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Journal of Water Process Engineering · 2024 · IF 6.3

The MOF-on-MOF hybrids of MIL-101(Fe)@CoZn-ZIFs as efficient catalyst for the removal of deys from wastewater

Mei Dong,Kuilong Liu,Guoqiang Song,Guiping Ma

In this study, MOF-on-MOF hybrids were successfully synthesized by interfacial growth method using CoZn-ZIF as guest MOF and MIL-101(Fe) as host MOF, and then employed as heterogeneous catalysts to activate peroxymonosulfate (PMS) in the degradation of dyes. The hybrids exhibited different morphologies depending on the Co/Zn ratios (10/0, 10/2, 10/10, and 2/10), all of which displayed exceptional catalytic performance. Notably, the hybrid with a Co/Zn ratio of 10/2 showed the highest degradation rate of MB, reaching 100 % removal within 3 min with a k obs value of 452.75 Lg −1  min −1 based on the pseudo-second-order kinetic model. Through EPR characterization and scavenging experiments, it was determined that the degradation of dyes occurred through a combination of radical (SO 4 •-, •OH)and non-radical ( 1 O 2 ) pathways, with 1 O 2 and SO 4 •- playing prominent roles. Various factors such as Co/Zn ratio, catalyst dosage, PMS concentration, initial pH, temperature, and MB solution concentration were systematically investigated to understand their influence on the catalytic performance. Furthermore, the influence of inorganic ions, humic acid (HA), and the reusability and stability of the catalyst was evaluated, demonstrating its potential for practical applications. Overall, this research provides valuable insights into the design and application of MOF-based catalysts for environmental remediation processes.

研究领域: 环境科学 · 催化 · 材料科学 · 化学工程
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Journal of Chemistry · 2019 · IF 1.727

Oxidative Degradation of Amoxicillin in Aqueous Solution by Thermally Activated Persulfate

Juanjuan Zhao,Yujiao Sun,Fachao Wu,Minjian Shi,Xurui Liu

Antibiotic residues and antibiotic resistance genes (ARGs) pose a great threat to public health and food security via the horizontal transfer in the food production chain. Oxidative degradation of amoxicillin (AMO) in aqueous solution by thermally activated persulfate (TAP) was investigated. The AMO degradation followed a pseudo-first-order kinetic model at all tested conditions. The pseudo-first-order rate constants of AMO degradation well-fitted the Arrhenius equation when the reaction temperature ranged from 35°C to 60°C, with the apparent activate energy of 126.9 kJ·mol−1. High reaction temperature, high initial persulfate concentration, low pH, high Cl− concentration, and humic acid (HA) concentration increased the AMO degradation efficiency. The EPR test demonstrated that both ·OH and SO4·− were generated in the TAP system, and the radical scavenging test identified that the predominant reactive radical species were SO4·− in aqueous solution without adjusting the solution pH. In groundwater and drinking water, AMO degradation suggested that TAP could be a reliable technology for water remediation contaminated by AMO in practice.

研究领域: 环境科学 · 化学工程 · 水处理
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International Journal of Electrochemical Science · 2023 · IF 1.5

Enhanced degradation of quinoline in three-dimensional electro-Fenton system using catalytic Fe-Co-Ni-P/g-C3N4 particles

Jun Chen,Boding Zhang,Bingxing Wang,Chengxing Cui,Songlin Wang,Jichao Wang,Wenlong Zhang

With high toxicity, carcinogenicity and teratogenicity, quinoline has been threatening human health and ecological environment. Herein, Fe-Co-Ni-P/g-C 3 N 4 particles are developed as electrochemical reactors to form a three-dimensional catalytic particle electrode system (3D-CPE) for efficient removal of quinoline from wastewater by electro-Fenton (EF) oxidation process. with reaction time of 30 min, the particles dosage of 50 g/L, pH of 3, conductivity of 11.5 ms/cm, and current density of 37.04 mA/cm 2 , the chemical oxygen demand (COD) removal rate can up to 90.95%. In addition, electron paramagnetic response (EPR) and radical scavenging tests are performed to determine the hydroxyl radicals of electrochemical processes produced. The degradation products are analyzed by high performance liquid chromatography-mass spectrometry (HPLC-MS). Finally, through theoretical calculation and analysis of degradation products, a reasonable degradation mechanism is proposed.

