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Precursor-driven structural tailoring of iron oxychloride for enhanced heterogeneous Fenton activity

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1533-1543 doi: 10.1007/s11705-023-2330-z

摘要： Iron oxychloride (FeOCl) is a unique layered material with tunable electronic properties. The conventional synthetic route of chemical vapor transition involves a thermodynamics-driven gas–solid interfacial reaction which often generates macroscopic crystals with stable facets. In this study, through analyzing the effects of the synthetic parameters on the FeOCl synthesis, we discovered the dominant contribution of the α-Fe2O3 precursors on the chemical property of the FeOCl product, and subsequently developed a highly-controllable synthetic route of tailoring the FeOCl structures into small sizes and exposed high-energy facets via a facile and scalable mechanical-chemical approach. The synthesized products could be systematically tuned by the ball-milling conditions of the α-Fe2O3 precursors. With increased milling time, the FeOCl crystallites demonstrated reduced sizes and more exposed (110) facets. Intriguingly, these small-sized FeOCl catalysts exhibited much faster Fenton-like kinetics than the pristine macroscopic FeOCl materials. Specifically, FeOCl catalysts with a 12-hour milling time showed nearly 39 times higher efficiency toward phenol degradation than the pristine FeOCl. The structure-reactivity relationship was further elucidated using the combinatory analysis via density functional theory calculation, electron paramagnetic resonance and radical quenching probe experiments. This work provides a rationale for tailoring the surface structures of FeOCl crystallites for potential applications in environmental catalysis.

关键词： FeOCl     mechanical activation     heterogeneous Fenton reaction     ball milling    

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Enhanced heterogeneous Fenton-like activity by Cu-doped BiFeO

Jie Mao, Xie Quan, Jing Wang, Cong Gao, Shuo Chen, Hongtao Yu, Yaobin Zhang

《环境科学与工程前沿（英文）》 2018年 第12卷 第6期 doi: 10.1007/s11783-018-1060-9

摘要：

OH played a key role in heterogeneous Fenton-like catalytic oxidation of organic pollutants.

Doping Cu into BiFeO3 promoted the generation of Fe2+ and then facilitated the effective formation of •OH.

Cu-doped BiFeO3 exhibited higher catalytic performance for phenol degradation than non-doped BiFeO3.

关键词： Cu doped BiFeO3     Heterogeneous Fenton-like catalysts     Oxidative degradation    

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Fe-Mn-sepiolite as an effective heterogeneous Fenton-like catalyst for the decolorization of reactive

Chengyuan SU,Weiguang LI,Xingzhe LIU,Xiaofei HUANG,Xiaodan YU

《环境科学与工程前沿（英文）》 2016年 第10卷 第1期   页码 37-45 doi: 10.1007/s11783-014-0729-y

摘要： A study of the decolorization of reactive brilliant blue in an aqueous solution using Fe-Mn-sepiolite as a heterogeneous Fenton-like catalyst has been performed. The Fourier transform infrared (FTIR) spectra of the catalyst showed bending vibrations of the Fe-O. The X-ray diffraction (XRD) patterns of the catalyst showed characteristic diffraction peaks of α-Fe O , γ-Fe O and MnO. A four factor central composite design (CCD) coupled with response surface methodology (RSM) was applied to evaluate and optimize the important variables (catalyst addition, hydrogen peroxide dosage, initial pH value and initial dye concentration). When the reaction conditions were catalyst dosage= 0.4 g, [H O ]= 0.3 mL, pH= 2.5, [reactive brilliant blue] = 50 mg·L , and volume of solution= 500 mL at room temperature, the decolorization efficiency of reactive brilliant blue was 91.98% within 60 min. Moreover, the Fe-Mn-sepiolite catalyst had good stability for the degradation of reactive brilliant blue even after six cycles. Leaching of iron ions (<0.4 mg·L ) was observed. The decoloring process was reactive brilliant blue specific via a redox reaction. The benzene ring and naphthalene ring were first oxidized to open ring; these were then oxidized to the alcohol and carboxylic acid. The reactive brilliant blue was decomposed mainly by the attack of ·OH radicals including surface-bound ·OH radicals generated on the catalyst surface.

