MACROMOLECULES
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2023
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IF 5.5
Yujie Lei,Xingyu Ma,Jieyao Wang,Bo Lin,Wangzhi Chen,Lei Li
Due to the characteristics of step polymerization, high monomer conversion and polymerization degree cannot be achieved simultaneously for polyimides. In our recent report, naphthalene-based microporous polyimides (MPIs) have been successfully prepared in 30 min with superior surface area and yield to their documented counterparts, benefiting from the improved solvothermal method developed by our group [Zhu et al. Green Chem. 2020, 22, 7003]. Inspired by the factor-optimizing protocol, we realize that some neglected polymerization parameters probably have a significant influence on the seemingly simple polymerization process. In this article, the detailed investigation indicates that either increasing the reaction temperature or decreasing the monomer content can effectively prohibit the early desolvation and phase separation during polymerization, resulting in the formation of long-range interpenetrating polymer networks. Eventually, five families of MPIs, totaling 15 samples, with high surface area were produced with the aid of the optimized polymerization parameters in 1.5 h, starting from commercially available dianhydride (or tetracid) and triamine monomers. Particularly, the maximum surface area of perylene-based MPIs achieves 447 m2 g–1. They can work as photocatalysts to produce H2O2 with a rate of 2195 and 2240 μmol g–1 h–1 under visible light (>420 nm) and simulated sunlight irradiation, respectively.
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Journal of Water Process Engineering
·
2023
·
IF 7
Yuyue Huang,Qingjie Xie,Huijuan Wang,Muhammad Imran Nawaz,Huihui Zhang,Shilin Song,Kun Hu,Qiangshun Wu
Trimethoprim (TMP), a kind of emerging pollutant, has attracted considerable attention. To achieve an effective degradation of the TMP, a simulated solar light/periodate (SSL/PI) system was set up by using the Xe lamp as the SSL source. The critical parameters affecting the degradation, including the PI content, the TMP concentration as well as the initial pH, were analyzed. The obtained results show that the TMP removal could reach 92 % after 50 min of treatment under the condition of 4 mM PI addition while lower TMP concentrations showed higher degradation percentages. The efficient TMP degradation in the SSL/PI system was achieved in a wide range of the solution pH. The quenching test proved that IO 3 , IO 4 , 1 O 2 , OH, and O 2 − were critical reactive species for the TMP degradation in the SSL/PI system and the electron spin resonance analysis proved the generation of 1 O 2 and OH. Three possible pathways of the TMP degradation were proposed according to the LC-MS detection and Pathway II might be the specific one according to the density functional theory (DFT) calculation. Toxicity evaluation showed that the toxicity of the initial TMP solution reduced after the treatment, which confirmed the effectiveness of the PI activation by the SSL.
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Advanced Therapeutics
·
2023
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IF 4.6
Tianliang Li,Lixing Lin,Dong Wang,Haowen Fang,Zhiwei Zhang,Yitong Wang,Yingying Chen,Lingyan Feng
The increasing bacterial resistance highlights the necessity of developing superior antibacterial materials. Metal-doped carbon dots (CDs), a crucial branch of carbon-based nanozymes, exhibit efficient antibacterial properties using the reactive oxygen species (ROS) effect. In this study, iron-doped carbon dots (Fe-CDs) are synthesized with high peroxidase-like (POD-like) activity using natural hemin as a precursor for the first time. The formation of Fe-CDs remarkably improves the water solubility of hemin showing excellent biocompatibility. Additionally, iron is doped from hemin to the CDs surface, reducing the risk of trial-and-error associated with adding an external iron source. The Fe-CDs-hydrogel system is constructed via the incorporation of Fe-CDs into a dual-crosslinked injectable hydrogel, taking advantage of the synergistic effects. The system enhances the mechanical properties of hydrogel and serves as an excellent carrier for Fe-CDs. It exhibits effective antibacterial activity at low hydrogen peroxide (H 2 O 2 ) concentrations (10 −4 m ) via the activation of Fenton-like reaction-triggered POD-like catalytic activity and the electrostatic interactions. The system further demonstrates excellent healing efficacy in a bacteria-infected wound model by reducing inflammation levels and accelerating the regeneration of tissues. This study provides a novel approach for applying nanozymes in antibacterial therapy and wound healing.
