CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Liang Zhang,Bofan Zhang,Yunxia Liu,Zinan Wang,Jafar Hussain Shah,Rile Ge,Wenhui Zhou,Shiro Kubuki,Junhu Wang
The radical-based Fenton-like reaction quenching by various inorganic anions or high concentration of organic matters restrict the practical value in future industrial application. Contrarily, the nonradical-dominated system could efficiently overcome above limitations and achieve excellent catalytic capacity under a wide category of water matrixes. Herein, a series of Zn-Fe double oxides were successfully fabricated via calcination of Zn 1-x Fe x -Fe Prussian blue analogues under ambient atmosphere. Under the coexistence of visible light and peroxymonosulfate (PMS), Zn-Fe double oxides manifested excellent catalytic performance towards various organic pollutants oxidation with trace amount of iron leaching, and even showed superior contaminant decomposition efficiency under high concentration of organic matter and practical aqueous system. Confirmed by radical trapping experiment and electron paramagnetic resonance spectroscopy, the photo-induced electrons and holes can act as triggers to PMS activation and thereby transform reaction routes from radicals to singlet oxygen ( 1 O 2 )-dominated nonradical pathway over the prepared Zn-Fe double oxides. This work provided new insights and comprehension into modulating radical and nonradical pathways of PMS-based advanced oxidation process for refractory contaminant oxidation via utilizing solar energy.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2022
·
IF 10.753
Jie Wang,Haibao Liu,Yue Gao,Qinyan Yue,Baoyu Gao,Bo Liu,Kangying Guo,Xing Xu
Advanced oxidation processes (AOPs) such as ozonation and Fenton processes are widely used in the treatment of high-salt wastewater. The UV/O 3 pressurization process was designed and applied at the pilot-scale for treatment of actual high-salt textile wastewater. The UV/O 3 pressurization process achieved the highest decolorization (85 %) and chemical oxygen demand (COD Cr , 43.2 %) removal efficiency at an O 3 dosage of 200 g·t −1 and a pressure of 0.2 MPa. Compared to ordinary ozonation, the UV/O 3 pressurization process improved the solubility and gas-liquid mass transfer efficiency of O 3 in wastewater and generated a large number of O 3 microbubbles. Hydroxyl radical (·OH), superoxide radicals (O 2 · − ) and single oxygen ( 1 O 2 ) all played a significant role on the removal of pollutants in wastewater during the UV/O 3 pressurization process. The reverse osmosis (RO) process was used to evaluate the effect of UV/O 3 pressurization and Fenton pre-oxidation processes on the desalination process as the last process in treating high-salt organic wastewater. The pre-oxidation processes improved the initial RO water flux . Compared with the Fenton process, the UV/O 3 pressurization process had less membrane fouling (thin fouling layer vs thick fouling layer), and final water flux (59.4 LMH) was higher than that of Fenton process (34.9 LHM). The total dissolved solids (TDS), Cl − and SO 4 2− of the effluent from UV/O 3 pressurization process (37.2, 7.6 and 3.0 mg·L −1 ) were better than that of Fenton process (65.7, 13.9 and 7.1 mg·L −1 ). Therefore, the UV/O 3 pressurization process without secondary pollution is more suitable for the advanced treatment of high-salt organic wastewater than the Fenton process.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Sheng Guo,Meng Chen,Liming You,Yu Wei,Chao Cai,Qingsong Wei,Huali Zhang,Kun Zhou
Three-dimensional (3D) printing has demonstrated great potential in wastewater purification. Herein, a facile 3D printing strategy is utilized to prepare zero-valent copper (3D-ZVC). The obtained 3D-ZVC framework displays a hierarchically porous structure and a rough surface, which correspond to excellent mechanical robustness and catalytic performance in degrading multiple organic pollutants through peroxymonosulfate (PMS) activation. The 3D-ZVC/PMS/Vis system is capable of achieving a tetracycline (TC) degradation efficiency of over 96.5 % within 20 min, which greatly exceeds that of homogeneous Cu 2+ /PMS/Vis and contemporary powder/PMS/Vis systems as a result of the unique hierarchical porous structure and cycling of Cu(I)/Cu(II) in 3D-ZVC. Furthermore, the 3D-ZVC/PMS/Vis system exhibits a broad pH resistance range (3.21–10.18), spectacular adaptability, unparalleled stability, and excellent reusability after 23 successive cycles. Electrons and various reactive oxygen species, including SO 4 − , OH, O 2 − , and 1 O 2 , are all involved in the decomposition of TC, with 1 O 2 playing a dominant role. The influence parameters and possible intermediates of the 3D-ZVC/PMS/Vis system are investigated. Toxicity estimation analysis indicates that the toxicity of TC degradation products has been significantly reduced, which is further confirmed through growth control experiments of bean sprouts. This study highlights a prospective and feasible application of 3D printing in environmental remediation through PMS activation.
