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学者姓名:孙治荣
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Abstract :
Herein, we fabricated a novel NiO@CuxO nanorods (NRs) composite electrode grown in-situ on copper foam (CF), designated as NiO@CuxO NRs/CF. This electrode demonstrates excellent performance in a heterogeneous electro-Fenton-like system. It efficiently activates O2 to generate 1O2 in-situ without the addition of oxidant precursors and effectively degrades chloroquine phosphate (CQ). The combination of NiO and CuxO nanoarrays created multiple synergistic sites for molecular oxygen adsorption and activation. The addition of NiO induced the formation of low-valence Cu species and effectively optimized oxygen reduction reaction (ORR) kinetics. This enhancement led to an increased generation of key intermediates (center dot O2- and center dot OH), which further promoted the efficient production of 1O2 through the chain reaction mediated by center dot O2- and center dot OH. NiO@CuxO NRs/CF achieved a 3.9-fold increase in 1O2 production compared to the CF electrode. NiO@CuxO NRs/CF electrodes exhibited exceptional performance in degrading CQ across a wide pH range (3-11). Meanwhile, it also displayed remarkable stability and anti-interference capability, highlighting their promising potential for practical applications. The study provides an innovative strategy for the in-situ production of 1O2 through molecular oxygen activation with a bimetallic composite catalyst to efficiently degrade organic pollutants.
Keyword :
Molecular oxygen activation Molecular oxygen activation Singlet oxygen Singlet oxygen Chloroquine phosphate Chloroquine phosphate Heterogeneous electro-Fenton-like Heterogeneous electro-Fenton-like Bimetallic composite catalyst Bimetallic composite catalyst
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GB/T 7714 | Shi, Xuelin , Yan, Zihao , Zhu, Tong et al. Insights into the in-situ generation of singlet oxygen via molecular oxygen activation over NiO@CuxO NRs/CF nanocomposite catalysts: Mechanisms of singlet oxygen evolution and chloroquine phosphate degradation [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 497 . |
MLA | Shi, Xuelin et al. "Insights into the in-situ generation of singlet oxygen via molecular oxygen activation over NiO@CuxO NRs/CF nanocomposite catalysts: Mechanisms of singlet oxygen evolution and chloroquine phosphate degradation" . | CHEMICAL ENGINEERING JOURNAL 497 (2024) . |
APA | Shi, Xuelin , Yan, Zihao , Zhu, Tong , Sun, Zhirong . Insights into the in-situ generation of singlet oxygen via molecular oxygen activation over NiO@CuxO NRs/CF nanocomposite catalysts: Mechanisms of singlet oxygen evolution and chloroquine phosphate degradation . | CHEMICAL ENGINEERING JOURNAL , 2024 , 497 . |
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Abstract :
The efficient degradation of antibiotics holds significant implications for mitigating environmental pollution. This study synthesized a montmorillonite chitosan composite material (MMT-CS) using the gel template method. Subsequently, a bio-enhanced reactor was constructed to facilitate the degradation of chlorotetracycline (CTC). The addition of MMT-CS composite material enables the degradation of different concentrations of CTC. MMTCS, a conductive carrier, effectively promotes microbial adhesion and boosts the metabolic activity of functional microorganisms. Additionally, it facilitates the maintenance of microbial activity under CTC pressure by promoting the secretion of extracellular polymeric substances, increasing critical enzyme activity, and enhancing the electron transfer capacity within the system. In this MMT-CS bio-enhanced process, Paracoccus (11.4%) and Bacillus (3.9%) are utilized as essential bacteria genes. The results of metabolic pathways prediction indicated significant enhancements in membrane-transport, nucleotide-metabolism, replication-repair, and lipidmetabolism. Thus, the developed self-supporting MMT-CS bio-enhanced process ensured the stability of the system during the removal of antibiotics.
