ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Mingming Wang,Yurui Fan,Qinyuan Hong,Wenjun Huang,Xing Han,Zan Qu,Naiqiang Yan,Haomiao Xu
Mercury emissions from acetylene hydrochlorination processes in polyvinyl chloride (PVC) production pose severe environmental risks yet remain poorly quantified due to methodological limitations in high-reactivity C2H2/HCl atmospheres. We reported an advanced operando mercury speciation platform named PVC-OHM, engineered through systematic optimization of the Ontario Hydro method (OHM), achieving simultaneous real-time detection of elemental mercury (Hg0) and divalent mercury (Hg2+) with unprecedented sensitivity (0.12 μg/m3) under industrially relevant conditions. Our mechanistic investigation reveals three dominant mercury escape pathways: (1) thermal desorption, wherein localized hotspots accelerate HgCl2 decomposition and elevate the saturated vapor pressure at carbon-mercury interface (from 0.9 to 20.3 atm), contributed to 80% of total Hg loss; (2) C2H2 driven reductive decomposition of HgCl2 catalyst at carbon–mercury interfaces, responsible for 65–78% of Hg0 emissions and (3) excess chlorine adsorption-induced desorption ([HgCl2/AC] Cl5, Eads > 0) accounting for >10% of Hg2+ emissions. Quantitative tracking demonstrates alarming mercury loss of per gram catalyst (5 wt % Hg) reached as 3.08 mg Hg0 and 9.01 mg Hg2+, directly linked to localized thermal gradients (ΔT = 250–300 °C) at reaction hotspots. This work establishes the first experimentally validated framework for mercury fate prediction in carbide-based PVC synthesis, providing actionable strategies for emission control through hotspot mitigation and coordination environment optimization.
研究领域:
环境化学
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化学工程
·
催化科学
·
污染控制
·
工业排放
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DOI
PubMed
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2016
·Vol. 18
·期 20
·14046-14054
·
IF 4.449
Qingxin Zeng,Tingting Yan,Kai Wang,Yinyan Gong,Yong Zhou,Yongli Huang,Chang Q. Sun,Bo Zou
In situ Raman spectroscopy revealed that transiting H2O/NaX (∼64) solutions into an ice VI phase and then into an ice VII phase at a temperature of 298 K requires excessive pressures with respect to pure water. The increase of the critical pressures varies with the solute type in the Hofmeister series order: X = I > Br > Cl > F ∼ 0. The results suggest that the solute hydration creates electric fields that lengthen and soften the O:H nonbond and meanwhile shorten and stiffen the H–O bond through O–O Coulomb repulsion. Compression, however, does the opposite to solute electrification upon the O:H–O bond relaxation. Therefore, compression of the aqueous solutions recovers the electrification-deformed O:H–O bond first and then proceeds to the phase transitions, which requires excessive energy for the same sequence of phase transitions. Ice exclusion of solute disperses the frequencies of characteristic phonons and the critical pressures with unlikely new bond formation.
研究领域:
物理化学
·
高压科学
·
材料科学
·
光谱学
·
水溶液物理
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DOI
高影响因子
Materials
·
2026
·Vol. 19
·期 8
·1641
·
IF 3.7
Lele Chen,Ruqing Chen,Yule Huang,Meiqing Liang,Yang Zhou,Danning Ma,Kai Guo
Bi2O2Se is an emerging oxyselenide semiconductor, noted for its promising thermoelectric properties and excellent chemical stability, and it is often regarded as an n-type counterpart to p-type BiCuSeO. However, its intrinsic thermoelectric figure of merit (zT) is severely limited by low electron concentration and high thermal conductivity. In this work, we employed Cl element as donator dopant to substantially enhance the carrier concentration. The room-temperature carrier concentration of Bi2O2Se0.98Cl0.02thereby reached 2.70 × 1020cm−3, representing an improvement of two orders of magnitude compared to that of pristine Bi2O2Se. Subsequently, multiple hot-pressing cycles were applied to the optimized composition Bi2O2Se0.98Cl0.02. The process induced significant grain refinement, and the resulting high density of grain boundaries effectively suppressed the lattice thermal conductivity, reducing it to 0.95 W·m−1·K−1at 823 K. Eventually, a maximumzTof 0.24 was achieved at 823 K for the three-time hot-pressed Bi2O2Se0.98Cl0.02sample, representing a 71% improvement compared with the pristine Bi2O2Se sample prepared by single hot-pressing (zT= 0.14 at 823 K). This work provides a new strategy for enhancing the thermoelectric performance of oxyselenide through the synergistic regulation of doping and microstructure.
