MATERIALS CHEMISTRY AND PHYSICS
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2022
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IF 4.778
Dan Zhao,Mengyu Xu,Kang Dai,Huan Liu,Yan Jiao,Xincai Xiao
Chirality is one of the most widespread properties in nature. After the successful application of non-optical active carbon dots (CDs) in the fields of detection, imaging, and antibacterial, the researchers turned more attention to the preparation and applications of chiral CDs. This paper reports the preparation of several chiral CDs with chiral amino acids as carbon sources through two different methods (one-step hydrothermal route and two-step coupling route), and further explores the difference in antibacterial abilities of these chiral CDs prepared by different carbon sources and synthesis methods. The experiments results showed that chiral D/LGU which are prepared through one-step method and with glutamic acid (Glu), are superior to those prepared by two-step method (NLDU/NDGU), or those prepared with cysteine as raw material (D/LCS). For D/LCS, the antibacterial ability of the L type is superior to that of the D type, proving that the synthesis method and the chirality of raw material are both important in the antibacterial behavior of prepared CDs. The chirality and optical properties of prepared CDs have been characterized by UV–vis spectrophotometer , fluorescence spectrology, and circular dichroism. Through MurA enzyme inhibition tests, SEM, and molecular docking design, the antibacterial mechanism of chiral CDs has been investigated. The research provides a sound foundation for the preparation, characterization, and application of chiral CDs, as well as the novel targeting antibacterial applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Peizhen Yang,Yuhan Long,Wenli Huang,Dongfang Liu
Singlet oxygen ( 1 O 2 )-dominated advanced oxidation processes has drawn widespread attention for selective oxidation of organic pollutants in complex water environments. However, the high efficiency and selectivity of 1 O 2 generation remains challenging. Herein, we develop single-atom copper anchored on Ti 3 C 2 T x MXene nanosheets (Cu-SA/MXene) by molten salt etching for the generation of 1 O 2 via peroxymonosulfate (PMS) activation. Particularly, it exhibits a high selectivity of 99.71% toward 1 O 2 generation by activating PMS, which shows outstanding catalytic activity for multiple pollutants, and strong resistance to inorganic anions. Experimental and theoretical results reveal that the Cu single atoms with three oxygen coordination environments (Cu-O 3 ) are more favorable for PMS absorption and selectively adsorb the terminal oxygen of PMS to promote the generation of SO 5 .- , resulting in the generation of 1 O 2 . A continuous-flow wastewater system by dispersing catalysts on poly (vinylidene fluoride) membrane exhibit stable catalytic activity for polycarbonate plant wastewater treatment over 8 h.
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International Journal of Nanomedicine
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2022
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IF 7.033
Rui Ni,Lele Huang,Zhen Li,Wenli Zhang,Yajie Wang,Yan Shen,Jianxin Wang,Weigen Lu
Purpose To enhance tumor penetration by formulation design and tumor microenvironment (TME) modulation, herein a novel reactive oxygen species (ROS)-responsive size/shape transformable lipid-polymer hybrid nanoparticle (LPN) has been fabricated for the co-delivery of an anticancer and collagen-inhibition drug. Methods A ROS-responsive poly(D, L-lactide)-thioketal-polyethylene glycol (PLA-TK-PEG) co-polymer was synthesized. LPNs were then fabricated by encapsulation of losartan (LST)-loaded micelles as the core to support paclitaxel (PTX)-loaded liposomes. The PEG content in the lipid shell of LPNs was then adjusted to obtain the size-/shape-transformable LPNs (M/LST-Lip/PTX-PEG 5% ). The ROS-responsiveness was observed in vitro by transmission electron microscopy and the tumor-penetration of the LPNs was evaluated in 3D tumor spheroids by confocal laser scanning microscopy. Tumor-targeting, tumor-penetrating, and antitumor efficacies of the NPs in 4T1 tumor-bearing mice were determined by in vivo imaging. Results ROS-responsive micellar core degradation and the transformation of spherical LPNs (120nm) to smaller 40 mm discoid nanoparticles (NP) were observed. The transformable LPNs exhibited enhanced capacity of penetration in contrast to the un-transformable preparations in three-dimensional (3D) tumor spheroids. Furthermore, synergetic penetrating enhancement was achieved by LST-loaded transformable LPNs in 4T1 and fibroblast cell mixed 3D tumor spheroids. The improved tumor penetration of LST-loaded transformable LPNs was observed in vivo, which could be due to their collagen inhibiting and size/shape transformable effect. Due to their enhanced penetrability, LST and PTX-loaded transformable LPNs demonstrated significant in vivo antitumor efficacy in comparison to other preparations. Conclusion The results confirmed the efficacy of M/LST-Lip/PTX-PEG 5% in tumor targeting, collagen inhibition in TME, and enhanced tumor penetration. This novel drug delivery system can therefore play a substantial role in improving the therapeutic efficacy of antitumor drugs combined with TME-improving agents.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Qingshan Zhao,Xiaojie Tan,Tengfei Liu,Shuai Hou,Wanxin Ni,Hao Huang,Jinqiang Zhang,Zhongxue Yang,Dawei Li,Han Hu,Mingbo Wu
