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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY · 2021 · IF 6.291

Minute Cu2+ coupling with HCO3− for efficient degradation of acetaminophen via H2O2 activation

Yimin Zhang,Jingkun Lou,Leliang Wu,Minghua Nie,Caixia Yan,Mingjun Ding,Peng Wang,Hua Zhang

Homogeneous Cu 2+ -mediated activation of H 2 O 2 has been widely applied for the removal of organic contaminants, but fairly high dosage of Cu 2+ is generally required and may cause secondary pollution. In the present study, minute Cu 2+ (2.5 μM) catalyzed H 2 O 2 exhibited excellent efficiency in degradation of organic pollutants with the assistant of naturally occurring level HCO 3 − (1 mM). In a typical case, acetaminophen (ACE) was completely eliminated within 10 min which followed the pseudo-first-order kinetics. Singlet oxygen and superoxide radical rather than traditionally identified hydroxyl radical were the predominant reactive oxygen species (ROS) responsible for ACE degradation. Meanwhile, Cu 3+ was deduced through Cu + and p -hydroxybenzoic acid formation analysis. CuCO 3 (aq) was the main complex with high reactivity for the activation of H 2 O 2 to form ROS and Cu 3+ . The removal efficiency of ACE depended on the operating parameters, such as Cu 2+ , HCO 3 − and H 2 O 2 dosage, solution initial pH. The presence of Cl − , HPO 4 2− , humic acid were found to retard ACE removal while other anions such as SO 4 2− and NO 3 − had no obvious effect. ACE exhibited lower degradation efficiency in real water matrices than that in ultra-pure water. Nevertheless, 58–100% of ACE was removed from domestic wastewater, lake water and tap water within 60 min. Moreover, eight intermediate products were identified and the possible degradation pathways of ACE were proposed. Additionally, other typical organic pollutants including bisphenol A, norfloxacin, lomefloxacin hydrochloride and sulfadiazine, exhibited great removal efficiency in the Cu 2+ /H 2 O 2 /HCO 3 − system.

研究领域: 环境科学 · 化学
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NEW JOURNAL OF CHEMISTRY · 2022 ·Vol. 46 ·期 45 ·21560-21567 · IF 3.925

CoS2-decorated CdS nanorods for efficient degradation of organic pollutants

Jinyang Liu,Yan Zhou,Xiuniang Tan,Shengjiang Zhang,Chunjiao Mo,Xiaobo Hong,Taolong Wu,Xuecai Tan,Yanjuan Liao,Zaiyin Huang

The establishment of heterojunctions is an effective way to improve the performance of semiconductor photocatalysts as a solution to solve environmental pollution problems; however, the decomposition efficiency of organic pollutants driven by sunlight remains a challenge. Herein, CoS2-decorated CdS hetero-junctions as highly efficient photocatalysts were rationally synthesized via a three-step process and CoS2-decorated CdS composites were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, UV-Vis diffusion reflectance spectrometry, fluorescence spectroscopy analysis, X-ray photoelectron spectroscopy, electron paramagnetic resonance spectroscopy, and transient photocurrent measurement. Using organic dyes rhodamine B (Rh B) and nitenpyram (NTP) as model pollutants, the performance of the CoS2-decorated CdS composites for the degradation of model pollutants were evaluated. Among them, the material with the best performance can degrade 99.5% Rh B and 92.5% NTP within 120 min. Furthermore, the catalyst still maintained its high catalytic activity after five cycles. This work provides a new idea for developing efficient and inexpensive hetero-junctions as photo-catalysts.

