LANGMUIR
·
2025
·
IF 3.9
Meiting Li,Bingxin Yuan,Chi Zhang,Jia Li,Xuejiao Wang
Hierarchical BiOCl/BiOI and BiO(Cl,I) photocatalysts were obtained via a solution-phase reaction for visible-light-driven elimination of aqueous pollutants, where the phase/morphology evolution, relationship between energy band/microstructure structure and photocatalytic properties, and photoreaction mechanism can be deciphered in detail. It was well-documented that the R = 8:1 BiOCl/BiOI heterojunctions with a coherent interface of Bi and O atoms showed a relatively strong redox capacity owing to their rapid Z-scheme charge transfer and large interfacial contact and eventually degraded ∼92.52% and 96.57% of rhodamine B (RhB) and tetracycline (TC) molecules under 10 min of visible light irradiation, which was larger than those of bare BiOCl and BiOI. However, their poor photocatalytic stability was proved to be unfavorable to practical applications. The best BiOCl0.88I0.12 solid solutions separately elucidated the optimal RhB and TC removal efficiency of ∼99.97% and 97.54% after 10 and 6 min of illumination, and it still maintained a high photodegradation efficiency toward RhB after five consecutive runs. The exceptional photocatalytic performance is cogoverned by the characteristics of in situ generated oxygen vacancies and defect energy levels.
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Journal of Physical Chemistry Letters
·
2021
·
IF 6.475
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
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
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
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
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催化
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环境科学
·
化学工程
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2026
·
IF 10.6
Lan Shi,Tianrui Gao,Zhipeng Zhu,Fan Yang,Bing Han,Jia Lv,Lin Tao,Yang Gao,Rong Hua,Huan Wu,Yichao Huang,Xiaojin He
Our recent large-scale population study demonstrated that several per- and polyfluoroalkyl substances (PFAS) are potential risk factors for sperm quality—with perfluorohexane sulfonate (PFHxS) and 6:2 chlorinated polyfluorinated ether sulfonate (6:2 Cl-PFESA) emerging as the strongest effect contributors to asthenospermia, yet their causal relationships remain unclear. Here, we provide in vivo experimental evidence and evaluation of the combined effects of 6:2 Cl-PFESA and PFHxS under human-relevant exposure. Male ICR mice were orally exposed to each compound alone or in combination for 35 days, covering one full spermatogenic cycle. Both single and combined exposures were associated with alterations of the male reproductive axis, including reduced serum testosterone and elevations in the gonadotropins luteinising hormone (LH) and follicle-stimulating hormone (FSH), and in sex hormone-binding globulin (SHBG). Testicular injury included disturbed seminiferous architecture, decreased sperm motility, and increased germ-cell apoptosis. Transcriptomics highlighted pathways related to cell adhesion, junctional integrity, and apoptosis, and Western blotting and TUNEL confirmed blood-testis barrier (BTB) protein disruption and increased germ-cell apoptosis. Toxic potency differed by endpoint, with endpoint-specific patterns across endocrine, BTB, and motility outcomes. Combined-effect analysis identified a positive non-additive interaction for LH, whereas most BTB-associated proteins showed no statistically significant interaction despite endpoint-specific deviations from the concentration-addition expectation. Collectively, these findings indicate that human-relevant co-exposure to 6:2 Cl-PFESA and PFHxS is associated with asthenospermia-related sperm and testicular alterations. The converging phenotypic, molecular, and functional findings support BTB impairment and germ-cell apoptosis as plausible contributing processes, yet the precise mechanisms still need further investigation.
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JOURNAL OF CHEMICAL THERMODYNAMICS
·
2024
·
IF 2.2
Yufeng Tang,Qichao Yang,Zhanping Qiao
The phase equilibrium of ternary systems RbX/CsX + CuX 2 + H 2 O (X = Cl, Br) at T = 298.15 K were investigated by the isothermal dissolution equilibrium method, in which the composition of equilibrium solid phases was determined by the Schreinemaker’s wet residue method. In the system RbCl + CuCl 2 + H 2 O, there were three crystallization regions corresponding to RbCl, Rb 2 CuCl 4 ·2H 2 O and CuCl 2 ·2H 2 O, respectively. Five crystallization fields corresponding to CsCl, CsCuCl 3 , Cs 3 Cu 2 Cl 7 ·2H 2 O, Cs 2 CuCl 4 and CuCl 2 ·2H 2 O were formed in the system CsCl + CuCl 2 + H 2 O. The ternary system RbBr + CuBr 2 + H 2 O had three crystalline regions corresponding to RbBr, Rb 2 CuBr 4 ·2H 2 O and CuBr 2 . In the system CsBr + CuBr 2 + H 2 O, the solid-phases of CsCuBr 3 , Cs 2 CuBr 4 , besides CsBr and CuBr 2 , were discovered. The results were compared with available literature data for cesium bromide/copper bromide salt-water system. The seven new solid phase were characterized using the X-ray diffraction method and thermogravimetric/differential analysis. The dissolution enthalpies of Rb 2 CuCl 4 ·2H 2 O, Rb 2 CuBr 4 ·2H 2 O, CsCuCl 3 , Cs 3 Cu 2 Cl 7 ·2H 2 O, Cs 2 CuCl 4 , CsCuBr 3 and Cs 2 CuBr 4 at T = 298.15 K were measured. Their standard enthalpies of formation were obtained, and the results were in order with −(1714.4 ± 3.2) kJ·mol −1 , −(1533.6 ± 3.3) kJ·mol −1 , −(697.8 ± 3.1) kJ·mol −1 , −(2418.9 ± 6.1) kJ·mol −1 , −(1134.8 ± 3.2) kJ·mol −1 , −(563.5 ± 3.2) kJ·mol −1 and −(966.2 ± 3.3) kJ·mol −1 , respectively.
