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APPLIED CATALYSIS A-GENERAL · 2024 · IF 4.7

Degradation of emerging pollutant CBZ by a novel hydrogen-promoted Fenton system constructed with Pd/UiO-66(Zr)-2OH

Xin-Hao Shen,Feng Liu,Qin-Qin Chen,Ying Gao,Xiao-Wen Wang,Xin Liu

The efficient degradation of emerging pollutants in water, represented by CBZ, is receiving increasing attention from all sectors of society. Although advanced oxidation reactions represented by Fenton reaction can efficiently degrade emerging pollutants, the problem of iron sludge that comes with it is hindering the further promotion of this technology. Herein, UiO-66(Zr)-2OH material was synthesized by hydrothermal method and loaded with Pd 0 NPs on the surface of the material by in situ reduction. The MOFs-H 2 -Accelerated Catalytic Fenton system was constructed by accelerating the regeneration of Fe(II) in the system by activating the [H] produced by H 2 introduced into the system at room temperature and pressure. Within 180 min, the removal of the target pollutant CZB could reach more than 99 % under the condition of only 25 µmol of Fe(II) and 25 mmol of H 2 O 2 .

研究领域: 环境科学 · 材料科学 · 化学工程
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Journal of Environmental Chemical Engineering · 2025 · IF 7.2

Selective FeOx deposition on BiVO4 (010) Facet: boosting visible-light-driven photo-Fenton degradation of PPCPs

Sha Shi,Jihui Wang,Chunhong Xu,Jie Mao,Yaohui Bai

Carbamazepine (CBZ), a typical pharmaceutical and personal care product (PPCP), has an annual global consumption exceeding several thousand tons. Its molecular structure contains symmetrical nitrogen-containing aromatic heterocycles, which resist degradation by conventional biochemical methods, resulting in persistent aquatic pollution. Integrating photocatalytic processes with Fenton reaction provides a targeted approach for its effective elimination from aquatic systems. However, traditional photo-Fenton systems suffer from inefficient Fe 3+ /Fe 2+ redox cycling due to sluggish Fe³⁺ regeneration and rapid recombination of photogenerated charge carriers. To address these challenges, this study designed a facet-engineered BiVO 4 photocatalyst through selective deposition of FeOx nanoparticles on the electron-rich (010) facets of monoclinic BiVO 4 via hydrothermal and photodeposition methods. The optimized FeOx/BiVO 4 composite exhibited exceptional degradation performance for CBZ, achieving a rate constant of 0.317   min -1 , which is 24-fold higher than that of pristine BiVO 4 . Mechanistic investigations revealed that the selective FeOx deposition not only promoted the valence-state transition of Fe 3+ to Fe 2+ but also enhanced charge carrier separation, thereby establishing a sustainable Fe 3+ /Fe 2+ redox cycle. Electron paramagnetic resonance (EPR) analysis and radical quenching experiments further identified hydroxyl radicals (·OH) as the dominant reactive species. This work provides a paradigm for designing efficient photo-Fenton reaction systems through targeted facet engineering, offering broad implications for the remediation of PPCPs.

研究领域: 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Fe3O4 decorated with α-cyclodextrin for enhanced peroxymonosulfate(PMS)-activated degradation of PPCPs

Xi Quan,Jun Zhang,Linlin Yin,Wei Zuo,Yu Tian

In this work, novel Fe 3 O 4 @α-CD nanoparticle was synthesized for the catalytic activation of peroxymonosulfate (PMS) towards carbamazepine (CBZ) degradation. The effect of α-CD content, Fe 3 O 4 @α-CD dosage and PMS concentration on the catalyst activity were systematically evaluated. The results showed the synergistic effect between α-CD and Fe 3 O 4 can greatly improve the removal efficiency of CBZ in the Fe 3 O 4 @α-CD/PMS system. CBZ removal efficiency gained 73.37% in 5 min at pH 7.0 with PMS 1 mM, Fe 3 O 4 @α-CD load 0.4 g/L and CBZ 10 μM. The variation in the removal efficiency of different PPCPs under the same conditions mainly ascribed to the adsorption of α-CD and the activation of PMS by Fe 3 O 4 to generate free radicals, in which sulfate radical (SO 4 ·− ) and hydroxyl radicals ( · OH) was determined as the reactive species in the Fe 3 O 4 @α-CD/PMS system. Density functional theory (DFT) calculations was also utilized to optimize the structure of composite and confirmed that the charge distribution mainly concentrate on Fe 3 O 4 . As deduced from the LC-MS analysis, the possible CBZ degradation pathways were proposed. CBZ degradation efficiency still reached 54% after three cycle, which indicates that Fe 3 O 4 @α-CD catalyst has a good reusability potential and practical applications.

