Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Lijun Guo,Liming Zhao,Yuling Tang,Jianfei Zhou,Bi Shi
The magnetic biochar catalyst (Fe@BC) was synthesized by pyrolyzing Fe–tanned collagen fiber based on the tanning process and used as a high–efficiency and recyclable persulfate (PS) activator to degrade refractory dyes. In this study, methylene blue (MB) was chosen as a model pollutant to evaluate the performance of the Fe@BC/PS system. Results illustrated that MB was completely removed within 20 min with a rate constant (k obs ) of 0.2246 min – 1 , which was much higher than that of pure biochar (0.0497 min – 1 ), and high mineralization efficiency (92%) for MB degradation was obtained. Notably, the MB removal rate still reached 72% after 20 cycles. The high catalytic activity and excellent recycling performance could be attributed to the uniformly dispersed iron species, abundant oxygen functional groups, and defective carbon matrix. Radical quenching experiments and electron paramagnetic resonance studies illustrated that SO 4 •– was the predominant free radical for MB degradation. Moreover, other refractory dyes could also be rapidly and efficiently removed from the Fe@BC/PS system. This work is expected to propose a promising catalyst for the degradation of refractory dyes and open a new possibility for the durable removal of refractory organic dyes.
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CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Yuxuan He,Jin Qian,Peifang Wang,Jie Wu,Bianhe Lu,Sijing Tang,Pan Gao
The nanocomposite of MoS 2 embedded manganese ferrite doped perovskite (SrCoO 3 /MnFe 2 O 4 /MoS 2 , abbreviated as SMM) was successfully synthesized for peroxymonosulfate (PMS) activation under visible-light. It was optimized that the SMM-3 (mass ratio of MoS 2 modified nanocomposite was 0.3) exhibited excellent catalytic performance to activate PMS for levofloxacin (LVF) degradation, with the degradation efficiency of 95.1% in 20 min. Besides, SMM-3 was able to efficiently degrade LVF under real water matrix. The quenching experiments and electron paramagnetic resonance (EPR) analysis revealed that SO 4 •- and HO • played a dominant role in reaction. Due to the photocatalytic property of nanocomposites, the visible light could excite electrons to react with oxygen and form O 2 •- , which further reacted with HO • to produce 1 O 2 . In the reaction process, the rapid redox cycle of metal ions (including Co, Mn, Fe and Mo) boosted the activation of PMS and promoted the degradation of LVF in a short time. The Density functional theory (DFT) calculation and LC-MS/MS further revealed that oxidation of piperazine ring, decarboxylation and defluorination processes were the main LVF degradation pathways. Finally, the toxicity analysis based on Toxicity Estimation Software Tool (T.E.S.T) verified the ecological risks of transformation residues.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Yuxuan He,Jin Qian,Bin Xu,Peifang Wang,Bianhe Lu,Sijing Tang,Pan Gao
Perovskite oxides and molybdenum sulfide (MoS 2 ) are both promising catalysts for advanced oxidation processes in environmental pollutant degradation. Herein, a core-shell structure of MoS 2 encapsulating Sr-Co perovskite microcrystalline (SC@MoS 2 ) was used to activate peroxymonosulfate (PMS) for degradation of organics. Levofloxacin (LVF) degradation by SC@MoS 2 /PMS system was improved obviously, and 0.2-SC@MoS 2 exhibited the optimized activation for PMS with best LVF degradation performance (97%) within 15 min. In the 0.2-SC@MoS 2 /PMS system, the dosage of catalyst was the key determinant of LVF degradation. Simultaneously, 0.2-SC@MoS 2 achieved outstanding reusability and good degradation capacity of different contaminants. The encapsulation of molybdenum disulfide layer facilitated electron transfer between PMS and core-shell structure. According to the EPR analysis and quenching experiments, both radicals (SO 4 − and OH), and nonradical ( 1 O 2 ) were involved in the degradation of LVF. Under visible light irradiation, O 2 − participated in the reaction and enhanced LVF degradation efficiency, because the valence band and conduction band of components are different. Furthermore, the density functional theory (DFT) calculation, intermediates determination and Toxicity Estimation Software Tool (T.E.S.T) analysis provided meaningful support in the degradation pathways and ecological risks of LVF residues.