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Reaction Kinetics Mechanisms and Catalysis
·
2022
·Vol. 135
·期 6
·3331-3342
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IF 1.843
Zhang Ning,Zheng Yu,Li Jianfeng,Du Zhiping,Cheng Fangqin
A reduced graphene oxide-P25 (rGO-P25) composite was synthesized by one-step hydrothermal method. The photocatalytic degradation of Rhodamine B (RhB) by the rGO-P25 composite and its settling performance was investigated with P25 as a control. The results showed that the rGO-P25 composite has a mesoporous structure, with the average particle size increased from 4.99 to 399.0 µm, and the specific surface area of the composite increased from 54.0 to 74.3 m 2 /g. The rGO-P25 composite has a much better photocatalytic and settling performance as compared to P25, which were 1.56 and 2.4 times higher. The increased photocatalytic performance by the rGO-P25 composite was mainly attributed to the increased adsorption capacity and charge transfer ability due to the introduction of rGO flakes in the composite. However, the improved settling performance mainly lies on the increase of the average particle size. The electron spin resonance (ESR) results shows that hydroxyl radical, superoxide radical and photogenerated hole were all generated in the degradation of RhB but the hydroxyl radicals are the leading reactive oxygen species. The as-synthesized rGO-P25 composite showed a good recycling ability as RhB degradation rate could still reach 98.6% after five times reuse. This study indicates that the rGO-P25 composite is a promising photocatalyst for practical wastewater treatment. Graphical abstract
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Jinyu Gu,Jinxin Xie,Shasha Li,Ge Song,Minghua Zhou
The oxygen-doped carbon nanotubes coated on the carbon felt acted as cathode to enhance the electro-peroxone (OCNT-EP) process. Owing to the introduction of oxygen-containing functional groups and defect sites, the OCNT modified cathode could achieve in-situ H 2 O 2 generation, activation, and catalytic ozonation in the EP process. The OCNT-EP showed a 2.3-folds apparent first-order rate constant ( k ) compared with the EP process using CNT cathode (CNT-EP) for atrazine (ATZ) degradation. According to the processes comparison, quenching experiments, electron paramagnetic resonance (EPR) analysis and determination of hydroxyl radical, it was proved that more . OH and 1 O 2 were generated by the in-situ H 2 O 2 activation and catalytic ozonation in the OCNT-EP process. Especially, this process improved pollutants degradation under acidic condition for the in-situ H 2 O 2 activation and catalytic ozonation, expanding the pH application range of the EP process with a lower energy consumption (0.10 kWh/g ATZ). What’ more, the OCNT modified cathode performed excellent stability with 20 cycle tests, and demonstrated all improved degradation rate (21.7%−78.0%) for various pollutants (carbamazepine, sulfamethazine, phenol and 2,4-dichlorophenol). Therefore, the OCNT-EP process could be considered as a promising and enhanced EP process for wastewater treatment.
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Journal of Cleaner Production
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2022
·
IF 11.072
Hua Chai,Chunyan Yang,Peng Xu,Peng Wang,Jianhua Qu,Guangshan Zhang
Heterojunction photocatalysts Fe 2 O 3 –ZnO@C/g-C 3 N 4 (FZCCN) were prepared by precipitation and calcination in this study. Systematic characterization demonstrated that the tight interfacial contact was established between Fe 2 O 3 –ZnO@C and g-C 3 N 4 , and the FZCCN-4 (theoretical mass ratios of ZnO and g-C 3 N 4 was 4) had large BET surface area (110.136 m 2 g −1 ). Bisphenol A (BPA) was selected to estimate the photocatalytic properties of FZCCN and the degradation reaction kinetics was analyzed at the same time. The results showed that, FZCCN-4 had the highest removal rate of BPA (100%, 60 min). The degradation rate of BPA by using FZCCN-4 was approximately 32 and 130 times higher than that of g-C 3 N 4 and Fe 2 O 3 –ZnO@C, respectively. ·O 2 − was proved to be the main active species by capture experiment and electron spin resonance. The UV–vis and PL results proved the formation of heterojunction in FZCCN. This study also identified the intermediates of BPA degradation and tested their toxicity. The excellent visible light catalytic performance of Fe 2 O 3 –ZnO@C/g-C 3 N 4 makes it an ideal material for degrading contaminants.
