作者机构：
[Li, Ye; Zhang, Yuexin; Li, Chunquan; Zhao, Yu; Huang, Xuemei; Xie, Liyuan; Zhang, Guorui; Zhao, Jun; Fan, Shifan; Song, Chao] Univ South China, Hengyang Med Sch, Affiliated Hosp 1, Hengyang 421001, Hunan, Peoples R China.;[Li, Ye; Zhang, Yuexin; Li, Chunquan; Zhao, Yu; Huang, Xuemei; Xie, Liyuan; Zhang, Guorui; Zhao, Jun; Fan, Shifan; Song, Chao] Univ South China, Hengyang Med Sch, MOE Key Lab Rare Pediat Dis, Hengyang 421001, Hunan, Peoples R China.;[Li, Ye; Zhang, Yuexin; Zhang, Qinyi; Li, Chunquan; Zhao, Yu; Huang, Xuemei; Xie, Liyuan; Zhang, Guorui; Fan, Shifan; Song, Chao] Univ South China, Sch Comp, Hengyang 421001, Hunan, Peoples R China.;[Li, Chunquan] Univ South China, Hunan Prov Maternal & Child Hlth Care Hosp, Hengyang Med Sch, Key Lab Birth Defect Res & Prevent,Natl Hlth Commi, Hengyang 421001, Hunan, Peoples R China.;[Li, Ye; Zhang, Yuexin; Li, Chunquan; Zhao, Yu; Huang, Xuemei; Xie, Liyuan; Zhang, Guorui; Fan, Shifan; Song, Chao] Univ South China, Affiliated Hosp 1, Cardiovasc Lab Big Data & Imaging ArtificialIntell, Hengyang Med Sch, Hengyang 421001, Hunan, Peoples R China.
通讯机构：
[Li, CQ ] U;Univ South China, Hengyang Med Sch, Affiliated Hosp 1, Hengyang 421001, Hunan, Peoples R China.;Univ South China, Hengyang Med Sch, MOE Key Lab Rare Pediat Dis, Hengyang 421001, Hunan, Peoples R China.;Univ South China, Sch Comp, Hengyang 421001, Hunan, Peoples R China.;Univ South China, Hunan Prov Maternal & Child Hlth Care Hosp, Hengyang Med Sch, Key Lab Birth Defect Res & Prevent,Natl Hlth Commi, Hengyang 421001, Hunan, Peoples R China.
关键词：
genes;mice;candidate disease gene;inference;multiomics;oncogenes;enhancer of transcription;cell lines;transcription factor
摘要：
Gene regulatory networks (GRNs) are interpretable graph models encompassing the regulatory interactions between transcription factors (TFs) and their downstream target genes. Making sense of the topology and dynamics of GRNs is fundamental to interpreting the mechanisms of disease etiology and translating corresponding findings into novel therapies. Recent advances in single-cell multi-omics techniques have prompted the computational inference of GRNs from single-cell transcriptomic and epigenomic data at an unprecedented resolution. Here, we present scGRN (https://bio.liclab.net/scGRN/), a comprehensive single-cell multi-omics gene regulatory network platform of human and mouse. The current version of scGRN catalogs 237 051 cell type-specific GRNs (62 999 692 TF-target gene pairs), covering 160 tissues/cell lines and 1324 single-cell samples. scGRN is the first resource documenting large-scale cell type-specific GRN information of diverse human and mouse conditions inferred from single-cell multi-omics data. We have implemented multiple online tools for effective GRN analysis, including differential TF-target network analysis, TF enrichment analysis, and pathway downstream analysis. We also provided details about TF binding to promoters, super-enhancers and typical enhancers of target genes in GRNs. Taken together, scGRN is an integrative and useful platform for searching, browsing, analyzing, visualizing and downloading GRNs of interest, enabling insight into the differences in regulatory mechanisms across diverse conditions. Graphical Abstract
摘要：
In this paper, nitrogen-doped carbon dots (NCDs) were synthesized via a facile hydrothermal method using gum arabic (GA) and tris(hydroxymethyl)methyl aminomethane (tris) as precursors. The resultant NCDs show uniform size distribution and stable optical performance. Then a fluorescent signal quenching probe based on NCDs was proposed for the quantitative detection of mercury ions (Hg2+). The developed fluorescent nanoprobe based on NCDs demonstrated a good linear relationship in the range of 10 to 120 mu M (R-2 = 0.99265) for toxic mercury(ii), with a detection limit of 4.87 mu M. Additionally, the present assay system could be efficiently used for the detection of Hg2+ in real water samples with a satisfactory recovery rate (96.11-104.04%). The metal-free NCDs, which exhibited little cytotoxicity, were successfully applied to in vitro fluorescence imaging of human triple negative breast cancer (TNBC) cells, achieving visualization of Hg2+ in cells. With good water solubility and biocompatibility, the nitrogen-doped carbon dots synthesized by this economical and ecologically friendly process are suitable for use in analytical testing and biological research.