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Analytical Methods
·
2023
·Vol. 16
·期 5
·731-741
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IF 3.1
Liyuan Yu,Mengxiao Lv,Ting Zhang,Qixin Zhou,Juanhua Zhang,Xuexiang Weng,Yongming Ruan,Jiuju Feng
Herein, we present a simple and mild method to in situ prepare CuO nanostructures for non-enzymatic glucose sensing. A Cu-metal organic framework (Cu-MOF) precursor was first directly grown on a pencil lead electrode with 3D graphene-like surfaces (EPLE) and then in situ transformed into CuO nanorods. The CuO nanorod-modified EPLE (CuO/EPLE) shows high sensitivity (1138.32 μA mM−1 cm−2), fast response time (1.5 s) and low detection limit (0.11 μM) for glucose oxidation. It has been found that NaOH promoted the generation of ˙OH groups and Cu(III) on the CuO surface, which then facilitated the electrochemical oxidation of glucose. Signals characteristic of hydroxyl and carbon-centered radical adducts were detected by EPR. Furthermore, the CuO/EPLE sensor also shows good accuracy in glucose determination in human serum samples.
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JOURNAL OF INORGANIC BIOCHEMISTRY
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2021
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IF 4.155
Rui-Xue Liu,Ru-Yi Luo,Meng-Ting Tang,Yan-Cheng Liu,Zhen-Feng Chen,Hong Liang
Based on the anticancer pharmacophore of anthrahydrazone and quinoline, a new quinolylanthrahydrazone ligand, 9-AQH (anthracene-9-quinolylhydrazone), was synthesized to further afford four metal complexes, [Co II (9-AQH)(NO 3 ) 2 (H 2 O)] ( 1 ), [Ni II (9-AQH) 2 (H 2 O) 2 ]·2NO 3 ( 2 ), [Cu I (9-AQH) 2 ]·NO 3 ( 3 ), [Zn II (9-AQH) 2 (NO 3 )]·NO 3 ( 4 ), determined by X-ray single crystal diffraction analysis. The reaction of Cu(NO 3 ) 2 with 9-AQH formed the stable and repeatable copper(I) complex 3 . In vitro screening demonstrated only 3 showed significant and broad-spectrum anticancer activity , indicating that Cu(I) played a key role in exerting the anticancer activity. In solution, Cu(I) was not naturally oxidized to Cu(II) suggested by 1 H-NMR (Nuclear Magnetic Resonance) and EPR (Electron Paramagnetic Resonance) analysis. The presence of 3 could also catalyze the H 2 O 2 system to give hydroxyl free radicals , suggested by further EPR and electrophoresis assay. At the cellular level, although no obvious Cu(II) signals were detected and the total ROS (Reactive Oxygen Species) scavenging in the tumor cells treated with 3 , the potential redox property between Cu(I)/Cu(II), as a key role, should not be denied for the significant anticancer activity of 3 , considering the much complicated circumstance and other reductive substances in cells. The anticancer mechanism of 3 on the most sensitive MGC-803 cells pointed to significant cell apoptosis through mitochondrial pathway, rather than cell cycle arrest . While the autophagy observed in tumor cells treated by 3 suggested its complicated anticancer mechanism, and whether there was an intrinsic correlation still needed to be further investigated.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Jie Yao,Yan Zhang,Zekun Dong
Electrochemically activated persulfate is an emerging advanced oxidation process for the removal of contaminants of emerging concern (CECs). The degradation of CECs, including carbamazepine (CBZ), bisphenol S (BPS), propranolol (PPL) and sulfamethoxazole (SMX) using electrochemically activated peroxymonosulfate (EA-PMS) was systematically investigated in this work. Over 80% of all the forementioned CECs were removed within 30 min. It exhibited a good synergistic effect between PMS and electrolysis on the degradation of CECs. The results of linear sweep voltammetry (LSV) indicated that a transition structure between BDD anode and PMS (BDD (PMS)*) was likely responsible for the synergistic effect. Hydroxyl radical (HO·) and sulfate radical (SO 4 · − ) were proved to be the primary reactive species, of which HO· played the leading role. The increase of current density and PMS dosage accelerated the degradation of SMX, while initial pH from 3.0 to 11.0 had a limited effect on the degradation of SMX. Moreover, the influences of common ions and natural organic matter (NOM) on the degradation of SMX were comprehensively assessed using response surface methodology (RSM), and a prediction model was built via RSM. The performance of EA-PMS on the degradation of SMX in actual water was even better than that in pure water in this study. EA-PMS can serve as a novel and promising technology for the degradation of CECs and has great potential in practical application.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 11
