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WASTE MANAGEMENT · 2021 · IF 7.145

Optimization of heterogeneous Fenton-like process with Cu-Fe@CTS as catalyst for degradation of organic matter in leachate concentrate and degradation mechanism research

Chengrui Guo,Xia Qin,Rui Guo,Yue Lv,Mingran Li,Ziyuan Wang,Tinghui Li

The heterogeneous Fenton-like process with bimetallic chelated magnetic chitosan aerogel (Cu-Fe@CTS) as catalyst was applied to treat pre-coagulated leachate nanofiltration concentrate. The process conditions were optimized by Box-Behnken Design (BBD) and the maximum UV 254 removal reached 96.06% under the conditions of temperature 87.62 °C, oxidant dosage 0.2395 mol/L and catalyst dosage 1 g/L. The TOC concentration was reduced from 847.5 to 99.7 mg/L and COD concentration was reduced from 1625 to 464 mg/L. The three-dimensional (3D) fluorescence analysis showed that most of Fulvic acid-like (FA-like) was removed. The adsorption experiment showed that the catalyst reached the adsorption balanced after 60 min and the corresponding FA adsorption removal reached 14.1%. The addition of Tert-butanol (TBA) reduced the FA removal by 59.4%, indicating that the hydroxyl radicals ( OH) was the main active species. Experiments of the OH capture at different pH showed that the Fenton-like system produced more OH at pH of 4, at which the maximum FA removal was 96.61%, while the FA removal still reached 94.26% at pH of 7. The OH capture at different temperature showed that the Fenton-like system produced more OH at 90 °C. KI and TBA shielding experiments showed that OH was produced on the catalyst surface rather than being produced by catalysis of free metal ions in the solution.

研究领域: 环境科学 · 催化化学
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION · 2025 · IF 7.8

Simultaneous removal of phosphate and hydroquinone using Fe3Ce1Ox(CA)/H2O2 Fenton-like system

Daoqing Liu,Qing Wang,Biao Wei,Shaoxia Yang,Qianwei Li,Huazhang Zhao

Phosphates and organic matter usually coexist in secondary effluent, adversely affecting the stable control of water quality. Therefore, achieving the simultaneous removal of phosphates and organic matter from water bodies is significant. This study reports an excellent Fe₃Ce₁Oₓ(CA) functional material synthesized via a simple one-step co-precipitation method for hydroquinone (HQ) degradation through a Fenton-like reaction while simultaneously adsorbing phosphate. Experimental results show that the Fe₃Ce₁Oₓ(CA) materials exhibit a 92 % HQ degradation efficiency and an 80 % phosphate adsorption efficiency. Systematic characterization confirms that the Fe–Ce synergistic effect enhances the Fe(II) content, significantly promoting H₂O₂ activation. Electron paramagnetic resonance and radical scavenger experiments reveal that ¹O₂, O₂ • ⁻, and •OH play essential roles in organic degradation, with •OH being the dominant reactive species. Introducing citric acid increases the Ce(III) content in the Fe–Ce bimetallic oxide composite, enhancing its phosphate adsorption performance. This material successfully achieves both HQ degradation and phosphate removal, and these findings suggest that the Fe₃Ce₁Oₓ(CA)/H₂O₂ system can potentially treat wastewater with combined organic and phosphate pollution. This approach, which achieves multifunctionality in water treatment by regulating the composition of environmental functional materials, enhances the practical application potential of such materials.

研究领域: 环境科学 · 材料科学
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Journal of Environmental Chemical Engineering · 2025 · IF 7.2

A trash-to-treasure approach of deriving Cu-doped carbonaceous catalysts from disposable masks motivating peroxymonosulfate decomposition and organics high-efficiency mineralization

Xue Bai,Min Hu,Baojia Tian,Yujia Han,Juan Shi,Lu Xu,Xin Jin,Xuan Shi,Pengkang Jin

