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CHEMISTRY OF MATERIALS · 2018 · IF 9.89

Postsynthetic Surface Trap Removal of CsPbX3 (X = Cl, Br, or I) Quantum Dots via a ZnX2/Hexane Solution toward an Enhanced Luminescence Quantum Yield

Fei Li,Ying Liu,Hongliang Wang,Qian Zhan,Quanlin Liu,Zhiguo Xia

The control of surface properties of all inorganic cesium lead halide perovskite (CsPbX3; X = Cl, Br, or I) quantum dots (QDs) is essential to achieve excellent stability and high photoluminescence quantum yields (PLQYs). Herein, a facile method was performed to simultaneously enhance the stability and PLQYs of CsPbX3 QDs by a ZnX2/hexane solution post-treatment. We show that the halogen defect on the surface of CsPbX3 QDs can be treated in a controlled way, whereby the “black dots” that adhered on the surface as observed by transmission electron microscopy have be completely removed, resulting in enhanced stability and photoluminescence. The PLQYs of CsPbCl3, CsPbBr3, and CsPbI3 increased from 4, 58, and 63% to 86, 93, and 95%, respectively, and the origin of the “black dots” as well as their transformation mechanism has been demonstrated. As a result, the poly(dimethylsiloxane) composite films created by encapsulating stable and nearly defect-free green-emitting CsPbBr3, the red-emitting K2SiF6:Mn4+ phosphor, and a blue emission GaN chip were prepared and used to fabricate a remote-type white light-emitting diode device, which exhibits a high luminescence efficiency (≤98 lm/W) and a wide color gamut (∼130% of the National Television Standard Committee standard), suggesting the potential for liquid crystal display backlight application.

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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY · 2022 ·Vol. 97 ·期 10 ·2805-2814 · IF 3.709

A bifunctional carbon catalyst with ?Cl and ?SO3H groups for hydrolyzing furfural residue to levulinic acid

Shuaibin Zhang,Bochao Yan,Zhihui Chen,Suping Zhang

BACKGROUND Levulinic acid, an important platform compound, is extensively used in textiles, dyes, antifreeze, animal feed, solvents and food additives. However, the use of lignocellulosic biomass to produce levulinic acid is difficult because of poor accessibility to cellulose and low hydrolytic yield. Thus a viable hydrolysis strategy and a suitable catalyst must be developed. RESULTS In this study, a bifunctional solid acid catalyst (HTC-SO 3 H) containing both cellulose binding sites (  Cl,  COOH and  OH) and catalytic sites (  SO 3 H) was prepared by a carbonization–grafting–oxidization method. X-ray photoelectron spectroscopy and Fourier transform infrared characterization confirmed the existence of  Cl and the successful modification of the  SO 3 H grafted hydrothermal carbon. The hydrogen bonds formed between cellulose and the binding sites (  Cl,  OH and  COOH) in the catalyst showed synergistic effects with the catalytic sites (  SO 3 H), leading to efficient hydrolysis of the furfural residue. A total of 74.81% (non-magnetic) and 70.18% (magnetic) levulinic acid yields were obtained after hydrolysis at 190 °C and 180 min in γ-valerolactone–H 2 O (1:1, v/v). Magnetic catalysts were synthesized using a co-precipitation method. Catalysts were recycled without any obvious reduction in catalytic activity. CONCLUSION Using sucralose as a raw material, the as-synthesized bifunctional solid acid catalyst improved the accessibility to cellulose and increased levulinic acid yield. Moreover, the grafted SO 3 H formed by hydroxyl hydration condensation exhibited superior stability. This study provides a valuable strategy for the efficient hydrolysis of lignocellulosic biomass. © 2022 Society of Chemical Industry (SCI).