·7198-7207
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IF 12.732
Xiaoyong Yu,Lijing Wang,Xin Wang,Hongzhi Liu,Ziyuan Wang,Yixuan Huang,Guoqiang Shan,Weichao Wang,Lingyan Zhu
Supported metal catalysts are widely used for heterogeneous catalytic processes (e.g., Fenton-like reaction), but the mechanisms of interfacial processes are still ambiguous. Herein, unique nanocarbon based catalysts with Co nanoparticles encapsulated in nitrogen (N)-doped graphene (Co@NG) were prepared by calcination of Co based metal–organic frameworks (MOFs), which showed excellent catalytic performance for peroxymonosulfate (PMS) activation. Comprehensive characterization revealed that there were strong interfacial interactions between Co and the NG layer due to the presence of special nitrogen species, especially graphitic-N. Density functional theory calculations suggested that the strong interfacial interactions provided optimal active sites with low adsorption energy (−1.99 eV) for PMS accumulation, which enabled the generation of highly oxidizing NG–PMS* intermediates as evidenced by in situ Raman microscopy. Electrochemical analyses revealed that the interfacial interactions facilitated surface-to-surface electronic communication across atomic interface-bonding (N–Co). Consequently, phenol was quickly degraded by the NG–PMS* via direct oxidation by an anodic-like nonradical process, and reasonable graphitic-N (G-N) content and pore size are important for this process. Phenol at 1 mM was completely removed within only 12 min by Co@NG-900 (which was prepared at 900 °C), with an apparent rate constant 20 times higher than that of pure NG-900. This work sheds new insights on the critical role of interfacial interactions in nonradical PMS activation.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Junjie You,Chengyang Zhang,Zelin Wu,Zhimin Ao,Weiyi Sun,Zhaokun Xiong,Shijun Su,Gang Yao,Bo Lai
In this paper, a type of Ni metal and Ni 3 ZnC 0.7 alloy nanoparticle catalyst encapsulated in N-doped graphite (NiZn@N-G-900), obtained by derivatization of metal–organic frameworks (MOF), was applied to activate peroxymonosulfate (PMS) to degrade Bisphenol A (BPA) in water. Characterizations and DFT calculations demonstrated that the encapsulation of graphite layer or N-doped graphite layer can not only adjust the surface charge distribution of the catalysts, but also improve the charge transfer ability between the catalyst and the adsorbate. These modifications were beneficial for the adsorption and activation of PMS. Based on the results of the modified radicals scavenging experiments and EPR, a typical 1 O 2 dominated non-radical system was proposed. Due to the characteristics of 1 O 2 , the NiZn@N-G-900/PMS system had strong inorganic anion resistance, high selectivity and satisfactory practical application. Moreover, two pathways of BPA degradation were put forward.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Quanhao Shen,Lingfei Wei,Rehana Bibi,Ke Wang,Dandan Hao,Jiancheng Zhou,Naixu Li
Graphitic carbon nitride is considered as one of the promising photocatalysts for pollution elimination from wastewater. Manipulating the microstructure of carbon nitride remains a challengeable task, which is essential for improving light absorption , separating photogenerated carrier and creating reactive sites. Herein, a carbon vacancy modified hierarchical carbon nitride microrod (CN1.5) has been prepared templated from a melamine-NH 2 OH·HCl complex. The hierarchical microrods are demonstrated to be comprised of interconnected nanosheets with rich carbon vacancies, which endows it with high specific surface area, enhanced light utilization efficiency, available reactive sites, improved charge carrier separation and numerous mass-transport channels. The resultant photocatalyst CN1.5 exhibits an excellent photodegradation efficiency of 87.9% towards tetracycline under visible light irradiation. The remarkable apparent rate constant of 4.91 × 10 −2 min −1 is 7.3 times higher than that of bulk CN. In addition, the degradation pathways are deduced base on the observation of degradation intermediates generating in the photocatalytic process. Mechanism investigation indicates that the major contribution for photodegradation is attributed to ·O 2 – , 1 O 2 and H 2 O 2 species. This work provides new insights into advancing carbon nitride's microstructure to improve photocatalytic degradation performance for highly efficient antibiotic removal and environment remediation.
