PLoS One
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2022
·Vol. 17
·期 8
·e0271075
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IF 3.752
Bicun Jiang,Fuqiang Liu,Yang Pan,Yan Tan,Chendong Shuang,Aimin Li
Tetracycline (TC) is widely-used antibiotic pollutant with high toxicity, refractory, persistence and bacteriostasis, and its removal from water needs to be enhanced. In this work, a novel Graphite-UiO-66(Zr)/Ti electrode was successfully prepared and evaluated for electrochemical oxidation degradation of TC. The electrochemical performance tests indicate the Graphite-UiO-66(Zr)/Ti electrode had higher electrochemical oxidation activity, which achieved higher TC removal efficiency (98.1% ± 1.5%) than Ti plate (65.2% ± 3.5%), Graphite-MIL-53(Al)/Ti electrode (79.5% ± 2.9%) and Graphite-MIL-100(Fe)/Ti electrode (89.0% ± 2.6%). The influence of operating condition was also systematically studied, and the optimized condition was pH 5.0, 20 mA/cm 2 current density and 0.1 M electrolyte (Na 2 SO 4 ). Through the liquid chromatography mass spectrometry (LC-MS), the TC degradation pathway by Graphite-UiO-66(Zr)/Ti electrode oxidation was proposed. Under the •OH free radical oxidative decomposition effect, the double bond, phenolic group and amine group of TC were attacked. TC was transformed into intermediate product ① (m/z = 447), then was further degraded to intermediates ② (m/z = 401) and ③ (m/z = 417). The latter was fragmented into small fractions ④ (m/z = 194), ⑤but-2-enedioic acid (m/z = 116) and ⑥oxalic acid (m/z = 90, the proposed intermediate). In addition, TC removal remained at 89.6% ± 2.7% in the sixth cycle of operation, which confirmed the efficient reusability and stability for antibiotics removal from water.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Jiefei Li,Kunhong Jiang,Suohong Bai,Chaohui Guan,Hang Wei,Haibin Chu
Selective electro-oxidation of glycerol to value-added chemicals has attracted much attention both for the upgrading of biodiesel industry and the coupled electrolytic hydrogen production . Here we report Pt nanoparticles decorated, Fe- and N co-doped carbon nanotube (Pt/FeNC) catalyst for the selective electro-oxidation of glycerol to tartronate, one of the valuable chemicals used in pharmaceuticals. In a high concentrated glycerol solution of 5.0 M, the Pt/FeNC catalyst reaches the glycerol conversion of 94% and tartronate yield over 47% at 0.9 V vs. RHE, equivalent to a tartronate production rate of 1182 mmol/h/gPt, about 20 times of the highest value ever reported in a batch electrocatalytic reactor. The valence band analysis and kinetic experiments reveal that the FeNC mediates the adsorption behavior of the glycerate intermediate on Pt surface, and promotes the glycerate-to-tartronate oxidation . Moreover, the anchoring effect of FeNC ensures the stable catalytic performance for ten cycles.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Zhen Chen,Shipeng Geng,Yawen Wang,Yi Wang,Shuqin Song
H 2 O 2 production by 2 electron water oxidation reaction (2e - WOR) is a promising approach, but still lacks mechanistic studies especially from a dynamic point of view. The interfacial water behavior on the solid/liquid interface is believed to play a crucial role in WOR activity. Here, F modification was used to accommodate the structure and dynamic process of interfacial water on WO 3 surface and boost the 2e- WOR activity. Electrochemical measurement, Raman spectra and computational techniques were used to investigate the mechanism. F modification was proved to guide the dipole moments of interfacial water molecules towards WO 3 surface, meaning more difficult to flip interfacial water molecules to perform the first step of WOR, in turn resulting in easy desorption of HO* and O-O*, thus benefiting for 2 e - WOR. This work paves a novel insight to understand mechanism of 2 e - WOR and rationally design the electrocatalysts for H 2 O 2 production from water.
