NANOTECHNOLOGY
·
2019
·Vol. 31
·期 1
·015101
·
IF 3.399
Keke Du,Qianqian Liu,Mei Liu,Rongmu Lv,Nongyue He,Zhifei Wang
Increasing the content of reactive oxygen species (ROS) with the assistance of nanoformulations in cancer cells via the Fenton reaction is considered an effective method to treat cancer. However, the efficiency of the Fenton reaction is affected by the level of H2O2, the selection of iron ions in different nanoformulations, etc. Herein, we use FeIII-tannic acid (FeIIITA) nanocomposites as the carrier to deliver glucose oxidase (GOD) which can solve the problem of insufficient endogenous H2O2 by catalytically converting the glucose. In comparison with traditional Fe2+/Fe3+, FeIIITA nanocomposites perform higher catalytic activity in converting H2O2 to high toxic hydroxyl radicals (·OH) due to the TA-mediated reduction of Fe3+. So, the integration of GOD and TA in the construction of nanocomposites significantly enhances the efficiency of the Fenton reaction. In vitro experiments show that ·OH produced by GOD-FeIIITA nanocomposites can not only achieve a good anticancer effect at a low concentration but also promote degradability of the nanocomposites. When it is only 1.08 μg · ml−1, the cell apoptosis rate has reached 76.91%. In vivo experiments further demonstrate that GOD-FeIIITA nanocomposites can significantly inhibit tumor growth. So this work lays a good foundation for Fenton reaction-based cancer treatment.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jiahang Liu,Xiaoyang Li,Yingying Chu,Ling Yuan,Ruolin Lv,Weiming Zhang
The conventional Fe(III)/H 2 O 2 system is of low efficiency on the removal of most organic pollutants. However, we discovered that the Fe(III)/H 2 O 2 system was robust on remediating tetracycline (TC) in water (0.109 min −1 for the pseudo-first kinetic constant), and the reaction was even slightly faster than that in the conventional Fe(II)/H 2 O 2 system (0.105 min −1 ). The addition of TC could also initiate the degradation of other refractory pollutants in the Fe(III)/H 2 O 2 system. Complexation between Fe(III) and TC with the stoichiometric ratio of 1:1 was observed. Electron transfer from TC to Fe(III) gave rise to the slight production of Fe(II), which served as the initiator of the following Fenton reaction. •OH was ascertained as the main reactive species through quenching experiments, EPR tests and the probe method, while O 2 • − /HO 2 • was also a subsidiary contributor. Hydroquinone intermediates were proved to be generated through the hydroxylation of the benzene ring of the TC molecule by •OH and thus facilitate the reductive transformation of Fe(III) to Fe(II). This study analyzes the relationship between molecular structural features of TC and the catalytic efficiency of ferric Fenton-like reactions. We expect to shed light on new mechanistic insights on autocatalysis in the Fenton-like catalytic processes.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 34
·期 2
·2308849
·
IF 19
Yashuai Pang,Minsen Xie,Xinghao Lu,Zhao Wan,Zhuohang Zhong,Waqas Muhammad,Xiang Long Huan,Yinghua Niu,Zhen Zhang,Weiqiang Lv
Lithium–sulfur (Li–S) batteries have attracted wide attention as high-energy-density energy storage devices, but their practical applications are hindered by the severe shuttle effect and sluggish kinetics of lithium polysulfides (LiPSs). To address these challenges, polar mediators are employed to chemisorb and catalyze LiPSs, but most of them suffer from low electronic conductivity and poor catalytic activity. Here, a novel strategy is reported to enhance both properties by dispersing Fe(III) atoms in VO 2 nanoribbons(Fe-VO 2 ), creating electronic metal-support interactions (EMSI) that modulate the electronic structure and charge transfer of VO 2 . Theoretical calculations reveal that EMSI lowers the energy barrier for the decomposition of Li 2 S from 1.60 to 1.32 eV and increases the electronic conductivity of VO 2 . Fe doping reduces the Li-ions diffusion barrier from 1.42 eV in VO 2 to 0.99 eV in Fe-VO 2 . The Fe-VO 2 catalyst shows strong adsorption and fast converstion of LiPSs, resulting in high energy density and long cycling life of Li-S batteries. The cathode with Fe-VO 2 maintains a higher capacity retention of 67% after 500 cycles at 1 C, compared with 52.4% and 53.6% for the carbon black based cathode and VO 2 based cathode, respectively. This work demonstrates the potential of EMSI for designing efficient catalysts for Li–S batteries and provides new insights into the electronic structure engineering of polar mediators.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Xinna Zhao,Guangbing Liang,Hui Wang,Zhenping Qu