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Journal of Water Process Engineering
·
2021
·
IF 5.485
Jialin Chen,Ruina Zhang,Dong Chen,Jianyong Liu,Shanping Chen
The generation process for the highly reductive carbon dioxide radical ( CO 2 − ) in the Fe(III)-oxalate system is enhanced under UV irradiation and used in nitrate (NO 3 − ) reduction with improved product selectivity to nitrogen (N 2 ). The combination of Fe(III) and residual oxalate forms Fe(III)-oxalate complexes again for an Fe(II)/Fe(III) species cycle and achieves generation of CO 2 − radical continually. The electron paramagnetic resonance (EPR) spectrum demonstrates the existence of CO 2 − radicals in this process. Some of the important control factors, such as initial concentrations of ferric ions (Fe(III)) (0.5, 1, 2, and 3 mM), NO 3 − (14, 21, and 42 mg N/L), oxalate (3, 7, and 10 mM), and pH values (2, 3, 4, 5, and 6), are systematically assessed for NO 3 − reduction efficiency and N-species selectivity. Among all the control factors mentioned, pH is a key parameter with an important role in the NO 3 − reduction process. Excellent NO 3 − reduction efficiency (∼90 %) was achieved at pH 3 in the presence of 1 mM Fe(III) and 10 mM oxalate under UV irradiation for 120 min. High Fe(III) and oxalate concentrations promote NO 3 − removal. In addition, there was an increase in the NO 3 − removal amount with a greater initial NO 3 − concentration. About 60 % of NO 3 − can be selectively reduced to N 2 with low selectivity to NO 2 − (∼3.4 % of total N) and NH 4 + (∼15.7 % of total N). In general, the UV/Fe(III)-oxalate system provided an alternative way to improve NO 3 − removal performance and selectivity to form N 2 in water and wastewater remediation processes.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Lijun Zou,Xin Xiao,Chiheng Chu,Baoliang Chen
A novel hierarchically porous CoFe 2 O 4 /reduced graphene oxide (rGO) aerogel (CFGA) was synthesized via a facile one-pot hydrothermal method and assessed in activating peroxymonosulfate (PMS) for the removal of organic pollutants. CoFe 2 O 4 nanoparticles were uniformly distributed onto the surface of rGO aerogels, with rGO aerogel support maintaining the three-dimensional (3D) interconnected porous framework. Efficient activation of PMS and rapid removal of phenol were achieved using CFGA , ascribed to the large surface area and 3D porous framework of rGO aerogel that promoted mass transfer and the dispersion of CoFe 2 O 4 nanoparticles catalytic sites. The great PMS-activation performance of CFGA was further demonstrated for the rapid removal of phenol under a broad pH range and in the presence of chloride or humic acid . Besides, the rapid removal of multiple organic pollutants was achieved in CFGA/PMS system. Mechanistic investigations suggest that PMS-activation by CFGA mainly follows a radical pathway. X-ray photoelectron spectroscopy analysis revealed that Co atom was involved in the PMS-activation process. Given the facile synthesis method and promising PMS-activation activity, CFGA represents a critical advance in the development of Fenton-like catalysts for pollutant removal .
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Feng Cheng,Peng Zhou,Xiaowei Huo,Yang Liu,Yongli Zhang
In this study, Fenton-like chain reaction is constructed by coupling nanoscale tungsten powders (nW 0 ) and peroxydisulfate (PDS). The nanoscale tungsten powders/peroxydisulfate (nW 0 /PDS) system exhibits a high oxidation efficiency toward diverse pollutants and expands the effective pH range up to 9.8. Results reveal • OH and sulfate radical (SO 4 •− ) were confirmed to be responsible for 4,4′-ethylidenebisphenol (EBP) degradation, especially • OH. The corrosion process of nW 0 results in the in-situ production of H 2 O 2 and the transient-state tungsten species (W (x, x < VI)), initiating the reaction of H 2 O 2 and tungsten species to generate • OH. PDS can accelerate nW 0 corrosion to enhance the Fenton-like reaction, and can be activated by tungsten species (nW 0 and W (x, x < VI)) to produce • OH and SO 4 •− . Integrated the analysis results of LC-QTOF-MS/MS, EBP degradation pathways were proposed. This study reveals the high oxidation efficiency over a wide pH range in the nW 0 /PDS system and provides new insight into the tungsten species induced Fenton-like reaction.
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