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学者姓名:孙治荣
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摘要 :
In this study, a coral-like Co-N-doped carbon (Co@NC) was prepared through a simple one-pot synthesis method. The catalyst effectively activated peroxymonosulfate (PMS) for sulfamethazine (SMZ) degradation via nonradical pathways, achieving a 100 % removal efficiency of SMZ within 20 min. The Co@NC/PMS system maintained excellent removal capability for SMZ under a broad range of pH (3.0-9.0) and pollutant concentrations (10 mg/L-50 mg/L). Mechanistic studies suggested that the synergistic interaction between Co-Nx sites and graphitic carbon facilitated the generation of singlet oxygen (1O2) and high valent cobalt-oxo species (Co (IV) = O), which played dominant roles in the degradation of SMZ. Investigating the effects of different concentrations of anions and humic acid on SMZ degradation, the Co@NC/PMS system demonstrated resistance to interference from common water constituents. Upon examining the degradation capability of the Co@NC/PMS system against different pollutants, the system exhibited selective oxidation towards organic pollutants containing electron-donating moieties, such as hydroxyl and amide groups. This study synthesized a novel Co-Ndoped carbon as a highly efficient activator for PMS and conducted an in-depth investigation into the mechanism of SMZ degradation dominated by non-radical pathways.
关键词 :
Singlet oxygen Singlet oxygen Sulfamethazine Sulfamethazine Selective oxidation Selective oxidation High-valent cobalt-oxo species High-valent cobalt-oxo species Peroxymonosulfate activation Peroxymonosulfate activation
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GB/T 7714 | Li, Yajing , Liu, Zhibin , Sun, Zhirong . A novel Co-N-doped carbon catalyst to activate peroxymonosulfate for efficient removal of sulfamethazine: Role of singlet oxygen and high-valent cobalt-oxo species [J]. | JOURNAL OF WATER PROCESS ENGINEERING , 2024 , 63 . |
MLA | Li, Yajing 等. "A novel Co-N-doped carbon catalyst to activate peroxymonosulfate for efficient removal of sulfamethazine: Role of singlet oxygen and high-valent cobalt-oxo species" . | JOURNAL OF WATER PROCESS ENGINEERING 63 (2024) . |
APA | Li, Yajing , Liu, Zhibin , Sun, Zhirong . A novel Co-N-doped carbon catalyst to activate peroxymonosulfate for efficient removal of sulfamethazine: Role of singlet oxygen and high-valent cobalt-oxo species . | JOURNAL OF WATER PROCESS ENGINEERING , 2024 , 63 . |
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摘要 :
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.
关键词 :
Active oxygen species Active oxygen species Heterogeneous electro-Fenton Heterogeneous electro-Fenton Sulfamethoxazole Sulfamethoxazole Copper -based nanocatalysts Copper -based nanocatalysts Synergistic effect 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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摘要 :
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.
关键词 :
Superoxide anion radical Superoxide anion radical Phosphorus doped electrode Phosphorus doped electrode Degradation pathways Degradation pathways Cu2PO4 Cu2PO4 Etched graphite felt 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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摘要 :
A new type of catalyst based on electrolytic manganese anode slime (EMAS) for heterogeneous peroxymonosulfate (PMS) activation in acetaminophen (APAP) degradation was prepared. The EMAS was modified by washing, pickling, and calcination to produce the DEMAS200 catalyst, and multi-types of refractory organic matter could be degraded by the DEMAS200/PMS system, of which 20 mg/L APAP can be removed within 4 min. A radical activation mechanism based on PMS was proposed through a series of APAP degradation experiments and material characterization. By quenching, probing, PMSO experiments, and electron paramagnetic resonance (EPR), the major contribution of various reactive oxygen species (ROS) (such as center dot OHfree, SO4 center dot-, high-valent Mn species, O-1(2) and O-2(center dot-)) was excluded, and center dot OHads was verified as the major ROS. Nuclear magnetic resonance (NMR) was applied to identify active hydrogen using the D2O exchange method to qualitatively identify the presence of center dot OHads, which was determined by comparing the appearance and disappearance of chemical shifts at 1.90 ppm (active hydrogen) and 7.96 ppm (hydrogen at the benzene ring on TPA). In this study, the modified EMAS was innovatively introduced for PMS activation in the degradation of APAP, and NMR technology successfully identified the presence of different hydroxyls.
