Advanced Optical Materials
·
2019
·Vol. 7
·期 23
·1901082
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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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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2019
·
IF 2.298
Zhongshu Li,Yuli Xue,Xiaoling Tan,Wenqing Li,Shaonan Xu,Ziyan Wang,Jian Wang,Lina Li,Shiding Miao
It is of great importance to separate potassium salts from carbonate-based lakes, especially the low-[K+] but high-[Na+] brine which has been discovered around the world. Here the phase diagram of the quaternary system Na+, K+//Cl–, CO32––H2O was experimentally studied at 298.15 K via the method of isothermal evaporation, and the results corrected the previous diagram reported by Blasdale (J. Am. Chem. Soc.1923, 45, 2935–2946). The type of salts appeared and their solubility during the evaporation, and the density vs composition diagram and the pH values were plotted based on the experimental data. It was found that there were six invariant points, seven univariant curves, and five crystallization fields in the equilibrium phase diagram. To extract single-salt of potassium, certain areas in the Na+, K+//Cl–, CO32––H2O diagram were chosen to be acidified by the compressed CO2, and potassium in the form of KHCO3 was precipitated from the mother solution. The compressed CO2 was able to avoid formation of NaKCO3·6H2O during evaporation of the original system Na+, K+//Cl–, CO32––H2O. Based on experiment data, the region area for potassium salt extraction was determined, and this area was suitable for extracting K+ salts from brines with a [Na+/K+] ratio even lower than 0.44. This strategy opened a new way to recovery of potassium with a maximum yield of 59.88% from the carbonate-chloride-based brine.
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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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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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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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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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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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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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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Xiaodong Chen,Jing Liao,Ke Yin,Lu Cheng,Zhewen Yang,Zewei Liu,Bichun Huang
Carbon materials derived from single biomass feedstock typically have serious defects such as low porosity and poor distribution of functional groups. In this work, a series of porous carbons with different mass ratios of porphyra and corn stalk (7:3, 1:1, and 3:7) were prepared by ingeniously utilizing co-pyrolysis coupled with KOH activation. The prepared porous carbon samples were characterized by N 2 adsorption/desorption isotherms, Field emission scanning electron microscopy, Transmission electron microscopy, X-ray diffraction, Raman spectroscopy, Elemental analysis, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and Thermo-gravimetric analysis. Results showed that the prepared CPPC73 possessed excellent adsorbent properties, including high specific surface area (2719 m 2 /g), large pore volume (1.225 cm 3 /g), hierarchical porous structure, and optimal distribution of N-containing functional groups. Chlorobenzene (CB) dynamic adsorption experiments indicated that CPPC73 had higher adsorption performance (1134 mg/g) than unmodified POPC (795 mg/g). A combination of density functional theory (DFT) calculations, correlation analysis, and Grand canonical Monte Carlo (GCMC) calculations was performed to clarify the CB adsorption mechanism. Correlation analysis and GCMC calculations confirmed that pores in the range of 0.7–2.0 nm were the best adsorption sites for CB. Furthermore, DFT calculations indicated that N/O-containing functional groups on the carbon surface enhanced the interaction between porous carbon and CB, especially the pyrrolic-N. This work offers a new strategy to convert waste seaweed into a high-performance adsorbent for Cl-VOCs removal.
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CHEMISTRY OF MATERIALS
·
2022
·
IF 10.508
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.
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