The past global pandemic of COVID-19 made people be accustomed to wear disposable face masks to defend against epidemic disease, posing significant challenges in proper disposal of numerous plastic wastes. Herein, a simple immersion and calcination approach was proposed to convert polypropylene-based masks into Cu-doped carbonaceous catalysts (Cu x -DMC) for efficient peroxymonosulfate (PMS) activation and wastewater purification. After immersion in a 0.02 M CuSO 4 solution, the resulting Cu 0.02 -DMC exhibited a larger surface area and highly abundant reactive sites than the undoped sample, indicating excellent catalytic performance. Upon the addition of 1 mM PMS, 100 mL 10 mg/L of seven representative organics were almost completely degraded within 30 min. The resulting mineralization efficiencies ranged from 41 % to 65 %. Additionally, rapid purification of both actual lake water and municipal secondary effluent was obtained. Such high efficiency was attributed to 1 O 2 , O 2 ·- , ·OH and SO 4 ·- produced in PMS activation process, during which the formed [Cu(Ⅱ)OOSO 3 - ] metastable intermediate on Cu 0.02 -DMC surface and the redox cycles between different Cu chemical states played crucial roles. Owing to the high efficiency in PMS activation, anti-interference ability for complex water matrices, and high stability for reuse, Cu x -DMC derived from “trash-to-treasure” approach exhibited potential applications in wastewater treatment.

研究领域: 环境科学 · 材料科学
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2024 · IF 4.1

Oxygen vacancy-induced nonradical degradation of nitroso-containing organics in Fe3O4@NC electro-Fenton reaction at a wide pH range

Qian Zhang,Xiaoqin Sun,Yuan Dang,Jun-Jie Zhu,Yuanzhen Zhou

In this work, Fe 3 O 4 -anchored nitrogen-doped carbon catalyst (Fe 3 O 4 @N–C) with abundant oxygen vacancies (V o ) and mesoporous structure was successfully synthesized for electro-Fenton (EF) catalytic process. The catalyst demonstrated impressive degradation efficiency towards nitroso-containing organics due to the superior electronic transfer of N–C skeleton and V o , making it easier for the electron-deficient –NO 2 groups to adsorb on the catalyst surface and oxidize rapidly. Typically, the degradation efficiency of p-nitrophenol (PNP) reached 95.6 % in natural pH. Notably, the catalyst exhibited excellent performance over a wide pH range (3 ∼ 11), and has strong anti-interference performance against anions and natural organic matter in water matrix. Mechanism analysis indicated that V o could promote the formation of highly active electron-rich Fe(II) species, and promote the activation of H 2 O 2 and O 2 as additional active sites, thus, a large amount of ·OH and O 2 ·- would be produced and then quickly converted into 1 O 2 . As a result, 1 O 2 is the main reactive species for PNP degradation in Fe 3 O 4 @N–C electro-Fenton reaction. The results will provide insights into the design of high-performance catalysts for the selective oxidation of organic pollutants in wastewater.

研究领域: 环境科学 · 催化材料
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Nano Energy · 2022 · IF 19.069

Self-powered triboelectric nanogenerator driven nanowires electrode array system for the urine sterilization

Xinmeng Zhang,Haoqiang Huang,Weinan Zhang,Zulu Hu,Xiang Li,Jia Liu,Gaixia Xu,Chengbin Yang

Urine is the primary source of pathogens (viruses, fungi, and bacteria) in urban sewage. The epidemic spread of these pathogens has a severe threat to human health and the ecological environment. The traditional sewage sterilization methods usually produce harmful by-products and have high energy consumption. These weaknesses restrict the quality of the purified water and economic benefits. Herein, we elaborately fabricated a triboelectric nanogenerator driving nanowires electrode array (T-NEA) system for removing bacteria in the urine. An irreversible electroporation damage results in high-efficiency bacteria inactivation. The sterilization efficiency of T-NEA system is more than 99.9999% in artificial urine contaminated by Escherichia coli ( E. coli ), Staphylococcus aureus ( S. aureus ) and Klebsiella pneumoniae (K. pneumoniae), Pseudomonas aeruginosa (P. aeruginosa) . Those bacteria could cause epidemic infection in hospital. The electroporation effect on the bacterial membrane was confirmed by SEM imaging and confocal laser scanning microscopy . In addition, it was demonstrated that the radical oxygen species accompanied by T-NEA working could degrade the organic components in artificial urine. After being treated by T-NEA for 30 mins, the reduction rates of the total organic carbon and total nitrogen in the artificial urine reached up to 30.41% and 33.79%. Meanwhile, the degradation degree of urea, uric acid, and creatinine reached 37.39%, 30.50%, 6.25%, respectively. And the degradation mechanism of organic materials in urine was also investigated. This work provided an effective self-powered system which could totally remove the hazardous bacteria and degrade the organics in the urine.