摘要：
Conceptual diagram illustrating shielding in polymer composite materials. Abstract Development of shielding materials for 222Rn and γ radiation has crucial implications for ensuring the safety of individuals. This paper reports the synthesis of modified graphene nanosheets (MGNPs) via the reaction of KH560 with graphene nanosheets (GNPs), while melt blending and hot‐press molding technique were used to fabricate a multifunctional polymer composite shielding material, MGNP/WB/PMMA (polymethyl methacrylate). Successful synthesis of MGNP was confirmed by Fourier transform infrared spectroscopy, and scanning electron microscope (SEM) analysis was utilized to assess the distribution of functional fillers within the cross‐section of the polymer composite. Additionally, thermogravimetric analysis (TGA) demonstrated that MGNP and WB particles enhance the thermal stability of the polymer composite materials. Compared to pure PMMA, 98.7% decrease in the radon diffusion coefficient was observed for MGNP1.5 wt%/PMMA composite material. In addition to enhance the radon‐blocking characteristics of the polymer composites, inclusion of WB particles also boosts their shielding capacity against gamma radiation. The 222Rn diffusion coefficient of MGNP1.5 wt%/WB25wt%/PMMA polymer composite material decreased by 99.6% and at energies of 60 KeV, 80 KeV, 122 KeV, 365 KeV, the mass attenuation coefficient (MAC) for the composite material increased by 0.79, 1.97, 0.57, and 0.05 cm2/g, respectively, compared to pure PMMA. Highlights The PMMA composite materials doped with graphene nanosheets demonstrate outstanding resistance to 222Rn. Graphene nanosheets modified by KH560 exhibit favorable dispersion within PMMA. WB can further enhance the radon resistance of MGNP/WB/PMMA composite materials. The polymer composites exhibit excellent 222Rn and gamma ray shielding properties.
期刊：
NEW JOURNAL OF CHEMISTRY,2024年48(6):2855-2865 ISSN：1144-0546
通讯作者：
Sun, YK;Sun, Yunkai;Yang, PF
作者机构：
[Ding, Yi; Sun, Yunkai] Changzhou Inst Technol, Sch Chem Engn & Mat, Changzhou 213032, Peoples R China.;[Yang, Pengfei; Liu, Cheng; Sun, Yunkai; Yin, Na] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Ding, Yi; Sun, Yunkai] Changzhou Inst Technol, Ind Coll Carbon Fiber & New Mat, Changzhou 213032, Peoples R China.
通讯机构：
[Sun, YK ] C;[Sun, YK; Yang, PF ] U;Changzhou Inst Technol, Sch Chem Engn & Mat, Changzhou 213032, Peoples R China.;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;Changzhou Inst Technol, Ind Coll Carbon Fiber & New Mat, Changzhou 213032, Peoples R China.
摘要：
Nanoscale zero-valent iron (nZVI) was cured by vulcanization and biochar functionalization to overcome the tendency of oxidation and aggregation, and the sulfurized nano-zero-valent iron functional material supported by amino biochar (SnZVI-BC-NH2) was obtained, which was used to remove U(VI) from wastewater in this study. A variety of measurements (SEM, TEM, XRD, BET, VSM, FT-IR, and XPS) were used to characterize the morphology, structure, magnetic properties, characteristic functional groups and chemical bonds of SnZVI-BC-NH2. Analysis results confirm that the aminated biochar can support sulfurized nZVI well. The good kinetics, thermodynamics, and large removal capacity data (at pH 6, T = 298 K, Q(m) = 158.1 mg g(-1)) indicate that SnZVI-BC-NH2 has excellent removal performance for U(VI), and the experimental data are in good agreement with the pseudo-second-order kinetic model. Cycling and anti-oxidation tests demonstrate that the FeSx shell plays a crucial role in enhancing the removal of SnZVI-BC-NH2 on U(VI). XPS and FT-IR analysis results show that SnZVI-BC-NH2 removes U(VI) through the synergistic effect of adsorption and reduction.
