CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Yang Li,Ting Yang,Shaohui Qiu,Wanqi Lin,Jinting Yan,Shisuo Fan,Qi Zhou
Iron-mediated activation of peroxymonosulfate (PMS) has been widely investigated for recalcitrant pollutants. However, maximizing the dispersion degree of the active iron sites in the catalysts is still a great challenge and attracting tremendous attention. Herein, we demonstrated that well-dispersed single atomic Fe sites embedded into N-doped porous carbon (Fe SA -N-C), which derived from chemically Fe-doped zeolitic imidazolate frameworks, could work as Fe-based catalyst for efficient catalytic oxidation of recalcitrant organics via PMS activation. As expected, Fe SA -N-C exhibited remarkably higher degradation activity (8.1 times faster) to BPA (a model pollutant) than that of Fe based nanoparticles-loaded N-doped carbon (Fe NP -N-C). The sufficient Fe-N x sites with single Fe atom as the building units were proposed to be the main active sites for PMS activation. Based on that, unlike the traditional sulfate radical-based advanced oxidation processes, BPA degradation was achieved via high-valent iron-oxo species. More particularly, it could be used over a wide range of pH 3.0–7.5 with almost no loss of degradation efficiency. This study will provide insights into the design of heterogeneous Fenton-like catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zeming Wang,Zihao Wang,Wei Li,Yeqing Lan,Cheng Chen
The hybrids of Co 3 O 4 anchored on different crystallographic MnO 2 (α-MnO 2 @Co 3 O 4 , β-MnO 2 @Co 3 O 4 , γ-MnO 2 @Co 3 O 4 , and δ-MnO 2 @Co 3 O 4 ) were synthesized and applied in peroxymonosulfate (PMS) activation for the degradation of sulfisoxazole (SIZ). Various characterizations were conducted to explore the physicochemical properties of the hybrids, and their catalytic activities were compared. The SIZ degradation followed pseudo-first-order kinetics, and the rate constants ( k obs ) were 0.1135, 0.0307, 0.1080, and 0.0285 min −1 for α, γ, β, and δ-MnO 2 , respectively. The introduction of Co 3 O 4 greatly improved the catalytic activities of the MnO 2 hybrids, and more than 94.7% of SIZ was degraded within 20 min. The k obs was in the order of γ-MnO 2 @Co 3 O 4 (0.3952 min −1 ) > α-MnO 2 @Co 3 O 4 (0.1573 min −1 ) > β-MnO 2 @Co 3 O 4 (0.1536 min −1 ) > δ-MnO 2 @Co 3 O 4 (0.1319 min −1 ). Obviously, the synergy of Co 3 O 4 and MnO 2 weakened the differences of catalytic performance of MnO 2 caused by their microstructures among α, β, and δ-MnO 2 . Due to its large surface area, γ-MnO 2 @Co 3 O 4 exhibited the most excellent catalytic performance for the SIZ removal. All the hybrids also displayed superior stability and reusability, and the degradation rates of SIZ maintained were above 97% during five consecutive cycles. The reactive oxygen species (ROS) including SO 4 •− , • OH, and 1 O 2 were responsible for the SIZ degradation in the system of MnO 2 @Co 3 O 4 /PMS, which was confirmed by electron paramagnetic resonance (EPR) technique and scavenger tests. Twelve intermediates of the SIZ degradation were identified via HPLC-TOF-MS 2 . Combined with the results of characterizations together with ROS identification, the possible catalytic mechanisms and pathways of the SIZ degradation were proposed. This study may shed some light toward the application of different crystallographic MnO 2 hybridized with other transition metals in PMS activation .
