ZEITSCHRIFT FUR KRISTALLOGRAPHIE-NEW CRYSTAL STRUCTURES
·
2023
·Vol. 238
·期 3
·541-543
·
IF 0.3
Chuanguo Cui,Jinxiao Zhang,Zhiyin Xiao
C 61 H 50 Cl 2 Fe 2 I 12 N 12 , orthorhombic, Pbcn (no. 60), a = 13.0247(4) Å, b = 17.0204(5) Å, c = 34.1475(9) Å, β = 90, V = 7570.0(4) Å 3 , Z = 4, R gt
( F ) = 0.0694, wR ref
( F
2 ) = 0.1605, T = 293(2) K.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2023
·
IF 3.8
Jinpei Huang,Xingwei Lu,Xuejing Zhang,Yiqiang Jin,Yifeng Zhou
1-Oxa-2-azaspiro [2.5] octane, as one of N-H oxaziridines , is a selective electrophilic aminating agent for N-, S-, C-, and O-nucleophiles. It has the features of stereoselectivity and the absence of formation of strongly acidic or basic byproducts, leading to considerable interest in the development of organic synthetic methods. Currently, the economically feasible route of production of 1-oxa-2-azaspiro [2.5] octane is the reaction of cyclohexanone with ammonia and sodium hypochlorite. However, due to strong exothermic reactions, massive gas release and heterogeneous reaction, the controllability, efficiency and safety of the reaction are in great difficulty using batch technology. In this paper, a microreaction system containing predispersion, reaction and phase separation was introduced into the preparation of 1-oxa-2-azaspiro [2.5] octane. The research results showed that precise control of the process including droplet dispersion, temperature control, reaction time control and fast continuous phase separation, was the key to process intensification. Under optimal conditions, the concentration of 1-oxa-2-azaspiro [2.5] octane in product obtained by microreaciton system (∼2.0 mol·L −1 ) was much higher than that obtained by batch technology (0.2–0.4 mol·L −1 ), which demonstrated that the continuous-flow synthesis would be a more efficient substitute for batch synthesis. Meanwhile, the results of the derivation experiments also showed that the aminating agent solution with higher concentration was more advantageous in the applications.
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Frontiers in Pharmacology
·
2023
·
IF 5.6
Wang Shuai,Bai Jie,Che Yilin,Qu Weikun,Li Jing
Background: Humans with hypertensive heart disease are more likely to experience heart failure, arrhythmia, myocardial infarction, and sudden death, and it is crucial to treat this condition. Fucoidan (FO) is a natural substance derived from marine algae that has antioxidant and immunomodulatory activities. FO has also been shown to regulate apoptosis. However, whether FO can protect against cardiac hypertrophy is unknown.Methods: We investigated the effect of FO in hypertrophic models in vivo and in vitro. C57BL/6 mice were given an oral gavage of FO (300 mg/kg/day) or PBS (internal control) the day before surgery, followed by a 14-day infusion of Ang II or saline. AC-16 cells were treated with si-USP22 for 4 h and then treated with Ang II (100 nM) for 24 h. Systolic blood pressure (SBP) was recorded, echocardiography was used to assess cardiac function, and pathological changes in heart tissues were assessed by histological staining. Apoptosis levels were detected by TUNEL assays. The mRNA level of genes was assessed by qPCR. Protein expression was detected by immunoblotting.Results: Our data showed that USP22 expression was lowered in Ang II-infused animals and cells, which could promote cardiac dysfunction and remodeling. However, treatment with FO significantly upregulated the expression of USP22 and reduced the incidence of cardiac hypertrophy, fibrosis, inflammation, and oxidative responses. Additionally, FO treatment lowered p53 expression and apoptosis while increasing Sirt 1 and Bcl-2 expression.Conclusion: By reducing the level of Ang II-induced apoptosis through the regulation of USP22/Sirt 1 expression, FO treatment might improve cardiac function. According to this study, FO might be potential targeted approach for treating heart failure.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Zening Huang,Kaixiang Xu,Lijuan Zhao,Li-e Zheng,Nana Xu,Caixia Yan,Xingjiang Hu,Qiao Zhang,Jian Liu,Qingwei Zhao,Yaokun Xia