作者：
Ji, Hong-Tao;Jiang, Jun;He, Wei-Bao;Lu, Yu-Han;Liu, Yuan-Yuan;...
期刊：
JOURNAL OF ORGANIC CHEMISTRY,2024年89(6):4113-4119 ISSN：0022-3263
通讯作者：
He, WM
作者机构：
[He, Wei-Bao; Lu, Yu-Han; He, Wei-Min; Li, Xiao; Ji, Hong-Tao; Liu, Yuan-Yuan; Jiang, Jun; He, WM] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
通讯机构：
[He, WM ] U;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
摘要：
The first example of an electrochemical multicomponent synthesis of selenium-containing compounds with inexpensive and abundant elemental selenium as the selenating reagent was developed. A variety of selenazol-2-amines were constructed in high yields with good functional group tolerance under metal-free and chemical oxidant-free conditions.
摘要：
Electrosorption holds extraordinary promise for uranium (U(VI)) capture but is still limited by the finite accessible active sites of electrode materials, poor surface wettability and its intrinsic co-ion repulsion effect. Here we originally designed KOH-etched porous graphitic carbon nitride (g-C3N4) as active material, and multi-functional crosslinked xanthan gum-polyacrylic acid (XG-PAA) as binder to fabricate g-C3N4-X electrode for U(VI) capture. The abundant in-plane nanopores on 2D g-C3N4 lamellar, rich O- and N-containing active sites, and 3D tough interconnected conductive architecture, endowed g-C3N4-X electrode with fast electron/ion transport channels, alleviated co-ions exclusion, superior electrochemical properties, and hydrophilicity. These unique structure characteristics enabled U(VI) ions to form micro electric-field attraction with negatively charged COO- groups in advance to alleviate co-ion repulsion, then to electro-migrate towards and coordinate with active sites, and eventually to be electrocatalytic reduced into U(IV) deposits. Consequently, the g-C3N4-X electrode exhibited a 1.87 times faster adsorption kinetics, a much higher removal ratio of 98.1% within 70 min than traditional PVDF-bound electrode. Meanwhile, the cumulative adsorption capacity of g-C3N4-X electrode after six cycles was up to 1459.1 mg g−1. This efficient, scalable, and cost-effective g-C3N4-X electrode represents a significant step forward toward the practical applications of U(VI) electrosorption.
期刊：
International Journal of Biological Macromolecules,2024年254(Pt 3):128008 ISSN：0141-8130
通讯作者：
Wang, HQ
作者机构：
[Wang, HQ; Wang, Hongqiang; Wang, Qingliang; Gan, Jiali; Xin, Qi; Hu, Eming; Le, Dongdong; Lei, Zhiwu] Univ South China, Sch Resource Environm & Safety Engn, Hengyang 421001, Peoples R China.;[Wang, Hongqing] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
通讯机构：
[Wang, HQ ] U;Univ South China, Sch Resource Environm & Safety Engn, Hengyang 421001, Peoples R China.
关键词：
Hydrogel;Phytic acid;Uranium adsorption
摘要：
In order to improve the removal rate of uranium and reduce the harm of radioactive pollution, a physically crosslinked polyvinyl alcohol/phosphorylated chitosan (PPP) hydrogel electrode was designed by freezing thawing method. The results show that PPP hydrogel has a good adsorption effect on uranium, and 200mL of uranium tailings leachate is absorbed, and the treatment efficiency reaches 100% within 15min. PPP hydrogel can adapt to a wide range of pH conditions and exhibit excellent adsorption efficiency in the range of 3-9. At the same time, PPP hydrogel maintains an adsorption efficiency of over 85% for 950mg/L uranium solution. This lays the foundation for the practical application of PPP hydrogel. In addition, PPP hydrogel also exhibits good repeatability, after 7cycles, the material still retains 95% of its initial performance. The synergistic effect of various functional groups such as phosphate, hydroxyl, and ammonium in the material is the main mechanism of PPP's adsorption capacity for uranium. Furthermore, electrochemical adsorption method significantly enhances the adsorption performance of PPP hydrogel.
