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Atomically dispersed Fe-N5 sites with optimized electronic structure for sustainable wastewater purification via efficient Fenton-like catalysis SCIE
期刊论文 | 2024 , 358 | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
摘要&关键词 引用

摘要 :

Herein, a single-atom catalyst (SAC) featuring Fe-N-5 sites (FeNC) with optimized electronic structures was constructed and applied to activate peroxymonosulfate (PMS) for wastewater purification. The high-coordinated Fe-N-5 sites was obtained by creating a high-nitrogen gas environment around fully exposed Fe atomic sites on chitosan surface during pyrolysis. The FeNC/PMS system demonstrated excellent decontamination capability, superior anti-pH interference ability, while also exceptional durability in a continuous-flow catalytic filtration reactor. Experiments and density functional theory calculations unveiled that Fe-N-5 site was the active center. Meaningfully, neighboring carbonyl groups narrowed the gap between d-band center of Fe 3d and Fermi level, which increased the adsorption energy of PMS on Fe-N-5 sites, thus lowering the energy barrier for singlet oxygen generation. This study brings a vivid electronic structure optimization strategy for enhancing the catalytic activity of Fe SAC as well as guiding the selection of desirable catalysts for wastewater purification by Fenton-like chemistry.

关键词 :

Electronic structure optimization Electronic structure optimization High-coordinated M-N-x sites High-coordinated M-N-x sites Density functional theory Density functional theory Fenton-like reaction Fenton-like reaction Single-atom catalysts Single-atom catalysts

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GB/T 7714 Li, Yanan , Wei, Jia , Cui, Nan et al. Atomically dispersed Fe-N5 sites with optimized electronic structure for sustainable wastewater purification via efficient Fenton-like catalysis [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2024 , 358 .
MLA Li, Yanan et al. "Atomically dispersed Fe-N5 sites with optimized electronic structure for sustainable wastewater purification via efficient Fenton-like catalysis" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 358 (2024) .
APA Li, Yanan , Wei, Jia , Cui, Nan , Li, Jiamei , Ji, Wei , Wang, Linhao et al. Atomically dispersed Fe-N5 sites with optimized electronic structure for sustainable wastewater purification via efficient Fenton-like catalysis . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2024 , 358 .
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Highly efficient elimination of organic contaminants by boron-doped biochar modified dual-cathode electro-Fenton system SCIE
期刊论文 | 2024 , 342 | SEPARATION AND PURIFICATION TECHNOLOGY
摘要&关键词 引用

摘要 :

Electro-Fenton (EF) process stands out as an energy-efficient and highly promising advanced oxidation technology for organic contaminants degradation. However, achieving optimal heterogeneous catalytic conditions for simultaneous H2O2 generation and spontaneous Fe2+ regeneration poses difficulties in conventional EF. This is due to the electric potential difference between H2O2 generation and Fe2+ regeneration at a single cathode. Therefore, the boron doped biochar modified dual-cathode EF (DCEF) system was designed in this work to overcome the defect of conventional EF system, which not only demonstrated outstanding accumulation of H2O2 (>300 mg L-1) but also exhibited a remarkable capability of degradation (>90 %). Furthermore, the system could also adapt to a broad pH range of 3-11. The superior doxycycline (DOX) degradation efficiency of DCEF system could be attributed to the dominant role played by C=O and BCO2 groups in the activation of H2O2 and subsequently generating reactive oxygen species (ROSs), as revealed by XPS analysis and DFT calculation. In addition, the DCEF system achieved an impressive TOC removal efficiency of 70.5 % and a minimal energy consumption (EC) of 0.32 kWh (g TOC)(-1). Therefore, this work introduced a DCEF system to address the challenges of conventional EF system, which shed light on the design of wastewater treatment technology and lied the groundwork for a strategy of resource utilization.

