Scientific Reports
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2019
·Vol. 9
·期 1
·1-13
·
IF 4.011
Huang Yifeng,Ma Yongwen,Wan Jinquan,Wang Yan
In this study, the hydrodynamic characteristic of a lab-scale internal circulation (IC) anaerobic reactor was investigated. We found that the gradual Increasing-Size Continuous Stirred-Tank Reactors (ISC) model is desirable to describe the hydraulic character of the reactor. As a generalized anaerobic digestion model, Anaerobic Digestion Model No.1 (ADM1) was combined simultaneously with the ISC model to simulate the effluent of the IC reactor. Both the stable running and overloading shock tests were carried out to validate the simulation. The mathematical simulation results agreed well with the experimental observation. This proposed model may be valuable to simulate the performance of the IC reactor effectively and to supply a useful tool to for designing and operating other anaerobic reactors.
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NANO
·
2019
·
IF 1.293
Qian Sun,Chun Zeng,Meng-Meng Xing,Bo Chen,Dan Zhao,San-Guo Hong,Ning Zhang
Deliberately engineering oxide composites on constructing and manipulating interactive structures particularly in surface layers was highly desirable for heterogeneous catalysis. Herein, upon the redox replacement reaction between Ce(IV) precursor (Ce(NO 3 ) 6 2 − ) and Cu 2 O nano-substrate, an attempt to directly engineer the surface structure of Cu-based substrate was performed by the Ce(IV)–Cu 2 O etching-embedding process, then the obtained powders were thermo-treated to get a series of Ce–O–Cu catalysts with different Ce:Cu molar ratios for NH 3 selective catalytic reduction (NH 3 -SCR) of NO. Characterized by ICP-OES, XRD, Raman, XPS, SEM, BET, H 2 -TPR, NO- and NH 3 -TPD measurements, it was demonstrated that the Cu–O–Ce catalysts were structured as CuO matrix with an interactive surface composed by co-present Cu(I)–Cu(II) and Ce(III)–Ce(IV) species, even the introduction of Ce was confined in a quite low loading range (0.83–2.3 wt.%); such a surface exhibited the distinct synergistic effect with positively manipulated physical-chemistry properties such as active site distributions, redox features and surface reactivity compared to pure CuO and traditional Cu–Ce composite catalyst, leading to attractive catalytic performance such as ≥ 9 0 % NO conversion with ≥ 9 5 % N 2 selectivity and the two-fold TOF enhancement versus traditional catalysts, even SO 2 was present in reactant mixture on well-manipulated catalyst (Ce loading at 1.6 wt.%) These results indicated that the etching-embedding strategy illuminated in this work could be referred as a feasible method to directly engineer and construct interactive oxide composite surface for advanced application as well as current efficient Ce–O–Cu catalytic interface for heterogeneous catalysis.
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ACS Applied Materials & Interfaces
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2018
·
IF 8.097
Lin Hou,Yinling Zhang,Xuemei Yang,Chunyu Tian,Yingshan Yan,Hongling Zhang,Jinjin Shi,Huijuan Zhang,Zhenzhong Zhang
Nitric oxide (NO) is an important biological messenger implicated in tumor therapy. However, current NO release systems suffer from some disadvantages, such as hydrolysis during blood circulation, poor specificity, and robust irradiation for stimuli. Accordingly, we constructed an intracellular enzyme-triggered NO-generator to achieve tumor cytoplasm-specific disruption and localized rapid drug release. Diethylamine NONOate (DEA/NO) was used as a NO donor and conjugated with hyaluronic acid (HA) to form self-assembly micelle (HA-DNB-DEA/NO), and encapsulate chemotherapeutic agent (doxorubicin (DOX)) into its hydrophobic core (DOX@HA-DNB-DEA/NO). After HA receptor mediated internalization into tumor cells, HA shell would undergo digestion into small conjugated pieces by hyaluronidase. Meanwhile, DOX@HA-DNB-DEA/NO also responded to the intratumoral overexpressed glutathion and glutathione S-transferase π, leading to the intracellular NO production and controlled DOX rapid release. In vitro and in vivo results proved the enzyme-dependent and enhanced targeting delivery profile, and demonstrated that NO and DOX could colocate in specific tumor site, which provided a precondition for exerting their synergistic efficacy. Moreover, expression of p53 protein was upregulated in tumor tissue after treatment, indicating that NO induced cell apoptosis mediated by tumor suppressor gene p53. Overall, this intelligent drug loaded NO-generator might perform as an enhancer to realize better clinical outcomes.
