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Recent advances in the synthesis and application of N-heterocyclic carbene-based molecular cages

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Science China Chemistry 2024年第5期67卷 1510-1523页

作者： Qiongjie Chai Lixin Duan Yanzhe Ma Tianheng Hou tao tu Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Department of ChemistryFudan UniversityShanghai 200438China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

N-Heterocyclic carbene(NHC)-based cages have emerged as a prominent and dynamic research area within the research field of chemistry. Leveraging the distinctive electronic and steric properties of NHC ligands, the design, synthesis, and application of these corresponding cages have garnered substantial scholarly interest. In recent years, we have witnessed the successful fabrication of diverse NHC-based cages through a range of synthetic methodologies, which hold significant potential for applications in molecular recognition and catalysis. In this review, we delve into the foundational synthetic strategies that underlie the creation of NHC-based cages, employing approaches encompassing metal–NHC chelation, coordination assembly,and covalent bonding. Additionally, we compile the diverse applications of these cages within catalytic processes and molecular recognition. Lastly, we shed light on the current limitations of synthesis and outline future trends in the development of NHCbased cages.

关键词： N-heterocyclic carbene molecular cages supramolecular chemistry synthetic strategies applications

Immobilization of Proteases on Nanoflower-Like Metal Organic Framework

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Chinese Journal of Chemistry 2023年第12期41卷 1504-1508页

作者： He Li Yunjie tu tao tu Qi Zhang Department of Chemistry Fudan University Shanghai 200438 China

Proteases have been widely used in pharmaceutics and industry,and an economic,convenient and robust procedure for protease immobilization is of high interest.In this study,we report immobilization of proteases by the nanoflower-like zeolitic imidazole framework (nfZIF).Using trypsin,protease K,and Glu-C as model enzymes,we show nfZIF represents an excellent material for protease immobilization,and the resulting [email protected] composites exhibit activities comparable to or even higher than the free proteases in solution.The [email protected] composites are stable in high temperature and organic solvents,and retain almost fully active after several reaction cycles.Our studies demonstrate the great potential of nfZIF in the immobilization of proteases,which could be of interest in various industrial applications.

关键词： Metal-organic frameworks ZiF-8 Enzymes Immobilization Lamellar material

A novel strain of Levilactobacillus brevis PDD-5 isolated from salty vegetables has beneficial effects on hyperuricemia through anti-inflammation and improvement of kidney damage

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Food Science and Human Wellness 2024年第2期13卷 898-908页

作者： Jue Xu Maolin tu Xiankang Fan Yuxing Guo tao Zhang Xiaoqun Zeng Zhendong Cai Zhen Wu Daodong Pan State Key Laboratory for Managing Biotic and Chemical Threats to the Quality and Safety of Agro-products Ningbo UniversityNingbo 315211China Key Laboratory of Animal Protein Food Deep Processing Technology of Zhejiang Province College of Food and Pharmaceutical SciencesNingbo UniversityNingbo 315211China Department of Food Science and Technology School of Food Science and Pharmaceutical EngineeringNanjing Normal UniversityNanjing 210023China

Hyperuricemia is a metabolic disorder caused by abnormal purine metabolism,resulting in abnormally high serum uric acid.In this study,a novel Levilactobacillus brevis PDD-5 isolated from salty vegetables was verified with the function of alleviating hyperuricemia.The relevant effects of L.brevis PDD-5 in lowering uric acid were analyzed by in vitro and in vivo experiments.The results showed that the L.brevis PDD-5 has(68.86±15.46)%of inosine uptake capacity and(95.75±3.30)%of guanosine uptake capacity in vitro.Oral administration of L.brevis PDD-5 to hyperuricemia rats reduced uric acid,creatinine,and urea nitrogen in serum,as well as decreased inosine and guanosine levels in the intestinal contents of rats.Analysis of relevant markers in the kidney by ELISA kits revealed that L.brevis PDD-5 alleviated oxidative stress and inflammation.Moreover,the gene expression of uric acid transporter 1(URAT1)and glucose transporter 9(GLUT9)was down-regulated,and the gene expression of organic anion transporter 1(OAT1)was up-regulated after treatment with L.brevis PDD-5.Western blot analysis showed that L.brevis PDD-5 alleviated hyperuricemia-induced kidney injury through the NLRP3 pathway.The se findings suggest that L.brevis PDD-5 can lower uric acid,repair kidney damage,and also has the potential to prevent uric acid nephropathy.