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WATER RESEARCH
·
2022
·
IF 13.4
Lingwei Gao,Yang Guo,Juhong Zhan,Gang Yu,Yujue Wang
Reactive species such as sulfate radicals ( SO 4 • − ), hydroxyl radicals ( • OH), and/or singlet oxygen ( 1 O 2 ) have often been proposed as the main reactive species for pollutant abatement during the persulfate-based process, and their relative importance is conventionally assessed by the quenching method based on an implicit fundamental assumption that the added high-concentration quenchers (e.g., tert-butanol and methanol) only scavenge their target reactive species, but do not considerably affect the other reaction mechanism of the system. To examine the validity of this assumption, this study evaluated the effects of several commonly used quenchers (tert-butanol, methanol, ethanol, isopropanol, furfuryl alcohol, and L-histidine) on the mechanism of a cobalt mediated peroxymonosulfate (Co(II)/PMS) process. The results demonstrate that besides quenching target reactive species, the added high-concentration quenchers can cause many confounding effects on the Co(II)/PMS process, e.g., accelerating PMS decomposition, interfering reactive species production, and quenching of non-target reactive species. Because of these confounding effects, the quenching method can actually lead to serious misinterpretation of the role of reactive species in pollutant abatement during the persulfate-based process. The findings of this study highlight that the underlying assumption of the quenching method is usually invalid for the persulfate-based process. Therefore, it should be cautious to apply the quenching method to investigate the mechanism of the persulfate-based process, and some debatable conclusions of prior studies obtained with the quenching method may require further verification.
研究领域:
环境化学
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水处理
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污染控制
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高级氧化过程
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高影响因子
JOURNAL OF SOILS AND SEDIMENTS
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2025
·
IF 3
Xie Xin,Liu Wei,Wang Mingxin,Pan Xinxing,Xue Jinjuan,Yao Meng
Purpose This study provides a novel resource utilization strategy for the carbonized soil derived from lubricant-contaminated soil. Materials and methods In this study, the lubricant-contaminated soil was treated by pyrolysis and ball milling with manganese carbonate to obtain Mn-loaded carbonized soil (Mn@BCS), which was then reused to activate peroxymonosulfate (PMS) oxidation for degradation of aniline (AN) in wastewater. Results and discussion When the dosage of Mn@BCS and PMS was both 1 g/L, 100 mg/L of AN was almost completely removed within 6 h. Three reactive oxygen species (ROS), including \({\text{SO}}_{4}^{\bullet -}\) , •OH and \({}^{1}{\text{O}}_{2}\) , were detected and verified. The probe-based kinetics models were established with atrazine, nitrobenzene and metronidazole as probes to quantify the generation of ROS. The exposure of the \({\text{SO}}_{4}^{\bullet -}\) , \(\bullet \text{OH}\) and \({}^{1}{\text{O}}_{2}\) at 6 h was 5.32 × 10 –11 , 5.40 × 10 –12 , 2.52 × 10 –10 M s, which contributed 33.62%, 2.02% and 2.98% to AN degradation, respectively. The main active sites include Mn–O, oxygen containing groups and graphitized carbon. The Mn–O and oxygen containing groups can activate PMS to produce \({\text{SO}}_{4}^{\bullet -}\) and \({}^{1}{\text{O}}_{2}\) , respectively. The graphitized carbon promotes AN degradation by generation of \({\text{SO}}_{4}^{\bullet -}\) and accelerating direct electron transfer. Conclusions Ball milling with manganese carbonate significantly improves the activation performance of carbonized soil for PMS oxidation, and thus promote the resource utilization of post-remediation soil.
