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CCS Chemistry 2024年第7期6卷 1698-1711页

作者： Zhongtang Li Xiaoyu Sun Yuchao Wang Ao Sun Linbo Fu Tongtong Geng Zihui Zhang Ximin Lv Qian Wang Jing Wang Baodi Gou Xiangbao Meng Zhongjun Li state key lab.ratory of natural and Biomimetic drugs School of Pharmaceutical SciencesPeking UniversityBeijing 100191

Capsular polysaccharides(CPS)of Colwellia psychrerythraea 34H consist of linear tetrasaccharides repeating units in a glycosaminoglycan-like *** biological function is likely involved in the cold adaptation of microbial *** low availab.lity of these glycosaminoglycan structures greatly limits the study of their functions and biological ***,an efficient semisynthetic strategy for CPS tetrasaccharide derivatives is achieved by using disaccharide units degraded from hyaluronic *** new synthetic process is suitable for largescale preparation,and several rare tetrasaccharide derivatives containing GalA-GalNAc were readily obtained in high *** evaluation of their anti-inflammatory effects demonstrated that these CPS tetrasaccharides effectively attenuated the lipopolysaccharide-induced sepsis and acute lung injury by decreasing macrophage infiltration and secretion of microphage-related cytokines in *** these results suggest that this new type of CPS tetrasaccharide can be developed as an anti-inflammation agent.

关键词： glycosaminoglycan oligosaccharide glycosylation anti-inflammatory agent acute lung injury

Structural transformation from Waugh-type to Keggin-type polyoxomolybdate-based crystalline material for photo/electrocatalysis

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Rare Metals 2024年第5期43卷 2241-2250页

作者： Pei-Sen Wang Zi-Tong Wang Ya-Ya Tan Peng Chen Xue-Cheng Zhang Lu-Nan Zhang Yong-Ge Wei Lu-Bin Ni School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China key lab.of Organic Optoelectronics and Molecular Engineering of Ministry of Education Department of ChemistryTsinghua UniversityBeijing 100084China state key lab.ratory of natural and Biomimetic drugs Peking UniversityBeijing100191China

An inorganicDorganic hybrid crystalline material(SiMo_(12)O_(40))[Cu(2,2'-bipy)_(2)]_(2)·2H_(2)O(Complex 1,2,2'-bipy=2,2'-bipyridine)was synthesized for the first time by using 2,2'-bipy and transition metal copper to convert Waugh-type polyoxometalate[MnMo_(9)O_(3)_(2)]_(6-)into a Keggin polyoxometalate structure[SiMo_(12)O_(40)]^(4-)under hydrothermal conditions in glass *** crystal tests and a series of characterizations were carried out on Complex *** structure of Complex 1 is composed of[SiMo_(12)O_(40)]^(4-)and[Cu^(Ⅱ)(2,2'-bipy)_(2)]^(2+).The five-coordinated Cu is connected to two 2,2'-bipy through CuDN bonds,forming an approximately square ***,Complex 1 exhibited good photocatalytic performance for methylene blue degradation and electrocatalytic nitrite reduction properties simultaneously.

关键词： Polyoxometalates Inorganic-organic hybrid materials Photocatalytic Electrocatalytic

Biodegradation of Crystalline Chitin: A Review of Recent Advancement, Challenges, and Future Study Directions

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Journal of Ocean University of China 2024年第5期23卷 1319-1328页

作者： SONG Jianlin SU Haipeng SUN Jianan MAO Xiangzhao Sanya Institute of Oceanography Ocean University of China state key lab.ratory of Marine Food Processing and Safety Control College of Food Science and Engineering Ocean University of China Qingdao key lab.ratory of Food Biotechnology key lab.ratory of biological Processing of Aquatic Products China National Light Industry lab.ratory for Marine drugs and Bioproducts of Laoshan lab.ratory

Chitin is the second most abundant renewable polysaccharide on Earth. The degradation of chitin into soluble and bioactive N-acetyl chitooligosaccharides(NCOSs) and N-acetyl-D-glucosamine(GlcNAc) has emerged as a pivotal step in the efficient and sustainable utilization of chitin resources. However, because of its dense structure, high crystallinity, and poor solubility, chitin typically needs pretreatment via chemical, physical, and other methods before enzymatic conversion to enhance the accessibility between substrates and enzyme molecules. Consequently, there has been considerable interest in exploring the direct biological degradation of crystalline chitin as a cost-effective and environment-friendly technology. This review endeavors to present several biological methods for the direct degradation of chitin. We primarily focused on the importance of chitinase containing chitin-binding domain(CBD). Additionally, various modification strategies for increasing the degradation efficiency of crystalline chitin were introduced. Subsequently, the review systematically elucidated critical components of multi-enzyme catalytic systems, highlighting their potential for chitin degradation. Furthermore, the application of microorganisms in the degradation of crystalline chitin was also discussed. The insights in this review contribute to the explorations and investigations of enzymatic and microbial approaches for the direct degradation of crystalline chitin, thereby fostering advancements in biomass conversion.

