NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 7
·3616-3627
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IF 3.3
Song Wang,Yonggang Zhang
Advanced oxidation processes are often applied to a variety of refractory wastewater, but rarely is the electro-Fenton process combined with the activated persulfate process applied to printing and dyeing wastewaters. In this study, we have delicately designed a new advanced oxidation process for the degradation of persistent pollutants in wastewater. The zero-valent iron (ZVI) activated peroxymonosulfate process coupled with an electro-Fenton (EF-PMS) oxidation process is applied to treat methylene blue (MB) wastewater. Its main advantage is to generate more reactive oxygen species (ROS) and reduce the cost of oxidants. Experimentally, it was found that the degradation rate of the MB by the EF-PMS process was significantly higher than that before the coupling, and the mineralization rate can reach 56.84% within 2 h. According to free radical scavenging experiments and electron spin resonance (ESR) spectroscopy, the main ROS in the EF-PMS process were identified as ˙OH, SO4˙− and 1O2, where free radical oxidation played an important role in the removal of MB, accounting for 70.39% of the total removal efficiency. The mechanism of ROS generation and action in the EF-PMS process was investigated, and the pathway of MB degradation was determined by the identification of intermediates. The EF-PMS process was also effective in degrading MB in different water quality backgrounds as well as for process reuse. The removal efficiency of other organic compounds was also evaluated. The results indicate that the EF-PMS process has good potential for application.
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WATER RESEARCH
·
2023
·
IF 12.8
Shouying Wu,Wei Wu,Jianing Fan,Linping Zhang,Yi Zhong,Hong Xu,Zhiping Mao
Developing high-performance catalytic systems for eliminating contaminants effectively in water has received a lot of attention. However, the complexity of practical wastewater poses a challenge for degrading organic pollutants. Non-radical active species with strong resistance to interference have shown great advantages in degrading organic pollutants under complex aqueous conditions. Herein, a novel system was constructed by Fe(dpa)Cl 2 (FeL, dpa = N, N' -(4-nitro-1,2-phenylene) dipicolinamide) activating peroxymonosulfate (PMS). The mechanism study verified that the FeL/PMS system had high efficiency in producing high-valent iron-oxo and singlet oxygen ( 1 O 2 ) to degrade various organic pollutants. In addition, the chemical bonding between PMS and FeL was elucidated by the density functional theory (DFT) calculations. The FeL/PMS system could remove 96% Reactive Red 195 (RR195) in 2 min, which was much higher than other systems involved in this study. More attractively, the FeL/PMS system demonstrated general resistance to interference from common anions (Cl − , HCO 3 − , NO 3 − and SO 4 2− ), humic acid (HA) and pH changes and were thus compatible with various natural waters. This work provides a new approach for producing non-radical active species, which is a promising catalytic system for water treatment.
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PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 16
·48088-48106
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IF 5.8
Musajan Zulhumar,Xiao Pengfei
Herein, mesoporous carbon-anchored cobalt ferrite nanocomposites (nano-CoFe 2 O 4 @MC) were fabricated using a hydrothermal method for application as heterogeneous catalysts to activate peroxymonosulfate (PMS), in order to solve the problems of low activation performance and secondary pollution caused by the inter-particle agglomeration, metal ion leaching, and difficult recovery of nano metal catalysts. Analysis techniques such as SEM, TEM, XRD, BET, FTIR, VSM, TGA, and Raman spectroscopy indicated that the prepared nanocomposites have excellent surface properties, structural stability, and magnetic properties. The performance of nano-CoFe 2 O 4 @MC for Congo red (CR) degradation was evaluated by comparison with other treatment systems and study of the influence of experimental parameters, including the anchoring ratios, catalyst dosage, PMS concentration, initial pH, CR concentration, coexisting anions, and humic acid. Both radical and nonradical pathways were observed in the activation process of PMS by nano-CoFe 2 O 4 @MC. The analysis results of the element composition and ionic state of the catalyst show that the redox cycle of two ion pairs, Co 3+ /Co 2+ and Fe 2+ /Fe 3+ , could enhance the multipath electron transfer on the catalyst surface to promote the generation of reactive oxygen species. Identification of the intermediate products revealed CR was transformed into 12 intermediates through two branch pathways in the nano-CoFe 2 O 4 @MC/PMS system. After five cycles of use, the catalytic efficiency of the catalyst did not decrease significantly. Nanocomposites with high catalytic performance, stability, recyclability, and a low ion leaching rate have broad application prospects in the treatment of antibiotic wastewater.