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ACS ES&T Engineering
·
2021
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IF 0
Shenyu Lan,Chuan Yu,Enya Wu,Mingshan Zhu,Dionysios D. Dionysiou
Ambient water motions presented in urban drainage systems is a rich source of renewable mechanical energy. Harvesting this energy to trigger the generation of reactive oxygen species (ROS) for water purification is a desirable yet underexplored solution. Herein, the water flow from a spiral reactor to simulate pipeline drainage was utilized to provide mechanical energy to power itself to initiate the piezo-response of molybdenum disulfide (MoS2) that was added into water flowing in the reactor. The piezocatalytic degradation efficiency of benzothiazole by MoS2 reached 94.8% after 24 cycles (ca. 144 s), which was 8.8 and 4.9 times higher than that of quiescent solution of MoS2 and non-piezoelectric commercial MoS2, respectively. Furthermore, the water flow-driven system can be extended to degrade different kinds of organic contaminants, including benzotriazole and various antibiotics (enrofloxacin, ciprofloxacin, metronidazole, etc.). All target pollutants were degraded with electric energy per order EEO in the range of 0.0161 to 0.0616 kW h/m3. In this process, the running water from the spiral reactor drove MoS2 to generate piezoelectric charges, which in turn reacted with dissolved oxygen and water to generate ROS including the hydroxyl radical, superoxide anion, and singlet oxygen to decompose the target pollutants. The system retained piezo-degradation efficiencies (>80%) in different aqueous matrices including rainwater, saline water, and pharmaceutical sewage and could be reused four times maintaining a good performance (>90%). This investigation provides a facile self-powered piezocatalytic process by harnessing ambient energy from the water flow of simulated water drainage to purify wastewater.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Xu Shi,Peidong Hong,Hongqi Huang,Dandan Yang,Kaisheng Zhang,Junyong He,Yulian Li,Zijian Wu,Chao Xie,Jinhuai Liu,Lingtao Kong
Fenton-like catalysts have usually superior catalytic activities, however, some drawbacks of ion leaching and difficult-to-recovery limit their applications. In this work, a hierarchical porous Fe 3 O 4 /Co 3 S 4 catalyst was fabricated via a simple phase change reaction to overcome these shortcomings. The introduced iron cooperates with cobalt achieving high-efficiency activation of peroxymonosulfate (PMS) to eliminate Rhodamine B (RhB). The results showed that 0.05 g/L Fe 3 O 4 /Co 3 S 4 and 1 mM PMS could quickly remove 100% of 200 mg/L RhB within 20 min, and the removal rate of RhB remained above 82% after 5 cycles. Moreover, the as-prepared Fe 3 O 4 /Co 3 S 4 possessed a great magnetic separation capacity and good stability of low metal leaching dose. Radical quenching experiments and electron paramagnetic resonance (EPR) techniques proved that sulfate radicals (SO 4 •− ) were the dominant reactive oxygen species responding for RhB degradation. X-ray photoelectron spectroscopy (XPS) pointed out that the synergism of sulfur promoted the cycling of Co 3+ /Co 2+ and Fe 3+ /Fe 2+ , boosting the electron transfer between Fe 3 O 4 /Co 3 S 4 and PMS. Moreover, the degradation pathways of RhB were deduced by combining liquid chromatography-mass spectrometry (LC-MS) analysis and density functional theory (DFT) calculations. The toxicities of RhB and its intermediates were evaluated as well, which provided significant assistance in the exploration of their ecological risks.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Qipu Ma,Yuyao Zhang,Xiaoying Zhu,Baoliang Chen
Reducing the agglomeration of nano-catalysts to retain the active catalytic sites is crucial for the advanced oxidation processes (AOPs) of peroxymonosulfate activation in wastewater treatments . Herein, Co 3 O 4 hollow multi-shelled structures (HoMSs) were successfully prepared as the nanoreactors to reduce the agglomeration of nano-catalysts in catalytic reaction . Compared with single-shelled and double-shelled Co 3 O 4 HoMSs, triple-shelled Co 3 O 4 HoMSs (TS-Co 3 O 4 ) exhibited best catalytic performance and the carbamazepine (5 mg L −1 ) degradation reached 100% within 30 min. The hollow multi-shelled structures showed a significant role in reducing the agglomeration of catalysts. The value of hydrodynamic diameter/true particle size of TS-Co 3 O 4 was 1.58, which meant TS-Co 3 O 4 could be regarded as a single dispersion or two together in aqueous solution. The shells of TS-Co 3 O 4 supported each other and outer shells could protect the inner ones, hence the stability increased. Besides, the hollow cavity between shells reduced the mass diffusion resistance and increased the contact of reactants with active sites. Mechanism studies showed sulfate radicals (SO 4 •– ) played a leading role in the degradation of carbamazepine. This work provided an effective way to reduce the agglomeration and retain the active sites of cobalt-based catalysts in AOPs, so as to balance the conflict between the reactivity and stability of nano-catalysts.
