ORGANIC & BIOMOLECULAR CHEMISTRY
·
2024
·Vol. 22
·期 14
·2764-2773
·
IF 2.9
Yue Song,Wenjie Fan,Chen Yao,Heng Wang,Xiuxiang Lu,Yumin Wang,Pengxiang Liu,Yanjie Ma,Zhen Zhang,Jiang Wang,BeiBei Chu,Lijun Shi,Guoyu Yang,Mengdi Wang
Pattern recognition receptors (PRRs) play a critical role in the innate immune response, and toll-like receptor 7 (TLR7) is an important member of PRRs. Although several TLR7 agonists are available, most of them are being tested clinically, with only one available on the market. Thus, it is imperative to develop new TLR7 agonists. In this study, we designed and synthesized three kinds of quinazoline derivatives and five kinds of pyrrolo[3,2-d]pyrimidine derivatives targeting TLR7. The antiviral efficacy of these compounds was evaluated in vitro and in vivo. Our findings indicated that four kinds of compounds showed exceptional antiviral activity. Furthermore, molecular docking studies confirmed that compound 11 successfully positioned itself in the pocket of the TLR7 guanosine loading site with a binding energy of −4.45 kcal mol−1. These results suggested that these compounds might be potential antiviral agents.
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高影响因子
DALTON TRANSACTIONS
·
2019
·Vol. 48
·期 15
·5072-5082
·
IF 4.052
Shuang Huang,Xi Hong,He-Zhen Cui,Quan Zhou,Yue-Jian Lin,Xiu-Feng Hou
Seven new chelated cyclometalated Ir complexes of ABON,P, ABON,O, and ABON,C(carbene) based on a rigid and tunable 2-arylbenzo[d]oxazole backbone have been prepared for the N-methylation of amines. Among these three coordinated modes, ABON,C(carbene)-chelated iridium-based catalysts exhibited good performance in the monomethylation of aromatic amines with methanol (MeOH) as the green methylation reagent. The steric-modified synthesis of ABON,C(carbene) complexes was described. The most active ABON,C(carbene) complex with marginal steric hindrance as a catalyst was obtained from the benzoxazole ring without a substituent and methyl group of the benzimidazole ring on the N-heterocyclic carbene (NHC) ligand. A variety of amines including para- and meta-substituted aromatic amines, as well as heterocyclic amines, were formulated as suitable substrates. Importantly, this catalyst considerably promoted the yield of the N-methylation of ortho-substituted aromatic amines. Controlled kinetic experiments and deuterium-labeling reactions of these ortho-substituted amines were conducted under optimized conditions. On the basis of the experimental results, a plausible mechanism was proposed.
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高影响因子
TALANTA
·
2020
·
IF 5.339
Lili Liu,Peng Bao,Juan Qiao,Hongyi Zhang,Li Qi
Herein, D- and L-oligopeptides were explored for the first time as chiral ligands in a chiral ligand exchange capillary electrophoresis (CLE-CE) protocol with Zn(II) as central ion for separation of derived d , l -amino acid enantiomers (Dns-D,L-AAs). The effect of four D- and L-oligopeptides, including glycine- l -lysine (Gly-L-Lys), glycine- d -lysine (Gly-D-Lys), l -lysine-lysine-OH and l -lysine-lysine-lysine-lysine-OH on the CLE-CE separation efficiency were evaluated. Thermodynamic calculations and circular dichroism spectra properties showed that the ternary species [(Gly-L-Lys)Zn(II)(D-AAs)] and [(Gly-L-Lys)Zn(II)(L-AAs)] presented the best stereoselectivity , possibly due to entropic effects. Notably, the migration order of Dns-D-AAs and Dns-L-AAs could be tuned by using Gly-D-Lys as the ligand for the CLE-CE system. To obtain satisfactory CLE-CE performance, the concentration ratio of Zn(II) to Gly-L-Lys, the pH of the buffer solution, and the concentration of Zn(II) were investigated. Under the optimized CLE-CE conditions using 100.0 mM H 3 BO 3 , 10.0 mM NH 4 Ac, 3.0 mM Zn (II) and 12.0 mM Gly-L-Lys as the buffer solution at pH 8.30, nine pairs of Dns-D,L-AAs achieved baseline separation, with the partial separation of another five pairs. Furthermore, the proposed CLE-CE protocol, which presented a good linear relationship with the concentration of the test analytes in the range of 75.0–625.0 μM (r 2 ≥ 0.994) and the limit of detection of the method was 5.0 μM, was successfully applied in the kinetics study of l -asparaginase using l -asparagine as the substrate. Our strategy shows the great potential of L-dipeptides in the CLE-CE separation of D,L-AAs enantiomers and bio-applications.