关键词： Fe-Mn-sepiolite catalyst     heterogeneous Fenton-like     reactive brilliant blue     homogeneous precipitation method     hydroxyl radical    

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A review on sustainable reuse applications of Fenton sludge during wastewater treatment

《环境科学与工程前沿（英文）》 2022年 第16卷 第6期 doi: 10.1007/s11783-021-1511-6

摘要：

• The sustainable approaches related to Fenton sludge reuse systems are summarized.

关键词： Fenton sludge     Heavy metals     Coagulant     Iron source     Heterogeneous catalyst    

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Degradation of antipyrine in the Fenton-like process with a La-doped heterogeneous catalyst

Shicheng Wei, Cuiping Zeng, Yaobin Lu, Guangli Liu, Haiping Luo, Renduo Zhang

《环境科学与工程前沿（英文）》 2019年 第13卷 第5期 doi: 10.1007/s11783-019-1149-9

摘要： Abstract A La-doped Co-Cu-Fe catalyst was synthesized for the antipyrine (ANT) removal. The La-doped catalyst had higher ANT removal than the control (95% vs. 54%). La reduced the particle size and increased the specific surface area of catalyst. The aim of this study was to synthesize a novel lanthanum (La) doped catalyst and to investigate antipyrine removal in wastewater using the Fenton-like process with the catalyst. The La-doped Co-Cu-Fe catalyst was synthesized using the modified hydrothermal method. Results showed that the La-doped catalyst had higher specific surface area and lower particle size than the catalyst without La doping (i.e., the control) (267 vs. 163 m2/g and 14 vs. 32 nm, respectively). Under the conditions of catalyst dosage 0.5 g/L, H2O2 concentration 1.70 g/L, and NaHCO3 0.1 g/L, the antipyrine removal within 60 min using the Fenton-like process with the La-doped catalyst was much higher than that with the control (95% vs. 54%). The hydroxyl radical concentration with the La-doped catalyst within 60 min was two times higher than that with the control (49.2 vs. 22.1 mg/L). The high catalytic activity of La-doped catalyst was mainly attributed to its high specific surface area based on the X-ray photoelectron spectroscopy result. Our La-doped catalyst should have great potential to remove antipyrine in wastewater using the heterogeneous Fenton-like process.

关键词： Antipyrine     Lanthanum     Catalyst     Fenton-like process    

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Dual-reaction-center catalytic process continues Fenton’s story

Chao Lu, Kanglan Deng, Chun Hu, Lai Lyu

《环境科学与工程前沿（英文）》 2020年 第14卷 第5期 doi: 10.1007/s11783-020-1261-x

摘要： Abstract • Dual-reaction-center (DRC) system breaks through bottleneck of Fenton reaction. • Utilization of intrinsic electrons of pollutants is realized in DRC system. • DRC catalytic process well continues Fenton’s story. Triggered by global water quality safety issues, the research on wastewater treatment and water purification technology has been greatly developed in recent years. The Fenton technology is particularly powerful due to the rapid attack on pollutants by the generated hydroxyl radicals (•OH). However, both heterogeneous and homogeneous Fenton/Fenton-like technologies follow the classical reaction mechanism, which depends on the oxidation and reduction of the transition metal ions at single sites. So even after a century of development, this reaction still suffers from its inherent bottlenecks in practical application. In recent years, our group has been focusing on studying a novel heterogeneous Fenton catalytic process, and we developed the dual-reaction-center (DRC) system for the first time. In the DRC system, H2O2 and O2 can be efficiently reduced to reactive oxygen species (ROS) in electron-rich centers, while pollutants are captured and oxidized by the electron-deficient centers. The obtained electrons from pollutants are diverted to the electron-rich centers through bonding bridges. This process breaks through the classic Fenton mechanism, and improves the performance and efficiency of pollutant removal in a wide pH range. Here, we provide a brief overview of Fenton’s story and focus on combing the discovery and development of the DRC technology and mechanism in recent years. The construction of the DRC and its performance in the pollutant degradation and interfacial reaction process are described in detail. We look forward to bringing a new perspective to continue Fenton’s story through research and development of DRC technology.