Keyword :
Antibiotic resistance gene Antibiotic resistance gene Antibiotic Antibiotic Bioaugmentation Bioaugmentation Metabolic pathways Metabolic pathways
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GB/T 7714 | Liu, Zhibin , Jiang, Bingyu , Sun, Zhirong . Mechanism of self-supporting montmorillonite composite material for bio-enhanced degradation of chlorotetracycline: Electron transfer and microbial response [J]. | BIORESOURCE TECHNOLOGY , 2024 , 404 . |
MLA | Liu, Zhibin et al. "Mechanism of self-supporting montmorillonite composite material for bio-enhanced degradation of chlorotetracycline: Electron transfer and microbial response" . | BIORESOURCE TECHNOLOGY 404 (2024) . |
APA | Liu, Zhibin , Jiang, Bingyu , Sun, Zhirong . Mechanism of self-supporting montmorillonite composite material for bio-enhanced degradation of chlorotetracycline: Electron transfer and microbial response . | BIORESOURCE TECHNOLOGY , 2024 , 404 . |
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Abstract :
Chloroquine phosphate (CQP), commonly used in treating autoimmune diseases and malaria, has been detected in various water bodies and poses potential hazards to the ecological environment. In this study, ZIF-67-derived Co 3 S 4 -modified graphite felt cathode (Co 3 S 4 /GF) was used to construct a heterogeneous electro-Fenton system for efficient CQP removal. The introduction of sulfur greatly improved the electron transfer rate and reduced the charge transfer resistance, garnering the Co 3 S 4 /GF composite cathode with excellent electrochemical activity. The Co 3 S 4 /GF electro-Fenton system completely removed CQP within 60 min at near -neutral initial pH and exhibited 19.3 % higher CQP removal efficiency than the ZIF-67/GF system. This enhanced performance was mainly attributed to the introduction of sulfur, which increased the proportion of low-valent metal in the material and promoted the Co III and Co II cycle. The hydroxyl radical was identified as the main radical involved in CQP degradation. The intermediates of CQP degradation were detected, and four possible degradation pathways of CQP were obtained. The ecotoxicity of CQP and its intermediates decreased during the degradation process. This work proposes novel ideas for the rapid development of metal -organic framework -derived Co/S-based materials for their application in the field of environmental catalysis.
Keyword :
CoII CoII Sulfur Sulfur Heterogeneous electro-Fenton Heterogeneous electro-Fenton Chloroquine phosphate Chloroquine phosphate ZIF-67-derived ZIF-67-derived
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GB/T 7714 | Peng, Huilin , Shi, Xuelin , Sun, Zhirong . ZIF-67-derived Co 3 S 4-modified cathode with high Co II content enhances the removal of chloroquine phosphate by the electro-Fenton system [J]. | JOURNAL OF WATER PROCESS ENGINEERING , 2024 , 63 . |
MLA | Peng, Huilin et al. "ZIF-67-derived Co 3 S 4-modified cathode with high Co II content enhances the removal of chloroquine phosphate by the electro-Fenton system" . | JOURNAL OF WATER PROCESS ENGINEERING 63 (2024) . |
APA | Peng, Huilin , Shi, Xuelin , Sun, Zhirong . ZIF-67-derived Co 3 S 4-modified cathode with high Co II content enhances the removal of chloroquine phosphate by the electro-Fenton system . | JOURNAL OF WATER PROCESS ENGINEERING , 2024 , 63 . |
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Abstract :
This study aimed to further improve the degradation efficiency of pollutants by electrochemical oxidation system and reduce the consumption of electric energy. A simple method of electrochemical exfoliation was used to modify graph-ite felt (GF) to prepare an anode material (Ee-GF) with high degradation performance. An anode and cathode cooper-ative oxidation system was constructed with Ee-GF as the anode and CuFe2O4/Cu2O/Cu@EGF as the cathode to efficiently degrade sulfamethoxazole (SMX). Complete degradation of SMX was achieved within 30 min. Compared with anodic oxidation system alone, the degradation time of SMX was reduced by half and the energy consumption was reduced by 66.8 %. The system displayed excellent performance for the degradation of different concentrations (10-50 mg L-1) of SMX, different pollutants, and under different water quality conditions. In addition, the system still maintained 91.7 % removal rate of SMX after ten consecutive runs. At least 12 degradation products and seven possible degradation routes of SMX were generated in the degradation process by the combined system. The eco-toxicity of degradation products of SMX was reduced after the proposed treatment. This study provided a theoretical basis for the safe, efficient, and low energy consumption removal of antibiotic wastewater.
