to their excellent optical properties and extensive application prospects. However, their inherent structural instability significantly hinders their practical application despite their outstanding optical performance. To enhance stability, an in situ electrospinning strategy was used to synthesize CsPbX3/polyacrylonitrile composite nanofibers. By optimizing process parameters (e.g., halide ratio, electrospinning voltage, and heat treatment temperature), all-inorganic CsPbX3PQDs have been successfully grown in a polyacrylonitrile (PAN) matrix. During the electrospinning process, the rapid solidification of electrospun fibers not only effectively constrained the formation of large-sized PQDs but also provided effective physical protection for PQDs, resulting in the improvement in the water stability of PQDs by minimizing external environmental interference. Even after storage in water for over 100 days, the PQDs maintained approximately 93.5% of their photoluminescence intensity. Through the adjustment of halogen elements, the as-obtained composite nanofibers exhibited color-tunable luminescence in the visible light region, and based on this, a series of multicolor anti-counterfeiting patterns were fabricated. Additionally, benefiting from the excellent water stability and optical performance, the CsPbBr3/PAN composite film was combined with red-emitting K2SiF6:Mn4+(KSF) on a blue LED (460 nm), producing a stable and efficient WLED device with a color temperature of around 6000 K and CIE coordinates of (0.318, 0.322). These results provide a general approach to synthesizing PQDs/polymer nanocomposites with excellent water stability and multicolor emission, thereby promoting their practical applications in multifunctional optoelectronic devices and advanced anti-counterfeiting.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Xiangcong He,Wenna Liu,Hui Fu,Chris R. Bowen,Jizhong Liu,Xie Li,Abdul Rehman Akbar,Jinju Zheng,Weiyou Yang
Incorporating perovskite nanocrystals (PNCs) into poly(vinylidene fluoride) (PVDF) is an effective method to improve the performance of PVDF-based piezoelectric nanogenerators (PENGs). The conventional techniques are typically performed via a two-step process, namely, the synthesis of PNCs and then introducing them into the PVDF matrix. Here, we report the exploration of flexible PENG with boosted performance by in situ growth of Zr-doped Cs2Ag0.3Na0.7InCl6 double perovskites (ZCDP) within the PVDF matrix (PENGin). The as-constructed PENGin delivers an open-circuit voltage of 44.4 V and a short-circuit current density of 10 μA cm–2, both of which are more than 2 times those of PENGs built by a conventional two-step process and ∼6 and ∼9 times the best ones of in situ grown Cs2InI6@PVDF-based PENGs ever reported, respectively. The enhanced performance could be ascribed to the optimized spontaneous polarization, thanks to the uniform dispersion of PNCs with a solid ZCDP/PVDF interface within the matrix, which collectively facilitates the electron migration and aggregation, thereby establishing a strong built-in electric field to amplify the dipole spontaneous polarizability. Additionally, the PENGin exhibits excellent performance with robust stability in pressure sensing, wearable energy harvesting, and DC power applications, representing its promise toward practical use.
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Journal of Materials Chemistry C
·
2024
·
IF 5.7
Junnan Wang,Zeyu Wang,Nikolai V. Gaponenko,Jindou Shi,Zheyuan Da,Chen Zhang,Yongqiang Ji,Qing Yao,Youlong Xu,Minqiang Wang
X-ray imaging technology has been integral to numerous aspects of people's lives since its inception. With the growing demand for advanced imaging technologies, lead-free metal halide perovskites have received significant attention due to their non-toxicity, stability, and excellent optical properties. This paper investigates the scintillation behaviour of a Te doped Cs2SnCl6 scintillator composite film (CF) prepared through an innovative in situ growth strategy. This approach achieves the direct growth of Cs2SnCl6:Te micro-crystals within polymethyl methacrylate (PMMA), mitigating the issues of optical property degradation and inhomogeneous distribution that are inevitable in a conventional two-step mixing method. By controllable optimization of the doping ratio of Te, the Cs2SnCl6:Te/PMMA CFs exhibited exceptional scintillation properties under X-ray irradiation, with the detection limit reaching up to 112 nGyairs−1. In X-ray imaging applications, the Cs2SnCl6:Te 15%/PMMA CF demonstrated advanced sensitivity, producing high-resolution structural images of the target object. This advancement highlights the promising potential of lead-free metal halide perovskites in the development and application of X-ray imaging technology.