CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Hao Xiong,Hanyou Zhang,Baisheng Sa,Ping Li,Lingyan Lin,Aijun Yang,Jiansheng Li,Jinquan Hong,Linqin Jiang,Yu Qiu
All-inorganic halide perovskite nanocrystals (PNCs) have attracted extensive attention due to their potential for the next-generation displays. The ammonium and halide composition affect strongly the photoelectrical properties and the long-term stability of PNCs. In this work, we present a novel class of mixed all-inorganic (Cs,NH 4 )Pb(Br,X) 3 (X = Cl, Br, I) NCs prepared via cation/anion co-exchange reaction between CsPbBr 3 NCs and the mechanochemically reacted NH 4 Pb n X 2n+1 (X = Cl, Br, I, n = 1 or 2) powders. The cubic morphologies of (Cs,NH 4 )Pb(Br,X) 3 NCs with different halogen element combinations were successfully obtained. In the meanwhile, the extended emission ranges from deep-blue (453 nm) to warm-yellow (564 nm). Higher PLQY and higher stability against ambient air and UV light were achieved simultaneously by controlling the ion co-exchanging process. The photoluminescence quantum yield (PLQY) of (Cs,NH 4 )Pb(Br,X) 3 (X = Cl, Br, I) NCs were also significantly enhanced compared with that of pure CsPbBr 3 after ions exchanging (>85% versus 58%). In addition, the stability of (Cs,NH 4 )Pb(Br,X) 3 (X = Cl, Br, I) NC thin films under the UV-irradiation and in the ambient atmosphere were also dramatically improved. The cation/anion co-exchanging synthetic strategy developed in our research provides a new pathway to modulate and realize mixed-ion PNCs with high optoelectronic performance.
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Advanced Optical Materials
·
2019
·Vol. 7
·期 23
·1901082
·
IF 7.125
Daqin Chen,Su Zhou,Feifan Tian,Haitao Ke,Naizhong Jiang,Shujin Wang,Yongzhao Peng,Yue Liu
Recently, Mn 2+ -doped CsPb(Cl/Br) 3 perovskite nanocrystals (NCs), showing the advantages of dual-color emissions via exciton-to-dopant energy transfer and reduced usage of toxic Pb 2+ heavy metal ions by nontoxic Mn 2+ substitution, are widely explored. However, photoluminescence quantum yields (PLQYs) for Mn 2+ -doped CsPb(Cl/Br) 3 NCs still need to be further improved. Here, a halogen-hot-injection strategy is developed to prepare Mn:CsPb(Cl 0.6 Br 0.4 ) 3 NCs with the maximal PLQY of 65%. With this method, intense blue narrowband emission from excitonic recombination and orange broadband emission from Mn 2+ 4 T 1 → 6 A 1 transition can be simultaneously achieved. The competitive luminescence between perovskite NCs and Mn 2+ dopants is systematically investigated by controlling the injected halogen types and ratios. As a proof-of-concept experiment, the present Mn 2+ -doped CsPb(Cl/Br) 3 perovskite NCs with highly efficient dual-color emissions are demonstrated to be applicable as color converter in UV-excitable solid-state lighting.