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MOLECULES
·
2022
·Vol. 27
·期 16
·5288
·
IF 4.927
Bangfu Liu,Zhijian Tan
(1) Background: Aqueous two-phase systems (ATPSs) have been widely used in the separation and purification of bioactive substances in recent years. (2) Methods: In this study, deep eutectic solvents (DESs)-based ATPSs were employed for the extraction and separation ofAstragalus membranaceuspolysaccharides (AMP). The optimal DES (choline chloride:urea = 1:1) was first screened to extract AMP, and the effect of DES concentration, solid–liquid ratio, pH, extraction temperature, and extraction time on the extraction yield of AMP were investigated. (3) Results: The maximum extraction yield was 141.11 mg/g under the optimum conditions. AMP was then preliminarily purified by ATPS, to further realize the recycling and reuse of DES. The effect of type of salts, salt concentration, and extraction temperature on extraction efficiency was investigated. The extraction efficiency was 97.85% for AMP under the optimum ATPS conditions. Finally, the obtained AMP was studied by molecular weight determination, infrared spectroscopy analysis, and monosaccharide composition analysis. (4) Conclusions: This ATPS extraction based on DESs is simple, environmentally friendly, low-cost, and has high extraction efficiency, which provides new ideas for the extraction of plant polysaccharides and other bioactive compounds.Keywords:Astragalus membranaceuspolysaccharides;deep eutectic solvents;solid–liquid extraction;aqueous two-phase system;separation and purification
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Current Research in Food Science
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2022
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IF 6.269
Xi Bao,Shiyao Zhang,Xueting Zhang,Yongli Jiang,Zhijia Liu,Xiaosong Hu,Junjie Yi
In this study, the effects of thermal processing (TP), high pressure processing (HHP), and preservatives addition, i.e. sodium metabisulfite (SMS), on flavor changes in acidified chili peppers were compared. In addition, their changes during different storage periods (25, 37, and 42 °C for 30 days) were also investigated. The results indicate that TP clearly changed the flavor properties of acidified chili peppers compared to other processing, such as an increase in organic acid contents and titratable acid (TA) values but a decrease in pH value, free amino acid (FAA) concentrations, and some aromatic compound contents (e.g., esters and aldehydes). For SMS groups, more biter FAAs and higher alcohol concentrations were detected. Some terpenes (e.g., β-ocimene) significantly increased in samples after HPP ( P < 0.05 ). In addition, storage conditions also clearly affected their flavor, particularly for high storage temperature. During storage, pH fast decreased but TA values and organic acids increased; FAAs firstly increased but followed decreased; esters and terpenes were the main compounds decreasing. Furthermore, some off-flavor related compounds were produced when samples were stored at high temperature, such as furans, aldehydes, and oxides. The outcome of this study could provide new insights into the effects of processing and storage conditions on flavor changes and guide production for the acidified chili pepper industry.
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Journal of Cleaner Production
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2022
·
IF 11.072
Jianyong Che,Wenjuan Zhang,Baozhong Ma,Chengyan Wang
A succinct process for recovering Cu from acidic waste etchant (AWE) was developed in this work, which included recycling Cu via oxalate precipitation, preparing CuO nanoparticles by thermal decomposing the precipitate, and recovering NaCl via evaporation crystallization. A comparison of copper precipitation by H 2 C 2 O 4 and Na 2 C 2 O 4 suggested that an efficient recovery efficiency of Cu was obtained by Na 2 C 2 O 4 (∼99%), which was higher than that by H 2 C 2 O 4 (80.31%). Through thermodynamic analysis, a H + -release mechanism was proposed to explain the significant difference in copper precipitation between Na 2 C 2 O 4 and H 2 C 2 O 4 . By parameter optimization, 99.8% of Cu was recovered without adjusting pH value under optimal conditions, such as temperature of 40 °C, sodium oxalate of 1.2 mol/mol, and reaction time of 2 h. Furthermore, CuO nanoparticles with a purity of 99.92% and particle size of 30 nm were prepared, and the phase transformation of Cu was investigated in-depth using X-ray diffraction (XRD), Scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared spectrum (FT-IR). Finally, the chloride ions were recovered as NaCl at 99.51% purity. This study provides a potential route to deal with strongly acidic waste etchant and achieve its high-value utilization.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2022
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IF 4.598
Chongjie Zou,Chenglong Ma,Fang Chen,Xiang Shao,Limei Cao,Ji Yang
Achieving the robust PbO 2 electrode with the high onset potential is of considerable importance for applying electrochemical pollutants degradation. Herein, the crystal plane strategy was adopted to modify the PbO 2 surface structure through the surfactant induction during synthesis in the electrodeposition process. PbO 2 (β(3 0 1)) and PbO 2 (α(2 0 0), β(3 0 1)) electrodes were obtained by the controlling conditions of surfactants sodium dodecyl sulfate (SDS) and hexadecyl trimethyl ammonium bromide (CTAB). Compared with conventional PbO 2 , the PbO 2 (CTAB) electrode exhibits outstanding performance in electrochemical stability and higher onset potential versus the PbO 2 (SDS). Accelerated life of the PbO 2 (CTAB) electrode is 147 h longer than that of the pure PbO 2 under a high current density of 1A·cm −2 , and the amount of lead ion dissolution is only 45% of that observed in pure PbO 2 . In this work, tetracycline (TC) was taken as an example to evaluate the degradation effect of electrodes. Due to its unique crystal texture, the PbO 2 (CTAB) electrode exhibits higher COD removal rate and TOC removal rate, 35% and 20% respectively beyond that of the conventional lead dioxide electrode. Therefore, it is of great value for its industrial electrode degradation of pollutants.