Platinum (Pt) is a nonrenewable mineral with limited reserves and a patchy distribution. Pt demand and consumption are growing year after year. As a result, recovering Pt from the secondary resources is critical. A new strategy for effective Pt recovery employing Fe(III)-oxalate complexes under UV and visible light irradiation is proposed in this paper. This approach can recover 98.9% of Pt in 30 min under the conditions of 365 nm UV irradiation, leaching time = 30 min, C2O42– concentration = 333.33 g/L, and H2O2 addition = 0.60 vol %. More importantly, 95.6% of Pt can also be recovered in 8 h under sunlight. The homogeneous photocatalytic reaction is rapid and efficient, and meanwhile, no strong acid, base, or volatile toxic organic solvent is required. Additionally, the iron utilized in the process may be well-recycled, solving the problem of recovery difficulty of homogeneous photocatalysts and lowering the cost of leaching. Simultaneously, the Pt complex recovered from the waste catalyst is utilized in situ to manufacture 0.1 wt % Pt/ZSM-5 catalyst, which shows the complete conversion of toluene at 200 °C and can remain stable during the long duration reaction of 1200 min. Overall, it can not only provide a new environmentally friendly technique to recycle Pt from spent catalysts but also save manufacturing cost of new catalysts.
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MOLECULES
·
2023
·Vol. 28
·期 8
·3445
·
IF 4.6
Lei Zhang,Heng Liu,Jiaqi Zhu,Xueling Liu,Likun Li,Yanjun Huang,Benquan Fu,Guozhi Fan,Yi Wang
A novel pyridine-modified chitosan (PYCS) adsorbent was prepared in a multistep procedure including the successive grafting of 2-(chloromethyl) pyridine hydrochloride and crosslinking with glutaraldehyde. Then, the as-prepared materials were used as adsorbents for the removal of metal ions from acidic wastewater. Batch adsorption experiments were carried out to study the impact of various factors such as solution pH value, contact time, temperature, and Fe (III) concentration. The results showed that the absorbent exhibited a high capacity of Fe (III) and the maximum adsorption capacity was up to 66.20 mg/g under optimal experimental conditions (the adsorption time = 12 h, pH = 2.5, and T = 303 K). Adsorption kinetics and isotherm data were accurately described by the pseudo-second-order kinetic model and Sips model, respectively. Thermodynamic studies confirmed that the adsorption was a spontaneous endothermic process. Moreover, the adsorption mechanism was investigated using Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). The results revealed the pyridine group forms a stable chelate with iron (III) ions. Therefore, this acid-resistant adsorbent exhibited excellent adsorption performance for heavy metal ions from acidic wastewater compared to the conventional adsorbents, helping realize direct decontamination and secondary utilization.Keywords:acidic wastewater;heavy metal ions;pyridine-modified chitosan adsorbent;adsorption mechanism
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HYDROMETALLURGY
·
2019
·
IF 3.465
Guang-jin Zhu,Hai-yan Tang,Hong-ling Zhang,Li-li Pei,Peng Zhou,Yi-lang Shi,Zai-hua Cai,Hong-bin Xu,Yi Zhang
An ion-imprinted polymer (IIP) was synthesized by radical copolymerization for use in the removal of trace Fe(III) ions from Cr(III)-containing solutions. During the synthesis process, Fe(III) ions, acrylic acid and ethylene glycol dimethacrylate were employed as the template ions, functional monomer and cross-linker, respectively. The optimal mole ratio of acrylic acid to Fe(III) ions, which significantly affected the adsorption performance, was determined. The maximum static adsorption capacity of the polymer for Fe(III) ions was 114.25 mg g −1 , with a selective factor ( k ) of 492.18 and a relative selective factor ( k′ ) of 50.87 for Fe(III)/Cr(III). The Fe(III) ions removal efficiency could reach 94.43%, leading to a final Fe(III) concentration of 0.053 mg L −1 in the treated solution. After the removal process, the mass ratio of Cr(III) ions to Fe(III) ions was higher than 26, 000:1 in the solution, with an initial mass ratio of Cr(III) to Fe(III) ions of 1500:1.