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Nanomaterials
·
2019
·Vol. 9
·期 2
·172
·
IF 4.034
Xinyue Lao,Xiyu Li,Hans Ågren,Guanying Chen
Although all-inorganic CsPbX3(X = Cl, Br, I) perovskite quantum dots (PQDs) have evoked exciting new opportunities for optoelectronic applications due to their remarkable optical properties, their emission color tunability has not been investigated to any appreciable extent. In this work, double/triple CsPbX3perovskite quantum dots with precise ratios of Cl/Br or Br/I are synthesized and their luminescence (410–700 nm) is explored. A group of down-converted CsPbX3(X = Cl, Br, I) perovskite quantum dot light-emitting diode (LED) devices were constructed to demonstrate the potential use of such double/triple-halide CsPbX3perovskite quantum dots with full-spectrum luminescence. Based on density functional theory, we theoretically explored the properties of CsPbX3with double/triple anion atoms. The calculated band gaps provided strong support that the full-spectrum luminescence (410–700 nm) of double/triple CsPbX3can be realized with the change of the mixed-halide ratios, and hence that such PQDs are of potential use in optoelectronic devices.Keywords:perovskite quantum dots;light-emitting diode;density functional theory;band gap
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CHEMISTRY OF MATERIALS
·
2024
·
IF 7.2
Zhongyuan Li,Mengdi Xu,Wuqi Liu,Xuesong Wang,Ye Li,Xianju Zhou,Zhen Fang,Lixin Ning
Broadband near-infrared (NIR) luminescent materials hold the key to next-generation, smart, NIR light sources. The emerging halide perovskite materials are regarded as promising candidates for optoelectronics because of their superior optical properties and easy solution processability. However, it remains a major challenge to realize efficient and thermally stable broadband NIR luminescence in these materials. Herein, we report a novel strategy to achieve broadband NIR luminescence by utilizing the transitions from the lowest 1T2 level of Mo4+ to the components of its 3T1 ground state in the soft Cs2Zr(Cl,Br)6 lattice. The multiple transitions, each occurring within the (4d2) t22 crystal-field configuration and containing zero-phonon and vibronic contributions, superimpose on each other to generate the broadband NIR emission. The emission spectrum encompasses the long wavelength region from 800 to 1400 nm centered at 970 nm with a full width at half-maximum of 170 nm. More importantly, the title NIR phosphor shows an exceptional quantum efficiency (66.9%) and thermal stability (67%@150 °C). The as-fabricated NIR phosphor-converted light-emitting diode shows great potential as an NIR lighting source. This research opens a new horizon for realizing high-performance broadband NIR luminescence by exploiting multiple electronic transitions of activators in the soft lattice.
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SENSORS AND ACTUATORS B-CHEMICAL
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2016
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IF 4.758
Rui Liu,Peng Zhang,Huijie Li,Chunsun Zhang
Flow chemiluminescence (CL) is widely applied for detection of heavy metal ions in environment, but it is seldom used in economical, practical, or affordable settings because non- and minimally instrumented flow driving is difficult to achieve. Here, we first report a gravity and capillary force-driven flow CL (GCF-CL) lab-on-cloth device, toward development of low-cost, easy-to-use, portable, minimally-instrumented platform for determination of trivalent chromium [Cr(III)] in water, where a difference in height between two zones on cloth creates a fast flow of CL trigger solution. Wax screen-printing was used to fabricate ultra-low-cost cloth-based devices, and the light emitted from the Cr(III)-catalysed oxidation of luminol by H 2 O 2 was imaged using an inexpensive portable CCD camera. Under optical conditions, Cr(III) could be determined over the range of 0.01–100 mg/L, with a detection limit of 6.2 μg/L, an analysis time of less than 30 s per sample, and RSDs of 6.2%, 3.1% and 1.7% for 0.05, 0.5 and 5 mg/L Cr(III) (n = 5). The proposed GCF-CL lab-on-cloth was successfully applied for measuring Cr(III) in water samples, with recoveries of 100.67-111.70% and RSDs of 4.73–6.88%. Thus, the presented method should have the potential for portable field applications in environmental and public health fields.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2015
·
IF 3.091
Zhihui He,Minjia Meng,Li Yan,Weihua Zhu,Fengquan Sun,Yongsheng Yan,Yan Liu,Shijuan Liu
Highly selective cellulose acetate (CA) blend imprinted membranes for salicylic acid (SA) was prepared by using phase inversion technique with sulfonated polysulfone (SPS) as a functional polymer, polyethylene glycol-4000 (PEG 4000) and ionic liquid 1-butyl-3-methylimidazolium chloride ([BMIM]Cl) as the additives. The membranes were characterized by several techniques including SEM, Raman, contact angle, membrane flux, and SA adsorption–desorption techniques. The SEM micrographs showed that the cross-sectional morphology of CA membranes was affected by polymer blend composition and applications of additives. Compared with the pure CA membrane the CA/SPS(90/10) + [BMIM]Cl membranes showed low contact angle, high membrane flux, strong adsorption capacity and high permeation selectivity. The experimental data of adsorption kinetic for CA/SPS(90/10) + [BMIM]Cl were well fitted to the pseudo-second-order kinetic model using multiple regression analysis. The selectivity coefficients of CA/SPS(90/10) + [BMIM]Cl-MIM for SA in relation to competition analogs p -hydroxybenzoic acid ( p -HB) and phenol were 5.8549 and 5.9062, respectively, which suggested that CA/SPS(90/10) + [BMIM]Cl-MIM had high selectivity and binding affinity for the template SA. Overall results suggest that [BMIM]Cl can be considered as an effective additive for CA imprinted membranes in the treatment of SA-contained water.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Tongqing Wu,Zhihui Hu,Jiaqi Yang,Yan Jia,Zekun Dong,Yu Tang,Yan Zhang
