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Abstract :
In this study, an electro-Fenton gas diffusion electrode featuring air self-respiration was fabricated by incorporating carbon nanotubes, carbon nitride, and polytetrafluoroethylene onto graphite felt. The fabrication process involved a synergistic approach of ultrasonic impregnation and vacuum filtration, establishing a gas-liquid-solid tri-phase interface both on the surface and within the electrode. This preparation method facilitates autonomous air intake, diffusing it to the tri-phase reaction interface, thereby eliminating the necessity for aeration and reducing operational costs. The optimal electrode preparation conditions were determined through Box-Behnken Design response surface experiments, leading to the enhancement of H2O2 production conditions. Under the optimized conditions, H2O2 accumulation reached 45.83 mg L-1 cm(-2)h(-1), surpassing the performance achieved with conventional ultrasonic impregnation and vacuum filtration methods. Furthermore, the performance of self-breathing and the impact factors are explored. Finally, the electrode's efficacy was demonstrated through the degradation of phenol and bisphenol A with concentrations of 100 mg L-1 exhibiting degradation rates of 92 % and 95 %, respectively, within 60 min.
Keyword :
Gas diffusion electrode H2O2 production Electro-Fenton Self-breathing
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GB/T 7714 | Zhang, Zilong , Qin, Xia , Xu, Cuicui et al. Enhancing H2O2 production with a self-breathing gas diffusion electrode fabricated via ultrasonic impregnation and vacuum filtration [J]. | JOURNAL OF ELECTROANALYTICAL CHEMISTRY , 2024 , 962 . |
MLA | Zhang, Zilong et al. "Enhancing H2O2 production with a self-breathing gas diffusion electrode fabricated via ultrasonic impregnation and vacuum filtration" . | JOURNAL OF ELECTROANALYTICAL CHEMISTRY 962 (2024) . |
APA | Zhang, Zilong , Qin, Xia , Xu, Cuicui , Zhang, Fanbin , Liu, Xinrui , Yang, Yumei . Enhancing H2O2 production with a self-breathing gas diffusion electrode fabricated via ultrasonic impregnation and vacuum filtration . | JOURNAL OF ELECTROANALYTICAL CHEMISTRY , 2024 , 962 . |
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Abstract :
Non-metallic atom doping is a good strategy to promote the cathode performance in the electro-Fenton process. Therefore, a mixed-valence copper (I and II) phosphate (Cu2PO4) catalyst on P-doped etched graphite felt (EGF), with a strip-groove rough surface, was prepared in this study. The P-doped Cu2PO4/EGF electrode completely removed sulfamethoxazole (SMX) from contaminated water within 90 min over a wide pH range of 5.6-9 and removed 99.6% of SMX at pH 11. Quenching experiments showed that the main reactive oxygen species (ROS) was center dot O-2(-). According to density functional theory calculations, the adsorption reaction energy (EP = 2.149) of P atoms doped on the EGF surface was lower than that of pyrrolic nitrogen atoms (EN = 0.434), indicating that they were more conducive to oxygen adsorption. Finally, we investigated the mechanism of P-doped Cu2PO4/ EGF adsorption and the catalytic production of center dot O-2(-) from O-2. Four main degradation pathways were identified based on the intermediates identified during degradation. Toxicity analysis of the intermediates showed that electro-Fenton degradation reduced the ecotoxicity of SMX. The enhanced electrocatalytic activity obtained by P doping of heterogeneous catalysts provides a new method for preparing efficient and stable composite electrodes for pollutant degradation.