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Journal of Environmental Chemical Engineering · 2022 · IF 7.968

β-Cyclodextrin and graphene oxide co-strengthened AgRu bimetal mesoporous nanozyme: An efficient strategy for visual detection and removal of toxic Hg2+ and Cl−

Zhengquan Yan,Lin Xing,Lin Zhao,Xinyi Zhang,Yingfan Zhang,Yulian Tang,Xuemei Zhou,Lei Hu,Nianlei Zhu

In this work, to efficiently eliminate the threat of toxic Cl − and Hg 2+ , a kind of AgRu bimetal mesoporous nanozyme co-stabilized by β-cyclodextrin and graphene oxide (AgRu@β-CD-co-GO) was first developed by a homogeneous redox and assembly method. The mesoporous microstructure and a large number of hydroxyl groups and GO aryl rings endowed AgRu@ β-CD-co-GO with superior peroxidase-mimic performance and enough active spots to adsorb more toxic Cl − and Hg 2+ . Under optimal conditions (pH 4.0, 350 μL 1.5 mM TMB and 200 μL 1.0 M H 2 O 2 and incubated for 30 min at 25 °C), AgRu@ β-CD-co-GO could accelerate the oxidation of colorless 3,3′,5,5′-tetramethylbenzidine (TMB) into blue oxTMB in the presence of H 2 O 2 . Toxic Cl − or Hg 2+ would exclusively alter its peroxidase-like activity, accompanied with the characteristic UV–vis absorption intensity at 653 nm ( A 653 ) decreased and color changed from blue to colorless. AgRu@ β-CD-co-GO was successfully applied for visual detection of Cl − and Hg 2+ and enriched removal of them after their detection. The detection limits were low to be 3.2 × 10 −10 mol∙L −1 for Hg 2+ and 6.4 × 10 −8 mol/L for Cl − . After detection, more than 94.9% Hg 2+ and 93.8% Cl − could be removed by only a simple filtration. The mechanisms for peroxidase-mimic activity of AgRu@ β-CD-co-GO and its exclusive recognition of Hg 2+ and Cl − were proposed.

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INORGANIC CHEMISTRY · 2022 · IF 5.436

Suppression of Thermal Quenching for CsPbX3 (X = Cl, Br, and I) Quantum Dots via the Hollow Structure of SrTiO3 and Light-Emitting Diode Applications

Wenli Song,Bing Zhang,Wenli Zhou,Jilin Zhang,Liping Yu,Shixun Lian

All-inorganic perovskite quantum dots (PQDs, CsPbX3, X = Cl, Br, and I) show outstanding application prospects in the field of photoelectric devices. In recent years, the development of PQDs has greatly improved their stability to water, oxygen, and light. However, thermal quenching of PQDs greatly limits their practical application. Herein, we embed PQDs into ATiO3 (A = Ca, Ba, and Sr) of three different mesoporous spherical structures to explore the effect on thermal quenching of PQDs. Because of the unique mesoporous hollow microsphere structure and low thermal conductivity of SrTiO3, it can effectively block the heat transfer and improve the thermal quenching of PQDs. The photoluminescence (PL) intensity of CsPbBr3@SrTiO3 composites is 72.6% of the initial intensity after heating to 120 °C. Moreover, the PL intensity of CsPbBr3@SrTiO3 composites remains about 80% of the initial value even when stored in air for 20 days or irradiated by 365 nm UV light for 48 h. A neutral white light-emitting diode is assembled by a blue chip, CsPbBr3@SrTiO3 composites, and red phosphor of K2SiF6:Mn4+, which has a color temperature of 5389 K and a color gamut covered 133% of National Television Standards Committee (NTSC).

✓ 已验证 产品关联 DOI PubMed 高影响因子
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MICROCHIMICA ACTA · 2024 ·Vol. 192 ·期 1 ·1-11 · IF 5.3

Colorimetric sensor array for sensitive detection and identification of bacteria based on the etching of triangular silver nanoparticles regulated by Cl− at various concentrations

Liu Shuang,Yan Peng,Naveed Shahzad,Zhu Yuheng,Fu Tao,Wu Ruijing,Wu Yayan

A colorimetric sensor array is proposed for ultrasensitive detection and identification of bacteria by using Cl − at various concentrations as sensing elements and triangular silver nanoparticles (T-AgNPs) as a single sensing nanoprobe. T-AgNPs are easily etched by Cl − . However, in the presence of bacteria, the etching process will be hindered. Different bacteria have differential protective effects on T-AgNPs due to their interactions, resulting in different etching degrees of T-AgNPs by Cl − , and visual color changes. By adjusting the antagonistic action between bacteria protection on T-AgNPs and the etching by using Cl − at various concentrations, different bacteria had their own color response patterns. Combined with linear discriminant analysis (LDA) and orthogonal partial least squares-discriminant analysis (OPLS-DA), the bacteria could be identified. The method was also used for bacteria mixtures identification and showed high sensitivity (OD 600  = 1.0 × 10 −6 ) for V. parahaemolyticus detection. Finally, the sensor array was successfully utilized in the identification of bacteria in pure and mineral bottled water. The method is low-cost, simple, sensitive, visual, and has potential application in point-of-care testing of bacteria. Graphical