关键词： Dual reaction centers     Fenton     Pollutant utilization     Electron transfer    

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Heterogeneous reaction mechanism of gaseous HNO

Nan ZHAO,Qingzhu ZHANG,Wenxing WANG

《环境科学与工程前沿（英文）》 2016年 第10卷 第5期 doi: 10.1007/s11783-016-0836-z

摘要： We studied the heterogeneous reaction mechanism of gaseous HNO with solid NaCl. HCl is released from heterogeneous reactions between gaseous HNO and solid NaCl. Water molecules induce surface reconstruction of NaCl to facilitate the reaction. Sea salt particles containing NaCl are among the most abundant particulate masses in coastal atmosphere. Reactions involving sea salt particles potentially generate Cl radicals, which are released into coastal atmosphere. Cl radicals play an important role in the nitrogen and O cycles, sulfur chemistry and particle formation in the troposphere of the polluted coastal regions. This paper aimed at the heterogeneous reaction between gaseous HNO and solid NaCl. The mechanism was investigated by density functional theory (DFT). The results imply that water molecules induce the surface reconstruction, which is essential for the heterogeneous reaction. The surface reconstruction on the defective (710) surface has a barrier of 10.24 kcal·mol and is endothermic by 9.69 kcal·mol , whereas the reconstruction on the clean (100) surface has a barrier of 18.46 kcal·mol and is endothermic by 12.96 kcal·mol . The surface reconstruction involved in water-adsorbed (710) surface is more energetically favorable. In comparison, water molecules adsorbed on NaCl (100) surface likely undergo water diffusion or desorption. Further, it reveals that the coordination number of the Cl is reduced after the surface reconstruction, which assists Cl to accept the proton from HNO . HCl is released from heterogeneous reactions between gaseous HNO and solid NaCl and can react with OH free radicals to produce atomic Cl radicals. The results will offer further insights into the impact of gaseous HNO on the air quality of the coastal areas.

关键词： Seasalt particles     NaCl     HNO3     Heterogeneous reaction     Reaction mechanism     Density functional theory    

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Atmospheric heterogeneous reaction of chlorobenzene on mineral -FeO particulates: a chamber experiment

《环境科学与工程前沿（英文）》 2023年 第17卷 第11期 doi: 10.1007/s11783-023-1734-9

摘要：

● Photochemical conversion of chlorobenzene (CB) on α-Fe2O3 was evaluated.

关键词： Photochemical conversion     Chlorobenzene     α-Fe2O3     PCDD/Fs     Mineral particulate    

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Remediation of 2,4-dichlorophenol-contaminated groundwater using nano-sized CaO in a two-dimensional scale tank

《环境科学与工程前沿（英文）》 2020年 第15卷 第5期 doi: 10.1007/s11783-020-1381-3

摘要：

• Nano CaO2 is evaluated as a remediation agent for 2,4-DCP contaminated groundwater.

关键词： Calcium peroxide     2     4-DCP     Reaction zone     Fenton reaction    

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Carbon nanotubes-incorporated MIL-88B-Fe as highly efficient Fenton-like catalyst for degradation of

Hang Zhang, Shuo Chen, Haiguang Zhang, Xinfei Fan, Cong Gao, Hongtao Yu, Xie Quan

《环境科学与工程前沿（英文）》 2019年 第13卷 第2期 doi: 10.1007/s11783-019-1101-z

摘要：

CNTs were incorporated into MIL-88B-Fe to get a new Fenton-like catalyst (C@M).

Fe(II) was introduced in C@M to get a fast initiation of Fenton-like reaction.

Fe(II) content in C@M was related with oxygen-containing functional groups on CNTs.

C@M shows efficient catalytic degradation of pollutants over a wide pH range.