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PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Rui Zhou,Tong Wang,Fei Wang,Dongnian Zhang,Zhihong Hu,Huaizhu Li,Na Huang,Sa Ban,Chuncai Kong,Zhimao Yang,Xiaojun Jia,Hao Zhu
The citrate sol-gel method was used to synthesize LaNi 0.6 Co 0.4 O 3 anchored at ZnO (LaNi 0.6 Co 0.4 O 3 /ZnO) for activation of peroxymonosulfate to degrade ofloxacin in simulated wastewater. LaNi 0.6 Co 0.4 O 3 nanoparticles were uniformly and firmly dispersed on ZnO support during the synthesis process. LaNi 0.6 Co 0.4 O 3 /ZnO had a rapid catalytic rate with an efficiency of 90% in 10 min, which was higher than that of LaNi 0.6 Co 0.4 O 3 (87.7%). Meanwhile, LaNi 0.6 Co 0.4 O 3 /ZnO significantly inhibited metal ion leaching compared to LaNi 0.6 Co 0.4 O 3 (Ni leaching: 0.128 mg/L to 0.022 mg/L, Co leaching: 0.083 mg/L to 0.012 mg/L). The composite material maintained great cyclic stability with efficiency of 93% after 5 cycles. Based on electron paramagnetic resonance studies and the quenching experiments, SO 4 ·− 、 · OH、 · O 2 − and 1 O 2 were the main reactive oxygen species involved in the reaction. The degradation intermediates of ofloxacin were detected by ICP-MS to propose the possible degradation pathways. This work provides an insight for perovskite catalyst for the activation of PMS to treat pharmaceutical wastewater.
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Molecular Catalysis
·
2023
·
IF 4.6
Siyuan Chang,Sen Zhang,Tianyi Chen,Lei Xu,Sumin Ge,Bingfeng Li,Chenke Yun,Guoxin Zhang,Xuejun He,Xin Pan
The important bio-based platform chemical 5-Hydroxymethylfurfural (HMF) can be oxidized for use in several products that serve as versatile building blocks of polymers. Previously, we had demonstrated that Pseudomonas aeruginosa PC-1 can selectively produce 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) from 800 mM HMF, with a yield greater than 90%. In this study, an aldehyde dehydrogenase (PaALDH64) was identified from P. aeruginosa PC-1 for selective HMF oxidation to HMFCA. The HMF tolerance level of E. coli /pET- PaALDH64 was over 300 mM, which was greater than the tolerance levels of all other reported enzymes. The proposed biocatalyst could be used to catalyze the biotransformation of other aldehydic furans, with carboxylic acid yields over 92%. Molecular docking revealed that the catalytic active site cleft in PaALDH64 formed more hydrogen bonds with HMF compared to other enzymes, which stabilized the enzyme–substrate interaction and enhanced the catalytic efficiency. In a fed-batch process, 547.8 mM HMFCA was produced from 600 mM HMF by E. coli /pET- PaALDH64 within 19 h only, which showed an excellent HMF conversion rate. Overall, PaALDH64 constitutes a promising enzyme for the industrial production of HMFCA.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Zhuyu Sun,Luxiang Zhu,Yujia Liu,Yanan Liu,Jin Wen
Polyhalogenated carbazoles (PHCZs) are a kind of emerging contaminants which have widespread distribution, strong potential persistence, high bioaccumulation, and dioxin-like toxicity. In this study, we used sulfidated zero-valent iron (S-ZVI) synthesized by ball-milling to activate peroxydisulfate (PDS) for the degradation of 1,3,6,8-tetrabromocarbazole (1,3,6,8-BCZ). The initial 1 mg/L 1,3,6,8-BCZ was degraded by 92.9 % within 30 min in S-ZVI/PDS system. The pseudo-first-order rate constant was estimated as high as 0.182 min −1 . Electron paramagnetic resonance (EPR) study and quenching experiments results revealed that •OH, 1 O 2 , O 2 •− , and SO 4 •− played roles in the degradation of 1,3,6,8-BCZ, with their contribution percentages of 32.8 %, 32.5 %, 24.8 % and 9.9 %, respectively. By further density functional theory (DFT) calculations, radical addition by •OH and 1,4-cycloaddition by 1 O 2 were suggested as the dominant channels for 1,3,6,8-BCZ degradation, while O 2 •− exerted an indirect synergistic influence. Based on the identification of intermediates and analysis of Fukui indices, 1,3,6,8-BCZ degraded through three degradation pathways, namely hydroxylation, debromination, and C–N bond cleavage. The S/Fe molar ratio, S-ZVI dosage, PDS dosage, reaction temperature, initial pH, and water matrices had influences on the degradation in 1,3,6,8-BCZ, result in a great toxicity reduction. Overall, this research developed an effective and feasible approach for the treatment of PHCZs, and which gave deep insights into the vital roles and synergistic effects of various reactive species based on the combination of experimental study and theoretical calculation.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Da Ouyang,Ronghao Wu,Zhaojun Xu,Xiaomin Zhu,Yimin Cai,Ruihuan Chen,Changyin Zhu,Damià Barceló,Haibo Zhang