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高影响因子
Systems Microbiology and Biomanufacturing
·
2022
·Vol. 2
·期 3
·507-522
·
IF 0
Du Juanjuan,Zhang Liang
N -methyl- d -aspartic acid (NMDA), an amino acid existing in human and animal central nervous system, exerts agonist action on one of the glutamate receptor subtypes and is clinically used for treatment of diabetes, Parkinson’s and Alzheimer’s syndrome. In this study, an enzymatic protocol for the chiral resolution of N -methyl- d , l -aspartic acid was built with a predicted N -demethylase (GenBank ID: OJV90073.1) from the genome of Chloroflexi bacterium 54-19. Through sequence alignment, the enzyme shares an identity of 32.19% to 2UZZ (PDB ID) with a conserved catalytic center. Recombinantly expressed in Bacillus subtilis WB600 , the N -demethylase was characterized with optimal temperature and pH at 55 ℃ and 7.5, and adaptive temperature and pH were 40–60 ℃ and 6–8. The effects of organic solvents and metal ions were investigated as well. Compared with other previously reported sarcosine oxidases, the enzyme showed a specific N -demethylation activity against N -methyl- l -aspartic acid according to the analysis by chiral liquid chromatography, LC–MS/MS and a detection by polarimeter. The results demonstrated 76% of 4.5 mM N -methyl- d , l -aspartic acid could be chirally separated by 7 mg·L −1 enzyme after reaction of 80 min. This work provided a foundation for mild synthesis of NMDA in industry. Graphical abstract
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ANALYTICAL BIOCHEMISTRY
·
2016
·
IF 2.243
Xiaoxia Shi,Shanshan Sha,Likun Liu,Xin Li,Yufang Ma
Mycobacterium tuberculosis dTDP- d -glucose 4,6-dehydratase (RmlB) is the second enzyme for the biosynthesis of dTDP- l -rhamnose, which is a sugar donor to the synthesis of the cell wall linker, d - N -acetylglucosamine- l -rhamnose. RmlB is essential to mycobacterial growth and is not found in humans; therefore, it is a potential target for developing new anti-tuberculosis drugs. So far, there has been no suitable method for high-throughput screening of RmlB inhibitors. Here, the recombinant M. tuberculosis RmlB was purified and an absorbance-based microtiter plate assay was developed for RmlB activity. It could be used for high-throughput screening of RmlB inhibitors. The kinetic properties of M. tuberculosis RmlB, including optimal pH, optimal temperature, the effect of metal ions , and the kinetic parameters , were determined with this assay. The inhibitory effects of dTTP and dTDP on M. tuberculosis RmlB were also studied with the assay.
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高影响因子
PHARMACOLOGICAL RESEARCH
·
2020
·
IF 5.893
Xiaotian Qi,Mengyue Fan,Nana Huang,Xinyu Zhang,Jing Liu,Xiaoyu Li,Rong Sun
Cancer chemotherapy induced neutropenia (CCIN) is one of the most common toxicity caused by cytotoxic anticancer agents . Despite granulocyte colony-stimulating factor (GCSF) is widely used in clinical practice, the infection and infection-related mortality rate is still high for lack of functionally mature neutrophils. Saikosaponin d (SSD) is one of the major bioactive constituents of Radix Bupleuri (RB), which exerts immune-modulatory properties. We explored the function of SSD in CCIN therapy, we found that SSD contributed to generate functional mature neutrophils which capable of fighting infection both in vitro and in vivo . Network pharmacology was employed to explore the mechanism, 61 signal pathways might play an important role in CCIN treatment. Western Blot was employed to further confirm the potential pathway involved. We found CBL-ERK1/2 pathway was activated by SSD, followed by upregulating PU.1 and CEBPβ expression and leading to neutrophil differentiation. Our findings suggest a natural regimen SSD which could regenerate microbicidal neutrophils to effectively reduce CCIN-associated infection via activating CBL-ERK1/2, providing a rationale for future therapeutic approaches.
