CRYSTAL GROWTH & DESIGN
·
2025
·
IF 3.4
Detao Li,Zichen Ning,Feiqiang He,Zhi Gao,Limin Zhou,Li Xu,Zhijian Zheng,Jerry Heng,Shichao Du,Jinbo Ouyang
To enable efficient separation of chiral drugs and enhance their practical utility, this study investigates cocrystallization as a novel separation and purification strategy. Using R/S-mandelic acid and d/l-prolinamide as model compounds, we screened potential cocrystal/salt coformers and successfully synthesized seven novel chiral salts. The proton transfer was elucidated by analyzing molecular electrostatic potential differences at the hydrogen-bonding sites. Moreover, the formation mechanism of salts was explored through structural analyses, such as Hirshfeld surface calculations, energy framework assessments, and crystal void analysis. Considering the distinct properties of various chiral salts, we conducted competitive cocrystallization experiments, establishing a complementary chiral pairing principle that provides a theoretical foundation for cocrystallization-based chiral resolution. Based on these findings, we developed multiple processes for the separation of R- and S-mandelic acid as well as l- and d-prolinamide, achieving product purities exceeding 80%, which strongly demonstrate the feasibility of cocrystallization separation technology for chiral resolution. This work not only introduces a groundbreaking approach to chiral separation but also highlights the vast potential of cocrystallization technology in pharmaceutical purification and beyond.
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高影响因子
ACS Catalysis
·
2024
·
IF 11.3
Ruilin Liu,Chao Wang,Yong Yan,Ruzhi Wang,Ge Chen
The direct hydrogen peroxide (H2O2) product from H2 and O2 is a promising anthraquinone replacement because it is environmentally friendly and has a high atom efficiency. Experimental and theoretical studies have proven that optimizing the adsorption of the critical intermediate OOH* on the metal site significantly promotes the further protonation of this intermediate and inhibits the O–O bond cleavage, thus enhancing the activity and selectivity. Redistributing the charge density of active sites to tuning the d-band center of the metal could effectively modulate the intermediates adsorption, and thus regulate the catalytic efficiency. Herein, we show that a Lewis acid (ZnCl2 solution) induces abundant oxygen vacancies (Ovs) on the TiO2 surface, which results in a reversal of charge transfer from TiO2–Ov support to the Pd atom, generating an electron-rich Pd configuration. Compared with pristine Pd/TiO2, Pd/TiO2–Ov possesses higher H2O2 selectivity and productivity, with values of 80.7% and 186 mol kgcat–1 h–1, respectively. In addition, Pd/TiO2–Ov maintains stability during the six cycles reaction due to its high resistance to the leaching of Pd species. Theoretical calculations reveal that the reversed charge transfer downshifts the d-band center of Pd, which promotes O2 adsorption on the Pd surface and weakens the OOH* intermediates adsorption. Thus, the energy barrier for the hydrogenation of the OOH* intermediate is significantly decreased, and the O–O band cleavage is inhibited. This study reports a reversal of charge transfer tuning the d-band center of the active site for efficient direct H2O2 synthesis, which may provide insight for designing high-performance catalysts.
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PHYTOMEDICINE
·
2025
·
IF 8.3
Guifang Fan,Xiaojiaoyang Li,Fanghong Li,Ranyun Chen,Xiaoyong Xue,Le Wang,Qi Zheng,Shuni Duan,Ranyi Luo,Rong Sun,Runping Liu
Background : Radix Bupleuri (RB) and acetaminophen (APAP) are two popular medications having potential hepatotoxicity and substantial risks of irrational co-administration and excessive use, posing an overlooked danger of drug-induced liver injury (DILI). Autophagy is a protective mechanism against APAP-induced DILI, yet, saikosaponin d (SSd) in RB has been characterized to regulate autophagy, although the current findings are controversial. Purpose : We aim to elucidate whether SSd promoted APAP-induced liver injury by regulating autophagy. Methods : UPLC-MS analysis was employed to measure the hepatic abundance of APAP-cysteine protein adducts. Multiple techniques such as fluorescence probe, proteinase K protection assay, immunoprecipitation-coupled proteomic analysis, surface plasmon resonance, molecular docking and et.al were applied to evaluate the SSd on autophagy flux. Results : We discovered that, by inhibiting autophagy, SSd impaired the removal of APAP-cysteine protein adducts and delayed the compensation of damaged mitochondria. This ultimately potentiated the development of severe liver toxicity induced by subtoxic APAP. The use of autophagy probes, transmission electron microscopy, membrane curative assay, and protein K assay collectively revealed that SSd predominately disrupted autophagosome-lysosome fusion, without affecting other stages of autophagic flux. Immunoprecipitation-coupled proteomic analysis and surface plasmon resonance further found that SSd directly bound to GABARAP, thus preventing the recruitment and autoactivation of STX17 and the following assembly of STX17-SNAP29-VAMP8 complex. Conclusion : In conclusion, our findings not only highlight the significant risk of drug-induced liver injury associated with the co-administration of RB and APAP in clinical practice but also unveils that GABARAP-SNARE complex is a novel druggable target for the treatment of autophagy-related diseases.