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ANALYTICAL CHEMISTRY
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2021
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IF 6.986
Yufeng Liu,Xiaoyu Wang,Quan Wang,Yihong Zhang,Quanyi Liu,Shujie Liu,Sirong Li,Yan Du,Hui Wei
Mimicking enzyme specificity via construction of on-demand geometric structures on nanozymes is of great interest in recent years. Although building substrate-specific polymers on nanozymes has achieved great success, polymer-blocked active sites would inevitably lead to decreased activity of nanozymes. Here, we have developed three photoactive metal–organic framework (MOF)-based nanozymes (called 2D-TCPP, 3D-TCPP, and AD-TCPP), which have different geometric structures as well as unshielded active sites. Together with their structural variations and excellent photoresponsive oxidase-like activities, these photoactive nanozymes exhibit structure-dependent specificity for three kinds of substrates (typical oxidase substrates, organic pollutants, and antioxidants). Moreover, AD-TCPP and 3D-TCPP show potential applications for environmental protection and bioanalysis, respectively. This work offers a promising approach to the development of nanozymes with enzyme-like specificity.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Tong Liu,Zhican Xie,Peng Zhou,Zhaokun Xiong,Heng Zhang,Zhicheng Pan,Yang Liu,Bo Lai
Transition metal activation of sulfite (S(IV)) is a promising wastewater treatment technology . In this study, the activation of potassium pyrosulfite (PPS) with ferric iron (Fe 3+ ) is proposed firstly to degrade carbamazepine (CBZ). PPS has the advantages of low cost, non-toxicity and acidic solution, which makes it unnecessary to adjust the pH. The results showed that the Fe 3+ cycle was realized during the reaction process, and the degradation trend of CBZ was consistent with the formation rate of Fe 2+ and the decay rate of S(IV). Moreover, oxygen (O 2 ) plays a decisive role in the system and was the initiator of free radical chain reactions. The existence of sulfite radical (SO 3 •− ), sulfate radical (SO 4 •− ) and hydroxyl radicals (HO • ) in Fe 3+ /PPS system was proved by electron paramagnetic resonance (EPR), quenching experiments and terephthalic acid (TA) photoluminescence probing technique. The contribution of SO 4 •− and OH • to the removal of CBZ in Fe 3+ /PPS system is 64% and 35%, respectively. In addition, intermediates of CBZ were identified by Liquid Chromatography–Tandem Mass Spectrometry (LC–MS/MS) and possible removal pathways were also proposed. Finally, the effects of PPS concentration, Fe 3+ concentration, initial pH, anions and humic acid (HA) were also investigated.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Xuedong Du,Wenyang Fu,Pei Su,Qizhan Zhang,Minghua Zhou
The reduced S-modified MIL-53(Fe) was prepared by sulfurizing MIL-53(Fe) at low temperature, which was an efficient electro-Fenton catalyst at wide pH range (3–9) for sulfamethazine (SMT) degradation. The best temperature and MIL-53(Fe)/S ratio were 350 °C and 1:2, at which the BET surface area was much enlarged. The MIL-53(Fe) surface was etched by S to many 2D nanosheets with the thickness of ~50 nm, while S 2–2 replaced OH - to coordinate with Fe 2+ and increased the Fe 2+ content, which improved the catalytic performance. Even at initial pH of 7.0, the SMT removal was 95.8%, and the rate constant ( k ) in the Hetero-EF process was 16-folds of that in the Homo-EF process. The turnover frequency (TOF d ) value of MIL-53(Fe)/S(1:2)−350 was 0.48 L g −1 min −1 , which was 6.8 times that of commercial FeS 2 . The S 2–2 in catalyst adjusted the pH superfast, and promoted the generation of Fe 2+ and thus efficiently activating H 2 O 2 to form surface · OH, which was verified to be the main radical by EPR and radical scavenger experiments. This catalyst showed promising prospect for environmental application and could be regenerated by sulfidation method. S-doped MIL-53(Fe) was an excellent pH regulator, thus promoting promising application in Hetero-EF processes.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Wei Xiang,Hao Chen,Zhenxing Zhong,Chunjie Zhang,Xiejuan Lu,Mingjie Huang,Tao Zhou,Peng Yu,Beiping Zhang