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DOI
PubMed
高影响因子
Processes
·
2021
·Vol. 9
·期 4
·652
·
IF 2.847
Huanong Cheng,Na Li,Rui Zhang,Ning Wang,Yuanyuan Yang,Yun Teng,Wenting Jia,Shiqing Zheng
The solubility of hydrogen sulfide in different mole ratios of ferric chloride and 1-butyl-3-methylimidazolium chloride ionic liquid (rFeCl3/[bmim]Cl,r= 0.6, 0.8, 1.0, 1.2, 1.4) at temperatures of 303.15 to 348.15 K and pressures of 100 to 1000 kPa was determined. The total solubility increased with the increase of pressure and the decrease of temperature. The solubility data were fitted using the reaction equilibrium thermodynamic model (RETM). The mean relative error between the predicted value and the measured value was less than 4%. Henry’s coefficient and the equilibrium constant of chemical reaction at each temperature were calculated. Henry’s coefficient first decreased and then increased with the increase of mole ratio, and increased with the increase of temperature. The equilibrium constant of the chemical reaction followed the same law as Henry’s coefficient. The chemical solubility was related to both Henry’s coefficient and the chemical equilibrium constant. H2S had the highest chemical solubility in FeCl3/[bmim]Cl at a mole ratio of 0.6 and a temperature of 333.15 K. The chemical solubility increased with the increase of pressure.
研究领域:
化学工程
·
环境科学
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Xin Lei,Yu Lei,Shuangshuang Cheng,Xin Yang
N -nitrosamines are great concern in potable water reuse. This study investigated the reaction kinetics of chlorine radicals (Cl • and Cl 2 •− ) with N -nitrosamines. The second-order reaction rate constants of Cl • ( k Cl • ) and Cl 2 •− ( k Cl2 •− ) with eight N -nitrosamines at pH 7.0 varied in the range of (5.02 ± 0.41)–(57.1 ± 4.25) × 10 8 M −1 s −1 and (0.46 ± 0.04)–(10.6 ± 0.73) × 10 8 M −1 s −1 , respectively. The numbers of methylene groups (#−CH 2 −) showed a good positive correlation with k Cl • (R 2 = 0.71), but not with k Cl2 •− . The degradation of eight N -nitrosamines under UV/chlorine advanced oxidation process (AOP) slightly increased by 1–18% in contrast to UV irradiation alone, and Cl − in the AOPs cannot inhibit their removal. The results improved the understanding of the fate of N -nitrosamines in chlorine radical-involved AOPs.
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高影响因子
CHEMISTRY OF MATERIALS
·
2022
·
IF 10.508
Jie Xue,Ziyu Wang,Andrew Comstock,Zhiyu Wang,Herman H. Y. Sung,Ian D. Williams,Dali Sun,Junwei Liu,Haipeng Lu
Recent discoveries of novel physics in two-dimensional (2D) magnetic materials have sparked the search of new layered magnetic semiconductors. Compared to the traditional inorganic 2D van der Waals crystals, hybrid organic–inorganic metal–halide frameworks offer significantly enhanced chemical and structural versatility, where their optical, electronic, and magnetic properties can be readily modulated with both organic and inorganic components. Here, we reported a series of new Fe–Cl-based layered double perovskites LnMIMIIICl8, [n = 4, L = phenylethylammonium or chiral R-(+)-β-methylphenethylammonium and n = 2, L = 1,4-butanediammonium; MI = Ag/Na; MIII = Fe/In]. UV–vis measurements show that their optical band gaps are highly tunable by varying the organic cations, MI ion, and MIII ion. Magnetic susceptibility measurements suggest an antiferromagnetic coupling between the nearest FeIII–FeIII, where the Curie–Weiss temperature, Néel temperature, and frustration factors can be easily modulated with their compositions and dimensionality. Our study demonstrates the rich and interesting magnetic properties in these layered transition-metal–halide double perovskites and paves the way for design of multifunctional magnetic materials.
