WATER RESEARCH
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2022
·
IF 13.4
Qinyue Wu,Yan Zhang,He Liu,Hongbo Liu,Jia Tao,Min-Hua Cui,Zhiyong Zheng,Donghui Wen,Xinmin Zhan
For preparing high performance biochar to be applicated in persulfate-based oxidation treatment of wastewater, the feasibility of deriving Fe-N biochar from pharmaceutical sludge by endogenous Fe and exogenous N doping was investigated. With exogenous urea doping, Fe x N contained biochar (PZBC800U) was successfully derived from endogenous Fe(OH) 3 contained pharmaceutical sludge . PZBC800U effectively activated peroxymonosulfate (PMS) to remove 80 mg·L −1 levofloxacin (LEV) within 90 min. The main mechanism of PMS activation by PZBC800U for LEV degradation was revealed as non-radical pathways dominated by 1 O 2 generation and direct electron transfer . The formation of Fe x N combined with the increase of pyridinic-N in the biochar changed the electronic structure, improved the electron transfer ability, and thus achieved the excellent PMS activation capacity of the biochar. The vital function of endogenous Fe(OH) 3 was verified by comparing PZBC800U to Fe leached and extra Fe added controls. A total of 18 intermediates in the degradation of LEV were identified, and degradation pathways were proposed. Combined with the average local ionization energy calculation, the priority of piperazine breakage during LEV degradation was experimentally proved and mechanistically elucidated. This study provides a new insight into Fe x N biochar preparation from pharmaceutical sludge and the mechanisms of its excellent PMS activation performance for LEV degradation.
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DESALINATION
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2022
·
IF 11.211
Wen-Han Yu,Yu-Jie Shen,Li-Feng Fang,Ze-Lin Qiu,Jun Han,Bao-Ku Zhu
Positively-charged nanofiltration (NF) membranes have attracted more attention compared with traditional negative NF membranes. In this work, one-step self-assembly strategy was designed to prepare positively-charged NF separation layer by the close packing of poly(styrene- r -quaternized 2-(dimethylamino)ethyl methacrylate) (P(St- r -QDMA)) nanoparticles (NPs) with intramolecular crosslinking structure. Meanwhile, the pore size of NF membrane was tailored by regulating the aggregation of the NPs using different ions and annealing conditions. Herein, water was used as a dispersant to obtain P(St- r -QDMA) NPs dispersion, which is non-toxic and green. The pore size cut-off (PSCO) of the separation layer is well controlled in the range of 0.98–4.04 nm. The optimal membrane showed molecular weight cut-off (MWCO) of 380 Da (i.e., PSCO, 0.98 nm) with the isoelectric point of 9.4, which effectively improved the separation performance for divalent cations (97.2 % for MgCl 2 and 96.0 % for CaCl 2 ) and neutral small molecules (97.7 % for VB 12 and 92.5 % for PEG400). This work gives a novel and convenient method to construct positively-charged NF membrane with controlled pore sizes, which will be a promising candidate for water softening and molecular separation.
