FREE RADICAL RESEARCH
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2020
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IF 2.839
Bo Yin,Rui Rui Liu,Ya Jie Meng,Hong Lin Zhai,Sha Sha Li,Jules Muhire
Found in various natural food products, many in vitro evidence indicated that resveratrol (RES) has been linked to neuroprotective and cardioprotective effects and prevent cancer development. However, human clinical trials have been conducted with varying results, making the usage of RES controversial. In this paper, we demonstrated that the drug RES could be conjugated with the high levels of endogenous GSin cancer cells. 5,5-Dimethyl-1-Pyrroline-N-Oxide (DMPO) was employed to capture the GS•. The molecular mechanism of the reaction between RES and GSwas further studied by UV-Vis spectrometry, mass spectrometry and Density Functional Theory (DFT) calculations. Besides, the formation of the adduct GS-RES in cancer cell was obtained when RES was added during incubation. Further study indicated that over 77.6% of the RES was consumed in cancer cells. This study suggested that endogenous GSmay be one of the important factors to cause the depletion of anti-tumour drugs during chemotherapy, which should be paid special attention in clinical therapeutics and drug development.
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高影响因子
Materials Science and Engineering B-Advanced Functional Solid-State Materials
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2020
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IF 4.706
Hongyu Luo,Ming Yan,Yilin Wu,Xinyu Lin,Yongsheng Yan
Porous TiO 2 nanorods were synthesized by H 2 SO 4 etching method, combined with the synthesis technology of BiOBr-TiO 2 heterojunction and NCQDs to synthesis the ternary NCQDs-BiOBr-TiO 2 photocatalyst. The micromorphology and structural composition of different powder catalysts and photocatalytic composite membranes were studied by means of various characterization methods. The UV–vis DRS results indicated that the formation of BiOBr-TiO 2 heterojunction and the introduction of NCQDs extended the visible light absorption range of photocatalytic materials. The BSA adsorption performances of different composite membranes were investigated, and the results showed that 0.5-NCQDs-BiOBr-TiO 2 /PVDF composite membranes had strong antifouling properties. Moreover, it was found that the 0.5-NCQDs-BiOBr-TiO 2 /PVDF composite membranes exhibited high regeneration stability and easy separation recovery performance. The results showed that the TC degradation rate of 0.5-NCQDs-BiOBr-TiO 2 /PVDF composite membranes reached 77% within 120 min. Moreover, the pseudo first order kinetic apparent rate constant k value of the 0.5-NCQDs-BiOBr-TiO 2 /PVDF composite membranes was 0.01342 min −1 .
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2020
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IF 5.774
Weike Zhao,Bo Zhou
In recent years, multi-walled carbon nanotubes (CNTs), which are emerging nanocatalysts, have received much attention in advanced oxidation processes. CNTs were introduced into H 2 O 2 /Fe(III) Fenton-like process to enhance the degradation of bisphenol A (BPA) in this study. The results of the study suggests that CNTs could effectively promote electron transfer from H 2 O 2 to Fe(III) and directly reduce Fe(III) to Fe(II) to accelerate Fe(III)/Fe(II) cycles, in which carbonyl groups and structural defects of CNTs were identified as the major active sites via SEM, Raman, XRD, FTIR and XPS analyses. It was revealed that hydroxyl radical (·OH) majorly contributed to the degradation of BPA, and the generation efficiency of ·OH was significantly increased by 3.2 times with the addition of CNTs. Also, nine intermediate products were identified, and the possible degradation pathways of BPA were proposed through the density functional theory (DFT) calculations and HPLC-MS/MS analysis. The ecotoxicity evaluation of BPA demonstrates that the oxidative degradation of BPA in CNTs/H 2 O 2 /Fe(III) system could effectively reduce its environmental risk. The critical experimental parameters including the dosage of Fe(III), H 2 O 2 , CNTs, initial pH and various anions (Cl − , HCO 3 – , SO 4 2− ) were investigated, and the reusability experiments indicate that CNTs maintained high stability and reusability during the reaction.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Lijun Guo,Jieting Zhao,Liming Zhao,Yuling Tang,Jianfei Zhou,Bi Shi