研究领域: 环境科学 · 材料科学 · 催化化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

Synergistic adsorption and degradation of CBZ by an adenine-anchored porous iron-based catalyst

Chengwen Zhang,Zihan Li,Chengbo Qian,Ziyang Ye,Feifan Yu,Yuyuan Yao

Developing porous iron-based catalysts with high metal loading for highly efficient removal of the organic pollutants has been a challenge in environmental catalysis. In this work, the preparation of porous iron–nitrogen-co-doped carbon catalyst (pNC-Fe) innovatively utilized zinc nitrate (Zn(NO 3 ) 2 ) as a pore-forming agent and adenine for metal anchoring. The resulting catalyst possessed a high Fe loading (18.49 wt%) and a high specific surface area (395.69 m 2 /g), which enhanced the adsorption and degradation of pNC-Fe. As a demonstration, the maximum adsorption capacity of pNC-Fe for CBZ (389.7 mg/g) surpassed nearly all recently reported CBZ adsorbents. Additionally, pNC-Fe possessed an excellent adsorption regeneration capability even after 5 cycles, enhancing its reusability. Surprisingly, pNC-Fe in PMS system removed almost 100 % of 50 μmol/L carbamazepine (CBZ) in 15 min and performed an excellent k obs (0.5895 min −1 ), outperforming the majority of metal-based catalysts. Interestingly, the adsorption of CBZ by pNC-Fe also remarkably facilitated the degradation of CBZ. Notably, different from the free radical mechanism of most reported work, the quenching experiments and EPR detection demonstrated that the main reactive oxygen species (ROS) of the pNC-Fe/PMS system was singlet oxygen ( 1 O 2 ), endowing pNC-Fe with potential environmental anti-interference capability (less affected by common anions and pH variations). This work provides a valuable insight for the design of porous iron-based catalysts for wastewater remediation.

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Applied Sciences-Basel · 2024 ·Vol. 14 ·期 13 ·5431 · IF 2.5

Visual Analysis of Carbendazim Residues in Carrot Tubers via Postionization Mass Spectrometry Imaging

Tianyu Wang,He Zhang,Yongjun Hu

Carbendazim (CBZ) residues in food are a severe threat to food safety, and their detection is a challenging problem in food science. We introduce here a new method based on laser desorption postionization mass spectrometry imaging (LDPI-MSI) for detecting CBZ residues in carrots. In the novel LDPI-MSI method, two distinct laser beams simultaneously exert dissociation and ionization, which offers several advantages over traditional techniques based on single-photon matrix-assisted laser desorption/ionization mass spectrometry imaging (MALDI-MSI), including simplified sample preparation, streamlined operation workflow, and a lower limit of detection (LOD). The LOD, in the proposed method, has been lowered to 0.019 ppm. Coupled with mass spectrometry imaging (MSI), the LDPI-MS method enabled in situ detection of small molecular compounds, such as chemical pesticides, and provided comprehensive and accurate results. The image obtained from the characteristic mass spectrometric signature of CBZ at m/z 191 illustrated that most of the CBZ could not enter the carrot tubers directly, but a small amount of CBZ entered the carrot root and was mainly concentrated in the central xylem. The results suggest that the proposed method could potentially be used in pesticide analysis.