关键词： biological degradation chitinase crystalline chitin engineering microorganisms

A proton-catalyzing prodrug for PDT and glycolysis inhibition-synergistic therapy of tumor in spatiotemporal dimensions

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Science China Chemistry 2024年第9期67卷 3162-3178页

作者： Miao Li Xueying Sun Xiuqin Ma Yang Tan Xiaoyi Jin Yi Wang Fan Yang Qian Li Honglei Zhan Xiaojun Peng School of biological Engineering Dalian Polytechnic UniversityDalian 116034China state key lab.ratory of Fine Chemicals Dalian University of TechnologyDalian 116024China

The reactive oxygen species(ROS)generation from photosensitizer in photodynamic therapy(PDT)is limited by tumor *** type-I photosensitizers,e.g.,sulfur-substituted Nile blue,still rely on oxygen as the main center for transferring electrons to generate *** off the pathway of oxygen consumption in tumor can help photosensitizers overcome the limitation of low oxygen,in order to efficiently generate more *** is known that glycolysis inhibitor 3-bromopyruvic acid(3-BP),which could specially target mitochondria,can provide more oxygen by inhibiting oxidative ***,we successfully designed and synthesized a new 3-BP-coupled sulfur-substituted Nile blue as prodrug(NBBP)for chemical/photodynamic synergistic *** results indicated that the protons in tumor catalyzed the hydrolysis of NBBP,inhibited photoinduced electron transfer between 3-BP and the photosensitizer in NBBP and further assisted the photosensitizer to be localized in mitochondria,utilizing local oxygen as much as possible and kill tumor cells more ***,the glycolysis inhibition-induced autophagy was combined with PDT-induced autophagy,which could promote the deaths of tumor *** other remedies exploiting nanomaterials,this construction method of NBBP achieves the efficient synergy of photodynamic therapy and glycolysis inhibition,stronger than their theoretical addition,in spatiotemporal *** study provides not only a highly efficient platform for tumor therapy but also a design approach for prodrugs with synergistic effects.

关键词： photodynamic therapy prodrug glycolysis inhibition autophagy tumor synergistic therapy

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POV-based molecular catalysts for highly efficient esterification of alcohols with aldehydes as acylating agents

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Chinese Chemical Letters 2024年第8期35卷 330-334页

作者： Zhikang Wu Guoyong Dai Qi Li Zheyu Wei Shi Ru Jianda Li Hongli Jia Dejin Zang Mirjana Colovic Yongge Wei key lab.of Organic Optoelectronics&Molecular Engineering of Ministry of Education Department of ChemistryTsinghua UniversityBeijing 100084China state key lab.ratory of natural and Biomimetic drugs Peking UniversityBeijing 100191China Institute of Materia Medica Shandong First Medical University&Shandong Academy of Medical SciencesJi'nan 250117China University of Belgrade VincaInstitute of Nuclear Sciences-National Institute of the Republic of SerbiaDepartment of Physical ChemistryBelgrade 11351Serbia

The selective oxidative esterification of aldehydes with alcohols to the corresponding esters has been one of the hot spots in scientific research and industrial ***,the application of precious metal catalytic systems is limited by their complicated synthetic steps and high *** a highly efficient,green,recyclab.e selective synthesis method of esters catalyzed by polyoxovanadate(POV)-based molecu-lar catalysts has been developed in this *** results show that supramolecular interaction between POV and 1,3-dibenzylimidazolium bromide(Act_(2)Im)can efficiently convert alcohols and aldehydes to the corresponding esters in high yield under much milder *** insight is also provided based on the control experiments,single crystal X-ray diffraction and cyclic voltammetry studies.

