CHEMISTRY OF MATERIALS
·
2024
·
IF 7.2
Yan Guo,Bin-Wen Liu,Chao-Hong Xie,Wen-Fa Chen,Ming-Xin Li,Xiao-Ming Jiang,Guo-Cong Guo
Rare-earth infrared nonlinear optical (IR NLO) compounds have garnered significant attention due to their abundant electronic structures. However, their NLO efficiency has been relatively modest, attributed to the localization of valence electron shells in rare-earth metals. Traditional design strategies for IR NLO materials have predominantly focused on MQ4 (M = metal, Q = S or Se) tetrahedra, with limited exploration of MQ6 octahedra. We introduce a novel approach to enhance NLO effects by incorporating distorted mixed anionic octahedral M(S/X)6 groups. To illustrate this strategy, we undertake structure modification and optimization of IR NLO performance using the Y–Ga–Ge–S system as an example. The synthesis of a new rare-earth chalcogenide, Y6Ga2GeS14 (1), serves as a foundation. Further halogen atom substitution yields Y6Ga4.2S13.6Cl3.4 (2), Y6Ga2.83Ge2S16.75Cl (3), and Y6Ga2.83Ge2S16.5Br1.5 (4). All compounds demonstrate remarkable NLO performance, including moderate NLO coefficients (0.17–0.70 × AgGaS2), large laser-induced damage thresholds (LIDTs) (3.78–6.19 × AgGaS2), and a broader transmission range (0.5–14.9 μm). The incremental enhancement of NLO efficiency in compounds 1–4 can be attributed to symmetry breaking induced by halogen atom substitution and increased distortion of the octahedral M(S/X)6 motifs in their structures, validating the effectiveness of our strategy. Notably, this strategy concurrently increases the band gap and LIDT, overcoming the NLO–LIDT incompatibility, being strikingly different from other reported approaches. This work provides new insights into optimizing the NLO performance of rare-earth IR NLO compounds through the modulation of octahedral motifs.
研究领域:
材料科学
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光学
·
化学
·
物理学
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INORGANIC CHEMISTRY
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2024
·
IF 4.3
Mengmeng Zhu,Junbo Wang,Lei Hou,Yiwen Yuan,Lili Liu,Yaoqing Chu,Chunmei Huang
The design and syntheses of new birefringent crystals will be of great importance in commercial applications and materials science. A series of ultraviolet (UV) birefringent crystals, AX·(H2SeO3)n (A = K, Cs; X = Cl, Br; n = 1, 2), with large sizes up to 23 × 6 × 3 mm3, was successfully synthesized by simple aqueous solution method. These four compounds belong to three different space groups. Isomorphic KCl·(H2SeO3)2 and CsCl·(H2SeO3)2 crystallize in the P1¯ space group, while CsBr·(H2SeO3)2 and CsCl·H2SeO3 crystallize in the P21/m and P21/c space groups, respectively. They exhibit cocrystal structures composed of [2(H2SeO3)]∞ and [AX]∞ frameworks, ingeniously inheriting the large optical anisotropy of selenite and the wide band gap of alkali metal halide. And it proves that these compounds indeed possess large birefringence (0.1–0.17 at 532 nm) and short UV cutoff edges (227–239 nm), achieving a balance of optical properties. This research affords a simple and viable strategy for the design and syntheses of new UV birefringent crystals. Besides, it is also found that the n value and ionic size (A and X ions) have important influences on the crystal structures and optical properties of AX·(H2SeO3)n. And this will promote further understanding of the alkali metal halide selenite family.