关键词： Lactic acid bacteria Purine nucleoside Hyperuricemia Uric acid nephropathy

Autophagy plays a pro-apoptotic role in arsenic trioxide-induced cell death of liver cancer

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Journal of Integrative Medicine 2024年第3期22卷 295-302页

作者： Zhengting Deng Shufang Liang Guokai Huang Yuqian Wang Xiaoyu tu Yani Zhang Shu Li tao Liu Binbin Cheng Taizhou Hospital of Traditional Chinese Medicine Nanjing University of Chinese MedicineTaizhou 225300Jiangsu ProvinceChina Oncology Department of Traditional Chinese Medicine The First Affiliated Hospital of Naval Medical UniversityShanghai 200433China School of Traditional Chinese Medicine Nanjing University of Chinese MedicineNanjing 210023Jiangsu ProvinceChina Department of Gastroenterology Baoshan Hospital of Integrated Traditional Chinese and Western MedicineShanghai University of Traditional Chinese MedicineShanghai 201900China

Objective: The effects of arsenic trioxide(As2O3) on hepatocellular carcinoma have been documented widely. Autophagy plays dual roles in the survival and death of cancer cells. Therefore, we investigated the exact role of autophagy in As2O3-induced apoptosis in liver cancer cells.Methods: The viability of hepatoma cells was determined using the MTT assay with or without fetal bovine serum. The rate of apoptosis in liver cancer cells treated with As2O3was evaluated using flow cytometry, Hoechst 33258 staining, and tuNEL assays. The rate of autophagy among liver cancer cells treated with As2O3was detected using immunofluorescence, Western blot assay and transmission electron microscopy.Results: Upon treatment with As2O3, the viability of HepG2 and SMMC-7721 cells was decreased in a time-and dose-dependent manner. The apoptosis rates of both liver cancer cell lines increased with the concentration of As2O3, as shown by flow cytometry. Apoptosis in liver cancer cells treated with As2O3was also shown by the activation of the caspase cascade and the regulation of Bcl-2/Bax expression.Furthermore, As2O3treatment induced autophagy in liver cancer cells;this finding was supported by Western blot, immunofluorescence of LC3-II and beclin 1, and transmission electron microscopy. In liver cancer cells, As2O3inhibited the phosphoinositide 3-kinase/protein kinase B/mammalian target of rapamycin(PI3K/AKT/mTOR) signal pathway that plays a vital role in both apoptosis and autophagy. The PI3K activator SC-79 partially reversed As2O3-induced autophagy and apoptosis. Furthermore, inhibiting autophagy with 3-methyladenine partially reversed the negative effects of As2O3on cell viability.Serum starvation increased autophagy and amplified the effect of As2O3on cell death.Conclusion: As2O3induces apoptosis and autophagy in liver cancer cells. Autophagy induced by As2O3may have a proapoptotic effect that helps to reduce the viability of liver cancer cells. This study provides novel insights into the effects of As2O3against liver cancer.

关键词： Apoptosis Arsenic trioxide Autophagy Primary liver cancer

Bimetal-containing covalent organic framework boosted photocatalytic amination

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Science China Chemistry 2023年第2期66卷 299-300页

作者： Weiwei Fang tao tu Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources International Innovation Center for Forest Chemicals and MaterialsCollege of Chemical EngineeringNanjing Forestry UniversityNanjing210037China Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Department of ChemistryFudan UniversityShanghai200433China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai200032China Green Catalysis Center and College of Chemistry Zhengzhou UniversityZhengzhou450001China

The design of new catalytic systems allowing for rapid,selective,and sustainable chemical transformations is of immense scientific importance.As ubiquitous skeleton motifs,during the past decades,a range of well-designed ligands and catalysts have been developed,which benefited the construction of C-N bond under mild reaction conditions[1].

关键词： skeleton photocatalytic mild

GmSTF accumulation mediated by DELLA protein GmRGAs contributes to coordinating light and gibberellin signaling to reduce plant height in soybean

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The Crop Journal 2024年第2期12卷 432-442页

作者： Zhuang Li Qichao tu Xiangguang Lyu Qican Cheng Ronghuan Ji Chao Qin Jun Liu Bin Liu Hongyu Li tao Zhao State Key Laboratory of Crop Gene Resources and Breeding Institute of Crop SciencesChinese Academy of Agricultural SciencesBeijing 100081China

Plant height influences plant architecture,lodging resistance,and yield performance.It is modulated by gibberellic acid(GA)metabolism and signaling.DELLA proteins,acting as central repressors of GA signaling,integrate various environmental and hormonal signals to regulate plant growth and development in Arabidopsis.We examined the role of two DELLA proteins,GmRGAa and GmRGAb,in soybean plant height control.Knockout of these proteins led to longer internodes and increased plant height,primarily by increasing cell elongation.GmRGAs functioned under different light conditions,including red,blue,and far-red light,to repress plant height.Interaction studies revealed that GmRGAs interacted with the blue light receptor GmCRY1b.Consistent with this,GmCRY1b partially regulated plant height via GmRGAs.Additionally,DELLA proteins were found to stabilize the protein GmSTF1/2,a key positive regulator of photomorphogenesis.This stabilization led to increased transcription of GmGA2ox-7b and subsequent reduction in plant height.This study enhances our understanding of DELLA-mediated plant height control,offering Gmrgaab mutants for soybean structure and yield optimization.