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PubMed
高影响因子
ENZYME AND MICROBIAL TECHNOLOGY
·
2020
·
IF 3.448
Jia-Qin Wu,Xiao-Mei Xu,Ding-Lin Wang,Neng-Bing Long,Rui-Feng Zhang
Novel nano-composites were prepared by coating epoxy resin-based cationic polymer in nano-thickness via in-situ curing on the nano-wall of macroporous SiO 2 with pore size of 0.5∼1 μm. By changing the thickness of polymer coating the specific surface area and porosity varied in range of 115∼74 m 2 /g and 90.4∼83.9 %, respectively. Through ion exchange phospholipase D (PLD, from Streptomyces sp ) was efficiently immobilized on the nano-composites as support and the immobilized PLD was applied for the highly efficient synthesis of phosphatidylserine (PS). The loading amount of PLD on the nano-composited support reached to a maximum of 90.2 mg/g support , 4 times as high as that on the pure macroporous silica. The specific activity of the immobilized PLD reached as high as 16,230 U/g protein , while that of free PLD was 18,780 U/g protein . Under a wide range of temperature and pH the stability and activity of the immobilized PLD were greatly improved as compared with the free ones. Under optimized conditions at 45 °C and pH 7.0, the PS yield reached as high as 96.2 % within 40 min. After 28 days storage the immobilized PLD retained 82.2 % of original activity, and after 12 cycling reuses it retained 79.3 % of PS yield, which indicated that the immobilized PLD exhibited good stability.
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PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Xiaojie Liu,Yong Zhao,Yahui Du,Quanliang Wang,Xin Jing,Liangmin Yu,Mingliang Sun
Conjugated donor (D)–acceptor (A) polymer heterojunctions have developed as attractive photocatalysts. However, it is a great difficulty in precisely keeping the batch-to-batch reproducibility of polymers and controlling the related photocatalytic activity . Herein, three ladder-like small molecules BTx (BT2F, BTORCAE, and BTORIC2Cl) are synthesized via molecular engineering and the corresponding BTx/g-C 3 N 4 heterojunctions are developed as photocatalysts for sterilization and contaminant degradation. It is demonstrated that employing another A unit into the D–A–D backbones of the small molecule could promote its intramolecular charge transfer and also improve the intermolecular charge transfer. Notably, BTORIC2Cl employing 2-(5,6-Dichloro-3-oxo-2,3 dihydro-1H-inden-1-ylidene)malononitrile as A 1 unit in its symmetric A 1 –D–A 2 –D–A 1 structure displays near-infrared absorption and extends the absorption edge of BTORIC2Cl/g-C 3 N 4 to 850 nm. With the synergy of efficient intermolecular charge transfer, BTORIC2Cl/g-C 3 N 4 contributes the champion photocatalytic activity of 98.9 % and 99.6 % antibacterial rates for Staphylococcus aureus and Escherichia coli . Moreover, the highest degradation reaction rate constant for Rhodamine B obtained by BTORIC2Cl/g-C 3 N 4 is 5.7 times that of g-C 3 N 4 . This study proposes new ideas of fabricating small molecules/g-C 3 N 4 OSHJs as photocatalysts via rational molecular engineering.
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产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2012
·Vol. 42
·期 10
·3402-3409
·
IF 3.838
Bo Chai,Tianyou Peng,Xiaohu Zhang,Jing Mao,Kan Li,Xungao Zhang
A novel nanostructured carbon/TiO2 nanocomposite photocatalyst is firstly fabricated via a facile hydrothermal process by using fullerene (C60) decorated single-walled carbon nanotubes (SWCNTs) as carbon source, which is denoted as C60-d-CNTs. The obtained nanostructured carbon/TiO2 nanocomposites are characterized by X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), UV-vis diffuse reflectance spectra (DRS), Raman spectra, X-ray photoelectron spectroscopy (XPS) and photoluminescence spectra (PL), and then are used as catalysts for photocatalytic hydrogen production. It is found that the kinds and contents of various carbon nanostructured materials (such as SWCNTs, C60 and C60-d-CNTs) coupled with TiO2 can significantly enhance the photoactivity for hydrogen production, and the 5 wt% C60-d-CNTs/TiO2 nanocomposite exhibits the best performance. Experimental results suggest that the C60-d-CNTs as a novel carbon nanostructured material could be more beneficial for the photogenerated carrier separation than SWCNTs and C60 when these carbon nanostructured materials are coupled with TiO2.