研究领域: 环境科学 · 生物医学工程 · 微生物学
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CHEMOSPHERE · 2022 · IF 8.943

Efficient organics heterogeneous degradation by spinel CuFe2O4 supported porous carbon nitride catalyst: Multiple electron transfer pathways for reactive oxygen species generation

Ting Chen,Zhiliang Zhu,Yue Wang,Hua Zhang,Yanling Qiu,Daqiang Yin

Facilitating reactive oxygen species (ROS) generation is an effective way to promote the heterogeneous catalytic efficiency for organics removal. However, the metal leaching in metal-based catalysts and the low activity of non-metallic materials restrict ROS production. In this work, the purpose was achieved by loading a small amount of spinel CuFe 2 O 4 onto porous carbon nitride substrate. The synthesized CuFe 2 O 4 @O–CN composite first to activate peroxymonosulfate (PMS), which produce a plenty of ROS (•OH, SO 4 • − and 1 O 2 ) for organics removal, leading to highly oxidation for diverse organics. Through the comparative analysis of the surface composition before and after reaction, we found that the interface multi-electron transfer routs, including surface Cu(II)/Cu(I), Fe(III)/Fe(II) and their cross interaction, participated in the redox cycle, giving rise to the rapid and massive production of ROS, so that DMPO and TEMP were instantly oxidized in electron paramagnetic resonance (ESR) detection. Importantly, the carrier of porous O–CN, which acted as the electron transfer mediator, not only favors PMS adsorption via surface –OH, but also facilitates the conversion between different metal species. As a result, the CuFe 2 O 4 @O–CN/PMS system can remove 99.1% BPA and achieve 52.6% mineralization under optimized conditions. Thus, this study not only sheds light on the tailored design of heterogeneous catalyst for organics removal and elucidates the interfacial catalytic mechanisms for PMS activation .

研究领域: 环境科学 · 催化化学
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SCIENCE OF THE TOTAL ENVIRONMENT · 2022 · IF 10.753

Efficient catalytic ozonation via Mn-loaded C-SiO2 Framework for advanced wastewater treatment: Reactive oxygen species evolution and catalytic mechanism

Shuning Chen,Tengfei Ren,Xiaoying Zhang,Zuoyong Zhou,Xia Huang,Xiaoyuan Zhang

Heterogeneous catalytic ozonation (HCO) is attractive for water decontamination and catalyst is a core element. However, it is difficult to maintain high efficiency and stability of catalysts under stern conditions. In this study, we proposed Mn-loaded C-SiO 2 -Framework (Mn-CSF) which contained stable silica core and robust carbon shell for efficient catalytic ozonation. The pseudo-first-order kinetic rate constant for oxalic acid removal of Mn-CSF catalytic ozonation was 160 % and 875 % higher than those of Mn-SiO 2 and pristine CSF, respectively. Mn-CSF was also proven effective in gasification wastewater treatment , where the COD was decreased to 46 mg·L −1 , 37 % lower than that of Mn-SiO 2 . These results indicated that the graphitization carbon layer and Mn significantly enhanced the activity of the catalyst. Furthermore, a fulvic-like component and a protein-like component were recognized through 3D-EEM in coal gasification wastewater. It was proven that Mn-CSF catalytic ozonation exhibited higher fulvic-like component and protein-like component removal compared with ozonation. Moreover, O 2 − and 1 O 2 were identified to be responsible for organic degradation in this research. Sufficient external specific surface area and porous structure were important for complex wastewater treatment. Specifically, external specific surface area could enhance the degradation of macromolecular organics while porous structures were vital for smaller molecular pollutant removal . The results highlighted that Mn-CSF was a promising HCO catalyst for advanced wastewater treatment, and this study provided evidence of relationship between structure of catalysts and HCO efficiency.