Heteroatom-doped carbon materials have been regarded as sustainable alternatives to the noble-metal catalysts for oxygen reduction reaction (ORR), while the catalytic performances still remain unsatisfactory. Herein, we develop a metal-free adjacent N, P and S-codoped hierarchical porous carbon nanoshells (NPS-HPCNs) through a novel layer-by-layer template coating method. The NPS-HPCNs is rationally fabricated by crosslinking of polyethyenemine (PEI) and phytic acid (PA) on nano-SiO 2 template surface and subsequently coating of viscous sulfur-bearing petroleum pitch, followed by pyrolysis and alkaline etching. Soft X-ray absorption near-edge spectroscopy (XANES) analysis and density functional theory (DFT) calculations prove the engineering of adjacent N, P and S atoms to generate synergistic and reinforced active sites for oxygen electrocatalysis. The NPS-HPCNs manifests excellent ORR activity with a half-wave potential (E 1/2 ) of 0.86 V, as well as promoted durability and methanol tolerance in alkaline medium. Remarkably, the NPS-HPCNs-based Zn-air battery delivers an open-circuit voltage of 1.479 V, a considerable peak power density of 206 mW cm −2 and robust cycling stability (over 200 h), even exceeding the commercial Pt/C catalyst. This study offers fundamental insights into the construction and synergistic mechanism of adjacent heteroatoms on carbon substrate, providing advanced metal-free electrocatalysts for Zn-air batteries and other energy conversion and storage devices.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Limin Duan,Huihao Jiang,Wenhao Wu,Daohui Lin,Kun Yang
Introducing crystal defects into iron based metal-organic frameworks (Fe-MOFs) is regarded as a promising strategy to enhance Fenton-like performance. However, developing a facile and effective strategy to construct defective Fe-MOFs as highly efficient Fenton-like catalyst is still a challenge. Herein, MIL-100(Fe) (Def-MIL-100(Fe)) with missing ligands defects was synthesized by a simple heterogeneous reaction using zero-valent iron. The bisphenol A degradation efficiency in the Def-MIL-100(Fe)/H 2 O 2 system reached up to 91.26% within 10 min at pH 4 with a low catalyst dosage of 0.05 g/L, while the perfect MIL-100(Fe) has almost no Fenton-like performance. It was observed that missing ligands defects in the Def-MIL-100(Fe) play a key role in the Fenton-like reaction. The missing ligands defects could increase the Lewis acidity for fast H 2 O 2 adsorption and accelerate the electron transfer between Fe II and Fe III cycling, leading to faster and more·OH generation. Moreover, the missing ligands defects could promote the mass transfer for improving·OH utilization efficiency. This work provides a novel strategy to construct defective Fe-MOFs as highly efficient Fenton-like catalyst to degrade organic pollutants in water.
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Advanced Materials Technologies
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2022
·Vol. 8
·期 5
·2201559
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IF 8.856
Qingli Qu,Weixia Cheng,Xiaoli Zhang,Hossein Ravanbakhsh,Guosheng Tang,Aying Zhou,Dong Pei,Ranhua Xiong,Chaobo Huang
Enzymatic cascade reactions are essential for metabolic pathway and biological signal transduction in living cells. More and more attention has been paid to artificial microreactors, which mimic these efficient, methodical, and selective biological cascade catalytic systems in cells. Natural hydrogels such as alginate and chitosan are thought of as suitable materials for matching the chemical, physical, and mechanical properties with extracellular matrix. Inspired by the structures of eukaryotic cells, alginate/chitosan multicompartment microcapsules for enzymatic cascade reaction are developed using an oil-free gas-shearing method. Multiple enzymes as biocatalysts are encapsulated in the particles to resemble complex physiological reactions. Biocatalysts, including glucose oxidase and peroxidase in alginate Janus core as a model, sense the external hyperglycemic environment, resulting in insulin release following chitosan shell protonation. The microcapsules show an excellent recyclability, room-temperature long-term and anti-proteolysis stability. The microreactor approach leads to the development of a multi-enzymatic cascade reaction system and provides an ideal carbohydrate platform to further understand the biomimetic metabolic function of organelles and organs.