研究领域:
环境科学
·
催化材料
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2025
·
IF 5.4
Yinxiao Zhang,Yanhui Li,Yan He,Jie Zhang,Xinxin Wang,Lianwei Yin,Qiuju Du,Xinxin Pi,Botong Chen,Yichen Li,Haitong Zhou
Adsorption, as a widely used water treatment method, has gradually revealed many drawbacks. Advanced oxidation processes, as emerging water treatment technologies, address some of the limitations of adsorption. However, designing bimetallic catalysts that are easy to synthesize and prevent metal ion leaching is crucial for activating peroxymonosulfate (PMS). To address these issues, this study designs a biochar reactor structure made by simple treatment and composite formation using wood as the base material. Biochar serves as an adsorbent to concentrate PMS and pollutants while preventing metal leaching. Additionally, Co Cu nitrogen-doped graphite carbon derived from metal-organic frameworks (MOFs) is encapsulated within the structure to efficiently activate PMS. The system achieved 100 % methylene blue degradation within one minute. Even after five cycles, it maintained a 95 % removal rate and exhibited excellent degradation performance across a wide pH range, proving its practical applicability. Furthermore, the synergistic pathway and transfer channels involved in adsorption-PMS activation were elucidated through various characterizations to reveal the underlying mechanism. This study aims to provide a novel material with adsorption and catalytic capabilities for the removal of organic pollutants through a simple and easily scalable synthesis method.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Qi Zhang,Wei Li,Siyuan Cao,Xu Yin,Hongwei Zhu,Liankai Gu,Haoming Chen,Xiaoyuan Zhang,Weiqing Han,Kajia Wei
Precisely controlling atomic occupancy in edge-sharing sites remains challenging and limits the application of spinel oxides in advanced oxidation processes (AOPs). Herein, a series of inverse spinel oxides featuring edge-sharing Co Oh -O-Mn Oh (Oh means octahedral) configurations were designed to leverage inter-octahedral electronic redistribution and spin-state modulation, thereby enhancing catalytic performance for peroxymonosulfate (PMS) activation and pollutant degradation. The energy redistribution induced by this structure enhances the O-p/Mn-d orbital hybridization, accelerates the electron transfer kinetics between Co and Mn, and promotes the generation of high-valent cobalt-oxo (Co IV =O) species and singlet oxygen ( 1 O 2 ), thereby increasing the degradation efficiency of organic pollutants. The optimized Co-Mn inverse spinel achieved complete BPA removal within 15 min, exhibiting 11.4-fold enhancement in PMS activation efficiency than unmodified cobalt oxide, and with < 6.5 % average efficiency deviation at 100 mM ionic concentration. This study offers a strategy for the precise design of edge-sharing reactive sites in inverse spinel oxides and their application in AOPs.
研究领域:
环境催化
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高级氧化技术
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材料化学
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无机化学
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WATER SCIENCE AND TECHNOLOGY
·
2022
·Vol. 85
·期 11
·3271-3284
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IF 2.43
Xu Jinghua,Hu Sisi,Min Lingli,Wang Shuhua
Advanced oxidation processes play an important role in the removal of organic pollutants from wastewater, in which it is essential to develop an eco-friendly, effective, stable, and inexpensive catalyst. Herein, waste eggshell-supported copper oxide (CuO/eggshell) was synthesized via a facile method and employed as peroxymonosulfate (PMS) activator for the elimination of reactive blue 19 (RB19). CuO/eggshell exhibited high degradation efficiency of RB19 (approximately 100%) by activation of PMS under the optimum conditions of 20 mg/L RB19, 0.2 g/L CuO/eggshell, 0.36 mM PMS, and initial pH 7.12 within 20 min. In addition, the effects of catalyst dosage, PMS concentration, initial pH, inorganic ions, and humic acid on RB19 degradation were investigated. Scavenging experiments and electron paramagnetic resonance revealed that multiple reactive oxygen species, including sulfate radicals (SO 4 ·− ), hydroxyl radicals ( · OH), superoxide radicals (O 2 ·− ), and singlet oxygen ( 1 O 2 ), contributed to RB19 degradation, and 1 O 2 played a dominant role. Finally, a possible PMS activation mechanism was proposed. This study suggests that loading catalytically active components onto waste eggshell is eco-friendly and effective for enhancing the degradation of dyes from wastewater. CuO/eggshell was synthesized through a simple impregnation method. CuO/eggshell exhibited excellent performance for PMS activation. CuO/eggshell and PMS system can effectively degrade RB19 in.a wide pH range (2–12). Singlet oxygen dominated the degradation of RB19.