CAS / MDL: 7778-53-2
研究领域: 环境科学 · 化学工程
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JOURNAL OF HAZARDOUS MATERIALS · 2023 · IF 13.6

Comparative study of UV/chlorine and VUV/chlorine as ultrafiltration membrane pretreatment techniques: Performance, mechanisms and DBPs formation

Shengnan Chen,Zhiwei Zhao,Fuyi Cui,Bingyan Liu

Membrane fouling , primarily resulting from natural organic matter (NOM) widely existing in water sources, has always been a chief hindrance for the prevalent application of ultrafiltration (UF). Thus, vacuum ultraviolet (VUV)/chlorine process was proposed as a strategy for UF membrane fouling control and ultraviolet (UV)/chlorine process was used for comparison. VUV/chlorine process exhibited more excellent performance on NOM removal than UV/chlorine process. [HO•]ss and [Cl•]ss were calculated as 1.26 × 10 −13 and 3.06 × 10 −14 M, respectively, and ClO• might not exist under the conditions of 0.08 mM chlorine and 30 min VUV irradiation. [HO•]ss, [Cl•]ss and [ClO•]ss were not available and the formation of reactive radicals was unsustainable in UV/chlorine system. Moreover, VUV/chlorine pretreatment also showed better performance on the reversible and irreversible membrane fouling control than UV/chlorine pretreatment. The dominated fouling mechanism in the final stage of filtration was cake filtration. Additionally, the amount of detected disinfection by-products (DBPs) in VUV/chlorine system was significantly lower than that in UV/chlorine system. During subsequent chlorination disinfection, the yield of DBPs with VUV/chorine pretreatment was higher than that with UV/chlorine pretreatment. VUV/chlorine pretreatment could effectively control DBPs formation when the pretreatment time was extended to 120 min. In summary, VUV/chlorine system presented a most excellent performance on membrane fouling control, NOM degradation and DBPs control.

研究领域: 环境科学 · 水处理工程
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CHINESE CHEMICAL LETTERS · 2023 · IF 9.1

Enhanced degradation of refractory organics in ORR-EO system with a blue TiO2 nanotube array modified Ti-based Ni-Sb co-doped SnO2 anode

Yifen He,Chao Qu,Na Ren,Dawei Liang

ABSTRACT Recently, a novel 2-electron oxygen reduction reaction (ORR) based electro-oxidation (EO) system was developed, which utilizes a H 2 O 2 generation cathode instead of H 2 evolution cathode. A Ti-based Ni-Sb co-doped SnO 2 (Ti/NATO) anode was selected for efficient degradation of refractory organics and O 3 production. The synergistic reaction of O 3 /H 2 O 2 further accelerated the generation of hydroxyl radicals ( • OH) in the ORR-EO system. However, the catalytic activity and long-term effectiveness of the Ti/NATO anode limited the large-scale application of the ORR-EO process. In this study, a blue TiO 2 nanotube array (blue-TiO 2 -NTA) inter-layer was introduced into the fabrication process between the Ti substrate and NATO catalyst layer. Compared to the Ti/NATO anode, the Ti/blue-TiO 2 -NTA/NATO anode achieved higher efficiency of organic removal and O 3 generation. Additionally, the accelerated lifetime of the Ti/blue-TiO 2 -NTA/NATO anode was increased by 7 times compared to the Ti/NATO anode. When combined with CNTs-C/PTFE air cathode in ORR-EO system, all anodic oxidation and O 3 /H 2 O 2 processes achieved higher • OH production. Over 92% of TOC in leachate bio-effluent was effectively eliminated with a relatively low energy cost of 45 kWh/t.

研究领域: 环境科学 · 材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Construction of hollow sphere MnOX with abundant oxygen vacancy for accelerating VOCs degradation: Investigation through operando spectroscopycombined with on-line mass spectrometry

Fada Feng,Yikui Zeng,Dengfeng Yan,Quanming Ren,Bang Lan,Jinping Zhong,Biyuan Liu,Tao Dong,Haibao Huang

To clarify the key role of oxygen vacancy defects on enhancing the oxidative activity of the catalysts, metal–organic frameworks (MOFs) derived MnO X catalysts with different morphologies and oxygen vacancy defects were successfully prepared using a facile in-situ self-assembly strategy with different alkali moderators. The obtained morphologies included three-dimensional (3D) triangular cone stacked MnO X hollow sphere (MnO X -H) and 3D nanoparticle stacked MnO X nanosphere (MnO X -N). Compared to MnO X -N, MnO X -H exhibited higher activity for the oxidation of toluene (T 90  = 226 °C). This was mainly due to the large number of oxygen vacancy defects and Mn 4+ species in the MnO X -H catalyst. In addition, the hollow structure of MnO X -H not only facilitated toluene adsorption and activation of toluene and also provided more active sites for toluene oxidation. Reaction mechanism studies showed that the conversion of toluene to benzoate could be realized over MnO X -H catalyst during toluene adsorption at room temperature. In addition, abundant oxygen vacancy defects can accelerate the activated oxidation of toluene and the formation of oxidation products during toluene oxidation.