摘要：
A novel polyvinyl alcohol-carbon nanotube containing an imidazolyl ionic liquid/chitosan composite hydrogel (termed CBCS) was prepared for highly selective uranium adsorption from seawater. The results show that CBCS has good adsorption properties for uranium within the pH range of 5.0-8.0. Kinetics and thermodynamics experiments show that the theoretical maximum adsorption capacity of CBCS to U(VI) is 496.049mg/g (288K, pH=6.0), indicating a spontaneous exothermic reaction. Mechanism analysis shows that the hydroxyl group, amino group, and CN bond on the surface of CBCS directly participate in uranium adsorption and that the dense pores on the surface of CBCS play an important role in uranium adsorption. The competitive adsorption experiment shows that CBCS has excellent uranium adsorption selectivity. In addition, CBCS exhibits good reusability. After five adsorption-desorption cycles, the uranium adsorption rate of CBCS can still reach >98%. Hence, CBCS has excellent potential for uranium extraction from seawater.
作者机构：
[Li, Chun-Quan; Tang, Hui-Fang; Qian, Feng-Cui] Univ South China, Hengyang Med Sch, Affiliated Hosp 1, Hengyang 421001, Hunan, Peoples R China.;[Li, Chun-Quan; Tang, Hui-Fang; Qian, Feng-Cui] Univ South China, Hengyang Med Sch, Hunan Prov Key Lab Multiom & Artificial Intelligen, Hengyang 421001, Hunan, Peoples R China.;[Li, Chun-Quan] Univ South China, Hengyang Med Sch, Hunan Prov Maternal & Child Hlth Care Hosp, Natl Hlth Commiss Key Lab Birth Defect Res & Preve, Hengyang 421001, Hunan, Peoples R China.;[Li, Chun-Quan; Qian, Feng-Cui] Univ South China, Sch Basic Med Sci, Dept Biochem & Mol Biol, Hengyang 421001, Hunan, Peoples R China.;[Li, Chun-Quan; Qian, Feng-Cui] Univ South China, Hengyang Med Sch, MOE Key Lab Rare Pediat Dis, Hengyang 421001, Hunan, Peoples R China.
通讯机构：
[Li, CQ ; Tang, HF ; Tang, HF] U;Univ South China, Hengyang Med Sch, Affiliated Hosp 1, Hengyang 421001, Hunan, Peoples R China.;Univ South China, Hengyang Med Sch, Hunan Prov Key Lab Multiom & Artificial Intelligen, Hengyang 421001, Hunan, Peoples R China.;Univ South China, Hengyang Med Sch, Hunan Prov Maternal & Child Hlth Care Hosp, Natl Hlth Commiss Key Lab Birth Defect Res & Preve, Hengyang 421001, Hunan, Peoples R China.;Univ South China, Sch Basic Med Sci, Dept Biochem & Mol Biol, Hengyang 421001, Hunan, Peoples R China.
关键词：
chromatin;genes;software;epigenetics
摘要：
Chromatin accessibility profiles at single cell resolution can reveal cell type-specific regulatory programs, help dissect highly specialized cell functions and trace cell origin and evolution. Accurate cell type assignment is critical for effectively gaining biological and pathological insights, but is difficult in scATAC-seq. Hence, by extensively reviewing the literature, we designed scATAC-Ref (https://bio.liclab.net/scATAC-Ref/), a manually curated scATAC-seq database aimed at providing a comprehensive, high-quality source of chromatin accessibility profiles with known cell labels across broad cell types. Currently, scATAC-Ref comprises 1 694 372 cells with known cell labels, across various biological conditions, >400 cell/tissue types and five species. We used uniform system environment and software parameters to perform comprehensive downstream analysis on these chromatin accessibility profiles with known labels, including gene activity score, TF enrichment score, differential chromatin accessibility regions, pathway/GO term enrichment analysis and co-accessibility interactions. The scATAC-Ref also provided a user-friendly interface to query, browse and visualize cell types of interest, thereby providing a valuable resource for exploring epigenetic regulation in different tissues and cell types.