Keyword :
Sulfamethoxazole degradation Sulfamethoxazole degradation Anode and cathode cooperative oxidation Anode and cathode cooperative oxidation Graphite felt Graphite felt Ecotoxicity Ecotoxicity Density functional theory Density functional theory
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GB/T 7714 | Qi, Haiqiang , Shi, Xuelin , Liu, Zhibin et al. An anode and cathode cooperative oxidation system constructed with Ee-GF as anode and CuFe2O4/Cu2O/Cu@EGF as cathode for the efficient removal of sulfamethoxazole [J]. | SCIENCE OF THE TOTAL ENVIRONMENT , 2023 , 875 . |
MLA | Qi, Haiqiang et al. "An anode and cathode cooperative oxidation system constructed with Ee-GF as anode and CuFe2O4/Cu2O/Cu@EGF as cathode for the efficient removal of sulfamethoxazole" . | SCIENCE OF THE TOTAL ENVIRONMENT 875 (2023) . |
APA | Qi, Haiqiang , Shi, Xuelin , Liu, Zhibin , Yan, Zihao , Sun, Zhirong . An anode and cathode cooperative oxidation system constructed with Ee-GF as anode and CuFe2O4/Cu2O/Cu@EGF as cathode for the efficient removal of sulfamethoxazole . | SCIENCE OF THE TOTAL ENVIRONMENT , 2023 , 875 . |
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Abstract :
Excess sludge fermentation is a commonly employed method for carbon sources in wastewater treatment plants, but its use as a carbon source for chlorophenol removal has been relatively underexplored. In this study, a laboratory-scale sludge fermentation SBR (FSBR) was integrated with a 2,4,6-trichlorophenol (2,4,6-TCP) degradation SBR (DSBR), resulting in a stable removal of 2,4,6-TCP without the need for external carbon sources. In this coupled system, the concentrations of volatile fatty acids in FSBR remained constant, with acetic acid, propionic acid, butyric acid, and valeric acid concentrations reaching 322.04 mg COD/L, 225.98 mg COD/L, 274.76 mg COD/L, and 149.58 mg COD/L, respectively, and the acid production efficiency increased to 88.40%. Throughout the 110-day operational period, the activated sludge concentration in the DSBR was consistently maintained at 3021 +/- 110 mg/L, and the sludge SVI remained stable at 70 mL/g. The maximum amount of 2,4,6-TCP removed reached 240.13 mg/L within a 12 h operating cycle. The use of excess sludge fermentation can completely replace commercial carbon sources for 2,4,6-TCP removal, leading to cost savings in chlorophenol treatment and broadening the applicability of this technology.
Keyword :
co-metabolism co-metabolism carbon source carbon source coupling process coupling process excess sludge fermentation excess sludge fermentation 2,4,6-trichlorophenol 2,4,6-trichlorophenol
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GB/T 7714 | Wang, Jianguang , Sun, Zhirong , Li, Jun . Feasibility Study of Using Excess Sludge Fermentation Broth as a Co-Metabolic Carbon Source for 2,4,6-Trichlorophenol Degradation [J]. | WATER , 2023 , 15 (22) . |
MLA | Wang, Jianguang et al. "Feasibility Study of Using Excess Sludge Fermentation Broth as a Co-Metabolic Carbon Source for 2,4,6-Trichlorophenol Degradation" . | WATER 15 . 22 (2023) . |
APA | Wang, Jianguang , Sun, Zhirong , Li, Jun . Feasibility Study of Using Excess Sludge Fermentation Broth as a Co-Metabolic Carbon Source for 2,4,6-Trichlorophenol Degradation . | WATER , 2023 , 15 (22) . |
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Abstract :
Bifunctional cathodes have attracted widespread interest in the heterogeneous electro-Fenton (hetero-EF) process. In this study, the bifunctional composite cathode co-modified with N-doped carbon CoFe alloy (CoFe@NC) and carbon nanotubes (CNTs), designated as CoFe@NC-CNTs/CNTs/NF, integrating hydrogen peroxide (H2O2) synthesis and catalysis, was prepared for efficient degradation of atrazine (ATZ) under the near-neutral condition (pHi = 5.9). The morphology properties, crystal structure, microstructures, and elemental composition were determined. The influences of current density, initial pH value, different anions, and water matrix on the removal of ATZ were systematically studied. In the hetero-EF process, high removal efficiencies of ATZ can be achieved over the broad pH range (3-9) under the current density of 4.5 mA cm-2. The removal efficiency of ATZ remained at 90.2 +/- 0.3% after 8 cycles under the near-neutral condition (pHi = 5.9). Radical quenching tests and EPR spectra have verified that both free radical pathways such as superoxide anion (O-2(center dot-)) and hydroxyl radical ((OH)-O-center dot) and non-radical pathway such as singlet oxygen (O-1(2)) contributed to ATZ removal. The degradation pathways and catalytic mechanism were proposed. Toxicity evaluation and Escherichia coli growth test showed that the toxicity gradually decreased during the degradation process. This work provided a new thought for developing an efficient and stable bifunctional cathode to construct an in-situ hetero-EF system for pollutants removal over the wide pH range.