Keyword :
Superoxide anion radical Phosphorus doped electrode Degradation pathways Cu2PO4 Etched graphite felt
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GB/T 7714 | Yan, Zihao , Qi, Haiqiang , Shi, Xuelin et al. Phosphorus doping to boost the electro-Fenton degradation of sulfamethoxazole using mixed-valence copper(I and II) phosphate/etched graphite felt cathode [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 339 . |
MLA | Yan, Zihao et al. "Phosphorus doping to boost the electro-Fenton degradation of sulfamethoxazole using mixed-valence copper(I and II) phosphate/etched graphite felt cathode" . | SEPARATION AND PURIFICATION TECHNOLOGY 339 (2024) . |
APA | Yan, Zihao , Qi, Haiqiang , Shi, Xuelin , Liu, Zhibin , Sun, Zhirong . Phosphorus doping to boost the electro-Fenton degradation of sulfamethoxazole using mixed-valence copper(I and II) phosphate/etched graphite felt cathode . | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 339 . |
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Abstract :
The inefficient electron transfer and Fe(III)/Fe(II) cycle remain significant obstacles in the electro-fenton process. Herein, a nitrogen-doped graphite felt (NGF)-supported CoFe/CoFe2O4 heterostructure is synthesized that achieves highly efficient interfacial electron transfer and stable Co/Fe redox cycle. Theoretical calculations demonstrate that the CoFe/CoFe2O4 heterointerfaces induce local charge redistribution benefiting from the electronic communication between electron acceptor (CoFe2O4) and electron donor (CoFe). Analysis of the Fermi level indicates that the introduction of CoFe alloy enhances the electron density of the catalyst. The CoFe/ CoFe2O4@NGF cathode can remove bisphenol A (BPA) completely in 90 min, and the pseudo-first-order kinetic constant (0.0625 min(-1)) is 23 times higher than the GF system. Notably, the CoFe/CoFe2O4@NGF electrode maintains excellent catalytic capability and stability within a broad pH range (3-11). The construction of the CoFe/CoFe2O4 heterostructure reduces the adsorption energy of oxygen, which ultimately increases the yield of reactive oxygen species (ROS). Quenching experiments revealed that hydroxyl radical (center dot OH) played a dominant role in the degradation of BPA, and significantly reduced the biotoxicity of intermediate products. This work offers a dependable approach for developing bimetallic catalysts with high catalytic activity.
Keyword :
Heterogeneous electro-Fenton Heterointerface Electron transfer Bimetallic catalyst
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GB/T 7714 | Zhu, Tong , Shi, Xuelin , Yan, Zihao et al. Constructing heterointerfaces to enhance electron transfer of CoFe/CoFe2O4 mediated electro-Fenton process for bisphenol A degradation: Mechanistic insights and performance evaluation [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 354 . |
MLA | Zhu, Tong et al. "Constructing heterointerfaces to enhance electron transfer of CoFe/CoFe2O4 mediated electro-Fenton process for bisphenol A degradation: Mechanistic insights and performance evaluation" . | SEPARATION AND PURIFICATION TECHNOLOGY 354 (2024) . |
APA | Zhu, Tong , Shi, Xuelin , Yan, Zihao , Sun, Zhirong . Constructing heterointerfaces to enhance electron transfer of CoFe/CoFe2O4 mediated electro-Fenton process for bisphenol A degradation: Mechanistic insights and performance evaluation . | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 354 . |
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Abstract :
The preparation of stable and high-efficiency heterogeneous electro-Fenton cathodes for the treatment of pollutants is important for environmental remediation. Herein, a novel N-doped MOF-derived Fe/Co bimetallic catalyst was in-situ grown on graphite felt (GF) surface to yield a composite cathode Fe/CoNHDC-400@GF for use in electro-Fenton process. The introduction of cobalt accelerated electron transfer due to existing polyvalent metals. The synergistic effect between Co-0, Co-II, Co-III, Fe-II, and Fe. enabled the continuous generation of reactive oxygen species ((OH)-O-center dot and O-center dot(2)-). Under near-neutral conditions (pH=6.5), complete removal of 10 mg L-1 chloroquine phosphate (CQP) was achieved within 60 min. Additionally, efficient removal was also achievable over a wide pH range (pH=3-11). The mechanistic investigations indicated (OH)-O-center dot as a major active oxygen species for CQP degradation. A combination of the experimental results with density functional theory calculations (DFT) clarified the degradation pathway and intermediate products of CQP. Moreover, the toxicity of degradation products significantly reduced. Overall, valuable insights on preparing composite cathodes grown in-situ for efficient removal of refractory pollutants from wastewater during the heterogeneous electro-Fenton process were provided, useful for future consideration.
