GREEN CHEMISTRY
·
2016
·Vol. 19
·期 4
·1109-1116
·
IF 8.506
Huan Liu,Dong-Liang Wang,Xia Chen,Yong Lu,Xiao-Li Zhao,Ye Liu
Mono-phosphines (L1 and L2) and diphosphines (L3 and L4) with typical π-acceptor character were prepared and applied in Ir(I)-catalyzed N-alkylation of amines with alcohols. It was found that the π-acceptor character of the applied phosphines is closely correlated to the catalytic efficiency of the [Ir(COD)Cl]2 complex for this green reaction. Compared to PPh3 as the typical σ-donor (i.e. with poor π-acceptor character), L1–L4 all resulted in the efficient N-alkylation of aniline to benzyl-aniline. While L1–L4 coordinated to the Ir(I)-catalyst, the consolidated Ir–P linkages due to π-backdonation could well protect the Ir-catalyst against deactivation, giving rise to the N-alkylation of aniline. On the other hand, the stabilized Ir-catalyst with the involvement of L2 could be recycled successfully for at least 4 runs in the ionic liquid of [MePh3P]Br without the detectable leaching of Ir and P elements in the organic products.
研究领域:
有机化学
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催化化学
·
绿色化学
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产品关联
DOI
高影响因子
BIOORGANIC CHEMISTRY
·
2025
·
IF 4.7
Lei Huang,Lichao Yu,Xiaohui Fang,Hangxin Gong,Yiting Qiu,Guohan Huang,Xiaoxia Ye,Lingtian Wang,Yun-Yun Quan,Zu-Sheng Huang
Photodynamic therapy (PDT), operates through a distinctive reactive oxygen species (ROS)-mediated cytotoxic mechanism, offering therapeutic potential against malignant tumors and bacterial infections. The development of multifunctional photosensitizers (PSs) capable of simultaneously exhibiting potent antitumor and antibacterial activities represents a promising yet challenging frontier in PDT research. Herein, three donor-π bridge-acceptor (D-π-A) aggregation induced emission (AIE) photosensitizers TPTM , TPTP and TPTQ with type I and type II ROS production abilities were successfully constructed by acceptor engineering strategy. TPTP stands out from others by advantages of rapid cellular internalization behavior, potent ROS production capacity, dual-organelle targeting (mitochondria and endoplasmic reticulum) ability. TPTP displayed antitumor effects in 4T1 tumor-bearing nude mice, inducing ROS-mediated apoptosis and suppressing tumor growth. Simultaneously, TPTP enhanced its affinity for bacteria through its cationic part, and exhibited potent antibacterial activity against Gram-positive (G+) bacteria Staphylococcus aureus ( S. aureus ), methicillin-resistant Staphylococcus aureus (MRSA), Staphylococcus epidermidis ( S. epidermidis ), and Gram-negative (G−) bacteria Escherichia coli ( E. coil ) and Acinetobacter baumannii ( A. baumannii ) upon light irradiation. TPTP also performed well in promoting infected wounds healing. This work provides a versatile molecular platform for future applications in infectious diseases and oncology, with potential for further applications in combination therapies.
研究领域:
光动力治疗
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生物有机化学
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药物化学
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材料科学
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纳米医学
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肿瘤学
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微生物学
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产品关联
DOI
PubMed
高影响因子
Nature Energy
·
2024
·
IF 49.7
Meng Hongguang,Mao Kaitian,Cai Fengchun,Zhang Kai,Yuan Shaojie,Li Tieqiang,Cao Fangfang,Su Zhenhuang,Zhu Zhengjie,Feng Xingyu,Peng Wei,Xu Jiahang,Gao Yan,Chen Weiwei,Xiao Chuanxiao,Wu Xiaojun,McGehee Michael D.,Xu Jixian
The manufacturing of perovskite solar cells under ambient conditions is desirable, yet the efficiency of p–i–n perovskite solar cells fabricated in air still lags behind those made in an inert atmosphere. Here we introduce an ionic pair stabilizer, dimethylammonium formate (DMAFo), into the perovskite precursor solution to prevent the degradation of perovskite precursors. DMAFo inhibits the oxidization of iodide ions and deprotonation of organic cations, improving the crystallinity and reducing defects in the resulting perovskite films. We show the generation of additional p-type defects during ambient air fabrication that suggests the need for improving bulk properties of the perovskite film beyond surface passivation. Upon addition of DMAFo, we demonstrate that the efficiency of inverted p–i–n solar cells based on perovskite layers with 1.53-eV and 1.65-eV bandgaps fabricated under ambient conditions (25–30 °C, 35–50% relative humidity) increases by 15–20%. We achieve a certified stabilized efficiency of 24.72% for the 1.53-eV cell, on a par with state-of-the-art counterparts fabricated in an inert atmosphere.