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INORGANIC CHEMISTRY
·
2018
·
IF 4.7
Qian Peng,J. Timothy Sage,Yulong Liu,Zijian Wang,Michael Y. Hu,Jiyong Zhao,E. Ercan Alp,W. Robert Scheidt,Jianfeng Li
Compared to well studied diatomic ligands (NO, CN–, CO), the axial bonds of carbene hemes is much less known although its significance in biological chemistry. The unusually large quadrupole splitting (ΔEQ = +2.2 mm·s–1) and asymmetric parameter (η = 0.9) of the five-coordinate heme carbene [Fe(TTP)(CCl2)], which is the largest among all known low spin ferrohemes, has driven investigations by means of Mössbauer effect Nuclear Resonance Vibrational Spectroscopy (NRVS). Three distinct measurements on one single crystal (two in-plane and one out-of-plane) have demonstrated comprehensive vibrational structures including stretch (429) and bending modes (472 cm–1) of the axial Fe–CCl2, and revealed iron vibrational anisotropy in three orthogonal directions for the first time. Frontier orbital analysis especially comparisons with diatomic analogues (NO, CN–, CO) suggest that CCl2, similar to NO, has led to strong but anisotropic π bonding in a ligand-based “4C”-coordinate which induced the vibrational anisotropies and very large Mössbauer parameters. This is contrasted to CN– and CO complexes which possess a porphyrin-based “4N”-coordinate electronic and vibrational structures due to inherent on-axis linear ligation.
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Nanoscale
·
2018
·Vol. 11
·期 9
·3814-3826
·
IF 7.233
Mingmao Chen,Feifei Song,Yan Liu,Jia Tian,Chun Liu,Ruyue Li,Qiqing Zhang
In cancer therapy, chemotherapeutic drugs frequently encounter multidrug resistance (MDR) induced by the overexpression of drug transporters such as P-glycoprotein (P-gp). Herein, in order to overcome MDR and improve the effectiveness of chemotherapy, we developed a novel pH-sensitive charge-reversal and NO generation liposomal system by modifying a pH-sensitive polymer (PEG-PLL-DMA) on the surface of cationic liposomes for delivering a NO donor (DETA NONOate) and a chemotherapy drug (paclitaxel, PTX) into MDR cells. The proposed liposomal system (PTX/NO/DMA-L) exhibited a distinctive charge-reversal capacity, which was negatively charged under physiological conditions (pH 7.4) but could reverse to positive charge in a tumor microenvironment (pH 6.5) due to the cleavable amide linkages formed between PEG-PLL and DMA, leading to the improvement of cell uptake. Once arrived in the endosomes and lysosomes (pH 5.0), DETA NONOate was triggered to decompose and release NO, which further promoted the quick release of PTX and inhibited the P-gp mediated efflux. The charge-reversal, NO generation and NO-triggered rapid release of drugs could significantly increase the accumulation of PTX in tumors and eventually improve the antitumor efficacy. These results indicate that this dual pH-sensitive liposomal system is a highly promising approach for chemotherapy and may pave a new avenue for overcoming MDR in cancer.