CAS / MDL: 10605-21-7 7782-42-5
研究领域: 食品安全 · 分析化学 · 植物科学
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Foods · 2023 ·Vol. 12 ·期 12 ·2277 · IF 5.2

Electrochemical Sensor Based on Laser-Induced Graphene for Carbendazim Detection in Water

Li Wang,Mengyue Li,Bo Li,Min Wang,Hua Zhao,Fengnian Zhao

Carbendazim (CBZ) abuse can lead to pesticide residues, which may threaten the environment and human health. In this paper, a portable three-electrode sensor based on laser-induced graphene (LIG) was proposed for the electrochemical detection of CBZ. Compared with the traditional preparation method of graphene, LIG is prepared by exposing the polyimide film to a laser, which is easily produced and patterned. To enhance the sensitivity, platinum nanoparticles (PtNPs) were electrodeposited on the surface of LIG. Under optimal conditions, our prepared sensor (LIG/Pt) has a good linear relationship with CBZ concentration in the range of 1–40 μM, with a low detection limit of 0.67 μM. Further, the sensor shows good recovery rates for the detection of CBZ in wastewater, which provides a fast and reliable method for real-time analysis of CBZ residues in water samples.Keywords:carbendazim;laser-induced graphene;platinum nanoparticles;electrochemical detection;water sample

CAS / MDL: 501-53-1 298-00-0
研究领域: 环境科学 · 分析化学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Oxygen vacancies enhanced natural manganese sand activation by PMS for CBZ degradation: Intermediate toxicity and DFT calculations

Weibao Liu,Ying Yang,Yunhe Li,Yuerong Zhou,Ce Wang,Yingtang Zhou,Jiangwei Shang,Xiuwen Cheng

The preparation of sulfate-based advanced oxidation catalysts is usually both complex and expensive. In this study, natural manganese sand enriched with oxygen vacancies was prepared by NaBH 4 reduction of natural manganese sand for activating peroxymonosulfate (PMS) to remove carbamazepine (CBZ). 70% of carbamazepine was degraded at 120 min when natural manganese sand enriched with oxygen vacancies and PMS were dosed at 0.4 g/L and 0.3 g/L respectively, and the reaction rate constant of the natural manganese sand system with rich oxygen vacancies was 7 times that of the common system. The mineralization of total organic carbon (TOC) reached 41.9%. Combined EPR and radical quenching assays revealed that degradation of pollutants relied on the involvement of free radicals and non-free radicals, in which singlet oxygen was dominant. The XPS results showed that the redox cycles of Fe 3+ /Fe 2+ and Mn 4+ /Mn 3+ /Mn 2+ promoted the generation of free radicals. Density functional theory results also showed that the energy required for PMS to adsorb on natural manganese sand with many oxygen vacancies was decreased, and the O O bond was elongated, which was beneficial to the catalytic reaction. According to LC-MS and Fukui function, the degradation route of CBZ was predicted, and the toxicity of the breakdown products was calculated. The research provides a reference for introducing oxygen vacancies in natural catalysts to improve degradation performance for “green (source) to green (application)”.

CAS / MDL: 7727-21-1
研究领域: 环境科学 · 催化化学
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Environmental Science-Nano · 2020 ·Vol. 7 ·期 4 ·1205-1213 · IF 7.683

Molten NaCl-induced MOF-derived carbon-polyhedron decorated carbon-nanosheet with high defects and high N-doping for boosting the removal of carbamazepine from water

Dezhi Chen,Shoujun Wang,Zhiming Zhang,Hongying Quan,Yachao Wang,Yijie Jiang,Matthew J. Hurlock,Qiang Zhang