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高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2022
·Vol. 28
·期 25
·e202104463
·
IF 5.02
Yue Liu,Yuxiang Wang,Haoran Cheng,Zheng Ma,Qian Li,Gang Wang,Daocheng Pan,Limin Wang,Jun Ming
Graphical A new soluble CsPbX 3 precursor to in-situ prepare luminescent CsPbX 3 nanocrystal film in the air readily was designed. The composition of the CsPbX 3 NCs films can be tuned by changing the solution precursors, allowing obtaining a high color purity and a narrow emission width. Inorganic cesium lead halide perovskite nanocrystals are candidates for lighting and display materials due to their outstanding optoelectronic properties. However, the dissolution issue of perovskite nanocrystals in polar solvents remains a challenge for practical applications. Herein, we present a newly designed one-step spin-coating strategy to prepare a novel multicolor-tunable CsPbX 3 (X=Cl, Br, I) nanocrystal film, where the CsPbX 3 precursor solution was formed by dissolving PbO, Cs 2 CO 3 , and CH 3 NH 3 X into the ionic liquid n-butylammonium butyrate. The as-designed CsPbX 3 nanocrystal films show high color purity with a narrow emission width. Also, the blue CsPb(Cl/Br) 3 film demonstrates an absolute photoluminescence quantum yields (PLQY) of 15.6 %, which is higher than 11.7 % of green CsPbBr 3 and 8.3 % of red CsPb(Br/I) 3 film. This study develops an effective approach to preparing CsPbX 3 nanocrystal thin films, opening a new avenue to design perovskite nanocrystals-based devices for lighting and display applications.
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DOI
PubMed
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2013
·
IF 2.04
Lingyun Dong,Shilie Pan,Hongping Wu,Xin Su,Hongwei Yu,Ying Wang,Zhaohui Chen,Zhenjun Huang,Zhihua Yang
A series of lead-containing halogen oxyborates, Pb 6 B 3 O 10 X ( X =F, Cl, Br), have been grown by high-temperature solution method and their crystal structures were determined by single-crystal X-ray diffraction. They are isostructural and crystallize in the space group Pbcm of the orthorhombic crystal system . The crystal structures are dominated by one-dimensional ∞ [(Pb 4 O)(BO 3 ) 3 ] “ Zig-Zag ”-chains, while the remaining Pb atoms and X ( X =F, Cl, Br) atoms are filled to balance the charge. Compared with the previously reported compound Pb 4 O(BO 3 ) 2 (the molecular formula Pb 4 O(BO 3 ) 2 can be regarded as Pb 6 B 3 O 10.5 ) with the space group Aba 2, the structures of Pb 6 B 3 O 10 X ( X =F, Cl, Br) are completely different from that of Pb 4 O(BO 3 ) 2 . IR spectroscopy , UV–vis-NIR diffuse reflectance spectroscopy , thermal analysis, and theoretical calculations were also performed on the reported materials.
研究领域:
材料科学
·
晶体学
·
光学
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DOI
高影响因子
NANOTECHNOLOGY
·
2020
·Vol. 31
·期 21
·215605
·
IF 3.551
Yu-Wei Liu,Shao-Hong Guo,Si-Qi You,Chun-Yi Sun,Xin-Long Wang,Liang Zhao,Zhong-Min Su
Halide perovskites have been employed as photocatalysts for CO2 photoreduction due to their excellent optical properties and unique electronic structure. However, their photocatalytic performance is relatively poor. Herein, we demonstrate a new strategy with Mn-doped CsPb(Br/Cl)3 mixed-halide perovskites as catalysts to enhance the efficiency of CO2 photoreduction. By tuning the content of Mn, a series of CsPb(Br/Cl)3:Mn perovskites are obtained and show high efficiency in CO2 conversion to CO and CH4. For the optimum catalyst sample, especially, the yields of CO and CH4 reach 1917 μmol g−1 and 82 μmol g−1 which are 14.2 and 1.4 times higher than those of CsPbBr3. This work provides new insights into improving the reactivity of perovskites in CO2 photoreduction.