✓ 已验证 产品关联 DOI PubMed 高影响因子
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APPLIED GEOCHEMISTRY · 2017 · IF 2.581

The solubility of fluorite in Na-K-Cl solutions at temperatures up to 260 °C and ionic strengths up to 4 mol/kg H2O

Wei Zhang,Li Zhou,Hongfeng Tang,Heping Li,Wenlei Song,Gang Xie

The solubility of fluorite in hydrothermal conditions is important in ore forming and geothermal processes and groundwater utilization. However, a quantitative description of the geochemical behavior of fluorite under hydrothermal conditions has not been previously reported. In this work, the solubility of fluorite in Na-K-Cl solutions at temperatures up to 260 °C and ionic strengths up to 4 M was determined by experiments and modeling. The solubility products obtained in this work at 30 and 50 °C under ambient pressure and those from literature were used to regress the density model parameters for fluorite solubility product calculation at high temperature. The Pitzer interaction model was adopted to calculate the activity coefficient . The fluorite solubility determined in KCl solution at 250 °C under vapor saturated pressure and that from the literature were combined with the low-temperature thermodynamic properties of heat capacity and osmotic coefficient to obtain the binary parameters of NaF and KF at temperatures up to 260 °C. A thermodynamic model was then developed for calculating the fluorite solubility in Na-K-Cl solution at temperatures up to 260 °C, under vapor saturated pressure and ionic strengths up to 4 M. As calculated from this model, fluorite solubility measured at 200 °C and 0.1 M NaCl was well predicted. Both temperature and ionic strength had significant effects on fluorite solubility, and fluorite exhibited a similar dissolution pattern in both NaCl and KCl solution. When the concentration was lower than 2 M, the solubility of fluorite first increased with temperature, reached a maximum at approximately 100 °C, and then decreased. When the concentration was higher than 2 M, the solubility of fluorite increased monotonically with temperature.

✓ 已验证 产品关联 DOI 高影响因子
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WATER RESEARCH · 2024 · IF 11.4

Wane-and-wax mechanism of nitrogenous disinfection byproducts with constant Cl/N peak under UV/chlorine treatment: Implication for new drinking water disinfection strategy

Jinxiu Lou,Lu Yin,Feilong Dong,Zhanfei He,Huijie Lu,Shuangxi Fang,Xiangliang Pan

Nitrogenous disinfection byproducts (N-DBPs) are notorious for their serious health risks, yet nitrate (NO 3 - ) mediates N-DBPs generation during UV/chlorine treatment remains unexplored. This study investigated the interaction of chlorine and NO 3 - on N-DBPs formation and developed a specific fragment-based screening method using UPLC-QTOF-MS to explore the underlying mechanism. Results showed that the chlorine-to-nitrogen (Cl/NO 3 - -N) molar ratio significantly affects dichloroacetonitrile (DCAN) and dichloroacetamide (DCAM) generation, with peak concentrations at a Cl/NO 3 - -N molar ratio of around 15. NO 3 - promotes the production of HO • , which positively correlates with DCAN and DCAM concentrations, also peaking at this ratio. Utilizing our developed method, three key hydroxyl-substituted intermediates that circumvent the previously reported “limiting-steps” in DCAN formation were identified. This reaction proceeds via a stepwise mechanism involving hydroxylation and chlorine substitution to produce hydroxyl-phenylacetonitrile and hydroxyl-chlorine-phenylacetonitrile. The conversion rate of hydroxyl-chlorine-phenylacetonitrile to DCAN was 8.6 times higher at Cl/NO 3 - -N molar ratio of 15 compared to conditions without NO 3 - , attributed to the weakened bond strength of the side chain, as supported by density functional theory calculations. This study provides novel insights into the mechanistic pathways of DCAN and DCAM formation, critical for developing more effective drinking water disinfection technologies to control N-DBPs.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Journal of Physical Chemistry Letters · 2021 · IF 6.475

Synthesis and Optical Properties of Mn2+-Doped Amino Lead Halide Molecular Clusters Assisted by Chloride Ion

