Journal of Water Process Engineering
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2025
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IF 6.7
Xuanying Cai,Tiansheng Chen,Zhenhua Dai,Peiren Ding,Yinhao Dai,Peng Fan,Jihong Xu,Yuankui Sun,Xiaohong Guan
In cold regions, the freezing process typically presents difficulties for the remediation of contaminated soil and groundwater. However, in this work we report a freeze-assisted activation of peroxydisulphate (PDS) by β -MnO 2 for the degradation of phenolic compounds. The results showed that 60.8 % of 2,4-dichlorophenol (2,4-DCP) could be abated in frozen solutions at an initial pH of 6.5 within 2 h, whereas only 12.4 % of 2,4-DCP disappeared in aqueous solutions under other identical conditions. This enhancing effect was highly associated with the well-known freeze concentration effect, which could decrease the solution pH at the ice grain boundary by 2.4 units. Electron spin resonance (ESR) spectroscopic analysis and experiments with quenching agents and D 2 O suggested that radicals and singlet oxygen were not the major reactive species involved in the β -MnO 2 /PDS system. Instead, Raman analysis indicated that PDS may be bound to the surface of β -MnO 2 to form a reactive inner-sphere complex of MnO 2 -PDS*, which is proposed to account for the oxidative degradation of 2,4-DCP in aqueous and frozen β -MnO 2 /PDS systems. Chronoamperometric experiments further showed the redox potential of the β -MnO 2 /PDS system was as high as 1.2 V. This work highlights the possibility of applying the freezing effect to accelerate PDS activation by minerals abundant in environment and thus offers a promising strategy for pollution remediation in cold regions.
研究领域:
环境科学
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化学
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DOI
高影响因子
BIOCHEMICAL AND BIOPHYSICAL RESEARCH COMMUNICATIONS
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2019
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IF 2.705
Zhi Li,Sha Jiang,Yanan Xie,Zemin Fang,Yazhong Xiao,Wei Fang,Xuecheng Zhang
Laccases (benzenediol: oxygen oxidoreductases , EC1.10.3.2) can oxidize various substrates, and those which are tolerant to and even activated by salts have attracted a lot of attention due to their application potential in certain industries. The mechanism of the salt activation of laccases is awaiting to be elucidated yet. Our previous study (Li, Xie et al. 2018) supposed that the salt activation of marine laccase Lac15 might be attributed to Cl - ion specifically binding to some local sites to interfere substrate binding and/or electron transfer . In this study, we found two sites whose mutations resulted in elimination of the salt activation of Lac15’s activity towards catechol and dopamine respectively, and revealed that the mutations affected the activity by altering both E m and k cat , demonstrating the supposed mechanism. A model for the salt activation of laccases was accordingly proposed, albeit some details are to be elucidated.
研究领域:
生物化学
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酶学
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工业生物技术
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Wei Yang,Yan Zou,Zhihui Pang,Yanrong Zhang,Manabu Fujii
Sulfite [S(IV)] activation processes have aroused increasing attention in the field of wastewater treatment. In this study, a novel humic acid-derived carbon (HAC-10) material was demonstrated as highly active and environmentally friendly S(IV) activator for the efficient elimination of recalcitrant pharmaceutical contaminants. The results suggested that quinone groups and conductivity served as the active site/structure for S(IV) activation, while the rapid adsorption process of contaminant significantly reduced the migration distance of generated SO 4 – , thus facilitating the degradation processes. The carbon–S(IV)* complexes were confirmed to be the primary step to produce SO 4 – . The mineralization process of tetracycline hydrochloride (TC, a model pharmaceutical) could effectively reduce its biological toxicity. In addition, S(IV)/HAC-10 system exhibited excellent adaptability to different pharmaceuticals, natural water matrix and was capable of effectively eliminating contaminants in actual wastewater. Furthermore, a continuous flow reactor consisting of HAC-10 catalyst membrane showed excellent reactivity and durability. Overall, this study provides novel insights into the activation mechanism of S(IV) by carbon materials, and advances the practical application of S(IV) activation processes in the decontamination and detoxification of pharmaceutical wastewater.