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高影响因子
ACS Omega
·
2024
·
IF 3.7
Jianwu Lu,Yinfei Shi,Xiaoxia Ye,Shun Yuan,Xiaolong Yang,Xun Sun,Taizhi Wu
The primary limitations of the quantitative analysis of thermally labile halogenated compounds by traditional gas chromatography (GC) are the inadequacy of identifying the insufficiently volatile impurity (often with a high boiling point) and the difficulty in obtaining a standard substance with a reliable standardized assay. Taking the 4-(Chloromethyl)-5-methyl-1,3-dioxol-2-one (DMDO-Cl, 1) as an example, we reported a triphenylmethanamino-derivatization method to overcome the challenges of the assay determination of such species. During the quantification of 1, the presence of GC-undetectable polymeric impurity 10 poses a critical challenge in assessing the material quality. Moreover, the standard substance of 1 is not available on the market due to its inherent instability during storage and handling, further complicating the quantitative analysis. In this work, a precolumn HPLC-UV derivatization method based on triphenylmethanamino-alkylation was developed to quantitatively analyze 1. The resulting derivative 2 exhibits excellent crystallinity and superior physical and chemical stability and possesses effective chromophores for UV detection. The conversion from analyte 1 to derivative 2 demonstrates desirable reactivity and purity, facilitating quantitative analysis using the external standard method. The chemical derivatization-chromatographic detection method was optimized and validated, demonstrating its high specificity, good linearity, precision, accuracy, and stability. This method offers a valuable alternative to the general quantitative NMR (qNMR) detection technique, which exhibits reduced specificity in the presence of increased levels of impurities in compound 1.
研究领域:
分析化学
·
药物分析
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DOI
PubMed
高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2011
·Vol. 399
·期 7
·2503-2509
·
IF 3.841
Chen Yang,Zhang Yanqin
Functionalization of the surfaces of silica particles is often the first step in their various applications. An improved heterogeneous Fmoc-Cl fluorescent assay using an aqueous solution was developed to detect the number of amino groups on solid-phase supports. The fluorescent Fmoc-Cl method is 50-fold more sensitive than the current UV assay using an organic solvent. This method, together with the homogeneous fluorescamine and OPA assays, is used to detect amino groups on the silica particle surface. The accuracy and effect factors of these methods were examined and the assays were optimized. The results showed that the amine groups on silica particles can produce stronger fluorescence than small amine molecules in solution, because the porous structure of the particle surface is a more hydrophobic environment. The number of active amino groups that can be conjugated with biomolecules is much less than the total number of amino groups on the silica particle. Compared with physical methods, chemical assays involving direct reaction with amino groups would furnish the closest result to the number of active amino groups on the particle surface.
Fluorescence emission of Fmoc-Cl in aqueous solution and linear correlation between intensity and concentration
研究领域:
纳米材料
·
分析化学
·
生物材料
·
表面科学
·
分子探针
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Min Deng,Jing Wei,Zikang Qin,Zheng Yan,Junfeng Zheng,Lin Yang,Lu Yao,Wenju Jiang,Zhongde Dai
Styrene-butadiene-styrene triblock copolymer (SBS) has attracted increasing research attention due to its low cost, excellent mechanical properties, and superior gas permeability performance. In this work, a series of novel SBS doped membranes were prepared by introducing polyphosphoric acid (PPA), lithium 2,2,2- trifluoroacetate (TFALi), and 1,3-dichloro-1,1,3,3-tetraisopropyldisiloxane (Siloxane-Cl) into SBS as dopants. The results indicated that the addition of dopants into SBS membranes simultaneously enhanced the CO 2 permeability and CO 2 /N 2 selectivity of SBS membranes. Specially, doping Siloxane-Cl expanded the d-spacing, introduced flexible siloxane (Si-O) groups to enlarge molecular spaces, and formed more crosslinked network structure. Therefore, the SBS/Siloxane-20 membrane showed an approximately 4-fold increase CO 2 permeability compared to the pristine SBS membranes (from 203.3 to 842.9 barrer), accompanied by an increase in CO 2 /N 2 selectivity from 15.8 to 22.0. The obtained membranes also exhibited attractive anti-plasticization and anti-physical aging properties, no obvious decline in CO 2 permeability and/or CO 2 /N 2 selectivity can be observed after 1-week continuous permeation test, making them promising candidates for CO 2 /N 2 separation.
研究领域:
材料科学
·
环境工程
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DOI
高影响因子
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