WATER RESEARCH
·
2018
·
IF 7.051
Yinan Bu,Mingrui Song,Jiarui Han,Zhenxuan Zhang,Baiyang Chen,Xiangru Zhang,Mengting Yang
Adsorbable organic halogen (AOX) is a parameter conventionally used to indicate the sum of organic halogenated disinfection byproducts (DBPs), which are formed from the reactions of disinfectants with dissolved organic matter , bromide and iodide in water. To overcome the issues of the AOX analytical method, we proposed a new facile and green pretreatment method to enable the analysis of nonionic total organic halogen (NTOX) via the following three steps: 1) separation of NTOX and halides with electrodialysis , 2) conversion of NTOX with ultraviolet (UV) photolysis, and 3) analysis of halides with ion chromatography . To verify this proposal, we mainly evaluated the efficiency of vacuum ultraviolet (VUV) coupled with UV photolysis (VUV−UV) in converting NTOX into halides. Results showed that by applying VUV irradiation for 60 min and UV irradiation at pH 10–11 for another 30 min, over 85.5% of each halide from 20 representative small molecular weight DBPs (each at 100 μg-X/L level) was recovered. The purpose of UV photolysis under alkaline conditions was to reduce oxyhalides (such as bromate and iodate) formed in the VUV process back to halides. With the aid of electrospray ionization-triple quadrupole mass spectrometry, we captured the whole pictures of high molecular weight polar DBPs in a chlorinated drinking water before and after VUV−UV, through which averagely 96.4% of dehalogenation with the VUV−UV treatment was observed. An illustrative comparison of the conventional AOX method and the proposed NTOX method indicates that although the detected NTOX was lower (by 2.3–30.6%) than AOX, the results of the two methods were highly correlated (R 2 > 0.97). All these hence verified the photolysis as a mature yet novel tool for sample pretreatment in environmental analytical chemistry.
研究领域:
环境科学
·
分析化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2022
·Vol. 105
·期 7
·4763-4774
·
IF 4.186
Nanchuan Wang,Shibo Guo,Qiaochu Chen,Fengmei Gao,Weiyou Yang,Hui Fu,Jinju Zheng
The thermodynamically viable halogen vacancy defects in CsPbCl 3 perovskite nanocrystals (NCs) are considered the main factor in weakening their optical quality. However, their separate impact on the dopant emission in Mn 2+ -doped CsPbCl 3 perovskite NCs is still under exploration owing to the absence of comparable samples. Herein, a series of Mn 2+ -doped CsPbCl 3 samples were synthesized with different oleylamine-Cl (OAm-Cl) contents based on a halogen-hot-injection strategy. It is found that the Mn 2+ concentration of as-prepared samples fixed at 0.65%, and the Mn 2+ photoluminescence (PL) also exhibited an OAm-Cl content-independent lifetime of ∼ 1.78 ms, implying the efficient and identical luminescence of isolated Mn 2+ ion in all samples. In contrast, the excitonic and Mn 2+ PL intensities of the NCs are strong related to the amount of OAm-Cl, which are attributed to the coordination effect of the suppressed excitonic nonradiative recombination owing to the passivation of chloride vacancies and the enhanced energy transfer from the host exciton to Mn 2+ ions in the samples with sufficient OAm-Cl contents. The temperature-dependent of Mn 2+ PL disclosed an initial increase and was followed by a decrease with increasing temperature for the samples with relatively higher OAm-Cl contents, while it monotonously decreases for the sample with lower OAm-Cl content of 0.4 mL. The different PL intensity change trend results from the effective passivation of chloride vacancies by extra OAm-Cl. Above results present here will help clarify the underlying influence mechanism of halogen vacancy on the PL properties of Mn 2+ -doped perovskite NCs, which is essential for targeted modulation of their optical properties.
研究领域:
材料科学
·
光学
✓ 已验证
DOI
高影响因子
Small
·
2024
·Vol. 20
·期 37
·2403198
·
IF 13
Dongying Fu,Yue Zhang,Zhuo Chen,Lin Pan,Yueyue He,Junhua Luo
Hydrogen bonding as a multifunctional tool has always influenced the structure of hybrid perovskites. Compared with the research on hydrogen bonding, the study of halogen-halogen interactions on the structure and properties of hybrid perovskites is still in its early stages. Herein, a polar bilayered hybrid perovskite (IEA) 2 FAPb 2 I 7 (IEA + is 2-iodoethyl-1-ammonium, FA is formamidinium) with iodine-substituted spacer is successfully constructed by changing the configuration of interlayer cations and regulating non-covalent interactions at the organic–inorganic interface, which shows a shorter interlayer spacing and higher density ( ρ = 3.862 g cm −3 ). The generation of structure polarity in (IEA) 2 FAPb 2 I 7 is caused by the synergistic effect of hydrogen bonding and halogen-halogen interactions. Especially, as the length of the carbon chain in organic cations decreases, the I---I interaction in the system gradually strengthens, which may be the main reason for the symmetry-breaking. Polarity-induced bulk photovoltaics ( V oc = 1.0 V) and higher density endow the device based on (I-EA) 2 FAPb 2 I 7 exhibit a high sensitivity of 175.6 µC Gy −1 cm −2 and an ultralow detection limit of 60.4 nGy s −1 at 0 V bias under X-ray irradiation. The results present a facile approach for designing polar multifunctional hybrid perovskites, also providing useful assistance for future research on halogen-halogen interactions.