关键词 :

Electro-Fenton Electro-Fenton Dual -cathode Dual -cathode Biochar Biochar Boron doping Boron doping Dual active sites Dual active sites

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GB/T 7714 Cui, Xueru , Wei, Jia , Jiang, Zijian et al. Highly efficient elimination of organic contaminants by boron-doped biochar modified dual-cathode electro-Fenton system [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 342 .
MLA Cui, Xueru et al. "Highly efficient elimination of organic contaminants by boron-doped biochar modified dual-cathode electro-Fenton system" . | SEPARATION AND PURIFICATION TECHNOLOGY 342 (2024) .
APA Cui, Xueru , Wei, Jia , Jiang, Zijian , Niu, Xiruo , Li, Yanan , Cui, Nan et al. Highly efficient elimination of organic contaminants by boron-doped biochar modified dual-cathode electro-Fenton system . | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 342 .
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一种高效产生H2O2的硼掺杂生物质炭阴极及其制备方法和应用 incoPat
专利 | 2023-07-06 | CN202310827712.X
摘要&关键词 引用

摘要 :

本发明提供了一种高效产生H2O2的硼掺杂生物质炭阴极及其制备方法和应用,属于水处理电化学高级氧化技术领域。本发明将硼酸溶液与生物质粉末混合后依次进行加热、第一冷却、过滤、烘干、煅烧、第二冷却、洗涤和干燥后获硼掺杂生物质炭粉末;将炭黑、硼掺杂生物质炭粉末、聚四氟乙烯分散液和无水乙醇混合并超声分散之后加热搅拌得到硼掺杂生物质炭浆料;将硼掺杂生物质炭浆料粘结于泡沫镍上通过高温固化得到硼掺杂生物质炭阴极。本发明利用非金属元素硼掺杂时,以缺电子硼取代碳形成B‑C键,在硼原子附近产生正电荷,有利于吸附H2O2,且无铁泥的产生。与传统电芬顿相比,无需外源加入H2O2和Fe2+,可在原位同时产生活化H2O2,产生羟基自由基降解污染物。

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GB/T 7714 魏佳 , 崔雪茹 , 李晓非 . 一种高效产生H2O2的硼掺杂生物质炭阴极及其制备方法和应用 : CN202310827712.X[P]. | 2023-07-06 .
MLA 魏佳 et al. "一种高效产生H2O2的硼掺杂生物质炭阴极及其制备方法和应用" : CN202310827712.X. | 2023-07-06 .
APA 魏佳 , 崔雪茹 , 李晓非 . 一种高效产生H2O2的硼掺杂生物质炭阴极及其制备方法和应用 : CN202310827712.X. | 2023-07-06 .
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一种八硫化七铁负载生物炭催化剂的制备方法及应用 incoPat
专利 | 2023-02-27 | CN202310170156.3
摘要&关键词 引用

摘要 :

本发明公开了一种八硫化七铁负载生物炭催化剂的制备方法及应用,属于污水处理技术领域。该催化剂的制备方法为:将生物炭原料、六水合氯化铁、硫脲在乙二醇中完全溶解,通过溶剂热法得到八硫化七铁负载生物质前驱体,经热解法后得到八硫化七铁负载生物炭催化剂,将该催化剂和过一硫酸盐加入含有抗生素的水体中,通过以单线态氧为主的非自由基途径实现水体中抗生素的去除,本发明的催化剂制备方法简单,对抗生素去除效率高,pH、温度适用范围广泛,具有较大的比表面积,易回收利用,适合工业化生产。

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GB/T 7714 魏佳 , 姜子建 . 一种八硫化七铁负载生物炭催化剂的制备方法及应用 : CN202310170156.3[P]. | 2023-02-27 .
MLA 魏佳 et al. "一种八硫化七铁负载生物炭催化剂的制备方法及应用" : CN202310170156.3. | 2023-02-27 .
APA 魏佳 , 姜子建 . 一种八硫化七铁负载生物炭催化剂的制备方法及应用 : CN202310170156.3. | 2023-02-27 .
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Highly dispersed Fe7S8 anchored on sp2/sp3 hybridized carbon boosting peroxymonosulfate activation for enhanced EOCs elimination though singlet oxygen-dominated nonradical pathway SCIE
期刊论文 | 2023 , 461 | JOURNAL OF HAZARDOUS MATERIALS
摘要&关键词 引用