Keyword :
Singlet oxygen Singlet oxygen Atrazine Atrazine Heterogeneous electro-Fenton Heterogeneous electro-Fenton CoFe alloy CoFe alloy Broad pH Broad pH
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GB/T 7714 | Sun, Xiuping , Qi, Haiqiang , Sun, Zhirong . Bifunctional nickel foam composite cathode co-modified with CoFe@NC and CNTs for electrocatalytic degradation of atrazine over wide pH range [J]. | CHEMOSPHERE , 2022 , 286 . |
MLA | Sun, Xiuping et al. "Bifunctional nickel foam composite cathode co-modified with CoFe@NC and CNTs for electrocatalytic degradation of atrazine over wide pH range" . | CHEMOSPHERE 286 (2022) . |
APA | Sun, Xiuping , Qi, Haiqiang , Sun, Zhirong . Bifunctional nickel foam composite cathode co-modified with CoFe@NC and CNTs for electrocatalytic degradation of atrazine over wide pH range . | CHEMOSPHERE , 2022 , 286 . |
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Abstract :
A novel gas diffusion electrode (GDE) device is proposed that can generate hydrogen peroxide (H2O2) efficiently and consume less energy than conventional GDE devices. By optimizing the mass fraction of PTFE (40%) and CB loading (0.4 mL cm(-2)), the three-dimensional nickel foam composite electrode (CB/PTFE/NF) was endowed with a stable solid-liquid-gas three-phase interface. CB/PTFE/NF was used as the cathode to efficiently generate H2O2 without external aeration using the natural air flow and evolution of oxygen at the mixed metal oxide (MMO) anode as the oxygen sources. After running for 150 min under optimal conditions, the H2O2 accumulation was 398 mg L-1, the yield of H2O2 reached 3.17 mg h(-1) cm(-2), and the current efficiency and energy consumption were 70% and 9.7 kWh kg( 1), respectively. The electrode had a good stability, and the H2O2 production could still reach 385 mg L-1 after 10 cycles. Based upon the proposed GDE device, the electro-Fenton degradation of amoxicillin (AMX) was investigated. When the Fe2+ concentration was 0.3 mM and the initial concentration of AMX was 50 mg L-1, the removal efficiency was 100% after 30 min. The active species that played a major role in the degradation of AMX was the hydroxyl radical.