研究领域:
环境科学
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废水处理
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污染控制
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Yaqian Pang,Junpeng Zhou,Xiaoli Yang,Yeqing Lan,Cheng Chen
In this study, the Co 3 O 4 -SnO 2 composite derived from bimetallic oxalates was rationally fabricated and utilized as a catalyst for peroxymonosulfate (PMS) activation towards the destruction of chloramphenicol (CAP). The physicochemical properties of the Co 3 O 4 -SnO 2 were systematically characterized to discover the relationship between its structure and catalytic performance. SnO 2 as a cocatalyst with high conductivity and stability immensely improved the activity of Co 3 O 4 in the Co 3 O 4 -SnO 2 composite. Approximately 98% of CAP (10 mg/L) was eliminated by the Co 3 O 4 -SnO 2 (0.1 g/L) activated PMS (1.0 mmol/L) at initial pH 7 within 20 min. The rationally designed Co 3 O 4 -SnO 2 composite exhibited higher catalytic activity than Co 3 O 4 , SnO 2 , and other cobalt-based bimetallic oxides (such as Co-Fe, Co-Mn, and Co-Cu) in the PMS activation for the CAP degradation. The synergistic effect of Co 3 O 4 and SnO 2 endowed the Co 3 O 4 -SnO 2 composite with higher conductivity and more electron transfer, which was proved by the electrochemical tests. The presence of SO 4 •− , • OH, O 2 •− , and 1 O 2 during the CAP degradation was testified by both quenching experiments and electron paramagnetic resonance (EPR) spectroscopy. In addition, the catalytic mechanism and degradation pathways were further proposed via the characterization of X-ray photoelectron spectroscopy (XPS) and the identification of transformation products, respectively. This work provides a new insight into the preparation of novel catalysts and their application in wastewater treatment.
研究领域:
环境科学
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催化材料
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Yuhan Wang,Longzhen Ding,Chang Liu,Yao Lu,Qianyuan Wu,Chao Wang,Qing Hu
A series of environmental-friendly and cost-effective 0D/2D/2D ZnFe 2 O 4 /Bi 2 O 2 CO 3 /BiOBr double Z-scheme heterojunctions (abbreviated as xZnCB) were fabricated by a hydrothermal method using an electrostatic self-assembly strategy. The removal efficiencies toward tetracycline (TC), oxytetracycline (OTC), and doxycycline (DOX) were 93%, 90.1%, and 89.4% in 10ZnCB/sunlight/permonosulfate (PMS) systems within 20 min, and the degradation rate constants of 10ZnCB were 5.7–8.2 times higher than those of ZnFe 2 O 4 and 2.6–2.9 times higher than those of Bi 2 O 2 CO 3 /BiOBr (CB) under the same conditions. XPS valence band spectra, quenching experiments, EPR measurements, and density functional theory (DFT) calculations demonstrated the existence of the double Z-scheme heterojunctions. The coexistence of radical and non-radical pathways caused by photocatalytic and non-photocatalytic degradation mechanisms was also elucidated. PMS was effectively activated by a photoinduced e − , · O 2 − , and Fe(II)/Fe(III) pathway, and active species including · O 2 − , 1 O 2 , SO 4 · − , · OH, and h + participated in the catalytic processes. Unexpectedly, 1 O 2 , and · OH were determined to be the primary species during the degradation processes instead of SO 4 · − . Recycling experiments, metal leaching measurements, and TC degradation experiments in the secondary effluent demonstrated the excellent catalytic and structural properties of these xZnCB hybrid materials.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Longfei Zhang,Luhong Zhang,Yongli Sun,Bin Jiang
Cobalt-based perovskite material, an effective activator of PMS, is widely employed for wastewater remediation, but still affected by the leakage of the cobalt ions. In this study, a porous core-shell structured perovskite LaFe 0.1 Co 0.9 O 3-λ /SiO 2 core @ZrO 2 shell (LFCS@ZrO 2 ) was fabricated and partially etched to enlarge channels to further enhance mass transfer ability. The well-designed core-shell structure can not only restrain metal ion leaching by changing the surface microenvironment but also provide an additional driving force attributed to the enriched concentration gradient, thus enhancing the catalytic oxidation performance. Results showed that the partially etched LFCS@ZrO 2 (eLFCS@ZrO 2 ) particles exhibited an increased pore size and showed an attractive catalytic performance as well as a suppressed cobalt ion leaching (3.61 to 0.67 mg/L). Over 99% of tetracycline hydrochloride (20 mg/L) could be degraded in 15 min, and the reaction rate increased 2 folds compared with pristine LaFe 0.1 Co 0.9 O 3-λ . Besides, quenching test and electron paramagnetic resonance analysis proved that sulfate radicals and singlet oxygen were the two predominant reactive oxygen species during the catalytic oxidation. This work provides a novel perspective for the fabrication of an environmentally friendly perovskite catalyst, which has a great potential application in organic pollutant degradation.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Yiwu Tang,Jin Kang,Min Wang,Chongyue Jin,Jiayun Liu,Mei Li,Siyan Li,Zhilin Li