摘要 :

The synergistic effect of carbon materials with high sp(2)/sp(3 )hybridized carbon ratio and metal materials can enhance the efficiency of peroxymonosulfate (PMS) based advanced oxidation processes. In this study, a composite of highly dispersed Fe(7)S(8 )anchored on sp(2)/sp(3) hybridized carbon (Fe7S8@HC) was developed by a facile synthesis for PMS activation. Within 10 min, the removal efficiency of the target pollutant doxycycline (DOX) could reach ca. 96 % in optimal Fe7S8@HC/PMS system through a O-1(2)-dominated non-radical pathway. Correlation mechanism analysis revealed that thiophene S, sp(2)/sp(3 )ratio and Fe(II) were critical factors for elongating of the O-O bond of PMS. Moreover, the Fe7S8@HC/PMS system exhibited favorable adaptability to interference such as common inorganic anions, humic acid and pH changes and could effectively remove various organic pollutants with low ionization potential. Moreover, the system maintained high DOX removal efficiency by running 30 cycles in a continuous flow reactor. Finally, susceptible sites of DOX and four degradation pathways were proposed by density functional theory calculation and LC-MS detection. This work not only offered new insights into the design of high-performance catalysts combining metal and biomass-based carbon materials, but also provided technical support for the remediation of water bodies containing emerging organic contaminants.

关键词 :

Peroxymonosulfate Peroxymonosulfate Singlet oxygen Singlet oxygen Hybridized carbon Hybridized carbon Fe7S8 Fe7S8 Emerging organic contaminants Emerging organic contaminants

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GB/T 7714 Jiang, Zijian , Wei, Jia , Niu, Xiruo et al. Highly dispersed Fe7S8 anchored on sp2/sp3 hybridized carbon boosting peroxymonosulfate activation for enhanced EOCs elimination though singlet oxygen-dominated nonradical pathway [J]. | JOURNAL OF HAZARDOUS MATERIALS , 2023 , 461 .
MLA Jiang, Zijian et al. "Highly dispersed Fe7S8 anchored on sp2/sp3 hybridized carbon boosting peroxymonosulfate activation for enhanced EOCs elimination though singlet oxygen-dominated nonradical pathway" . | JOURNAL OF HAZARDOUS MATERIALS 461 (2023) .
APA Jiang, Zijian , Wei, Jia , Niu, Xiruo , Cui, Xueru , Li, Yanan , Cui, Nan et al. Highly dispersed Fe7S8 anchored on sp2/sp3 hybridized carbon boosting peroxymonosulfate activation for enhanced EOCs elimination though singlet oxygen-dominated nonradical pathway . | JOURNAL OF HAZARDOUS MATERIALS , 2023 , 461 .
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Biochar-activated persulfate oxidation of arsenic(III): Nonnegligible roles of environmentally persistent free radicals SCIE
期刊论文 | 2023 , 11 (5) | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
摘要&关键词 引用

摘要 :

The water ecosystem and public health are often threatened by Arsenic (As). The primary type of As in paddy field and ground water is As(III), which is more toxic and mobile than As(V). In this research, biochar prepared from sewage sludge (SBC) through hydrothermal technique was used to activate persulfate (PS) to oxidate As (III), making it less toxic As(V). The developed SBC/PS system could oxidate As(III) effectively in the wide pH values (2-10). Excluding the influence of specific surface area and functional groups, the concentration of environmental persistent free radicals (EPFRs) had a good linear relationship with the oxidation of As(III), reaching above 0.96. According to a mechanism analysis, EPFRs on SBC could transfer electrons to directly activate PS to produce SO4-center dot, center dot OH, O-2(-)center dot, and O-1(2) to improve the oxidation of As(III). These results not only indicated that the biochar/PS system's application scope can be successfully increased by adjusting the preparation conditions, but also revealed the invaluable role of EPFRs in As(III) oxidation process.