研究领域:
材料科学
·
太阳能
·
化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Huan Su,Chao Shan,Xiaolin Zhang,Bingcai Pan
Chemical oxidation is essential in treating P(I)/P(III)-bearing wastewater, while conventional oxidation processes suffer from low selectivity and high cost induced by oxidant reagents. Herein, a low-cost catalyst PdNi 10 was developed to rival the noble metal Pd, which had been known as the only catalyst enabling chemical-free oxidation of P(I)/P(III) into P(V) by ambient O 2 . The PdNi 10 fabricated via optimized method even outperformed Pd in catalytic activity at identical dosage (0.10 g L −1 ), achieving efficient conversion of 1.00 mM of P(I) into P(V) (>94% in 30 min) with wide applicable pH range from 3.0 to 9.0. The aerobic oxidation of P(I) and P(III) over PdNi 10 was confirmed via scavenging experiments to be both dominated by non-radical pathways with apparent activation energies of 44.5 and 21.3 kJ mol −1 , respectively. Interestingly, the individual roles of Ni components of PdNi 10 in the catalytic oxidation were found negligible. The H 2 O-methanol binary solvent experiment suggested that H 2 O mediated the catalytic reaction and the interfacial OH groups as a result of H 2 O dissociation served as the main reactive oxidant species for P(I)/P(III) oxidation. Furthermore, synergistic mechanism was proposed for the Ni and Pd sites with favorable roles in the essential reaction steps of dehydrogenation and hydroxylation, respectively. This study is believed to advance the treatment strategy of P(I)/P(III)-rich wastewater and to shed new light on the development of low-cost catalysts enabling chemical-free aerobic oxidation processes under facile condition.
研究领域:
环境科学
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催化
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化学工程
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材料科学
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DOI
高影响因子
Journal of Integrative Neuroscience
·
2025
·Vol. 24
·期 8
·40079
·
IF 2.7
Jixin Chen,Guoyou Chen,Yueheng Wu,Shuai Liu,Yifan Ma,Maonan Liu,Wei Yu
Background and Purpose:Ciprofol, a novel intravenous anesthetic, has been shown to exert protective effects against ischemic stroke, a leading cause of death and disability; however, its molecular mechanisms remain unclear. This study aimed to explore the molecular mechanisms underlying the neuroprotective effects of ciprofol using metabolomics.Methods:This study used a middle cerebral artery occlusion (MCAO) rat model to simulate cerebral ischemia-reperfusion injury (CIRI). The rats were divided into ciprofol, MCAO, and sham groups. Histological and neurobehavioral testing methods were used to investigate the therapeutic effects of ciprofol in rats. Ultra-high-performance liquid chromatography-quadrupole time-of-flight mass spectrometry was used to screen for differential metabolites and related metabolic pathways in the serum and brain of the three groups. Spectrophotometry was used to detect in vitro mitochondrial respiratory chain complex I (MRCC-I) activity.Results:Neurological behavioral scores and cerebral infarct volumes of rats in the ciprofol group were significantly lower than those of rats in the MCAO group. Metabolomic analysis revealed 19 differential metabolites in serum samples and 31 differential metabolites in brain samples, including flavin mononucleotide (FMN). These metabolites were mainly enriched in the tricarboxylic acid cycle, respiratory electron transport chain, and amino acid and lipid metabolism. In vitro experiments demonstrated that ciprofol promoted the activity of MRCC-I during CIRI by increasing FMN levels.Conclusion:The mechanisms of action of ciprofol during treatment of cerebral ischemia involve the tricarboxylic acid cycle, respiratory electron transport chain, and amino acid and lipid metabolism and may directly affect MRCC-I activity by regulating FMN.
研究领域:
麻醉药理学
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神经生物学
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代谢组学
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线粒体功能
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脑血管病
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分子药理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Small
·
2024
·
IF 13
Jing Gao,Yuan Gao,Jinghua Hao,Xiaolin Sun,Fuhua Zhao,Yuan Zhang,Wenyan Si,Jianfei Wu
All-solid-state lithium sulfide-based batteries (ASSLSBs) have drawn much attention due to their intrinsic safety and excellent performance in overcoming the polysulfide shuttle effect. However, the sluggish kinetics of Li 2 S cathode severely impede commercial utilization. Here, a Cu + , I − co-doping strategy is employed to activate the kinetics of Li 2 S to construct high-performance ASSLSBs. The electronic conductivity and Li-ion diffusion coefficient of the co-doped Li 2 S are increased by five and two orders of magnitude, respectively. Cu + as a redox medium greatly improves the reaction kinetics, which is supported by ex situ X-ray photoelectron spectroscopy. Density functional theory calculation (DFT) shows that Cu + , I − co-doping reduces the Li-ions diffusion energy barrier. The co-doped Li 2 S exhibits a remarkable improvement in capacity (1165.23 mAh g −1 (6.65 times that of pristine Li 2 S) at 0.02 C and 592.75 mAh g −1 at 2 C), and excellent cycling stability (84.58% capacity retention after 6200 cycles at 2 C) at room temperature. Moreover, an ASSLSB, fabricated with a lithium-free (Si─C) anode, obtains a high specific capacity of 1082.7 mAh g −1 at 0.05 C and 97% capacity retention after 400 cycles at 0.5 C. This work provides a broad prospect for the development of ASSLSBs with practical energy density exceeding that of traditional lithium-ion batteries.
