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Advanced Optical Materials · 2021 ·Vol. 9 ·期 11 ·2100012 · IF 9.926

One-Pot Synthesis of CsPbX3 (X = Cl, Br, I)@Zeolite: A Potential Material for Wide-Color-Gamut Backlit Displays and Upconversion Emission

Yao Tong,Qin Wang,Enrou Mei,Xiaojuan Liang,Wei Gao,Weidong Xiang

All-inorganic perovskite (CsPbX 3 , X = Cl, Br, I) nanocrystals (NCs) with promising optical properties are recognized as a rising star among photoelectric materials, but their inevitable instabilities limit extensive application. Herein, a new one-step strategy for encapsulating CsPbX 3 NCs with porous zeolite via the hot injection method is explored. By altering the mole ratio of PbX 2 , the emission wavelength of CsPbX 3 @zeolite is found to be regularly modulated from blue-emission (CsPbCl 2 Br@zeolite, 436 nm) to red-emission (CsPbBrI 2 @zeolite, 648 nm), thus enabling full spectrum adjustment. Due to the surface passivation of zeolite to CsPbX 3 NCs, CsPbX 3 @zeolite possess an outstanding quantum yield and display excellent thermal/photo/air stability. Subsequently, white light-emitting diodes based on green-CsPbBr 3 @zeolite and red-CsPbBrI 2 @zeolite are constructed and applied to the backlit display, achieving a wide color gamut of 134.2% for NTSC 1953 and 99.8% for Rec. 2020. The CsPbX 3 @zeolite implanted with a polymethyl methacrylate film is used to realize upconversion emission under an 800 nm laser at room temperature. Furthermore, amplified spontaneous radiation based on CsPbBr 3 @zeolite films is achieved. These results convincingly indicate broad application prospects for CsPbX 3 @zeolite prepared via this simple method.

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ADVANCED FUNCTIONAL MATERIALS · 2023 ·Vol. 34 ·期 3 ·2308341 · IF 19

Trade-Off Between Efficiency and Stability of CsPbBr3 Perovskite Quantum Dot-Based Light-Emitting Diodes by Optimized Passivation Ligands for Br/Pb

Mingyang Li,Jindi Wang,Jisong Yao,Shalong Wang,Leimeng Xu,Jizhong Song

Although significant progress has been made in improving the external quantum efficiencies (EQEs) of perovskite quantum dot (QD) light-emitting diodes (QLEDs), understanding the degradation mechanism and enhancing stability remain a challenge. Herein,  increasing the content of Br-based passivation ligands is shown to enhance the EQE up to 16.1% by reducing the defects of CsPbBr 3 QDs in a Br-rich environment. However, the operational lifetimes of perovskite QLEDs gradually decrease with the increase of halide content, owing to the intensified ion migration under continuous electric field confirmed by the current behavior of QLEDs and time-of-flight secondary-ion mass spectrometry. Furthermore, a thorough analysis of the relationship between electricity and luminance of QLEDs suggests that a small amount of residue oleic acid ligands could weaken ion migration. Accordingly, a halide- and acid-hybrid (HAH) co-passivation strategy is proposed to optimize the content of Br- and acid-based ligands, and achieve a maximum EQE of 18.6% and an operational lifetime ( T 50 , extrapolated) of 213 h for CsPbBr 3 QLEDs. This approach for passivating QDs combines the high efficiency of Br-based ligands with the improved stability of acid-based ligands. The study elucidates the correlation between ligands and device performance, highlighting the significance of two or even multiple ligands for efficient and stable perovskite QLEDs.

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POLYMER · 2023 · IF 4.6

Cellulose-Br-initiated imidazolium cation and ether linkage regulation of all-solid-state polymer electrolyte for advanced lithium transfer and battery performance

Xinlin Zhu,Jiacheng Yi,Wenjie Wang,Siyu Qu,Qinghua Deng,Jingyu Wu,Yang Zhou,Wuwei Yan,Yong Yang