关键词 :
Adsorbed center dot OH Adsorbed center dot OH Electrolytic manganese anode slime Electrolytic manganese anode slime PMS activation PMS activation NMR NMR
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GB/T 7714 | Wan, Qiuyue , Yang, Jingjie , Sun, Zhirong . Adsorbed hydroxyl radicals dominated peroxymonosulfate activation in acetaminophen degradation using modified electrolytic manganese anode slime: Catalyst evaluation and free radical identification [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 486 . |
MLA | Wan, Qiuyue et al. "Adsorbed hydroxyl radicals dominated peroxymonosulfate activation in acetaminophen degradation using modified electrolytic manganese anode slime: Catalyst evaluation and free radical identification" . | CHEMICAL ENGINEERING JOURNAL 486 (2024) . |
APA | Wan, Qiuyue , Yang, Jingjie , Sun, Zhirong . Adsorbed hydroxyl radicals dominated peroxymonosulfate activation in acetaminophen degradation using modified electrolytic manganese anode slime: Catalyst evaluation and free radical identification . | CHEMICAL ENGINEERING JOURNAL , 2024 , 486 . |
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摘要 :
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.
关键词 :
Heterogeneous electro-Fenton process Heterogeneous electro-Fenton process In-situ catalysis In-situ catalysis Chloroquine phosphate Chloroquine phosphate Polyvalent metals synergistic effect 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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摘要 :
Peracetic acid (PAA), as a disinfectant with powerful oxidation and exceptional antimicrobial efficiency, has gained considerable attention for its application in advanced oxidation processes (AOPs). However, leaching of metal ions and low recovery efficiency limited the application of heterogeneous AOPs. Herein, we synthesized a Co-Fe bimetallic oxide (Co -Fe -O) derived from Prussian blue analogs to serve as an activator for PAA, efficiently eliminating sulfamethazine (SMZ) in a wide pH range (5-9). Electron paramagnetic resonance and quenching test revealed the coexistence of radical species in the system, and R-O & sdot; were the main factors of SMZ elimination. The steady-state model evaluation showed that 3.1 x 10-14 M R-O & sdot; and 2.05 x 10-14 M & sdot;OH existed in the system. Co-Fe bimetallic synergies expedite the generation of radical species. Based on density functional theory, the aniline ring and heterocyclic ring of SMZ were regarded as the susceptible sites for radical attack and electron transfer. Furthermore, the elimination pathway of SMZ was proposed by combining the results of intermediate products. Additionally, the toxicity of SMZ and intermediates as well as the reaction conditions, water matrices, stability, and oxidation capacity of Co-Fe-O/PAA were subjected to evaluation. Results indicate that the Co-Fe-O/PAA system has significant application potential in the elimination of micropollutants.
关键词 :
Co(II)/Co(III) redox cycle Co(II)/Co(III) redox cycle Peracetic acid Peracetic acid Prussian blue analogs Prussian blue analogs Bimetallic synergy Bimetallic synergy Organic radicals Organic radicals
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GB/T 7714 | Jiang, Bingyu , Liu, Zhibin , Sun, Zhirong . Co-Fe bimetallic oxides derived from Prussian blue analogs to activate peracetic acid for eliminating sulfamethazine: Contribution and identification of radical species [J]. | JOURNAL OF WATER PROCESS ENGINEERING , 2024 , 60 . |
MLA | Jiang, Bingyu et al. "Co-Fe bimetallic oxides derived from Prussian blue analogs to activate peracetic acid for eliminating sulfamethazine: Contribution and identification of radical species" . | JOURNAL OF WATER PROCESS ENGINEERING 60 (2024) . |
APA | Jiang, Bingyu , Liu, Zhibin , Sun, Zhirong . Co-Fe bimetallic oxides derived from Prussian blue analogs to activate peracetic acid for eliminating sulfamethazine: Contribution and identification of radical species . | JOURNAL OF WATER PROCESS ENGINEERING , 2024 , 60 . |
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摘要 :
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.