关键词 :

Sludge-derived biochar Sludge-derived biochar Persulfate Persulfate Oxidation Oxidation Arsenic Arsenic Environmentally persistent free radicals Environmentally persistent free radicals

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GB/T 7714 Zhu, Yuhan , Wei, Jia , Li, Jun . Biochar-activated persulfate oxidation of arsenic(III): Nonnegligible roles of environmentally persistent free radicals [J]. | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING , 2023 , 11 (5) .
MLA Zhu, Yuhan et al. "Biochar-activated persulfate oxidation of arsenic(III): Nonnegligible roles of environmentally persistent free radicals" . | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING 11 . 5 (2023) .
APA Zhu, Yuhan , Wei, Jia , Li, Jun . Biochar-activated persulfate oxidation of arsenic(III): Nonnegligible roles of environmentally persistent free radicals . | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING , 2023 , 11 (5) .
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Decontamination of Cr(VI) from water using sewage sludge-derived biochar: Role of environmentally persistent free radicals SCIE
期刊论文 | 2023 , 56 , 97-103 | CHINESE JOURNAL OF CHEMICAL ENGINEERING
摘要&关键词 引用

摘要 :

Biochar is a well-known material for pollutant removal owing to its low cost and rich surface function-ality. A kind of highly active substance, called environmentally persistent free radicals (EPFRs), can be produced in the preparation process of biochar, playing an important role in the removal of pollutants. In this study, sludge-derived biochars (SBC120 and SBC270) were prepared by the hydrothermal carboniza-tion under two temperatures (120 degrees C and 270 degrees C) to investigate their removal abilities of Cr(VI). The max-imum removal amounts of Cr(VI) by SBC120 and SBC270 were 16.58 and 22.93 mg center dot g(-1), respectively. It was further revealed that the appearance of Cr(III), as a result of EPFRs on sludge-derived biochar (SBC) trans-ferred electrons to Cr(VI) in neutral solutions. That is to say, oxygen-centered (O-centered) EPFRs on SBC120 and carbon-centered (C-centered) EPFRs on SBC270 all could be used as electron donors to Cr (VI) to make it become Cr(III). This study not only provides a theoretical basis for the mechanism of pol-lutants removal by sludge-derived biochar but also offers a new perspective on the direct effect of EPFRs on pollutants.(c) 2022 The Chemical Industry and Engineering Society of China, and Chemical Industry Press Co., Ltd. All rights reserved.

关键词 :

Environmentally persistent free radicals Environmentally persistent free radicals Sludge-derived biochar Sludge-derived biochar Removal Removal Reduction Reduction Chromium Chromium

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GB/T 7714 Zhu, Yuhan , Wei, Jia , Li, Jun . Decontamination of Cr(VI) from water using sewage sludge-derived biochar: Role of environmentally persistent free radicals [J]. | CHINESE JOURNAL OF CHEMICAL ENGINEERING , 2023 , 56 : 97-103 .
MLA Zhu, Yuhan et al. "Decontamination of Cr(VI) from water using sewage sludge-derived biochar: Role of environmentally persistent free radicals" . | CHINESE JOURNAL OF CHEMICAL ENGINEERING 56 (2023) : 97-103 .
APA Zhu, Yuhan , Wei, Jia , Li, Jun . Decontamination of Cr(VI) from water using sewage sludge-derived biochar: Role of environmentally persistent free radicals . | CHINESE JOURNAL OF CHEMICAL ENGINEERING , 2023 , 56 , 97-103 .
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A state-of-the-art review on heterogeneous catalysts-mediated activation of peracetic acid for micropollutants degradation: Classification of reaction pathways, mechanisms, influencing factors and DFT calculation SCIE
期刊论文 | 2023 , 477 | CHEMICAL ENGINEERING JOURNAL
摘要&关键词 引用