The all-solid-state polymer electrolyte (SPE) with superior electrochemical performance and stability is the most significant part for the development of high safety and reliable batteries . In this work, the ether linkage and imidazolium ionic liquid are incorporated into the modified macromolecular cellulose network via atom transfer radical polymerization for the construction of brush-like cellulose bromide-poly(ethylene glycol) methyl ether methacrylate@1-vinylimidazole ionic liquid (CB-PEGMA@IL) and cellulose bromide-1-vinylimidazole ionic liquid@poly(ethylene glycol) methyl ether methacrylate (CB-IL@PEGMA) composite polymers . The crystallinity of pristine CB is largely decreased on account of the synergistic effect of ionic liquids and ether linkage. In particular, CB-PEGMA@IL presents a lower crystallinity and superior electrochemical performances than that of the CB-IL@PEGMA. With a wide electrochemical stability window (5.3 V vs Li/Li + ), the CB-PEGMA@IL based SPE presents a high ionic conductivity (1.2 × 10 −4  S cm −1 ) and record Li + transference number (0.32). LiFePO 4 /Li battery assembled with CB-PEGMA@IL-SPE shows excellent cycling performance (beyond 150 cycles at 0.2 C) and good rate capacity. Moreover, the overpotential of CB-PEGMA@IL-SPE based symmetric battery can keep ∼0.03 V even after 200 h cycling (100 μA cm −2 ). The soft-packed battery based on CB-PEGMA@IL-SPE can withstand bending and present stable voltage output upon folding at various angles. This rigid-flexible hybrid SPE provides a unique candidate for the fabrication of wearable high-tech electronic devices.

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JOURNAL OF APPLIED POLYMER SCIENCE · 2017 ·Vol. 134 ·期 17 · IF 1.86

Improving the charged and antifouling properties of PVDF ultrafiltration membranes by blending with polymerized ionic liquid copolymer P(MMA-b-MEBIm-Br)

Chunhui Du,Xumin Ma,Jing Li,Chunjin Wu

This study describes the fabrication and properties of poly(vinylidene fluoride) (PVDF) filtration membranes modified by blending with ionic liquid block copolymer P(MMA- b -MEBIm-Br), which is synthesized via reversible addition-fragmentation chain transfer polymerization method. The attenuated total reflectance-Fourier transform infrared spectroscopy and X-ray photoelectron analyses reveal that the ionic liquid block copolymers are immobilized on PVDF membrane surface. The modified PVDF membrane exhibits excellent charged and antifouling properties because of the charged and hydrophilic properties of the copolymer. Scanning electron microscopy and atomic force microscopy also indicate the morphological characteristics of the membrane and demonstrate that the surface porous structure becomes denser after adding the copolymer. The data of filtration and the zeta potential of the membranes suggest that the charged properties of the ionic liquid block copolymers are mainly responsible for the improvement of the reversible fouling ratio and the decrease in the total fouling ratio of the membranes. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134 , 44751.

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Energy Storage Materials · 2024 · IF 18.9

Self-stratified aqueous biphasic Zn–I and Zn–Br batteries enabled by spontaneous phase separation and halogen extraction effects of ionic liquids

Kaiqiang Zhang,Yang Ge,Qianchuan Yu,Pengbo Zhang,Yuge Feng,Zuoxiu Tie,Jing Ma,Zhong Jin

Self-stratified liquid electrode batteries are considered as a viable solution for large-scale energy storage applications due to their high safety and low cost. However, achieving long-term operation stability with high efficiency of selective ion migration/separation in multiple liquid phases remains a challenge. Here, we report an aqueous biphasic system based on imidazolium ionic liquids (ILs) for constructing membrane-free self-stratified aqueous biphasic Zn–I and Zn–Br batteries. The limited intersolubility and density difference between the IL-dominated catholyte and the aqueous anolyte create a self-stratified liquid-liquid phase separation structure, promising a reliable battery construction. Molecular dynamics simulations identify the internal association of IL, which forms a 3D H–bond network with the C–H···O interaction being the primary contributor, along with a thermodynamic electron transfer of ≤0.03 e. Additionally, a unique π + –bond effect is found between the positively charged imidazole ring of cation and the anion of IL. The as-constructed self-stratified aqueous biphasic Zn–halogen batteries work stably without the necessity of air isolation and exhibit long-term cycling stability (with a capacity mentation of 81.0 % for Zn–I batteries and 76.8 % for Zn–Br batteries over 1000 cycles), high energy efficiencies (93.5 % for Zn–I batteries and 86.7 % for Zn–Br batteries), inherent fire resistance and good scalability, demonstrating great potential for large-scale energy storage applications.

