CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Meiyun Feng,Zhiqiang Xu,Xue Bai,Kuangfei Lin,Meng Zhang
In this study, the morphology and surface characteristics of different M x Mn 3-x O 4 (M = Co, Zn, Cu, Fe; x = 1, 2) nanoparticles and their catalytic performance for peroxymonosulfate (PMS) activation to degrade trichloroethylene (TCE) were compared. The characterization results showed that a highly crystalline manganese structure was synthesized, and cubic spinel (M 2 MnO 4 ) and tetragonal spinel (MMn 2 O 4 ) were confirmed. The experimental results indicated that, compared with the tetragonal spinel catalysts, the cubic spinel catalysts exhibited higher PMS-specific catalytic activity and TCE removal efficiency due to the reduction in electron transfer resistance and the increase of the surface area. In addition, all the synthesized nanoparticles exhibited remarkable reusability, a low metal dissolution rate, and a wide applicable pH range (4 to 11) for efficient PMS activation . The free radical-scavenging experiments and electron paramagnetic resonance (EPR) analysis further verified the role of ∙HO and SO 4 ∙− in the removal of TCE and the large amount of stronger free radicals (SO 4 ∙− ) generated by the cubic spinels. This study revealed that stable cubic spinel nanoparticles can be synthesized at room temperature by adjusting the ratio of manganese and transition metals; these nanoparticles showed excellent catalytic performance for PMS activation. These research results are important for the synthesis of heterogeneous catalytic oxidation catalysts.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
·
IF 11.357
Mei-Mei Wang,Li-Juan Liu,Jia-Tai Wen,Ying Ding,Jia-Rui Xi,Jia-Cheng Li,Fang-Zheng Lu,Wei-Kang Wang,Juan Xu
In situ growth of nanostructures on substrates is a strategy for designing highly efficient catalytic materials. Herein, multimetallic CuCoNi oxide nanowires are synthesized in situ on a three-dimensional nickel foam (NF) substrate (CuCoNi–NF) by a hydrothermal method and applied to peroxydisulfate (PDS) activation as immobilized catalysts. The catalytic performance of CuCoNi–NF is evaluated through the degradation of organic pollutants such as bisphenol A (BPA) and practical wastewater. The results indicate that the NF not only plays an important role as the substrate support but also serves as an internal Ni source for material fabrication. CuCoNi–NF exhibits high activity and stability during PDS activation as it mediates electron transfer from BPA to PDS. CuCoNi–NF first donates electrons to PDS to arrive at an oxidized state and subsequently deprives electrons from BPA to return to the initial state. CuCoNi–NF maintains high catalytic activity in the pH range of 5.2–9.2, adapts to a high ionic strength up to 100 mM, and resists background HCO3– and humic acid. Meanwhile, 76.6% of the total organic carbon can be removed from packaging wastewater by CuCoNi–NF-catalyzed PDS activation. This immobilized catalyst shows promising potential in wastewater treatment, well addressing the separation and recovery of conventional powdered catalysts.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yu Chen,Xianhu Long,Rongfu Huang,Igor Ying Zhang,Gang Yao,Bo Lai,Zhaokun Xiong
In this study, an electrochemical/peroxymonosulfate/Fe(III) (EC/PMS/Fe(III)) system was established for efficient degradation of four naphthenic acids (NAs) compounds including cyclohexanecarboxylic (CHA), heptanoic (HPA), benzoic (BA) and 2-methylhexanoic acids (2-MHA). The introduction of electric field enhances the redox cycle of Fe(III)/Fe(II) to activate PMS for degredation of NAs. Complete degradation of NAs compounds (5 mg/L) has been achieved within 30 min in the EC/PMS/Fe(III) system. The results of electron paramagnetic resonance (EPR) analysis, scavenging experiment, and chemical probe experiments indicated hydroxyl radical ( • OH), sulfate radical (SO 4 •− ) and singlet oxygen ( 1 O 2 ) are primary reactive oxygen species (ROS) in the EC/PMS/Fe(III) system. NAs compounds with different structures exhibit inconsistent degradation efficiency in current system ( k CHA > k BA > k HPA > k 2-MHA ), depending on the selectivity of the different ROS and stability of respective intermediate organic radicals. Besides, multiple degradation pathways of CHA, mainly including hydroxylation and carbonylation , were proposed by combining the results of mass spectrometry analysis with the calculated Fukui index based on density functional theory (DFT) calculation. In addition, the EC/PMS/Fe(III) system exhibited robust performance with the addition of co-existing ions. This work provides a novel strategy for efficient degradation of NAs for future remediation of petroleum wastewater.
