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Cystine-assisted accumulation of gold nanoparticles on ZnO to construct a sensitive surface-enhanced Raman spectroscopy substrate
Qi Qu, Chuan Zeng, Jing Huang, Mengfan Wang, Wei Qi, Zhimin He
Frontiers of Chemical Science and Engineering. 2023, 17 (1): 15-23.
https://doi.org/10.1007/s11705-022-2177-8
Recently, various semiconductor/metal composites have been developed to fabricate surface-enhanced Raman spectroscopy substrates. However, low metal loading on semiconductors is still a challenge. In this study, cystine was introduced to increase the accumulation of gold nanoparticles on zinc oxide, owing to the biomineralization property of cystine. Morphological analysis revealed that the obtained ZnO/Au/cystine composite not only had a higher metal loading but also formed a porous structure, which is beneficial for Raman performance. Compared with ZnO/Au, the ZnO/Au/cystine substrate displayed a 40-fold enhancement in the Raman signal and a lower limit of detection (10–11 mol·L−1) in the detection of rhodamine 6G. Moreover, the substrate has favorable homogeneity and stability. Finally, ZnO/Au/cystine displayed excellent performance toward crystal violet and methylene blue in a test based on river water samples. This study provided a promising method to fabricate sensitive semiconductor/noble metal-based surface-enhanced Raman spectroscopy substrates for Raman detection.
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A novel flavonol-based colorimetric and turn-on fluorescent probe for rapid determination of hydrazine in real water samples and its bioimaging in vivo andin vitro
Ahui Qin, Yan Zhang, Shuai Gong, Mingxin Li, Yu Gao, Xu Xu, Jie Song, Zhonglong Wang, Shifa Wang
Frontiers of Chemical Science and Engineering. 2023, 17 (1): 24-33.
https://doi.org/10.1007/s11705-022-2171-1
Hydrazine is extremely toxic and causes severe harm to human body. Herein, a novel fluorescent probe 4-oxo-2-styryl-4H-chromen-3-yl thiophene-2-carboxylate (FHT) was synthesized for detecting hydrazine by using natural cinnamaldehyde as starting material. This probe exhibited significantly enhanced fluorescence response towards hydrazine over various common metal ions, anions, and amine compounds. The detection limit of probe FHT for hydrazine was as low as 0.14 μmol·L–1, significantly lower than that of the threshold value of 0.312 μmol·L–1, imposed by the Environmental Protection Agency. Moreover, the proposed probe was able to detect hydrazine within wide pH (5–10) and linear detection ranges (0–110 μmol·L–1). This probe was employed for determining trace hydrazine in different environmental water samples. The probe FHT-loaded filter paper strips were able to conveniently detect hydrazine of low concentration through distinct naked-eye and fluorescent color changes. Importantly, the probe FHT with low cytotoxicity was successfully applied to visualize hydrazine in living Hela cells and zebrafish.
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Systematic screening procedure and innovative energy-saving design for ionic liquid-based extractive distillation process
Tuanjie Shen, Liumei Teng, Yanjie Hu, Weifeng Shen
Frontiers of Chemical Science and Engineering. 2023, 17 (1): 34-45.
https://doi.org/10.1007/s11705-022-2234-3
In the traditional extractive distillation process, organic solvents are often used as entrainers. However, environmental influence and high energy-consumption are significant problems in industrial application. In this study, a systematic screening strategy and innovative energy-saving design for ionic liquid-based extractive distillation process was proposed. The innovative energy-saving design focused on the binary minimum azeotrope mixtures isopropanol and water. Miscibility, environmental impact and physical properties (e.g., melting point and viscosity) of 30 ionic liquids were investigated. 1-Ethyl-3-methyl-imidazolium dicyanamide and 1-butyl-3-methyl-imidazolium dicyanamide were selected as candidate entrainers. Feasibility analysis of these two ionic liquids was further performed via residue curve maps, isovolatility line and temperature profiles. An innovative ionic liquid-based extractive distillation process combining distillation column and stripping column was designed and optimized with the objective function of minimizing the total annualized cost. The results demonstrate that the total annualized cost was reduced by 19.9% with 1-ethyl-3-methyl-imidazolium dicyanamide as the entrainer and by 24.3% with 1-butyl-3-methyl-imidazolium dicyanamide, compared with that of dimethyl sulfoxide. The method proposed in this study is conducive to the green and sustainable development of extractive distillation process.