In this work, FeVO 4 nanorods were successfully synthesized and employed as peroxymonosulfate (PMS) activators for oxytetracycline (OTC) degradation. The obtained FeVO 4 nanorods exhibited excellent catalytic performance for PMS activation because of the synchronous transformations of Fe 3+ /Fe 2+ , V 5+ /V 4+ and Fe 3+ /V 4+ , and abundant adsorbed oxygen (O ads ). Almost 100% of OTC can be decomposed via FeVO 4 activating PMS in 40 min and the reaction rate constant (k) was 0.1073 min −1 , being 5.65 times of commercial Co 3 O 4 (0.0219 min −1 ). Meanwhile, FeVO 4 exhibited a good stability and reusability. In addition, the impacts of experimental parameters (catalysts and PMS dosage, temperature, pH, and co-existing anions) on OTC degradation were detected in detail. It was proved that •O 2 − , •OH and 1 O 2 were generated and the contribution role in OTC degradation followed the sequence” •OH > 1 O 2 ≈ •O 2 − . The possible mechanism of PMS activation by FeVO 4 was deeply explored and the OTC degradation pathway was deduced according to the detected degradation intermediates. This study develops one new environmental-friendly, low cost, high efficiency and stable PMS activator for the efficient removal of antibiotics.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Peng Xu,Xiang Li,Rui Wei,Chunyan Yang,Tianyao Shen,Peng Wang,Guangshan Zhang
The adaptability and stability of catalysts guarantee efficient catalytic performance. Hence, we fabricated FeCo 2 O 4 /diatomite for efficient peroxymonosulfate (PMS) activation. Distinct from stacked FeCo 2 O 4 , FeCo 2 O 4 /diatomite possessed a 1.2-fold larger specific surface area (94.84 m 2 g −1 ), achieving 100% ATZ removal within 10 min at 0.2 g L −1 PMS and 0.1 g L −1 FeCo 2 O 4 /diatomite. The system could adapt to a broad pH range (3–11) and complex water matrices, efficiently removing multiple contaminants. High removal performance (>92%) and mineralization (>57%) were maintained after six cycles with minimal leached Co (0.10 mg L −1 ). The conversion between ≡Fe(III)/≡Fe(II) and ≡Co(III)/≡Co(II) could trigger PMS persistently, producing abundant active species, in which SO 4 •− was dominant. Then, intermediates and degradation pathways were proposed based on DFT calculations and ESI-QTOF-MS/MS data. Toxicity analysis showed that most intermediates were more eco-friendly than ATZ. This study developed FeCo 2 O 4 /diatomite with superior catalytic performance, high adaptability, and stability for eliminating refractory organic pollutants.
研究领域:
环境科学
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催化材料
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Nguyen Quang Tung,Do Thi Cam Van,Dam Xuan Thang,Nguyen Thi Kim An,Tran Thi Trang,Bui Dinh Nhi,Nguyen Phuong Thao,Le The Son,Nguyen Nhat Huy,Nguyen Trung Dung
In this study, the CuCoFe-LDH catalyst was synthesized by hydrothermal method and applied to degrade levofloxacin (LFX) by peroxymonosulfate (PMS) activation. The physicochemical properties of the synthesized samples were analyzed by X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), Brunauer-Emmett-Teller (BET), X-ray photoelectron spectroscopy (XPS), and thermogravimetric analysis (TGA). The influence of various factors such as catalyst system, pH, catalyst content, PMS , pH, and coexisting ions on the degradation of LFX was systematically investigated. The results showed that after 10 min, 94.57 % of LFX was decomposed under the conditions of 200 mg/L of catalyst, 500 mg/L of PMS, 10 mg/L of LFX, and pH 7.0. Besides, the CuCoFe-LDH/PMS system can effectively remove LFX over a wide pH range from 3.5 to 9.0. Both radical superoxide (O 2 •- ) and non-radical singlet oxygen ( 1 O 2 ) were major reactive oxygen species in the CuCoFe-LDH/PMS system. Mass spectrometry identified 16 major degradation products of LFX, and 38.43 % of LFX was mineralized after 30 min of reaction. Besides, the CuCoFe-LDH/PMS system had the ability to effectively degrade different groups of antibiotics (e.g., fluoroquinolone, tetracycline , and sulfonamide). The mechanism of PMS activation by CuCoFe-LDH and the LFX degradation pathway were proposed. Finally, testing the reusability of CuCoFe-LDH in LFX degradation showed that a decrease of nearly 7 % occurred after five consecutive cycles, suggesting its stability for practical applications.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
ENVIRONMENTAL POLLUTION
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2023
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IF 8.9
Lingxiang Zhao,Xinyue Cheng,Zhaoxian Wang,Enzhe Zhang,Zilian Liu,Huajing Zhou,Liang He,Qingqing Guan
