ACS ES&T Engineering
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2024
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IF 7.4
Lin-Feng Zhai,Shu-Ya Xu,Jun Yu,Zhao-Jian Hu,Min Sun,Yan Wang
Nonradical oxidation is a promising pathway for the selective removal of organic pollutants in complex wastewaters. However, traditional catalytic oxidation processes generally depend on free radicals to achieve favorable pollutant removal. Herein, we developed a nonradical pathway-governed catalytic oxidation process by applying an electric field to selectively activate a surface O2-complex on a MnO catalyst. On the surface of positively polarized MnO, adsorbed O2 was activated into positively charged peroxide species as the main reactive species. A Langmuir–Hinshelwood model based on irreversible bimolecular reaction between adsorbed reaction species was developed to kinetically differentiate the oxidation behaviors of twelve substituted phenolic compounds. The surface reaction rate constant was identified as the key parameter controlling the reaction kinetics. To unveil the substrate-dependent reaction rules of the nonradical pathway, quantitative structure–activity relationship (QSAR) analysis was performed to correlate the surface reaction rate constants of phenolic compounds to their molecular features. A QSAR model was constructed by synergizing IE, EHOMO, and q(C–)n together to predict the reactivity of a phenolic compound in the nonradical pathway. Guided by the QSAR model, the catalytic oxidation process was applied for safe and energy-saving treatment of triclosan-contaminated water. This work is anticipated to provide valuable information for triggering and manipulating nonradical catalytic oxidation processes as well as understanding their selective oxidation nature.
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JOURNAL OF CHROMATOGRAPHY A
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2024
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IF 3.8
Wenhui Lu,Shanchao Fu,Xiuqi Lang,Huizhen Zhao,Deyi Zhu,Shan Cao,Lingxin Chen,Jinhua Li
Magnetic multi-template molecularly imprinted polymers (M-mt-MIPs) were successfully synthesized by surface imprinting and multi-template imprinting strategy, using polydopamine coated magnetic multi-walled carbon nanotubes as supporting materials, five typical chlorophenols (CPs) as templates, methacrylic acid as functional monomer and ethylene glycol dimethacrylate as cross-linker. Compared to non-imprinted polymers (NIPs), the as-prepared M-mt-MIPs showed high adsorption capacity (32.58‒80.63 mg g −1 ), rapid mass transfer and specific selectivity for the five targeted CPs, which were applied as magnetic solid-phase extraction (MSPE) adsorbents. Parameters affecting MSPE efficiency were detailed investigated, such as adsorbents dosage, sample pH, extraction time, type and volume of desorption solvent and salt effect. Combined with HPLC-DAD, a simple, rapid and sensitive method was established, showing good linearity (2‒200 μg L −1 ), low limits of detection (0.32‒0.49 μg L −1 ), and high enrichment factors (35.2‒108). The developed M-mt-MIPs-MSPE-HPLC method was applied to enrich and determine CPs in tannery wastewater, wet-blue and crust leather, and satisfactory spiking recoveries were attained in the range of 73.95‒109.7% with relative standard deviations (RSDs) of 2.13–8.48%. This study provided a new alternative material and method to rapid simultaneously extract and analyze low concentration of typical CPs in complicated matrices.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Yuqian Zhou,Zhongxin Tan
Soft rot is one of the most susceptible soil-borne diseases of pakchoi ( Brassica chinensis L.), severely hindering its industrial development. The research aimed to evaluate the application effect of polyphenols extracted from pineapple peel waste in improving the rhizosphere soil environment of pakchoi infected by soft rot and promoting plant health and growth. We found that using pineapple peel polyphenols (PPPs) at 4 mg/mL concentration (P1 treatment) significantly improved soil quality, reduced pakchoi disease incidence, and effectively promoted pakchoi growth. Compared with the control group (CK), the P1 treatment led to a marked 79.97% reduction in diseased pakchoi leaves. Meanwhile, the rhizosphere soil structure showed reduced diseased genera and increased beneficial bacterial phyla, along with boosted soil enzyme activities. Furthermore, P1 treatment improved key growth parameters of pakchoi, including neck thickness (62.07%), plant height (57.43%), fresh weight (154.52%), dry weight (121.88%), maximum leaf length (47.28%), width (30.98%), and total chlorophyll content (50.11%). The application of PPPs has shown significant effects in enhancing the ecological environment of the diseased soil and reducing the incidence of soft rot disease of pakchoi and has great potential in increasing the yield of pakchoi. This study offers an eco-friendly and sustainable approach for the valorization of PPPs and the management of soil-borne diseases, which holds profound implications for enhancing crop quality, soil health, and human well-being.