Textile wastewater was typically characterized by high concentrations of chloride ions, with Acid Red 14 (AR14) representing a significant pollutant. Nevertheless, research into the degradation of AR14 by electrochemical advanced oxidation processes (EAOPs) had largely overlooked the influence of chloride ions. In this regard, the EC-Chlorine-MMO/Ti system was designed, and the degradation mechanism of AR14 was subjected to meticulous investigation. The adopted anode was composed of Ti/IrO 2 -Ta 2 O 5 (mixed metal oxide, MMO). It demonstrated superior efficiency in degrading AR14 within a sodium chloride (NaCl) electrolyte, registering an apparent kinetic constant rate approximately 16.76 times greater than that observed within a sodium perchlorate (NaClO 4 ) electrolyte. The optimal chloride ion concentration was identified as 0.04 mol/L. Besides, alkaline conditions were not conducive to the degradation of AR14. It was noteworthy that the electrochemical byproducts chlorite (ClO 2 − ), chlorate (ClO 3 − ), perchlorate (ClO 4 − ), and trihalomethane (THMs) were not produced in the solution treated by the EC-Chlorine-MMO/Ti system. Electron paramagnetic resonance (EPR) spectroscopy, probe, and quenching experiments identified that hydroxyl radicals ( • OH), superoxide radicals (O 2 •− ), and dichloride radicals/chlorine monoxide radicals (Cl 2 •− / ClO • ) were the major reactive species. Of these, • OH played a pivotal role in AR14 degradation. Additionally, the three principal degradation pathways of AR14 were deduced by LC-MS analysis, UV–vis spectra, density-functional theory (DFT) calculations, and excitation-emission matrix (EEM) fluorescence spectroscopy. Furthermore, the generation mechanism of reactive species and the proposed mechanism of AR14 degradation by the EC-Chlorine-MMO/Ti system were presented. The study made a significant contribution to the understanding of the electrochemical reactions occurring in textile wastewater and provided valuable insights into the rational control of electrolytic conditions for the treatment of saline wastewater.
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Journal of Energy Chemistry
·
2023
·
IF 13.1
Han Yan,Ruifeng Song,Ruonan Xu,Shulin Li,Qiaoquan Lin,Xinlin Yan,Zhenyu Wang,Chuang Yu,Long Zhang
The (electro)chemical stability and Li dendrite suppression capability of sulfide solid electrolytes (SEs) need further improvement for developing all-solid-state Li batteries (ASSLBs). Here, we report advanced halogen-rich argyrodites via I and Cl co-occupation on the crystal lattice. Notably, a proper I content forms a single phase, whereas an excessive I causes precipitation of two argyrodite phases like a superlattice structure. The resultant synergistic effect of the optimized composition allows to gain high ionic conductivities at room temperature and −20 °C, and enhances the (electro)chemical stability against Li and Li dendrite suppression capability. The Li|argyrodite interface is very sensitive to the ratio of I and Cl. A LiCl- and LiI-rich double-layer interface is observed from the cell using the SE with optimized composition, whereas too high I content forms only a single interface layer with a mixture of LiI and LiCl. This double-layer interface is found to effectively mitigate the Li/SE reaction. The proper designed argyrodite enables ASSLBs to achieve good electrochemical properties at a broad temperature range regardless of the electrode materials. This co-occupation strategy provides a novel exploration for advanced halogen-rich argyrodite system.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
·
IF 4.9
Jin Wang,Xu Guo,Qixiang Zhou,Yan Cai,Bing Lu,Yang Wang,Yong Yao
The functional photoelectric materials based on bismuth oxyhalides (BiOX, X = Cl, Br and I) have been widely used in the field of photo-electrochemistry (PEC) due to their excellent physical, chemical and optical properties. Herein, a series of BiOX nanoflowers conjugated water-soluble pillar[5]arenes functionalized Au (Au@WP5/BiOX) modified PEC sensor are constructed and investigated for the PEC detection of serotonin. Upon exploring the physical properties, such as size, visible light absorption capacity, band gap and impedance, of the three BiOX materials, it is discovered that BiOBr is more effective in detecting 5-HT due to its high redox ability, moderate band gap (∼2.03 eV), and low impedance. BiOBr can provide a high and stable starting photocurrent compared to the other two bismuth oxyhalides. When used in acidic or neutral environments, 5-HT with a positive charge can undergo electrostatic adsorption and host-guest complexation behavior with WP5, which has a negative charge. By using WP5, the recognition ability of the material to 5-HT molecules can be enhanced, and the adsorption of 5-HT molecules on Au@WP5/BiOBr can be accelerated. The local surface plasmon resonance effect (LSPR) of gold nanoparticles (Au NPs) can accelerate the electrochemical reaction rate and charge transfer rate, which ultimately leads to the amplification of the photocurrent signal. As a result, the 5-HT detection sensor based on Au@WP5/BiOBr has a wide detection range from 0.01 to 100 μM and a low detection limit of 3 nM (S/N = 3) compared to other sensors, including Au@WP5/BiOCl and Au@WP5/BiOI. The proposed PEC sensor also exhibits good stability and selectivity, making it a promising strategy for detecting biological small molecules using pillar[5]arene functionalized PEC active materials.