Although alkaline sulfite activation of ferrate (Fe(VI)) has advantages of fast response and high activity for degradation of organic contaminants , the specific production pathways of active species and the pH conditions still hinder its widespread application. Based on this, our study constructed a novel advanced oxidation process of calcium sulfite (CaSO 3 ) could activated Fe(VI) continuously by Ca 2+ buffering and investigated the mechanism under different pH values and CaSO 3 dosages with ciprofloxacin as a target organic pollutant. The results showed that Ca 2+ stabilized the process at a neutral/weakly alkaline microenvironment of pH 7–8, which could alleviate the hydrolysis of ≡Fe IV =O by protons and iron hydroxyl groups. Besides, the removal of pollutants occurred efficiently when sulfate (SO 3 2− ) was excessive and had a 3:1 ratio of SO 3 2− to Fe(VI), achieving more than 99% removal of electron-rich phenolic organic pollutants within 2 min. By adding different radical scavengers and combining electrochemical analysis methods and electron paramagnetic resonance spectroscopy techniques to revealed that the main active species in Fe(VI)/CaSO 3 process were ≡Fe IV =O/≡Fe V =O. Furthermore, the reactivity of various sulfate species (such as SO 3 2− , SO 3 •− , SO 4 •− , SO 5 •− ) with Fe(VI) was calculated using density functional theory (DFT), and it was found that Fe(VI)–SO 3 2− reaction has a much lower energy barrier (−36.08 kcal/mol), indicating that SO 3 2− can readily activate Fe(VI) and generate ≡Fe IV =O to attack the atoms with high Fukui index (f - ) in organic pollutants. The above results confirm the feasibility of Fe(VI)/CaSO 3 process. Thus, this study can theoretically and practically prove that the main active species is ≡Fe IV =O, rather than SO 4 •− or • OH in Fe(VI)/CaSO 3 process.
研究领域:
环境科学
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化学
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产品关联
DOI
PubMed
高影响因子
INORGANICA CHIMICA ACTA
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2025
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IF 3.2
Xiaoyu Qiu,Zhimei Li,Jianmei Cen,Hong Tang
Transition metal-based materials have emerged as a promising catalyst for peroxymonosulfate (PMS) activation in pollutant removal. However, challenges such as nano-material agglomeration, high metal ion leaching, and low reactive oxygen species (ROS) yield still hinder their practical application. In this work, the CoP/NF successfully was synthesized to tune PMS activation from a radical pathway to a non-radical dominated pathway for efficient degradation of organic pollutants. The incorporation of phosphorus element modulated the cobalt-based catalyst surface charge state and induced local charge density, facilitating the catalytic activity. Consequently, at optimal conditions (catalyst = 1.5 cm 2 , PMS = 0.3 g/L), CoP/NF achieved nearly complete removal of 40 mg/L rhodamine B (RhB) within 2 min over a wide pH (3.0–9.0), and maintained a strong anti-interference capacity for NO 3 − , PO 4 2− , Cl − . Furthermore, the degradation efficiency of RhB in the CoP/NF + PMS system remained 98 % even after 5 cycles. Impressively, ROS trapping and electron spin resonance (EPR) analyses revealed that the degradation process was dominantly driven by superoxide radicals (O 2 •– ) and singlet oxygen ( 1 O 2 ), which served as the key mechanism for the CoP/NF + PMS system. This work provided further insights into tuning PMS activation pathway via the integration of metal phosphides growth on nickel foam for sustainable water treatment.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Yudi Wang,Xinyi Shen,Sainan Sun,Xinyun Li,Jiayi Gao,Yifan Shao,Shi-Wen Lv,Yanqing Cong
Heterogeneous persulfate-based advanced oxidation processes (PS-AOPs) have been regarded as one of the most promising methods in the treatment of wastewater containing antibiotic. Herein, the Co 3 O 4 /NiO composite with built-in electric field is prepared. The existence of built-in electric field can reduce the interface resistance and accelerate the charge transfer, promoting the electron transfer between the Co 3 O 4 /NiO composite and peroxymonosulfate (PMS). Meanwhile, built-in electric field can induce the formation of electron-deficient and electron-rich active areas. With built-in electric field intervention, the activation pathway of PMS over Co 3 O 4 component with electron-deficient area of Co 3 O 4 /NiO is transformed from radical to 1 O 2 , while electron-rich area makes NiO component that has no ability can activate PMS producing SO 4 •− and OH • . As a result, the Co 3 O 4 /NiO composite can effectively activate PMS to realize the rapid degradation of tetracycline. More significantly, a micro reactor equipping with Co 3 O 4 /NiO composite not only displays high removal efficiency of total organic carbon (TOC), but also improves the biodegradability of wastewater containing antibiotic. In short, current work not only clarifies the role of built-in electric field in PMS activation, but also shares some valuable insights into the application of PS-AOPs in practical engineering.
研究领域:
环境科学
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化学工程
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废水处理
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）