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Minerals
·
2022
·Vol. 12
·期 9
·1097
·
IF 2.818
Dongyue Wang,Yuhang Meng,Aidong Tang,Huaming Yang
Engineered nanoparticle–support interaction is an effective strategy for tuning the structures and performance of engineered nanoparticles. Here, we show that tuning the dehydroxylation of kaolinite nanoclay as the support could induce zinc oxide–kaolinite interactions. We used free energy theory, electron microscopy, and X-ray photoemission spectroscopy to identify interaction strengths between metal oxides and the underlying nanoclay induced by dehydroxylation. Desirable exposure of nanoparticle sites and the geometrical and crystal structure were obtained by tuning the interface interactions between ZnO nanoparticles and nanoclay. The surface free energy of zinc oxide–nanoclay results in different interfacial interactions, and the properties of the surface free energy electron-donating (γ−) and electron-accepting (γ+) parameters have significant effects on the electron acceptor. This could, in turn, promote stronger interactions between zinc oxide and the kaolinite surface, which produce more active (0001) Zn-polar surfaces with promoting zinc oxide nanoparticles growing along the <0001> direction. Reactive oxygen species, leached zinc ions, and electron transfer can modulate the antibacterial activities of the samples as a function of interface free energy. This further demonstrates the interfacial interactions induced by dehydroxylation. This work has new application potential in biomedicine and materials science.Keywords:kaolinite;dehydroxylation;interfacial interactions;ZnO nanoparticles;antibacterial activities
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ACS Nano
·
2022
·
IF 18.027
Ruoyao Li,Yuanyuan Fan,Lulu Liu,Hongna Ma,Deyan Gong,Zhaohua Miao,Hua Wang,Zhengbao Zha
The exciting success of NBTXR3 in the clinic has triggered a tumult of activities in the design and development of hafnium-based nanoparticles. However, due to the concerns of nondegradation and limited functions, the biomedical applications of Hf-based nanoparticles mainly focus on tumors. Herein, tannic acid capped hafnium disulfide (HfS2@TA) nanosheets, a 2D atomic crystal of hafnium-based materials prepared by liquid-phase exfoliation, were explored as high-performance anti-inflammatory nanoagents for the targeted therapy of inflammatory bowel disease (IBD). Benefiting from the transformation of the S2–/S6+ valence state and huge specific surface area, the obtained HfS2@TA nanosheets were not only capable of effectively eliminating reactive oxygen species/reactive nitrogen species and downregulating pro-inflammatory factors but also could be excreted via kidney and hepatointestinal systems. Unexpectedly, HfS2@TA maintained excellent targeting capability to an inflamed colon even in the harsh digestive tract environment, mainly attributed to the electrostatic interactions between negatively charged tannic acid and positively charged inflamed epithelium. Encouragingly, upon oral or intravenous administration, HfS2@TA quickly inhibited inflammation and repaired the intestinal mucosa barrier in both dextran sodium sulfate and 2,4,6-trinitrobenzenesulfonic acid induced IBD models. This work demonstrated that ultrathin HfS2@TA atomic crystals with enhanced colon accumulation were promising for the targeted therapy of IBD.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yao Xiong,Tianshun Wang,Lei Liu,Yuanqi Kou,Zhengyu Zhao,Min Yuan,Yan Chen,Dan Wang,Shiyong Song
D-ɑ-tocopheryl poly(ethylene glycol)1000 succinate (TPGS) has been extensively applied in drug delivery systems for its amphiphilic property and inherent bioactivity. But TPGS has not always been utilized solely for the unstability of TPGS micelle. Inspired by the hydrogels made from other amphiphilic molecules, thermosensitive TPGS hydrogels were firstly discovered and developed in the presence of specific anions, which self-assembled from the aggregation of TPGS micelles stimulated by heating and salting-out effect. Subsequently, hydrophobic doxorubicin (DOX) loaded TPGS micelles were likewise prepared and converted into DOX loaded hydrogel with the help of β-Glycerol phosphate disodium (β-GP). It was found that the amount of TPGS and β-GP in the solution considerably affected the gelation time and critical temperature. One of the formulations containing 4 wt% TPGS and 15 wt% β-GP was selected due to its appropriate gelation time and temperature for subcutaneously injection. Pristine and drug-loaded TPGS hydrogels were explored for their potential values in clinic applications. Derived from the bioactivity of TPGS, the pristine TPGS hydrogel exhibited a certain tumor inhibiting efficiency comparable to the DOX-containing formulations. And the efficiency of DOX-loaded TPGS hydrogels were dosage-dependent and superior to systemically administrated free DOX, which demonstrated a synergistic effect between DOX and TPGS hydrogel. In short, this study developed a multifunctional injectable hydrogel and provided a new synergetic strategy for tumor therapy.