Advanced oxidation processes (AOPs) based on persulfate (PDS) activation by iron materials have attracted significant attention due to their high organic pollution removal efficiency and relatively low remediation costs. However, one of the iron-based materials’ shortcomings is the weak activation ability of Fe 3+ on PDS and the low sustainability of Fe 2+ in the oxidation environment. In this study, biochar-supported molybdenum dioxide (MoO 2 @BC) was employed as a co-catalyst to enhance the Fe 3+ based PDS activation for Bisphenol A (BPA) degradation. Results showed that >96 % of BPA was removed during 60 min, and the BPA degradation efficiencies only slightly decreased after four reuses of MoO 2 @BC. Electron paramagnetic resonance (EPR) analysis and quenching experiments indicated that reactive oxidation species (ROSs) contributing to the degradation of BPA were SO 4 − , OH and 1 O 2 . Besides, it was found that biochar supporting favours the adsorption of Fe 3+ on the MoO 2 surface and promotes the electron transfer from Mo(IV) to Fe 3+ based on the combination of X-ray photoelectron spectroscopy (XPS) analysis, electrochemical tests and density functional theory calculation (DFT). This work provides a new insight for enhancing the performance of organic contaminants degradation through AOPs based on persulfate activation by iron material.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yong Liu,Le Zhang,Ting Liu,Jianlong Wang
The selective oxidation of ammonium nitrogen (NH 4 + -N) to dinitrogen (N 2 ) by advanced oxidation processes (AOPs) is of paramount significance, but it is still a great challenge. In this study, a novel composite (FeO x -MgO) was synthesized to activate persulfate (PS) for selective oxidation of ammonium (NH 4 + ) to N 2 under simulated solar-light irradiation ( hv ). The results demonstrated that the conversion of NH 4 + to ammonia (NH 3 ) on the basic sites of FeO x -MgO was a key step for the selective oxidation of NH 4 + . Fe(IV) species formed in FeO x -MgO/PS/ hv system could enhance both the efficiency and N 2 selectivity of the NH 4 + -N oxidation through the oxidation of ammonia hydride to N 2 . The 100 % NH 4 + -N removal and over 95.5 % N 2 selectivity could be achieved after 30 min when initial pH was in range of 2–10, and the initial NH 4 + -N concentration was 30 mg N/L. This study could provide a promising technology for the selective oxidation of NH 4 + -N to N 2 in water and wastewater.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Shiwen Dong,Wen Xu,Qingqing Guo,Kai Luo,Haijun Cheng,Juntao Tang,Da Wang,Zhiqiao He,Lizhang Wang,Shuang Song,Jun Ma
Designing efficient and environmentally friendly catalysts is essential to activating ozonation for wastewater remediation. This study prepared soybean biochar (SB), adzuki beans biochar (AB), and mung beans biochar (MB) catalysts using moldy legumes as precursors. The biochars were characterized to investigate the surface characters’ effect on ozone activation toward 2, 6-dimethylpyrazine (2,6-DMP) degradation. All prepared samples drastically facilitated the degradation more than with sole ozonation. It was found that at pH 7 with 10 mg L −1 catalysts, the removal rates of 5 μM 2,6-DMP were 88.3 %, 90.7 %, and 87.3 % by SB, MB, and AB at 30 min, respectively. The surface-area-normalized reaction rate constants (k obs /S BET ) showed that AB exhibited the best catalytic activity with the rate of 1.5 × 10 −2 mg·m 2 ·min −1 , which is 2.3- and 23.1-fold higher than that of SB and MB, respectively. Further characterization confirmed that oxygen- (C–O/C = O and –OH) and nitrogen-containing groups (pyridine N and pyrrole N) were crucial to the catalytic degradation, as electron transfer was promoted to form more ROS. In addition, the quenching test and electron paramagnetic resonance (EPR) revealed OH, O 2 − , and 1 O 2 as the main reactive oxygen species (ROS) during the heterogeneous catalytic ozonation (HCO), indicating that 2,6-DMP degradation followed the radical and non-radical oxidation pathways. Overall, this study helped to understand the relationship between surface functional groups and intrinsic activity. It also provided a new direction for utilizing agricultural waste.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Zhitong Xu,Ye Qi,Yueguang Fang,Peng Tian,Guiling Ning,Junwei Ye
Core-shell Fe 3 O 4 @UiO-66-NH 2 nanospheres with superior photocatalytic activity and photo-Fenton performance were synthesized using a layer-by-layer growth strategy. The synthesis involved the use of FeCl 3 , trisodium citrate, sodium acetate, ZrCl 4 , and 2-aminoterephthalic acid as raw materials, with mercaptoacetic acid serving as a modifier. Fe 3 O 4 @UiO-66-NH 2 demonstrated improved visible-light-driven photocatalytic performance in the oxidation degradation of Rhodamine B (RhB) in the presence of trace amounts of H 2 O 2 under visible light irradiation. The Fe(II)/Fe(III) cycle was accelerated by the transfer of the photogenerated electrons (e-) from UiO-66-NH 2 to Fe 3 O 4 , which in turn encouraged the Fenton reaction to produce hydroxyl radicals (•OH). With only 10 mmol/L H 2 O 2 , the removal rate of RhB approached 94% in 120 min. Furthermore, when exposed to visible light, Fe 3 O 4 @UiO-66-NH 2 exhibited 99% efficacious antibacterial activity against Escherichia coli and Staphylococcus aureus . Overall, the as-prepared Fe 3 O 4 @UiO-66-NH 2 core-shell nanospheres show promise for practical applications as photocatalysts for the degradation of organic pollutants and the inactivation of bacteria in wastewater.