Keyword :
Heterogeneous electro-Fenton process In-situ catalysis Chloroquine phosphate Polyvalent metals synergistic effect
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GB/T 7714 | Fu, Bo , Yan, Zihao , Sun, Zhirong . Novel MOF-derived Fe/CoNHDC-400@GF cathode with improved in-situ catalytic degradation of chloroquine phosphate during heterogeneous electro-Fenton process [J]. | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING , 2024 , 12 (3) . |
MLA | Fu, Bo et al. "Novel MOF-derived Fe/CoNHDC-400@GF cathode with improved in-situ catalytic degradation of chloroquine phosphate during heterogeneous electro-Fenton process" . | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING 12 . 3 (2024) . |
APA | Fu, Bo , Yan, Zihao , Sun, Zhirong . Novel MOF-derived Fe/CoNHDC-400@GF cathode with improved in-situ catalytic degradation of chloroquine phosphate during heterogeneous electro-Fenton process . | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING , 2024 , 12 (3) . |
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Abstract :
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.
Keyword :
Electro-Fenton Dual -cathode Biochar Boron doping 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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Abstract :
Electro-Fenton (EF) process, featuring in-situ hydrogen peroxide (H2O2) production, has received increasing attention for its efficacy in degrading organic pollutants. However, challenges such as low oxygen utilization efficiency and high energy consumption persist. In this study, a novel Carbon Black-loaded Carbon Felt (CB-CF) electrode using the electrophoretic deposition (EPD) technique was prepared to boost the efficiency of H2O2 production. Various aeration patterns and aeration gas were systematically introduced to assess the oxygen utilization pathway and improve oxygen utilization efficiency. The CB-CF cathode, forming an efficient triphase interface, coupled with the side-oxygen mode, demonstrates rapid H2O2 production (48.82 mg/h) at a remarkably low energy consumption (14.46kWh & sdot;kg- 1) with the current density of 15 mA/cm2. The fabricated CB-CF exhibited exceptional performance, achieving over 90% degradation efficiency of Fulvic Acid (FA) within 60 minutes in the EF system. Stability experiments underscored the impact of current density and hydrophobicity on the electrode but revealed that PTFE recoating effectively preserves stability. Furthermore, the straightforward and efficient electrode preparation process, combined with the favorable electrochemical properties of CBCF, positions it as a promising candidate for large-scale applications in H2O2 electro-synthesis and environmental remediation.
Keyword :
Electrophoretic deposition Oxygen utilization efficiency Three-phase interface In-situ H 2 O 2 production Side-Aeration Electro-Fenton
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GB/T 7714 | Yang, Yumei , Qin, Xia . Efficient electrosynthesis of H2O2 through electrodeposition-modified cathode and side-aeration integration [J]. | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING , 2024 , 12 (3) . |
MLA | Yang, Yumei et al. "Efficient electrosynthesis of H2O2 through electrodeposition-modified cathode and side-aeration integration" . | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING 12 . 3 (2024) . |
APA | Yang, Yumei , Qin, Xia . Efficient electrosynthesis of H2O2 through electrodeposition-modified cathode and side-aeration integration . | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING , 2024 , 12 (3) . |
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Abstract :
Cu-based nanocatalysts have received much attention for their high efficiency and environmental friendliness in heterogeneous electro-Fenton (hetero-EF) technology. However, designing catalysts posses high stability and efficient pollutant degradation performance remains challenging. In this work, a novel binder-free copper foam (CF)-supported CuxO nanorod array electrode was prepared by solvothermal and calcination methods and used for the degradation of sulfamethoxazole (SMX). The hetero-EF system with CuxO NRs/CF-300 C as cathode achieved 100 % SMX degradation in 90 min. Experimental and theoretical calculations showed that the coexistence of Cu-0, Cu+, and Cu(2+ )in Cu-based catalysts promotes the generation of & sdot;O-2(-) and facilitates redox cycling of Cu species (Cu+/Cu2+), thus enhancing SMX degradation efficiency. In addition, CuxO NRs/CF-300 C expanded the pH range (3-11) and exhibited remarkable stability, making it an excellent synthetic electrode material with production potential. This discovery successfully overcame the low and unstable Cu+ activation capacity and the short lifetime of reactive oxygen species in conventional heterogeneous reactions. This work provides a practical approach for developing reliable Cu-based nanocatalysts and facilitating the degradation of organic contaminants.
