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Chinese Journal of Chemistry 2024年第10期42卷 1128-1132页

作者： Chao Li Lei Chen Hongye Wang Zixi Yan Bin Lyu Weiping Lyu Changwei Jiang Dehua Lu Jiaxing Li Ning Jiao Song Song state key laboratory of natural and Biomimetic Drugs School of Pharmaceutical SciencesPeking UniversityXue Yuan Rd.38Beijing 100191China

A mild and practical method for synthesizing fluorinated quinoline derivatives,which have a wide range of applications in pharmaceuticals,materials,and organic synthesis,was described through C—F bond insertion into indoles using CHBr_(2)*** simple conditions,readily availability of CHBr_(2)F,as well as the versatility of the transformations make this strategy very powerful in synthesizing 3-fluoroquinoline and *** mechanistic studies reveal that bromofluorocarbene generated in-situ under basic condition was the key intermediate.

关键词： Skeleton edit Fluorocarbene Ring expansion Quinoline Quinolone

Rapid and controllable in-situ self-assembly of main-group metal nanofilms for highly efficient CO_(2)electroreduction to liquid fuel in flow cells

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Nano Research 2024年第6期17卷 5718-5725页

作者： Miao Wang Huaizhu Wang Yaoda Wang Junchuan Liang Mengfei Zhu Jiarui Li Zuoxiu Tie Zhong Jin state key laboratory of Coordination Chemistry MOE Key Laboratory of Mesoscopic ChemistryMOE Key Laboratory of High Performance Polymer Materials and TechnologyJiangsu Key Laboratory of Advanced Organic MaterialsTianchang New Materials and Energy Technology Researc

The electrocatalytic reduction of CO_(2)is a promising pathway to generate renewable fuels and ***,its advancement is impeded by the absence of electrocatalysts with both high selectivity and ***,we present a scalable in-situ thermal evaporation technique for synthesizing series of Bi,In,and Sn nanofilms on carbon felt(CF)substrates with a high-aspect-ratio *** resulting main-group metal nanofilms exhibit a homogeneously distributed and highly exposed catalyst surface with ample active sites,thereby promoting mass transport and ad-/desorption of reaction *** from the unique fractal morphology,the Bi nanofilms deposited on CF exhibit optimal catalytic activities for CO_(2)electroreduction among the designed metal nanofilms electrodes,with the highest Faradaic efficiency of 96.9%for formate production at−1.3 V *** hydrogen electrode(RHE)in *** an industrially relevant current density of 221.4 mA·cm−2 in flow cells,the Bi nanofilms retain a high Faradaic efficiency of 81.7%at−1.1 V(***)and a good long-term stability for formate ***,a techno-economic analysis(TEA)model shows the potential commercial viability of electrocatalytic CO_(2)conversion into formate using the Bi nanofilms *** results offer a green and convenient approach for in-situ fabrication of stable and inexpensive thin-film catalysts with a fractal structure applicable to various industrial settings.

关键词： CO_(2)electroreduction non-noble metal nanofilms flow cells efficiency and selectivity techno-economic analysis

Traditional Chinese medicine Pien-Tze-Huang ameliorates LPS-induced sepsis through bile acid-mediated activation of TGR5-STAT3-A20 signalling

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Journal of Pharmaceutical Analysis 2024年第4期14卷 601-614页

作者： Bei Li Yong Zhang Xinyuan Liu Ziyang Zhang Shuqing Zhuang Xiaoli Zhong Wenbo Chen Yilin Hong Pingli Mo Shuhai Lin Shicong Wang Chundong Yu state key laboratory of Cellular Stress Biology School of Life SciencesXiamen UniversityXiamen361102China Fujian Pien Tze Huang Enterprise key laboratory of natural medicine Research and Development ZhangzhouFujian363000China Xiang'an Hospital of Xiamen University School of MedicineXiamen UniversityXiamen361005China Department of Cardiology Xiamen Key Laboratory of Cardiac ElectrophysiologyXiamen Institute of Cardiovascular DiseasesThe First Affiliated Hospital of Xiamen UniversitySchool of MedicineXiamen UniversityXiamen361003China