研究领域: 环境科学 · 材料科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

Graphene quantum dot @ Flower-like Bi2S3 composites for photodegradation of organic pollutants combined photosynthesis of H2 and H2O2 from treated water

Jingjing Wang,Ruonan Liu,Yuxin Qiao,Shuxin Liu,Chuanguang Qin

In this work, flower-like Bi 2 S 3 was prepared by hydrothermal method using different solvents, and materials with better performance were selected. Graphene quantum dots (GQD, which is rich in specific amino groups) was prepared by aqueous phase fusion technology. Ultimately, a straightforward one-step hydrothermal process was used to successfully manufacture composite materials in order to build GQD(4)/Bi 2 S 3 heterostructures. The study results have shown that the H 2 production efficiency of 2% GQD(4)/Bi 2 S 3 is the best, and its photocatalytic hydrogen production efficiency within 3 h is 5.92 times that of GQD(4) and 3.03 times that of Bi 2 S 3 . The H 2 O 2 production and tetracycline (TC) degradation efficiency of 2% GQD(4)/Bi 2 S 3 are the best, while the methylene blue (MB) degradation efficiency of 1% GQD(4)/Bi 2 S 3 is relatively better. The research results show that as a perfect combination of GQD(4)/Bi 2 S 3 heterostructures, it offers a productive plan for eliminating organic pollutants in water and producing clean oxidant and hydrogen energy.

CAS / MDL: 10035-06-0
研究领域: 材料科学 · 环境科学 · 能源科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Interfacial complexation between Fe3+ and Bi2MoO6 promote efficient persulfate activation via Fe3+/Fe2+ cycle for organic contaminates degradation upon visible light irradiation

Chengbo Bai,Yuhan Zhang,Qiong Liu,Chengxin Zhu,Jun Li,Rong Chen

To address the observed decrease in efficiency during Fe 2+ -mediated persulfate (PDS) activation caused by slow electron transfer rates and challenges in cycling between Fe 3+ /Fe 2+ states, we devised a strategy to establish interfacial complexation between Fe 3+ and Bi 2 MoO 6 in the presence of PDS. The proposed approach facilitates more efficient capture of photogenerated electrons, thereby accelerating the rate-limiting reduction process of the Fe 3+ /Fe 2+ cycle under visible light irradiation and promoting PDS activation. The Bi 2 MoO 6 /Fe 3+ /PDS/Vis system demonstrates complete degradation of organic pollutants, including Atrazine (ATZ), carbamazepine (CBZ), bisphenol A (BPA), and 2,4-dichlorophenol (DCP) at a concentration of 10 mg/L within a rapid reaction time of 30 min. Radical scavenging experiments and electron paramagnetic resonance spectra (EPR) confirm that the sulfate radical (•SO 4 − ) is the dominant species responsible for organic contaminant degradation. The real-time conversion process between Fe 3+ and Fe 2+ was monitored by observing changes in iron species forms and concentrations within the reaction system. X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy verify the formation of a complexation between Fe 3+ and Bi 2 MoO 6 , facilitating anchoring of Fe 3+ onto material surface. Based on these findings, we propose a reliable mechanism for the activation reaction. This work presents a promising heterogeneous PDS activation method based on Fe 3+ /Fe 2+ cycle for water treatment.

研究领域: 环境科学 · 化学
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Desalination and Water Treatment · 2024 · IF 1

In situ-growth of Fe2S3 ultrathin layer on CdS nanorod through cation-exchange for efficient photocatalytic degradation of organic pollutants under visible light coupled oxidant activation

Junyi Wang,Jiaojiao Song,Qi Zhou

A new core-shell structure CdS@Fe 2 S 3 material was synthesized by in situ cation exchange method to enhance the degradation of organic pollutants in water under visible light. It is proved that Fe 2 S 3 nanolayer is successfully loaded on CdS nanorods by TEM and UV-Vis spectra and other means. The representative Rhodamine B was selected as the target pollutant and the results of degradation experiment showed that after 60 min of exposure to LED visible light with a low energy (25 W), the removal efficiency for this dye could reach 98 % in the presence of peroxymonosulfate (PMS) forming free radicals, which displayed a observed kinetic rate constant exceeding 0.62 min −1 that is approximately 5 times higher than the system without PMS addition and 10 times than the system with original CdS as catalyst. The result of inhibition experiments shows that sulfate radical (SO 4 ·- ) and singlet oxygen ( 1 O 2 ) play as important roles during the photocatalytic process. In addition, this core-shell material can be recycled at least four times. Generally, this study can make full use of visible light which can be easily obtained and effectually resolve the organic pollution problems.