Keyword :
Active oxygen species Heterogeneous electro-Fenton Sulfamethoxazole Copper -based nanocatalysts Synergistic effect
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GB/T 7714 | Shi, Xuelin , Qi, Haiqiang , Liu, Zhibin et al. Copper foam-supported CuxO nanorod array electrode without binder: Synergistic effects of Cu0, Cu+, and Cu2+ during ⋅O2- generation and sulfamethoxazole degradation [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 483 . |
MLA | Shi, Xuelin et al. "Copper foam-supported CuxO nanorod array electrode without binder: Synergistic effects of Cu0, Cu+, and Cu2+ during ⋅O2- generation and sulfamethoxazole degradation" . | CHEMICAL ENGINEERING JOURNAL 483 (2024) . |
APA | Shi, Xuelin , Qi, Haiqiang , Liu, Zhibin , Yan, Zihao , Yang, Jingjie , Sun, Zhirong . Copper foam-supported CuxO nanorod array electrode without binder: Synergistic effects of Cu0, Cu+, and Cu2+ during ⋅O2- generation and sulfamethoxazole degradation . | CHEMICAL ENGINEERING JOURNAL , 2024 , 483 . |
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Abstract :
In this study, a graphite felt (GF) electrode material supporting a Cu-based catalyst (CuHDC-400/GF) was pre-pared by a hydrothermal process and subsequent heat treatment. A heterogeneous electro-Fenton (EF) system was built to investigate the degradation of sulfamethoxazole (SMX) by the composite cathode. Scanning electron microscopy, X-ray diffraction, Raman spectroscopy, and X-ray photoelectron spectroscopy were used to char-acterize the physical and chemical properties of the composite cathode. The results show that the composite cathode CuHDC-400/GF has excellent catalytic performance, achieving 100 % removal of SMX (10 mg/L) within 45 min (aeration rate = 0.6 L min(-1), current density = 5 mA cm(-2), initial pH = 5.6). Furthermore, efficient removal of SMX can be achieved over a wide pH range (pH = 3-9). The electrode material can still efficiently degrade SMX after eight cycles. Compared with a heterogeneous EF system, in which the Cu catalyst was directly added to the reaction solution, using CuHDC-400/GF as the cathode realizes the in-situ catalysis of H2O2, leading to reduced catalyst consumption and enhanced electrode stability. The investigation of potential SMX degra-dation pathways and mechanisms revealed that the continuous production of active free radicals is facilitated by the redox cycle between Cu-I and Cu-II on the electrode surface, which can enable SMX degradation. Unlike the Fe-based Fenton reaction, the active superoxide radical O-center dot(2)- was identified as the major contributor to SMX degradation in this system, followed by the hydroxyl radical (OH)-O-center dot. The active sites for SMX degradation were predicted by density functional theory calculations. Combined with the measured mass/charge ratios, the possible degradation paths and intermediates of SMX were predicted. Furthermore, toxicity analysis shows that toxicity significantly declines after degradation. This work is expected to inspire subsequent research on het-erogeneous EF cathode materials with high catalytic performance.
Keyword :
Metal-organic framework Heterogeneous electro-Fenton Sulfamethoxazole Degradation mechanism In-situ catalysis
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GB/T 7714 | Wang, Jiong , Liu, Zhibin , Sun, Zhirong . In-situ cathode induction of HKUST-1-derived polyvalent copper oxides in electro-Fenton systems for effective sulfamethoxazole degradation [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2023 , 316 . |
MLA | Wang, Jiong et al. "In-situ cathode induction of HKUST-1-derived polyvalent copper oxides in electro-Fenton systems for effective sulfamethoxazole degradation" . | SEPARATION AND PURIFICATION TECHNOLOGY 316 (2023) . |
APA | Wang, Jiong , Liu, Zhibin , Sun, Zhirong . In-situ cathode induction of HKUST-1-derived polyvalent copper oxides in electro-Fenton systems for effective sulfamethoxazole degradation . | SEPARATION AND PURIFICATION TECHNOLOGY , 2023 , 316 . |
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Abstract :
The electrocatalytic activity towards two electron oxygen reduction reaction of graphite felt was advanced by incorporating carbon nitride, carbon nanotubes and polytetrafluoroethylene through vacuum filtration, which prevented the cleavage of O-O bond, facilitated the charge transfer, and established more three-phase active sites. To ameliorate the oxygen transfer process, the configuration of side-aeration was proposed, providing forced convection to reduce the thickness of diffusion layer, and increasing the dissolved oxygen. By simplified combination of refining the orientation of gas flow and modified graphite felt, the dual-chamber configuration rendered a qualitative leap in H2O2 generation capacity to 4.44-6.89 mg h-1 cm-2. The alkaline affinity of developed system was discussed in terms of a beneficial outer-sphere electron transfer pathway, the variation on adsorption strength of oxygenated species and working electrode potential range. Finally, Long-term operation stability and successful application in Electro-Fenton indicated great potential of developed system for H2O2 synthesis and environmental remediation.