Carbonaceous materials have attracted considerable attention as promising catalysts of persulfate (PS) activation for antibiotic degradation. In this work, an environment-friendly and low-cost carbonaceous material (Cr 2 O 3 /BC) was prepared by pyrolyzing chrome shavings, and the catalytic ability of Cr 2 O 3 /BC for PS activation was evaluated using tetracycline (TC) as the model antibiotic. The Cr 2 O 3 /BC/PS system exhibited ultrafast TC removal efficiency (99.9% removal rate within 5 min), which was owing to persistent free radicals, defective sites, and dispersed Cr 2 O 3 particles, which were beneficial for the generation of free radicals, such as OH·, SO 4 ·- , ·O 2 – and 1 O 2 . Coexisting substances, such as inorganic ions and humic acid, exerted little effect on TC removal. In addition, 99.9% of TC removal rates were achieved in TC contaminated tap water. Cr 2 O 3 /BC/PS system also exhibited the high removal rates towards ciprofloxacin (98% removal rate within 5 min) and sulfadiazine (99.8% removal rate within 5 min). Surprisingly, no chromium was detected after TC degradation, indicating that no secondary pollution was generated. This work provides a feasible strategy for the high-value use of chrome shavings and a practical method for antibiotic removal.
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APPLIED SURFACE SCIENCE
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2020
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IF 6.182
Jinge Du,Zhe Xu,Hui Li,Haijun Yang,Shengjun Xu,Jun Wang,Yanan Jia,Shuanglong Ma,Sihui Zhan
A novel Z-scheme Ag 3 PO 4 /g-C 3 N 4 heterostructures was constructed successfully for Escherichia coli inactivation and organic pollutants degradation under visible light irradiation. The Ag 3 PO 4 (8)/g-C 3 N 4 possessed the highest photocatalytic effect with more than 7 log of live Escherichia coli ( E. coli ) totally inactivated within 75 min and complete BPA degradation within 180 min. By mimicking the components of natural water individually, humic acid (HA) and inorganic anion were found to deeply affected the photocatalytic disinfection activity. Moreover, the Ag 3 PO 4 (8)/g-C 3 N 4 revealed significantly boosted visible-light-driven photocatalytic performance for ciprofloxacin and sulfadiazine degradation. The satisfying degradation effects of bisphenol A in nature waters were also obtained. The improved photocatalytic efficiency of Ag 3 PO 4 /g-C 3 N 4 may be attributed to the formation of Z-scheme heterostructure structure and matching valence band and conduction band, resulting in rapid separation of photo-induced carrier, enhanced electronic transport capacity and prolonged carrier lifetime. The possible mechanism was studied using radical quenching tests and electron spin resonance, suggesting that the hole, electron and hydroxyl radical were the paramount active species during Escherichia coli disinfection. This work pioneers a novel strategy for upgrading the photocatalytic disinfection and degradation capacities of g-C 3 N 4 based catalysts.
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ENVIRONMENTAL RESEARCH
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2020
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IF 5.715
Zhuo Shen,Lingling Fan,Shangkun Yang,Yuyuan Yao,Haixiang Chen,Wentao Wang
The Fenton-like process has been regarded as a clean and efficient approach to generate reactive oxygen species (ROS) to deal with the ever-growing environmental pollution . However, developing improved catalysts with adequate activity and stability remains a long-term goal for practical application. Herein, crystalline carbon nanotubes (CNTs) interconnected Fe/Fe 3 C-doped nanoporous carbonitride (Fe-NC) was easily prepared by the pyrolysis of ZIF-8 confined with Fe 3+ . The obtained Fe–NCs possessed high degrees of graphitic carbon and nitrogen. Such Fe–NCs can enhance the activation of peroxymonosulfate (PMS) for the removal of multiple organic contaminants . The optimized Fe-NC/PMS system exhibited impressive catalytic performance, with a TOF as high as 4.43 min −1 for 3BF degradation, and the removal efficiency of other dyes, phenols and antibiotics was up to 96.2% within 10 min. The removal efficiency of 3BF was 93.4% within 10 min with extremely low iron ions leaching (<0.052 mg/L) even after five cycles. In addition, the effects of pH on the catalytic performance demonstrated that the decomposition of 3BF exceeded 95.6% even when the initial pH varied from 5 to 10. We confirmed that SO 4 - , OH, O 2 - and 1 O 2 were generated in the catalytic system of Fe-NC/PMS, which played a critical role in degrading the organics. These findings provide new insights into the design of environmental-friendly Fenton-like catalysts with high efficiency and favorable stability in environmental remediation.