The development of a strategy for imaging of glutathione (GSH) and apurinic/apyrimidinic endonuclease 1 (APE1) in an organism remains challenging despite their significance in elaborating the correlated pathophysiological processes. Therefore, in this study, we propose a DNA-based AND-gated nanosensor for fluorescence imaging of the GSH as well as APE1 in living cells, animals, and organoids. The DNA probe is composed of a G-strand and A-strand. The disulfide bond in the G-strand is cleaved through a GSH redox reaction, and the hybridization stability between the G-strand and A-strand is decreased, leading to a conformational change of the A-strand. In the presence of APE1, the apurinic/apyrimidinic (AP) site in the A-strand is digested, producing a fluorescence signal for the correlated imaging of GSH and APE1. This nanosensor enables monitoring of the expression level change of GSH and APE1 in cells. Additionally, we illustrate the capability of this “dual-keys-and-locked” conceptual methodology in achieving specific tumor imaging when GSH and APE1 are present simultaneously (overexpressed GSH and APE1 in tumor cells) with improving tumor-to-normal tissue ratio in vivo. Furthermore, using this nanosensor, the GSH and APE1 also are visualized in organoids that recapitulate the phenotypic and functional traits of the original biological specimens. Overall, this study demonstrates the potential of our proposed biosensing technology in investigating the roles of various biological molecules involved in specific diseases.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
He Huang,Huahua Fan,Yuzhen Ge,Wanyue Ye,Yingcen Liu,Caicheng Song,Hua Lin,Xiaotong Zhang,Bing Li,Xiaowa Nie,Shufen Zhang,Rongwen Lu
The selective oxidation of the primary C H bonds in hydrocarbons to corresponding high-valued oxygenates is highly desired but challenging to realize. The difficulty arises from the high homolytic bond dissociation enthalpy of the C H bond, the relatively high reactivity of oxygenated intermediates, and the diversity of resultant products. Herein, we reported the in situ confinement of Au clusters in Silicalite-1 for the selective solvent-free oxidation of toluene to benzaldehyde. The doping of an alkali metal (K or Na) resulted in the formation of electron-rich Au species, which readily facilitate the activation of oxygen, In turn, toluene is activated by the produced reactive oxygen species in a single step, as confirmed through density functional theory (DFT) calculations. At optimal alkali metal doping, the selectivity to benzaldehyde could reach > 90 %, with the toluene conversion being 19.8 %. Remarkably, the total turnover number (TTN) of Au@Silicalite-1–0.2 K was found to be 29,658, which is one or two orders of magnitudes higher than the previously reported values. These findings are expected to inspire the design of highly efficient catalysts for the activation of fundamental feedstock with C H bonds.
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Journal of Energy Chemistry
·
2023
·
IF 13.1
Zhongying Fang,Ziwei Zhang,Shemsu Ligani Fereja,Jinhan Guo,Xinjie Tong,Yue Zheng,Rupeng Liu,Xiaolong Liang,Leting Zhang,Zongjun Li,Wei Chen
Direct formic acid fuel cell (DFAFC) is an important research project in clean energy field. However, commercialization of DFAFC is still largely limited by the available catalysts with unsatisfied activity, durability and cost for formic acid electrooxidation (FAEO). Using Pt- and Pd-based nanoclusters as electrocatalysts is a particularly promising strategy to solve the above problem, but two attendant problems need to be solved firstly. (I) The controllable synthesis of practicable and stable sub-2 nm clusters remains challenging. (II) The catalyzing mechanism of sub-2 nm metal clusters for FAEO has not yet completely understood. Herein, different from traditional solution synthesis, by designing a novel supporting material containing electron-rich and electron-deficient functional groups, size- and dispersion-controllable synthesis of ∼1 nm PtPd nanoclusters is realized by an electrochemical process. The electrocatalytic properties and reaction mechanism of the PtPd nanoclusters for the FAEO were studied by different electrochemical techniques, in-situ fourier transform infrared (FTIR) spectra and density functional theory (DFT) calculations. The tiny PtPd nanoclusters have much higher catalytic activity and durability than commercial Pt/C, Pd/C and 3.5 nm PtPd nanoparticles. The present study shows that the metal-reactant interaction plays a decisive role in determining the catalytic activity and cluster-support interaction plays a decisive role in enhancing the durability of electrocatalyst. The ratio and arrangement of Pt and Pd atoms on the surface of 1 nm PtPd cluster as well as the overall valence state, d-band center and specific surface area make them exhibit different catalytic performance and reaction mechanism from nanoparticle catalysts. In addition, in situ FTIR and DFT calculations showed that on the surface of PtPd clusters, the generation of CO 2 through trans-COOH intermediate is the most optimal reaction pathway for the FAEO.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Haike Li,Lijinhong Huang,Xindong Li,Wanfu Huang,Lang Li,Wenhao Li,Meng Cai,Zhaohuang Zhong