关键词： POV Oxidation Supramolecular Esterification Catalyst

Recent advances in the microfluidic generation of shape-controllab.e hydrogel microparticles and their applications

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Green Chemical Engineering 2024年第1期5卷 16-30页

作者： Yingzhe Liu Zhuo Chen Jianhong Xu The state key lab.of Chemical Engineering Department of Chemical EngineeringTsinghua UniversityBeijing100084China

Hydrogel microparticles,generally accepted as significant green materials,have been widely used in chemical,biological,and biomedical fields owing to their excellent biocompatibility,biodegradability,and *** these,non-spherical hydrogel microparticles with diverse shape anisotropy have great potential in applications such as drug delivery,cellular interaction,micromotors,*** from their shapes,their functionalities in such fields cannot be satisfied by the typical spherical ***,microfluidics with precise control and domination of fluids at microflow sizes has emerged as a powerful method for synthesizing shape-controllab.e hydrogel microparticles with good monodispersity and unique *** this review,we tried to provide an overview of the production of non-spherical microparticles composed of green hydrogel materials,emphasizing the microfluidic ***,a brief introduction to their current applications is also presented.

关键词： Microfluidics Hydrogel Microparticles Non-spherical Anisotropic Green materials

A novel TNKS/USP25 inhibitor blocks the Wnt pathway to overcome multi-drug resistance in TNKS-overexpressing colorectal cancer

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Acta Pharmaceutica Sinica B 2024年第1期14卷 207-222页

作者： Hongrui Zhu Yamin Gao Liyun Liu Mengyu Tao Xiao Lin Yijia Cheng Yaoyao Shen Haitao Xue Li Guan Huimin Zhao Li Liu Shuping Wang Fan Yang Yongjun Zhou Hongze Liao Fan Sun Houwen Lin Research Center for Marine drugs Department of PharmacyRen Ji HospitalShanghai Jiao Tong University School of MedicineShanghai 200127China Department of Oncology Shanghai General HospitalShanghai Jiao Tong University School of MedicineShanghai 200080China Institute of Marine drugs Guangxi University of Chinese MedicineNanning 530200China state key lab.ratory of New Drug and Pharmaceutical Process Shanghai Professional and Technical Ser-vice Center for Biological Material Drug-ability EvaluationShanghai Institute of Pharmaceutical IndustryChina State Institute of Pharmaceutical IndustryShanghai 200437China Institute of Marine Biomedicine Shenzhen PolytechnicShenzhen 518055China

Modulating Tankyrases(TNKS),interactions with USP25 to promote TNKS degradation,rather than inhibiting their enzymatic activities,is emerging as an alternative/specific approach to inhibit the Wnt/β-catenin ***,we identified UAT-B,a novel neoantimycin analog isolated from Streptomyces conglobatus,as a small-molecule inhibitor of TNKS-USP25 protein-protein interaction(PPI)to overcome multi-drug resistance in colorectal cancer(CRC).The disruption of TNKS-USP25 complex formation by UAT-B led to a significant decrease in TNKS levels,triggering cell apoptosis through modulation of the Wnt/β-catenin ***,UAT-B successfully inhibited the CRC cells growth that harbored high TNKS levels,as demonstrated in various in vitro and in vivo studies utilizing cell line-based and patient-derived xenografts,as well as APC^(min/+)spontaneous CRC ***,these findings suggest that targeting the TNKS-USP25 PPI using a small-molecule inhibitor represents a compelling therapeutic strategy for CRC treatment,and UAT-B emerges as a promising candidate for further preclinical and clinical investigations.

关键词： Colorectal cancer TNKSeUSP25 interaction Multi-drug resistance TNKS overexpression Wnt pathway Apoptosis Neoantimycin analog

Living Chinese Herbal Scaffolds from Microfluidic Bioprinting for Wound Healing

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Research 2024年第1期2023卷 107-118页

作者： Xiaocheng Wang Jinxuan Jia Mengying Niu Wenzhao Li Yuanjin Zhao Department of Rheumatology and Immunology Nanjing Drum Tower HospitalSchool of Biological Science and Medical EngineeringSoutheast UniversityNanjing 210096China Oujiang lab.ratory(Zhejiang lab.for Regenerative Medicine Vision and Brain Health)Wenzhou InstituteUniversity of Chinese Academy of SciencesWenzhouZhejiang 325001China state key lab.ratory of Bioelectronics School of Biological Science and Medical EngineeringSoutheast UniversityNanjing 210096China Chemistry and Biomedicine Innovation Center Nanjing UniversityNanjing 210023China