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FUEL PROCESSING TECHNOLOGY
·
2018
·
IF 3.956
Ting Lu,Yucui Hou,Weize Wu,Muge Niu,Wei Li,Shuhang Ren
Carboxylic acids are considered as an important group of chemicals. Direct conversion of cellulose to formic acid (FA) by vanadium(V(V))-contained catalyst is of significant conceptual and practical interest. A second metal (from Mg(II), Ca(II), Al(III), Cr(III), Mo(VI), Mn(II), Cu(II), or Fe(III)) incorporated into V(V)-contained catalyst system was screened to further improve the oxidation of cellulose by O 2 to yield FA. Fe(III) exhibited the best performance and effects of reaction parameters on the conversion of cellulose in NaVO 3 -FeCl 3 -H 2 SO 4 aqueous solution were investigated. Cellulose could be rapidly converted, and the yield of FA (66.8%) was higher than that obtained by the single use of FeCl 3 (48.4%) or NaVO 3 (57.6%). The conversion of cellulose in another V(V)-contained catalyst system (H 5 PV 2 Mo 10 O 40 ) was explored to verify the universal enhancement of FeCl 3 . Influences of the second metal Fe(III) on the V(V)-contained catalyst system and mechanism of cellulose oxidation in the V(V)-Fe(III)-H 2 SO 4 system were studied. Compared with single use of V(V), the employment of Fe(III) alone is not active enough in the oxidative C C bond cleavage . V(V) other than Fe(III) is the main active species for selective oxidation of substrates. The incorporation of Fe(III) and V(V) shows both synergistic and competitive relationships. Both the synergistic and competitive effects are beneficial to increase FA yield, as they promote the oxidation of V(IV) to V(V), increase oxidative ability, and inhibit the overoxidation to by-product CO 2 . The catalyst system was reused four times without decline in activity.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Changjian Li,Yueqi Wang,Xiaojie Zhang,Xueling Guo,Xiaoxuan Kang,Libo Du,Yang Liu
Carbon dots have attracted considerable attention in the field of biosensors and bioimaging because of their excellent optical performance and low toxicity. However, the cellular uptake of the reported carbon dots generally has a low efficiency, which limits their practical applications. In this study, we reported a novel red fluorescent sulfur and nitrogen co-doped carbon dots with small molecular phenylboronic acid tags (i.e. S, N-CDs-PBA). The S, N-CDs-PBA can be taken up rapidly by PC12 cells in twenty minutes and showed high sensitivity for the detection of Fe 3+ ions. The maximum emission wavelength is at 593 nm under the excitation of 550 nm. The absolute fluorescence quantum yield is 23% in water. The fluorescence can be effectively and selectively quenched by Fe 3+ ions and the linear response range of Fe 3+ ions was obtained from 0.3 µM to 5.0 µM with a detection limit as low as 0.1 µM. It could be concluded that the rapid uptake of S, N-CDs-PBA into cells and high photoluminescence quantum yield of red emission are beneficial for quick detection of Fe 3+ ions.
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ENVIRONMENTAL TOXICOLOGY AND PHARMACOLOGY
·
2018
·
IF 2.776
Chen Zhou,Huiqing Wang,Youbin Si,Kang Wu,Amina Yousaf
The ability of anthraquinone-2,6-disulfonate (AQDS) and riboflavin to enhance the sulfamethoxazole (SMX) degradation coupled with the Fe(III) reduction by Shewanella oneidensis MR-1 was investigated. The results indicated that the SMX degradation rate was 38.5% with an initial SMX concentration at 0.04 mM. For the overall performance of AQDS and riboflavin mediated SMX degradation and iron reduction, the SMX degradation rate was gradually increased with the enhancement of iron reduction. Riboflavin had a stronger enhancement on SMX degradation and iron reduction than AQDS, but the enhancement was not positively correlated with electron shuttles concentration. A quantitative characterization of the electron transfer capacity (ETC) of the electron shuttles showed that the ETC was higher for riboflavin than AQDS. The S. oneidensis MR-1 16S rRNA gene copies results indicated that electron shuttles had a positive effect on the microbial activity of S. oneidensis MR-1. The LC MS result indicated that the products of the SMX biodegradation were 3-amino-5-methylisoxazole and 4-aminobenzenesulfonic acid, which suggested that the SMX biodegradation was caused by S N bond cleavage. This study indicates that the biochemical mechanisms play a vital role in SMX transformation and Fe(II) generation in this system.