研究领域: 催化材料科学 · 环境科学 · 化学工程
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Surfaces and Interfaces · 2024 · IF 5.7

Photocatalytic peroxydisulfate activation for dissolved organic matter degradation in eutrophic lake water using S-scheme BiVO4/g-C3N4 3D/2D heterojunction under visible light

Feihu Mu,Shengpan Xu,Meixin Li,Yuqiu Yang,Xiaozhong Chu,Zhipeng Cheng,Xujing Guo,Jiming Xu,Benlin Dai,Chang-Ha Lee

Large amounts of carbon are stored primarily in dissolved organic matter (DOM), which plays an important indicator of lake eutrophication. However, removing DOM from eutrophic lakes remains a major challenge. Herein, a novel S-scheme flower-like microsphere BiVO 4 /nanosheet g-C 3 N 4 3D/2D heterojunction was successfully constructed using a two-step method for DOM degradation of real eutrophic lake water in the presence of peroxydisulfate (PDS). 1.0-BiVO 4 /g-C 3 N 4 /PDS exhibited highly efficient photocatalytic performance with an 87.8 % removal rate of DOM for 60 min, which was 5.3 and 8.9 times higher than BiVO 4 /PDS and g-C 3 N 4 /PDS, respectively. Sulfate radical (·SO 4 − ), hydroxyl radical (·OH) and singlet oxygen ( 1 O 2 ) were mainly responsible for DOM degradation in the 1.0-BiVO 4 /g-C 3 N 4 /PDS system, and the transformation pathway of 1 O 2 was emphatically analyzed. In addition, the changes of fluorescence components in DOM were detected using synchronous fluorescence spectra, second derivative spectra, and two-dimensional correlated spectroscopy analysis. Humic-like fluorescence, fulvic-like fluorescence, and protein-like substances were removed higher than 85.30 %, 73.02 %, and 67.23 % by the 1.0-BiVO 4 /g-C 3 N 4 catalyst activating the PDS under visible light (VL), respectively. When the toxicity of catalytically treated eutrophic lake water was estimated by growth inhibition of Escherichia coli , the biotoxicity of DOM decreased continuously in the BiVO 4 /g-C 3 N 4 /PDS/VL coupling process. Theoretical calculations and photoelectrochemical tests suggested that the BiVO 4 /g-C 3 N 4 /PDS catalytic activity enhancement was attributed to the S-scheme mechanism and hybrid advanced oxidation process. It is expected that this work can provide new insight into DOM degradation in eutrophic lake water by the heterogeneous photocatalysis combined with the PDS activation system.

CAS / MDL: 7727-54-0
研究领域: 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Construction of Pd/Mn3O4 heterojunction catalyst for efficient photothermal synergetic catalytic propane total oxidation

Chao Feng,Yuxi Bi,Chong Chen,Yunxia Wang,Shuangju Li,Yuan Pan,Hongchuan Xin,Yukun Lu,Fang Liu,Xuebing Li,Yunqi Liu,Runduo Zhang,Zhong Wang

Photothermal synergistic low-temperature catalytic volatile organic compounds (VOCs) degradation has an advantage on energy efficiency and reduction of carbon emissions. Herein, an impregnation-pyrolysis-oxidation strategy was adopted to synthesize Pd/Mn 3 O 4 heterojunction catalyst. Under photothermal synergistic conditions, 0.60Pd/Mn 3 O 4 catalyst exhibited an excellent activity for propane total oxidation, with a T 90 value of 219.1 ℃, which was 115.3 ℃ lower than that of Mn 3 O 4 . Enhancement effect of the heterojunction structure on photothermal synergy was detected by various characterization techniques and density functional theory calculation. The presence of Pd species enhanced the low-temperature reducibility of Mn 3 O 4 . Meanwhile, O 2 molecules were more easily activated at the Pd sites and overflow to the surface of Mn 3 O 4 for reaction. Besides, the formation of p-n junction between Pd species and Mn 3 O 4 in heterojunction structure promoted the charge separation and the migration of carriers, and boosted the generation of oxygen free radical, resulting in a significant improvement in photothermal catalytic activity. Overall, this study provided new strategy and deep insight for constructing heterojunction to enhance photothermal catalytic performance of VOC elimination.

研究领域: 环境科学 · 催化化学 · 材料科学
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