研究领域:
物理化学
·
无机化学
·
热力学
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ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE
·
2020
·Vol. 646
·期 5
·288-295
·
IF 1.24
Yalan Li,Yuandong Wu,Dajiang Mei,Thomas Doert
Three new tin coordination compounds (4,4'-Hbipy) 2 [Sn 2 (C 2 O 4 ) 3 ] ( 1 ), (4,4'-H 2 bipy)[Sn(C 2 O 4 ) 2 ] ( 2 ), and SnCl 2 (4,4'-bipy) ( 3 ) were synthesized under hydro-(solvo-)thermal conditions and their crystal structures were determined by single-crystal X-ray diffraction. Compound 1 exhibits a ionic structure based on discrete [4,4'-Hbipy] + cations and [Sn 2 (C 2 O 4 ) 3 ] 2– anions. These two units are linked via N–H ··· O hydrogen bonds to form a pseudo-one-dimensional zigzag hydrogen-bonded chain. In compound 2 , four-coordinate Sn atoms form monomeric tin dioxalato complexes, which are connected to the doubly protonated [4,4'-H 2 bipy] 2+ cations through N–H ··· O hydrogen bonded to give a one-dimensional zigzag hydrogen-bonded chain. Compound 3 forms a three-dimensional hydrogen-bonded network, in which 1 ∞ [SnCl 2 (4,4'-bipy)] linear chains are interconnected to each other by C–H ··· Cl hydrogen bonding. The solid-state UV/Vis/NIR diffuse reflectance spectroscopy shows that three compounds are broadband semiconductors. The thermogravimetric analysis evidences the thermal stability of the three compounds up to 175, 201, and 246 °C, respectively.
研究领域:
无机化学
·
材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Geying Liu,Chaoyue Xie,Yan Zhang,Ye Du,Jie Wang,Jia Lin,Jing Bai,Jinhua Li,Changhui Zhou,Tingsheng Zhou,Baoxue Zhou
Urea electrolysis is an appealing topic for hydrogen production due to its ability to extract hydrogen at a lower potential. However, it is plagued by sluggish kinetics and noble-metal catalyst requirements. Herein, we developed nickel-iron-layered double hydroxide (NiFe-LDH) nanolayers with abundant oxygen vacancies (O V ) via synergistically etching nickel foam with Fe 3+ and Cl - ions, enabling the efficient conversion of urea into H 2 and N 2 . The synthesized O V -NiFe-LDH exhibits a lower potential (1.30 vs. reversible hydrogen electrode, RHE) for achieving 10 mA cm −2 in the urea oxidation reaction (UOR), surpassing most recently reported Ni-based electrodes. O V provides favorable conductivity and a large surface area , which results in a 4.1-fold in electron transport and a 5.1-fold increase in catalyst reactive sites. Density Functional Theory (DFT) calculations indicate that O V can lower the adsorption energy of urea, and enhance the bonding strength of *CONHNH, giving rise to improved UOR. This study provides a viable path toward economical and efficient production of high-purity hydrogen.
研究领域:
材料科学
·
能源化学
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Advanced Science
·
2023
·Vol. 10
·期 13
·2207630
·
IF 15.1
Wen-Fa Chen,Bin-Wen Liu,Shao-Min Pei,Xiao-Ming Jiang,Guo-Cong Guo
In contrast to anionic group theory of nonlinear optical (NLO) materials that second-harmonic generation (SHG) responses mainly originate from anionic groups, structural regulation on the cationic groups of salt-inclusion chalcogenides (SICs) is performed to make them also contribute to the NLO effects. Herein, the stereochemically active lone–electron-pair Pb 2+ cation is first introduced to the cationic groups of NLO SICs, and the resultant [K 2 PbX][Ga 7 S 12 ] (X = Cl, Br, I) are isolated via solid-state method. The features of their three-dimensional structures comprise highly oriented [Ga 7 S 12 ] 3− and [K 2 PbX] 3+ frameworks derived from AgGaS 2 , which display the largest phase-matching SHG intensities (2.5−2.7 × AgGaS 2 @1800 nm) among all SICs. Concurrently, three compounds manifest band gap values of 2.54, 2.49, and 2.41 eV (exceeding the criterion of 2.33 eV), which can avoid two-photon absorption under the fundamental laser of 1064 nm, along with the relatively low anisotropy of thermal expansion coefficients, leading to improved laser-induced damage thresholds (LIDTs) values of 2.3, 3.8, and 4.0 times that of AgGaS 2 . In addition, the density of states and SHG coefficient calculations demonstrate that the Pb 2+ cations narrow the band gaps and benefit SHG responses.