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SENSORS AND ACTUATORS B-CHEMICAL
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2015
·
IF 4.097
Han Jin,Youju Huang,Jiawen Jian
Plate-like Cr 2 O 3 has been proved to be highly selective in sensing of nitric oxide (NO), while the sensing response of irregular shape and cubic-like Cr 2 O 3 toward NO was significantly interfered by hydrocarbons (HCs), e.g. C 3 H 6 . In this paper, sensing mechanism of the plate-like Cr 2 O 3 for selective sensing of NO (against HCs) was studied via crystallographic phase analysis, lattice fringes investigation and evaluation of the catalytic activity (gas-phase catalytic activity & electrochemical catalytic activity). The Cr 2 O 3 samples with plate-like, irregular shape and cubic-like microstructures have been confirmed to be the same crystallographic phase through XRD measurements, however, significant difference in the lattice fringes of these Cr 2 O 3 samples were observed via high-resolution transmission electron microscopy (HRTEM) & selected-area electron diffraction (SAED). The comparison results of catalytic activity for plate-like, irregular shape and cubic-like Cr 2 O 3 indicated that the unique selectivity for the plate-like Cr 2 O 3 was mainly caused by the electrochemical reaction specifically toward NO, which occurred near the interface between plate-like Cr 2 O 3 and zirconia-based electrolyte.
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Small
·
2014
·Vol. 10
·期 18
·3750-3760
·
IF 7.514
Jiangsheng Xu,Fang Zeng,Hao Wu,Caiping Hu,Changmin Yu,Shuizhu Wu
The therapeutic applications of exogenous nitric oxide are usually limited by its short half-life and its vulnerability to many biological substances, thus straightforward and precise spatiotemporal control of NO delivery may be critical to its therapeutic effects. Herein, the mitochondria-targeted and photoresponsive NO-releasing nanosystem is demonstrated as a new approach for cancer treatment. The nanosystem is fabricated by covalently incorporating a NO photo-donor and a mitochondria targeting ligand onto carbon-dots; accordingly, multi-functionalities (mitochondria-targeting, light-enhanced efficient NO-releasing, and cell imaging) are achieved. The in vitro NO release profiles for the nanosystem show that the duration of NO release from the present C-dot-based nanosystem containing immobilized SNO can be extended up to 8 hours or more. Upon cellular internalization, the nanosystem can target mitochondria and release NO. The action of the nanosystem on three cancer cell lines is evaluated; it is found that the targeted NO-releasing system can cause high cytotoxicity towards the cancer cells by specifically damaging their mitochondria. Additionally, light irradiation can amplify the cell apoptosis by enhancing NO release. These observations demonstrate that incorporating mitochondria-targeting ligand onto a NO-releasing system can enhance its pro-apoptosis action, thereby providing new insights for exploiting NO in cancer therapy.
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APPLIED CATALYSIS A-GENERAL
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2017
·
IF 4.339
Baohuai Zhao,Rui Ran,Xingguo Guo,Li Cao,Tengfei Xu,Ze Chen,Xiaodong Wu,Zhichun Si,Duan Weng
Mn/Ce/Ti and Mn/Ce/Nb/Ti catalysts were synthesized using a precipitation method and their catalytic activities for NO selective reduction with NH 3 at low temperatures were evaluated. Nb doping not only improved the activity of the catalyst over a wide temperature range but also restricted the generation of NO 2 and N 2 O. The Mn/Ce/Nb/Ti catalyst displayed 100% NO conversion from 150 to 250 °C and >90% N 2 selectivity below 250 °C. The specific surface area of the catalyst was increased and its surface acidity was strengthened after Nb doping. Moreover, Nb doping increased the NO oxidation ability and lowered the NH 3 oxidation activity of the catalyst. All the above factors contributed to enhancing the overall NH 3 -SCR performance of the Mn/Ce/Nb/Ti catalyst compared with that of the Mn/Ce/Ti one. The long-term stability and resistance to H 2 O and SO 2 of the Mn/Ce/Nb/Ti catalyst were also evaluated.
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RSC Advances
·
2016
·Vol. 6
·期 74
·69855-69860
·
IF 3.289
Baohuai Zhao,Rui Ran,Li Sun,Xingguo Guo,Xiaodong Wu,Duan Weng
The perovskite oxides LaMnO3+δ were prepared by a citrate method and then etched by acid solution with different times. After etching, the perovskite structures of all the catalysts remained, the surface area enlarged apparently, and the NO catalytic oxidation activities were obviously promoted by increasing the etching time. Long-term experiments revealed the acceptable stability of the etched catalysts. The favorable activities of the etched LaMnO3+δ catalysts were mainly due to their high specific surface area, abundant activated oxygen species and vacancies, as well as the higher valence state of Mn ions resulting from the loss of La3+ in the perovskite structure.