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高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Shuang Liu,Hong Wu,Huaili Zheng,Weizhen Zhang,Wei Ding,Hong Li,Chao Liu
Sulfite (S(IV))-based advanced oxidation process has attracted widespread attention due to the generation of strongly oxidizing sulfate radicals (SO 4 •− ) and hydroxyl radicals (HO • ) for contaminants remediation. However, the contaminant degradation by singlet oxygen ( 1 O 2 ) through a nonradical pathway was still unclear in the S(IV) activation system. Herein, a magnetic Fe 3 O 4 /g-C 3 N 4 (MCN) composite was synthesized for the utilization as a visible-light catalyst to activate S(IV) under visible-LED (Vis-LED) for the organic degradation . The incorporation of Fe 3 O 4 in g-C 3 N 4 up-regulated the photocatalytic performance in the S(IV) activation for X-3B degradation, and > 98% of X-3B (20 mg L −1 ) was degraded with the degradation rate constant ( k obs ) of 0.110 min −1 within 30 min. The SO 4 •− and 1 O 2 produced in the MCN/S(IV)/Vis-LED system were identified as the primary reactive species through the quenching experiments and electron spin resonance. Interestingly, the light-induced generation of superoxide radical (O 2 •− ) played a negligible role in the formation of 1 O 2 , and most of 1 O 2 was corroborated to be originated from SO 4 •− besides SO 5 •− , which was rarely reported in other S(IV) activation processes. The catalysts before and after utilization were characterized to further elucidate the mechanisms for the S(IV) activation. There were two possible pathways for the S(IV) activation: the electron transfer from S(IV) to the photo-generated holes and the ligand-to-metal charge-transfer (LMCT) within the surface Fe(III)−S(IV) complexes. Furthermore, the MCN/S(IV)/Vis-LED system was of high resistance to complex water matrixes (pH, inorganic anions, etc.), demonstrating its application perspective in the purification of wastewater containing organic pollutants .
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lu Xu,Xiaojia Wei,Yuetong Qi,Wei Qiao,Juan Shi,Yabo Shang,Keqian Li,Xin Jin,Xue Bai,Xuan Shi,Pengkang Jin
The activation of persulfate (PS) in dissolved organic matter (DOM) solution using visible light has demonstrated potential for advanced wastewater treatment. This study presents a novel visible light-assisted homogeneous Fenton-like process (DOM-Fe 3+ -PS-Vis) for the efficient DOM degradation, based on the ligand-to-metal charge transfer (LMCT)-induced enhanced Fe 3+ reduction and PS activation. The simultaneous addition of Fe 3+ and PS to DOM-enriched solutions under visible light significantly improved PS activation, leading to the degradation of DOM and coexisting organic contaminants. The PS decomposition rate constant in the DOM-Fe 3+ -PS-Vis process was calculated to be 3.5–20.69 times higher than that of the DOM-PS-Vis, Fe 3+ -PS-Vis, and DOM-Fe 3+ -PS-Dark systems. Notably, over half of the decomposed PS in the DOM-Fe 3+ -PS-Vis process was activated by Fe 2+ generated via the LMCT between DOM and Fe 3+ . SO 4 − and OH were identified as the dominant reactive species present in the DOM-Fe 3+ -PS-Vis process with the steady-state concentration of 1.63–4.11 × 10 −13 M and 0.07 × 10 −13 M, respectively, which were 2.4–81.5 and 0.5–7 times higher than those in the DOM-PS-Vis, Fe 3+ -PS-Vis, and DOM-Fe 3+ -PS-Dark systems. Additionally, hydrophobic components with more aromatic carbon in DOM were found to promote the catalytic performance of the DOM-Fe 3+ -PS-Vis process. This study highlights the efficiency and promise of LMCT-induced enhanced Fe 3+ reduction and PS activation in DOM-enriched solutions under visible light for advanced wastewater treatment.
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高影响因子
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