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WATER RESEARCH
·
2022
·
IF 13.4
Xiwen Liu,Penghui Shao,Shanshan Gao,Zhaoyu Bai,Jiayu Tian
Benzoquinone (BQ) is of great significance for enhancement of contaminants degradation in the homogeneous oxidation system of peroxymonosulfate (PMS). However, the role of BQ in the heterogeneous activation of PMS for contaminants oxidation is still not clear. Herein, this work reported that the addition of BQ into the Fe 3 S 4 /PMS system could effectively enhance the degradation and mineralization of bisphenol A (BPA). Mechanistic study uncovered that the BQ and PMS would form active complexes (BQ-PMS*) on the surface of Fe 3 S 4 and the excited BQ-PMS* can oxidize the BPA. To be specific, the electron of BPA was extracted by BQ-PMS* and then transfer to the surface of Fe 3 S 4 . The surface electron can induce the change of valence state of S and Fe elements, which can trigger the degradation of BPA and inhibit the decomposition of BQ itself. To the best of our knowledge, it is the first time to unveil the positive role of BQ in the heterogeneous activation of PMS, which may shed new light on the establishment of high-efficient PMS-based oxidation technology for remediation of organic pollutant.
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NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 38
·18251-18261
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IF 3.925
Jiabao Sun,Qiang Li,Dajie Zhang,Dongsheng Xia
Oxytetracycline (OTC) is a typical antibiotic that poses a serious threat to the environment. However, traditional treatment methods suffer from low treatment efficiencies and potential secondary contamination. Therefore, there is a need to develop efficient, convenient, and environmentally friendly removal technology. In this paper, magnetic nano-Cu/Fe composites were successfully synthesized and used as the activator of peroxymonosulfate (PMS) to degrade OTC. The obtained catalysts with different ratios showed excellent degradation effects, especially the Cu/Fe-1 catalysts. The highest removal efficiency of OTC (93%) was achieved with 0.2 g L−1 PMS and 0.1 g L−1 catalyst in 60 min. The impacts of the catalyst and PMS dosages, initial temperature and pH, coexisting anions, microplastics, and real-life water samples were investigated. To explore the mechanism for OTC degradation, radical scavenging and electron spin resonance (EPR) experiments were carried out, and non-radical 1O2 was identified to be the main radical. TEM and XRD results show the presence of CuFe2O4 composites in Cu/Fe-1, which can promote the production of 1O2 and thus improve the OTC degradation efficiency. This work provides a new efficient, stable, low-cost, and environmentally friendly approach for the degradation of oxytetracycline.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Lu-Lu Wang,Shun-Feng Jiang,Jing Huang,Hong Jiang
Oxygen-containing functional groups in functionalized biochar (BC) play an important role in its environmental applications. Herein, we introduced oxygen atoms into BC by copyrolysis of sawdust and magnesium carbonate basic pentahydrate (MgCO 3 ) 4 ·Mg(OH) 2 ·5 H 2 O for the preparation of O-enriched porous BC (OPBC). OPBC800 (OPBC pyrolyzed at 800 °C) exhibited ultrahigh activity to activate ferrate (K 2 FeO 4 ) for the oxidation of sulfadiazine (SDZ, 100% removal of SDZ in 2 min at pH = 5). We found that SDZ molecules can be rapidly adsorbed by the hierarchical porous structure of OPBC and were expediently oxidized by in situ generated Fe(IV) and Fe(V) active species on the surface of OPBC. The degradation mechanism of SDZ involved is quite different from the well-confirmed mechanism in which only active species in the solution play a role. Electrochemical impedance spectroscopy showed that O-doping in OPBC improved the electron-donating ability and expedited the electron transfer to ferrate, thus enhancing the catalytic activity of OPBC. This provides a new functionalization method for BC and provides more information about the activation of ferrate.
