CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Lu-Lu Zhou,Peng-Xi Liu,Ying Ding,Jia-Rui Xi,Li-Juan Liu,Wei-Kang Wang,Juan Xu
Heterogeneous catalysts with hierarchically porous structure are highly efficient to catalyze chemical reactions. In this work, two-dimensional (2D) nano-flakes assembled flower-like NiO is fabricated and utilized for activating peroxydisulfate (PDS) to degrade organic pollutants bisphenol A (BPA). The results demonstrate that the prepared catalyst exhibits well organized flower structure composed of uniform 2D nano-flakes. PDS combines with the catalyst to form surface-activated NiO-PDS complex, subsequently depriving electrons from BPA. For the optimized NiO-12 catalyst, large specific surface area and hierarchically porous structure benefit to exposes abundant active sites while low resistance promotes electrons transfer, bringing the high BPA degradation rate constant of 0.28 min −1 under the condition of 20 mg/L initial concentration. NiO-12 exerts a capability of catalyzing PDS to mineralize 34% of practical packaging wastewater. This study provides a new strategy to fabricate hierarchical 2D porous catalysts for persulfate activation, with application potential in practical 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
ACS ES&T Water
·
2022
·
IF 0
Yibing Sun,Hongchao Li,Shengli Zhang,Ming Hua,Jieshu Qian,Bingcai Pan
Heterogeneous peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) are under extensive investigation for their great potential in water remediation. The understanding of the PMS activation mechanism is crucial but still debatable. Here, we describe a thorough investigation of the mechanism involved in PMS activation by using molybdenum disulfide (MoS2) as a catalyst. This MoS2/PMS system exhibited intriguing target-dependent reactivity. Further comprehensive experimental results excluded the major contributions of various possible species, including HO•, SO4•–, O2•–, 1O2, homogeneous Mo(VI), and heterogeneous Mo(VI). We then proposed a surface ≡Mo–OOSO3– complex as the major reactive species, while SO4•– derived from the decomposition of ≡Mo–OOSO3– acted as the secondary reactive species for pollutant removal. This complex could oxidize pollutants through the oxygen-atom-transfer mechanism and perform both nucleophilic and electrophilic attacks. This work provides novel perspectives for the mechanistic understanding of heterogeneous PMS-based AOPs for water remediation.
研究领域:
环境科学
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化学工程
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DOI
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2022
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IF 7.926
Junyuan Guo,Jianying Jiang,Yihua Chen,Xiaoying Wen,Wenjing Chen,Yifan Wang,Lin Su,Jing Cao
In order to achieve efficient adsorptive and oxidative removal of pyrene, a persulfate oxidation system with composite nZVI-BC prepared by loading nano-zero-valent iron on coconut shell biochar as an activator was established and applied. The results of adsorption experiments showed that at pH 3, when the dosages of BC, nZVI and nZVI-BC were all 1.5 g/L, the removal efficiency of pyrene reached 64.9%, 19.0%, and 61.2%, respectively after 120 min of adsorption. The best performance of nZVI-BC-persulfate system was achieved at pH 3, nZVI-BC 1.2 g/L and persulfate concentration 6 mM, and after 60 min of degradation, the removal efficiency of pyrene reached 99.4%. The pre-adsorption process was a promoting-step for pyrene degradation. The conversion of nZVI to Fe 2+ and Fe 3+ played an important role in the activation of persulfate to produce SO 4 •− and • OH, both of which were responsible for non-selectively oxidization pyrene. The support of BC could improve the dispersibility and activity of nZVI and improve of the above conversion. The intermediates with relatively lower toxicity were identified during pyrene degradation, and they were successively oxidized into CO 2 and H 2 O finally. In summary, nZVI-BC can be a promising catalyst for persulfate activation to degrade PAHs in wastewater.