研究领域:
材料科学
·
电化学
·
电池技术
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DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Xuan He,Dan Liang,Jun Zhou,Kangjing Li,Beibei Xie,Chunyun Liang,Cong Liu,Zhiyong Chen,Xinxin Chen,Ao Long,Shufang Zhuo,Xiaoping Su,Ying Luo,Wenxia Chen,Fengfeng Zhao,Xinglu Jiang
The cell nucleus serves as the pivotal command center of living cells, and delivering therapeutic agents directly into the nucleus can result in highly efficient anti-tumor eradication of cancer cells. However, nucleus-targeting drug delivery is very difficult due to the presence of numerous biological barriers. Here, three antitumor drugs (DNase I, ICG: indocyanine green, and THP: pirarubicin) were sequentially triggered protein self-assembly to produce a nucleus-targeting and programmed responsive multi-drugs delivery system (DIT). DIT consisted of uniform spherical particles with a size of 282 ± 7.7 nm. The acidic microenvironment of tumors and near-infrared light could successively trigger DIT for the programmed release of three drugs, enabling targeted delivery to the tumor. THP served as a nucleus-guiding molecule and a chemotherapy drug. Through THP-guided DIT, DNase I was successfully delivered to the nucleus of tumor cells and killed them by degrading their DNA. Tumor acidic microenvironment had the ability to induce DIT, leading to the aggregation of sufficient ICG in the tumor tissues. This provided an opportunity for the photothermal therapy of ICG. Hence, three drugs were cleverly combined using a simple method to achieve multi-drugs targeted delivery and highly effective combined anticancer therapy.
研究领域:
癌症研究
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药物递送系统
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纳米技术
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生物医学工程
·
药学
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产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Changxin Xiang,Zehua Wang,Qing Zhang,Zijian Guo,Xiaona Li,Weiyi Chen,Xiaochun Wei,Pengcui Li
Poly(vinyl alcohol) (PVA) hydrogels exhibit great potential as ideal biomaterials for tissue engineering, owing to their non-toxicity, high water content, and strong biocompatibility. However, limited mechanical strength and low bioactivity have constrained their application in bone tissue engineering. In this study, we have developed a tough PVA-based hydrogel using a facile physical crosslinking method, comprising of PVA, tannic acid (TA), and hydroxyapatite (HA). Systematic experiments were conducted to examine the physicochemical properties of PVA/HA/TA hydrogels, including their compositions, microstructures, and mechanical and rheological properties. The results demonstrated that the PVA/HA/TA hydrogels possessed the porous microstructures and excellent mechanical properties. Furthermore, collagen type I (Col I) was used to further improve the biocompatibility and bioactivity of PVA/HA/TA hydrogels. In vitro experiments revealed that PVA/HA/TA/COL hydrogel could offer a suitable microenvironment for the growth of MC3T3-E1 cells and promote their osteogenic differentiation. Meanwhile, the PVA/HA/TA/COL hydrogel demonstrated the ability to promote bone regeneration and osteointegration in a rat femoral defect model. This study provides a potential strategy for the use of PVA-based hydrogels in bone tissue engineering.