摘要 :

Emerging micropollutants (MPs) in water present growing environmental concerns, drawing considerable attention in recent years. Of the numerous advanced oxidation processes (AOPs) for MPs removal, the approach based on peracetic acid (PAA) has especially attracted interest from both the academic and industrial realms. This comprehensive review systematically investigates the activation of PAA for MPs degradation using heterogeneous catalysts. The discussion starts with an overview of the fundamental aspects of PAA, along with the research background and prospects of PAA-AOPs. Subsequently, the generation and detection methods of organic radical (R-O center dot) and non-organic radical (non-R-O center dot) pathways in heterogeneous catalyst/PAA systems are discussed. Furthermore, the activation mechanisms of metal- and carbon-based catalysts are extensively revealed. After that, the influencing factors that significantly affect the performance of heterogeneous catalyst/PAA systems are proposed. Additionally, the application of density functional theory (DFT) calculation associated with heterogeneous catalyst/PAA systems is summarized. Finally, the current limitations and future research directions of heterogeneous catalyst/PAA systems are taken over. This review strives to enhance the comprehension of the heterogeneous catalyst-activated PAA systems in removal of MPs, while offering innovative perspectives and outlining future research avenues regarding the applications of these systems.

关键词 :

Peracetic acid Peracetic acid Emerging micropollutants Emerging micropollutants Advanced oxidation processes Advanced oxidation processes Heterogeneous catalysts Heterogeneous catalysts

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GB/T 7714 Wang, Linhao , Wei, Jia , Li, Yanan et al. A state-of-the-art review on heterogeneous catalysts-mediated activation of peracetic acid for micropollutants degradation: Classification of reaction pathways, mechanisms, influencing factors and DFT calculation [J]. | CHEMICAL ENGINEERING JOURNAL , 2023 , 477 .
MLA Wang, Linhao et al. "A state-of-the-art review on heterogeneous catalysts-mediated activation of peracetic acid for micropollutants degradation: Classification of reaction pathways, mechanisms, influencing factors and DFT calculation" . | CHEMICAL ENGINEERING JOURNAL 477 (2023) .
APA Wang, Linhao , Wei, Jia , Li, Yanan , Huo, Jiangkai , Ji, Wei , Cui, Nan et al. A state-of-the-art review on heterogeneous catalysts-mediated activation of peracetic acid for micropollutants degradation: Classification of reaction pathways, mechanisms, influencing factors and DFT calculation . | CHEMICAL ENGINEERING JOURNAL , 2023 , 477 .
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A porous graphitic biochar wrapped Co9S8 core-shell composite enables pH-universal activation of peroxymonosulfate for highly efficient and rapid antibiotics degradation SCIE
期刊论文 | 2022 , 9 (9) , 3629-3645 | ENVIRONMENTAL SCIENCE-NANO
WoS核心集被引次数: 9
摘要&关键词 引用

摘要 :

Metal sulfides have been found to be effective in removing organic pollutants from water in environmental catalysis. In this study, a porous graphitic biochar wrapped Co9S8 core-shell composite (Co9S8@N-O-BC) was designed for efficient activation of peroxymonosulfate (PMS) and degradation of sulfamethoxazole in an aqueous environment. Based on complementary characterizations and reactive oxygen species (ROS) quenching experiments, we proposed that boosted Co(ii) regeneration by various existing S species along with formed N and O active sites in Co9S8@N-O-BC facilitated the cleavage of the O-O bond of PMS, thus resulting in a high-efficiency non-radical pathway. Consequently, Co9S8@N-O-BC/PMS achieved an outstanding degradation of sulfamethoxazole (100%) within 4 min in a wide pH range (3-11) and its turnover frequency (TOF) value was 11.96 min(-1), up to 117 times higher than other reported catalysts as far as we know. The superior stability and wide applicability in sulfamethoxazole degradation with a series of inorganic ions, especially the production of very few harmless intermediates and the exceptional mineralization efficiency, also further demonstrated that the obtained catalyst possessed excellent potential for practical wastewater treatment.