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Fabrication of a superhydrophilic/underwater superoleophobic stainless steel mesh for oil/water separation with ultrahigh flux
Jiawei Wang, Jie Hu, Junjie Cheng, Zefei Huang, Baoqian Ye
Frontiers of Chemical Science and Engineering. 2023, 17 (1): 46-55.
https://doi.org/10.1007/s11705-022-2170-2
Because of the increasing amount of oily wastewater produced each day, it is important to develop superhydrophilic/underwater superoleophobic oil/water separation membranes with ultrahigh flux and high separation efficiency. In this paper, a superhydrophilic/underwater superoleophobic N-isopropylacrylamide-coated stainless steel mesh was prepared through a simple and convenient graft polymerization approach. The obtained mesh was able to separate oil/water mixtures only by gravity. In addition, the mesh showed high-efficiency separation ability (99.2%) and ultrahigh flux (235239 L∙m–2∙h–1). Importantly, due to the complex cross-linked bilayer structure, the prepared mesh exhibited good recycling performance and chemical stability in highly saline, alkaline and acidic environments.
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Vanadium(IV) solvent extraction enhancement in high acidity using di-(2-ethylhexyl)phosphoric acid with [Cl−] present: an experimental and theoretical study
Hong Liu, Yi-Min Zhang, Jing Huang, Tao Liu
Frontiers of Chemical Science and Engineering. 2023, 17 (1): 56-67.
https://doi.org/10.1007/s11705-022-2185-8
Separation of vanadium from black shale leaching solution at low pH is very meaningful, which can effectively avoid the generation of alkali neutralization slag and the resulting vanadium loss. In this study, coordination mechanism of vanadium in acid leaching solution at low pH was investigated with the intervention of chloride ions. Under the conditions of pH 0.8, di-(2-ethylhexyl)phosphoric acid concentration of 20%, phase ratio of 1:2, and extraction time of 8 min, the vanadium extraction could reach 80.00%. The Fourier transform infrared and electrospray ionization results reveal that, despite the fact that the chloride ion in the leachate could significantly promote vanadium extraction, the chloride ion does not enter the organic phase, indicating an intriguing phenomenon. Among Cl−–V, SO42−–V, and H2O–V, the V–Cl bond is longer and the potential difference between coordinate ions and vanadium is smaller. Therefore, VO2+ gets easily desorbed with chloride ions and enter the organic phase. At the same time, the hydrogen ions of di-(2-ethylhexyl)phosphoric acid also enter the water phase more easily, which reduces the pH required for the extraction reaction.
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Cobalt nitride enabled benzimidazoles production from furyl/aryl bio-alcohols and o-nitroanilines without an external H-source
Chuanhui Li, Li-Long Zhang, Hu Li, Song Yang
Frontiers of Chemical Science and Engineering. 2023, 17 (1): 68-81.