关键词 :
Heterogeneous electro-Fenton Heterogeneous electro-Fenton Heterointerface Heterointerface Electron transfer Electron transfer Bimetallic catalyst 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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摘要 :
In this study, a 3D CoNiO2/Co core-shell structure biochar catalyst derived from walnut shell was synthesized by hydrothermal and ion etching methods. The prepared BC@CoNi-600 catalyst exhibited exceptional peroxymonosulfate (PMS) activation. The system achieved 100 % degradation of sulfamethoxazole (SMX). The reactive oxygen species in the BC@CoNi-600/PMS system included SO4 center dot-, center dot OH, and O-2(center dot-). Density functional theory calculations explored the synergistic effects between nickel-cobalt bimetallic and carbon matrix during PMS activation. The unique 3D core-shell structure of BC@CoNi-600 features an outer nickel-cobalt bimetallic layer with exceptional PMS adsorption capacity, while protecting the zero-valence Co of the inner layer from oxidation. Based on the experimental-data, machine learning modeling mechanism, and information theory, a nonlinear modeling method was proposed. This study utilizes a machine learning approach to investigate the degradation of SMX in complex aquatic environments. This study synthesized a novel biochar-based catalyst for activated PMS and provided unique insights into its environmental applications.
关键词 :
Biochar Biochar Active species transformation Active species transformation Peroxymonosulfate Peroxymonosulfate Machine learning Machine learning Density functional theory Density functional theory
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GB/T 7714 | Liu, Zhibin , Shi, Xuelin , Yan, Zihao et al. Synergistic activation of peroxymonosulfate by 3D CoNiO2/Co core-shell structure biochar catalyst for sulfamethoxazole degradation [J]. | BIORESOURCE TECHNOLOGY , 2024 , 406 . |
MLA | Liu, Zhibin et al. "Synergistic activation of peroxymonosulfate by 3D CoNiO2/Co core-shell structure biochar catalyst for sulfamethoxazole degradation" . | BIORESOURCE TECHNOLOGY 406 (2024) . |
APA | Liu, Zhibin , Shi, Xuelin , Yan, Zihao , Sun, Zhirong . Synergistic activation of peroxymonosulfate by 3D CoNiO2/Co core-shell structure biochar catalyst for sulfamethoxazole degradation . | BIORESOURCE TECHNOLOGY , 2024 , 406 . |
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摘要 :
一种用于非均相电芬顿体系的负载铜铝层状双金属氧化物改性石墨毡电极的制备及应用,属于电化学水处理技术领域。本发明以热处理的石墨毡为基体,通过水热法将铜铝双金属氢氧化物分散于热处理石墨毡表面,在强持续通入氮气的条件下高温煅烧,可获得以Cu2O、CuO为主要活性组分的改性石墨毡电极。与原始石墨毡及热处理石墨毡相比,以负载铜铝双金属氧化物改性石墨毡电极作为阴极材料时,非均相电芬顿体系对磺胺甲恶唑废水的降解效率得到了较大提高,且该阴极的离子浸出率较低,稳定性较强,具有较好的应用前景。
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GB/T 7714 | 孙治荣 , 李耀红 . 一种用于非均相电芬顿体系的负载铜铝层状双金属氧化物改性石墨毡电极的制备及应用 : CN202310258855.3[P]. | 2023-03-16 . |
MLA | 孙治荣 et al. "一种用于非均相电芬顿体系的负载铜铝层状双金属氧化物改性石墨毡电极的制备及应用" : CN202310258855.3. | 2023-03-16 . |
APA | 孙治荣 , 李耀红 . 一种用于非均相电芬顿体系的负载铜铝层状双金属氧化物改性石墨毡电极的制备及应用 : CN202310258855.3. | 2023-03-16 . |
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摘要 :
一种生物质炭原位生长钴和钴钨氧化物复合催化剂的制备及应用,属于高级氧化技术领域。本发明以核桃壳为回收生物质,通过水热、钨掺杂和高温煅烧的方法,合成了生物质炭原位生长钴和钴钨氧化物复合催化剂,用于活化过氧单硫酸盐降解金霉素。该催化剂以回收生物质为基体,实现了资源的回收与利用。钨的修饰使催化剂具有丰富的氧空位,使催化剂活化过氧单硫酸盐时产生大量的单线态氧,有利于提高污染物降解速率。并且氧空位促进了钴的价态循环,可有效减少离子浸出,提高了催化剂的催化效率和循环使用能力。在难降解有机废物处理方面具有较好的应用前景。
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GB/T 7714 | 孙治荣 , 刘智斌 . 一种生物质炭原位生长钴和钴钨氧化物复合催化剂的制备及应用 : CN202310558918.7[P]. | 2023-05-17 . |
MLA | 孙治荣 et al. "一种生物质炭原位生长钴和钴钨氧化物复合催化剂的制备及应用" : CN202310558918.7. | 2023-05-17 . |
APA | 孙治荣 , 刘智斌 . 一种生物质炭原位生长钴和钴钨氧化物复合催化剂的制备及应用 : CN202310558918.7. | 2023-05-17 . |
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