摘要：
This study proposes and develops a novel ionic concentration gradient electric generator (i‐CGEG) based on the evaporation rate difference of electrolytes. The i‐CGEG with PVA–Na electrolyte achieves a thermovoltage greater than 200 mV and an energy density of 77.94 J m−2 at a temperature of 323 K. Wearable devices and their corresponding cell modules are also developed to recycle body heat. Abstract Constructing concentration differences between anions and cations at the ends of an ionic conductor is an effective strategy in electricity generation for powering wearable devices. Temperature gradient or salinity gradient is the driving force behind such devices. But their corresponding power generation devices are greatly limited in actual application due to their complex structure and harsh application conditions. In this study, a novel ionic concentration gradient electric generator based on the evaporation difference of the electrolyte is proposed. The device can be constructed without the need for semipermeable membranes, and operation does not need to build a temperature difference. As a demonstration, a PVA–Na ionic hydrogel is prepared as an electrolyte for the device and achieved a thermovoltage of more than 200 mV and an energy density of 77.94 J m−2 at 323 K. Besides, the device exhibits the capability to sustain a continuous voltage output for a duration exceeding 1500 min, as well as enabling charging and discharging cycles for 100 iterations. For practical applications, a module comprising 16 sub‐cells is constructed and successfully utilized to directly power a light‐emitting diode. Wearable devices and their corresponding cell modules are also developed to recycle body heat.
摘要：
In this study, a crystal material UIO-66-NH2-BPDA was designed by grafting BPDA onto UIO-66-NH2 and applied to extract U(VI) from aqueous solution. According to performance tests, UIO-66-NH2-BPDA exhibits excellent chemical and thermal stability. The experimental results show that U(VI) adsorption by UIO-66-NH2-BPDA was tested to be 346.58 mg g(-1) at pH = 4 and T = 298 K. The data simulation demonstrates that the adsorption process was consistent with Langmuir isotherm and pseudo-second-order model. Meanwhile, the thermodynamic parameters suggest that the adsorption process was spontaneous and endothermic. Most noteworthy is the good selectivity for U(VI) adsorption by UIO-66-NH2-BPDA. It can be seen that UIO-66-NH2-BPDA can be used as a potential effective adsorbent to remove U(VI) from wastewater.
摘要：
Land-based uranium resources are becoming scarce because of the widespread development and use of nuclear energy. Therefore, to make up for the shortage of uranium resources, a new chitosan/carboxymethyl-β-cyclodextrin/quaternary ammonium salt-functionalized amidoxime carbon adsorbent (CSAOCF) was designed and synthesized for extracting uranium from seawater. Experimental studies show that the adsorption of uranium by CSAOCF is a spontaneous endothermic reaction and chemical adsorption. The theoretical maximum adsorption capacity of uranium can reach 726mg/g at 308K and pH=6. Moreover, the adsorption efficiency and selectivity of CSAOCF for uranium were significantly improved after the introduction of the carboxymethyl group, and the selection and partition coefficient of CSAOCF for uranium and vanadium increased from 16-fold to 30-fold under the same conditions. This indicates that there is a synergistic effect between carboxyl and amidoxime groups, which can promote the adsorption of uranium by CSAOCF. Furthermore, CSAOCF exhibits good oil resistance and can be reused more than five times. Therefore, CSAOCF containing carboxymethyl and amidoxime functional groups can considerably improve the selective adsorption of uranium and has great potential in the extraction of uranium from seawater.
期刊：
European Journal of Medicinal Chemistry,2024年263:115956 ISSN：0223-5234
通讯作者：
Mi, Pengbing;Yuan, Zhonghua;Zheng, X;Lin, YW
作者机构：
[Tan, Yan; Yuan, Zhonghua; Mi, Pengbing; Jiang, Jinhuan; Chen, Limei; Luo, Jianxiong; Zheng, Xing; Ye, Shiying; Lin, Yuqing; Zheng, X] Univ South China, Dept Pharm, Hengyang Med Sch, Hengyang 421001, Hunan, Peoples R China.;[Lang, Jia-Jia; Lin, Ying-Wu] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.;[Lang, Jia-Jia; Lin, Ying-Wu; Mi, Pengbing] Univ South China, Key Lab Prot Struct & Funct Univ Hunan Prov, Hengyang 421001, Hunan, Peoples R China.;[Zheng, Xing] Hunan Vocat Coll Sci & Technol, Dept Pharm, Changsha 410004, Hunan, Peoples R China.;[Lv, You] Shaanxi Univ Sci & Technol, Coll Bioresources Chem & Mat Engn, Xian 710021, Shaanxi, Peoples R China.
