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Carrimycin inhibits coronavirus replication by decreasing the efficiency of programmed–1 ribosomal frameshifting through directly binding to the RNA pseudoknot of viral frameshift-stimulatory element

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Acta Pharmaceutica Sinica B 2024年第6期14卷 2567-2580页

作者： Hongying Li Jianrui Li Jiayu Li Hu Li Xuekai Wang Jing Jiang Lei Lei Han Sun Mei Tang Biao Dong Weiqing He Shuyi Si Bin Hong Yinghong Li Danqing Song Zonggen Peng Yongsheng Che Jian-Dong Jiang CAMS Key Laboratory of Antiviral Drug Research Institute of Medicinal BiotechnologyChinese Academy of Medical Sciences&Peking Union Medical CollegeBeijing 100050China Beijing Key Laboratory of Antimicrobial Agents Institute of Medicinal BiotechnologyChinese Academy of Medical Sciences&Peking Union Medical CollegeBeijing 100050China Key Laboratory of Biotechnology of Antibiotics the National Health and Family Planning Commission(NHFPC)Institute of Medicinal BiotechnologyChinese Academy of Medical Sciences&Peking Union Medical CollegeBeijing 100050China

The pandemic of SARS-CoV-2 worldwide with successive emerging variants urgently calls for small-molecule oral drugs with broad-spectrum antiviral ***,we show that carrimycin,a new macrolide antibiotic in the clinic and an antiviral candidate for SARS-CoV-2 in phase III trials,decreases the efficiency of programmed–1 ribosomal frameshifting of coronaviruses and thus impedes viral replication in a broad-spectrum *** binds directly to the coronaviral frameshift-stimulatory element(FSE)RNA pseudoknot,interrupting the viral protein translation switch from ORF1a to ORF1b and thereby reducing the level of the core components of the viral replication and transcription *** carrimycin with known viral replicase inhibitors yielded a synergistic inhibitory effect on *** the FSE mechanism is essential in all coronaviruses,carrimycin could be a new broad-spectrum antiviral drug for human coronaviruses by directly targeting the conserved coronaviral FSE *** finding may open a new direction in antiviral drug discovery for coronavirus variants.

关键词： Carrimycin Coronavirus Broad-spectrum antiviral activity Programmed-1 ribosomal frameshifting RNA pseudoknot Antiviral agent RNA target Synergistic inhibitory effect

The chlorine evolution reaction promoted by organocatalysts with amide functional groups

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Science China chemistry 2024年第3期67卷 749-750页

作者： Lan Zhao Liang-Nian He State Key Laboratory and institute of Elemento-Organic chemistry College of ChemistryNankai UniversityTianjin 300071China

Since the nineteenth century, the chlor-alkali process entails the electrochemical oxidation of sodium chloride solutions to Cl_(2) by the chlorine evolution reaction(CER) and the simultaneous production of sodium hyd... 详细信息

关键词： chlorine hydroxide promoted

Ink-structing the future of vascular tissue engineering:a review of the physiological bioink design

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Bio-Design and Manufacturing 2024年第2期7卷 181-205页

作者： Judith Synofzik Sebastian Heene Rebecca Jonczyk Cornelia Blume institute for Technical chemistry Leibniz University Hannover30167 HannoverGermany

Three-dimensional(3D)printing and bioprinting have come into view for a plannable and standardizable generation of implantable tissue-engineered constructs that can substitute native tissues and *** tissue-engineered structures are intended to integrate with the patient’s *** tissue engineering(TE)is relevant in TE because it supports the sustained oxygenization and nutrition of all tissue-engineered *** have a specific role,representingthenecessarymedium for printability and vascular cell *** review aims to understand the requirements for the design of vascular ***,an in-depth analysis of vascular cell interaction with their native environment must be gained.A physiological bioink suitable for a tissue-engineered vascular graft(TEVG)must not only ensure good printability but also induce cells to behave like in a native vascular vessel,including self-regenerative and growth *** review describes the general structure of vascular walls with wall-speciﬁc cell and extracellular matrix(ECM)components and biomechanical properties and ***,the physiological role of vascular ECM components for their interaction with vascular cells and the mode of interaction is *** currently available or imaginable bioinks are described from physiological matrix proteins to nonphysiologically occurring but natural chemical compounds useful for vascular *** physiological performance of these bioinks is evaluated with regard to biomechanical properties postprinting,with a view to current animal studies of 3D printed vascular ***,the main challenges for further bioink development,suitable bioink components to create a self-assembly bioink concept,and future bioprinting strategies are *** concepts are discussed in terms of their suitability to be part of a TEVG with a high potential for later clinical use.