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LANGMUIR
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2025
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IF 3.9
Junli Yu,Jihong Fu,Boshen Wang,Haipeng Zhang,Qichao Wu,Mengdie Li,Ronglan Wu
With the rapid development of petroleum resources and the chemical industry, the release of oily wastewater has increased dramatically and environmental pollution has become increasingly serious. In this study, an inexpensive, simple, and environmentally friendly technique was established to synthesize a multifunctional melamine sponge (MS) with both superhydrophobic and photocatalytic properties through polydopamine (PDA) functionalization, followed by the immobilization of CNZ (C3N4@ZnO) nanoparticles and the grafting of stearic acid (SA). The prepared SA@CNZ/PMS sponge exhibited outstanding superhydrophobicity with a water contact angle (WCA) of 150.5°. The sponge possesses superior hydrophobic–oleophilic selectivity, which can effectively separate various oil/water mixtures as well as oil-in-water emulsions. Meanwhile, the sponge exhibits high oil sorption capacity (11.55–52.76 times its own weight) and oil–water separation efficiency (99.3% after 10 cycles). In addition, superhydrophobic SA@CNZ/PMS is resistant to chemical corrosion and demonstrates good mechanical stability. Moreover, SA@CNZ/PMS exhibits a rapid removal efficiency for organic dyes (96.4% for methylene blue) through synergistic adsorption and visible light photocatalysis. This research provides new insights into the design of multifunctional materials for treating oily and dye-containing wastewater.
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PubMed
高影响因子
Journal of Water Process Engineering
·
2022
·
IF 7.34
Yanzhuo Zhang,Shengxu Liang,Rui He,Jing Zhao,Jinghua Lv,Wei Kang,Jian Zhang
Antibiotics in the water environment pose harm to animals, plants, and humans. In this study, biochar doped with sulfur (S), nitrogen (N), and NS was used to adsorb and activate peroxymonosulfate (PMS) to degrade the antibiotics chlortetracycline, ofloxacin, and sulfadiazine in an aqueous solution. The adsorption capacity of the biochar doped with single atoms increased significantly, and the maximum saturated adsorption capacities of undoped, N-doped, S-doped, and NS-doped biochar were 40.7, 85.5, 63.3, and 40.7 mg/g, respectively. The increase in specific surface area and the number of functional groups was the main cause for the increase in the adsorption capacity of heteroatom-doped biochar. The antibiotic degradation process involved the use of biochar to activate PMS and produce reactive oxygen species (ROS) for complete removal. The concentration of environmentally persistent free radicals (EPFRs) increased in response to heteroatom-doped biochar, and the type of EPFRs changed, which enhanced the ability of biochar to degrade antibiotics. At the 500 °C preparation temperature, the degradation rates of antibiotics by the undoped, N-doped, S-doped, and NS-doped biochar were 73.83%, 84.32%, 79.60%, and 74.10%, respectively, whereas the degradation rates at 900 °C were 82.38%, 93.78%, 91.11%, and 81.55%, respectively. The sulfate radical was produced during the activation process and made the largest relative ROS contribution to the increased adsorption capacity, followed by singlet oxygen, hydroxyl radical , and superoxide radical. Recycling experiments confirmed that the heteroatom-doped biochar was highly reusable and that the removal rates of N-doped biochar and S-doped biochar were high (81.94% and 78.06%, respectively).
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ENVIRONMENTAL RESEARCH
·
2023
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IF 8.3
Zhenyi Hu,Geng Su,Shujun Long,Xiaoting Zhang,Linkun Zhang,Yilin Chen,Chang Zhang,Gonggang Liu
Highly efficient resource recycling and comprehensive utilization play a crucial role in achieving the goal of reducing resource wasting, environmental protection, and achieving goal of sustainable development . In this work, the two kinds waste resources of agricultural rice husk and metal ions (Co, Ni, and Mn) from spent lithium-ion batteries have been skillfully utilized to synthesize novel Fenton-like catalysts. Desiliconized rice husk carbon (DRHC) with rich pore structure and large specific surface area from rice husk has been prepared and used as scalable carrier, and dandelion-like nanoparticles cluster could be grown in situ on the surface of the carrier by using metal ions contained waste water. The designed catalysts (X@DRHC) as well as their preparation process were characterized in detail by SEM, TEM, BET, XRD and XPS, respectively. Meanwhile, their catalytic abilities were also studied by activating potassium peroxomonosulfate (PMS) to remove methylene blue (MB). The results indicate X@DRHC displays excellent degradation efficiency on MB with wide pH range and stable reusability, which is suitable for the degradation of various dyes. This work has realized the recycling and high-value utilization of waste resources from biomass and spent lithium-ion batteries, which not only creates an efficient way to dispose waste resources, but also shows high economic benefits in large-scale water treatment .