CAS / MDL: 10108-64-2 81-88-9
研究领域: 环境科学 · 材料科学
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Environmental Science-Water Research & Technology · 2024 ·Vol. 10 ·期 8 ·1785-1794 · IF 3.5

Strongly enhanced persulfate activation by bicarbonate accelerated Cu(III)/Cu(I) redox cycles

Jun Zhang,Shenjun Wang,Yuhao Wu,Jiahai Ma

In advanced oxidation systems, the promoting effect of bicarbonate is relatively overlooked. Bicarbonate, as an inorganic anion widely present in natural waters, is extremely important for water treatment. Therefore, bicarbonate was added to a PDS/Cu2+ system to investigate the degradation mechanisms of organic contaminants. The generation of alkyl radicals in the PDS/Cu2+/HCO3− system was first demonstrated through Electron Paramagnetic Resonance (EPR) testing. This study reveals that the introduced bicarbonate ions undergo transformation into alkyl radicals. The presence of alkyl radicals promotes the cycling of monovalent, divalent, and trivalent copper ions, facilitating the degradation of contaminants. The production of monovalent and trivalent copper ions in the reaction system was confirmed through UV-vis absorption spectroscopy and quenching experiments. Furthermore, the change in the oxidation state of copper ions was further confirmed through EPR testing. These findings not only shed new light on the degradation mechanism of the PDS/Cu2+ system in the presence of bicarbonate but also open up new avenues for the further application of bicarbonate in advanced oxidation processes.

CAS / MDL: 144-55-8 70693-62-8
研究领域: 环境科学 · 化学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Uncovering the high-activity origin of sulfur doping in Co3O4 for organic pollutant degradation via peroxymonosulfate activation

Jiahong Pan,Zherui Wang,Jiajia Luo,Liwen Fan,Xinyun Li,Chenyi Wang,Yanqing Cong,Tong Wei,Shi-Wen Lv

Herein, a simple method for effective treatment of organic wastewater containing ofloxacin is proposed. Specifically, sulfur-doped Co 3 O 4 (abbreviated as S-Co 3 O 4 ) is first prepared and used then as a mediator to activate peroxymonosulfate (PMS). The sulfur doping can facilitate the conversion of low spin state Co to high spin state Co, thereby reducing the work function of Co 3 O 4 to improve internal electron escape probability. Meanwhile, the sulfur doping also induces to form more oxygen vacancies, decreasing interface resistance and accelerating charge transfer. As a result, the activation efficiency of PMS over S-Co 3 O 4 is enhanced. More importantly, the adsorption energy of PMS over S-Co 3 O 4 is reduced after the sulfur doping, leading to generate more S-Co 3 O 4 -PMS* complexes. Due to small activation energy, the S-Co 3 O 4 -PMS* complexes can be easily decomposed into SO 4 − and 1 O 2 . As predicted, the S-Co 3 O 4 -mediated PMS system shows excellent performance in ofloxacin degradation, and the removal efficiency is as high as 96.4 % within 20 min. In the S-Co 3 O 4 -2-mediated PMS system, the contribution rate of active species for ofloxacin degradation follows an order of SO 4 −  >  1 O 2  >  Co 4+ O > OH . Furthermore, the S-Co 3 O 4 -2-mediated PMS system with good stability exhibits strong removal ability towards other organic pollutants.

研究领域: 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Mn2O3@Mn5O8 as an efficient catalyst for the degradation of organic contaminants in aqueous media through sulfite activation

Aimal Khan,Xianjie Feng,Chuankun Yin,Habib Ullah,Asif Ali Tahir,Bowen Li,Weiming Wang,Xiaoxia Li,Aihua Xu