通讯机构：
[Yuan, ZH; Mi, PB; Lin, YW ; Zheng, X ] U;Univ South China, Dept Pharm, Hengyang Med Sch, Hengyang 421001, Hunan, Peoples R China.;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.
关键词：
Human monoamine oxidase B inhibitor;Thiochromone;Thiochromone S,S-dioxide
摘要：
Developing new scaffolds for highly potent and selective inhibitors of human Monoamine Oxidase B (hMAO-B) is a crucial objective in enhancing the efficacy and safety in the clinical treatment of neurodegenerative diseases. In this study, we have identified a series of C-3 isoxazole-substituted thiochromone S,S-dioxide derivatives that exhibit strong inhibitory activity against hMAO-B. The strategy of oxidizing thiochromone to thiochromone S,S-dioxide solves the key defect of extreme insolubility observed for thiochromone analogues. In addition, the sulfone group contributes extra hydrogen(H)-bonding interactions with Tyr435, which significantly increases the activity of thiochromone S,S-dioxide derivatives against hMAO-B. Furthermore, the presence of isoxazole group provides potential H-bonding interaction and electrostatic interaction with the residue of Tyr326, while the rigid aryl ring introduces a potential steric conflict with Phe208 of hMAO-A to improve both potency and selectivity. In our investigations, several compounds (9c, 10c, 10e, 10g, 10l and 10m) demonstrate remarkable single-digit nanomolar potency. These compounds exhibit favorable cytotoxicity profiles in both differentiated SH-SY5Y and HVSMC cells, without apparent cardiotoxic effects. Moreover, compounds 10e and 10h do not lead to an increase in ROS levels in differentiated SH-SY5Y cells, further demonstrating their potential as safe and effective hMAO-B inhibitors. These findings indicate that the C-3 isoxazole substituted thiochromone S,S-dioxide analogues are potential leading compounds for the development of selective inhibitors with high potency.
作者机构：
[Peng, Guo-wen; Guo, Meng-zhen; Xiao, Xi-lin; Wang, Yun; Kong, Xiang-he; Nie, Chang-ming; Ouyang, Wen-jun] Univ South China, Sch Chem & Chem Engn, Hengyang, Peoples R China.;[Peng, Guo-wen; Guo, Meng-zhen; Xiao, Xi-lin; Wang, Yun; Kong, Xiang-he; Nie, Chang-ming; Ouyang, Wen-jun] Theoret Res Dept, Key Lab Hunan Prov Design & Applicat Nat Actinide, Hengyang, Peoples R China.;[Peng, Guo-wen; Peng, GW; Nie, Chang-ming; Nie, CM] Theoret Res Dept, Key Lab Hunan Prov Design & Applicat Nat Actinide, Hengyang 421001, Peoples R China.
通讯机构：
[Peng, GW ; Nie, CM] T;Theoret Res Dept, Key Lab Hunan Prov Design & Applicat Nat Actinide, Hengyang 421001, Peoples R China.
关键词：
chiral pesticides;chiral-at-uranium complex;density functional theory (DFT);enantioseparation;R/S-malaoxons
摘要：
Unraveling uranium complexes has become a popular study topic in recent years to address the problem of spent fuel treatment. An important and promising investigation is the enantiomer separation of chiral organophosphorus pesticides (OPs) via uranyl-containing receptors. Among them, malaoxon (MLX), as a chiral OP with high toxicity and good selectivity, is controversial because of the different toxicity differences caused by the R and S configurations to target and non-target organisms. Therefore, it is crucial to explore effective methods for separating its enantiomers. In this work, a novel 2-(9-[1H-pyrazole-1-carbonyl]-1,10-phenanthrolin-2-yl)-1H-inden-1-one (HPIDO) ligand, which combines with uranyl to form the chiral-at-uranium complex (Uranyl-HPIDO receptor), was designed for the enantioseparation of R/S-malaoxons (R/S-MLXs). Based on density functional theory (DFT), we explored the potential coordination modes between the Uranyl-HPIDO receptor and R/S-MLXs at various sites. The analyses of bonding properties, orbital interactions, and weak interactions of intramolecular groups of the complexes, along with the study of thermodynamic properties, revealed that the Uranyl-HPIDO receptor preferred to bind to the phosphoryl oxygen (O5) of R/S-MLXs to form stable complexes. Good enantioseparations of the two enantiomers were achieved in various solvents (water, n-Butanol, n-Octanol, dichloromethane, propanoic acid, toluene, and cyclohexane); the separation factors (SFR/S) ranged 21-853, and