Keyword :
Two oxygen sources Two oxygen sources Electro-Fenton Electro-Fenton Floating gas diffusion electrode Floating gas diffusion electrode Hydroxyl radical Hydroxyl radical Absence of external aeration Absence of external aeration
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GB/T 7714 | Sun, Xiuping , Lv, Jiajing , Yan, Zihao et al. A three-dimensional gas diffusion electrode without external aeration for producing H2O2 and eliminating amoxicillin using electro-Fenton process [J]. | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING , 2022 , 10 (2) . |
MLA | Sun, Xiuping et al. "A three-dimensional gas diffusion electrode without external aeration for producing H2O2 and eliminating amoxicillin using electro-Fenton process" . | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING 10 . 2 (2022) . |
APA | Sun, Xiuping , Lv, Jiajing , Yan, Zihao , Sun, Zhirong . A three-dimensional gas diffusion electrode without external aeration for producing H2O2 and eliminating amoxicillin using electro-Fenton process . | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING , 2022 , 10 (2) . |
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Abstract :
An iron-copper graphite felt (Fe-Cu/HGF) electrode was successfully prepared by heat treatment and impregnation of graphite felt as the support followed by calcination, and an electro-activated peroxydisulfate (E-PDS) system with Fe-Cu/HGF as the cathode was constructed to degrade Diuron. This system synergistically activated PDS through electrochemical processes and transition metal catalysis. High-valence metal ions could be converted into low-valence metal ions by reduction at the cathode, and low-valence metal ions continuously activated PDS to generate more sulfate radicals (SO4 & BULL;-) and hydroxyl radicals (& BULL;OH) to accelerate Diuron degradation. The Fe-Cu/HGF composite cathode exhibited a performance superior to graphite felt (RGF) obtained using pretreatment only, including increased hydrophilicity, significantly increased number of defect sites and larger electroactive surface area. Under optimized experimental degradation conditions, Diuron could be completely removed in 35 min, at which time copper ion leaching was not detected in the solution, while the total iron ion concentration was 0.27 mg L-1. Extending the reaction time to 6 h, the amount of total organic carbon was reduced to 32.2%. In addition, the free radicals that degraded Diuron were identified as mainly SO4 & BULL;- and & BULL;OH with a slightly higher contribution of SO4 & BULL;-. The mechanism and pathways of Diuron degradation in the E-PDS system were determined. The E-PDS system was successfully applied to the degradation of other pollutants and the degradation of Diuron in different simulated water environments. In summary, the E-PDS system using Fe-Cu/HGF as the cathode is a promising treatment method for Diuron-containing wastewater.
Keyword :
Peroxydisulfate Peroxydisulfate Transition metal activation Transition metal activation Diuron Diuron Electro-activated Electro-activated Graphite felt Graphite felt
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GB/T 7714 | Zhu, Lijing , Li, Mengya , Qi, Haiqiang et al. Using Fe-Cu/HGF composite cathodes for the degradation of Diuron by electro-activated peroxydisulfate [J]. | CHEMOSPHERE , 2022 , 291 . |
MLA | Zhu, Lijing et al. "Using Fe-Cu/HGF composite cathodes for the degradation of Diuron by electro-activated peroxydisulfate" . | CHEMOSPHERE 291 (2022) . |
APA | Zhu, Lijing , Li, Mengya , Qi, Haiqiang , Sun, Zhirong . Using Fe-Cu/HGF composite cathodes for the degradation of Diuron by electro-activated peroxydisulfate . | CHEMOSPHERE , 2022 , 291 . |
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Abstract :
The heterogeneous electro-Fenton (hetero-EF) technology is an attractive but challenging method used to degrade organic pollutants. The development of a catalysts for the stable and efficient degradation of pollutants under neutral conditions remains a challenging task. In this study, a microsphere catalyst consisting of magnetic Cu-Fe-FeC3 on nitrogen-doped biochar (Cu-Fe-Fe3C@NDB) was prepared using chitosan as the carrier material in a two-step process. A hetero-EF system using Cu-Fe-Fe3C@NDB as the catalyst was constructed to efficiently degrade amoxicillin. The catalyst exhibited a wide pH application range, a good stability, and a low metal ion leaching. The main reasons behind the remarkable catalytic performance and excellent stability of the Cu-Fe-Fe3C@NDB catalyst are: (i) The presence of a core-shell structure, in which Cu-Fe bimetallic particles are wrapped in the structure of biomass carbon to slow down the loss of the metal active component in the catalyst and maintain its stability; (ii) The uniform dispersion of nanoparticles on the surface of the Cu-Fe-Fe3C@NDB catalyst, N-doped carbon, and the combined effect of Cu and Fe, which are beneficial to improve the charge transfer efficiency and regulate the electronic structure, which in turns improve the activity of the catalyst. This work demonstrates that the efficient degradation of pollutants under neutral conditions can be achieved and provides useful information for the design and synthesis of efficient and stable catalysts in hetero-EF reaction systems.