https://doi.org/10.1007/s11705-022-2174-y
Benzimidazole derivatives have wide-spectrum biological activities and pharmacological effects, but remain challenging to be produced from biomass feedstocks. Here, we report a green hydrogen transfer strategy for the efficient one-pot production of benzimidazoles from a wide range of bio-alcohols and o-nitroanilines enabled by cobalt nitride species on hierarchically porous and recyclable nitrogen-doped carbon catalysts (Co/CNx-T, T denotes the pyrolysis temperature) without using an external hydrogen source and base additive. Among the tested catalysts, Co/CNx-700 exhibited superior catalytic performance, furnishing 2-substituted benzimidazoles in 65%–92% yields. Detailed mechanistic studies manifest that the coordination between Co2+ and N with appropriate electronic state on the porous nitrogen-doped carbon having structural defects, as well as the remarkable synergetic effect of Co/N dual sites contribute to the pronounced activity of Co/CNx-700, while too high pyrolysis temperature may cause the breakage of the catalyst Co–N bond to lower down its activity. Also, it is revealed that the initial dehydrogenation of bio-alcohol and the subsequent cyclodehydrogenation are closely correlated with the hydrogenation of nitro groups. The catalytic hydrogen transfer-coupling protocol opens a new avenue for the synthesis of N-heterocyclic compounds from biomass.
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Reductive amination of n-hexanol to n-hexylamine over Ni–Ce/γ-Al2O3 catalysts
Pengfei Li, Huijiang Huang, Zheng Wang, Ziying Hong, Yan Xu, Yujun Zhao
Frontiers of Chemical Science and Engineering. 2023, 17 (1): 82-92.
https://doi.org/10.1007/s11705-022-2181-z
The amination of alkyl alcohols is one of the most promising paths in synthesis of aliphatic amines. Herein, cerium doped nickel-based catalysts were synthesized and tested in a gas-phase amination of n-hexanol to n-hexylamine. It was found that the activity of the Ni/γ-Al2O3 catalyst is significantly improved by doping an appropriate amount of cerium. The presence of cerium effectively inhibits the agglomeration of nickel particle, resulting in better Ni dispersion. As Ni particle size plays critical role on the catalytic activity, higher turnover frequency of n-hexanol amination was achieved. Cerium doping also improves the reduction ability of nickel and enhances the interactions between Ni and the catalyst support. More weak acid sites were also found in those cerium doped catalysts, which promote another key step—ammonia dissociative adsorption in this reaction system. The overall synergy of Ni nanoparticles and acid sites of this Ni–Ce/γ-Al2O3 catalyst boosts its superior catalytic performance in the amination of n-hexanol.
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Synergistic effect of V and Fe in Ni/Fe/V ternary layered double hydroxides for efficient and durable oxygen evolution reaction
Lihong Chen, Ruxin Deng, Shaoshi Guo, Zihuan Yu, Huiqin Yao, Zhenglong Wu, Keren Shi, Huifeng Li, Shulan Ma
Frontiers of Chemical Science and Engineering. 2023, 17 (1): 102-115.
https://doi.org/10.1007/s11705-022-2179-6
High-performance and stable electrocatalysts are vital for the oxygen evolution reaction (OER). Herein, via a one-pot hydrothermal method, Ni/Fe/V ternary layered double hydroxides (NiFeV-LDH) derived from Ni foam are fabricated to work as highly active and durable electrocatalysts for OER. By changing the feeding ratio of Fe and V salts, the prepared ternary hydroxides were optimized. At an Fe:V ratio of 0.5:0.5, NiFeV-LDH exhibits outstanding OER activity superior to that of the binary hydroxides, requiring overpotentials of 269 and 274 mV at 50 mA·cm–2 in the linear sweep voltammetry and sampled current voltammetry measurements, respectively. Importantly, NiFeV-LDH shows extraordinary long-term stability (≥ 75 h) at an extremely high current density of 200 mA·cm–2. In contrast, the binary hydroxides present quick decay at 200 mA·cm–2 or even reduced current densities (150 and 100 mA·cm–2). The outstanding OER performance of NiFeV-LDH benefits from the synergistic effect of V and Fe while doping the third metal into bimetallic hydroxide layers: (a) Fe plays a crucial role as the active site; (b) electron-withdrawing V stabilizes the high valence state of Fe, thus accelerating the OER process; (c) V further offers great stabilization for the formed intermediate of FeOOH, thus achieving superior durability.
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