This study aimed to further enhance the solvent stability and flux of organic solvent-resistant nanofiltration (OSN) membranes. Based on hexane diamine cross-linked polyetherimide (PEI) ultrafiltration membranes, in-situ calcium alginate (CaAlg) hydrogel doped with HKUST-1 was constructed as an interlayer, and then the OSN membrane with an integral covalent bond structure was constructed from interfacial polymerization reaction and N N dimethylformamide (DMF) activation. The membrane showed ultra-thinness (polyamide (PA) layer thickness reduced from 97 to 11 nm), large surface area (surface roughness increased from 75.6 to 113 nm), high hydrophilicity (water contact angle reduced from 60.1° to 54.45°), and negative charge. The CaAlg-HKUST-1 interlayer limited the piperazine diffusion rate by hydrogen bonding and covalent bonding, etc., reduced the thickness of the PA layer, and linked the base membrane and the PA layer by its internal integral covalent bonding, which effectively enhanced the structural stability of the OSN membrane. The PA/CaAlg-HKUST-1 6 /PEI membrane achieved a flux of 29.4 L·m −2 ·h −1 in ethanol and a rejection of 94.7 % in 0.1 g·L -1 methyl blue. Different dye rejection tests, solvent flux tests, DMF and acetone immersion tests, fouling resistance tests, and continuous operation tests show PA/CaAlg-HKUST-1 6 /PEI membrane has better solvent resistance, dye separation performance, and stable membrane flux. Hence, it has great application prospects in the fields of organic solvents and other types of wastewater treatment.
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Molecular Catalysis
·
2023
·
IF 4.6
Xiuqin Dong,Chen Xin,Lingtao Wang,Hao Gong,Yifei Chen
Immobilization of the Rh active sites in novel porous materials has attracted attentions for solving the problems of separation and recycling of homogeneous catalysts. In this work, a comparative study of phosphine modified 1Rh/MOF-5 using three different methods was reported, namely 1Rh-P/MOF-5, 1Rh/MOF-5-P and 1Rh/MOF-5-PPh 3 . Similar with the traditional methods, PPh 3 was etched on Rh particles by impregnation in 1Rh-P/MOF-5 and encapsulated in the pores by solvothermal method in 1Rh/MOF-5-P. Moreover, we proposed a novel post-synthesis strategy for grafting phenyl phosphine on the organic linkers in 1Rh/MOF-5-PPh 3. The position of phenyl phosphine in MOFs and the effect of phosphine on the Rh active sites in hydroformylation were investigated by XRD, IR, XPS, TGA and DRIFTS. 1Rh/MOF-5-PPh 3 exhibited the best catalytic activity and stability than 1Rh-P/MOF-5 and 1Rh/MOF-5-P in the hydroformylation of 1-butene. Different P/Rh ratio in P-modified 1Rh/MOF-5 led to the spatial environment change around the Rh active sites. This study showed details in the role of phosphine ligands played in hydroformylation reactions and provided some guidance for MOFs materials in the immobilization of homogeneous catalysts.
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RSC Advances
·
2022
·Vol. 12
·期 53
·34208-34216
·
IF 4.036
Yilan Zhang,Xiaoguang Ying,Bo Liu,Bo Yang,Xiao Li
Nanofiber membranes have recently been considered as promising supports for the immobilization of microorganisms due to the simplicity and cost-effectiveness of electrostatic spinning technology and the ability to control fiber morphology, such as obtaining higher surface area and porosity. In this study, electrospun polyvinyl alcohol/sodium alginate/attapulgite (PVA/SA/ATP) nanofiber membrane was prepared as support for immobilized Bacillus cereus LY-1 for diesel degradation in an aqueous medium and a significant improvement in diesel removal efficiency was realized. The effect of modified ATP concentration on diesel removal was investigated. The results showed that the nanofiber membranes complexed with cetyl trimethyl ammonium bromide (CTAB) and 1% ATP (w/w) had the best capacity for diesel removing. When the initial diesel concentration was 2 g L−1, about 87.8% of diesel was removed by the immobilized LY-1 cells after 72 h. Immobilization of bacteria improves the ability of bacteria to survive in adverse environments. Immobilized LY-1 cells maintain the nature to remove diesel at high salinity or pH range of 6–9. Furthermore, the reusability of the LY-1 cells-immobilized PVA/SA/CTAB–ATP nanofiber membrane was tested. A diesel removal rate of 64.9% could be achieved after 4 times of use. PVA/SA/CTAB–ATP nanofibrous membranes with immobilized LY-1 cells are feasible, economical and environmentally friendly for remediation of diesel contamination in the aqueous medium, and have potential applications in the future.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 12