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PubMed
高影响因子
Metabolic Engineering Communications
·
2018
·
IF 0
Xiaojing Jia,Robert M. Kelly,Yejun Han
( R )-acetoin is a four-carbon platform compound used as the precursor for synthesizing novel optically active materials. Ethylene glycol (EG) is a large-volume two-carbon commodity chemical used as the anti-freezing agent and building-block molecule for various polymers. Currently established microbial fermentation processes for converting monosaccharides to either ( R )-acetoin or EG are plagued by the formation of undesirable by-products. We show here that a cell-free bioreaction scheme can generate enantiomerically pure acetoin and EG as co-products from biomass-derived D -xylose. The seven-step, ATP-free system included in situ cofactor regeneration and recruited enzymes from Escherichia coli W3110, Bacillus subtilis shaijiu 32 and Caulobacter crescentus CB 2. Optimized in vitro biocatalytic conditions generated 3.2 mM ( R )-acetoin with stereoisomeric purity of 99.5% from 10 mM D -xylose at 30 °C and pH 7.5 after 24 h, with an initial ( R )-acetoin productivity of 1.0 mM/h. Concomitantly, EG was produced at 5.5 mM, with an initial productivity of 1.7 mM/h. This in vitro biocatalytic platform illustrates the potential for production of multiple value-added biomolecules from biomass-based sugars with no ATP requirement.
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Nano Energy
·
2020
·
IF 16.602
Zheng Zhou,Xiangxin Du,Zhao Zhang,Jikui Luo,Shaoyu Niu,Da Shen,Yuanyu Wang,Hui Yang,Qilong Zhang,Shurong Dong
Flexible piezoelectric nanogenerator (PENG) has been regarded as one of the promising solutions to harvesting mechanical energy, as a sustainable energy source for wearable devices , etc. Here, a universal strategy of carbon coating modulation is proposed to synthesis carbon coated 0-D piezoceramics nanoparticles (NPs). Owing to the good electric conductivity of carbon shell, the redistribution and accumulation of mobile charges in carbon layer gives rise to reinforcement of electric field, results in the much-enhanced piezoelectric effect. Polydimethylsiloxane (PDMS) composites with those 0-D piezoceramics NPs are used to fabricate PENGs. The peak power density of BT@C, PZT@C and KNN@C based PENGs reaches up to 45.4 μW/cm 2 , 59.8 μW/cm 2 and 9.9 μW/cm 2 , that are 20, 20.4 and 13.4 times larger than those of control PENGs incorporated with bare 0-D piezoceramic NPs, respectively. A theoretical model based on Lewis diffusion theory is constructed to reveal the mechanism of piezoelectric enhancement in the poling process. This research provides a new strategy for synthesis of high piezoelectric characteristic composites by embedding carbon coated 0-D piezoceramic NPs.
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JOURNAL OF MOLECULAR LIQUIDS
·
2021
·
IF 6.165
Yannan Du,Hongjun Zang,Yimo Feng,Kai Wang,Yaxin Lv,Zhipeng Liu
This paper briefs the emerging strategies for the designing of catalytic systems, which direct conversion of chitin biomass monomer N -acetyl- d -glucosamine (NAG) to 3-acetylamino-5-acetylfuran was studied systemically. Twelve catalysts were investigated, and pyrazine hydrochloride ([Pyz]Cl) ionic liquid exhibited the good performance-achieving 3A5AF with yields of 36.94% from NAG . Further adding boric acid and CaCl 2 , treating at 190 °C for 60 min, the conversion rate of NAG is 100%, and the yield of 3A5AF can be increased to 69.54% in DMA. Furthermore, functional group changes before and after the reaction have been characterized by FTIR, HPLC-MS and 13 C NMR were applied to monitor the reaction process with [Pyz]Cl as the catalyst. The reactive intermediate was clearly detected by these techniques. Accordingly, a possible reaction pathway was proposed. The results of this experiment provide a mild and efficient reaction route for the degradation of biomass, and enrich the theoretical research of quaternary amine catalysts in the conversion of biomass waste into high value-added chemicals.