研究领域:
环境科学
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化学工程
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高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
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2025
·Vol. 39
·期 5
·e70103
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IF 0
Palanisamy Vasudhevan,Dong Yu,Ruoyu Zhang,Mysoon M. Al-Ansari,Velu Manikandan,Hui Ma,Saurav Dixit,Shengyan Pu
Chlorinated aromatic chemicals are highly hazardous, transmissible, and bioaccumulative. Developing an economically feasible catalytic method to facilitate the effective removal of chlorinated aromatic pollutants is critical for contamination prevention. The current study extensively investigated the utilization of organic ligands such as citrate (CA) and ethylenediaminetetraacetic acid (EDTA) to increase Fe(II)-activated persulfate (PS) for 4-chlorophenol (4-CP) and 3-chlorobenzoic acid (3-CB) degradation in water. The decomposition and consumption ability of persulfate in PS alone and Fe(II)/PS systems for 4-CP and 3-CB was very low because of the rapid utilization as well as discontinuous availability of Fe(II), which indicates the decline of Fe(III) to Fe(II). But, when using the citrate/Fe(II)/PS and EDTA/Fe(II)/PS combinations, the degradation of 4-CP and 3-CB was 78.86%, 75.01% and 84.84%, 80.99% within 30 min, respectively. The significant enhancement is due to both ligand-to-metal transfer of charges process, and this increased the process of rate determination through carrying electrons into the citrate and EDTA ligands to Fe(III), generating Fe(II). In addition, the 4-CP and 3-CB degradation facilitated with citrate/Fe(II)/PS and EDTA/Fe(II)/PS systems was efficiently degraded at acidic pH (2.0–6.0) conditions. The pseudo-first-order kinetics model accurately predicted 4-CP and 3-CB degradation in the organic ligand/Fe(II)/PS systems. The degradation percentage of 4-CP and 3-CB increased with increasing PS and Fe(II) concentrations. Moreover, both sulfate and hydroxyl radicals formed by citrate/Fe(II)/PS and EDTA/Fe(II)/PS systems were identified as major reactive oxygen species for 4-CP and 3-CB decomposition. The present investigation recommends an alternate strategy to enhance the Fe(II)-activated persulfate mechanisms.
研究领域:
环境科学
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化学
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DOI
Journal of Environmental Sciences
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2025
·
IF 6.3
Mengqi Bu,Li Yi,Yingjie Wen,Minli Wang,Hao Yang,Chaohao Chen,Dengsong Zhang,Xu Chen,Zhiyi Lu
Electro-activating peroxydisulfate (PDS) based on the cathode represents a highly promising advanced oxidation process; however, its longevity is constrained by cathode leaching. In this work, we demonstrate that the γ-FeOOH/Fe Foam and α-Fe 2 O 3 /Fe Foam obtained by engineering a protective layer containing iron and oxygen on Fe Foam exhibit significantly extended service life of 53 h and 47 h, 2.94-fold and 2.61-fold longer than that of the original Fe Foam (18 h), while showing similar pseudo-first-order kinetics. Structural evolution analysis and density functional theory simulations reveal that surface oxygen plays a crucial role in reducing the leaching of Fe from the cathode by immobilizing Fe ions and converting them in-situ into stable Fe 3 O 4 . The electro-activation mechanism of PDS on the cathode, the degradation pathways of atrazine (ATZ), and the effects of operating conditions are systematically investigated and elucidated. This work underscores the pivotal role of surface oxygen in prolonging the longevity of Fe-based cathodes, thereby contributing to the development of protective layers.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2019
·
IF 7.65
Suding Yan,Xinping Zhang,Hui Zhang
The combination of persulfate (PS) activation by iron ions with electrochemical process (electro/Fe 3+ /PS) is a promising advanced oxidation process. However, almost all these systems were performed in an unbuffered solution and actually under acidic pH condition, with the electricity being frequently supplied by external power. Considering the high buffering capacity of wastewater and energy saving, peroxydisulfate (PDS) activation by Fe(III) species with bioelectricity provided by microbial fuel cell (MFC) for bisphenol A (BPA) oxidation was investigated at fixed near-neutral pH as well as acidic pH. The results indicate that 90.8% of BPA could be removed at pH 2.5. Though the iron existed in the form of precipitate, BPA could still be efficiently removed at pH 6.0. The precipitate formed in the system at pH 6.0 was identified as the amorphous iron oxyhydroxides. Sulfate radicals in the bulk solution and that adsorbed on the precipitate were the dominant reactive species responsible for the oxidation of BPA in the homogeneous and heterogeneous MFC/Fe(III)/PDS processes, respectively. The mechanisms of BPA degradation at both pH values were proposed via EPR and quenching tests as well as XPS analysis. The effects of operating parameters, the mineralization, the mineralization current efficiency and energy consumption were also explored.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Lu Huang,Tao Zeng,Xuyang Xu,Zhiqiao He,Jianmeng Chen,Shuang Song
Immobilized activators of persulfate (PS) with high activity and stability are highly desirable from an industrial and environmental point of view. In this work, nitrogen-doped carbon (CNx) was successfully hybridized with stainless steel (SS) derived Fe 3 O 4 to construct a SS supported CNx/Fe 3 O 4 heterogeneous catalyst (CNx/Fe 3 O 4 /SS). When used in a sulfate radical (SO 4 − )-based advanced oxidation process (SR-AOP), CNx/Fe 3 O 4 /SS displayed significantly higher activity towards the degradation of aqueous carbamazepine (CBZ) when compared to the single Fe 3 O 4 and CNx activators. The removal of CBZ had the most rapid progression, with an initial pH of 3.5, a temperature of 35 °C, an initially added PS concentration of 250 mg L −1 and an added amount of CNx/Fe 3 O 4 /SS of 0.30 g. The removal efficiency of CBZ was ∼100% after 35 min of SR-AOPs. In addition, the CNx/Fe 3 O 4 /SS catalyst was stable, as demonstrated by six successive cycling experiments. The results obtained from the electron paramagnetic resonance (EPR) spectra and radical quenching experiments indicated that both SO 4 − and HO contributed to the CBZ oxidation process. On the basis of X-ray photoelectron spectroscopy (XPS) and Fermi level analyses, it can be concluded that SO 4 − and HO originated from the Fe 3 O 4 catalyzed decomposition of aqueous PS. CNx facilitated the redox cycle of Fe(III)/Fe(II) in Fe 3 O 4 . This study demonstrated the potential application of SR-AOPs to efficiently degrade organic contaminants.