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CARBON
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2024
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IF 10.5
Aiying Song,Rong Liu,Xinghe He
A novel strategy for fabricating deeply reduced three-dimensional inter-porous graphene oxide (drtdipGO)-coated solid-phase microextraction (SPME) fibers was developed. The reduced graphene oxide (rGO) coating was initially immobilized onto a stainless steel wire (SSW) through natural contraction from water loss during the drying process. This was achieved via deoxygenation of graphite oxide using ascorbic acid in an aqueous medium. To enhance the hydrophobicity, surface area, and adhesion strength between the coating and SSW, the rGO coating was calcined and further deoxidized in an H 2 /Ar atmosphere at 1100 °C. The as-fabricated fiber exhibited a homogeneous and wrinkled surface, high Brunauer-Emmett-Teller (BET) surface area (520 m 2 g −1 ), increased hydrophobicity, and unique three-dimensional inter-porous structure. The drtdipGO-coated fibers were employed for sensitive headspace solid-phase microextraction (HS-SPME) of petroleum hydrocarbons (PHCs) in water samples. Enrichment factors ranging from 1.2 to 32.1 were achieved for PHCs. The extraction efficiency per unit volume of the drtdipGO coating for all 31 PHCs was higher than that of five commercial SPME fiber coatings (1.5–1275.0-fold improvement). The proposed method exhibited a linear range of 5–500 μg L −1 (R ≥ 0.990), with limits of detection and quantification ranging from 0.71 to 14.4 μg L −1 and 2.4–48.0 μg L −1 , respectively. Recoveries (C10–C26) of 83%–108 % were obtained for water samples sourced from river, sewage, lake, and artificial water samples.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Huaimin Wang,Shuang Meng,Zixuan Zhang,Chenying Zhou,Heng Zhang,Yang Liu,Chuan-shu He,Peng Zhou,Bo Lai
It has been reported that the ultrasonic agitation coupled system (US/A) has higher oxidation efficiency than the pure ultrasonic system (US), and the atomic hydrogen ( H) and hydroxyl radicals ( OH) produced by H 2 O cracking and in situ hydrogen peroxide (H 2 O 2 ) can be significantly detected. In order to utilize the residual H 2 O 2 and explore the role and fate of H, US/A/Fe(III) as an in situ Fenton oxidation system, was constructed in this study. The experimental results proved that the system can generate H 2 O 2 in situ , and adding Fe(III) could significantly promote the oxidation of refractory organic pollutants. Quenching tests, probes experiments and EPR test were performed to successfully monitor the existence of OH. The contribution of H to Fe(III) reduction was speculated and confirmed. In addition, the kinetic model showed the decomposition rate of water molecule and the reduction rate of Fe(III) by H under different ultrasonic power. The effects of the factors (pH, coexisting substance, and actual water environment) on degrading organic pollutants were evaluated. Therefore, this work provides new strategy and mechanistic insight into in situ Fenton technique by coupling ultrasonic agitation and Fe(III) without external oxidants.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Jiangyun Zhe,Huan He,Zhanwei Yi,Ziwei Guo,Haisheng Xu,Bin Huang,Xuejun Pan
Landfill leachate usually contains a substantial content of refractory dissolved organic matter (RDOM), which mainly consists of humic acid and fulvic acid. RDOM easily blocks the membrane pores resulting in membrane fouling when treated using membrane technologies, and it costs abundant chemical regents using advanced oxidation processes. To achieve the economically efficient treatment of RDOM in landfill leachate, this study established the electroflocculation coupled with ozone (EFCO) system. EFCO achieved a higher removal for organic matter than single electroflocculation and ozonation, where RDOM was the main component of organic matter in landfill leachate. The remaining RDOM was decomposed into lots of micromolecule weight and biodegradable proteins and lipids. Ozone improved the removal of dissolved organic matter (DOM) mainly by changing the functional groups on its surface and improving the mechanical strength of flocs to enhance the complexation between flocs and DOM. Cl 2 − and ClO produced in the EFCO system were the main active chlorine species, which enhanced the mineralization of RDOM. The study provides an efficient method for the pretreatment of RDOM in landfill leachate.