Less-toxic, cost-effective, stable, and highly efficient catalysts for sodium sulfite (S(IV)) activation are required to degrade organic pollutants from wastewater. Herein, we report the facile thermal synthesis of Mn 2 O 3 @Mn 5 O 8 that activates S(IV) more efficiently than other Mn and transition-metal oxides. Mn 2 O 3 @Mn 5 O 8 exhibits good performance and long-term stability for eliminating various contaminants from aqueous media, including phenol, bisphenol A, nitrobenzene, 2,4-dichlorophenol, and acetaminophen. Its high performance is attributed to its multivalency, unique architecture, surface hydroxyl groups (–OH), and high surface area. X-ray diffractometry and high-resolution transmission electron microscopy revealed that Mn 2 O 3 @Mn 5 O 8 comprises well-combined cubic Mn 2 O 3 and monoclinic Mn 5 O 8 crystalline structures, whereas electron paramagnetic resonance spectroscopy and scavenging tests showed that SO 5 •− , SO 4 •− , and •OH radicals are generated during S(IV) activation, with SO 3 •− as a precursor. The mixed-valence state provides effective and favorable electron transfer via Mn redox cycling (Mn(II) ↔ Mn(III) ↔ Mn(IV)), improving the S(IV) activation performance and catalytic activity. Mn 2 O 3 @Mn 5 O 8 /S(IV) system shows stable performance in the 3.0–7.0 pH range. Density functional theory calculations confirmed the higher catalytic activity as indicated by high –OH adsorption energy and significant inter-charge transformation. This study provides new insights and strategies for the activation of S(IV) using less-toxic metal oxides as catalysts and broadens the scope of heterogeneous Mn-based catalysts and S(IV) chemistry in real-world applications, particularly for the treatment of wastewater.

研究领域: 环境科学 · 材料科学 · 化学
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WATER SCIENCE AND TECHNOLOGY · 2021 ·Vol. 85 ·期 1 ·39-51 · IF 1.915

Peroxydisulfate activation by LaNiO3 nanoparticles with different morphologies for the degradation of organic pollutants

Wei Yan,Leng Yanqiu,Wang Rongyao,Ren Xiaohua,Guo Weilin

A series of LaNiO 3 perovskite nanoparticles with different morphologies, such as spheres, rods and cubes, were prepared through co-precipitation and hydrothermal methods, and used as the catalysts for peroxydisulfate (PDS) activation. The physical and chemical characterization of LaNiO 3 perovskites was performed, including X-ray diffraction (XRD), scanning electron microscopy (SEM), nitrogen isotherm absorption (BET), electrochemical impedance spectroscopy (EIS), and X-ray photoelectron spectroscopy (XPS). The LaNiO 3 with different shapes showed different activities in Acid Orange 7 (AO7) degradation. Sphere-like LaNiO 3 exhibited the highest catalytic activity, which is probably due to the largest specific surface area, higher proportion of reductive Ni 2+ and the higher electron transfer ability. The radical scavenging experiments and electron paramagnetic resonance (EPR) revealed the production of massive sulfate radicals (SO 4 •− ) and hydroxyl radicals ( • OH) during the oxidation. Finally, the possible mechanisms of PDS activation and AO7 degradation were proposed. The prepared LaNiO 3 perovskites also showed excellent reusability and stability. Three LaNiO 3 perovskites with different morphologies were synthesized. Sphere-like LaNiO 3 exhibited the highest catalytic activity for activating PDS. Produced • OH and SO 4 •− were main active species in the reaction system. The mechanism of AO7 degradation reaction in the system was proposed. LaNiO 3 can be reused for multiple cycles to activate PDS for AO7 degradation.

研究领域: 环境科学 · 材料化学 · 催化化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Mechanism of contaminants degradation in aqueous solution by persulfate in different Fe(II)-based synergistic activation environments: Taking chlorinated organic compounds and benzene series as the targets

Zhengyuan Zhou,Jingyao Huang,Zhiqiang Xu,Meesam Ali,Ali Shan,Rongbing Fu,Shuguang Lyu