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Journal of Water Process Engineering
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2024
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IF 6.3
Chuangbin Hong,Jiehang Zhou,Wenguang Wang,Liangpeng Wu,Shimin Long,Wentao Zhou,Yuxi Guo
Catalytic activation of peroxymonosulfate (PMS) is one of the important research areas in the development of advanced oxidation technology for wastewater treatment. At present, the development of high-performance catalysts for PMS activation has become a research hotspot. Herein, (Cu + decorated g-C 3 N 4 )/Bi 2 WO 6 ((Cu + /g-C 3 N 4 )/Bi 2 WO 6 ) composite was prepared successively by calcination and solvothermal method, which was used in visible light-assisted PMS activation for the degradation of rhodamine B (RhB). The construction of S-scheme heterojunctions between Cu + decorated g-C 3 N 4 and Bi 2 WO 6 facilitated the activation of PMS, leading to a RhB degradation ratio of 98.46 % within 50 min. The corresponding reaction kinetic was significantly improved by a factor of 2.32 and 7.94 compared with that of CCN and BWO, respectively. The enhanced performance of the (Cu + /g-C 3 N 4 )/Bi 2 WO 6 can be attributed to the successful construction of S-scheme heterojunction, which facilitates the separation of photogenerated carriers and accelerates the PMS activation to produce abundant active species. Furthermore, the (Cu + /g-C 3 N 4 )/Bi 2 WO 6 composites exhibit strong stability and reusability following three cycles. In addition, the intermediates produced during the RhB degradation process were investigated by liquid chromatograph mass spectrometer (LC-MS). This study provides a new insight into the preparation of S-scheme photocatalysts for the photocatalytic-PMS activation system that will achieve efficient removal of dyes from wastewater.
研究领域:
环境科学
·
材料科学
·
化学工程
·
水处理
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CATALYSIS LETTERS
·
2025
·Vol. 155
·期 9
·1-16
·
IF 2.4
Hu Rui,Wang Haiyin,Luo Jiahui,Song Jianjun,Jia Haiyuan
Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) have been proven to be an effective method for the removal of tetracycline in water. In this study, the Co 3 O 4 /molecular sieve catalyst synthesized by the incipient wetness impregnation method was used for PMS activation. The effect of specific surface area on the catalytic performance of Co 3 O 4 /molecular sieve catalyst was investigated and analyzed in detail by characterization techniques. In the Tetracycline hydrochloride (TCH) degradation experiment, the Co 3 O 4 /13X catalyst exhibited the highest specific surface area (490.584 m 2 /g) and provide abundant active sites, enabling 98.0% TCH degradation within 30 min under optimal conditions (1.5 g catalyst, 0.3 mM PMS, pH 8.0, 25℃), with a reaction rate constant (k obs ) of 0.0977 min -1 . In addition, the degradation mechanism of TCH was explored using electron paramagnetic resonance (EPR) spectroscopy and quenching experiments. It was confirmed that free radicals (SO 4 •− , •OH, O 2 •− ) and non-free radical species ( 1 O 2 ) generated during the reaction play a crucial role in the degradation process of TCH. In summary, the Co 3 O 4 /13X catalyst, when activating PMS, exhibits a remarkable synergistic effect on the degradation of TCH, and shows good repeatability and environmental adaptability. This study provides valuable insights into the design and optimization of catalysts for degrading antibiotic pollutants in water treatment processes. Graphical
研究领域:
环境科学
·
催化
·
水处理
·
化学工程
·
污染物降解
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高影响因子
危险品化学品经营许可证（带存储）