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RSC Advances · 2023 ·Vol. 13 ·期 9 ·5993-6001 · IF 3.9

Scale-up synthesis of high-quality solid-state-processed CsCuX (X = Cl, Br, I) perovskite nanocrystal materials toward near-ultraviolet flexible electronic properties

Zhi Jiang,Hezhuang Liu,Jihua Zou,Yixuan Huang,Zhaoquan Xu,Denys Pustovyi,Svetlana Vitusevich

High-quality CsCu2X3 and Cs3Cu2X5 (X = Cl, Br, I) nanocrystals (NCs) exhibit excellent optoelectronic, physical, and chemical properties for detection of UV radiation due to large carrier mobility and lifetime, and heavy atoms. The nanocrystal materials can be prepared via a low-cost and simple solid-state synthesis. However, poor reproducibility and complex synthesis methods of obtaining perovskite NC thin films represent a drawback for the fabrication of the commercial photoelectric device. To address these issues, we develop highly stable CsCu2X3 and Cs3Cu2X5 NC materials using a facile solid-state reaction method for the scale-up production of halogen lead-free perovskites. We suggest a distinctive way to design a series of nanocrystalline perovskites using short-term synthesis and study the mechanism of perovskite formation using thermal solid-state synthesis. These all-inorganic and lead-free CsCu2X3 and Cs3Cu2X5 exhibit large photoluminescence quantum yields (PLQYs) up to 95.2%. Moreover, flexible paper photodetectors based on this series of lead-free perovskites show strong photoselectivity and bending stability at 254 nm, 365 nm, and 405 nm wavelengths. High-quality responses with a responsivity of 1.1 × 10−3 A W−1 and detectivity of 2.71 × 109 jones under UV illumination (10 μW cm−2) at a bias voltage of 5 mV are demonstrated. These results open prospects for designing photodetectors, LEDs, and other photosensitive devices.

研究领域: 材料科学 · 光电技术
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MICROCHEMICAL JOURNAL · 2026 · IF 5.1

A novel “ON–OFF–ON” fluorescent sensor based on N,Br-doped carbon dots for the rapid detection of tannic acid and erythromycin

Chenyan Lu,Dajie Zou,Ning Zhang,Huye Li,Yanyan Jia,Huan Wang

In this study, the hexane extract of Asters tataricus was used as the carbon source, and ethylenediamine and 4-bromophenylene diamine were selected as dopants to prepare nitrogen and bromine co-doped carbon dots (N,Br-CDs) by the hydrothermal synthesis method. The obtained fluorescent probe has a uniform particle size distribution, good water solubility and high stability, with a fluorescence quantum yield of 48.43%. Under 420 nm excitation conditions, N,Br-CDs exhibited the strongest fluorescence emission at 513 nm, indicating that the sensing system was in the “ON” state. Subsequently, TA was introduced as a quencher to induce static quenching of the N,Br-CDs system, significantly weakening the fluorescence intensity and switching the sensing system from “ON” to “OFF”. Finally, after EM was introduced into the N,Br-CDs/TA system, EM preferentially formed a complex with TA and weakened its quenching effect on the quantum dots, thereby achieving fluorescence recovery and returning the sensing system from the “OFF” state to the “ON” state. Based on the above mechanism, an “ON-OFF-ON” fluorescence sensing system with N,Br-CDs as the luminescent substrate was constructed for the sensitive detection of TA and EM. The results showed that the system exhibited good linear response to TA, with the linear ranges being 1.50–22.94 μM and 34.88–348.42 μM, respectively, and the limits of detection being 0.2168 μM and 2.1797 μM, respectively (LOD, S/N = 3). The linear range for EM was 1.93–377.08 μM, with a detection limit of 0.6693 μM. Furthermore, the sensor system was capable of quantitatively determining TA and EM in human serum, Huangshui River water, and milk matrices, demonstrating its potential for broad application in environmental monitoring and bioanalysis.