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APPLIED OPTICS
·
2019
·Vol. 58
·期 31
·8583-8588
·
IF 1.973
Suyi Zhong,Tian Guan,Yang Xu,Chongqi Zhou,Lixuan Shi,Cuixia Guo,Xuesi Zhou,Zhangyan Li,Yonghong He,Yanhong Ji
The ability to identify L(+)-ascorbic acid from D(-)-isoascorbic acid in medicinal products is of practical interest. Based on the method of frequency domain weak measurement, a set of common optical path sensors for identification of L(+)-ascorbic acid and D(-)-isoascorbic acid is established. By quantificationally analyzing the magnitude and offset direction of the spectral central wavelength, a good identification of the concentration and the optically active forms of ascorbic acid has been achieved. The sensitivity and resolution of the sensor for optical rotation can reach 34.35 nm/° and ${5.53} \times {{10}^{ - 5}}^\circ $, respectively. The detection resolution for L(+)-ascorbic acid is ${2.00} \times {{10}^{ - 4}}\;{\rm mol}/{\rm mL}$, and that for D(-)-isoascorbic acid is ${2.73} \times {{10}^{ - 4}}\;{\rm mol}/{\rm mL}$. The potential of the sensor in the detection of transparent but optically inactive impurities has been verified by comparative experiments of sodium chloride solution. The sensor also has been applied to identify medicinal vitamin C tablets, which verified the feasibility of the method in optically active pharmaceutical solutions with water-insoluble, optically inactive impurities. Since the sensor has the advantages of high precision, real-time, high robustness, and being non-destructive, it has a great prospect in the field of drug detection containing chiral molecules.
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PubMed
高影响因子
DYES AND PIGMENTS
·
2023
·
IF 4.5
Peiyu Wu,Shengxiong Zhang,Wenjun Zhang,Weijie Song
Dual functional electrochromic (EC)/electrofluorochromic (EFC) materials play a pivotal role in wearable and smart electronic equipments. Developing new materials with high performance of EC/EFC properties is still a big challenge. Here a new D-A structure polymer PPDOTTPD based on thieno(3,4-c)pyrrole-(4,6)dione ( TPD ) was synthesized by Stille coupling, and the EC/EFC properties were investigated for the first time. PPDOTTPD film exhibits reversible color changes from purple neutral state to transparent colored state in the process of reversible redox. Photophysical and electrochemical studies revealed that the polymer has outstanding EC properties, including high optical contrast (52%), fast response time (0.5 s/0.7 s), high coloring efficiency (427.1 cm 2 C −1 ) and good stability. What's more, PPDOTTPD exhibited EFC phenomenon. PPDOTTPD film showed an intense red near-infrared fluorescence with a peak of 672 nm, which gradually doped with the increase of applied potential with a maximum contrast ratio of 12.9. The EC/EFC dual-functional device based on PPDOTTPD was also successfully fabricated, which exhibited high optical and fluorescence contrast. The fine dual-functional performance indicates TPD can be further explored as potential acceptors for synthesizing high performance D-A molecules for intelligent optical devices.
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高影响因子
Journal of Materials Chemistry C
·
2019
·Vol. 7
·期 33
·10379-10388
·
IF 6.641
Tao Hua,Keyi Zhang,Zu-Sheng Huang,Lingyun Wang,Hao Tang,Herbert Meier,Derong Cao
In this paper, the encapsulated insulated molecular wire (EIMW) and 2′,7′-bis(hexyloxy)spiro[cyclopenta[2,1-b:3,4-b′]dithiophene-4,9′-fluorene] (SPDF) were specifically designed as efficient anti-aggregation π-bridges for two novel D–A–π–A metal-free sensitizers (IBT1 and IBT2). Compared with the reference dye IBT3 with 3,3′-dihexyl-2,2′-bithiophene (DHBT) as an anti-aggregation π-bridge, both the dyes IBT1 with EIMW and IBT2 with SPDF as π-bridges can suppress intermolecular aggregation more efficiently. The π-bridge of SPDF shows the strongest anti-aggregation ability due to the rigid ‘T’ configuration among these dyes. Meanwhile, the π-bridge of EIMW shows better anti-aggregation ability than DHBT because of the larger steric hindrance of the former. Finally, when the dyes IBT1 and IBT2 are co-sensitized with IBT3, respectively, the new devices exhibit high efficiencies of 7.85% and 7.64%, respectively, which are comparable to that of N719 (7.85%). The results demonstrate that the dyes with EIMW and SPDF as anti-aggregation π-bridges are promising candidates for efficient DSSCs and dye aggregation can be effectively inhibited by structural engineering of the π-spacer.