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MICROCHEMICAL JOURNAL
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2022
·
IF 5.304
Die Deng,Shaohua Wen,Ya Wang,Jia Liu,Fang Li,Xiupei Yang
Cerium dioxide (CeO 2 ) has usually been used as a catalyst for colorimetric assays. However, the low catalytic efficiency has limited their further application. Covalent organic frameworks (COFs) have sparked increasing interest in the unique properties of large surface area, high porosity, and good thermochemical stability. Herein, a novel covalent organic framework composite (TpPa@CeO 2 ) with dual mimic enzyme activities (oxidase and peroxidase) was successfully synthesized via a facile hydrothermal method. TpPa@CeO 2 showed higher catalytic activity than CeO 2 . The excellent catalytic performance of TpPa@CeO 2 could be attributed to the higher surface area, more surface active species and higher Ce 3+ /Ce 4+ ratio in the composite than CeO 2 . Based on this, a visual and sensitive colorimetric sensor was constructed to detect ascorbic acid (AA) in the linear range of 0.2–35 μM with a low detection limit (LOD) of 0.061 μM. Moreover, the excellent colorimetric sensor was successfully applied to detect AA in beverage and tablet samples with satisfactory recoveries ranging from 95.78 % to 100.84 %. The catalytic mechanism could be that the composition of TpPa and CeO 2 improved the ratio of Ce 3+ /Ce 4+ , which promoted the decomposition of dissolved oxygen and H 2 O 2 by CeO 2 to produce superoxide radicals (·O 2 – ) and hydroxyl radicals (·OH), respectively. The facile and sensitive sensor system constructed by TpPa@CeO 2 with promising applications provides a new platform for the detection of AA in real sample analysis.
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Advanced Science
·
2022
·Vol. 9
·期 29
·2201541
·
IF 17.521
Jiawei Huo,Jie Li,Yang Liu,Libin Yang,Xinran Cao,Chong Zhao,Yicheng Lu,Wei Zhou,Shumu Li,Jianan Liu,Jiao Li,Xing Li,Jing Wan,Rui Wen,Mingming Zhen,Chunru Wang,Chunli Bai
Malignant proliferation and metastasis are the hallmarks of cancer cells. Aminated [70]fullerene exhibits notable antineoplastic effects, promoting it a candidate for multi-targeted cancer drugs. It is an urgent need to reveal the structure–activity relationship for antineoplastic aminated fullerenes. Herein, three amphiphilic derivatives of [60]fullerene with clarified molecular structures are synthesized: TAPC-4, TAPC-3, and TCPC-4. TAPC-4 inhibits the proliferation of diverse tumor cells via G0/G1 cell cycle arrest, reverses the epithelial–mesenchymal transition, and abrogates the high mobility of tumor cells. TAPC-4 can be excreted from the organism and achieves an in vivo inhibition index of 75.5% in tumor proliferation and 87.5% in metastatic melanoma with a wide safety margin. Molecular dynamics simulations reveal that the amphiphilic molecular structure and the ending amino groups promote the targeting of TAPC-4 to heat shock protein Hsp90-beta, vimentin, and myosin heavy chain 9 (MYH9), probably resulting in the alteration of cyclin D1 translation, vimentin expression, and MYH9 location, respectively. This work initially emphasizes the dominant role of the amphiphilic structure and the terminal amino moieties in the antineoplastic effects of aminated fullerenes, providing fundamental support for their anti-tumor drug development.