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Wen Li,Yongrun Dong,Ting Xie,Tongzhou Li,Chuang Ning,Tao Huang,Zequan Li,Wei Gao,Bingsuo Zou
Lead-free double perovskites (DPs) have superior phase stability and optical properties, which make them competitive for future applications in illumination and displays. However, the preparation of DPs was mainly based on high-temperature heating and hydrochloric acid as a solvent to form powders, which increased the risk and cost of the preparation process and limited its further application. In this study, the growth of Cs2NaInCl6: Sb3+ DPs in polyvinylidene difluoride (PVDF) films was achieved using an in situ fabrication strategy with DMSO as the solvent. The prepared Cs2NaInCl6: Sb3+@PVDF composite films (CFs) can achieve a bright blue emission under 302 nm irradiation. To achieve the optimal luminescent performance of CFs, the photoluminescence (PL) intensity of Cs2NaInCl6: Sb3+@PVDF CFs under various in situ preparation conditions was compared. In addition, the photoluminescence quantum yield (PLQY) of CFs was increased from 0.72% to 83.77% by adjusting the doping amount of Sb3+, and the fluorescence lifetimes t1 and t2 were 131.08 and 1048.52 ns, respectively. Temperature-dependent PL spectroscopy and density functional theory (DFT) calculations indicate that these excellent optical properties are derived from the self-trapped excitons (STEs) at the [SbCl6]3– octahedron and [InCl6]3– octahedron connected via Cl–Na–Cl. The CFs also demonstrated excellent environmental stability, maintaining a relatively stable PL intensity even under conditions of water immersion, high temperatures, and ultraviolet (UV) radiation. Finally, we used the CFs to assemble a blue light-emitting device (LED), which showed good and stable blue emission performance at different currents. This work can provide a new idea for preparing DPs, which is conducive to promoting their commercial application in high-performance optoelectronic devices.
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Journal of Energy Chemistry
·
2024
·
IF 14
Baofei Sun,Wei Chen,Yanyi Huang,Daofu Wu,Heng Luo,Faguang Kuang,Hongmei Ran,Yichen Liu,Liqin Gao,Jinchen Zhou,Bo Gao,Qiang Huang,Xiaosheng Tang
Metal halide perovskites (MHP) are potential candidates for the photocatalytic reduction of CO 2 due to their long photogenerated carrier lifetime and charge diffusion length. However, the conventional long-chain ligand impedes the adsorption and activation of CO 2 molecules in practical applications. Here, a ligand modulation technology is employed to enhance the photocatalytic CO 2 reduction activity of lead-free Cs 2 AgInCl 6 microcrystals (MCs). The Cs 2 AgInCl 6 MCs passivated by Oleic acid (OLA) and Octanoic acid (OCA) are used for photocatalytic CO 2 reduction. The results show that the surface defects and electronic properties of Cs 2 AgInCl 6 MCs can be adjusted through ligand modulation. Compared with the OLA-Cs 2 AgInCl 6 , the OCA-Cs 2 AgInCl 6 catalyst demonstrated a significant improvement in the catalytic yield of CO and CH 4 . The CO and CH 4 catalytic yields of OCA-Cs 2 AgInCl 6 reached 171.88 and 34.15 µmol g −1 h −1 which were 2.03 and 12.98 times higher than those of OLA- Cs 2 AgInCl 6 , and the total electron consumption rate of OCA-Cs 2 AgInCl 6 was 615.2 µmol g −1 h −1 which was 3.25 times higher than that of OLA-Cs 2 AgInCl 6 . Furthermore, in situ diffuse reflectance infrared Fourier transform spectra revealed the enhancement of photocatalytic activity in Cs 2 AgInCl 6 MCs induced by ligand modulation. This study illustrates the potential of lead-free Cs 2 AgInCl 6 MCs for efficient photocatalytic CO 2 reduction and provides a ligand modulation strategy for the active promotion of MHP photocatalysts.