Keyword :
Two electron oxygen reduction reaction Graphite felt Oxygen mass transfer. alkaline preference Hydrogen peroxide
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GB/T 7714 | Li, Mingran , Lan, Huachun , An, Xiaoqiang et al. Highly efficient electrosynthesis of hydrogen peroxide through the combination of side aeration and vacuum filtration modified graphite felt [J]. | APPLIED CATALYSIS B-ENVIRONMENTAL , 2023 , 339 . |
MLA | Li, Mingran et al. "Highly efficient electrosynthesis of hydrogen peroxide through the combination of side aeration and vacuum filtration modified graphite felt" . | APPLIED CATALYSIS B-ENVIRONMENTAL 339 (2023) . |
APA | Li, Mingran , Lan, Huachun , An, Xiaoqiang , Qin, Xia , Zhang, Zilong , Li, Tinghui . Highly efficient electrosynthesis of hydrogen peroxide through the combination of side aeration and vacuum filtration modified graphite felt . | APPLIED CATALYSIS B-ENVIRONMENTAL , 2023 , 339 . |
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In this study, CuAl-LDH precursor was loaded on heat-treated graphite felt (HGF) to obtain CuAl-LDH/HGF. Then, the CuAl-LDO/HGF composite electrode was synthesized by calcination under a high-temperature nitrogen atmosphere. CuAl-LDO/HGF composite electrodes were used to remove sulfamethoxazole (SMX) in a heterogeneous electro-Fenton (hetero-EF) system. Both the hydrophilicity and redox capacity of CuAl-LDO/HGF composite cathode were significantly improved, and the SMX removal effect of CuAl-LDO/HGF in the hetero-EF system was superior to that of HGF. After the preparation conditions and reaction factors were optimized, SMX was completely eliminated within 60 min using the hetero-EF system under nearly-neutral conditions. 69.33% of the total organic carbon (TOC) was removed from the solution after 6 h of reaction. The SMX removal efficiency approached 94.4% after eight reuse cycles. Radical quenching experiments showed that surface hydroxyl radicals (& BULL;OH) were crucial to the degradation of SMX in this hetero-EF system. The biological toxicity of SMX and the products generated during its degradation were assessed, and the probable SMX degradation mechanism was also discussed. This work provides a feasible new insight for hetero-EF systems to remove antibiotics from wastewater.
Keyword :
Heterogeneous electro-Fenton Sulfamethoxazole Graphite felt Layered bimetallic oxides Degradation mechanism
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GB/T 7714 | Li, Yaohong , Yan, Zihao , Sun, Zhirong . Efficient electrocatalytic degradation of sulfamethoxazole with CuAl-LDO/ HGF cathode in a neutral heterogeneous electro-Fenton process [J]. | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING , 2023 , 11 (3) . |
MLA | Li, Yaohong et al. "Efficient electrocatalytic degradation of sulfamethoxazole with CuAl-LDO/ HGF cathode in a neutral heterogeneous electro-Fenton process" . | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING 11 . 3 (2023) . |
APA | Li, Yaohong , Yan, Zihao , Sun, Zhirong . Efficient electrocatalytic degradation of sulfamethoxazole with CuAl-LDO/ HGF cathode in a neutral heterogeneous electro-Fenton process . | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING , 2023 , 11 (3) . |
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