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GB/T 7714 Li, Jiamei , Wei, Jia , Xu, Mengdie et al. A porous graphitic biochar wrapped Co9S8 core-shell composite enables pH-universal activation of peroxymonosulfate for highly efficient and rapid antibiotics degradation [J]. | ENVIRONMENTAL SCIENCE-NANO , 2022 , 9 (9) : 3629-3645 .
MLA Li, Jiamei et al. "A porous graphitic biochar wrapped Co9S8 core-shell composite enables pH-universal activation of peroxymonosulfate for highly efficient and rapid antibiotics degradation" . | ENVIRONMENTAL SCIENCE-NANO 9 . 9 (2022) : 3629-3645 .
APA Li, Jiamei , Wei, Jia , Xu, Mengdie , Pan, Guoping , Zhang, Yifei , Xing, Luyi et al. A porous graphitic biochar wrapped Co9S8 core-shell composite enables pH-universal activation of peroxymonosulfate for highly efficient and rapid antibiotics degradation . | ENVIRONMENTAL SCIENCE-NANO , 2022 , 9 (9) , 3629-3645 .
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Satisfactory degradation of tetracycline by a pH-universal MnFe-LDH@BC cathode in electric Fenton process: Performances, mechanisms and toxicity assessments SCIE
期刊论文 | 2022 , 10 (5) | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
WoS核心集被引次数: 26
摘要&关键词 引用

摘要 :

The ubiquitous and ineffective treatment of antibiotics in aquatic systems leads to serious environmental problems, threatening ecology and human health. Herein, layered double metal hydroxides (LDH) and biochar (BC) were successfully combined through a facile hydrothermal method to prepare a novel pH-universal electric Fenton (EF) cathode (MnFe-LDH@BC). The developed MnFe-LDH@BC-EF system exhibited superior perfor-mance in the degradation of tetracycline (TC) (94.2%) than both of MnFe-LDH-EF (64.1%) and BC-EF system (67.0%) and showed a well-pleasing performance in a wide pH range. It was proposed that the nanostructures of LDH favored the multivalent cycle of Fe and Mn, promoting the electron transfer of BC as well as the release of Fe2+, leading to continuously generation of extensive free radicals and non-radicals. The co-existing ions (Cl-, NO3-, CO32-, HCO3- and H2PO4-) had different impact on the removal of TC. The studied system exhibited satis-factory degradation of various selected contaminants as well as fantastic stability in successive cycles. The possible degradation pathways were proposed and the toxicity of intermediate products were assessed by the Estimation Program Interface (EPI) Suite analysis. This work demonstrated the great potential of the developed cathode in water treatment area and provided insights into the utilization of biomass waste resources.

关键词 :

Biochar Biochar Toxicity assessment Toxicity assessment Layered double hydroxide Layered double hydroxide Antibiotic Antibiotic Heterogeneous electro-Fenton Heterogeneous electro-Fenton

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GB/T 7714 Xu, Mengdie , Wei, Jia , Chen, Xiujuan et al. Satisfactory degradation of tetracycline by a pH-universal MnFe-LDH@BC cathode in electric Fenton process: Performances, mechanisms and toxicity assessments [J]. | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING , 2022 , 10 (5) .
MLA Xu, Mengdie et al. "Satisfactory degradation of tetracycline by a pH-universal MnFe-LDH@BC cathode in electric Fenton process: Performances, mechanisms and toxicity assessments" . | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING 10 . 5 (2022) .
APA Xu, Mengdie , Wei, Jia , Chen, Xiujuan , Pan, Guoping , Li, Jiamei , Xing, Luyi et al. Satisfactory degradation of tetracycline by a pH-universal MnFe-LDH@BC cathode in electric Fenton process: Performances, mechanisms and toxicity assessments . | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING , 2022 , 10 (5) .
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