the enantioselectivity coefficients (ESCR/S) were more than 95%. The findings could theoretically offer useful information and guidance for the separation of R/S-MLXs, in addition to providing fresh concepts for the creation of novel uranyl receptors. A novel chiral-at-uranium complex (Uranyl-HPIDO) was designed for enantioseparation of R/S-malaoxons (R/S-MLXs). Based on density functional theory, we unraveled complexation between Uranyl-HPIDO and R/S-MLXs. The results indicated that Uranyl-HPIDO preferred to bind to phosphoryl oxygen of R/S-MLXs to form stable complexes and realized the enantioseparation of chiral MLXs. image
摘要：
In the classical route of synthesizing of avanafil, the last step of the reaction uses EDCI and HOBT as an acid and amine binding agent. HOBT may contain residues of hydrazine, and potential mutagenic impurities containing acylhydrazide structures may be formed. The intermediate product (M6) of avanafil was synthesized by 6 steps using diethyl ethoxylmethylmalonate and S-methyl isothiourea semisulfide as starting materials. The potentially genotoxic impurity E (Imp-E) of avanafil was given by the reaction of M6 and hydrazine sulfate acid amine, yield of 20%. The single crystal of Imp-E was cultivated by solvent volatilization method, and its structure was analyzed by high resolution mass spectrometry (HRMS) and nuclear magnetic resonance spectroscopy (NMR). The Flack parameter of Imp-E was -0.03(3) by X-ray single crystal diffraction analysis, and the absolute configuration of Imp-E was determined as S configuration. The intramolecular / intermolecular hydrogen bonds of Imp-E make the molecules maintain a stable arrangement in space.
摘要：
Electrochemical conversion of nitrate to valuable ammonia (NH3) is a green and widely used approach to NH3 synthesis that can be an attractive and complementary alternative to the Haber-Bosch process. However, due to the multi-step reactions in the nitrate reduction pathway, there are still challenges in developing efficient catalysts that can selectively guide the reaction route towards NH3. Herein, B doping is proposed as an effective strategy to enhance nitrate conversion to NH(3 )on the Co3O4 nanoarrays, which not only improves the electrical conductivity of Co3O4, but also lowers the energy barrier of the potential-determining step. Such B-Co3O4/TM delivers a high faradaic efficiency of 94.7% and a large NH3 yield rate of 407.3 mu mol h(-1) cm(-2). Theoretical calculations further elucidate that the introduction of B enhances the adsorption characteristic of Co3O4 for NO3-, consequently facilitating the reduction kinetics.
摘要：
The coating of mesoporous silica nanoshells can improve the stability of gold nanorods while improving the corresponding drug‐carrying capacity. Mesoporous silica coated gold nanorod (GNR@MSN) provides the opportunity to integrate different treatments into a single nanoplatform combining cancer treatment with real‐time diagnosis. This review discusses the advancements of GNR@MSN in synthetic process, bio‐imaging techniques and tumor therapy. Abstract For unique surface plasmon absorption and fluorescence characteristics, gold nanorods have been developed and widely employed in the biomedical field. However, limitations still exist due their low specific surface area, instability and tendency agglomerate in cytoplasm. Mesoporous silica materials have been broadly applied in field of catalysts, adsorbents, nanoreactors, and drug carriers due to its unique mesoporous structure, highly comparative surface area, good stability and biocompatibility. Therefore, coating gold nanorods with a dendritic mesopore channels can effectively prevent particle agglomeration, while increasing the specific surface area and drug loading efficiency. This review discusses the advancements of GNR@MSN in synthetic process, bio‐imaging technique and tumor therapy. Additionally, the further application of GNR@MSN in imaging‐guided treatment modalities is explored, while its promising superior application prospect is highlighted. Finally, the issues related to in vivo studies are critically examined for facilitating the transition of this promising nanoplatform into clinical trials.