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Journal of Cleaner Production
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2024
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IF 9.7
Weijuan Zhang,Hui Lin,Yousef Faraj,Ruzhen Xie
Electrochemical persulfate activation (E-PS) has recently emerged as a highly effective advanced oxidation process in water decontamination . However, the presence of chloride ions (Cl − ) in waters can accelerate anodic corrosion as well as lead to the formation of toxic chlorinated byproducts (i.e., ClO 4 − ), limiting its practical application. In this study, we introduce a novel Nd/Bi@SnO 2 anode to construct E-PS, which exhibits high stability in chloride-containing water with a long-expected service lifetime of 13.7 years. The Nd/Bi@SnO 2 electrode can effectively convert Cl − to reactive chlorine with the assistance of PMS , triggering singlet oxygen ( 1 O 2 ) generation for superior organic removal while avoiding toxic chlorinated byproducts (i.e., ClO 4 − ) generation as well as greatly reducing the energy consumption. Comprehensive structural and electrochemical characterization results demonstrate Nd/Bi co-doping introduces oxygen vacancy on Nd/Bi@SnO 2 , enabling the anode with high oxygen evolution potential , excellent conductivity and superior stability. Scavenging experiments and electron paramagnetic resonance illustrate the generation of various reactive species in the system, among which 1 O 2 predominantly contributes to organic removal and results in harmless intermediates. This innovative approach transforms Cl − into ROSs for eco-friendly, energy-efficient water decontamination.
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Reaction Kinetics Mechanisms and Catalysis
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2024
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IF 1.7
Liu Zhi,Xie Shiwei,Xiao Tian,Fang Chengyi,Liu Xixiang,Liu Yan
In this study, Ti-Sn-Sb/γ-Al 2 O 3 particle electrodes were prepared by sol–gel method and a three-dimensional electrocatalytic system was constructed to treat methylene blue (MB) dye wastewater. The experimental results demonstrate that the degradation of methylene blue conforms to the pseudo-first order reaction kinetics and had a low activation energy (E a = 36.97 kJ/mol). Through quenching experiments, linear voltammetry tests, and radical trapping experiments utilizing benzoic acid as a probe, we have determined that the oxidation of MB by the particle electrode is primarily induced through direct surface electron transfer (86 ~ 88%) and surface-bound radicals (12 ~ 14%). Graphical abstract Methylene blue undergoes degradation through the synergistic interplay of direct electron transfer (86% ~ 88%) and surface-bound radicals ·OH ads (12% ~ 14%) on the particle electrode’s surface.
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ACS Food Science & Technology
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2024
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IF 2.6
Cailin Kong,Yun Wu,Qi Zhang,Faisal Eudes Sam,Aihua Li,Yongsheng Tao
Extended wine storage often leads to a reduction in volatile compounds, diminishing the fruity aroma. Yeast mannoproteins (MPs) have been identified as a mitigating factor against this effect, although the mechanisms involved remain poorly understood. This study examines the impact of MPs from Pichia strains, noting differences in chemical composition and structure, on the volatility of wine fruity esters. Gas chromatography, high-performance liquid chromatography, and Fourier transform infrared spectroscopy were used to analyze MPs from Saccharomyces cerevisiae SC-19 (MP-SC), Pichia fermentans Z9Y-3 (MP-PF), and Pichia kluyveri MP-PK. The influence of MPs on wine ester volatility was further explored through headspace solid-phase microextraction and gas chromatographic-mass spectrometry, alongside thermodynamic assessments. The findings revealed that mannose predominates in the monosaccharide composition of MPs, with MP-SC presenting the highest mannose levels. MP-PF and MP-PK, however, exhibited higher protein concentrations and significantly more hydrophilic amino acids, contributing to a 3–6-fold reduction in ester volatility compared with MP-SC, likely due to enhanced van der Waals forces and hydrogen bonding.