biological scaffolds have been widely employed in wound healing applications,while their practical efficiency is compromised by insufficient oxygen delivery to the 3-dimensional constructs and inadequate nutrient supply for the long-term healing ***,we present an innovative living Chinese herbal scaffold to provide a sustainable oxygen and nutrient supply for promoting wound *** a facile microfluidic bioprinting strategy,a traditional Chinese herbal medicine(Panax notoginseng saponins[PNS])and a living autotrophic microorganism(microalgae Chlorella pyrenoidosa[MA])were successfully encapsulated into the *** encapsulated PNS could be gradually released from the scaffolds,which promoted cell adhesion,proliferation,migration,and tube formation in *** addition,benefiting from the photosynthetic oxygenation of the alive MA,the obtained scaffolds would produce sustainable oxygen under light illumination,exerting a protective effect against hypoxia-induced cell *** on these features,we have demonstrated through in vivo experiments that these living Chinese herbal scaffolds could efficiently alleviate local hypoxia,enhance angiogenesis,and thereby accelerate wound closure in diabetic mice,indicating their great potential in wound healing and other tissue repair applications.

关键词： healing wound protective

Recent Advances of Bioactive Marine natural Products in Drug Discovery

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Journal of Ocean University of China 2024年第5期23卷 1297-1318页

作者： ZHANG Qun LV Liuxia WANG Wenhui WEI Meiyan GU Yucheng SHAO Changlun key lab.ratory of Marine drugs Ministry of Education of China School of Medicine and Pharmacy Ocean University of China lab.ratory for Marine drugs and Bioproducts Qingdao Marine Science and Technology Center key lab.ratory of Tropical Medicinal Resource Chemistry of Ministry of Education College of Chemistry and Chemical Engineering Hainan Normal University Syngenta Jealott's Hill International Research Centre

Marine natural products(MNPs) are valuable resources for drug development. To date, 17 drugs from marine sources are in clinical use, and 33 pharmaceutical compounds are in clinical trials. Presently the success of drug development from the marine resources is higher than the industry average. It is a feasible strategy to conduct the discovery of drug-lead compounds based on marine chemical ecology by fully exploiting the pharmacological potential of marine chemical defense matters. In the search for bioactive MNPs, our group has constructed a biological resources library including more than 1500 strains of fungi. Focusing on the strategy of Blue Drug Library, we have discovered a series of novel MNPs with abundant biological functions. Highly efficient and scalab.e total synthesis of(+)-aniduquinolone A(44) and pesimquinolone I(48) have been completed, which will facilitate access to sufficient quantities of candidates for in vivo pharmacological and toxicological studies. As a nucleoprotein(NP) inhibitor, QLA(75) possesses significant anti-influenza A virus(IAV) activities both in vitro and in vivo. CHNQD-00803(76) is a potent and selective AMPactivated kinase(AMPK) activator that can effectively inhibit metabolic disorders and metabolic dysfunction-associated steatohepatitis(MASH) progression. Moreover, we identified two new candidate molecules with potent anti-hepatocellular carcinoma effects. Particularly, as a natural guanine-nucleotide exchange factors for ADP-ribosylation factor GTPases(Arf-GEFs) inhibitor prodrug, CHNQD-01255(78) is qualified to be developed as a targeted candidate anticancer drug, which may be promising to apply for cancer immunotherapy. Hence, it is evident that MNPs play an important role in drug development.

关键词： discovery and optimization drug development marine drug marine medicinal organisms natural products

基于电子给体-受体复合物的脂肪烃碳氢键多样性转化

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Science Bulletin 2024年第3期69卷 345-353页

作者：王泽敏闫超咸刘瑞华李晓伟戴佳佳李祥乾史大永 state key lab.ratory of Microbial Technology Shandong UniversityQingdao 266237China School of Chemistry&Chemical Engineering Ankang UniversityAnkang 725000China lab.ratory of Marine drugs and biological Products Pilot National Laboratory for Marine Science and TechnologyQingdao 266237China

The ability to selectively introduce diverse functionality onto hydrocarbons is of substantial value in the synthesis of both small molecules and *** this endeavour,as a photocatalyst-and metalfree process,the electron donor–acceptor(EDA)strategy has not been well *** we report an approach to aliphatic carbon-hydrogen bond diversification through an EDA complex constituted by HCl and S^(IV)=O *** an efficient hydrogen atom transfer(HAT)reagent,chlorine radical can be produced via a proton-coupled electron transfer process in this *** on this unusual path,a photopromoted versatile aliphatic C–H functionalization is developed without photo-and metal-catalysts,including thiolation,arylation,alkynylation,and *** conversion has concise and ambient reaction conditions,good functional group tolerance,and substrate diversity,and provides an alternative solution for the high value-added utilization of bulk light alkanes.

关键词： Photoreaction Electron donor-acceptor Aliphatic C-H functionalization Chlorine radicals Gaseous alkanes