摘要：
The development of highly selective Janus Kinase 1 (JAK1) inhibitors is crucial for improving efficacy and minimizing adverse effects in the clinical treatment of autoimmune diseases. In a prior study, we designed a series of C-5 4-pyrazol substituted pyrrolopyridine derivatives that demonstrated significant potency against JAK1, with a 10∼20-fold selectivity over Janus Kinase 2 (JAK2). Building on this foundation, we adopted orthogonal strategy by modifying the C-5 position with 3-pyrazol/4-pyrazol/3-pyrrol groups and tail with substituted benzyl groups on the pyrrolopyridine head to enhance both potency and selectivity. In this endeavor, we have identified several compounds that exhibit excellent potency and selectivity for JAK1. Notably, compounds 12b and 12e, which combined 4-pyrazol group at C-5 site and meta-substituted benzyl tails, displayed IC(50) value with 2.4/2.2nM and high 352-/253-fold selectivity for JAK1 over JAK2 in enzyme assays. Additionally, both compounds showed good JAK1-selective in Ba/F3-TEL-JAK1/2 cell-based assays. These findings mark a substantial improvement, as these compounds are 10-fold more potent and over 10-fold more selective than the best compound identified in our previous study. The noteworthy potency and selectivity properties of compounds 12b and 12e suggest their potential utility in furthering the development of drugs for autoimmune diseases.
作者机构：
[Wang, Hongqing; Xiao, Qianxiang; Li, Na; Meng, Lingyuan; Yan, Zhe; Wang, Xiao-Feng; Cao, Meng; Tan, Chunhong] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Tan, Chunhong] Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Peoples R China.
通讯机构：
[Xiao, QX; Wang, XF ; Tan, CH] U;[Tan, CH ] C;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Peoples R China.
摘要：
We report the controlled preparation of kinetically and thermodynamically luminescent multinuclear cuprous coordination complexes. On reaction of the bidentate P/N-ligand (2-(diphenylphosphino)pyridine, abbreviated as dppy) and copper(I) with a similar stoichiometry but in different concentration conditions at ambient temperature, hexagonal crystals of [Cu-2(mu-dppy)(3)Cl]PF6 center dot CH2Cl2 (1) or polyhedron crystals of [Cu-4(mu-dppy)(6)Cl](PF6)(3) (2) were formed as kinetic or thermodynamic products, respectively. Investigation of the structures, morphologies, theoretical calculation, and photophysical properties of the multinuclear cuprous coordination complexes demonstrates the formation of and differences between kinetically and thermodynamically stable conformations. Single-crystal X-ray structural analyses indicated that 1 features the head-to-head orientation dppy bridged dinuclear trefoil-like Cu-2-core with one terminal Cl-, and tetranuclear 2 can be regarded as a Cl- bridged dimer of 1 with two-third flipping head-to-tail dppy ligands. The density functional theory (DFT) calculations demonstrated that 2 had a lower frontier molecular orbital energy than 1, with an energy difference of 320.76 kJ/mol. Intriguingly, the controllable reversible transformation between 1 and 2 can be achieved under suitable conditions. By soaking the crystal in the mother liquor or alcohol, the kinetically stable 1 can slowly transform to the thermodynamically stable 2, or conversely, 2 can also quickly reconstruct to 1 when it is soaked in a chloride solution. Steadily changing morphologies, photoluminescence, as well as powder X-ray diffraction patterns were observed during the gradual transformation process. Based on structural analyses, a feasible transforming mechanism was proposed. The energetic and structural analyses of and the interconversion process between kinetically and thermodynamically stable multicuprous complexes here provide insights into the relations among the structures, morphologies, and properties of the metal-organic coordination materials at the molecular level. [GRAPHICS]
摘要：
Self -assembled nanomaterials have aroused enormous interest owing to their enhanced physicochemical properties as compared to monomers. Herein, two-dimensional Nd-based polyoxometalate clusterphene (Nd-POMCene) with a highly ordered honeycomb structure is synthesized by self -assembly, which is demonstrated with efficient photocatalytic degradation performance towards organic dyes, such as Rhodamine B (RhB), methylene blue, and crystal violet. Especially, RhB can be totally photodegraded by Nd-POMCene under the simulated sunlight within 1 h while a degraded efficiency of 97.50 % can be achieved under natural light within 2 h. As proved by the density functional theory results, the highly ordered structure of POMCene is beneficial for enhancing photocatalytic performance associated with the improved separation/transmission of photogenerated electron/hole pairs and large-scale electron delocalization. The mechanism study provides compelling evidence to demonstrate that all of holes, hydroxyl radicals, and superoxide radicals chemically account for the efficient photodegradation by Nd-POMCene. Finally, it is verified that there is much less toxicity in the degradation products of RhB.