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JOURNAL OF COORDINATION CHEMISTRY
·
2020
·
IF 1.41
Kun Lu,Zihan Zhu,Lin Peng,Hai Fu,Xinlong Wang,Enbo Wang
An unusual metal-organic framework, {H[Ag(I)L][Mo(VI)4O13]}n (1) (L=(4-((1H-1,2,4-triazol-1-yl)methyl)phenyl)methanol)), has been obtained under ionothermal conditions. According to the single-crystal X-ray diffraction analysis, 1 is a new 3-D framework based on β-[Mo8O26]4− type polymolybdate anions with two kinds of channels (A and B) along the b-axes and c-axes in the framework. The neighboring inorganic Mo8-Ag chains are linked by the organic ligands through the Ag centers resulting in 2-D layers. These adjacent 2-D layers extend into a 3-D framework through Ag1 nodes and β-[Mo8O26]4− anions, respectively, resulting in a topological symbol (64 · 82)2(64 · 82). In addition, the gas adsorption, proton conduction and luminescent properties of 1 are also discussed in detail. Moreover, the electrochemical impedance spectroscopy (EIS) measurements show a conductivity (1.9 × 10−4 S cm−1 at 65 °C and 95% relative humidity (RH)), with an activation energy of 0.41 eV for 1. The mechanism of proton conduction for 1 is proved to be the vehicular mechanism.
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MOLECULES
·
2016
·Vol. 21
·期 8
·970
·
IF 2.465
Ying Han,Erli Tian,Dongbo Xu,Min Ma,Zixin Deng,Kui Hong
During our search for interesting bioactive secondary metabolites from mangrove actinomycetes, the strainStreptomycessp. 219807 which produced a high elaiophylin yield of 4486 mg/L was obtained. A new elaiophylin derivative, halichoblelide D (1), along with seven known analogues2–8was isolated and identified from the culture broth. Their chemical structures were determined by detailed analysis of 1D and 2D NMR and HRMS data. The absolute configuration of halichoblelide D (1) was confirmed by comparing the CD spectrum with those of the reported analogues. Compounds1–7exhibited potent cytotoxic activities against HeLa and MCF-7 cells with IC50values ranging from 0.19 to 2.12 μM.Keywords:mangrove actinomycetes;Streptomycessp. 219807;elaiophylin;cytotoxic
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高影响因子
Catalysis Science & Technology
·
2020
·Vol. 10
·期 6
·1609-1618
·
IF 5.721
Chao Zhang,Jiandong Liu,Xingliang Liu,Shiai Xu
Two novel covalent bond photocatalysts, namely, g-C3N4NSs/TC1 and g-C3N4NSs/TC2 were prepared for the first time via the generation of an amide covalent bond between g-C3N4 nanosheets (g-C3N4NSs) and acyl chloride synthesized from triphenylamine-type dyes, 2-cyano-3-(4-(diphenylamino)phenyl)acrylic acid (TC1) or 3,3′-(4,4′-(phenylazanediyl)bis(4,1-phenylene))bis(2-cy-anoacrylic acid) (TC2). The experimental results indicated that triphenylamine D–π–A-type organic dye moieties covalently bonded to g-C3N4 successfully and the spectral response regions of both g-C3N4NSs/TC1 and g-C3N4NSs/TC2 could be extended from ∼460 nm to more than 600 nm. Due to the introduced amide covalent bond, the constructed g-C3N4NSs/TC1 photocatalyst showed remarkably enhanced H2 evolution activity with about 73 555.8 μmol h−1 g−1 and exhibited high apparent quantum yields (AQY) of 35.2%, 27.1%, 16.9% and 5.4% at 420 nm, 500 nm, 520 nm and 600 nm monochromatic light, respectively. Compared with the results for pure g-C3N4 NSs, about 100 times higher H2 production rate and 978 times higher AQY value were obtained for g-C3N4NSs/TC1 with the amide covalent bond under visible light irradiation. Compared to g-C3N4NSs/TC1, g-C3N4NSs/TC2 exhibited slightly lower H2 evolution activity with about 70 986.8 μmol h−1 g−1. Combining the experimental and density functional theory (DFT) calculation results, a possible mechanism can be conjectured that the electronic and geometric structures of g-C3N4NSs/TC1 are more conducive to the charge separation and the unidirectionality of electron transport in the excited state than those of g-C3N4NSs/TC2. The research reveals that this introduction of simple triphenylamine-type dyes into the surface of g-C3N4via covalent links results in a strong covalent interaction between functionalized moieties and g-C3N4 to synergistically improve the electronic and optical properties and photocatalytic performance. The present work highlights the potential use of organic dye covalent-functionalized g-C3N4via post modification as a novel photocatalyst in applications such as H2 production.
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危险品化学品经营许可证（带存储）