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高影响因子
ACS Applied Materials & Interfaces
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2020
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IF 8.758
Dahu Ding,Liang Zhou,Fuxing Kang,Shengjiong Yang,Rongzhi Chen,Tianming Cai,Xiaoguang Duan,Shaobin Wang
Biochar is a promising candidate for the adsorptive removal of organic/inorganic pollutants, yet its role in metal-free catalyzed advanced oxidation processes still remains ambiguous. In this work, five biochar samples (PPBKx, where x represents the pyrolysis temperature) were prepared by using metal-enriched phytoremediation plant residue as the feedstock. Notably, PPBK exhibited a high specific surface area (as high as 1090.7 m2 g–1) and outstanding adsorption capacity toward ciprofloxacin (CIP, as much as 1.51 ± 0.19 mmol g–1). By introducing peroxymonosulfate (PMS, 5 mM) as the chemical oxidant, over 2 mmol g–1 CIP was synergistically adsorbed and oxidized within 30 min although PMS itself could not oxidize CIP efficiently, suggesting the formation of reactive oxidative species. Theoretical calculations revealed that PMS anions preferentially adsorbed on the activated C atoms adjacent to the graphitic N dopant, where the carbon matrix served as the electron donor, instead of as an electron mediator. The adsorbed PMS possessed a smaller molecular orbital energy gap, indicating that it was much easier to be activated than free PMS anions. Surface-bound reactive species were elucidated to be the dominant contributor through chemical quenching experiments and electrochemical characterizations. The catalytic activity of PPBK700 could be greatly retained in repeated oxidations because of the stable N species, which serve as the active catalytic sites, while the CIP adsorption was greatly deteriorated because of the diminishing active adsorption sites (carbon matrix edge) caused by the partial oxidation of PMS. This work not only provides a facile and low-cost approach for the synthesis of functional biochar toward environmental remediation but also deepens the understanding of biochar-catalyzed PMS activation and nonradical oxidation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Bihui Niu,Min Yu,Changduo Sun,Luhan Wang,Kun Zang,Xiaowen Hu,Lei Zhou,Yian Zheng
Perfluorooctanoic acid (PFOA) is an anthropogenic persistent organic compound that resistant to traditional oxidative decomposition, bringing thus huge pressure to the environment. Here, the open hollow structured Calotropis gigantea fiber (CGF) was developed using a facile pyrolysis and subsequent magnetization method, and the resulting magnetic carbonized fiber (MC-CGF) was applied as an efficient catalyst for PFOA decomposition at room temperature in persulfate-based oxidation process. The experimental results indicated that with the addition of MC-CGF, the removal efficiency of PFOA could reach to 75.76% at 30℃ and pH 2.0. By calculation, the apparent activation energy was reduced from 62.76 kJ/mol to 22.49 kJ/mol, demonstrating that in the presence of MC-CGF, a lower reaction temperature and a shorter time were enough to reach the higher efficiency for PFOA decomposition. Mechanism research showed that during the decomposition process, PFOA underwent a first decarboxylation process and two possible decomposition pathways should also be taken into discussion. Taking pakchoi as the plant model, the process toxicity was finally evaluated, and the changes in chlorophyll content stated that the decomposition process of PFOA by MC-CGF assisted persulfate system was relatively harmless and environmental-friendly.