关键词： DELLA protein GmRGAs GmSTFs Plant height Soybean

Lamellar Enzyme-Metal-Organic Framework Composites Enable Catalysis on Large Substrates

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CCS Chemistry 2022年第3期4卷 872-879页

作者： Yunjie tu He Li tao tu Qi Zhang Department of Chemistry Fudan UniversityShanghai 200433

Zeolitic imidazolate framework(ZIF)is a representative type of metal–organic framework that has been extensively used as a carrier in enzyme immobilization.However,thus far the immobilization studies have mainly been carried out on enzymes with small substrates(e.g.,peroxide and glucose),and the general applicability of ZIF in enzyme immobilization has not been investigated.In this study,we show that,owing to its small aperture size,the canonical sodalite ZIF[ZIF-8 or sod-Zn(mIM)_(2)(mIM=2-methylimidazolate)]cannot be used for enzymes with large substrates.Instead,we show that the lamellar,nanoflower-like ZIF[nf-Zn(mIM)_(2)]synthesized in low precursor concentrations overcomes the size limitation of sod-Zn(mIM)_(2) and is suitable for immobilization of various enzymes with large substrates.Remarkably,the lamellar ZIF can work with a thioesterase,which acts on a peptide with 11 amino acids to produce an analog of teixobactin,a superantibiotic with no antimicrobial resistance thus far.The lamellar ZIF scaffold is highly efficient in enzyme loading and significantly increases enzyme stability against disfavorable conditions,serving as a general carrier in enzyme immobilization.

关键词： MOF ZIF-8 enzyme immobilization SAM teixobactin

Directly Knitted Ruthenium Pincer Complexes with Enhanced Activity as Recyclable Single-Site Catalysts for Hydrogenation of CO_(2)to Methanol

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CCS Chemistry 2023年第7期5卷 1602-1611页

作者： Daheng Wen Jiangbo Chen Qingshu Zheng Siqi Yang tao tu Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Department of ChemistryFudan UniversityShanghai 200438 State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032 Green Catalysis Center and College of Chemistry Zhengzhou UniversityZhengzhou 450001

Considering the importance of the valorization of CO_(2),a number of phosphine-containing ruthenium pincer complexes have been successfully heterogenized using a“direct knitting”strategy without any premodification.The resulting porous organometallic polymers(POMPs)with high specific-surface areas,hierarchical pores,and uniformly dispersed Ru single-sites exhibited outstanding catalytic activity toward the N-formylation of diverse amines with CO_(2).Besides excellent turnover number(TON,5×10^(5))and turnover frequency(TOF,5592 h-1),the obtained formamides were readily hydrogenated to methanol with the same catalyst.Consequently,an amine-assisted direct hydrogenation system of CO_(2)to methanol was established by POMPs with higher activity and TON(1.46×10^(4))than their molecular precursors,shedding light on the direct valorization of CO_(2)and carbon neutral recycling.

关键词： direct knitting hydrogenation of CO_(2) porous organometallic polymers ruthenium pincer complexes single-site catalyst

Phosphine ligands featuring C-N chiral axis applicable to tetra-ortho-substituted biaryl synthesis

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Chinese Chemical Letters 2023年第7期34卷 3-5页

作者： Weiwei Fang Meiying Kuai James H.Clark tao tu Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources International Innovation Center for Forest Chemicals and MaterialsCollege of Chemical EngineeringNanjing Forestry UniversityNanjing 210037China Circa Renewable Chemistry Institute Green Chemistry Centre of ExcellenceUniversity of YorkYork YO105DDUnited Kingdom Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Department of ChemistryFudan UniversityShanghai 200433China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China Green Catalysis Center and College of Chemistry Zhengzhou UniversityZhengzhou 450001China

Asymmetric catalysis has been one of the most effective strategies for building up a chirality in the favored stereoisomer. Over the past decades, various sophisticated chiral ligands and catalysts have been well-designed, which enable great advances in enantioselective chemical transformations, for achieving excellent selectivity and activity.

关键词： chiral substituted applicable