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MOLECULES · 2023 ·Vol. 28 ·期 13 ·5170 · IF 4.6

Synergistic Promotion of Photocatalytic Degradation of Methyl Orange by Fluorine- and Silicon-Doped TiO2/AC Composite Material

Jinyuan Zhu,Yingying Zhu,Yifan Zhou,Chen Wu,Zhen Chen,Geng Chen

The direct or indirect discharge of organic pollutants causes serious environmental problems and endangers human health. The high electron–hole recombination rate greatly limits the catalytic efficiency of traditional TiO2-based catalysts. Therefore, starting from low-cost activated carbon (AC), a photocatalyst (F-Si-TiO2/AC) comprising fluorine (F)- and silicon (Si)-doped TiO2loaded on AC has been developed. F-Si-TiO2/AC has a porous structure. TiO2nanoparticles were uniformly fixed on the surface or pores of AC, producing many catalytic sites. The band gap of F-Si-TiO2/AC is only 2.7 eV. In addition, F-Si-TiO2/AC exhibits an excellent adsorption capacity toward methyl orange (MO) (57%) in the dark after 60 min. Under the optimal preparation conditions, F-Si-TiO2/AC showed a significant photodegradation performance toward MO, reaching 97.7% after irradiation with visible light for 70 min. Even under the action of different anions and cations, its degradation efficiency is the lowest, at 64.0%, which has good prospects for practical application. At the same time, F-Si-TiO2/AC has long-term, stable, practical application potential and can be easily recovered from the solution. Therefore, this work provides new insights for the fabrication of low-cost, porous, activated, carbon-based photocatalysts, which can be used as high-performance photocatalysts for the degradation of organic pollutants.Keywords:F-Si-TiO2;methyl orange;visible light;doped;electronic cage

CAS / MDL: 11138-49-1
研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING SCIENCE · 2024 · IF 4.1

Decoding the zeolite cage effect in one-step ethylene purification from CO2/C2H2/C2H4 mixtures

Hongwei Chen,Xiangqiong Jiang,Binyu Wang,Yongheng Ren,Bin Zhang,Jiabao Gui,Xili Cui,Linbing Sun,Jiuxing Jiang,Wenfu Yan,Jinping Li,Libo Li

Utilizing physical adsorption for ethylene purification from complex mixtures can significantly reduce the energy cost for production. The purification of multi-component systems through a single adsorption process presents a considerable challenge, largely stemming from the absence of customized strategies and thorough investigations into adsorption behaviours. We aim to understand adsorbents through a unique cage recognition approach and leverage these insights to develop an effective purification adsorbent, with the successful synthesis of SSZ-16 zeolite meeting requirements for multi-component purification. This zeolite, featuring a long aft supercage and a narrow gme cage construct two adsorption cages. The dense π -electron cloud of C 2 H 2 enables a stronger interaction in aft cage, while CO 2 is selectively captured within the environmentally compatible gme cage, demonstrating significantly higher C 2 H 2 and CO 2 adsorption capacity. The separation experiments reveal that SSZ-16 exhibits exceptional performance, with an unprecedented polymer-grade C 2 H 4 productivity of 2099.16 L/kg from the CO 2 /C 2 H 2 /C 2 H 4 mixture.

研究领域: 化学工程 · 材料科学
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS · 2022 ·Vol. 24 ·期 20 ·12550-12562 · IF 3.945

Understanding of the interactions between azole-anion-based ionic liquids and 2-methyl-3-butyn-2-ol from the experimental perspective: the cage effect

Xue Fu,Xiaochen Tang,Tingting Chen,Yingjie Xu,Xiang Luo,Yueqing Lu,Xuming Wang,Dandan Qin,Lin Zhang

The interactions between azole-anion-based ionic liquids (AILs) and 2-methyl-3-butyn-2-ol (MBY) play an important role in AIL-promoted carboxylative cyclization of MBY with CO2. To better understand the interactions between AILs ([P66614][Im], [P66614][4-MeIm], and [P66614][4-BrIm]) and MBY, a detailed investigation from the experimental perspective has been carried out in this study. The results show that the derivative of viscosity (η) with the mole fraction of AIL (xAIL) of AIL + MBY mixtures appears to have the maximum value when xAIL ≈ 0.3, while 1H NMR chemical shifts of P-CH2 of [P66614]+ reach the minimum value at xAIL ≈ 0.3, indicating that [P66614]+ of AILs tend to self-aggregate. The interaction parameters (gji–gii) of the systems obtained from η by the Eyring-UNIQUAC equation are positive, and the difference between the bulk and local composition (xi–xii) is always negative, indicating that AILs can interact with MBY. Moreover, excess molar volumes and isentropic compressibility deviations are all negative deviations and become more negative as the temperature increases, reaching a minimum value at xAIL ≈ 0.30, indicating that azole-based anions can form H-bonds with MBY, and MBY molecules tend to enter the aggregates formed by AILs. Consequently, the cage effect is proposed to describe the interactions between AILs and MBY: MBY first enters the cage formed by the aggregation of [P66614]+, and then forms H-bonds with azole-based anions. Finally, the sizes of the particles of the [P66614][Im] + MBY mixture from dynamic light scattering increase first and then decrease with xAIL, with the maximum of 122 nm at xAIL ≈ 0.25, which confirms the rationality of the cage effect.