研究领域:
材料科学
·
纳米技术
·
光催化
·
氢能
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 21.1
Donglei Fu,Wei Zhang,Zhengxiong Zhao,Zhonglin Chen,Pengwei Yan,Jinxiang Zuo,Lianpeng Sun
Element-doped catalysts with oxygen vacancies (OVs) are highly effective in water purification by activating oxidants; however, the interfacial mechanisms and specific contributions of reactive oxygen species (ROS) in metal-doped catalysts featuring OVs for peroxymonosulfate (PMS) activation remain insufficiently elucidated. In this study, Cu-doped NiFe 2 O 4 catalysts with abundant OVs were synthesized via a hydrothermal-calcination process, endowing efficient PMS activation for ROS generation. Remarkably, it mediated more sulfate radicals (SO 4 · − ) and hydroxyl radicals (·OH) generation, accounting for 50.4% and 36.5% of 2,4-dichlorophenoxyacetic acid (2,4-D) degradation, respectively. Benefiting from the formation of OVs, it significantly enhanced PMS adsorption ( E ads = -7.17 eV), markedly lower than that of the pristine NiFe 2 O 4 ( E ads = -4.11 eV). Meanwhile, inducing the regulation of the d-band center of Fe and Ni sites towards the Fermi level, thereby enhancing more electron transfer (0.84 e of NiCu x Fe 2-x O 4 compared to 0.60 e of NiFe 2 O 4 ) from OVs to surface-complexed PMS, and thus voluntarily forming SO 4 · − with lower free energy (△G = -11.7 eV). This work elucidates the OVs-mediated structural regulation of the d-band center and interfacial electron transfer pathway, highlighting a synergistic multi-metal activation mechanism in response to PMS activation, which offers a novel strategy for designing efficient catalysts to trigger interfacial ROS formation.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Jiarui Qu,Hongyao Gu,Dong-Feng Chai,Di Wu,Yutong Wang,Yingyi Liu,Xinhui Yu,Guohua Dong,Dongxuan Guo
A metallic salt solution quenching strategy enables lattice-confined Ce doping in Fe 9 S 10 /FeS nanoflowers, overcoming surface adsorption limitations. • Quenching-induced grain boundaries and lattice strain narrow the Fe d -band width and downshift the d -band center, optimizing oxygen intermediate adsorption. • The optimized electronic structure lowers the OER rate-determining energy barrier from 2.22 eV to 1.82 eV, achieving an overpotential of 274 mV and 300 h AEMWE stability. Lattice confinement of large-radius cerium enables atomic-level electronic modulation for oxygen evolution reaction (OER) electrocatalysts in anion exchange membrane water electrolyzer (AEMWE) applications but remains challenging. Herein, a metallic salt solution quenching strategy achieves lattice-confined cerium doping in iron sulfide composite nanoflowers (Fe 9 S 10 /FeS). The ultrafast cooling generates abundant grain boundaries and lattice strain, which collectively reduce Fe Fe orbital overlap, narrow the Fe d -band width, and shift the d -band center upward. These electronic modifications consequently optimize the adsorption energetics of oxygen-containing intermediates on the pristine Fe 9 S 10 /FeS surface, mitigating their excessively strong binding. According to density functional theory (DFT) calculations, the energy barrier for the rate-determining step is reduced from 2.22 eV to 1.82 eV. Consequently, the cerium-doped iron sulfide catalyst (Ce-FeS-4th) exhibits a low overpotential of 274 mV at 10 mA cm −2 and a Tafel slope of 68 mV dec −1 . An AEMWE using this anode achieves 1.0 A cm −2 at 2.48 V and operates stably for over 300 h. Overall, this work establishes quenching-induced lattice confinement as a versatile paradigm for d -band center engineering in advanced electrocatalysts. Download: Download high-res image (81KB) Download: Download full-size image
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高影响因子
Nature Communications
·
2026
·
IF 18.1
Zhang Zhenlin,Yan Lang,Li Weiwei,Hu Jinyan,Wang Yang,Dou Hongjing,Pan Dengyu,Shen Longxiang,Shi Sheng,Geng Bijiang
In the development of clinically translatable triplet photosensitizers for hypoxia regulated photodynamic therapy (PDT), there is an unmet need for engineering sensitizers as near-infrared (NIR)-responsive, type I/type Ⅱ dual photosensitizers and mild photothermal agents. Herein, we develop a binary precursor-engineering strategy for precise regulation of the D-π-A configuration of carbon dots (CDs) as ultralong-lived triplet, type I/Ⅱ dual photosensitizers by utilizing phenolic hydroxyl as an electron-rich donor and pyridine N as an electron-withdrawing acceptor. The photodynamic performance of CDs is enhanced by intramolecular charge transfer and mild photothermal conversion. We further design M1-like macrophage-derived cell membrane‑camouflaged CDs to realize preferential tumor accumulation while guaranteeing rapid systemic clearance. D-π-A sensitized CD-mediated PDT induces anti-tumor activity against primary and distant tumors. Our work highlights the crucial roles of D-π-A sensitization of CDs in boosting PDT by triplet state tuning, surface charge transfer, and mild photothermal relief of hypoxia.
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PubMed
高影响因子
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