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CHEMOSPHERE
·
2022
·
IF 8.943
Shule Duan,Huiyu Dong,Pin Hou,Gangsheng Han,Bochao Zhang,Zhimin Qiang
Permanganate (Mn(VII)) is a widely used oxidant in water treatment , which can oxidize trace organic contaminants (TrOCs) and Mn(II). Interestingly, this study found that presence of Mn(II) could accelerate the abatement of bisphenol A by Mn(VII) only under oxic condition . Herein, the effects of Mn(II) and dissolved oxygen (DO) on the abatement of TrOCs by Mn(VII) oxidation and the related mechanism were investigated. Results indicate that DO was involved in the Mn(VII)/Mn(II) reaction, with the reaction stoichiometry of Δ[Mn(VII)]:Δ[Mn(II)] determined to be 1:2 and 1:1.5 in the presence and absence of DO, respectively. Quenching and electron paramagnetic resonance tests verified that both superoxide radicals (O 2 •− ) and reactive Mn species contributed to the accelerated abatement of TrOCs (bisphenol A, methyl phenyl sulfoxide, and methyl phenyl sulfone) in the Mn(VII)/Mn(II) process. Specifically, O 2 •− was produced through the one-electron reduction of DO and made an important contribution (32.4%–100%) to the abatement of selected TrOCs. This study reveals that Mn(II) could enhance TrOC abatement by Mn(VII) oxidation, and DO played a pivotal role in the Mn(VII)/Mn(II) process.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Xinfa Cai,Fei Ma,Jun Jiang,Xianglong Yang,Zhaowei Zhang,Zelang Jian,Meijuan Liang,Peiwu Li,Li Yu
Sensitive, on-site and multiple detection of mycotoxins is a vital early-warning tool to minimize food losses and protect human health and the environment. Although paper-based lateral flow immunoassay (LFIA) has been extensively applied in mycotoxins monitoring, low-cost, portable, ultrasensitive and quantitative detection is still a formidable challenge. Herein, a series of Fe-N-C single-atom nanozymes (SAzymes) were synthesized and systematic characterized. The optimal Fe-N-C SAzyme with highly efficient catalytic performance was successfully used as both label and catalyst in lateral flow immunoassays for mycotoxin detection. By taking advantage of the catalytic amplified system, the qualitative and quantitative detection can be easily and flexibly done via observing the test lines by naked eyes or a smartphone, with the limit of detections (LODs) of 2.8 and 13.9 pg mL −1 for AFB 1 and FB 1 , which were respectively over 700- and 71,000-fold lower than the maximum limit set by the European Union. Besides, underlying catalytic mechanisms and the active sites of the Fe-N-C SAzyme are also investigated by DFT simulation. This work not only provides a promising detection strategy for the application of advanced SAzymes but also offers experimental and theoretical guidelines to understand the active centers of Fe-N-C SAzymes and the catalytic process.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yi Su,Qizhan Zhang,Ge Song,Wenyang Fu,Minghua Zhou,Ying Zhang
A novel continuous-flow H 2 O 2 electrochemical generator using a natural air diffusion electrode (NADE) as the cathode was designed and the two compartments of the generator were separated by a cation exchange membrane. The reactor did not require aeration, which saved aeration energy consumption. The reactor showed good performance in generating H 2 O 2 up to 50.8 mg/h/cm 2 with the energy consumption of 25.2 kWh/kg H 2 O 2 , and maintained a high current efficiency of about 70–94% in the current density range of 20 to 100 mA/cm 2 . The yield of H 2 O 2 and current efficiency remained high and stable in a wide pH range of 3 ∼ 9. H 2 O 2 produced in the generator was delivered to a flow-Fenton reactor for the occurrence of the Fenton reaction and the degradation of sulfamethazine (SMT), which avoided the problem of excessive generation and ineffective consumption of H 2 O 2 in the electro-Fenton process and improved the utilization rate of H 2 O 2 . Moreover, due to the introduction of H 2 O 2 solution with low pH to the flow-Fenton reactor, the pH of the working solution did not need adjustment. The flow-Fenton process achieved 99% of SMT removal, 90% of H 2 O 2 utilization rate, and 54% of TOC removal within 20 min under the optimum conditions. The degradation of several other contaminants (2,4-dichlorophenoxyacetic acid, tetracycline and carbamazepine) was investigated and all of the removals were maintained above 97%. The study is promising for the practical electrochemical production of H 2 O 2 and application of flow-Fenton for contaminants degradation.
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