In this study, trichloroethene (TCE) removal was remarkably enhanced with the addition of Fe(II)/CA (citric acid), Fe(II)/nZVI (nano zero-valent iron) and Fe(II)/S-nZVI (sulfidated nano zero-valent iron), respectively, as synergistic activated catalysts in persulfate environment. Among them, the better performance of TCE removal followed the order of PS/Fe(II)/S-nZVI > PS/Fe(II)/nZVI > PS/Fe(II)/CA ≫ PS/Fe(II), and the majority of TCE was declorinated to Cl − . The scavenger and EPR tests indicated that HO and SO 4 − were responsible for TCE degradation. Further study was conducted through the calculation of reaction rate constants, demonstrating HO produced from SO 4 − was of greater significance than SO 4 − itself. With the presence of CA , the concentration of Fe(II) was maintained at a desired level to proceed the catalytic activity. Meanwhile, S-nZVI and nZVI had ability to convert Fe(III) to Fe(II), and sulfur species, especially S(-II) in S-nZVI acted as an reductant to a certain extent. Sufficient Fe(II) in solution activated PS to produce adequate HO for TCE degradation. Furthermore, the broad-spectrum reactivity in different systems were investigated, and the results indicated that most of the chloroalkenes and benzene series frequently detected in contaminated sites could also be removed at the desired chemicals ratio. In conclusion, this research revealed the superiority of synergistic activated catalysts and provided theoretical bases for the remediation of TCE and other pollutants in actual contaminated groundwater.

研究领域: 环境科学 · 化学工程
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING · 2019 · IF 2.722

Design and synthesis of Mo2C/MoO3 with enhanced visible-light photocatalytic performance for reduction of Cr (VI) and degradation of organic pollutants

Xinbo Jing,Xueying Peng,Xiyin Sun,Wu Zhou,Wei Wang,Shufen Wang

In this study, a facile impregnation-calcination strategy was applied in order to synthesize Mo2C modified MoO3 (Mo2C/MoO3), which was then employed as catalyst for the photoreduction of Cr (VI) and photodegradation of methyl orange (MO) upon irradiation by visible light (λ > 400 nm). The apparent rate constant (k) of Mo2C/MoO3 for the MO photocatalyzed degradation reaction under visible-light irradiation was found to be 0.0171 min-1, which was 4.59 and 67.38 times higher than that of Pt/MoO3 and pristine MoO3, respectively. Study of the photocatalytic mechanism revealed that the •O2- species played a major role in MO degradation. Moreover, the addition of Mo2C enhanced the light response region of MoO3, and also promoted the photocatalytic activity of MoO3. This was due to the enhanced separation efficiency of photogenerated electron-hole pairs and broader photoresponse region. This work suggests a new use for the easily accessible Mo2C/MoO3 heterostructure and could facilitate the application of photocatalysts for wastewater treatment.

研究领域: 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2020 · IF 5.774

Enhancement of organic contaminants degradation at low dosages of Fe(III) and H2O2 in g-C3N4 promoted Fe(III)/H2O2 system under visible light irradiation

Hao Xu,Qian Ye,Qingguo Wang,Peng Zhou,Xiaowei Huo,Yunqi Wang,Xue Huang,Guanyu Zhou,Jing Zhang

Developing a low-cost and environmental friendly way to promote the Fe(III)/Fe(II) cycling is crucial to enhance the efficiency of Fenton reaction. In this study, g-C 3 N 4 was introduced into the Fe(III)/H 2 O 2 system as electron donor to accelerate Fe(III)/Fe(II) cycling and improve the degradation of organic pollutants under visible light. The g-C 3 N 4 /Fe(III)/H 2 O 2 /light system can achieve excellent degradation of different kinds of organic pollutants under low Fe(III) and H 2 O 2 dosages. The central composite design (CCD) and response surface methodology (RSM) were applied to evaluate the effects of g-C 3 N 4 dosage, Fe(III) dosage, H 2 O 2 dosage and light intensity on the DMP degradation efficiency. The mechanisms were investigated by quenching experiments and electron spin resonance (EPR) analyses that the photo-generated electrons and O 2 – were responsible to the Fe(III) reduction through interfacial and aqueous pathways, respectively. OH was the dominant reactive radical in the DMP degradation. Moreover, DMP degradation routes were proposed including the elimination of specific groups, the hydroxylation process and the ring-opening reactions. This study demonstrates an economical and green approach which provides a promising direction for the practical application of g-C 3 N 4 based photocatalysis by integrating it with the Fe(III)/H 2 O 2 Fenton process.

研究领域: 环境科学 · 化学工程
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