Keyword :
Degradation pathway Degradation pathway Heterogeneous electro-Fenton process Heterogeneous electro-Fenton process Chitosan Chitosan Amoxicillin Amoxicillin Nitrogen-doped biochar Nitrogen-doped biochar Toxicity Toxicity
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GB/T 7714 | Qi, Haiqiang , Pan, Guifang , Shi, Xuelin et al. Cu-Fe-FeC3@nitrogen-doped biochar microsphere catalyst derived from CuFe2O4@chitosan for the efficient removal of amoxicillin through the heterogeneous electro-Fenton process [J]. | CHEMICAL ENGINEERING JOURNAL , 2022 , 434 . |
MLA | Qi, Haiqiang et al. "Cu-Fe-FeC3@nitrogen-doped biochar microsphere catalyst derived from CuFe2O4@chitosan for the efficient removal of amoxicillin through the heterogeneous electro-Fenton process" . | CHEMICAL ENGINEERING JOURNAL 434 (2022) . |
APA | Qi, Haiqiang , Pan, Guifang , Shi, Xuelin , Sun, Zhirong . Cu-Fe-FeC3@nitrogen-doped biochar microsphere catalyst derived from CuFe2O4@chitosan for the efficient removal of amoxicillin through the heterogeneous electro-Fenton process . | CHEMICAL ENGINEERING JOURNAL , 2022 , 434 . |
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Abstract :
ABS T R A C T In this paper, a CuCo-O@CNTs/NF electrode was successfully prepared and used for in-situ degradation of sulfamethoxazole (SMX) in an electro-Fenton-like system. Carbon nanotubes (CNTs) and coral-like copper-cobalt oxides were successively loaded on nickel foam (NF). CNTs contributed to improving the dispersibility and stability of copper-cobalt oxides, and the coral-like copper-cobalt oxide catalyst was anchored on CNTs without any adhesive. In the electro-Fenton-like system, dissolved oxygen can be reduced to superoxide anions in a one-electron step, which could be further transformed into hydrogen peroxide and then reacted with the active components on the electrode to generate reactive oxygen species (ROS) to participate in the degradation of SMX. Almost 100% SMX removal was obtained within 60 min in a wide near-neutral pH range (5.6-9.0), and the electrode could still achieve a 90.4% removal rate after ten recycle runs. Radical-quenching results showed that superoxide anions were the main species in the degradation of SMX. In addition, a possible degradation pathway of SMX was proposed. According to the result of toxicological simulations, the toxicity of the pollutant solution during the degradation process exhibited a decreasing trend. This study provides new insights for in-situ catalysis of electrodes with bimetallic active components to generate ROS for high-efficiency degradation of refractory organic pollutants.
Keyword :
Copper-cobalt oxides Copper-cobalt oxides Electro-Fenton-like process Electro-Fenton-like process Degradation pathway Degradation pathway In-situ generation of ROS In-situ generation of ROS Sulfamethoxazole Sulfamethoxazole Carbon nanotubes Carbon nanotubes
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GB/T 7714 | Zou, Yelong , Qi, Haiqiang , Sun, Zhirong . In-situ catalytic degradation of sulfamethoxazole with efficient CuCo-O@CNTs/NF cathode in a neutral electro-Fenton-like system [J]. | CHEMOSPHERE , 2022 , 296 . |
MLA | Zou, Yelong et al. "In-situ catalytic degradation of sulfamethoxazole with efficient CuCo-O@CNTs/NF cathode in a neutral electro-Fenton-like system" . | CHEMOSPHERE 296 (2022) . |
APA | Zou, Yelong , Qi, Haiqiang , Sun, Zhirong . In-situ catalytic degradation of sulfamethoxazole with efficient CuCo-O@CNTs/NF cathode in a neutral electro-Fenton-like system . | CHEMOSPHERE , 2022 , 296 . |
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