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Inorganics
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2022
·Vol. 10
·期 11
·202
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IF 3.149
Liang Qin,Fenglan Liang,Yan Li,Jiana Wu,Shiyuan Guan,Meiyin Wu,Shiling Xie,Manshi Luo,Deyun Ma
A hydrostable 2D Zn-based MOF, {[Zn(5-PIA)(imbm)]·2H2O}n(1) (5-H2PIA = 5-propoxy-isophthalic acid, imbm = 1,4-di(1H-imidazol-1-yl)benzene), was synthesized and structurally characterized. Complex1shows good water and thermal stability based on the TGA and PXRD analyses and displays a 2D framework with 1D channels of 4.8 × 13.8 and 10.0 × 8.3 Å2along theaaxis. The 5-fluorouracil (5-FU) payload in activated complex1(complex1a) is 19.3 wt%, and the cumulative release value of 5-FU at 120 h was about 70.04% in PBS (pH 7.4) at 310 K. In vitro MTT assays did not reveal any cytotoxic effect of NIH-3T3 and HEK-293 cells when the concentration of1was below 500 μg/mL and 5 μg/mL, respectively. No morphological abnormalities were observed on zebrafish exposed to complex1.Keywords:zinc-organic framework;drug delivery;5-fluorouracil;MTT assays;zebrafish toxicity
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JOURNAL OF POLYMER SCIENCE
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2022
·Vol. 61
·期 4
·346-354
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IF 3.046
Die Li,Mei Hong,Yan Wang,Chunyang Bao,Xiaoling Xu,Jing Chen,Bin Peng,Jingyu Zhang,Bingyu Wang,Qiang Zhang
Porous carbon nanospheres have attracted extensive attention due to their excellent advantages in specific surface area, pore distribution, and electronic conductivity. Herein, boron-doped hollow carbon nanospheres with mesoporous walls have been successfully synthesized via a combination of hard/soft templating and boronic acid/sugar ligation. Surface-initiated Cu(0) mediated reversible deactivation radical polymerization was used to initiate the polymerization of 2-hydroxyethyl acrylate and poly(ethylene glycol) methyl ether acrylate from the surface of silica. 4-carboxy-3-fluorophenylboronic acid was introduced as a boron precursor by N -(3-dimethylaminopropyl)- N ′-ethylcarbodiimide hydrochloride coupling and fructose was introduced as a carbon precursor by boronic esters. After carbonization and template etching, boron-doped porous carbon spheres could be obtained. We believe such in-situ heteroatom-doped method has great potential in preparing hollow mesoporous carbon nanospheres with excellent properties. Graphical
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Kexuan Gao,Li-an Hou,Xiaoqiang An,Doudou Huang,Yu Yang
The rapid recombination rate of photogenerated charges make the rational design of high-performance stable photocatalysts challenging. Herein, the features of heterojunctions, oxygen vacancies (OVs), and MXene quantum dots (MQDs) were simultaneously collected in CBM (gC 3 N 4 /BiOBr/MXene) using a simple solvothermal method for the first time. OVs promoted the chemisorption of O 2 , MQDs not only accelerated electron transport but also promoted a photogenerated charge to selectively generate singlet oxygen, 99% of the tetracycline hydrochloride (TC-HCl) was degraded by CBM within 30 min under visible light irradiation. Thirteen intermediates and possible photocatalytic degradation pathways were proposed. It was discovered that CBM is nontoxic to the environment but can swiftly produce an excellent antibacterial effect when exposed to visible light irradiation. This research provides fresh insights into the effective removal of organic pollutants from water by combining cutting-edge defect engineering and quantum dot doping technology in photocatalytic heterojunctions.