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 ENVIRONMENTAL MANAGEMENT
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2022
·
IF 8.91
Yunjiang Yu,Haobo Guo,Zijuan Zhong,Anqi Wang,Mingdeng Xiang,Senhao Xu,Chenyin Dong,Zhaofeng Chang
In this study, pristine biochar (BC), ball milling biochar (MBC), Fe 3 O 4 modified BC (Fe 3 O 4 @BC), and Fe 3 O 4 modified MBC (Fe 3 O 4 @MBC) were prepared to compare the Bisphenol A (BPA) removal efficiency by activating persulfate (PDS). All catalysts exhibited excellent degradation rather than adsorption in the PDS system, and Fe 3 O 4 @MBC800 had the best BPA removal efficiency, with 96.73% degradation and negligible 1.43% adsorption due to the synergistic effect between MBC800 and Fe 3 O 4 particles. Radical quenching experiments and electron paramagnetic resonance analysis indicated radical pathways, namely, SO 4 ∙ - and ∙OH, O 2 ∙ - , and non-radical pathway ( 1 O 2 ) involving BPA degradation. The abundant oxygen-containing groups, increased graphitization and mesopores of MBC800, and Fe 3+ /Fe 2+ conversion of Fe 3 O 4 particles facilitated PDS activation to produce reactive oxygen species . In addition, the superior electrochemical performance accelerated the electron transfer between the catalyst and PDS, promoting BPA degradation in the Fe 3 O 4 @MBC800/PDS system. More importantly, Fe 3 O 4 @MBC800 is resistant to environmental interference, including pH, anions, cations, and humic acid , and has good catalytic reusability and stability, which fulfills the requirements of engineering applications . Therefore, Fe 3 O 4 loaded on ball-milled biochar provides a convenient strategy for preparing environmentally friendly, economical, and efficient carbon-based catalysts to remove organic contaminants .
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
PubMed
高影响因子
ACS ES&T Engineering
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2021
·
IF 0
Cong Wang,Shao-Yi Jia,You Han,Yang Li,Yong Liu,Hai-Tao Ren,Song-Hai Wu,Xu Han
Enzymatic polymerization of phenolic contaminants to polyphenolics by H2O2 is an effective method to turn phenolic wastes to useful polymers. However, the sensitivities and the high costs of enzymes always limit their applications in the long-run treatment of industrial wastewater. In this study, a highly efficient CuO-persulfate (PS) system is reported to be a promising candidate for enzyme–H2O2 and shows high reactivity to polymerize various phenolic contaminants to polymers under alkaline conditions with the ratio of PS/phenolics less than 2.0. Compared with the generally accepted mechanism that the oxidizing species of SO4•– and ·OH generated during PS activation primarily contribute to the oxidation of various organic contaminants, quenching experiments, EPR (electron paramagnetic resonance) analysis and DFT calculations in this study indicate that PS is activated on CuO via a nonradical pathway under alkaline conditions, and the O–O bond in PS is moderately elongated from 1.45 to 1.58 Å. The inversely linear relationship between log kobs and BDEO–H values of various phenolics in the Hammett plot confirms H-abstraction from various phenolics under alkaline conditions. DFT calculations further reveal the formation of phenolic radicals after the activated PS abstracts H from phenolic −OH, followed by subsequent polymerization of phenoxyl radicals to polyphenolics. Characterizations of the oxidation products confirm that more than 80% phenolic contaminants have been transformed to polyphenolics. This study provides a new alternative for recovering various phenolic contaminants from industrial wastewater.