Li Liu,Keliang Pan,Ke Xu,Xitian Peng,Jin Z. Zhang

Mn2+-doped amino lead halide molecular clusters (MCs) are synthesized using amine (e.g., n-octylamine, or butylamine) as passivating ligand and MnX2 (X = Cl or Br) as the Mn2+ doping source at room temperature. Their optical properties are investigated with UV–visible absorption, photoluminescence (PL), and PL excitation spectroscopy. The Mn2+ precursor plays a vital role in the synthesis of Mn2+-doped MCs. MnCl2 seems to facilitate the incorporation of Mn. The MnCl2 doping causes electronic absorption blue shift and leads to a spin-forbidden 4T1 → 6A1 Mn d-electron emission. With the help of time-resolved PL, Fourier transform infrared, and electron paramagnetic resonance results, a model is proposed to explain the formation mechanism. We suggest that Mn2+ doping replaces Pb2+ is assisted by Cl– ions that replace Br– ions. This study demonstrates the possibility of doping MCs and has important implications in gaining new fundamental insight into the growth mechanisms of perovskite nanostructures.

研究领域: 材料科学 · 无机化学 · 光学光谱学 · 纳米技术 · 凝聚态物理
✓ 已验证 DOI 高影响因子
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JOURNAL OF HAZARDOUS MATERIALS · 2022 · IF 14.224

Lead-chlorine synergistic immobilization mechanism in municipal solid waste incineration fly ash (MSWIFA)-based magnesium potassium phosphate cement

Xing Cao,Qiushi Zhang,Weichen Yang,Lin Fang,Shiwei Liu,Rui Ma,Kai Guo,Ning Ma

The high chlorine (Cl) and lead (Pb) content characteristics of municipal solid waste incineration fly ash (MSWIFA) pose environmental risks and hinder resource utilization. Herein, an MSWIFA-based magnesium potassium phosphate cement (MKPC) preparation strategy was developed, which allowed the MSWIFA recycling and the Pb-Cl synergistic immobilization without the washing pretreatment . The compressive strength of the resulting 10 wt% MSWIFA-based MKPC was 28.44 MPa, with over 99.2% reduction in leaching toxicity of Pb and Cl. The high-angle annular dark field scanning transmission electron microscope (HAADF-STEM) and X-ray absorption spectroscopy (XAS) analyzes showed that Pb, phosphate and Cl - formed Pb 5 (PO 4 ) 3 Cl in MKPC. In-situ X-ray diffraction (XRD) tests showed that Pb 3 (PO 4 ) 2 was gradually transformed to Pb 5 (PO 4 ) 3 Cl through a dissolution-precipitation process. The formation energy, Bader charge, charge density difference and density of states (DOS) of Pb 5 (PO 4 ) 3 Cl were analyzed by first-principles calculations, confirming that Pb 5 (PO 4 ) 3 Cl was more thermodynamically stable than Pb 3 (PO 4 ) 2 and PbCl 2 and that electronic interactions between Pb-p, O-p, P-p and Cl-p orbits were the origin of Pb-Cl synergistic immobilization. This work provides a new strategy for the resource utilization of MSWIFA without washing pretreatment, and provides an in-depth understanding of the Pb-Cl synergistic immobilization mechanism.

研究领域: 环境科学 · 材料科学 · 化学工程
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Journal of Cleaner Production · 2022 · IF 11.072

Highly efficient photocatalytic nitrogen fixation on bio-inspired triphase interface with improved diffusion of nitrogen