研究领域:
材料科学
·
光电子学
·
辐射探测
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产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Jingzhen Su,Yong Wang,Cong Li,Zhengming He,Kai Zhang,Mingqiang Ren,Qile Wang,Tianxing Chen,Jibran Ali Ghumro,Virender K. Sharma,Hyunook Kim,Yunshu Zhang
Natural seawater contains abundant halide ions that remain largely untapped, while peracetic acid often requires activation to enhance its oxidative properties. The interaction mechanisms between these components have not been thoroughly investigated. This study investigated the activation effect of high concentrations of Cl − and Br⁻ coexisting in seawater on PAA by adding PAA to seawater. Quenching experiments, along with Electron Paramagnetic Resonance (EPR) spectroscopy and UPLC-TQ-MS, were conducted to determine the reaction mechanism and degradation process of SMX. Seawater systems containing 35 ‰ salinity or Br − -PAA systems (0.5 mM Br − ) degraded 100 % SMX within 10 min or 12 min, respectively ( k obs =0.4873 min⁻ 1 or 0.3581 min⁻ 1 ). While the Cl − -PAA system, though slower, still degraded 97.7 % within 180 min (300 mM Cl − , k obs =0.0173 min⁻ 1 ). SMX degradation rates remained above 95 % across the pH range of 3–9, with optimal performance at pH= 3. However, the presence of HA inhibited SMX degradation efficiency by over 40 %. Results indicate that SMX degradation efficiency correlates positively with Cl⁻/Br⁻ content and PAA concentration. The superior removal efficiency stems from activated PAA not only generating HOCl and HOBr via oxygen atom transfer but also further producing 1 O 2 , which dominates the non-selective degradation process. This approach adapts to a wide pH range but is consumed by coexisting HA. The superiority of the Br − -PAA system over Cl − -PAA stems from the strong oxidizing power of HOBr. The oxidation pathways include halogenation, bond cleavage, and hydroxylation. ECOSAR predictions indicated that most transformation products exhibited higher toxicity than the parent SMX compound.
研究领域:
环境化学
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水处理技术
·
氧化过程
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污染物降解
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海洋环境工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Polymer Materials
·
2024
·
IF 4.4
Jiang Liu,Zhaoheng Zhu,Yukun Huang,Long Wang,Kai Jia
There is a critical need to develop cost-effective and efficient adsorption materials for the removal of technetium-99 (99Tc) from contaminated water sources. This research presents the synthesis of amino-modified cellulose microspheres (CM-APTS) through the addition of 3-amino-propyl triethoxysilane (APTS) to regenerated cellulose microspheres (CM), followed by a subsequent reaction with ethylene dibromide (EDB) to produce halogen-modified amino cellulose microspheres (CM-APTS-EDB). These are engineered for the effective absorption of ReO4–, serving as a chemical surrogate for TcO4–. By altering the amount of ethylene dibromide used, two variations of bromine-modified cellulose microspheres, CM-APTS-EDBs and CM-APTS-EDBe, are synthesized. Among these, CM-APTS-EDBe exhibits robust adsorption capabilities for ReO4– across a pH spectrum of 2.5–10, attaining a peak capacity of 281 mg·g–1, and demonstrates selective adsorption of ReO4– even in the presence of competing anions such as NO3–, Cl–, and SO42–. Characterization through X-ray photoelectron spectroscopy (XPS) and Fourier-transform infrared spectroscopy (FTIR) indicates that the adsorption mechanism predominantly involves interactions between ReO4– and N+, hydrogen bonding with amino hydrogen, and σ-hole-anion interactions between Re–O and C–Br. After eight adsorption–desorption cycles, CM-APTS-EDBe retains notable stability and reusability. Additionally, the material efficiently captures ReO4– from simulated Hanford Low Activity Waste (LAW) wastewater, achieving an adsorption efficiency of 77.26% at a solid–liquid ratio of 40 g·L–1. This investigation underlines the potential of halogenated regenerated cellulose microspheres in designing advanced adsorbents for the removal of radioactive pollutants like TcO4–/ReO4–, offering a strategy for environmental remediation efforts.