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JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Ningxuan Xue,Zhaobing Guo,Xinyu Gai,Yiyang Chen,Siyue He,Guanjie Lin,Fengling Liu,Shuai Zhang,Pengxiang Qiu
Ferrate (Fe(VI)) is a widely used water purifier and is easily affected by external factors. Given that the actual water environment conditions are complicated, this study designed an oxygen-doped carbon nitride (CNO) with rich electron sites to explore whether direct electron transfer promotes the degradation efficiency of Fe(VI) for pollutants under visible light. For comparison, we also prepared phosphorus-doped carbon nitride (CNP), which has electron-deficient sites and indirect electron transfer. In the CNO/Fe(VI)/light system, not only more high-valent iron and reactive oxygen species were generated, but also the pollutant degradation rate, reaction kinetics, and electron yield were significantly better than those of the CNP and CN systems, verifying the superiority of direct electron transfer. In addition, CNO showed excellent performance in both actual solar photocatalysis and continuous flow experiments. Therefore, the photocatalysis/direct electron transfer mechanism proposed provides an innovative strategy for improving the application potential of Fe(VI) in the field of pollution control and its industrialization application.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Jing Lv,Hui Ye,Shurui Han,Jinli Zhao,Guodong Yang,Han Zhang,Xiaojian Fu,Jing Zhang,Qingping Xin,Lizhi Zhao,Hong Li,Ligang Lin,Xiaoli Ding,Yuzhong Zhang
Two-dimensional (2D) structural materials as catalyst supports is crucial for improving the heterogeneous catalytic activity, while the relationships between their porous structure and catalytic performance are still not very clear. Herein, four kinds of porous 2D Fluorine-Cerium (F-Ce) nanosheets were fabricated and used as catalyst support, aiming to investigate the effect of porous structure on the catalytic properties by heterogeneous Fenton oxidation and unveil the structure-activity relationships. Compared with 2D non-porous GO, Ti 3 C 2 , and porous g-C 3 N 4 , F-Ce nanosheets exhibited superior catalytic activity. Specifically, FeOOH/F-Ce-3 catalysts achieved 95.5 % phenol removal within 40 minutes, with the deposition sites and electronic structures of the loaded Fe-active species being modulated by tuning the pore structures. In addition, we demonstrated that large pore size and high pore volume are more conducive to high catalytic performance, as well as the uniform pore shape and well-ordered pore distribution are more favorable for mass transfer during catalysis. This work emphasizes the great advantage of using porous 2D F-Ce nanosheets as support in the construction of heterogeneous Fenton catalysts while elaborating the relationship between pore structure and catalytic activity.
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JOURNAL OF RARE EARTHS
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2024
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IF 5.2
Chen Di-Ming,Han-Dong Qiao,Shao-Ming Fang
Introduction of porosity and fluorescent properties into lanthanide metal–organic frameworks (MOFs) with rational design to achieve multifunctional use is of great significance from the energy and environmental viewpoint. In this study, a microporous Tb(III)-based MOF with the formula of {[Tb 2 (oba) 3 (Phen) 2 ](DMF) 2 (H 2 O) 4 } n ( 1 ) was solvothermally prepared via using the mixed ligands of 1,10-phenanthroline (Phen) and 4,4′-oxybis(benzoic acid) (H 2 oba) as organic connecters. The structural evaluation results indicate that complex 1 is composed of binuclear Tb 2 (CO 2 ) 6 (Phen) 2 clusters which are extended by the oba 2− ligands to afford a two-fold interpenetrated framework with one-dimensional microporous channels along the b -axis. Gas sorption studies show that the activated 1 demonstrates a high ideal adsorption solution theory (IAST) sorption selectivity of 7.4 toward C 2 H 2 in a C 2 H 2 /CO 2 gas mixture, which are further supported by the dynamic breakthrough experiments. The grand canonical Monte Carlo (GCMC) simulation results indicate that the synergistic effects of the H-bond interactions of C 2 H 2 with oba 2− ligands and the C–H···π interactions with Phen ligand contribute to the strong binding of the framework toward C 2 H 2 molecules. What's more, the luminescent measurements reveal that the emission of 1 features both the characteristic peaks of Phen ligand and Tb(III) ion, which could be further applied as a self-calibrating sensor for the Cr(VI) detection in water. To the best of our knowledge, complex 1 represents the first example of Tb-MOF holding such a high C 2 H 2 /CO 2 selectivity together with ratiometric Cr(VI) detection performances.
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