Pien Tze Huang(PZH),a class-1 nationally protected traditional Chinese medicine(TCM),has been used to treat liver diseases such as hepatitis;however,the effect of PZH on the progression of sepsis is ***,we reported that PZH attenuated lipopolysaccharide(LPS)-induced sepsis in mice and reduced LPS-induced production of proinflammatory cytokines in macrophages by inhibiting the activation of mitogen-activated protein kinase(MAPK)and nuclear factor-kappa B(NF-κB)***,PZH stimulated signal transducer and activator of transcription 3(STAT3)phosphorylation to induce the expression of A20,which could inhibit the activation of NF-κB and MAPK *** of the bile acid(BA)receptor G protein-coupled bile acid receptor 1(TGR5)in macrophages abolished the effects of PZH on STAT3 phosphorylation and A20 induction,as well as the LPS-induced inflammatory response,suggesting that BAs in PZH may mediate its anti-inflammatory effects by activating ***,deprivation of BAs in PZH by cholestyramine resin reduced the effects of PZH on the expression of phosphorylated-STAT3 and A20,the activation of NF-κB and MAPK signalling,and the production of proinflammatory cytokines,whereas the addition of BAs to cholestyramine resin-treated PZH partially restored the inhibitory effects on the production of proinflammatory ***,our study identifies BAs as the effective components in PZH that activate TGR5-STAT3-A20 signalling to ameliorate LPS-induced sepsis.

关键词： Pien Tze Huang Bile acids Sepsis Inflammation TGR5 STAT3-A20 signalling

Organocatalytic radical aminoacylation of alkenes forβ-aminoketone synthesis

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Science China Chemistry 2024年

作者： Ayisenbati Jialingbieke Xinying Hu Zuquan Liu Xiyun Lin Yiwen Yin Jibin Li Yatian Huang Ding Du state key laboratory of natural medicines School of Science China Pharmaceutical University

An NHC organocatalytic radical aminoacylation of alkenes has been developed by using aldehydes as the acylating reagents and activated aryloxy-amides as the N-radical precursors, providing a new platform for modular access to highly functionalized β-aminoketones. The key to the success of this reaction relies on the single electron transfer(SET) event between the enolates of Breslow intermediates and carefully screened N-radical precursors, followed by a radical addition and radical-radical coupling relay process. The protocol features simple and readily available materials(abundant and feed-stock aldehydes and alkenes),mild reaction conditions(metal-, photo-and oxidant-free, in EA at room temperature), easily removable protecting group for late-stage functionalization.

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Photocaged activity-based probes for improved monitoring of protein S-sulfenylation in living cells

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Chinese Chemical Letters 2024年第2期35卷 451-454页

作者： Jiahao Zhang Haiyue Peng Zi'an Chen Guorui Li Jing Huang state key laboratory of Chemo/Biosensing and Chemometrics Hunan Provincial Key Laboratory of Animal Models and Molecular MedicineSchool of Biomedical SciencesHunan UniversityChangsha 410082China

Protein S-sulfenylation(protein sulfenic acid),as one of the most significant oxidative post-translational modifications(OxiPTMs),plays a vital role in regulating protein function.A variety of activity-based probes have been developed to profile sulfenic acid in living ***,due to the transient presence and low content of sulfenic acid in living cell,high doses of probes are needed to achieve efficient *** importantly,current probes have no temporal control over sulfenic acid *** overcome these limitations,two caged cysteine sulfenic acid probes DYn-2-ONB and DYn-2-Cou with either an o-nitrobenzyl or coumarin protecting group were developed in this *** probes can be efficiently uncaged via irradiation to produce the active C-nucleophile probe *** assay in living cells demonstrated DYn-2-ONB exhibited better labeling capacity compared with DYn-2,providing it as a powerful tool for improved monitoring of protein S-sulfenylation in living cells.

关键词： Cysteine Sulfenic acid Activity-based probe Photocage Light activation Protein S-sulfenylation

Energy transfer, anticounterfeiting, white light emission and sensing in fine-regulating series of lanthanide metal-organic frameworks

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Journal of Rare Earths 2024年第3期42卷 446-454,I0001页

作者： Juanjuan Xue Yao Wang Guoping Yang Yaoyu Wang key laboratory of Synthetic and natural Functional Molecule Chemistry of the Ministry of Education Shaanxi Key Laboratory of Physico-Inorganic ChemistryCollege of Chemistry&Materials ScienceNorthwest UniversityXi'an710127China