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CHEMICAL ENGINEERING JOURNAL
·
2022
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IF 16.744
Yiming Sun,Peng Zhou,Peng Zhang,Shuang Meng,Chenying Zhou,Yang Liu,Heng Zhang,Zhaokun Xiong,Xiaoguang Duan,Bo Lai
Fenton reaction is most important in advanced oxidation processes, however, the sluggish kinetics of H 2 O 2 induced Fe(II) regeneration relatively limits the hydroxyl radicals generation. This study finds that carbon catalysis is a green and sustainable strategy to boost the Fenton chemistry and provides a new insight to carbon mediated Fe(III)/Fe(II) cycles. Multilayer graphene (MG), as a typical carbon material, can significantly enhance the Fe(III)/H 2 O 2 system to produce hydroxyl radicals. Unlike the classical electron sacrifices, MG can enhance the Fe-O bond of FeOH 2+ and Fe(III) oxidation potential, thus MG can further mediate and accelerate Fe(III) induced H 2 O 2 oxidation to produce Fe(II) and initiate Fenton chain reactions. Kinetics model results reveal that the reaction rate constant between Fe(III) and H 2 O 2 on MG surface is at least 100 times higher than that in aqueous solution. Therefore, carbon catalysis can overcome the speed-limiting process of Fenton system by elevating Fe(III) reactivity at acidic conditions.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 30
·期 1
·1386-1398
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IF 5.19
Yan Shiquan,Lai Xinting,Fan Lingling,Wang Tianhao,Yao Yuyuan,Wang Wentao
Wastewater containing organic pollutants with high toxicity and poor biodegradability poses a considerable threat to human health and the ecosystem. Although adsorption and advanced oxidation processes (AOPs) are currently the most widely used technologies for wastewater treatment, limitations of these two independent processes make the treatment effect unsatisfactory. Herein, a system of integrating adsorption and subsequent in situ AOPs is established by a 3D carbon aerogel embedded with Fe-doped carbonitrides (Fe-NC/CAG). The SEM and BET analysis demonstrate that Fe-NC/CAG possesses porous structures with a specific surface area of 518.7 m 2 /g. The XRD result indicates the formation of Fe 0 and Fe 3 O 4 in Fe-NC/CAG. The impacts of operational parameters such as Fe-NC/CAG dosage, pollutants concentration, temperature, initial pH, and inorganic ions on the adsorption efficiency are investigated. The adsorption kinetics is predominantly based on the pseudo-second-order model. After adsorbing organic pollutants, the Fe-NC/CAG is immersed in peroxymonosulfate (PMS) solution. The adsorbed pollutants are in situ degraded by PMS-based AOPs, leading to the regeneration of Fe-NC/CAG. At optimum conditions, the integrating process established by Fe-NC/CAG achieves over 90% removal of antibiotics, phenolics, and dyes as well as keeps stable performance even after 6 cycles. This integrating adsorption and AOPs system is expected to open up a rich field for wastewater treatment.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Jia Xie,Yingpeng Yang,Hao Zhang,Saisai Chen,Zhengjun Lv,Yujun Zhou,Junwen Qi,Xiuyun Sun,Jiansheng Li
Advanced oxidation processes (AOPs) were appealing wastewater treatment options yet practices were hampered by reactor design and diminished performance in complex water matrices. Herein, one-step-pyrolysis strategy was proposed for large-scale synthesis of ZIF-67 derived conductive Co/N carbon hollow fiber ultrafiltration membrane to achieve exceptional availability of catalytic sites and interference prevention from macro molecular substances by size exclusion. Benefitting from the microenvironment modulation and electric field assistance (−1 V, membrane as the cathode), the bisphenol A (as a model micropollutant) can be efficiently removed with enhanced mass transfer of flow-through process (modified apparent reaction rate constant of 1260 μM g cat -1 s −1 ) and the active cobalt species were cycled via electroreduction thus showing exceptional sustainability with nearly zero Co leaching even after 24 h operation. The synergy effects between separation and catalysis alleviated the deteriorated AOPs efficiency and membrane fouling caused by macromolecular organic matter. The integrated membrane system provides new insight into rational design of catalytic membrane and system engineering for advanced water purification.