关键词： Vascular wall histology Vascular cells Microenvironment Extracellular matrix Cell–matrix interaction Bioink Printability

Modularized viromimetic polymer nanoparticle vaccines(VPNVaxs) to elicit durable and effective humoral immune responses

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National Science Review 2024年第3期11卷 200-214页

作者： Zichao Huang Xinyu Zhuang Liping Liu Jiayu Zhao Sheng Ma Xinghui Si Zhenyi Zhu Fan Wu Ningyi Jin Mingyao Tian Wantong Song Xuesi Chen Key Laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of Sciences School of Applied chemistry and Engineering University of Science and Technology of China Changchun Veterinary Research institute Chinese Academy of Agricultural Sciences Jilin Biomedical Polymers Engineering Laboratory State Key Laboratory of Polymer Physics and chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences

Virus-like particle(VLP) vaccines had shown great potential during the COVID-19 pandemic, and was thought to be the next generation of antiviral vaccine technology due to viromimetic structures. However,the time-consuming and complicated processes in establishing a current recombinant-protein–based VLP vaccine has limited its quick launch to the out-bursting pandemic. To simplify and optimize VLP vaccine design, we herein report a kind of viromimetic polymer nanoparticle vaccine(VPNVax), with subunit receptor-binding domain(RBD) proteins conjugated to the surface of polyethylene glycol-b-polylactic acid(PEG-b-PLA) nanoparticles for vaccination against SARS-CoV-2. The preparation of VPNVax based on synthetic polymer particle and chemical post-conjugation makes it possible to rapidly replace the antigens and construct matched vaccines at the emergence of different viruses. Using this modular preparation system, we identified that VPNVax with surface protein coverage of 20%–25% had the best immunostimulatory activity, which could keep high levels of specific antibody titers over 5 months and induce virus neutralizing activity when combined with an aluminum adjuvant. Moreover, the polymer nano-vectors could be armed with more immune-adjuvant functions by loading immunostimulant agents or chemical chirality design. This VPNVax platform provides a novel kind of rapidly producing and efficient vaccine against different variants of SARS-CoV-2 as well as other viral pandemics.

关键词： vaccine polymer nanomaterials SARS-CoV-2

General radical difluoromethylation using difluoroacetic anhydride via photoredox catalysis

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Science China chemistry 2024年第8期67卷 2637-2646页

作者： Meng He Yankai Yang Heng Zhang Zhipeng Guan Zhi-Bing Dong Hong Yi Aiwen Lei School of chemistry and Environmental Engineering Wuhan Institute of TechnologyWuhan 430205China College of chemistry and Molecular Sciences and institute for Advanced Studies(IAS) Wuhan UniversityWuhan 430072China

CF_(2)H-containing molecules play pivotal roles in diverse fields from medicinal chemistry to materials science. However, the application of existing CF_(2)H reagents as a source of CF_(2)H radical is limited by their reactivity and preparation. Herein, we develop a simple and general visible-light-catalyzed radical difluoromethylation reaction of alkenes, dienes, and heteroaromatics using commercially available, easy-to-handle, and low-cost difluoroacetic anhydride as the CF_(2)H reagent. This scalable protocol enables the convenient synthesis of a range of CF_(2)H-containing compounds under mild conditions, exhibiting a broad substrate scope and functional group tolerance. Potential applications are further demonstrated by gram-scale synthesis, sunlight experiments, derivatization experiments as well as the synthesis of bioactive molecules.

关键词： radical difluoromethylation alkenes/dienes/heteroaromatics difluoroacetic anhydride photoredox

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Electrostatic and hydrophobic interaction cooperative nanochaperone regulates protein folding

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Aggregate

Aggregate 2024年第1期5卷 419-426页

作者： Xiaohui Wu Fei Deng Yujie Chen Mengchen Xu Feihe Ma Linqi Shi Key Laboratory of Functional Polymer Materials of Ministry of Education State Key Laboratory of Medicinal Chemical BiologyInstitute of Polymer Chemistry and College of ChemistryNankai UniversityTianjinP.R.China School of Materials Science and Engineering and State Key Laboratory of Separation Membranes and Membrane Processes Tiangong UniversityTianjinP.R.China

Natural molecular chaperones utilize spatially ordered multiple molecular forces to effectively regulate protein ***,synthesis of such molecules is a big *** concept of“aggregate science”provides insights to construct chemical entities(aggregates)beyond molecular levels to mimic both the structure and function of natural *** by this concept,herein we fabricate a novel multi-interaction(i.e.,electrostatic and hydrophobic interaction)cooperative nanochaperone(multi-co-nChap)to regulating protein *** multi-co-nChap is fabricated by rationally introducing electrostatic interactions to the surface(corona)and confined hydrophobic microdomains(shell)of traditional single-hydrophobic interaction *** demonstrate that the corona electrostatic attraction facilitates the diffusion of clients into the hydrophobic microdomains,while the shell electrostatic interaction balances the capture and release of *** finely synergizing corona electrostatic attraction with shell electrostatic repulsion and hydrophobic interaction,the optimized multi-co-nChap effectively facilitated de novo folding of nascent ***,the synergy between corona electrostatic attraction,shell electrostatic attraction and shell hydrophobic interaction significantly enhanced the capability of multi-co-nChap to protect native proteins from denaturation at harsh *** work provides important insights for understanding and design of nanochaperone,which is a kind of ordered aggregate with chaperone-like activity that beyond the level of single molecule.