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Science China-Materials · 2020 ·Vol. 64 ·期 1 ·158-168 · IF 6.098

Facial synthesis of highly stable and bright CsPbX3 (X=Cl, Br, I) perovskite nanocrystals via an anion exchange at the water-oil interface

Fang Cong,Li Ye,Cai Yuting,Zhou Tian-Liang,Tang Xueyuan,Xie Rong-Jun

Cesium lead halide perovskite nanocrystals (NCs) have attracted unprecedented attention owing to their compelling properties for optoelectronic applications. Compared with the classical hot-injection method, the room-temperature (RT) synthetic strategy is more facile and tender, but it is hard to obtain stable CsPbI 3 NCs and it usually uses polar solvents that sometimes reduce the stability and properties of NCs. Here, we reported a simple approach to synthesize highly efficient and stable CsPbI 3 as well as other color-tunable CsPbX 3 NCs with high quantum efficiency at room temperature via an anion exchange at the water-oil interface, in which the as-synthesized pristine CsPbBr 3 NCs in toluene were treated in aqueous solutions of HX (X=Cl, Br, and I) and protonated oleylamine (OAm) acted as a carrier. The synthesized CsPbI 3 NCs had an emission at 680 nm and even showed excellent colloidal stability after being stored for 32 d. The high efficiency and stability of the obtained CsPbX 3 NCs were ascribed to the facts that: (i) the polar reagents were almost removed from the surface of NCs; (ii) the defect-related nonradiative recombination was suppressed efficiently by surface passivation.

研究领域: 纳米材料 · 光电子学 · 钙钛矿化学 · 胶体合成
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DALTON TRANSACTIONS · 2023 ·Vol. 52 ·期 23 ·7893-7905 · IF 4

Designed anion and cation co-doped Na3Sb(WM)xS4 (M = Cl, Br, I) sulfide electrolytes with an improved conductivity and stable interfacial qualities

Lingjun Shu,Jingxuan Yin,Zhemin Gon,Chengwei Gao,Yongxing Liu,Xiaolong Zhou,Hongli Ma,Xianghua Zhang,Xiang Shen,Shixun Dai,Changgui Lin,Qing Jiao

The fabrication of all electrolytes from noncombustible ceramic materials offers a superior option for providing safer and higher-capacity batteries to fulfill future energy needs. To achieve a competitive performance with combustible liquid electrolytes used in commercial Li-ion batteries, the creation of ceramic material compositions with a high electrical conductivity is necessary. Here, we report that co-doping with W and halogens results in a superconductivity of 13.78 mS cm−1 in a cubic-phase Na3SbS4 glass ceramic electrolyte. After undergoing high-temperature heat treatments, the W ions in the electrolyte can facilitate the replacement of S atoms with halogens, introducing many Na vacancies. The samples also had a high degree of cycling stability. An excellent glass ceramic electrolyte for Na ion batteries will be constructed for Na3SbW0.25Cl0.25S4.

研究领域: 材料科学 · 电化学 · 固态离子学 · 能源存储 · 无机非金属材料 · 电池技术
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CHEMISTRY OF MATERIALS · 2022 · IF 10.508

Multiple Anion Chemistry for Ionic Layer Thickness Tailoring in Bi2+2nO2+2nSenX2 (X = Cl, Br) van der Waals Semiconductors with Low Thermal Conductivities

Ruiwen Ji,Meng Lei,Cécile Genevois,Wenda Zhang,Xing Ming,Lunhua He,Mathieu Allix,Congling Yin,Xiaojun Kuang,Xianran Xing