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Genes & Genomics
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2022
·Vol. 45
·期 1
·1-11
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IF 2.164
Cao Qingfei,Ma Jiaji,Li Weitao,Hong Peng,Shen Tong,Tong Ming
Background Guanine nucleotide-binding protein 2 (GNBP2) is a GTPase that has critical roles in host immunity and some types of cancer, but its function in clear cell renal cell carcinoma (ccRCC) is not fully understood. Objective This work explored the role of GNBP2 in ccRCC progression and the underlying molecular mechanism. Methods Two public human cancer databases TNMplot and TISIDB were employed to analyze the expression pattern of GNBP2 during ccRCC progression and the correlation between GNBP2 expression and clinical features of ccRCC patients. GNBP2 functions in ccRCC cells were determined by EdU staining, flow cytometry, scratch wound assay, transwell assay, and xenograft model. Gene expression was evaluated using qPCR, Western blot, immunofluorescence staining, and immunohistochemical staining. Results GNBP2 expression was significantly elevated in ccRCC tissues and increased gradually with the increasing tumor grades. Patients with higher GNBP2 expression had shorter overall survival times. Knockdown of GNBP2 suppressed tumor cell proliferation and cell cycle progression and reduced the capability of migration and invasion, while GNBP2 overexpression exhibited protumor effects. GNBP2 silencing by RNA interference significantly inhibited the tumor growth of tumor-bearing nude mice and decreased the proliferation marker Ki67. Mechanistically, GNBP2 downregulation suppressed the STAT3 signaling transduction, as it reduced the phosphorylation of STAT3 and modulated the expression of the target genes, including c-Myc, MMP2, N-cadherin, and E-cadherin. Conclusion These findings reveal that GNBP2 promotes ccRCC progression by regulating STAT3 signaling transduction, indicating that GNBP2 might be a promising molecular target for ccRCC therapy.
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Biomaterials Research
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2022
·Vol. 26
·期 1
·1-20
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IF 15.863
Luan Zhaohui,Liu Shuang,Wang Wei,Xu Kaige,Ye Shaosong,Dan Ruijue,Zhang Hong,Shu Zhenzhen,Wang Tongchuan,Fan Chaoqiang,Xing Malcolm,Yang Shiming
Background Wound closure in the complex body environment places higher requirements on suture’s mechanical and biological performance. In the scenario of frequent mechanical gastric motility and extremely low pH, single functional sutures have limitations in dealing with stomach bleeding trauma where the normal healing will get deteriorated in acid. It necessitates to advance suture, which can regulate wounds, resist acid and intelligently sense stomach pH. Methods Based on fish swim bladder, a double-stranded drug-loaded suture was fabricated. Its cytotoxicity, histocompatibility, mechanical properties, acid resistance and multiple functions were verified. Also, suture’s performance suturing gastric wounds and Achilles tendon was verified in an in vivo model. Results By investigating the swim bladder’s multi-scale structure, the aligned tough collagen fibrous membrane can resist high hydrostatic pressure. We report that the multi-functional sutures on the twisted and aligned collagen fibers have acid resistance and low tissue reaction. Working with an implantable “capsule robot”, the smart suture can inhibit gastric acid secretion, curb the prolonged stomach bleeding and monitor real-time pH changes in rabbits and pigs. The suture can promote stomach healing and is strong enough to stitch the fractured Achilles tendon. Conclusions As a drug-loaded absorbable suture, the suture shows excellent performance and good application prospect in clinical work.
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Antioxidants
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2022
·Vol. 11
·期 9
·1831
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IF 7.675
Xue Lin,Yousheng Shi,Pan Wen,Xiaoping Hu,Lu Wang
Free, conjugated, and bound phenolic fractions of peel and pulp in four wampee varieties from South China were analyzed for their contents, composition, antioxidant capacities, and inhibitory activities againstα-glucosidase. We found that there were significant differences in phenolic/flavonoid contents among diverse varieties and different parts (peel and pulp), and the contents were highest in the peel’s bound form. The results of UHPL-Q-Exactive HF-X and HPLC showed that chlorogenic acid, gentisic acid, and rutin were abundantly distributed over the three phenolic fractions in peel and pulp of all wampee samples, while isoquercitrin was the most abundant in the conjugated form of peel/pulp and myricetin had the richest content in the free form of peel/pulp. Wampee peel had stronger antioxidant capacities of ABTS+, DPPH, ·OH, and FRAP than the pulp, and the bound phenolic fraction of the peel/pulp had much higher antioxidant activities than FP and CP fractions. It is interesting that the same phenolic fraction of the wampee peel displayed roughly close IC50values ofα-glucosidase inhibition to those from the pulp samples. The relationship between individual phenolic and TPC/TFC/the bio-activities and the similarity among the free, conjugated, and bound phenolic fractions in peel and pulp samples were explored by using Pearson correlation analysis, principal component analysis, and hierarchical cluster analysis. This work provides a systematic and comprehensive comparison of the three phenolic fractions of diverse wampee varieties and different parts, and a rationale for applying phenolics from wampee fruits.Keywords:wampee varieties;free phenolic;conjugated phenolic;bound phenolic;antioxidant capacities;inhibitory activity againstα-glucosidase;multivariate analysis
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