In this study, a novel ultrasound enhanced FeS/persulfate Fenton-like system (US/FeS/PDS) was developed for the synergistic degradation of a typical drug carbamazepine (CBZ) under neutral circumstances. Factors such as FeS dosage, PDS dosage, initial pH and temperature, as well as coexisting anions were investigated. High dosages of FeS and PDS, elevated temperature and acidic circumstances were favorable for the oxidation of CBZ. Presence of HCO 3 − strongly inhibited the CBZ degradation in the US/FeS/PDS system, while slight suppression was observed with either NO 3 − or Cl − . Seven intermediates were identified as the products from the decomposition of CBZ by hydroxyl radicals (OH·) and sulfate radicals (SO 4 − ·). Time-dependent radical examination indicated that homogeneous OH· and SO 4 − · would contribute to the CBZ removal from 22.6 to 34.7% and 12.9 to 50.5%, respectively, while the contribution of solid-liquid interfacial radicals decreased from 64.5 to 20.2%. Meanwhile, the oxidation of S 2− occurred concurrently with reduction of Fe(III) to Fe(II). The reaction mechanism in the US/FeS/PDS system was proposed based on the sonochemical heterogeneous-homogeneous sulfur-iron cycle in the US/FeS/PDS system. US would firstly enhance the interfacial sulfur-iron electron transfer and the disintegration of the passivation layer, and then lead to the overall improvement in both interfacial and bulk sulfur-iron cycle, as well as the degradation of CBZ.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Meng Li,Zilong Li,Xiaolong Yu,Yinlong Wu,Cehui Mo,Mi Luo,Ligui Li,Shaoqi Zhou,Qiming Liu,Nan Wang,King Lun Yeung,Shaowei Chen
Development of low-cost, high-performance catalysts for the effective degradation of organic dyes is of both fundamental and technological significance for environmental remediation. Herein, FeN 4 -doped carbon nanotubes exhibit a remarkable catalytic activity towards the degradation of acid orange 7 (AO7) in the presence of peroxymonosulfate (PMS). This is accounted for by the abundant well-dispersed FeN 4 sites and appropriate adsorption energy. Radical quenching experiments and electron paramagnetic resonance measurements suggest that singlet oxygen is the main reactive oxygen species. 57 Fe Mossbauer spectroscopy measurements show that the FeN 4 moieties contain multiple spin states, and in conjunction with density functional theory calculations, confirm that FeN 4 with a low/medium spin state serves as the key sites for PMS activation and hence AO7 degradation. Results from this study highlight the critical role of spin states in FeN 4 in the generation of singlet oxygen for effective degradation of organic pollutants.
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Analytical Methods
·
2021
·Vol. 13
·期 46
·5542-5548
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IF 2.896
Xinfa Cai,Meijuan Liang,Fei Ma,Sherif Ramzy Mohamed,Amira Abdel Goda,Dawood H. Dawood,Li Yu,Peiwu Li
A direct competitive nanozyme-linked immunosorbent assay (dcNLISA) based on MnO2 nanosheets (MnO2 NSs) as a nanozyme label was developed for the highly sensitive determination of fumonisin B1 (FB1). MnO2 NS-labeled fumonisin B1-bovine serum albumin was easily synthesized as a competing antigen for the dcNLISA. And color changes derived from the MnO2–3,3′,5,5′-tetramethylbenzidine (TMB) system were exploited as the output signals of the dcNLISA. Several experimental parameters including the concentrations of the coating antibody, pH values, ionic strength and methanol concentration were optimized. Under the optimal conditions, the proposed method demonstrated a linear range (1.17–20.74 ng mL−1) with a reliable correlation coefficient (R2 = 0.9989), a satisfactory limit of detection (0.63 ng mL−1) and high selectivity for the detection of FB1. The recoveries of FB1 in spiked corn and wheat samples were in the range of 85.31–108.16% with coefficients of variation (CVs) ranging from 6.14% to 9.23%. Meanwhile, the testing results showed good consistency (R2 = 0.9892) between the developed dcNLISA and the reference method, liquid chromatography/mass spectrometry/mass spectrometry (LC-MS/MS) method. The proposed method was proven to be simple, sensitive, cost-effective and reliable for the screening of FB1 in cereals.
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