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ENERGY & FUELS
·
2022
·
IF 4.654
Wei-Wei Yan,Xian-Yong Wei,Jun Li,Meng-Xiao Wang,Hong-Cun Bai,Zhi-Min Zong
Several liquid deep eutectic solvents (DESs) at room temperature were screened and used to extract phenols from an acetonitrile-extractable portion (ANEP) of the oil from oil shale pyrolysis. Among choline chloride (CC)/ethylene glycol (EG) with lowest viscosity and neutral oil entrainment (molar ratio = 1:3) was selected as an optimal DES for isolating phenols from ANEP. As a result, the CC/EG-extractable portion contains 56.7% of oxygen-containing aromatics, among which phenols account for 75.1% by magnetically stirring the isometric mass mixture of ANEP and the CC/EG at room temperature and 500 rpm for 0.5 h. Intermolecular interaction energy and type between different DESs and solutes were calculated by molecular dynamics simulation, independent gradient model analysis, energy decomposition analysis based on the force field, and electrostatic potential analysis to uncover the mechanism for the priority separation of phenols. The result shows that the DES that contains polar HBD with lower viscosity and carbon number and asymmetric HBA with shorter alkyl chains, e.g., CC/EG, could strongly interact with phenols by the strong hydrogen bond, X-H···π and/or cation/anion···π compared to other aromatics.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Guilu Zeng,Rumin Yang,Shuang Tian,Zelong Zhou,Qi Wang,Xiu Yu,Rongbing Fu,Shuguang Lyu
In this work, the effect of different desorbents (low molecular weight organic acids (LMWOAs), surfactants, and inorganic salts) on naphthalene (NAP) desorption in soil was investigated, and the results showed that NAP desorption pattern fitted the pseudo-second-order kinetics. The addition of LMWOAs, especially citric acid (CA), could stimulate the reactive oxygen species (ROS) generation and NAP degradation in Fe(II) activated persulfate (PS) system, while the presence of surfactants and CaCl 2 could inhibit the NAP removal due to the competitive consumption of ROS. The maximum removal of NAP was 97.5% within 120 min at the PS/Fe(II)/CA/NAP molar ratio of 15/5/1/1, and the pseudo-first-order kinetic constant of NAP removal increased from 0.0110 min −1 to 0.0783 min −1 with the addition of CA. Compared with surfactants and inorganic salts, LMWOAs, especially CA, were more suitable as desorbent in soil washing coupled with in situ chemical oxidation technique. Moreover, 1.86 mg L −1 desorbed amount and 36.1% removal of NAP from soil could be obtained with the presence of 1 mM CA. Finally, the significant removal of NAP and other contaminants (phenanthrene, fluoranthene , and benzene series) in actual groundwater could provide theoretical basis and technical support for the remediation of organic contaminated sites with desorbents.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2022
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IF 4.598
Yang Zhou,Xiaoyan She,Qiong Wu,Jiangrong Xiao,Tianyou Peng
A novel and sensitive electrochemical sensor based on monoclinic tungsten trioxide (WO 3 ) nanosheets-carbon nanotubes nanocomposite (WO 3 -CNT) modified glass carbon electrode (GCE) is developed for the direct detection of endocrine disruptor bisphenol A (BPA) in textile sample for the first time. The electrochemical behavior of BPA on the resultant WO 3 -CNT/GCE sensor is investigated using electrochemical impedance spectroscopy (EIS), cyclic voltammetry (CV) and chronocoulometry (CC). Under the optimized conditions, the proposed sensor can be adopted to the quantification of BPA using differential pulse voltammetry (DPV), and the electro-oxidation peak current is proportional to the BPA concentration in the range of 0.03–3.0 μM and 3.0–100 μM with a correlation coefficient of 0.9993 and 0.9992, respectively. Moreover, the proposed sensor with a detection limit of 16.3 nM (S/N = 3) exhibits good reproducibility, selectivity and stability, and can be successfully applied to detect the BPA concentrations in real samples (textile, plastic and tap water) with satisfactory recovery (99.4%-110.1%). The present strategy on the hybridization of CNTs and WO 3 enables more opportunities for the electrochemical detection of BPA in the practical applications.