研究领域:
环境科学
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放射化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
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.
研究领域:
材料科学
·
化学
✓ 已验证
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Shengyan Jin,Lingdong Kong,Kejing Yang,Chao Wang,Lianghai Xia,Yuwen Wang,Jie Tan,Lin Wang
Free radicals and nitrogen-containing species produced by nitrate photolysis can affect various atmospheric chemical processes, and thereby the photochemical behavior of atmospheric nitrate aerosols has been attracting much attention. However, the photolysis mechanism of NH 4 NO 3 and its products under different atmospheric conditions remain unclear. In this study, the effects of relative humidity (RH), pH, NH 3 , ultraviolet (UV) light intensity and halogen ions (Cl − , Br − and I − ) on the photolysis of particulate NH 4 NO 3 have been investigated through a flow tube reactor. The results show that RH can significantly enhance the production of gaseous NO 2 from the photolysis of NH 4 NO 3 when RH is higher than its deliquescence RH, but almost no NO 2 is generated under dry conditions. Under high RH and UV light, the main product of NH 4 NO 3 photolysis is NO 2 , rather than NO and HONO, and another main species HNO 3 which mainly comes from the hydrolysis of product NO 2 in the gas path was detected. Almost no NO 2 and HNO 3 are produced under high RH without UV light or low RH with UV light, showing the combined effect of high RH and UV irradiation on the photolysis of NH 4 NO 3 . In addition, under high RH, the lower the pH and the stronger the light intensity, the higher the NO 2 production. Furthermore, surprising yields of NO and HONO are detected in the presence of halogen ions, especially in the presence of I − , indicating the important role of halogen ion in the nitrate photolysis. These results provide new insights into the photolysis of atmospheric nitrate aerosols, and may contribute to elucidating the formation and migration of atmospheric nitrate aerosols and the potential mechanisms of the occurrence and evolution of atmospheric pollution and ozone pollution.
研究领域:
大气化学
·
环境科学
✓ 已验证
DOI
高影响因子
ACS ES&T Engineering
·
2022
·
IF 0
Jiazhen Cao,Yao Chen,Hengjun Shang,Xiang Chen,Qianyu Qiao,Hexing Li,Zhenfeng Bian
Gold and palladium are the most widely used precious metal materials in the field of electronic devices and industrial catalysis. How to realize the green recycling of gold and palladium is important and challenging. In this work, we found that gold and palladium in wastes, such as electronic devices and industrial catalysts, can be completely dissolved and recycled by photocatalysis. Gold and palladium are oxidized to the ionic state in water, which does not involve strong acids, strong alkalis, toxic cyanides, or an organic medium. More interestingly, the dissolution of gold and palladium in different halogen aqueous solutions has special selectivity, which depends on the coordination stability constants between gold and palladium with halide ions. Therefore, gold and palladium can be selectively dissolved in iodine ion solution and bromine ion solution, respectively, then gold and palladium can be obtained by a one-step reduction. This work opens up a new direction for optimizing the photocatalytic dissolution technology and promoting the green recycling of precious metals.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
JOM
·
2021
·Vol. 74
·期 2
·622-633
·
IF 2.474
Liu Zhihong,Ye Fengchun,Chen Rui,Wang Hongjun,Xia Longgong
Halogen-containing organic components in waste electrical and electronic equipment have an obvious influence on the distribution behaviors of valuable metals during the smelting processes. However, the mechanism is still incomplete in the literature. The equilibration-quenching-(ICP+EPMA) experimental technique has been applied in studying the partitioning behaviors of Au, Ag, and Sn in the Cu-FeO x -SiO 2 -CaO-Al 2 O 3 smelting system in the presence of halogen elements (F, Cl, Br). The obtained results showed that: (1) 93% Au terminated into the alloy phase in CaF 2 adding experiments, and a maximum of 32% Au reported to the gas phase in CaCl 2 or CaBr 2 adding experiments; (2) 22–49% Ag entered the gas phase when adding CaF 2 into the system, and 3–34% Ag entered into the gas phase when adding CaCl 2 or CaBr 2 ; and (3) halogen elements influenced Sn dramatically, and portions of Sn in the gas phase and slag phase increased along with increasing temperature or halides dosage.