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Journal of Materials Chemistry B
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2021
·Vol. 9
·期 8
·2042-2053
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IF 6.331
Xiaolu Guo,Changchun Wen,Qianxin Xu,Changping Ruan,Xing-Can Shen,Hong Liang
The second near-infrared (NIR-II) window (1000–1350 nm) usually offers further improved light penetration, a higher maximum permissible exposure (MPE), and a lower background signal. Development of NIR-II optical diagnosis and phototherapy technologies is of great significance for precise, efficient tumor therapy. In this work, a new type of Ti-based targeting agent (B-TiO2@SiO2–HA) nanotheranostic system with strong NIR-II absorption was designed and fabricated for the first time. Oxygen vacancies were formed in B-TiO2 and its band gap was narrowed, resulting in nanotheranostic systems with full-spectrum responses to stimulation with light. The experimental results showed that B-TiO2@SiO2–HA not only can enable high NIR-II photothermal conversion and provide excellent reactive oxygen species (ROS) production capacity, but also can enable high-resolution photoacoustic imaging (PAI) under NIR-II laser irradiation. Moreover, HA modification gives the nanotheranostic systems the useful ability to target high-CD44-expression tumor cells and tissues. In vitro and in vivo experiments demonstrated that B-TiO2@SiO2–HA exhibited a targeted photothermal/photodynamic (PTT/PDT) effect that produced tumor-cell ablation and apoptosis under the guidance of real-time NIR-II PA imaging. B-TiO2@SiO2–HA exhibits precise nanotheranostic potential for PAI-guided tumor-targeting phototherapy.
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SOLID STATE SCIENCES
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2021
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IF 3.059
Yong Cao,Kangping Cui,Yihan Chen,Minshu Cui,Guanghong Li,Dong Li,Xiaojun Yang
Iron Oxychloride (FeOCl) was prepared by partial thermal decomposition and was studied as a heterogeneous Fenton catalyst to degrade tetracycline (TC). SEM, XRD , XPS technology were used to characterize its performance. The influencing factors of TC degradation efficiency were studied, including pH value, H 2 O 2 content, catalyst dosage and initial TC concentration. The results showed that under the optimal conditions, the degradation rate of 60 mg L −1 TC reached 92.9% within 60 min of reaction. The degradation process follows a second-order kinetic equation. Compared with other iron-based catalysts, FeOCl exhibited better catalytic and degradation effects. Moreover, FeOCl/H 2 O 2 system exhibited a wide pH range (from 3.0 to 7.0) for efficient degradation of TC and showed excellent stability and reusability. Meanwhile, based on the intermediates identified by HPLC-MS, two possible pathways for the degradation of TC were proposed. Further, the results of electron spin-resonance spectroscopy and radical quenching tests suggested that the ·OH formed in the FeOCl/H 2 O 2 system was mainly responsible for the degradation of TC.
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Nano Research
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2020
·Vol. 14
·期 7
·2383-2389
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IF 8.183
Zhang Yuwei,Liu Fei,Yang Zhichao,Qian Jieshu,Pan Bingcai
In the pursuit of heterogeneous catalysts with high reactivity, metal organic framework (MOF) nanomaterials have received tremendous attentions. However, many MOF catalysts especially Fe-based MOFs need to be utilized immediately after synthesis or being activated using high temperature, because of the easy loss of reactivity in humid environments resulting from the occupation of active Fe sites by water molecules. Here, we describe an inspiring strategy of growing MIL-101-Fe nanoparticles inside the three-dimensional confined space of graphene aerogel (GA), generating shapeable GA/MIL-101-Fe nanocomposite convenient for practical use. Compared to MIL-101-Fe, GA/MIL-101-Fe as catalyst demonstrates much higher reactivity in Fenton-like reaction, attributing to smaller MIL-101-Fe particle size, presence of active Fe(II) sites, and abundant defects in GA. Strikingly, the weakly hydrophobic nature of the composite greatly inhibits the loss of catalytic reactivity after being stored in humid air and accelerates the recovery of reactivity in mild temperature, by resisting the entrance of water molecules and helping to exclude water molecules. This work demonstrates that a delicate design of nanocomposite structure could not only improve the reactivity of the catalytic component, but also overcome its intrinsic drawback by taking advantage of the properties of host. We hope this functional nanoconfinement strategy could be extended to more scenarios in other fields.
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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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