·127515
·
IF 4.386
Wenrui Zhao,Beibei Wang,Xueping Ji,Kai Kang,Bing Wang,Lin Wang,Jujie Ren
Herein, a novel electrochemiluminescence (ECL) sensor was developed using a dual signal amplification mechanism based on a typical HKUST-1 metal-organic framework, [Cu3(BTC)2(H2O)3, BTC=1,3,5-benzene tricarboxylate], CdS quantum dots (QDs) and multi-walled carbon nanotubes (MWCNTs) for ultrasensitive determination of catechol. HKUST-1 not only has a dispersion effect to carry more CdS QDs for enhancing stability, but also acts as effective catalyzer to accelerate the transformation of persulfate ion (S2O82−) for generating more sulfate radical anions (SO4•−), therefore amplifying the signal of the ECL sensor. Meanwhile, the introduction of MWCNTs to the ECL process could promote the electron transfer rate and accelerate the kinetics of the electro-catalytic reaction attributing to its stronger conductivity, achieving dual-amplifying effect, which could obviously increase the sensitivity of the ECL sensor. The proposed sensor displayed a wide linear range of 1 × 10−7 − 1 × 10−3 M and a low detection limit of 3.8 × 10−8 M with excellent stability, high repeatability and outstanding anti-interference ability under the optimal conditions. Impressively, the sensor possessed commendable feedback when detecting catechol in real samples. Therefore, this research provided a new strategy combining the advantages of MOFs, QDs and MWCNTs materials for phenolic pollutants detection.
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FUEL PROCESSING TECHNOLOGY
·
2023
·
IF 7.5
Luoming Kang,Airong Li,Yuan Lu,Yuling Ma,Cheng Wang
Mercaptans as volatile organic sulfur compounds would cause environmental pollution. Researches are focused on the removal of mercaptans by solvent absorption method. In this work, a new efficient absorbent of 1-butyl-3-methylimidazolyl alanine ([Bmim]Ala) was prepared and evaluated by the removal of mercaptans from the model gas containing methyl mercaptan (MeSH, 307.6 mg/m 3 ), ethyl mercaptan (EtSH, 201.1 mg/m 3 ) and propyl mercaptan (PrSH, 149.9 mg/m 3 ) in nitrogen. The results showed that the removal rate of MeSH, EtSH and PrSH was 97.77, 98.12 and 100.00%, respectively, at a temperature of 35 °C and a pressure of 1.00 bar for 2 min. After 6 recycling times, [Bmim]Ala remained a good performance for the removal of mercaptans. The desulfurization mechanism was proposed that the absorption sites were mainly on the alanine anion (Ala − ) and Ala − could be replaced by the thiol anion (RS − ) to form a new ionic liquid 1-butyl-3-methylimidazolyl thiolate ([Bmim] + RS − ). Meanwhile, since the electrostatic interaction between -COO − in Ala − and H -g on the imidazolium cation could be destroyed by the -SH group, the -COO − group would interact with mercaptans to form a strong H-bond. The amino in Ala − and the -SH group could form Lewis acid-base compounds.
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SYNTHETIC COMMUNICATIONS
·
2023
·
IF 2.1
Jun Yang,Guang-Ping Liang,Xiong-Li Liu
To investigate the effects and mechanisms of 4-(1H-indol-1-yl)-4-oxobutanoic acid spliced podophyllotoxin derivatives (3a–3l) on tumor cells. The MTT method was adopted to evaluate (3a–3l) antitumor activity in vitro against A549 cells, A549/DDP cells, MCF-7 cells. The results showed that compound 3l had the most prominent inhibitory effect and high selectivity with IC50 18.53 ± 1.51 µM against A549/DDP cells. Meanwhile, the effects of compound 3l on the nuclear state, cell cycle and apoptosis of A549/DDP cells showed that compound 3l induced apoptosis by delaying the G2/M phase of A549/DDP cell cycle. In addition, molecular docking of compound 3l also showed that it could form a good hydrogen bond with ARG-158 (d = 2.6, 2.7 Å) and HIS-406 (d = 2.5 Å) at the colchicine site of tubulin. Compound 3l could provide lead compound for the development of new multi-drug resistant anti-tumor drugs.
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