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JOURNAL OF RARE EARTHS
·
2025
·
IF 7.2
Zehua Zhang,Lili Wang,Ruiliang Zuo,Zhenzhen Jiang,Guangyong Jin
The single-component white light emission microcrystals were synthesized in Bi 3+ /Sb 3+ /Ho 3+ ions tri-doped Cs 2 Ag 0.2 Na 0.8 LuCl 6 double perovskites by a simple precipitation method. In Bi 3+ /Sb 3+ ions double-doped Cs 2 Ag 0.2 Na 0.8 LuCl 6 microcrystals, the tunable emission from yellow (Bi 3+ ) to blue (Sb 3+ ) can be achieved under ultraviolet light excitation. Particularly, the white light emission is obtained after doping Ho 3+ ion because of the energy transfer processes of Bi 3+ →Ho 3+ and Sb 3+ →Ho 3+ . The chromaticity coordinates (CIE) of Cs 2 Ag 0.2 Na 0.8 LuCl 6 :5 mol% Bi 3+ ,1 mol% Sb 3+ ,15 mol% Ho 3+ microcrystal are (0.3354, 0.3394) under 315 nm excitation. Meanwhile, the white light emissions with different color temperatures are obtained through varying the excitation wavelength (255–365 nm). Additionally, temperature-dependent fluorescence spectra show that the emission intensity of Bi 3+ /Sb 3+ /Ho 3+ tri-doped Cs 2 Ag 0.2 Na 0.8 LuCl 6 microcrystal at 423 K remains 54% of that at 303 K. Moreover, the fluorescence intensity ratio (FIR) of 641 and 665 nm is highly temperature-dependent, the relative sensitivity ( S r ) reaches 1.06%/K at 303 K under 315 nm excitation. Simultaneously, the microcrystal shows thermochromism phenomenon, and the emission changes from white to blue-purple with the increase of temperature from 303 to 513 K. The novel temperature sensing is achieved based on CIE coordinates and temperature technology in Cs 2 Ag 0.2 Na 0.8 LuCl 6 :5 mol% Bi 3+ ,1 mol% Sb 3+ ,15 mol% Ho 3+ microcrystal by exciting at 315 nm. The corresponding maximum S r is 0.34%/K. Accordingly, Bi 3+ /Sb 3+ /Ho 3+ ions tri-doped Cs 2 Ag 0.2 Na 0.8 LuCl 6 double perovskite has potential applications in the fields of white light emitting diode and optical temperature sensing.
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JOURNAL OF LUMINESCENCE
·
2024
·
IF 3.3
Yiying Zhu,Yining Wang,Yixin Sun,Zheng Xu,Mengmeng Shang
Lead-free double perovskites (LFDPs) usually exhibit poor luminescent performance, and doping lanthanide ions (Ln 3+ ) presents a promising solution to solve this problem. However, most Ln 3+ ions face difficulties in incorporating into LFDPs due to the mismatch in radius or valence state. Here, we successfully synthesized rare-earth (RE 3+ ) based Cs 2 NaLuCl 6 (CNLC) LFDPs and achieved efficient green emission through doping Tb 3+ into CNLC. Introducing Sb 3+ improves the absorption efficiency of CNLC: Tb 3+ from 25.1 % to 73.5 % by establishing an energy transfer channel from Sb 3+ to Tb 3+ . Benefiting from the energy transfer, the CNLC: 0.01Sb 3+ , 0.10Tb 3+ phosphor produces blue-green dual emissions, highlighting its potential in white light-emitting diodes (WLEDs). In addition, an anti-counterfeiting pattern composed of CNLC: Sb 3+ , CNLC: Tb 3+ , and CNLC: Sb 3+ , Tb 3+ samples was fabricated, which shows their promising prospect in anti-counterfeiting applications.
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CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Huabiao Tao,Yuyin Fang,Yuanpeng Zhang,Yuepin Zhang,Jianxu Hu
Optical temperature sensing based on luminescence intensity ratio shows significant potential in achieving accurate temperature detection. In this work, Sb 3+ /Mn 2+ co-doped Cs 2 NaYCl 6 double perovskites were synthesised via a hydrothermal method . Introducing Sb 3+ ions to the host significantly enhances the radiative recombination of self-trapped excitons (STEs), resulting in a broad blue emission. The co-doping of Mn 2+ ions to the composition leads to a tunable dual-emission in the spectra, originating from the energy transfer between the STEs and Mn 2+ ions. The dependence of the dual-emission on temperature is employed for optical temperature sensing. The maximum relative sensitivity, optimal thermal resolution, and optimal thermal repeatability are determined as 1.40 % K −1 , 0.002 K and 99.3% at 250 K, respectively. The results indicate that the synthesised Cs 2 NaYCl 6 : Sb 3+ /Mn 2+ double perovskites are promising candidates for high-sensitivity optical thermometers.
