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学者姓名：孙治荣
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摘要 ：
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.
关键词 ：
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 等. "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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摘要 ：
The heterogeneous electro-Fenton process is an effective technology to remove organic pollutants. However, developing efficient heterogeneous electro-Fenton catalysts remains challenging. In this paper, an iron-cerium layered double hydroxide (Fe-Ce-LDH) was successfully loaded via a solvothermal method onto the defect sites of the molecular sieve 13X to form a novel heterogeneous catalyst (Fe-Ce-LDH/13X). The catalytic performance of Fe-Ce-LDH/13X was evaluated in the heterogeneous electro-Fenton (EF) degradation of diuron. Compared with a traditional powder catalyst, this catalyst was easier to recycle and exhibited good stability. The layered structure of the catalyst provided more active sites. Doping with Ce greatly improved the catalytic performance of the catalyst, which was caused by the synergistic effect of Ce and Fe. At a molar Fe to Ce ratio of 7:3, diuron could be completely degraded within 60 min. According to the catalytic mechanism, the hydroxyl radical center dot OH is the main reactive species. Possible degradation pathways in the heterogeneous EF process were proposed based on the intermediates identified in the degradation of diuron. Toxicity analysis indicated that the heterogeneous EF process could not only degrade diuron but also reduce toxicity. This work presents a novel preparation method of a composite catalyst with excellent catalytic performance in an EF system, which supports the development of efficient heterogeneous EF catalysts.
关键词 ：
Layered double hydroxides Layered double hydroxides Heterogeneous catalyst Heterogeneous catalyst Heterogeneous electro-Fenton Heterogeneous electro-Fenton Hydroxyl radical Hydroxyl radical Organic pollutant Organic pollutant
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| GB/T 7714 | Xuan, Fangfang , Yan, Zihao , Sun, Zhirong . Efficient degradation of diuron using Fe-Ce-LDH/13X as novel heterogeneous electro-Fenton catalyst [J]. | JOURNAL OF ELECTROANALYTICAL CHEMISTRY , 2022 , 910 . |
| MLA | Xuan, Fangfang 等. "Efficient degradation of diuron using Fe-Ce-LDH/13X as novel heterogeneous electro-Fenton catalyst" . | JOURNAL OF ELECTROANALYTICAL CHEMISTRY 910 (2022) . |
| APA | Xuan, Fangfang , Yan, Zihao , Sun, Zhirong . Efficient degradation of diuron using Fe-Ce-LDH/13X as novel heterogeneous electro-Fenton catalyst . | JOURNAL OF ELECTROANALYTICAL CHEMISTRY , 2022 , 910 . |
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摘要 ：
The generation of H2O2 and the regeneration rate of Fe2+ both affect the degradation performance of the electro-Fenton (EF) process. Therefore, it is important to develop a cathode that efficiently produces H2O2 and re-generates Fe2+. In this study, graphite felt (GF) was modified via a simple hydrothermal method using ammonium persulfate as the modifier. The physicochemical and electrochemical properties of hydrothermally modified GF (H-GF) were substantially improved. The surface of H-GF was successfully doped with O and N, and its oxygen reduction reaction activity increased significantly. Compared with raw GF, the yield of H2O2 and the regeneration rate of Fe2+ of H-GF were considerably improved. The EF system constructed with H-GF as the cathode could completely remove diuron at-0.65 V/SCE within 40 min. In the EF system, H-GF exhibited an excellent degradation effect in different types of water (tap and river water) and different pollutants (amoxicillin, atrazine, and sulfamethoxazole). After the 40th cycle, the H-GF cathode retained excellent stability. According to density functional theory calculations, H2O2 and Fe2+ were easily generated due to the low energy barrier required for the adsorption of O-2 and Fe3+ on H-GF. Finally, a possible degradation path of diuron in the EF process was proposed, and the toxicity of the intermediates produced in the degradation process of diuron was analyzed.