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ANALYTICA CHIMICA ACTA
·
2022
·
IF 6.911
Zongjia Li,Xinyue Guo,Juan Qin,Yanxue Guan,Jiang Li,Haoran Guo,Bailin Zhang,Miaomiao Zhang,Jilin Tang
Nanoparticles-based antioxidative therapy has been highlighted in a series of diseases triggered by excessive reactive oxygen species (ROS). Prussian blue nanoparticles (PBNPs), as a representative artificial nanozyme, have been proved as highly effective ROS scavengers. However, its detailed intracellular antioxidant mechanism is not clear yet. Herein, a series of PBNPs with different particle sizes were synthesized and their intracellular antioxidant activities were studied by atomic force microscopy (AFM) from a biomechanical perspective. We first validated the ROS scavenging ability of PBNPs in vitro. It indicated that PBNPs had great scavenging effect on multiple ROS, such as hydroxyl radicals (•OH), superoxide radicals (O 2 •− ) and hydrogen peroxide (H 2 O 2 ). By observing the changes in morphology and mechanical properties of human umbilical vascular endothelium cells (HUVECs), it was further found that PBNPs could apparently alleviate the decrease of Young's modulus caused by oxidative stress damage and kept cells in their normal morphology. In addition, the distribution of F-actin revealed that the enhancement of cytoskeleton stability by PBNPs might be a key way to protect HUVECs from oxidative damage. Importantly, the antioxidant activities of PBNPs were found to be size-dependent, which indicated the smaller particle size had better antioxidant activities compared with the larger particle size. This study serves as a novel medium to reveal the mechanism of nanoparticles on cells at the single-cell level and demonstrates the great potential of atomic force microscopy in studying the application of nanoparticles in cell biology.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Yangtao Wu,Dongxu Qu,Lingjun Bu,Shumin Zhu,Shiqing Zhou
This study explored the risk of trichloronitromethane (TCNM) formation during chlorination of the nitrite-containing water after pre-chlorination and subsequent UV irradiation (i.e., the chlorine-UV process). The competitive reaction between amino acid (AA) and NO 2 − for chlorine produced organic chloramine and reduced the oxidation from NO 2 − to NO 3 − , resulting in a significant enhancement of TCNM in the presence of AA (>5.52 μg L −1 ) as compared to the absence of AA (0.42 μg L −1 ). The generation of HO • during UV photolysis of organic chloramines was confirmed. Among the process parameters, pre-chlorination time (from 5 min to 30 min) had no significant effect on TCNM formation; the highest TCNM formation occurred at pH 7 (from pH 6 to pH 8); prolonged UV irradiation time (from 5 min to 30 min) and increased chlorine to AA ratio (Cl 2 :AA) (from 1 to 3) decreased the TCNM formation. The hydroxylated, chlorinated and nitrosated products were detected. The quantum chemical calculation results indicated the attack of NO 2 • was more likely to occur at the meta and para positions of benzoic acid (BZA), because of the steric hindrance of the carboxylic group in BZA to the ortho position. Based on the results of the toxicity assessment, pre-chlorination with a higher chlorine dosage could be an effective method of controlling both TCNM formation and acute toxicity. Overall, the results of this study contributed to the understanding of the TCNM formation mechanism as well as optimizing the parameters of the chlorine-UV process to reduce the risk of TCNM formation.
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Antioxidants
·
2022
·Vol. 11
·期 9
·1662
·
IF 7.675
Yibin Xu,Xiaoqing Ding,Yuanyuan Wang,Danlei Li,Lingyu Xie,Shuang Liang,Yunfeng Zhang,Weifen Li,Aikun Fu,Xiuan Zhan
Reuterin is well-known for its broad-spectrum antimicrobial ability, while the other potential bioactivity is not yet clear. The present study aims to investigate the immunomodulatory activity of reuterin on chicken macrophage HD11 cells for the first time and evaluate whether reuterin is able to regulate the lipopolysaccharide-stimulated inflammatory response. The results showed that the safe medication range of reuterin was less than 250 μM. Reuterin treatment for 6 h decreased the transcriptional ofCD86,IL-1βandiNOSand increased the expression ofCD206in a dose-dependent way, but reuterin treatment for 12 h contrary increased the expression ofIL-1β,IL-6andIL-10. However, it was noticed that reuterin treatment for 12 h significantly decreased the production of reactive oxygen species (ROS) and suppressed the phagocytosis activity of HD11 macrophages against bacteria. Further, the results showed that preincubation or coincubation with reuterin significantly attenuated the promotive effects of lipopolysaccharide (LPS) on transcription of proinflammatory cytokines (includingIL-1β,IL-6andTNF-α) and obviously inhibited nitric oxide (NO) production as well as the protein expression of inducible nitric oxide synthase (iNOS). Meanwhile, Mechanism studies implied that reuterin might exert an anti-inflammatory effect on LPS-stimulated cells by downregulating the expression ofTLR4/MyD88/TRAF6and blocking the activation of NF-κB as well as MAPKs signaling pathways. Additionally, it was found that both pretreatment and cotreatment with reuterin remarkably inhibited the oxidative stress induced by LPS stimulation by activating the Nrf2/HO-1 signaling pathway and enhancing the activities of antioxidative enzymes. These findings suggested the immunoregulatory function of reuterin and indicated this bacterial metabolite was able to inhibit the inflammation and oxidative stress of HD11 macrophages once exposed to LPS stimulation.Keywords:reuterin;HD11 cell line;lipopolysaccharide (LPS);inflammation response;oxidative stress
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PLoS One
·
2022
·Vol. 17
·期 8
·e0271408
·
IF 3.752
Daihua Hu,Tingting Gao,Xingang Kong,Na Ma,Jinhong Fu,Lina Meng,Xiaolong Duan,Ching Yuan Hu,Wang Chen,Zili Feng,Salman Latif
The green synthesis of silver nanoparticles (AgNPs) using a water extract of Ginger (Zingiber officinale) root by microwave irradiation and its antibacterial activities have been reported. However, AgNPs prepared from different parts of ginger root water or ethanol extract by ultrasound synthesis and their antioxidant activity and whether the biogenic could be used to catalyze the reduction of hazardous dye are unknown. This study concentrated on the facile green synthesis of AgNPs prepared from different parts (unpeeled ginger, peeled ginger, and ginger peel) of ginger root water or ethanol extract by the ultrasound-assisted method. We studied their antioxidant activity and catalytic degradation of hazardous dye Direct Orange 26 (DO26) and Direct Blue 15 (DB15). The surface plasmon resonance (SPR) peak of AgNPs was at 428–443 nm. The biogenic AgNPs were approximately 2 nm in size with a regular spherical shape identified from TEM analysis. The ethanol extracts of dried unpeeled ginger and peeled ginger, fresh peeled ginger and ginger peel. The Z . officinale AgNPs synthesized by dried unpeeled ginger ethanol extract showed the best antioxidant activity. Their scavenging activities were significantly better than BHT ( p <0.05). The different parts of ginger extracts showed no catalytic degradation activities of DB15 and DO26. Still, the synthesized Z . officinale AgNPs exhibited good catalytic degradation activities, while their ability to catalytic degradation to DB15 was better than DO26. In the additive ratio of 3 mL DB15, 0.1 mL NaBH 4 and 0.1 mL AgNPs, the degradation rates of DB15 (or DO26) at 15 min, 30 min and 60 min were only 1.8% (0.9%), 2.8% (1.4%) and 3.5% (1.6%) in the absence of AgNPs. When adding Z . officinale AgNPs prepared from dried ginger peel ethanol extract or fresh ginger peel water extract, the degradation rates of DB15 sharply increased to 97% and 93% after 30 min, respectively. In conclusion, ginger extract has good antioxidant properties. Z . officinale AgNPs biosynthesis from ginger extract exhibit excellent catalytic degradation activities, especially for the ginger peel extract. They have application value in the treatment of textile effluents and provide a new idea and method for the comprehensive development and utilization of ginger resources.
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Journal of Cleaner Production
·
2022
·
IF 11.072
Huiping Zeng,Jianxue Li,Jiaxin Xu,Wei Qi,Ruixia Hao,Da Lin,Dong Li,Jie Zhang
In this study, a novel magnetic biochar (BC-Fe n ), synthesized by one-step pyrolysis at 800 °C using platanus leaves and iron-containing sludge in different mass ratios, was used to activate persulfate (PS) for tetracycline (TC) degradation. Results show that BC-Fe 1:2 exhibited excellent degradation performance (91.4%), much better than the raw biochar (BC) (77.1%). And electron paramagnetic resonance (EPR) techniques demonstrated radical ( S O 4 · − , ·OH, O 2 · − ) and non-radical ( 1 O 2 ) pathways in BC-Fe 1:2 /PS, S O 4 · − was further proved to be the main active species by quenching experiments. Liquid chromatography-mass spectrometry (LC-MS) was utilized to identify the intermediates of TC and three possible degradation pathways were proposed. Additionally, the BC-Fe 1:2 was weakly affected by pH and the coexisting anions in wastewater, and could still remove 80% of TC in the third cycle experiment. This study provides a new idea for converting backwash iron-containing sludge from groundwater treatment plants into valuable catalysts, and provides new insights into the key role of low-cost magnetic biochar in PS activation.
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