研究领域:
材料科学
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晶体工程
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光学材料
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无机化学
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JOURNAL OF HAZARDOUS MATERIALS
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2023
·
IF 13.6
Shiwei Liu,Xing Cao,Weichen Yang,Runjie Liu,Lin Fang,Rui Ma,Juan Peng,Shuaifei Zheng,Fei Ji
Higher chlorine (Cl) content than lead (Pb) content in municipal solid waste incineration fly ash (MSWIFA) impeded the practical application of Pb 5 (PO 4 ) 3 Cl-derived magnesium potassium phosphate cement (MKPC) preparation strategy. Herein, Pb/Ca-rich lead slag (LS) was co-blended with MSWIFA to prepare MKPC for the synergistic treatment of both two solid wastes and the Pb-Cl solidification. The results showed that the resulting 15–15 (15 wt% MSWIFA and 15 wt% LS incorporation) sample achieved 25.44 MPa compressive strength , and Pb and Cl leaching toxicity was reduced by 99.18 % and 92.80 %, respectively. The X-ray diffraction (XRD) and transmission electron microscopy (TEM) analyses showed that Pb 2+ , Ca 2+ , phosphate and Cl - formed Pb x Ca 5−x (PO 4 ) 3 Cl in samples. The formation of Pb x Ca 5−x (PO 4 ) 3 Cl was also demonstrated by the high-angle annular dark field scanning transmission electron microscope (HAADF-STEM), while differences in the lattice characteristics of Pb x Ca 5−x (PO 4 ) 3 Cl and Pb 5 (PO 4 ) 3 Cl were found. In-situ XRD indicated that Ca 2+ accelerated the transformation of Pb 2+ to Pb 5 (PO 4 ) 3 Cl. After co-precipitating with Ca 2+ to form Pb x Ca 5−x (PO 4 ) 3 Cl, Pb 2+ continuously substituted Ca 2+ to eventually transform to Pb 5 (PO 4 ) 3 Cl. This work informs the synergistic treatment of MSWIFA and LS and offers new insights into the reaction mechanism between Pb 2+ , phosphate and Cl - under Ca 2+ induction.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Junhao Li,Dacheng Zhou,Ying Liu,Yan Chen,Jiayuan Chen,Yong Yang,Yuan Gao,Jianbei Qiu
All inorganic perovskite (CsPbX3, X = Cl, Br, I) quantum dot (QD) glass samples are considered the next generation of lighting materials for their excellent luminescence properties and stability, but crystallization conditions are difficult to control, which often leads to the inhomogeneous crystallinity of QDs. Here, we provided evidence that the presence of sodium fluoride induced self-crystallization of CsPbBr3 QDs during routine glass formation without the need for additional heat treatment. We showed that NaF simultaneously affected the network structure of glass and promoted the formation of CsPbBr3 QDs, that is, Na+ ions entered the glass network skeleton, partially interrupting the network structure, while the strong electronegativity of F– ions attracted Cs+ and Pb2+ ions into the gaps formed in the glass networks that had been loosened up by Na+ ions, which reduced the activation energy of crystallization processes. Our results showed that NaF-induced CsPbBr3 QDs glass had excellent thermal stability, high photoluminescence quantum efficiency (49%), and luminescent stability under high-power laser irradiation. Finally, this work also demonstrated the general applicability of this method in the making of a series of CsPbX3 (X = Cl, Br, I) QD glass samples by NaF-induced self-crystallization, which drastically expanded the color gamut to a range of full spectrum for luminescence and laser-driven projection displays. We believe that the work presented here represents a new direction for the research and development of full-color gamut inorganic perovskite quantum dot glass samples, which could have a significant impact on the future applications of laser-driven projection displays as well.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2021
·
IF 4.098
Yanxia Xiao,Wenjuan Dong,Huiping Wang,Yumin Hao,Zihan Wang,Shaomin Shuang,Chuan Dong,Xiaojuan Gong
A novel visual nanoprobe was developed for the sequential detection of morin and zinc ion (Zn 2+ ) based on Cl and N co-doped carbon quantum dots (ClNCQDs) via a fluorometric and colorimetric dual-readout mode. The yellow fluorescence ClNCQDs was synthesized by the one-step hydrothermal treatment of o -chlorobenzoic acid and p -phenylenediamine. The most distinctive property of the ClNCQDs is the large stokes shift (177 nm), which is significantly higher than other reported CQDs. The fluorescence of the ClNCQDs can be effectively quenched by morin based on the synergistic effect of IFE, electrostatic interaction, and dynamic quenching process, and recovered upon the addition of Zn 2+ due to strong interaction between morin and Zn 2+ . The nanoprobe exhibited favorable selectivity and sensitivity toward morin and Zn 2+ with detection limits of 0.09 µM and 0.17 µM, respectively. Simultaneously, the color of the ClNCQDs solution was changed (light-pink → faint-yellow → dark-yellow) along with the variation of the fluorescence signal of the ClNCQDs. This proposed nanoprobe was successfully applied for morin and Zn 2+ analyses in actual samples and live cells with high accuracy. The results of this study demonstrate the great application prospects of the ClNCQDs for morin and Zn 2+ detection in complex actual samples and biosystems.