关键词 ：
Hydrothermal modification Hydrothermal modification Electro-Fenton Electro-Fenton Diuron Diuron Toxicity Toxicity Graphite felt Graphite felt
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| GB/T 7714 | Qi, Haiqiang , Ren, Wenyang , Shi, Xuelin et al. Hydrothermally modified graphite felt as the electro-Fenton cathode for effective degradation of diuron: The acceleration of Fe2+ regeneration and H2O2 production [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2022 , 299 . |
| MLA | Qi, Haiqiang et al. "Hydrothermally modified graphite felt as the electro-Fenton cathode for effective degradation of diuron: The acceleration of Fe2+ regeneration and H2O2 production" . | SEPARATION AND PURIFICATION TECHNOLOGY 299 (2022) . |
| APA | Qi, Haiqiang , Ren, Wenyang , Shi, Xuelin , Sun, Zhirong . Hydrothermally modified graphite felt as the electro-Fenton cathode for effective degradation of diuron: The acceleration of Fe2+ regeneration and H2O2 production . | SEPARATION AND PURIFICATION TECHNOLOGY , 2022 , 299 . |
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摘要 ：
The synergistic activation of persulfate (PS) by electrochemical oxidation (EO) and transition metals has gradually attracted attention as an emerging wastewater method. In this work, a Co-Fe oxide modified graphite felt composite cathode (FeO-CoFeO/GF) was prepared by in-situ solvothermal growth and calcination for PS activation to degrade atrazine (ATZ). The surface morphology, phase composition, microstructure, specific surface area, element valence, and electrochemical properties of the materials were characterized. The EO/FeO-CoFeO/ GF + PS system achieved 100% ATZ removal within 35 min and PS was effectively activated by the electrically enhanced FeO-CoFeO/GF compared with other control experiments. The FeO-CoFeO/GF composite cathode exhibited superior catalytic activity in a wide pH range (3-9) and demonstrated good stability in six consecutive cycles. Reactive oxide species were identified by radical quenching tests and electron paramagnetic resonance. Electrochemical oxidation, radical oxidation and non-radical oxidation jointly participate in attacking ATZ. A catalytic mechanism for this synergistic system was proposed to explain PS activation and subsequent ATZ degradation. Furthermore, potential ATZ degradation pathways were proposed. Toxicity changes were evaluated using the Ecological Structure Activity Relationships and Escherichia coli growth inhibition tests. This work provides a feasible strategy for synergistically strengthening PS activation and promoting the degradation of persistent organic pollutants.
关键词 ：
Persulfate Persulfate Electro-activation Electro-activation Layered double oxide Layered double oxide Toxicity Toxicity Atrazine Atrazine
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| GB/T 7714 | Sun, Xiuping , Liu, Zhibin , Sun, Zhirong . Electro-enhanced degradation of atrazine via Co-Fe oxide modified graphite felt composite cathode for persulfate activation [J]. | CHEMICAL ENGINEERING JOURNAL , 2022 , 433 . |
| MLA | Sun, Xiuping et al. "Electro-enhanced degradation of atrazine via Co-Fe oxide modified graphite felt composite cathode for persulfate activation" . | CHEMICAL ENGINEERING JOURNAL 433 (2022) . |
| APA | Sun, Xiuping , Liu, Zhibin , Sun, Zhirong . Electro-enhanced degradation of atrazine via Co-Fe oxide modified graphite felt composite cathode for persulfate activation . | CHEMICAL ENGINEERING JOURNAL , 2022 , 433 . |
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摘要 ：
The effective degradation of Sulfamethoxazole (SMX) is of great importance to alleviate environmental pollution. In this study, the degradation capacity of an ordinary sequencing batch activated sludge system (SBR) and montmorillonite (MMT) system was compared for their ability to degrade different concentrations of SMX. Compared with SBR system, the MMT system exhibited higher stability and degradation capacity. The changes in the composition of tightly bound extracellular polymeric substances (TB-EPS) were likely key to the observed stability of the system. High concentrations of SMX inhibited the degradation performance of SBR. MMTsupplemented reduced the generation of antibiotic resistance genes (ARGs). Thauera is a gene that is able to degrade SMX, and its abundance in MMT system reached 7.84%. As potential hosts of ARGs, the proportions of Paenarthrobacter and Caldilineacea were significantly correlated with sulfonamide resistance genes (sul1 and sul2). Overall, MMT-supplemented system was found to be a favorable method of treating antibiotic.