The efficient removal of endocrine-disrupting pollutants (EDCs) from water is a crucial issue for improving the quality of drinking water. Herein, hierarchically structured carbon composites (HCCs) composed of carbon-polyhedron decorated carbon nanosheets were fabricated using the zeolite imidazole framework-8 (ZIF-8) as the precursor in the presence of molten NaCl. The as-prepared hierarchical carbon composites showed higher specific surface areas, more defects, high N-doping, and hydrophilicity compared with the NaCl-free ZIF-8-derived carbon polyhedrons (CPs). In addition, the as-prepared HCCs exhibited boosted adsorption performances for the removal of the model EDC, namely carbamazepine (CBZ), surpassing CPs and commercial powdered activated carbon (AC). The adsorption kinetics showed that HCCs possessed a higher sorption rate as compared to CPs and AC. In the initial 5 min, the adsorption amount of CBZ on HCCs reached 94.9% of the adsorption quantity at equilibrium. Furthermore, the maximum adsorption capacity of CBZ on HCCs is 248.7 mg g−1, which is superior to that of CPs and AC. X-ray photoelectron spectroscopy characterizations indicated that the predominant factors for controlling the adsorption of CBZ on HCCs are π–π electron donor–acceptor interactions and hydrogen bonding, although, some of the adsorbed CBZ molecules were decomposed by oxidation. Finally, a fixed-bed experiment demonstrated that the HCCs have great potential as a filler for the purification of tap water.

研究领域: 环境科学 · 材料科学
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BIOTECHNOLOGY LETTERS · 2016 ·Vol. 38 ·期 7 ·1121-1129 · IF 1.639

PEGylation of cytochrome c at the level of lysine residues mediated by a microbial transglutaminase

Zhou Jian Qin,He Ting,Wang Jian Wen

Objectives To establish a method for microbial trans glutaminase (mTG)-mediated PEGylation of proteins at the level of lysine (Lys) residues. Results Carboxybenzyl-glutaminyl–glycinyl-methoxypolyethylene glycol (CBZ-QG-mPEG) was prepared by introducing carboxybenzyl-glutaminyl-glycine (CBZ-QG) to mPEG amine. The analysis by Fourier transform infrared spectroscopy and SDS-PAGE showed that CBZ-QG-mPEG was successfully synthesized and can be recognized by mTG as an acyl donor to modify therapeutic protein, cytochrome c (cyt c ). Finally, under an optimized condition (cyt c 0.5 mg/ml, CBZ-QG-mPEG 11.25 mg/ml, mTG 0.5 mg/ml, 37 °C, 2 h), the PEGylation yield reached 76.5 %. Conclusions This is the first study regarding the PEGylation of protein at the level of Lys residues catalyzed by mTG. The novel method could be employed to immobilize active proteins and modify therapeutic proteins.

CAS / MDL: 6066-82-6
研究领域: 生物化学 · 蛋白质工程 · 药学
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JOURNAL OF HAZARDOUS MATERIALS · 2021 · IF 10.588

Carbamazepine removal by the synergistic effect of manganese-oxidizing microalgae and biogenic manganese oxides

Quanfeng Wang,Haoxuan Wei,Wenbo Liu,Jun Zhai

Forty strains of Mn-oxidizing microalgae (MnOMs) with different Mn 2+ oxidation mechanisms were identified from two aquatic environments. Among them, three strains of isolates ( Chlamydomonas sp. WH1–1, Chlamydomonas sp. WH1–4 , and Chlorella sp. WH2–5) oxidize Mn 2+ by increasing the ambient pH and by secreting Mn oxidation factors (e.g., superoxide-production enzymes and/or other Mn oxidases) into the extracellular environment at the same time. In carbamazepine (CBZ) removal by MnOMs and/or Bio-MnOx, the combination of MnOMs and Bio-MnOx significantly increased the CBZ (1 mg/L) removal efficiency from 36.05% (by MnOMs alone) and 20.11% (by Bio-MnOx alone) to 80.13% by two synergistic mechanisms. One of the synergistic mechanisms was confirmed as that the Mn 2+ was re-oxidized by MnOMs to Bio-MnOx, which can promote the CBZ removal, and another was the mutual exchange of degradation products of CBZ as shared reactants between MnOMs and Bio-MnOx. The degradation intermediates of CBZ were analyzed using high-performance liquid chromatography-tandem mass spectrometry , based on which the CBZ degradation pathway by MnOMs and Bio-MnOx was proposed. These findings expand existing knowledge on the Mn 2+ oxidation mechanisms of MnOMs, and indicate that MnOMs and their generated Bio-MnOx are promising for the removal of CBZ or other pharmaceutical contaminants from wastewater.