研究领域: 环境科学 · 化学工程 · 水处理 · 电化学
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Nanoscale · 2015 ·Vol. 8 ·期 1 ·104-116 · IF 7.394

pH-Sensitive self-assembling nanoparticles for tumor near-infrared fluorescence imaging and chemo–photodynamic combination therapy

Wenxiu Hou,Xin Zhao,Xiaoqing Qian,Fei Pan,Chunlei Zhang,Yuming Yang,Jesús Martínez de la Fuente,Daxiang Cui

The development of visual tumor theranostic nanoparticles has become a great challenge. In this study, D-α-tocopheryl polyethylene glycol 1000 succinate (TPGS) was conjugated to acid-sensitive cis-aconitic anhydride-modified doxorubicin (CAD) to obtain pH-sensitive anti-tumor prodrug nanoparticles (TCAD NPs) via self-assembling. Subsequently, the photosensitizer chlorin e6 (Ce6) was loaded into the resulting prodrug nanoparticles to prepare a novel tumor near-infrared fluorescence imaging and chemo–photodynamic combination therapy system (TCAD@Ce6 NPs). An accelerated release of doxorubicin (DOX) and chlorin e6 (Ce6) from the TCAD@Ce6 NPs could be achieved due to the hydrolysis of the acid-sensitive amide linker under mild acidic conditions (pH = 5.5). An in vitro experiment showed that A549 lung cancer cells exhibited a significantly higher uptake of DOX and Ce6 by using our delivery system than the free form of DOX and Ce6. An in vivo experiment showed that TCAD@Ce6 NPs displayed better tumor targeting gathering through the enhanced permeability and retention (EPR) effect than free Ce6, thus improving fluorescence imaging. Moreover, the chemo–photodynamic combination therapy of TCAD@Ce6 NPs combined with near-infrared laser irradiation was confirmed to be capable of inducing high apoptosis and necrosis of tumor cells (A549) in vitro and to display a significantly higher tumor growth suppression in the A549 lung cancer-bearing mice model. Furthermore, compared with exclusive chemotreatment (DOX) or photodynamic treatment (Ce6), our system showed enhanced therapeutic effects both in vitro and in vivo. In conclusion, the high performance TCAD@Ce6 NPs can be used as a promising NIR fluorescence imaging and highly effective chemo–photodynamic system for theranostics of lung cancer, etc. in the near future.

研究领域: 纳米技术 · 癌症治疗 · 生物医学工程 · 药学 · 分子生物学
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Tumor-targeted supramolecular catalytic nanoreactor for synergistic chemo/chemodynamic therapy via oxidative stress amplification and cascaded Fenton reaction

Xiaoyu Xu,Zishan Zeng,Jie Chen,Binyao Huang,Zilin Guan,Yanjuan Huang,Zeqian Huang,Chunshun Zhao

Utilizing intratumoral iron mediated Fenton reaction to induce cancer cells destruction, chemodynamic therapy (CDT) is an emerging tumor-specific therapeutic strategy. However, the CDT efficacy is severely restrained by insufficient endogenous H 2 O 2 and catalytic ferrous ions in tumor site. Herein, based on innovative small molecule prodrug design concept, an acid-labile ferrocene-modified cinnamaldehyde prodrug (Fc-CA) was first synthesized. Skillfully combining ROS-generator CA with Fenton catalyst Fc in its molecular structure, Fc-CA could synchronously elevate H 2 O 2 level and catalytic iron amount for enhanced CDT efficacy. Then, hydrophobic Fc-CA was efficiently encapsulated into hydrophilic cyclodextrin-modified hyaluronic acid conjugate (HA-CD) via host-guest interactions, to spontaneously form pH/redox dual-responsive supramolecular catalytic nanoreactor (HA-CD/Fc-CA NPs). The nanoreactor with high drug loading and stability, excellent catalytic activity and tumor specificity could preferentially accumulate in tumor tissues via EPR effect and CD44 receptor-mediated internalization. Through the cleavage of acid-labile hydrazone bond under acidic lysosome environments, the nanoreactor would be dissociated and release pre-protected CA for reinforced oxidation therapy and amplified H 2 O 2 level, which would in turn react with Fc through cascaded Fenton reaction, to generate highly cytotoxic •OH for enhanced cancer killing in a positive feedback process. Both in vitro and in vivo results verified excellent cascade-amplifying therapeutic performance and favorable biocompatibility of this nanoreactor. This study provides an innovative strategy for exploiting versatile organic therapeutic nanoplatforms, simultaneously activating tumor-specific oxidative stress amplification and cascaded enhanced Fenton reaction for superior cancer therapy with excellent biosafety.

研究领域: 纳米技术 · 癌症治疗 · 化学生物学 · 材料科学 · 药学
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OPTICAL MATERIALS · 2022 · IF 3.754

Pd nanoparticle-modified TiO2-x composites as efficient visible-light active photocatalysts for tetracycline degradation and microbial disinfection

Jingtao Zhang,Mengwan Zhai,Xueying Wang,Shurui Liu,Lijuan Zhang,Xing Liu,Yao Geng,Xiaodong Sun,Bingkun Liu

In the present work, Ti 3+ -self-doped TiO 2 heterostructure photocatalysts were prepared by coupling with different additions of palladium quantum dots by means of deposition-reduction methodology. The electron paramagnetic resonance (EPR) analysis indicated the existence of Ti 3+ in synthesized samples. The transmission electron microscopy (TEM) images presented the modification of TiO 2-x nanoparticles by coupling with nano palladium. Photoluminescence (PL) results demonstrated the lowest charge carrier recombination rate in 5% Pd/TiO 2-x composites. Photocatalytic performances of photocatalysts were evaluated by degrading Tetracycline (TC) and inactivating Escherichia coli ( E. coli ) and Fusarium oxysporum f. sp. Vasinfectum ( Fov ) with the presence of visible light , in which an enhanced photocatalytic degradation and inactivation activity was found in all Pd coupled composites with the highest efficiency in 5% Pd/TiO 2-x . The improved photocatalytic activity of Pd/TiO 2-x was associated to the generation of more hydroxyl radicals (•OH) and superoxide anions radicals (•O 2- ) during photocatalytic process which were demonstrated by the electron spin-resonance spectroscopy (ESR) technique. Moreover, 5% Pd/TiO 2-x composites were found to remain high photocatalytic properties in a circulating photo-disinfection system.