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JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Yufan Yuan,Danping Li,Huajun Huang,Jinbao He,Chenglong Yu,Yanpeng Gao,Davide Vione,Hansun Fang
The direct photodegradation quantum yields ( Φ ) of five representative aromatic carbamate pesticides - carbaryl, carbofuran, propoxur, isoprocarb, and metolcarb - were examined in both aqueous and non-aqueous solutions, the latter mimicking hydrophobic environments such as leaf surfaces. For carbaryl, carbofuran, isoprocarb, and metolcarb, the Φ values generally followed the order Φ water < Φ MeOH < Φ n - hexane , while propoxur showed a different trend, Φ MeOH < Φ n-hexane < Φ water . Scavenging and laser flash photolysis experiments, combined with quantum chemical calculations, were used to clarify the photodegradation mechanisms. Photodegradation is primarily initiated by the singlet excited state (S*), with the triplet state (T*) also contributing in compounds with conjugated structures, such as carbaryl. Upon excitation, MCAEs generated both radical cations (S •+ ) and phenoxyl radicals (S-O • ), and S •+ would convert to S-O • subsequently. S-O • is predominantly generated through the cleavage of C-O bonds in ester groups, subsequently abstracting hydrogen from solvent molecules. The reactivity of hydrogen donors in these solvents follows the order: -CH 2 - > -CH 3 > -OH. For propoxur, the ether group also contributes to the formation of S-O • , which further reacts with H 2 O and enhances degradation in aqueous environments. Solvent polarity had a minimal effect on photodegradation. This comparative study of degradation in aqueous and nonaqueous phases provides insights for designing and selecting pesticides that are effective during use in nonaqueous environments, such as on leaf surfaces, yet degrade rapidly in aqueous environments in the post-application phase.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Xiaoxi Li,Yinsheng Xu,Weiwei Li,Ying Ye,Xianghua Zhang,Mengling Xia,Chao Liu,Guangda Niu,Jiang Tang
Laser lighting devices, comprising an ultraviolet (UV) laser chip and a phosphor material, have emerged as a highly efficient approach for generating high-brightness light sources. However, the high power density of laser excitation may exacerbate thermal quenching in conventional polycrystalline or amorphous phosphors, leading to luminous saturation and the eventual failure of the device. Here, for the first time, we raise a single-crystal (SCs) material for laser lighting considering the absence of grain boundaries that scatter electrons and phonons, achieving high thermal conductivity (0.81 W m–1 K–1) and heat-resistance (575 °C). The SCs products exhibit a high photoluminescence quantum yield (89%) as well as excellent stability toward high-power lasers (>12.41 kW/cm2), superior to all previously reported amorphous or polycrystalline matrices. Finally, the laser lighting device was fabricated by assembling the SC with a UV laser chip (50 mW), and the device can maintain its performance even after continuous operation for 4 h. Double perovskite single crystals doped with Yb3+/Er3+ demonstrated multimodal luminescence with the irradiation of 355 and 980 nm lasers, respectively. This characteristic holds significant promise for applications in spectrally tunable laser lighting and multimodal anticounterfeiting.
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PHYSICA B-CONDENSED MATTER
·
2024
·
IF 2.8
Xiumei Dong,Ruikun Pan
Recently Cu-doped all-inorganic zero-dimensional (0D) metal halides Cs 2 ZnX 4 (X = Cl, Br) have attracted many researchers due to their excellent fluorescence (FL) performance and low toxicity compared to lead-based perovskites . Although these 0D metal halides nanocrystals or small-sized single crystals are prepared via solution methods in most of the reports, we used the solid-state synthesis method to get Cu-doped Cs 2 ZnCl 4 powders and characterized their FL properties. The results and analysis indicate that Cu 2+ can be doped in Cs 2 ZnCl 4 up to 12 at.%, which enhances the FL of Cs 2 ZnCl 4 powder. The photoluminescence quantum yield (PLQY) at 480 nm rises from 1.11 % (undoped) to 20.06 % (6 at.% Cu doping). A modified triplet self-trapped excitons mechanism is presented to explain the enhanced Cu − doped Cs 2 ZnCl 4 powder.
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