关键词： chaperone-like activity cooperative effect nanochaperones ordered aggregates protein folding

Advancements in synthetic and electrocatalytic exploitation of guest-host intercalated 2D materials

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Progress in Natural Science:Materials International 2024年第3期34卷 454-469页

作者： Qian Yang Kun Wang Meiling Zhang Feihong Du Jiayang Li Chen Zheng Jinyang Li School of chemistry Southwest Jiaotong University Yibin institute of Southwest Jiaotong University

The emergence and development of layered materials have shown great promise for many applications, especially in recent years, the effective modulation of the physicochemical properties of layered materials by intercalation chemistry has led to great potential in material design. In this paper, we review the reaction mechanisms of different guest species(metal atoms/ions, organic molecules/ions, inorganic molecules and inorganic ions)intercalated into the host layered materials as well as the recent progress. It is also reviewed that layered intercalated materials with controllable structure and tunable physicochemical properties can be prepared through the occurrence of interactions between different subjects and guests. The specific applications of intercalation chemistry in the field of electrocatalysis, such as the hydrogen evolution reaction, oxygen evolution reaction, oxygen reduction reaction and other electrocatalytic reactions, are then discussed, with emphasis on the mechanism of the improved catalytic activity and stability of the layered materials after guest intercalation.

关键词： Electrocatalysis Guest species Intercalation chemistry Layered materials

Structural insight into the dual-antagonistic mechanism of AB928 on adenosine Areceptors

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Science China Life Sciences 2024年

作者： Yuan Weng Xinyu Yang Qiansen Zhang Ying Chen Yueming Xu Chenyu Zhu Qiong Xie Yonghui Wang Huaiyu Yang Mingyao Liu Weiqiang Lu Gaojie Song Shanghai Key Laboratory of Regulatory Biology Institute of Biomedical Sciences and School of Life Sciences East China Normal University Department of medicinal chemistry School of Pharmacy Fudan University

The adenosine subfamily G protein-coupled receptors A2AR and A2BR have been identified as promising cancer immunotherapy *** of the A2AR/A2BR dual antagonists, AB928, has progressed to a phase II clinical trial to treat rectal cancer. However, the precise mechanism underlying its dual-antagonistic properties remains elusive. Herein, we report crystal structures of the A2AR complexed with AB928 and a selective A2AR antagonist 2-118. The structures revealed a common binding mode on A2AR, wherein the ligands established extensive interactions with residues from the orthosteric and secondary pockets. In contrast, the cAMP assay and A2AR and A2BR molecular dynamics simulations indicated that the ligands adopted distinct binding modes on A2BR. Detailed analysis of their chemical structures suggested that AB928 readily adapted to the A2BR pocket, while 2-118 did not due to intrinsic differences. This disparity potentially accounted for the difference in inhibitory efficacy between A2BR and A2AR. This study serves as a valuable structural template for the future development of selective or dual inhibitors targeting A2AR/A2BR for cancer therapy.

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Compositional evolution for mixed aerosols containing gluconic acid and typical nitrate and the effect of multiply factors on hygroscopicity

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Journal of Environmental Sciences 2024年第5期139卷 206-216页

作者： Yue Zhu Shufeng Pang Yunhong Zhang School of chemistry and Chemical Engineering Beijing Institute of TechnologyBeijing 100081China

The aging process of atmospheric aerosols usually leads to a mixture of inorganic salts and organic compounds of anthropogenic *** organic compounds,polyhydroxy organic acids are important components,however,the study on composition and hygroscopic properties of the mixture containing inorganics and polyhydroxy organic acids is *** this study,gluconic acid,the proxy of polyhydroxy organic acids,is mixed with the representative nitrate(Mg(NO_(3))_(2),Ca(NO_(3))_(2))to form ***-FTIR and optical microscopy are employed to study the component changes and hygroscopicity as a function of relative *** relative humidity fluctuates,the FTIR-ATR spectra display that the internal mixed gluconic acid(CH_(2)(CH)_(4)(OH)_(5)COOH)and nitrate can react to release acidic gases,forming relevant gluconate and further affecting the *** specific presentation is particles cannot be recovered to their original size after the dehydration-hydration process and there will be some disparities in GF for mixed *** the gluconic acid-Ca(NO_(3))_(2)/Mg(NO_(3))_(2)mixtures with molar ratios of 1:1,higher degree of reaction resulting in the production of large amounts of gluconate should be responsible to the lower hygroscopicity compared to ZSR *** 1:2 gluconic acid-nitrate mixed systems(with higher nitrate content),the hygroscopicity of mixtures are higher than the ZSR prediction.A possible reason could be‘salt-promoting effect’on the organic fractions of the surplus inorganic salt in the *** data can improve the chemical composition list evaluation,in turn hygroscopic properties and phase state of atmospheric aerosol,and then the climate effect.

关键词： Hygroscopicity Gluconic acid Reaction ZSR simulation Size growth factors