关键词： Heterogeneous Fenton-like catalysts     MIL-88B-Fe     CNTs     Organic pollutants     Mechanism    

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Lignin-based electrospun nanofiber membrane decorated with photo-Fenton Ag@MIF-100(Fe) heterojunctions

《化学科学与工程前沿（英文）》 2023年 第17卷 第7期   页码 930-941 doi: 10.1007/s11705-023-2309-9

摘要： Membrane technology for wastewater remediation has aroused wide interest owing to its unique properties and potential applications. However, it remains challenging to explore green, efficient and robust membrane material and technique for complex wastewater treatment. Herein, we proposed using a simple electrospinning and in situ seeding method to fabricate a lignin-based electrospun nanofiber membrane (LENM) decorated with photo-Fenton Ag@MIL-100(Fe) heterojunctions for efficient separation of oil/water emulsions and degradation of organic dye. Thanks to the embedded lignin in LENM, an ultrahigh MIL-100(Fe) loading (53 wt %) with good wettability and high porosity was obtained. As a result, the hybrid Ag@MIL-100(Fe)/LENM exhibited excellent oil/water emulsions separation efficiency (more than 97%) without a compromise of water flux. Moreover, the hybrid membrane showed an excellent dye removal with degradation of 99% methylene blue within 30 min under illumination, which is attributed to a synergy of dye adsorption/enrichment and photo-Fenton catalytic degradation from Ag@MIL-100(Fe). Therefore, the lignin-based photo-Fenton hybrid membrane can lay the foundation for the preparation and application of green, sustainable and versatile membrane materials and technologies for efficient complex wastewater remediation.

关键词： lignin     electrospinning     heterojunctions     photo-Fenton catalysis     wastewater remediation    

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Physical and chemical processes of wintertime secondary nitrate aerosol formation

Qi YING

《环境科学与工程前沿（英文）》 2011年 第5卷 第3期   页码 348-361 doi: 10.1007/s11783-011-0343-1

摘要： The UCD/CIT model was modified to include a process analysis (PA) scheme for gas and particulate matter (PM) to study the formation of secondary nitrate aerosol during a stagnant wintertime air pollution episode during the California Regional PM /PM Air Quality Study (CRPAQS) where detailed measurements of PM components are available at a few sites. Secondary nitrate is formed in the urban areas from near the ground to a few hundred meters above the surface during the day with a maximum modeled net increase rate of 4 μg·m ·d during the study episode. The secondary nitrate formation rate in rural areas is lower due to lower NO . In the afternoon hours, near-surface temperature can be high enough to evaporate the particulate nitrate. In the nighttime hours, both the gas phase N O reactions with water vapor and the N O heterogeneous reactions with particle-bound water are important for secondary nitrate formation. The N O reactions are most import near the surface to a few hundred meters above surface with a maximum modeled net secondary nitrate increase rate of 1 μg·m ·d and are more significant in the rural areas where the O concentrations are high at night. In general, vertical transport during the day moves the nitrate formed near the surface to higher elevations. During the stagnant days, process analysis indicates that the nitrate concentration in the upper air builds up and leads to a net downward flux of nitrate through vertical diffusion and a rapid increase of surface nitrate concentration.

关键词： secondary nitrate aerosol     N2O5 heterogeneous reaction     process analysis    

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Hydroxyl radical-involved cancer therapy via Fenton reactions

《化学科学与工程前沿（英文）》 2022年 第16卷 第3期   页码 345-363 doi: 10.1007/s11705-021-2077-3

摘要： The tumor microenvironment features over-expressed hydrogen peroxide (H2O2). Thus, versatile therapeutic strategies based on H2O2 as a reaction substrate to generate hydroxyl radical (•OH) have been used as a prospective therapeutic method to boost anticancer efficiency. However, the limited Fenton catalysts and insufficient endogenous H2O2 content in tumor sites greatly hinder •OH production, failing to achieve the desired therapeutic effect. Therefore, supplying Fenton catalysts and elevating H2O2 levels into cancer cells are effective strategies to improve •OH generation. These therapeutic strategies are systematically discussed in this review. Furthermore, the challenges and future developments of hydroxyl radical-involved cancer therapy are discussed to improve therapeutic efficacy.

关键词： hydroxyl radical     Fenton catalyst     hydrogen peroxide     cancer therapy    

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Enhanced Fenton-like process over Cu/L(+)-ascorbic acid co-doping mesoporous silica for toxicity reduction

《环境科学与工程前沿（英文）》 2023年 第18卷 第4期 doi: 10.1007/s11783-024-1804-7

摘要：

● Cu-C-MSNs are developed via a co-doping step of Cu with L(+)-ascorbic acid.