CAS / MDL: 56-23-5
研究领域: 化学 · 材料科学
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Soft Matter · 2014 ·Vol. 10 ·期 44 ·8905-8912 · IF 4.151

Bridging and caging in mixed suspensions of microsphere and adsorptive microgel

Chuanzhuang Zhao,Guangcui Yuan,Charles C. Han

Gelation and glass transition in a mixed suspension of polystyrene (PS) microsphere and poly(N-isopropylacrylamide) (PNIPAM) microgel were studied as a function of the total colloid volume fraction and mixing ratio of these two components. The PNIPAM microgel, which is adsorbable on the PS microsphere surface, can induce bridging or stabilizing effect between microspheres depending on whether the volume fraction of microgel (ΦMG) is smaller or larger than the saturated adsorption concentration (Φ*MG) for a given volume fraction of the microsphere (ΦMS). Φ*MG is in a linear relationship with ΦMS, and the value of ΦMG/Φ*MG can be taken as an approximate measure of surface coverage. A state diagram of gelation and glass transition is constructed with the short-ranged attractive interaction, resulting from the well-defined bridging bonding. Keeping ΦMG/Φ*MG = 0.20 and increasing ΦMS from 0.25 to 0.55, the mixed suspension transforms from a bridging gel into an attractive glass; moreover, while keeping ΦMS = 0.45 and increasing ΦMG/Φ*MG from 0.20 to 1.2, the mixed suspension changes from a bridging gel into an attractive glass, and then to a repulsive glass. The bridging effect and the cage effect can be distinguished by the yielding behaviors in rheological measurements. In the nonlinear dynamic rheological experiments, one-step yielding, corresponding to the disconnecting of bridge network, is observed in the bridging gel, and one-step yielding, corresponding to the breaking of cage, is observed in the repulsive glass. However, a two-step yielding behavior is found in the bridging-induced attractive glass, which is attributed to the bridging effect of microgels and the caging effect of the dense environment.

CAS / MDL: 2210-25-5
研究领域: 材料科学 · 软物质物理 · 胶体化学
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Polymer Chemistry · 2013 ·Vol. 4 ·期 16 ·4450-4460 · IF 5.231

Dendritic molecular brushes: synthesis via sequential RAFT polymerization and cage effect for fluorophores

Sipei Li,Chao Gao

Multifunctional dendritic molecular brushes (DMBs) with pendent poly(glycidyl methacrylate) (PGMA) chains were synthesized via a sequential reversible addition–fragmentation chain transfer (RAFT) polymerization approach. By controlling the kinetics of the polymerization, DMBs with a high number-averaged molecular weight (Mn) of ∼1.4 × 106 g mol−1 and narrow polydispersity index (PDI) of 1.50 were obtained. DMBs were reacted with sodium azide, giving rise to giant macromolecules with a high density of hydroxyl and azide bifunctional groups. Pyrene moieties (with a conventional chromophore) were efficiently attached to the DMBs by esterification, affording solution-emissive blue-light DMBs. Ultrahigh excimer emission at 475 nm was achieved for these fluorescent DMBs at a very low concentration of pyrene (∼10−7 mol L−1). Alternatively, tetraphenylethylene (TPE, with an aggregation-induced emission (AIE) chromophore) units were attached to DBMs with a conversion of 100% by copper-catalyzed alkyne–azide click chemistry. The solid-state-emissive blue-light TPE-functionalized DMBs exhibited typical AIE (rather than aggregation enhanced emission, AEE) effect which was rarely observed for dendritic scaffolds and its quantum yield at aggregated state is two times higher than that of fluorophore monomer. Such topology-induced unusual emission phenomena were attributed to the cage effect of DMBs.

研究领域: 高分子化学 · 材料科学 · 光化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Effect of cross-linking density on the rheological behavior of ultra-soft chitosan microgels at the oil–water interface

Xuxi Ma,Songmei Kong,Zhenzhen Li,Shiyu Zhen,Fusheng Sun,Nan Yang

In this paper, microgels with uniform particle size were prepared by physically cross-linking the hydrophobically modified chitosan ( h -CS) with sodium phytate (SP). The effects of cross-linking density on the interfacial adsorption kinetics , viscoelasticity , stress relaxation, and micorheological properties of the hydrophobically modified chitosan microgels ( h -CSMs) at the oil–water interface were extensively investigated by the dilatational rheology, compressional rheology, and particle tracing microrheology. The results were correlated with the particle size, morphology, and elasticity of the microgels characterized by dynamic light scattering and atomic force microscopy . It was found that with the increase of cross-linking density, the h -CSMs changed from a polymer-like state to ultra-soft fussy spheres with higher elastic modulus . The compression isotherms demonstrated multi-stage increase caused by the interaction between the shells and that between the cores of the microgels successively. As the increase of cross-linking density, the h -CSMs diffused slower to the oil–water interface, but demonstrating faster permeation adsorption and rearrangement at the oil–water interface, finally forming interfacial layers of higher viscoelastic modulus due to the core-core interaction. Both the initial tension relaxation and the microgel rearrangement after interface expansion became faster as the microgel elasticity increased. The interfacial microrheology demonstrated dynamic caging effect caused by neighboring microgels. This article provides a more comprehensive understanding of the behaviors of polysaccharide microgels at the oil-water interface.

CAS / MDL: 25952-53-8
研究领域: 材料科学 · 化学工程 · 胶体与界面科学 · 高分子科学
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