研究领域:
环境科学
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化学工程
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DOI
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Qi Wang,Yu Mei,Ruoxue Zhou,Sridhar Komarneni,Jianfeng Ma
The Ti 3 C 2 -based MXene with unique lamellar nanostructure and high conductivity is expected to effectively improve photocatalytic ability of composites as a cocatalyst. Herein, two dimensional Ti 3 C 2 -based MXene nanosheets decorated with copper sulfide particles (CuS@MXene) were synthesized by hydrothermal treatment to boost catalytic persulfate (PS) activation under light, exhibiting remarkable reactivity and stability for the rapid removal of Orange II. The phase composition of CuS@MXene was detected by X-ray diffraction (XRD), the morphology of CuS@MXene was characterized by scanning electron microscope (SEM), and the results of X-ray photoelectron spectroscopy (XPS) proved the elemental composition and valence state of elements in the CuS@MXene. The dosage of PS and initial pH of solution were the main factors affecting the removal rate of Orange II, and the quenching experiment showed that 1 O 2 was the primary reactive species for the removal of Orange II in CuS@MXene -PS system. In addition, this study showed that CuS@MXene provided bi-active centers for PS activation, which was mainly attributed to the rapid charge transfer between dual electron-rich active centers of Cu and Ti. This system may be applicable to the degradation of other challenging organic pollutants .
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
Materials Research Express
·
2022
·Vol. 9
·期 9
·095504
·
IF 2.025
Xiaohui Zhao,Hui Zhou,Qiong Hua,Chengyu Wang,Xiaodan Wang,Ke Zhang,Hongpei Zhang,Binguo Zheng,Junling Niu
The chemical degradation of sulfate by activated Oxyone has the advantages of high degradation capacity, wide pH range and convenient transportation and storage, making it one of the most attractive advanced oxidation processes (AOPs). Besides, Co is the metal most capable of activating Oxone to produce sulfate. Therefore, it is critical to develop Co-based catalyst, an effective and recyclable heterogeneous catalyst, for activating Oxone to degrade tetracycline. In this study, CoTiO3 was extensively investigated for the activation of Oxone to generate sulfate radicals and degrade tetracycline antibiotics. The results showed that more than 95% of tetracyclines could be degraded at the amount of CoTiO3 catalyst of 0.02 g, the Oxone reagent concentration of 0.4 mmol l−1, and the pH value of 7. The removal rate of tetracyclines could still reach more than 85% after the CoTiO3 composite was repeatedly used for four consecutive cycles. These results indicate that CoTiO3/Oxone can be explored as an effective system for degrading long-lived organic pollutants.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yuhang Zhou,Jiafeng Ding,Wen Yan,Yunjuan Meng,Bingzhi Yu,Teer Wen,Yao Yue,Yuchi Zhong,Hangjun Zhang
Degradation of endocrine disrupting compounds by optimizing advanced oxidation processes is highly feasible, but remains a daunting challenge. In this work, a novel copper and molybdenum co-doped g -C 3 N 4 (Cu/Mo@CN) were successfully synthesized via a simple dip-calcination approach, of which highly dispersed Cu and Mo atom sites were doped in the ring of g -C 3 N 4 . The Cu/Mo@CN catalysts were characterized by XRD, SEM, TEM, XPS, UV–vis DRS analyses, etc. The optimized system of Cu 1 /Mo 3 @CN catalyst in the visible light-persulfate oxidation (Vis + PS + Cu 1 /Mo 3 @CN system) had high photocatalytic activity to remove 97.2 % of bisphenol A (BPA, 5 mg/L) within 60 min. Compared to pure g -C 3 N 4 , Cu/Mo@CN has better visible-light (Vis) response function and narrower band gap (2.58 eV), which are easier to get excited by Vis illuminate. The results showed that reactive oxygen species of SO 4 • − , • OH and • O 2 − could be stably produced to contribute to the BPA degradation in Vis + PS + Cu/Mo@CN systems. Meanwhile, the Cu and Mo elements co-doped in g -C 3 N 4 can also effectively activate PS to promote the production of reactive oxygen substances. In addition, the continuous production of photoelectrons enhanced the cycling of Cu 2+ /Mo 6+ and Cu + /Mo 4+ , which could be further improved the removal efficiency of Vis + PS + Cu/Mo@CN towards BPA. The degradation mechanism of BPA were proposed according to the identification of intermediate products and DFT calculation. Overall, this study provides a viable pathway for BPA abatement in actual wastewater treatment applications.
研究领域:
环境科学
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催化材料
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废水处理
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DOI
高影响因子
危险品化学品经营许可证（带存储）