研究领域:
冶金学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Micromachines
·
2024
·Vol. 15
·期 9
·1150
·
IF 3
Xinqiang Ma,Shengying Fan,Wenwen Yang,Jiajie Wei,Xiaolei Wang,Jincheng Ni,Wei Cheng,Qinhe Zhang
Perovskite as an emerging semiconductor luminescent material has attracted widespread attention due to its simple preparation, high luminescence quantum yield, high color purity, tunable spectrum, and ability to cover the entire visible light band. However, due to the influence of water or other highly polar solvents, oxygen, temperature, and radiation, perovskite nanocrystals will aggregate or collapse in the lattice, eventually leading to luminescence quenching. This study starts from the postprocessing of perovskite, uses methyl methacrylate as the monomer and TPO as the photoinitiator, and encapsulates the perovskite powder prepared by the hot injection method through ultraviolet light initiation. A method is proposed to improve the luminescence and crystal structure stability of perovskite. By eliminating the influence of environmental factors on perovskite nanocrystals through the dense structure formed by organic polymers, the resistance of perovskite to strong polar solvents such as water will be greatly improved, and it has great potential in the protection of perovskite. Finally, by changing the proportion of halogen elements in the perovskite resin to change the color of the luminescent resin, a fluorescent coating emitting light in all visible light bands is prepared. Fluorescent coatings are widely used in life and industry fields such as plastics, sol, and paper.
研究领域:
材料科学
·
光学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Frontiers in Environmental Science
·
2024
·
IF 3.3
Zhao Yilong,Liu Chengwei,Tu Xiang,Huang Wenkai,Liu Yu,Fu Hongbo
Field observations have confirmed that halide ions are widely distributed among aerosols from the marine boundary layer and on the surfaces of ice and snow in polar regions. Consequently, the coexistence of halide ions may play a more significant role in nitrate photolysis than previously thought. In this study, we simultaneously measured HONO, NO2, and NO2− in situ to gain a deeper understanding of the coexisting system, including the photogenerated nitrogen products and the effects on nitrate photolysis rates due to enhanced aqueous nitrite and HONO transfer rates by halides. The presence of halides significantly increased the photogenerated nitrogen products across various molar ratios ([X–]/[NO3−]) at pH 3.5. By eliminating oxygen flux, the transformation of the primary photogenerated products was affected, resulting in higher concentrations of N(III) as both HONO and NO2−. Experiments involving OH scavengers indicated that the attack from·OH initiated by halides leads to side reactions that enhance nitrate photolysis. Both theoretical calculations and nitrate actinometry were used to determine the photolysis rate of nitrate solutions, which together indicated that the presence of halides enhances nitrate photolysis. A newly developed model was used to determine the HONO transfer rate, finding that the presence of halides ([X–]/[NO3−] = 0.2) enhanced the evaporation of N(III) in solution by factors of 0.68, 0.95, and 1.27 for Cl−, Br−, and I−, respectively. To our knowledge, this is the first determination of halide effects on the mass transfer of HONO. The enhanced nitrate photolysis rate can be attributed to the differential surface effects of halides and parallel reactions initiated via ·OH stemming from nitrate photolysis, with varying rates leading to different quantities of nitrogenous products. Additionally, simultaneous measurements of photoproducts in both gas and condensed phases are recommended to better constrain the rate constants of NO3− photolysis.
研究领域:
环境科学
·
大气化学
✓ 已验证
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Xiaoyan Ma,Kunming Wei,Hongwei Liu,Qi Zheng,Wenqing Cao,Liang Zhang,Liangjie Tang,Stefanos Giannakis,Jing Deng,Su Jiang,Daniel L. Gallagher,Andrea M. Dietrich
Haloacetic acids (HAAs) are prevalently occurred in drinking water after disinfection by chlorine or chloramine, classified as the non-volatile and thermally stable disinfection byproducts (DBPs). To minimize the existed HAAs, catalytical electrolysis based on effective cathode was employed. Dehalogenation of HAAs were improved by vitamin B12 (VB12) coating on the stainless steel (SS), iron, copper, and aluminum electrodes. The VB12/SS composite electrode proved to be the optimal for the synergistic effect of VB12 and metal substrate on the DCAA degradation. Target chloro-, bromo-, and iodo-HAAs were catalytically decomposed, and their dehalogenation efficiency and mechanistic pathway were compared. The results show that HAAs electrolytic dehalogenation rates were significantly related with both the degree of halogenation (tri > di > mono) and the halogen atomic weight (I > Br > Cl). Dehalogenation of HAAs follows a first-order kinetic model, and kinetic variations were well described by a linear model. The logarithm base 10 of the dehalogenation rate constant k was proportional to its HAA molecular weight: log 10 (k) =0.00237 MW -0.85. The intermediate dehalogenation products were identified as less-halogenated acetic acids, and the final were acetic acid and halide ions. No mineralization occurred according to carbon conservation analysis. ESR detection and quenching experiments confirmed that HAAs dehalogenation was mainly an indirect reduction mediated by atomic H*. The synergistic effect between atomic H* and VB12 occurred through the electron transfer. This comparative study of various HAAs dehalogenation provides a mechanism of dehalogenation and a predictive linear model for electrolysis of HAAs.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）