Layered materials coupling a two-dimensional strong-bonding layered network with much weaker van der Waals (vdW) interaction between the layers are sought after for the development of nanoelectronics and energy conversion devices. It is important to elucidate the layer stacking rules in these vdW materials and control the thickness of the strong-bonding layers for tuning the nanosheet height during exfoliation and therefore tailor physical properties. Here, we show that the single Bi2O2Se ionic layer in the three-anion vdW semiconductor Bi4O4SeCl2 showing extremely low thermal conductivity can be expanded to higher-order layers forming a homologous series Bi2+2nO2+2nSenX2 (X = Cl, Br) with variable ionic layer thicknesses. Bi4O4SeX2 (n = 1) and Bi6O6Se2X2 (n = 2) were isolated as single-phase materials, while materials with larger layer thicknesses such as Bi8O8Se3Cl2 (n = 3) contain different defect-intergrowth structures at the crystallite scale. The anionic disorder of Se and X within the Bi2O2Se and Bi2O2X2 slabs is a critical factor in the stabilization of Bi2+2nO2+2nSenX2. The ∼50% Se substitution by X anions in the Bi2O2Se slab as related to the weak interlayer interaction can serve as a stabilization criterion of Bi2+2nO2+2nSenX2. All of these materials show similar optical indirect band gaps of ∼1.05 eV, originating from the electronic states in the Bi2O2Se slabs. Pellets prepared from these vdW materials possessed low bulk resistivities (100 Ω·cm) and exceptionally low and tunable thermal conductivities (0.66 W/mK and lower) parallel to the pressing axis of the pellets (heavier the halogen is, lower is the thermal conductivity). The results presented here provide important multiple anion chemistry for tailoring the ionic-bonding network into different thicknesses in the vdW layered structures and therefore their physical properties.

研究领域: 材料科学 · 化学
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CRYSTAL GROWTH & DESIGN · 2021 · IF 4.076

Synthesis and Characterization of New-Type Ionic Cocrystals with Cyanuric Acid and Alkali Halides: AX·(H3C3N3O3)2 (A = Rb, Cs; X = Cl, Br)

Jinhui Wang,Xinyuan Zhang,Fei Liang,Zhanggui Hu,Yicheng Wu

Recently, neutral cyanurate acid and negative (iso-)cyanurates (HxC3N3O3)(3–x)– (x = 0–2) with strong conjugated π-bonds have been proposed as a new possible type of structural motifs for exploring high-performance birefringent materials. Especially, ionic cocrystals (ICCs) with neutral H3C3N3O3 molecules have attracted much attention due to their extended ultraviolet transparent range and concurrently improved birefringence. Herein, three ICC single crystals, RbCl·(H3C3N3O3)2 (I), CsCl·(H3C3N3O3)2 (II), and RbBr·(H3C3N3O3)2 (III), combining cyanurate acid and alkali halides have been designed and synthesized in ethanol solution. They simultaneously exhibit wide band gaps more than 5.4 eV, large birefringence (Δnexp ≈ 0.096–0.115, Δncal ≈ 0.071–0.105 at 800 nm), and high thermal stability above 325 °C. In addition, theoretical calculations have also been performed to evaluate the relationship of the molecular arrangement and their anisotropic optical properties. This work suggests that cyanurate-based cocrystals could be a promising structural family for the discovery of ultraviolet birefringent crystals.

研究领域: 材料化学 · 光学材料 · 晶体工程 · 无机化学
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JOURNAL OF LUMINESCENCE · 2021 · IF 3.599

Stable and multicolor solid-state luminescence of Mn doped CsPb(Cl/Br)3 perovskite quantum dots and its application in light-emitting diodes

Kewei Ma,Yuhang Sheng,Guizhen Wang,Xiaowei Zhang,Yunsong Di,Cihui Liu,Liyan Yu,Lifeng Dong,Zhixing Gan

Mn 2+ doping has been developed to modulate the photoluminescence (PL) of CsPbCl 3 perovskite quantum dots (PQDs). However, the doped Mn 2+ may be expelled from the PQDs host with the long-term storing, resulting in inferior stability. Herein, CsPbCl 3 PQDs doped with different concentrations of Mn 2+ (Mn:CsPbCl 3 ) are prepared by a hot injection method. Our photostability tests reveal that when the doping concentration is <25%, or 40%–50%, the Mn 2+ doped PQDs are intrinsically stable. Anion exchange reactions are conducted between the stable CsPb 0.796 Mn 0.204 Cl 3 and CsPbBr 3 PQDs. Fluorescence color gamut of the resulting Mn:CsPb(Cl/Br) 3 PQDs almost covers the entire visible spectrum except for the deep red color. Benefiting from the intrinsic stability and wide color gamut, multicolor solid-state luminescence are acquired by incorporating the Mn:CsPb(Cl/Br) 3 PQDs in polymethyl methacrylate (PMMA) matrices, which are used as color converters for constructing light-emitting diodes (LEDs) with different colors.

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