关键词 ：
Antibiotic resistance gene Antibiotic resistance gene Extracellular polymeric substance Extracellular polymeric substance Bacterial community Bacterial community Sulfamethoxazole Sulfamethoxazole Metabolism Metabolism
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| GB/T 7714 | Liu, Zhibin , Sun, Xiuping , Sun, Zhirong . Degradation mechanism of montmorillonite-enhanced antibiotic wastewater: performance, antibiotic resistance genes, microbial communities, and functional metabolism [J]. | BIORESOURCE TECHNOLOGY , 2022 , 352 . |
| MLA | Liu, Zhibin et al. "Degradation mechanism of montmorillonite-enhanced antibiotic wastewater: performance, antibiotic resistance genes, microbial communities, and functional metabolism" . | BIORESOURCE TECHNOLOGY 352 (2022) . |
| APA | Liu, Zhibin , Sun, Xiuping , Sun, Zhirong . Degradation mechanism of montmorillonite-enhanced antibiotic wastewater: performance, antibiotic resistance genes, microbial communities, and functional metabolism . | BIORESOURCE TECHNOLOGY , 2022 , 352 . |
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摘要 ：
The development of new heterogeneous Cu-based solid catalysts for hydroxyl radical (center dot OH) generation plays a crucial role in degradation of pollutants at neutral pH circumstance. In this work, a Cu-doped graphitic carbon nitride (g-C3N4) complex was synthesized in one-step pyrolysis process using copper chloride dihydrate and dicyandiamide as precursors. The results reveal that after Cu doping, the bulk structure of g-C3N4 was destroyed with fragmentary morphology formation. Besides, Cu-0 and Cu+ were successfully embedded in g-C3N4 sheet. Moreover, amoxicillin (AMX) removal by heterogeneous electro-Fenton process was performed to evaluate the catalytic activity of the Cu-doped g-C3N4. 99.1% AMX removal efficiency was obtained after 60 min electrolysis under neutral pH condition when the current density was 12 mA cm(2) and the catalyst dosage was 0.3 g L-1. Both Cu-0 and Cu+ were stably retained in the Cu-doped g-C3N4 catalyst and AMX removal efficiency reached 91.1%, even after 5 cycles, manifesting the remarkable stability of Cu-doped g-C3N4. Also, Cu-doped g-C3N4 possessed excellent catalytic activities for AMX removal in various waterbodies. According to the catalytic mechanism analysis, the center dot OH was proved to be the primary reactive species for AMX removal in heterogeneous electro-Fenton process. Based on the identification of sixteen different intermediate products, the possible degradation pathways were proposed. This work provides a simple method to synthesize a Cu-based solid catalyst containing stable Cu-0 and Cu+ for degradation of pollutants in wastewater.
关键词 ：
Catalytic activity Catalytic activity Graphitic carbon nitride Graphitic carbon nitride Hydroxyl radical Hydroxyl radical Mechanism Mechanism One-step pyrolysis One-step pyrolysis
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| GB/T 7714 | Pan, Guifang , Sun, Zhirong . Cu-doped g-C3N4 catalyst with stable Cu-0 and Cu+ for enhanced amoxicillin degradation by heterogeneous electro-Fenton process at neutral pH [J]. | CHEMOSPHERE , 2021 , 283 . |
| MLA | Pan, Guifang et al. "Cu-doped g-C3N4 catalyst with stable Cu-0 and Cu+ for enhanced amoxicillin degradation by heterogeneous electro-Fenton process at neutral pH" . | CHEMOSPHERE 283 (2021) . |
| APA | Pan, Guifang , Sun, Zhirong . Cu-doped g-C3N4 catalyst with stable Cu-0 and Cu+ for enhanced amoxicillin degradation by heterogeneous electro-Fenton process at neutral pH . | CHEMOSPHERE , 2021 , 283 . |
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摘要 ：
The metal organic framework derived materials (CoFe2O4@NC) activated peroxymonosulfate (PMS) to degrade Norfloxacin (NOR) owing to the characteristics of high surface area (109.658 m2 g-1) and abundant mesoporous structure. The characterization results demonstrated that the optimal ratio of bimetal and of bimetallic to organic ligands (M/O) had good crystal structure and stability (Fe/Co = 3:1, M/O = 2:1). Moreover, NOR (10 mg L-1) removal of 98.78% was achievable in 60 min with an optimum concentration of PMS (0.32 mM) and dosage of CoFe2O4@NC (0.1 g L-1). The radical quenching results suggested that SO4·-, ·OH and 1O2 functioned in the presence of the system certificated by XPS spectra. The presence of Cl- and CO32-/HCO3- promoted the catalyst reaction. The recoverability revealed high removal efficiency of NOR of 93.55% could still be maintained. Furthermore, four pathways of NOR degradation were proposed, including dehydroxylation, defluorination, quinolone group conversion and piperazine ring transformation, which were attributed to the synergy of reactive oxygen species. The above results highlight that the method is of great significance to the practical application of heterogeneous catalysts in aqueous solutions.