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ADVANCED FUNCTIONAL MATERIALS
·
2019
·Vol. 29
·期 36
·1904056
·
IF 15.621
Jing Zhu,Chengchao Chu,Dongsheng Li,Xin Pang,Huili Zheng,Junqing Wang,Yesi Shi,Yang Zhang,Yi Cheng,En Ren,Jingliang Cheng,Xiaoyuan Chen,Gang Liu
To address the urgent need for effective sonodynamic therapy (SDT), a facile and efficient strategy is developed for fabricating a new class of sonotheranostics. Herein, a Fe(III)-porphyrin nano-sonosensitizer is prepared by a one-step coordination synthesis, and then anchored with Bis(DPA-Zn)-RGD and manganese superoxide dismutase (SOD2) siRNA. Benefiting from the delicate interactions of the Fe(III)-coordinated nanoformulations, a highly potent sono/gene combinational therapy guided by fluorescence/magnetic resonance imaging is achieved. Importantly, this sonotheranostics significantly enhances the SDT effect of porphyrin through the cancer-targeted delivery capability and enhanced reactive oxygen species production via triple-regulated approaches, including down-regulation of SOD2, depletion of glutathione, and generation of Fenton reaction. This work opens up new perspectives for developing versatile sonotheranostics to overcome the clinical challenges of SDT.
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CRYSTENGCOMM
·
2025
·
IF 2.6
Han Fang,Jia-Peng Han,Bo Zhang,Deng-Bo Liu,Xing-Wang Li,Jing-Yu Li,Yutong He,Mei-Hui Yu
The heavy metal ion pollution has become one of the most serious environmental problems, which promotes the continuous exploration of new materials and methods to achieve efficient detection of heavy metal ions. Luminescent metal-organic frameworks (LMOFs) featuring the designable and functional structures and tunable luminescence properties exhibit excellent potential for the recognition and detection of heavy metal ions. Herein, a Cd(II)-based luminescence MOF {[Cd2(2F-bpdc)2(tib)]}n (NKM-103) (tib=1,3,5-tris(1-imidazolyl)benzene, 2F-H2bpdc= 3,3'-difluorobiphenyl-4,4'-dicarboxylic acid) has been designed and synthesized successfully. Derived from the characteristic of ligand with conjugated units, NKM-103 shows well fluorescence emission performance and potential as a sensor for detecting both Fe(III) cations and Cr(VI) anions (Cr2O72- and CrO42-) through turn-off effect. Moreover, NKM-103 for all three kinds of ions shows low detection limit and high selectivity.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Shishun Wang,Shuang Gai,Kui Cheng,Zhuqing Liu,Markus Antonietti,Fan Yang
The degradation efficiency of organic contaminants using Fenton-like system based on Fe(II) and peroxymonosulfate (PMS) has been hindered by the rapid transformation from Fe(II) to Fe(III) and the slow regeneration of Fe(II). To address this challenge, artificial humic acid (AHA) derived from biomass was incorporated into Fe(III)/PMS system to build AHA/Fe(III)/PMS system. The results demonstrated that the degradation rate of atrazine (ATZ) in AHA/Fe(III)/PMS system (98.83%) is significantly superior to those in Fe(III)/PMS (16.51%) and AHA/PMS system (41.76%) within 90 min. Furthermore, Fe(II) measurement experiments revealed that AHA exhibited more significant iron-reducing potential. The analysis of FTIR, 3D-EEM, and liquid NMR indicated that AHA possessed more structures with reductive potential in comparison to commercial humic acid (CHA) and humic acid extracted from lignite (LHA). The results of persistent free radicals indicated that CHA possessed oxidative potential, which also accounted for the lowest Fe(II) concentration in those system containing CHA. Furthermore, quenching experiments, EPR analysis, and PMSO probe analysis have indicated the presence of reactive species such as •OH, SO 4 •- , and Fe(IV) within AHA/Fe(III)/PMS system. The degradation products from ATZ were identified and determined to exhibit reduced toxicity relative to parent compound. Collectively, these findings presented an in-depth understanding to reactivate Fe(III)/PMS system, offering a promising alternative strategy for efficient degradation of organic pollutants in water treatment processes.
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