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COMBUSTION AND FLAME
·
2021
·
IF 4.185
Tingting Zhou,Xiaodong Li,Chunjiao Liu,Xianrui Shi,Bo Wu,Xiaohui Duan,Guangcheng Yang
To meet the requirement of miniaturization and integration of the micro thrusters based on the chemical fuels, high-energy density compound is an emerging material as the chemical fuel. However, it is still challenging to realize the high-efficiency, stable and self-sustaining microcombustion of the high-energy density chemical fuels. Herein, we report the high-performance microcombustion of CWs/AP/CL-20 composite with nanoscale 2,4,6,8,10,12-(hexanitrohexaaza)cyclododecane (CL-20) and oxidizer ammonium perchlorate (AP) confined in a self-standing carbonized butterfly wing scales (CWs) matrix. CWs with multi-channeled hierarchical porous structure provide a model architecture for loading of AP and CL-20. CL-20 is designed to serve as heat/pressure loss compensate agent due to its high-energy density, fast energy release rate and large amounts of gas release during combustion process. The combustion of CWs/AP/CL-20 is greatly enhanced due to the enhanced heat and mass transfer originating from the multi-channeled hierarchical porous structure and synergistic reactions between components at nanoscales, which is demonstrated as promising solid-propellant for the micro thruster. It is found that the sample with oxygen balance close to zero, which can be conveniently regulated by adjusting the mass ratio of CL-20 and AP, has the best microcombustion performance, resulting in a specific impulse of 383.5 N·s/kg.
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CHEMICAL ENGINEERING COMMUNICATIONS
·
2016
·
IF 1.433
Lu Bai,Shu-Ni Li,Quan-Guo Zhai,Yu-Cheng Jiang,Man-Cheng Hu
In the present work, physicochemical properties, such as density (ρ), refractive index (nD) and viscosity (η), for six binary systems containing [Cnmim]Cl (Cnmim = 1-alkyl-3-methylimidazolium; n = 6, 8) and three dipolar aprotic solvents [N-methyl-2-pyrrolidinone, 1,3-dimethyl-2-imidazolidinone and 1,3-dimethyl-3,4,5,6-tetrahydro-2(1H)-pyrimidinone)] were measured at wide composition ranges and temperatures from T = 288.15 to 333.15 K at atmosphere pressure. Moreover, the derived properties, such as excess molar volumes (), apparent molar volumes (Vφ,i), deviations in refractive index (ΔnD), and isobaric thermal expansivity coefficients (αP), were calculated. The Redlich–Kister polynomial equation was fitted to the excess molar volumes and the deviation in refractive index data. The experimental results in this work allow us to discuss the interactions in the mixtures. The physicochemical properties of such systems may be useful for applications of imidazolium-based ionic liquids in the field of chemical engineering.
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JOURNAL OF ORGANIC CHEMISTRY
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2024
·
IF 3.3
Yangyi Zhang,Guisheng Deng
In the Au(PPh3)Cl/AgOTf/TsOH/MeCN/N2/25 °C system, diastereoselective synthesis of cis-3a,8a-dihydrofuro[2,3-b]benzofuran derivatives with a substituent at the 8a-position has been achieved by using 1-(2-hydroxyphenyl)-3-arylprop-2-yn-1-ols and β-oxoketones (amides, acid) as starting materials. The studies revealed that the acidity of methylene in substrates plays a key role in the differential reactions. A stronger acidity of the methylene is favorable in the desired conversion. The unique role of TsOH as an additive acid in the synthesis strategy has been rationalized. 2-Oxo-phosphonate, 2-oxo-sulfonate, and 3-oxobutanoate are suitable for the conversion.