关键词 ：
Metal organic framework Metal organic framework Norfloxacin Norfloxacin Oxidative degradation Oxidative degradation Peroxomonosulfate Peroxomonosulfate Radical Radical Water treatment Water treatment
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| GB/T 7714 | Fan Yan , Liu Yanru , Hu Xiang et al. Preparation of metal organic framework derived materials CoFe2O4@NC and its application for degradation of norfloxacin from aqueous solutions by activated peroxymonosulfate. [J]. | Chemosphere , 2021 , 275 : 130059 . |
| MLA | Fan Yan et al. "Preparation of metal organic framework derived materials CoFe2O4@NC and its application for degradation of norfloxacin from aqueous solutions by activated peroxymonosulfate." . | Chemosphere 275 (2021) : 130059 . |
| APA | Fan Yan , Liu Yanru , Hu Xiang , Sun Zhirong . Preparation of metal organic framework derived materials CoFe2O4@NC and its application for degradation of norfloxacin from aqueous solutions by activated peroxymonosulfate. . | Chemosphere , 2021 , 275 , 130059 . |
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摘要 ：
Etched graphite felt (EGF) was successfully fabricated using in situ CoOX etching process and used as a cathode to degrade diuron in the electro-Fenton (E-Fenton) process. The graphite felt prepared using the in situ CoOX etching process could markedly enhance the electrochemical properties with high electroactive surface area and rapid electron transfer capacity. Due to the high content of defects and porous structure, EGF electrode exhibited superior performance with high yield of hydrogen peroxide and rapid regeneration capacity of Fe2+, achieving 100% removal of diuron (20 mg/L) at -0.7 V/SCE within 50 min. In addition, the stability of the EGF cathode showed no significant decay in the performance after 35 cycles. EGF electrode had achieved good degradation effect for different pollutants, such as atrazine, amoxicillin, atenolol and 2, 4, 6-trichlorophenol. In three runs, the EGF cathode showed low Co leaching (< 1 ppm). Moreover, the possible degradation pathways of diuron were proposed by analyzing the intermediates in this work. The results obtained in this work highlight the potential of EGF electrode for use as an E-Fenton cathode.
关键词 ：
Defects Defects Degradation pathway Degradation pathway Electro-fenton Electro-fenton Graphite felt Graphite felt Porous structure Porous structure
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| GB/T 7714 | Qi, Haiqiang , Sun, Xiuping , Sun, Zhirong . Porous graphite felt electrode with catalytic defects for enhanced degradation of pollutants by electro-Fenton process [J]. | CHEMICAL ENGINEERING JOURNAL , 2021 , 403 . |
| MLA | Qi, Haiqiang et al. "Porous graphite felt electrode with catalytic defects for enhanced degradation of pollutants by electro-Fenton process" . | CHEMICAL ENGINEERING JOURNAL 403 (2021) . |
| APA | Qi, Haiqiang , Sun, Xiuping , Sun, Zhirong . Porous graphite felt electrode with catalytic defects for enhanced degradation of pollutants by electro-Fenton process . | CHEMICAL ENGINEERING JOURNAL , 2021 , 403 . |
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摘要 ：
Wastewater containing 2,4,6-trichlorophenol (2,4,6-TCP) is highly toxic and causes harmful effects on aquatic ecosystems and human health. In this study, wastewater containing high levels of 2,4,6-TCP was successfully co-metabolized by introducing municipal domestic wastewater (MDW) as the co-catabolic carbon source. The concentration of degraded 2,4,6-TCP increased from 0 to 208.71 mg/L by adjusting the influent MDW volume during a 150-day-long operation. An MDW dose of 500 mL was found optimal, with an average concentration of 250 mgCOD/L. Unlike the long-term experiment, changing the MDW adding mode in a typical cycle further increased the concentration of 2,4,6-TCP removed to 317 mg/L. The main MDW components, such as the sugars, VFAs, and slowly biodegradable organic substances, improved 2,4,6-TCP degradation, achieving a TOC removal efficiency of 90.98% and a dechlorination efficiency of 100%. The MDW level did not change the 2,4,6-TCP degradation rate (μTCP) in a typical cycle compared to the single carbon source, and the μTCP remained at a high level of 50 mg 2,4,6-TCP/h. Macrogenetic analysis demonstrated that MDW addition promoted the growth of 43 bacterial genera (41.49%) responsible for 2,4,6-TCP degradation and intermediates' metabolism. The key genes for 2,4,6-TCP metabolism (pcpA, chqB, mal-r, pcaI, pcaF, and fadA) were detected in the activated sludge, which were distributed among the 43 genera. To conclude, this study proposes a new carbon source for co-metabolism to treat 2,4,6-TCP-polluted wastewater.