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Science China-Chemistry
·
2025
·
IF 9.7
Kang Kai,Wang Qiuxiang,Huang Hongpu,Zhuang Xinxin,Cai Junlin,Wang Tao,Wang Xue,Xie Zhaoxiong,Xie Shuifen
Despite utilization of state-of-the-art Cu-based catalysts, achieving high selectivity and stability in multicarbon (C 2+ ) compounds production through electrocatalytic CO 2 reduction reaction (CO 2 RR) remains a critical and challenging objective. Here we employ lattice chlorine-doped Cu 2 O nanocubes (Cl d -Cu 2 O NCs) with well-defined {100} facets as a model catalyst to demonstrate that halogen doping can serve as a versatile and effective strategy for modulating surface charge distribution, thereby enhancing asymmetric C–C coupling toward high-selectivity C 2+ products in CO 2 RR. Compared to Cl-free Cu 2 O NCs, Cl d -Cu 2 O NCs exhibit a greatly enhanced C 2+ Faraday efficiency, i.e., ∼85% at −1.1 V (versus the reversible hydrogen electrode). Additionally, the Cl d -Cu 2 O NCs demonstrate significantly enhanced long-term durability, attributed to better preservation of the cubic morphology and more stable Cu δ + states. In-situ electrochemical studies reveal that Cl d -Cu 2 O NCs facilitate the formation of the key asymmetric *COH and *OCCOH intermediates, ultimately leading to higher C 2+ products. Density functional theory (DFT) calculations confirm that the introduced Cl-dopants disrupt the charge balance of the Cu 2 O(100) surface, enriching the Cl-adjacent Cu atoms with more electrons compared to those near O atoms. This unbalanced charge distribution significantly reduces the free energy of the rate-determining step for asymmetric C–C coupling from the *CO to *OCCOH on Cl-doped Cu 2 O (100) surface, requiring only 1.04 eV, in contrast to 1.50 eV on pristine Cu 2 O(100) surface. This study provides valuable insights into the surface charge modulation of Cu 2 O catalysts via halogen doping for enhancing asymmetric C–C coupling and C 2+ production in CO 2 RR.
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RSC Advances
·
2023
·Vol. 13
·期 9
·5993-6001
·
IF 3.9
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.
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ACS Applied Materials & Interfaces
·
2017
·
IF 7.504
Daqin Chen,Gaoliang Fang,Xiao Chen
Tunability of emitting colors of perovskite quantum dots (PQDs) was generally realized via composition/size modulation. Due to their bandgap absorption and ionic crystal features, the mixing of multiple PQDs inevitably suffers from reabsorption and anion-exchange effects. Herein, we address these issues with high-content Mn2+-doped CsPbCl3 PQDs that can yield blue-excitable orange Mn2+ emission benefited from exciton-to-Mn energy transfer and Cl-to-Br anion exchange. Silica-coating was applied to improve air stability of PQDs, suppress the loss of Mn2+, and avoid anion-exchange between different PQDs. As a direct benefit of intense multicolor emissions from Mn2+-doped PQD@SiO2 solid phosphors, a prototype white light-emitting diode with excellent optical performance and superior light stability was constructed using green CsPbBr3@SiO2 and orange Mn: CsPb(Cl/Br)3@SiO2 composites as color converters, verifying their potential applications in the field of optoelectronics.
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