研究领域:
有机化学
·
合成化学
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2020
·Vol. 22
·期 30
·17299-17305
·
IF 3.43
Chenyang Zhou,Ya Chu,Linlin Ma,Yingqian Zhong,Chao Wang,Yalan Liu,Haoyue Zhang,Beibei Wang,Xia Feng,Xi Yu,Xiaotao Zhang,Yan Sun,Xiaozeng Li,Guangjiu Zhao
In this work, we introduced halogen-substituted chiral molecules as A-site cations to synthesize a series of novel organic–inorganic hybrid two-dimensional (2D) chiral perovskite materials (R-X-p-mBZA)2PbBr4 (X = H, F, Cl, Br; p: para-position; mBZA = α-methylbenzylamine) for the first time. This halogen-substituted cation strategy collectively solved problems of narrow emission, weak chirality and low photoluminescence quantum yield (PLQY) for the emerged chiral perovskites. Photoluminescence (PL) spectra are significantly broadened due to the additional emission from self-trapped excitons (STEs) besides free excitons (FEs) states modulated by introducing significant disorder to the Pb–Br–Pb angle. The chirality of A-site chiral molecules is transferred and amplified to entire perovskite materials by fixing the chiral molecules at A-site via the interaction of halogen atoms. Furthermore, their PLQYs are improved with the reduction of energy gap and inhibition of the non-radiative transition from STEs to ground state. The halogen-substituted A-site cation strategy can be performed to develop organic–inorganic hybrid chiral perovskites with various optoelectronic applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2016
·
IF 8.328
Kexin Li,Zhenxing Zeng,Liushui Yan,Mingxin Huo,Yihang Guo,Shenglian Luo,Xubiao Luo
A series of nonmetallic elements co-doped titanium dioxide coated carbon nitride nanotubes (C/X-TiO 2 @C 3 N 4 NTs, X = N, F, Cl) was successfully prepared by a simple sol-gel-pyrolysis process using phenolic organic pollutants, titanium butoxide, and carbon nitride nanotubes as precursors. The morphology, porosity, phase and chemical structure, and optical and electronic property of as-prepared C/X-TiO 2 @C 3 N 4 NTs were well characterized. The as-prepared C/X-TiO 2 @C 3 N 4 NTs exhibited excellent visible-light photocatalytic activity in the conventional degradation and hydrogen evolution systems compared with traditional TiO 2 /g-C 3 N 4 heterojunction, which is attributed to their unique tubular nanostructure and nonmetallic elements co-doped TiO 2 component. Subsequently, the visible-light photocatalytic activity of C/X-TiO 2 @C 3 N 4 NTs was further studied in the simultaneous hydrogen evolution with organic pollutant degradation system on the basis of our previous work. The reaction mechanisms in different photocatalytic systems were further discussed in detail.
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JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Yanli Kong,Siyu Dai,Qingwu Chen,Yong Nie,Jiangya Ma
Slow transformation efficiency of Fe(III)/Fe(II) limits the generation of radicals in peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs), and these radicals was easy to be interfered by the presence of water constituents. In addition, in-situ coagulation during this oxidation process was neglected. This study proposed Fe(II)/PMS-Mn(VII) in the presence of chlorides ions (FPMC) process to reveal multiple promoting effects of Mn on redox cycle of Fe(III)/Fe(II) and different reactive mechanisms of Cl − on types of radicals generation pathways, and the in-situ coagulation enhanced mechanisms was investigated. Results showed that the dual functionality of oxidation and in-situ coagulation in FPMC process was significantly enhanced that carbamazepine (CBZ) could be efficiently and quickly removed. The reduction product Mn(III) of Mn(VII) could promote the redox cycle of Mn(II)/Mn(III) and Mn(III)/Mn(IV) that facilitated Fe(III)/Fe(II), sustaining the reactivity of the system. Cl − could significantly promote the cycling of Mn(Ⅲ)/Mn(Ⅳ) that indirectly affected the cycle of Fe(III)/Fe(II).
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yan Xiao,Lei Hu,Li Gao,Mengting Di,Xiaojun Sun,Jie Liu,Xiaoming Yan,Gaohong He
Neutral aqueous organic redox flow battery (NAORFB) has been considered as a promising energy-storage device in the stationary storage field. Yet the insufficient Cl − conductivity of anion exchange membrane (AEM) has become a crucial obstacle for neutral energy systems compared to their counterparts, such as H + and OH – in acidic and alkaline conditions, respectively. Here, by proper microstructure design in AEM, a membrane with high Cl − conductivity is constructed by coupling the hydrophobic fluorinated poly(arylene ether) backbone and hydrophilic piperazinium groups, which exhibits excellent Cl − conductivity up to 55.9 mS cm −1 at room temperature. Moreover, the developed piperazinium functional fluorinated poly(arylene ether) (QPFPAE) membrane exhibits excellent low swelling, low organic redox-active species permeability, and high chemical stability. The constructed NAORFB using QPFPAE membrane shows a remarkable energy efficiency (85.6% at 80 mA cm −2 ), which has outperformed the other best-performing membranes. In addition, the membrane demonstrates outstanding stability and state-of-the-art performance over 1000 charge–discharge cycles. This work provides a rational design strategy toward high anion-selective conductivity in the membrane for large-scale NAORFB development.
研究领域:
储能技术
·
材料科学
·
电化学
·
电池技术
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