关键词 ：
2,4,6-Trichlorophenol 2,4,6-Trichlorophenol Co-metabolism Co-metabolism Metagenomics Metagenomics Mixed carbon source Mixed carbon source Municipal domestic wastewater Municipal domestic wastewater
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| GB/T 7714 | Wang Jianguang , Sun Zhirong . Successful application of municipal domestic wastewater as a co-substrate in 2,4,6-trichlorophenol degradation. [J]. | Chemosphere , 2021 , 280 : 130707 . |
| MLA | Wang Jianguang et al. "Successful application of municipal domestic wastewater as a co-substrate in 2,4,6-trichlorophenol degradation." . | Chemosphere 280 (2021) : 130707 . |
| APA | Wang Jianguang , Sun Zhirong . Successful application of municipal domestic wastewater as a co-substrate in 2,4,6-trichlorophenol degradation. . | Chemosphere , 2021 , 280 , 130707 . |
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摘要 ：
In this paper, nanoscale Cu2O particles was successfully anchored at defect sites of carbon nanotubes (CNTs), which doped on three-dimensional copper foam (CF) electrode (Cu2O@CNTs/CF). The compound as cathode was synthesized via dip-coating and rapid electrodeposition followed by annealing procedure, and conducted in heterogeneous electro-Fenton (EF) system. The Cu2O@CNTs/CF composites electrode enabled activate O-2 to generate H2O2 in situ and further Cu-0/Cu2O synergistic catalysis to produce reactive oxygen species for a broad pH-range via the heterogeneous EF process. Cu-0 on the surface of CF also contributed to the reduction of Cu2+ to Cu+, thereby enhancing the stability of the electrode. The effects of critical parameters such as precursorligand dosage, the initial pH value, initial pollutant concentration and current density on the degradation of the antibiotic sulfamethoxazole (SMX) were investigated. The as-obtained electrode performed both effective catalytic activity and good reusability. Almost 100% removal rate was reached within 75 min over a broad pH range (3 to 11) during the heterogeneous EF process, with the current density of 12 mA cm(-2) and the removal efficiency of SMX decreased by only 9.0% after 8 recycle runs. Furthermore, quenching experiments indicated that hydroxyl radicals (center dot OH) were main species responsible for the SMX oxidation. In addition, the possible degradation pathways of SMX were proposed, which were based on nine identified intermediates. The comprehensivework is elucidated to accelerate the development of the in-situ production of H2O2 during the heterogeneous EF system and provide new insights to achieve high-efficiency degradation of pollutants via copper-based catalytic materials. (C) 2021 Elsevier B.V. All rights reserved.
关键词 ：
Cu+/Cu-0 Cu+/Cu-0 Heterogeneous electro-Fenton Heterogeneous electro-Fenton Sulfamethoxazole Sulfamethoxazole Broad pH Broad pH Copper foam Copper foam
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| GB/T 7714 | Mao, Shiqin , Sun, Xiuping , Qi, Haiqiang et al. CuO nanoparticles anchored on 3D bifunctional CNTs/copper foam cathode for electrocatalytic degradation of sulfamethoxazole over a broad pH range [J]. | SCIENCE OF THE TOTAL ENVIRONMENT , 2021 , 793 . |
| MLA | Mao, Shiqin et al. "CuO nanoparticles anchored on 3D bifunctional CNTs/copper foam cathode for electrocatalytic degradation of sulfamethoxazole over a broad pH range" . | SCIENCE OF THE TOTAL ENVIRONMENT 793 (2021) . |
| APA | Mao, Shiqin , Sun, Xiuping , Qi, Haiqiang , Sun, Zhirong . CuO nanoparticles anchored on 3D bifunctional CNTs/copper foam cathode for electrocatalytic degradation of sulfamethoxazole over a broad pH range . | SCIENCE OF THE TOTAL ENVIRONMENT , 2021 , 793 . |
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