Xiuyan Wang,Bingdi Wang,Shengyan Yin,Mingwei Xu,Lixue Yang,Hang Sun

Low solubility and slow diffusion of nitrogen (N 2 ) in water are significant impediments for enhancing the efficiency of fixation nitrogen into ammonia (NH 3 ). Herein, we have prepared bio-inspired hierarchical assembly of carbonized loofah sponge@BiOBr-OV/Au (CL@BiOBr-OV/Au) to improve diffusion of nitrogen by immobilization of hydrophilic BiOBr-OV/Au onto hydrophobic CL sponge. The hydrophobic CL sponge provides an optimized directional channel for N 2 diffuse to the triphase interface N 2 (gas)-H 2 O (liquid)-BiOBr-OV/Au (solid), which supplies generous N 2 for the photocatalytic reaction and replaces the slow diffusion of N 2 through the liquid phase . Continuous delivery of N 2 can effectively capture generated electrons , thereby preventing the recombination of generated electron-hole and promoting N 2 activation. The modification of AuNPs can broaden the photoresponse range of BiOBr-OV, increase oxygen vacancies concentration and enhance N 2 adsorption and activation. CL@BiOBr-OV/Au shows an impressive in nitrogen fixation performance with high selectivity and recyclability of 2.64 mmol·g cat −1 ·h −1 , that is 10.2 and 8.0 times compared to CL@BiOBr-OV and BiOBr-OV/Au, respectively. Our work affords a convenient method for the construction of bio-inspired triphase catalysts with a directional N 2 transport channel to enhance the efficiency of nitrogen fixation, which also holds great promise for the application in other reactions involving gas consumption.

研究领域: 材料科学 · 催化 · 环境科学 · 化学工程
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TALANTA · 2020 · IF 5.339

A novel red-emission phenothiazine fluorescent protein chromophore based on oxygen‒chlorine bond (O–Cl) formation for real-time detection of hypochlorous acid in cells

Xu Zhi,Ying Qian

Hypochlorous acid (HOCl/ClO − ), a reactive oxygen species (ROS), plays an indispensable role in the human immune system. In this article, a novel red-emission phenothiazine fluorescent protein chromophore RFP-Ptz was developed for the detection of HOCl in cells. In the presence of HOCl, the fluorescence signal 610 nm rose gradually and reached its plateau with 15-fold enhancement; the fluorescence quantum yield increased from 0.01 to 0.12. The electrophilic substitution of Cl + towards phenolic hydroxyl group made the probe exhibited a high selective fluorescence response with a limit of detection (LOD) of 6.76 × 10 −7  M over other analyte species and ROS. This recognition mechanism of oxygen‒chlorine bond (O–Cl) formation has confirmed by HRMS . Finally, the RFP-Ptz can be used to response HOCl with low cytotoxicity and good biocompatibility (MTT cytotoxicity assay > 89.5%). The biocompatible RFP-Ptz was successfully applied to the fluorescence imaging of HOCl-related in SGC-7901 cells.

研究领域: 生物化学 · 医学检测 · 分子生物学
✓ 已验证 DOI PubMed 高影响因子
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Research · 2022 · IF 11.036

Low Trap Density Para-F Substituted 2D PEA2PbX4 (X = Cl, Br, I) Single Crystals with Tunable Optoelectrical Properties and High Sensitive X-Ray Detector Performance

Jiayu Di,Haojin Li,Li Chen,Siyu Zhang,Yinhui Hu,Kai Sun,Bo Peng,Jie Su,Xue Zhao,Yuqi Fan,Zhenhua Lin,Yue Hao,Peng Gao,Kui Zhao,Jingjing Chang

Exploring halogen engineering is of great significance for reducing the density of defect states in crystals of organic-inorganic hybrid perovskites and hence improving the crystal quality. Herein, high-quality single crystals of PEA2PbX4 (X = Cl, Br, I) and their para-F (p-F) substitution analogs are prepared using the facile solution method to study the effects of both p-F substitution and halogen anion engineering. After p-F substitution, the triclinic PEA2PbX4 (X = Cl, Br) and cubic PEA2PbX4 (X = I) crystals unifies to monoclinic crystal structure for p-F-PEA2PbX4 (X = Cl, Br, I) crystals. The p-F substitution and halogen engineering, together with crystal structure variation, enable the tunability of optoelectrical properties. Experimentally, after the p-F substitution, the energy levels are lowered with increased Fermi levels, and the bandgaps of p-F-PEA2PbX4 (X = Cl, Br, I) are slightly reduced. Benefitting from the enhancement of the charge transfer and the reduced trap density by p-F substitution and halogen anion engineering, the average carrier lifetime of the p-F-PEA2PbX4 is obviously reduced. Compared with PEA2PbI4, the X-ray detector based on p-F-PEA2PbI4 perovskite single-crystal has a higher sensitivity of 119.79 μC Gyair-1·cm-2. Moreover, the X-ray detector based on p-F-PEA2PbI4 single crystals exhibits higher radiation stability under high-dose X-ray irradiation, implying long-term operando stability.

研究领域: 材料科学 · 光电材料 · 辐射探测
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