Three lanthanide ions and a rigid(1,1'-biphenyl)-2,4,6-tricarboxylic acid(H_(3)bptc) ligand led to the isostructural lanthanide metal-organic frameworks(Ln-MOFs) {[Ln(bptc)(H_(2)O)_(3)]·3H_(2)O}_n(Lnbptc, Ln = Eu,Tb, Gd, Eu_(x)Tb_(1—x), Eu_(x)Gd_(1-x), Tb_(x)Gd_(1-x), and Eu_(0.12)Tb_(0.52)Gd_(0.36)). The density functional theory(DFT) and time-dependent DFT calculation were expanded on H_3bptc, which point to the occurrence of “antenna effect”. The minor diameter samples of Eubptc, Tbbptc, and Gdbptc can also be attained via the microwave synthesis and employed for handwriting anticounterfeiting. Interestingly, the typical red emission of Eu^(3+) and green emission of Tb~(3+) could be fine-tuned by Gd^(3+) via chemical mixing to be full-color emissions bimetallic doped Eu_(x)Tb_(1-x)bptc, Eu_(x)Gd_(1-x)bptc, and Tb_(x)Gd_(1-x)bptc. The above synthetic bimetallic MOFs can be fixed in positioning boxes of quick response(QR) codes with diverse emission for anticounterfeiting. The message can be decoded under the irradiation of 365 nm ultraviolet lamp while invisible in the daylight. Notably, the trimetallic doped Eu_(0.12)Tb_(0.52)Gd_(0.36)bptc emits white light with the CIE color coordinate(0.34, 0.34). Furthermore, Tbbptc is demonstrated to be a sensitive probe toward nitrobenzene and acetone with multiple mechanisms.

关键词： Metal-organic frameworks Anticounterfeiting White light-emitting Sensing Rare earths

Recent advances in protein conformation sampling by combining machine learning with molecular simulation

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Chinese Physics B 2024年第3期33卷 80-87页

作者：唐一鸣杨中元姚逸飞周运谈圆王子超潘瞳熊瑞孙俊力韦广红 Department of Physics State Key Laboratory of Surface Physicsand Key Laboratory for Computational Physical Sciences (Ministry of Education)Shanghai 200438China

The rapid advancement and broad application of machine learning(ML)have driven a groundbreaking revolution in computational *** of the most cutting-edge and important applications of ML is its integration with molecular simulations to improve the sampling efficiency of the vast conformational space of large *** review focuses on recent studies that utilize ML-based techniques in the exploration of protein conformational *** first highlight the recent development of ML-aided enhanced sampling methods,including heuristic algorithms and neural networks that are designed to refine the selection of reaction coordinates for the construction of bias potential,or facilitate the exploration of the unsampled region of the energy ***,we review the development of autoencoder based methods that combine molecular simulations and deep learning to expand the search for protein ***,we discuss the cutting-edge methodologies for the one-shot generation of protein conformations with precise Boltzmann ***,this review demonstrates the promising potential of machine learning in revolutionizing our insight into the complex conformational ensembles of proteins.

关键词： machine learning molecular simulation protein conformational space enhanced sampling

Revealing the Structure-Property Difference of natural Rubber Prepared by Different Methods: Protein and Gel Content are key Factors

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Chinese Journal of Polymer Science 2024年第4期42卷 457-467页

作者： Shao-Qi Huang Jun-Qi Zhang Yong Zhu Ling-Min Kong Lu-Sheng Liao Fu-Quan Zhang Zheng-Tian Xie Jin-Rong Wu state key laboratory of Polymer Materials Engineering College of Polymer Science and EngineeringSichuan UniversityChengdu610065China Hainan Provincial key laboratory of natural Rubber Processing Agricultural Products Processing Research Institute of Chinese Academy of Tropical Agricultural SciencesZhanjiang524001China

natural rubber (NR) is widely used in various fields including aerospace, military industry and transportation due to its superior elasticity and comprehensive mechanical properties. Nonetheless, the commercial NR prepared by different methods usually exhibits different mechanical properties, primarily due to variations in processing conditions during the conversion from latex to bulk rubber material. Consequently, this poses challenges in scientific research and industrial production of NR. In order to assess the properties of various commercially available NR and identify key structural and compositional components, this study systematically compares and analyzes four representative NR raw materials: air dried sheet (ADS), ribbed smoked sheets (RSS), constant viscidity NR (CV), and whole field latex rubber (WF). The investigation focuses on evaluating their static mechanical behavior, SIC behavior, wear resistance, and fatigue resistance. The findings indicate that protein and gel content exhibit a crucial influence on the NR properties. These constituents contribute to the formation of a high-crosslinking density region, generating a heterogeneous network structure within the rubber. This structure amplifies strains during deformation, leading to earlier and stronger strain-induced crystallization (SIC). Among the four commercial NR brands, RSS demonstrates superior overall mechanical and dynamic properties owing to its high protein and gel content. This study serves as a valuable reference for comprehending the differences in properties among various commercial NR, thereby offering guidance for the actual processing and selection of NR.