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Nano Research
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2022
·Vol. 16
·期 5
·6057-6066
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IF 10.269
Zhao Man,Cheng Xiaoru,Xiao He,Gao Jianru,Xue Shoufeng,Wang Xiaoxia,Wu Haishun,Jia Jianfeng,Yang Nianjun
Highly active, stable, and cut-price (photo-)electrocatalysts are desired to overwhelm high energy barriers for anodic oxygen evolution reaction processes. Herein, a heterostructure of cobalt-iron oxide/black phosphorus nanosheets is in-situ synthesized via a facile and novel three-electrode electrolysis method. Bulky black phosphorus is exfoliated into its nanosheets at the cathode while the CoFe oxide is derived directly from the metal wire anode during the electrolysis process. This heterostructure exhibits excellent electrocatalytic oxygen evolution reaction (OER) performance, and the overpotential at 10 mA·cm −2 is 51 mV lower than that of the commercial RuO 2 catalyst. Its superior OER performance stems from the favorable adsorption behavior and an enlarged electrochemical active surface area of the catalyst. To reveal the origin of excellent OER performance from the point of adsorption strength of OH*, methanol oxidation reaction (MOR) test is applied under the identified OER operating conditions. Further introduction of light illumination enhances the OER activity of this heterostructure. The overpotential drops down to 280 mV, benefiting from pronounced photochemical response of black phosphorus nanosheets and iron oxide inside the heterostructure. This work develops a new electrochemical method to construct high performance and light-sensitive heterostructures from black phosphorus nanosheets for the OER.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Mingzhe Li,Wenli Yao,Min Yu,Changduo Sun,Xinquan Deng,Fengjuan Chen,Lei Zhou,Yian Zheng
Hydrogels possess 3D network with abundant reactive groups, and can bind with active metal ions within their confined 3D structure for fabricating functional materials . In this study, a chitosan grafted polyacrylic acid (CTS-g-PAA) hydrogel was prepared for loading Fe 2+ , which was then converted into magnetic Fe@C via subsequent pyrolysis process . In Fe@C activated peroxymonosulfate (PMS) (Fe@C/PMS) system, the degradation behaviors of ciprofloxacin (CIP) were systematically investigated, including influencing parameters, reactive oxygen species (ROSs), degradation mechanism and potential eco-toxicity of degradation intermediates. The results showed that CTS-g-PAA supported, in-situ derived magnetic Fe@C had not only stable catalytic ability at pH 3.0–9.0, but also high degradation efficiency in the presence of inorganic Cl − and HCO 3 − (5–20 mM) as well as organic humid acid (10 and 20 mg/L). Under the optimized conditions, the degradation efficiency of CIP could reach to 96.84 % within 1 h. In Fe@C/PMS system, the main ROSs involved free radicals SO 4 •− , •OH, O 2 •− and non-free radical 1 O 2 . Through free radical quantitative experiments, the concentration of SO 4 •− and •OH at 60 min was determined respectively to be 11.84 µM and 0.14 µM, proving the dominant role of SO 4 •− . By HPLC-MS analysis, the degradation products were proposed via four degradation pathways, including hydroxylation, defluorination and decarboxylation, as well as the ring opening of quinolone and piperazine. Finally, the potential eco-toxicity of CIP and its degradation intermediates was evaluated by using ECOSAR method based on quantitative structure–activity relationships analysis.
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Journal of Environmental Sciences
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2022
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IF 6.796
Xuedong Du,Wenyang Fu,Pei Su,Qizhan Zhang,Minghua Zhou
An ultra-efficient electro-Fenton catalyst with porous carbon coated Fe-Mo metal (FeMo@PC), was prepared by calcining MIL-53(Fe)@MoO 3 . This FeMo@PC-2 exhibited impressive catalytic performance for sulfamethazine (SMT) degradation with a high turnover frequency value (7.89 L/(g·min)), much better than most of reported catalysts. The mineralization current efficiency and electric energy consumption were 83.2% and 0.03 kWh/g TOC , respectively, at low current (5 mA) and small dosage of catalyst (25.0 mg/L). The removal rate of heterogeneous electro-Fenton (Hetero-EF) process catalyzed by FeMo@PC-2 was 4.58 times that of Fe@PC/Hetero-EF process. Because the internal-micro-electrolysis occurred between PC and Fe 0 , while the co-catalysis of Mo accelerated the rate-limiting step of the Fe 3+ /Fe 2+ cycle and greatly improved the H 2 O 2 utilization efficiency. The results of radical scavenger experiments and electron paramagnetic resonance confirmed the main role of surface-bound hydroxyl radical oxidation. This process was feasible to remove diverse organic contaminants such as phenol, 2,4-dichlorophenoxyacetic acid, carbamazepine and SMT. This paper enlightened the importance of the doped Mo, which could greatly improve the activity of the iron-carbon heterogeneous catalyst derived from metal-organic frameworks in EF process for efficient removal of organic contaminants.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Hongji Li,Dandan Wang,Chun Miao,Fengwu xia,Yubo Wang,Yutong Wang,Chunbo Liu,Guangbo Che