CAS / MDL: 75-05-8 64-19-7 67-56-1
研究领域: 环境科学 · 微生物学 · 制药工程 · 分析化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Coupled radical and nonradical activation of peroxymonosulfate by the piezo-photocatalytic effect of α-SnWO4/ZnO heterojunction to boost the degradation and detoxification of carbamazepine

Xiaoyue Zhou,Yunying Liu,Yingqi Miao,Wenwen He,Yanan Pan,Adela Jing Li,Junhao Qin,Huashou Li,Renli Yin,Rongliang Qiu

Piezo-photocatalytic processes based on heterogeneous catalysts, by establishing electronic fast track to realize electronic storage and conversion, are proved to be effective ways to improve the efficiency of PMS activation. Herein, α-SnWO 4 /ZnO catalyst with p-n heterojunction was constructed to testify the piezo-photocatalytic effect on peroxymonosulfate (PMS) activation for pollution control. The decomposition rate of carbamazepine (CBZ) in the piezo-photocatalytic PMS activation process by α-SnWO 4 /ZnO heterojunction was 12.6 and 5.2 times to that by ZnO and α-SnWO 4 processes, respectively. In addition, the total organic carbon (TOC) removal rate of CBZ reached 89%, and TOC in the actual water body was also effectively removed. Free radical quenching and detection experiments showed that nonradicals ( 1 O 2 ) and free radicals (O 2 − , OH) were the mainly active species of the process, by which the toxicity of the intermediates of CBZ was significantly reduced by the combination of the radical and nonradical pathways through hydroxylation and singlet oxygen oxidation . Furthermore, the influences of the experimental factors, including the initial pH, PMS concentration, temperature and reuse of catalysts on CBZ degradation were evaluated. Notably, the activation energy (Ea) in this work was calculated as 34.2 kJ mol −1 , which was lower than that of other reported systems. Overall, this work can scientifically guide the design of high-performance piezo-photocatalysts to use common metals for efficient activation of PMS as economical alternatives over expensive rare metal catalysts for water purification.

研究领域: 环境科学 · 催化 · 水处理
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APPLIED CATALYSIS A-GENERAL · 2022 · IF 5.723

Dual-functional Mo2C quantum dots enriched N-doped graphitic carbon layers in advanced oxidation processes (AOPs)

Chencheng Dong,Yan Bao,Mingyang Xing,Masakazu Anpo,Jinlong Zhang

Advanced oxidation processes (AOPs) are reckoned effective for removing persistent and recalcitrant pollutants by reactive oxygen species (ROSs), including hydroxyl radicals (•OH), sulfate radicals (SO 4 • - ), and superoxide radicals (•O 2 - ), as well as singlet oxygen ( 1 O 2 ). In this work, the Mo 2 C quantum dots enriched N-doped graphitic carbon layers (Mo 2 C QDs/NGCLs) were constructed via a facile two-step methodology. Interestingly, the Mo 2 C QDs/NGCLs acted as a highly efficient cocatalyst and/or catalyst simultaneously in AOPs, in particular visible-light-driven (VLD) Fenton and VLD PMS activation. In the hydroxyl radical-based AOPs (•OH-AOPs), it exhibited a remarkable removal efficiency for a range of aromatic organic pollutants , including rhodamine B (RhB) (99.9 %), phenol (90 %), benzophenone-3 (BZP) (83 %), methyl orange (MO) (58 %), methyl blue (MB) (89 %), ibuprofen (IBU) (100 %), and carbamazepine (CBZ) (50 %). Sulfate radicals-based AOPs (SR-AOPs) effectively degrade RhB (72 %), MO (83 %), IBU (70 %), and BZP (100 %). Thus, the present findings confirmed the potential of transition metal carbides for AOP applications and established a solid theoretical and technical basis for further research.

研究领域: 环境科学 · 材料科学 · 化学工程 · 水处理
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