研究领域: 材料科学 · 环境科学 · 纳米技术 · 光催化 · 水处理
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PROGRESS IN ORGANIC COATINGS · 2024 · IF 6.5

Photopolymerization initiated by p-diethylene glycol monomethyl ether cinnamyl formamide-based disulfide under 455 nm LED with minimized volume shrinkage

Yuhan Zhang,Nan Xiao,Yanjing Gao,Fang Sun

This study introduces a novel p -diethylene glycol monomethyl ether cinnamyl formamide-based disulfide monomer , N,N′ -(disulfanediylbis(2,1-phenylene)) bis(4-(4-(2-(2-methoxyethoxy)ethoxy) phenyl)-2-oxobut-3-enamide) (Mp-BSCF), designed to reduce the volume shrinkage of photosensitive resins and initiate monomer polymerization under 455 nm LED light irradiation. The photochemical properties and photoinitiation efficiency of Mp-BSCF are systematically investigated using UV–vis absorption spectroscopy , electron paramagnetic resonance (EPR) and real-time infrared spectroscopy . Although its weak absorption around 455 nm, Mp-BSCF can generate arylthiyl radicals under 455 nm LED irradiation, and then effectively initiate the polymerization of triethylene glycol dimethacrylate (TEGDMA)/A glycerolate dimethacrylate (Bis-GMA) system. Increasing Mp-BSCF addition enhances the final double bond conversion and maximum polymerization rate of the TEGDMA/Bis-GMA system, reaching up to 82.0 % and 2.02 % s −1 , respectively. Notably, Mp-BSCF significantly reduces the volume shrinkage of the photopolymerization system, with the addition of 10 % Mp-BSCF resulting in a 50 % reduction compared to the control system. This reduction is attributed to the dynamic reversible nature of the S S bond “breaking-recovery” and the intermolecular hydrogen bond interaction. Additionally, Mp-BSCF improves the thermal stability, friction resistance, and hardness of the TEGDMA/Bis-GMA photopolymerization system.

研究领域: 材料科学 · 高分子化学 · 光化学
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Journal of Cleaner Production · 2023 · IF 11.1

Research on the reaction path of chlorobenzene oxidation by electrochemical-sodium persulfate system

Shicheng Yuan,Hui Hu,Hao Huang,Zhongming Chen,Jiaxin Chen,Mi Zhang,Kunpeng Li,Ting Zhou,Ruibin Lv

Chlorobenzene (CB) is an important organic chemical material that is volatile and difficult to degrade, and has received much attention because of its strong ozone generation potential. An electrochemical-sodium peroxydisulfate (PDS) system was constructed and the oxidation reaction path of chlorobenzene in this system was analyzed. The effects of current density, PDS concentration, initial pH, CB blow-off gas ratio and temperature on the oxidation and mineralization rate of chlorobenzene in the system were investigated respectively. At a current density of 168 A/m 2 , a PDS concentration of 0.5 mol/L, an initial pH of 10, a CB blow-off gas ratio of 20% and a reaction temperature of 60 °C, the CB conversion and mineralization rates were able to reach more than 90%. The results of electron paramagnetic resonance (EPR) experiments using 5,5-dimethyl-1-pyrroline N-oxide (DMPO) and 2,2,6,6-tetramethyl-4-piperidone hydrochloride (TEMP) as spin trapping agents indicate the presence of ⦁OH, · S O 4 − and 1 O 2 in the system. The signal of · O 2 − was also captured after the quenching of ⦁OH, which further indicates the presence of 1 O 2 . And the results of active substance quenching experiments showed that the active species that mainly contributed to the oxidation of chlorobenzene included ⦁OH, · S O 4 − and 1 O 2 , and their contributions to the oxidation of chlorobenzene were 25.0%, 31.7% and 22.2%, respectively. The Liquid Chromatograph Mass Spectrometer (LC-MS) characterization results showed that the formation of chlorophenol and hydroquinone and their ring-opening reactions were the most critical processes in the oxidative decomposition of chlorobenzene, and the reaction pathways for the oxidation of chlorobenzene by ⦁OH, · S O 4 − and 1 O 2 were proposed by these characterization results.

CAS / MDL: 3317-61-1
研究领域: 环境科学 · 化工工程 · 分析化学
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