研究领域:
材料科学
·
光学
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Huiying Liu,Ruxangul Jamal,Tursun Abdiryim,Rena Simayi,Lielie Liu,Yajun Liu
In this paper, carboxylated cellulose (CLC) dissolved in [BMIM]Cl as a soft template combined with the functional group (−NH2, −SH)-grafted poly(3,4-ethylene dioxythiophene) (PEDOT) derivatives was synthesized by an in situ polymerization method. Structural analysis revealed that CLC increased the degree of conjugation of the polymers in the composites and also led to the formation of the fibrous and sheet structure of the composite. The results of the electrochemical performance measurements revealed that the electrode modified by PEDOT-MeNH2/CLC and PEDOT-MeSH/CLC had detection limits (S/N = 3) of 0.38(0.1–380 μM) and 0.042(0.02–520 μM) for the detection of guanine (G), while for the detection of uric acid (UA), the corresponding detection limits (S/N = 3) were 0.255(5–400 μM) and 0.085(0.4–650 μM). The PEDOT-MeSH/CLC-based electrochemical sensor also possessed a wide linear response with the detection limits of 0.077(0.6–620 μM) and 0.144(0.2–460 μM) for the simultaneous detection of UA and G, respectively.
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RSC Advances
·
2018
·Vol. 8
·期 34
·18784-18791
·
IF 2.936
Yuyan Xiao,Xirong Huang
Via heating first and then cooling, binary ionic liquid (IL) mixture of N-methyl-2-pyrrolidonium methylsulfonate ([HNMP][CH3SO3]) and 1-butyl-3-methylimidazolium chloride ([Bmim]Cl) could form a liquid at room temperature. The glass-transition temperature (Tg) characterized by DSC depends on its composition with Tg being as low as −63 °C. The physicochemical properties of the binary IL mixtures also vary with the composition. With the increase of the mole fraction of [Bmim]Cl, the hydrogen-bond accepting ability (β) of the binary IL mixture increases, but the hydrogen-bond donating ability (α) deceases. In this binary IL mixture, fructose could be effectively converted into 5-hydroxymethylfurfural (HMF) at room temperature. The HMF yields at a given time are found to be well correlated with the physicochemical properties of the binary mixture, especially the α and β values. Under specified conditions, the present IL mixture as medium for fructose dehydration into HMF is comparable to the medium formed by ILs and alcohol, where the alcohols have negative effect on the HMF formation.
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CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Peng Hu,Xiaopeng Liang,Muhammad Yaseen,Xiaodan Sun,Zhangfa Tong,Zhongxing Zhao,Zhenxia Zhao
A novel mechano-chemical strategy using dopamine to modify UiO-66(Zr) by N-coordination was proposed to enhance its competitive adsorption for acetaldehyde, chlorobenzene/H 2 O, both thermodynamically and kinetically. The newly synthesized material was characterized by SEM, EDX, XPS, PXRD, FT-IR, TGA/DTG and BET techniques. Results showed that N was successfully grafted into UiO-66(Zr) frameworks through coordination interaction with Zr-O clusters resulting in M-UiO-66(Zr-N 3.0 ). The obtained M-UiO-66(Zr-N 3.0 ) exhibited a significant increase in adsorption of chlorobenzene (4.94 mmol/g) and acetaldehyde (9.42 mmol/g) compared to parent UiO-66(Zr) and UiO-66(Zr)-NH 2 . The H 2 O adsorption uptake of M-UiO-66(Zr-N 3.0 ) decreased by 20% that of UiO-66(Zr) and 47% of UiO-66(Zr)-NH 2 indicating higher hydrophobicity of the modified material. Kinetic performance indicated that diffusivity of chlorobenzene on M-UiO-66(Zr-N 3.0 ) was about 7.8 and 40 times higher than that of the parent UiO-66(Zr) and UiO-66(Zr)-NH 2 respectively and 15.4 times higher than that of H 2 O on itself. Based on the results, the current N-modification strategy can be deemed as an efficient way to improve MOFs competitive adsorption towards VOCs under humid conditions and it might play active role in industries involving adsorbent applications.
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