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ChemCatChem
·
2022
·Vol. 14
·期 16
·e202200509
·
IF 5.497
Jiefei Li,Zhenyu Li,Zexuan Zheng,Xueqiong Zhang,Hao Zhang,Hang Wei,Haibin Chu
Graphical Biomass conversion : Electro-oxidation of glycerol over the Pt/CNT catalyst suffers from the poor activity, low glyceric acid (GLYA) selectivity, and high cost of the noble metal. The incorporation of CeO 2 into Pt/CNT achieves much enhanced yield of GLYA with even half dosage of Pt. Electrocatalytic oxidation of glycerol is a highly efficient way for upgrading glycerol toward fine chemicals. Currently, electro-oxidation of glycerol into the high value-added C3 products remains a big challenge because of the poor catalytic activity, low selectivity, and high cost of the noble metal catalysts, especially in the alkaline medium. Here, we report that the Pt−CeO 2 /CNT (CNT=carbon nanotubes) catalyst remarkably promotes the conversion (86.5 % vs. 37.6 %) and recycling stability for glycerol electro-oxidation reaction, as compared with Pt/CNT. However, the improved catalytic activity of Pt−CeO 2 /CNT is accompanied by the further oxidation of C3 products including glyceric acid (GLYA). By tuning the product distribution by the ratio of CeO 2 and CNT, applied potential, and the Pt loading amount, the high selectivities of C3 products (95 %) and GLYA (59 %) are achieved together with the high glycerol conversion (86 %), leading to the impressive yields of C3 products (81 %) and GLYA (50 %). The unique contributions of CeO 2 includes not only the enhanced catalytic activity and recycling stability, but also the suppressed further oxidation of GLYA. Moreover, higher yield of GLYA is reached over Pt−CeO 2 /CNT even with half loading of Pt, as compared with Pt/CNT.
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Nanomaterials
·
2022
·Vol. 12
·期 9
·1468
·
IF 5.719
Dan Zhang,Chunfei Wang,Changfeng Wu,Xuanjun Zhang
Here, we confined fluorescent probes to solid nanochannels to construct nanosensors, which not only significantly improved the reusability of the molecular probes, but also achieved ion current and fluorescence dual gating for more reliable detection. The combination of optical and electrical modalities can provide comprehensive spatiotemporal information that can be used to elucidate the sensing mechanism within the nanochannel. As a proof-of-concept experiment, fluorescein isothiocyanate (FITC)–hydrazine (N2H4) was selected to modify nanochannels for the effective detection of Hg2+. Based on spirolactam opening tactics, the system synergistically alters the surface charge and fluorescence intensity in response to Hg2+, establishing a dual open state of current and fluorescence. The newly prepared nanosensor exhibited a fast response (<1 min), high sensitivity, and selectivity towards Hg2+. Importantly, the nanodevice could be recovered by simple N2H4treatment. Such sensing behavior could be used to implement optoelectronic dual-output XOR logical gates under the management of Hg2+and N2H4. This strategy is anticipated to find broad applications in other nanochannel-based systems for various sensing applications used for monitoring of pollutants, food additives, and biomolecules.Keywords:nanochannel sensor;dual gating;ion current;fluorescence;Hg(II);reusable
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