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APPLIED SURFACE SCIENCE
·
2016
·
IF 3.15
Huihui Li,Xiaoyong Wu,Shu Yin,Kenichi Katsumata,Yuhua Wang
Novel g-C 3 N 4 /rutile-brookite TiO 2-x N y composite photocatalysts were fabricated through a facile solvothermal approach. The effect of rutile phase TiO 2 with brookite TiO 2 and g-C 3 N 4 on the photocatalytic activity of g-C 3 N 4 /nitrogen-doped TiO 2 composite was studied. The photocatalytic performance of the photocatalyst was evaluated by measuring the degradation of NO gas under visible and UV light irradiation. It is suggested that g-C 3 N 4 /rutile-brookite TiO 2-x N y forms a Z-scheme photocatalytic system, which shows improvement on the photocatalytic activity than that of g-C 3 N 4 /single brookite TiO 2-x N y . By importing rutile phase TiO 2-x N y , the photogenerated electrons can efficiently transfer from rutile TiO 2 to g-C 3 N 4 , which results in the separation of electron and hole pairs, enhancing the photocatalytic ability. However, single brookite TiO 2-x N y can not remove the photogenerated electrons efficiently and the photocatalytic performances of composites decrease with g-C 3 N 4 amount increase.
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JOURNAL OF MEDICINAL CHEMISTRY
·
2024
·
IF 6.8
Lie-Feng Ma,Li−Li Xu,Ling-Jie Yuan,Xi Yang,Rui Wu,Shu-Min Bao,Yi-Li Chen,Hong-Liang Duan,Luo Fang,Hua-Jun Zhao,Zha-Jun Zhan
Triple-negative breast cancer (TNBC) is a highly lethal malignancy, and its clinical management encounters severe challenges due to its high metastatic propensity and the absence of effective therapeutic targets. To improve druggability of aurovertin B (AVB), a natural polyketide with a significant antiproliferative effect on TNBC, a series of NO donor/AVB hybrids were synthesized and tested for bioactivities. Among them, compound 4d significantly inhibited the proliferation and metastasis of TNBC in vitro and in vivo with better safety than that of AVB. The structure−activity relationship analysis suggested that the types of NO donor and the linkers had considerable effects on the activities. Mechanistic investigations unveiled that 4d induced apoptosis and ferroptosis by the reduction of mitochondrial membrane potential and the down-regulation of GPX4, respectively. The antimetastatic effect of 4d was associated with the upregulation of DUSP1. Overall, these compelling results underscore the tremendous potential of 4d for treating TNBC.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Yan Ji,Changpeng Zuo,Jie Chen,Qiuyang Zhang,Yuchi Sun,Qingping Xiong,Changjiang Pan
Polyurethanes (PU) is widely applied in the blood-contact biomaterials. However, its biocompatibility still cannot meet the requirements for long-term service. In this work, a polydopamine (PDA) layer was first prepared on the PU surface, and then an anticoagulant polymer with an endothelial glycosaminoglycan-mimicking structure capable of catalyzing the release of nitric oxide (NO) gas molecules 6-arm-poly (ethy1ene glycol)-Heparin-Selenocystamine (PEG-Hep-SeCA) was grafted on the PDA-modified PU surface to construct a bioactive coating with the capacity to catalyze the release of NO from the endogenous donors. The findings indicated that the modified PU surfaces had excellent hydrophilicity, selective albumin adsorption as well as good blood compatibility and endothelial cell growth properties. The hemocompatibility and endothelial cell growth were further significantly improved in the case of catalytic NO generation. Therefore, the surface modification strategy of this study can significantly improve the biocompatibility of PU and thus lay the foundation for future clinical applications of medical polyurethane.
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