Photo-degradation of pollutant and photo-reduction of CO 2 are efficient ways to address challenges of water pollution , the greenhouse effect and energy crisis, respectively. In our work, via fastening two-dimensional (2D) BiOI nanoplates on 2D g-C 3 N 4 nanosheets , a BiOI/g-C 3 N 4 (BI/CN) S-scheme photocatalyst with closely stacked structure were prepared though a self-assembly process. The prepared BI/CN S-scheme heterojunction could improve the transfer and separation efficiency of photo-generated electron-hole pairs by facilitating the electrons transfer from BiOI to g-C 3 N 4 . Under visible light exposure, the photo-degradation efficiencies of tetracycline hydrochloride (TC) and p-chlorophenol (4-PC) by BI/CN-50% reached nearly 100% and 46%, respectively, which were more excellent in comparison with other samples. And BI/CN-50% sample exhibited the best CO production (12.45 μmol∙g −1 ) with visible-light irradiation of 4 h. This value was approximately 4.37 and 5.41 times higher than that of BI (2.85 μmol∙g −1 ) and CN materials (2.30 μmol∙g −1 ), respectively. Moreover, the excellent photocatalytic performance had no visible decay during five cycles. Meanwhile, an S-scheme charge transfer process was confirmed by species trapping experiments and electron spin-trap analysis. This study offers new insights into the activity, kinetics, and mechanism over BiOI-based materials for photocatalysis technology .
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Huihui Zhang,Sisi Xiao,Yansheng Du,Shilin Song,Kun Hu,Yuyue Huang,Huijuan Wang,Qiangshun Wu
Herein, dielectric barrier discharge (DBD) plasma and MnO 2 -cellulose acetate (MnO 2 /CA) composite films was coupled together to degrade sulfamethoxazole (SMX) in water. The MnO 2 /CA composite films were firstly prepared successfully though heating blending method in this study and then characterized by scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), Raman spectra, X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR) and thermogravimetric analysis (TG). Catalytic effect of the MnO 2 /CA films was investigated by comparing the removal percentages, the kinetic constants, the energy utilization efficiencies ( G 50 ) as well as the COD and TOC removal during the SMX degradation in the DBD plasma system with or without the MnO 2 /CA films addition under different reaction conditions. The optimal catalytic performance was obtained by adding the 3% MnO 2 /CA films into the DBD plasma system and the alkaline solution condition was favorable for the SMX degradation. After four times using, the MnO 2 /CA composite films still maintained the catalytic activity. Catalytic mechanism of the MnO 2 /CA films was speculated by analyzing the changes of solution pH and conductivity during the reaction, concentrations of the formed O 3 and H 2 O 2 in water and the generated active species ( 1 O 2 and ·OH) in both the DBD plasma system and the DBD-MnO 2 /CA films system. The quenching test was also carried out to figure out the important effect of the ·O 2 − , 1 O 2 and ·OH for the SMX degradation in the synergistic system. Finally, LC-MS was used to analyze the main intermediates generated during the SMX degradation and the possible degradation pathways were accordingly speculated. The research could provide a new direction for the development and application of the DBD plasma technology as well we the composite films catalyst.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Jiao Shen,Feng Cheng,Yichi Chen,Zeyu Li,Yang Liu,Yue Yuan,Peng Zhou,Wen Liu,Bo Lai,Yongli Zhang
In this study, vanadium trioxide (V 2 O 3 ) was adopted to activate PMS via a Fenton-like reaction to degrade metronidazole (MNZ). The V 2 O 3 -PMS system can almost completely degrade MNZ at 30 min with 42.4% TOC removal. Comparative tests reveal that V 2 O 3 stands out among a variety of heterogeneous catalysts, including metallic oxides and carbon materials. Sulfate radicals (SO 4 •− ) and hydroxyl radicals ( • OH) derived from PMS decomposition are major reactive oxygen species, based on quenching tests, electron spin resonance (ESR) analysis, the steady-state concentrations of radicals ([SO 4 •− ] ss = 5.1 × 10 -13 M and [ • OH] ss = 4.0 × 10 -14 M), and kinetics model. The process of stepwise electron transfer from vanadium species to PMS to produce reactive radicals was proved by small-molecule simulation experiments and pickling experiments of vanadium oxides. Possible pathways of MNZ degradation were proposed based on the results of LC-MS and Fukui function, including two stages of the hydroxylation and bond cleavage of nitro and the subsequent ring-opening. This study reveals the high reusability and practicability of the V 2 O 3 -PMS system over a relatively wide pH range, which puts forward a new vision on V 2 O 3 induced Fenton-like reactions and a new reference method for the removal of medical organic contaminants in water.
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