关键词： Cation-π structures     Polarization electric field     Fenton-like process     Contaminants cleavage    

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treatment using the combination of the microbial electrolysis desalination and chemical-production cell and Fenton

Songwei Lin, Yaobin Lu, Bo Ye, Cuiping Zeng, Guangli Liu, Jieling Li, Haiping Luo, Renduo Zhang

《环境科学与工程前沿（英文）》 2020年 第14卷 第1期 doi: 10.1007/s11783-019-1191-7

摘要： MEDCC combined with Fenton process was developed to treat real pesticide wastewater. Pesticide removal was attributable to desalination in the MEDCC. High COD removal was attributable to organic distributions in different chambers. The combination of the microbial electrolysis desalination and chemical-production cell (MEDCC) and Fenton process for the pesticide wastewater treatment was investigate in this study. Real wastewater with several toxic pesticides, 1633 mg/L COD, and 200 in chromaticity was used for the investigation. Results showed that desalination in the desalination chamber of MEDCC reached 78%. Organics with low molecular weights in the desalination chamber could be removed from the desalination chamber, resulting in 28% and 23% of the total COD in the acid-production and cathode chambers, respectively. The desalination in the desalination chamber and organic transfer contributed to removal of pesticides (e.g., triadimefon), which could not be removed with other methods, and of the organics with low molecular weights. The COD in the effluent of the MEDCC combined the Fenton process was much lower than that in the perixo-coagulaiton process (<150 vs. 555 mg/L). The combined method consumed much less energy and acid for the pH adjustment than that the Fenton.

关键词： Pesticide wastewater     COD removal     Microbial electrolysis desalination and chemical-production cell     Energy consumption     Fenton oxidation    

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标题 作者 时间 类型 操作

Precursor-driven structural tailoring of iron oxychloride for enhanced heterogeneous Fenton activity

期刊论文

Enhanced heterogeneous Fenton-like activity by Cu-doped BiFeO

Jie Mao, Xie Quan, Jing Wang, Cong Gao, Shuo Chen, Hongtao Yu, Yaobin Zhang

期刊论文

Fe-Mn-sepiolite as an effective heterogeneous Fenton-like catalyst for the decolorization of reactive

Chengyuan SU,Weiguang LI,Xingzhe LIU,Xiaofei HUANG,Xiaodan YU

期刊论文

A review on sustainable reuse applications of Fenton sludge during wastewater treatment

期刊论文

Degradation of antipyrine in the Fenton-like process with a La-doped heterogeneous catalyst

Shicheng Wei, Cuiping Zeng, Yaobin Lu, Guangli Liu, Haiping Luo, Renduo Zhang

期刊论文

Dual-reaction-center catalytic process continues Fenton’s story

Chao Lu, Kanglan Deng, Chun Hu, Lai Lyu

期刊论文

Heterogeneous reaction mechanism of gaseous HNO

Nan ZHAO,Qingzhu ZHANG,Wenxing WANG

期刊论文

Atmospheric heterogeneous reaction of chlorobenzene on mineral -FeO particulates: a chamber experiment

期刊论文

Remediation of 2,4-dichlorophenol-contaminated groundwater using nano-sized CaO in a two-dimensional scale tank

期刊论文

Carbon nanotubes-incorporated MIL-88B-Fe as highly efficient Fenton-like catalyst for degradation of

Hang Zhang, Shuo Chen, Haiguang Zhang, Xinfei Fan, Cong Gao, Hongtao Yu, Xie Quan

期刊论文

Lignin-based electrospun nanofiber membrane decorated with photo-Fenton Ag@MIF-100(Fe) heterojunctions

期刊论文

Physical and chemical processes of wintertime secondary nitrate aerosol formation

Qi YING

期刊论文

Hydroxyl radical-involved cancer therapy via Fenton reactions

期刊论文

Enhanced Fenton-like process over Cu/L(+)-ascorbic acid co-doping mesoporous silica for toxicity reduction

期刊论文

treatment using the combination of the microbial electrolysis desalination and chemical-production cell and Fenton

Songwei Lin, Yaobin Lu, Bo Ye, Cuiping Zeng, Guangli Liu, Jieling Li, Haiping Luo, Renduo Zhang

期刊论文