关键词： natural rubber Processingmethod Protein Gel content Property

Bazi Bushen alleviates reproductive aging in aged male mice

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Chinese Journal of natural medicines 2024年第5期22卷 416-425页

作者： MA Kun LI Mengnan SONG Yahui MAO Xinjing ZHANG Shaolan ZHANG Yaping JIANG Yuning JI Chuanyuan NIU Kunxu LI Hongrong HOU Yunlong WEI Cong Graduate School Hebei University of Chinese MedicineShijiazhuang 050091China state key laboratory for Innovation and Transformation of Luobing Theory Shijiazhuang 050035China key laboratory of state Administration of TCM(Cardio-Cerebral Vessel Collateral Disease) Shijiazhuang 050035China College of Traditional Chinese medicine·College of Integrated Traditional Chinese and Western medicine Nanjing University of Chinese MedicineNanjing 210023China Hebei Provincial key laboratory of Luobing Shijiazhuang 050035China key Disciplines of state Administration of TCM for Luobing Shijiazhuang 050035China

Bazi Bushen(BZBS),a traditional Chinese medicine(TCM),has demonstrated therapeutic efficacy in testicular dysfunction within D-galactose and NaNO_(2)mouse *** study aimed to ascertain if BZBS could also mitigate the decline in testicular function associated with natural ***,male aged mice were employed to evaluate the preventive effects of BZBS on male reproductive *** was achieved by assessing sex hormone production,testicular histomorphology,and *** to the untreated aged control group,BZBS administration elevated the levels of sex hormones and spermatocyte populations and preserved normal testicular structure in aged ***,spermatogenesis was *** analyses,including malondialdehyde(MDA)assays and real-time PCR,indicated that BZBS diminished testicular oxidative stress and the inflammatory *** these findings,mice treated with BZBS exhibited reductions in the populations of senescent and apoptotic cells within the seminiferous tubules,suggesting alleviated cellular *** contrast,we observed that rapamycin,a drug known for its longevity benefits,induced excessive testicular apoptosis and did not decrease lipid ***,our results highlight BZBS’s promising clinical potential in counteracting male reproductive aging,underlining its mechanisms of action.

关键词： Traditional Chinese medicine Male reproductive aging Spermatogenic cells Cell senescence Apoptosis

A High-Performance Electrochemical Analysis Platform for Ultrasensitive Detection of HTLV-1 DNA: Integrating Cascade Signal Amplifi cation with λ-Exonuclease-Assisted Target Recycling and Enzyme Catalysis

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Journal of Analysis and Testing 2024年第03期8卷 361-373页

作者： Qi Xiao Shuai Liu Yali Wang Huihao Li Mingli Yang Yi Fang Sijing Chen Shan Huang Guangxi key laboratory of natural Polymer Chemistry and Physics College of Chemistry and Materials Nanning Normal University

Human T-cell lymphophilic virus type 1 (HTLV-1), the known retrovirus causing cancer in humans, is closely associated with adult T-cell leukemia/lymphoma and HTLV-1 associated myelopathy/tropical spastic paraparesis. Due to its ability to evade the host's defense mechanisms, early tracking of HTLV-1 becomes crucial. In this study, we integrateλ-Exonuclease(λ-Exo)-assisted target recycling with a terminal deoxynucleotidyl transferase (TdT)-mediated template-free DNA extension process to develop an electrochemical analysis platform for the specifi c and sensitive detection of HTLV-1 DNA. During theλ-Exo-assisted target recycling, HTLV-1 DNA is recognized by hairpin DNA (Hp-DNA), forming double-stranded DNA(dsDNA) through DNA hybridization. The dsDNA, featuring blunt 5'terminal phosphorylation, is cleaved byλ-Exo, generating abundant short output sequence (sDNA). HTLV-1 DNA is released, initiating a cyclic hybridization-cleavage ***, thiol-labelled capture DNA (CP-DNA) assembled on gold electrode surface captures a substantial amount of the generated sDNA, forming CP-DNA-sDNA nanostructures. When TdT and dNTPs are present on the electrode surface, the3'-OH terminal of sDNA extends to generate long single-stranded DNA (ssDNA) structure. Methylene blue (MB) is selected as the electrochemical signal molecule. MB not only binds with ssDNA but also interacts specifi cally with dsDNA, resulting in a signifi cantly enhanced electrochemical signal on modifi ed electrode surface. The detection limit of HTLV-1 DNA is as low as 19 amol/L (S/N=3) when the two signal amplifi cation strategies are combined. The analysis platform exhibits excellent analytical performance and holds promise as a novel tool for the early tracing and diagnosis of HTLV-1 DNA.

关键词： Cascade signal amplification Electrochemical DNA sensor Enzyme-assisted target recycling HTLV-1 DNA