研究领域:
生物材料
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组织工程
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生物医学工程
·
骨再生
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产品关联
DOI
PubMed
高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2024
·Vol. 416
·期 10
·2541-2551
·
IF 3.8
Niu Yanyan,Chen Yuxue,Zhou Juan,Sun Wei
In this study, an online electrochemistry coupling high-performance liquid chromatography-mass spectrometry (EC-HPLC-MS) technology has been developed for simulating metabolic reactions and rapid analysis of metabolites of flavone, quercetin, and rutin, which are not only widely present compounds with pharmacological activity in nature, but also have structural similarity and variability. The simulated metabolic processes of the substrates (phase I and phase II metabolism) were implemented on the surface of glassy carbon electrode (GCE) by using different electrochemical methods. After online chromatographic separation, the products were transmitted to a mass spectrometer for detection, in order to speculate relevant reaction pathways and structural information of the reaction product. The main metabolites, including methylation, hydroxylation, hydrolysis, and conjugation reaction products, had been successfully identified through the designed in situ hyphenated technique. Furthermore, compared with metabolites produced by in vitro incubation of rat liver microsomes, it was found that the products of electrochemical simulated metabolism were more abundant with diverse metabolic pathways. The results indicated that the proposed method exhibited advantages in the sample pretreatment process and detection cycle without compromising the reliability and accuracy of the results. Graphical
研究领域:
分析化学
·
药物化学
·
电化学
·
代谢组学
·
生物分析化学
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DOI
高影响因子
Environmental Chemistry and Ecotoxicology
·
2025
·
IF 8.2
Gao Feiyue,Zhou Chuncai,Li Chen,Xu Shihai,Li Zhiguo,Li Xin,Liu Guijian
The novel ultra-micro porous carbon sheet (PCs) with exceptionally high surface area (3034 m 2 /g) were synthesized through green potassium citrate (K 3 C 6 H 5 O 7 ) activation for efficient thallium(I) [Tl(I)] removal from wastewater. The static adsorption results revealed that PCs achieved exceptional removal efficiencies above 95 % across pH 6–12, maintained high selectivity against competing ions (K + , Na + , Cl − , F − ) and organic interferents, and retained above 80 % capacity after five regeneration cycles. Adsorption followed Pseudo-second order kinetics and Freundlich isotherm models, indicating multilayer adsorption on heterogeneous surfaces, with thermodynamics confirming spontaneous exothermic processes. The density functional theory (DFT) calculation results demonstrated that lone pair electrons involved in complexation and π-electrons participating in coordination were supplied by oxygen-containing functional groups and aromatic rings, respectively. The sorption mechanisms included surface complexation, ion exchange, electrostatic attraction, and cation-π interaction. The column sorption results demonstrated the influent flow rate, bed height, and initial Tl(I) concentration-dependent removal performance. The Tl(I)-containing wastewater at ppm level could meet the discharge standard by optimizing influent flow rate and bed height in column adsorption. The dynamic sorption process was described properly by Thomas and Yoon-Nelson models. This study provides a systematic theoretical foundation for designing porous carbons in Tl-contaminated water remediation.
研究领域:
环境科学
·
材料工程
·
水处理技术
·
物理化学
·
计算化学
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产品关联
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2015
·
IF 4.513
Zhong Feng Gao,Dong Mei Chen,Jing Lei Lei,Hong Qun Luo,Nian Bing Li
Improving the reproducibility of electrochemical signal remains a great challenge over the past decades. In this work, i-motif oligonucleotide probe-based electrochemical DNA (E-DNA) sensor is introduced for the first time as a regenerated sensing platform, which enhances the reproducibility of electrochemical signal, for label-free detection of glucose and urea. The addition of glucose or urea is able to activate glucose oxidase-catalyzed or urease-catalyzed reaction, inducing or destroying the formation of i-motif oligonucleotide probe. The conformational switch of oligonucleotide probe can be recorded by electrochemical impedance spectroscopy. Thus, the difference of electron transfer resistance is utilized for the quantitative determination of glucose and urea. We further demonstrate that the E-DNA sensor exhibits high selectivity , excellent stability, and remarkable regenerated ability. The human serum analysis indicates that this simple and regenerated strategy holds promising potential in future biosensing applications.
研究领域:
分析化学
·
生物传感器
·
电化学
·
分子生物学
✓ 已验证
DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2026
·
IF 7.3
Huidan Li,Ye Liu,Jun Ding
Abstract Isothiocyanates (ITCs) are bioactive hydrolysis products of glucosinolates in Brassicaceae plants with diverse health-promoting properties. However, comprehensive profiling of ITCs remains challenging due to the limited availability of authentic standards, the underexplored structural diversity of naturally occurring ITCs, and poor mass spectrometry (MS) detection sensitivity. Here, we established a N,N-dimethylethylenediamine (DMEDA) derivatization strategy and constructed an in silico MS/MS library for systematic ITC annotation. DMEDA derivatization markedly improved LC–MS detection sensitivity, enabling the reliable detection of low-abundance ITCs with limits of detection at the nanomolar level. Detailed characterization of the MS/MS fragmentation behaviors of derivatized ITC standards revealed subclass-dependent fragmentation patterns, which were subsequently translated into spectral prediction rules for the generation of an in silico mass spectral library with 2209 simulated ITC structures. Application of the developed workflow to Brassicaceae plant samples enabled the annotation of 50 endogenous ITCs, including 4 low-abundance compounds that were previously not reported. Our work provides a valuable resource for the systematic exploration of ITC structural diversity and facilitates functional studies of glucosinolate-derived bioactive metabolites.
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DOI
高影响因子