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Constantin Tnase Lucia Pintilie Raluca Elena Tnase 《International journal of molecular sciences》2021,22(4)
In the total stereo-controlled synthesis of natural prostaglandins (PGs) and their structural analogs, a vast class of compounds and drugs, known as the lactones, are encountered in a few key steps to build the final molecule, as: δ-lactones, γ-lactones, and 1,9-, 1,11-, and 1,15-macrolactones. After the synthesis of 1,9-PGF2α and 1,15-PGF2α lactones, many 1,15-lactones of E2, E3, F2, F3, A2, and A3 were found in the marine mollusc Tethys fimbria and the quest for understanding their biological role stimulated the research on their synthesis. Then 1,9-, 1,11-, and 1,15-PG lactones of the drugs were synthesized as an alternative to the corresponding esters, and the first part of the paper describes the methods used for their synthesis. The efficient Corey procedure for the synthesis of prostaglandins uses the key δ-lactone and γ-lactone intermediates with three or four stereocenters on the cyclopentane fragment to link the PG side chains. The paper describes the most used procedures for the synthesis of the milestone δ-Corey-lactones and γ-Corey-lactones, their improvements, and some new promising methods, such as interesting, new stereo-controlled and catalyzed enantioselective reactions, and methods based on the chemical/enzymatic resolution of the compounds in different steps of the sequences. The many uses of δ-lactones not only for the synthesis of γ-lactones, but also for obtaining 9β-halogen-PGs and halogen-substituted cyclopentane intermediates, as synthons for new 9β-PG analogs and future applications, are also discussed. 相似文献
3.
Jan Rinkel Prof. Dr. Jeroen S. Dickschat 《Chembiochem : a European journal of chemical biology》2020,21(6):807-810
Isotopic labeling experiments performed with a newly identified bacterial trichoacorenol synthase established a 1,5-hydride shift occurring in the cyclization mechanism. During EI-MS analysis, major fragments of the sesquiterpenoid were shown to arise via cryptic hydrogen movements. Therefore, the interpretation of earlier results regarding the cyclization mechanism obtained by feeding experiments in Trichoderma is revised. 相似文献
4.
Dr. Santosh Shivakumaraswamy Nivedita Pandey Dr. Lionel Ballut Dr. Sébastien Violot Prof. Dr. Nushin Aghajari Prof. Dr. Hemalatha Balaram 《Chembiochem : a European journal of chemical biology》2020,21(19):2805-2817
GMP synthetase catalyses the conversion of XMP to GMP through a series of reactions that include hydrolysis of Gln to generate ammonia in the glutamine amidotransferase (GATase) domain, activation of XMP to adenyl-XMP intermediate in the ATP pyrophosphatase (ATPPase) domain and reaction of ammonia with the intermediate to generate GMP. The functioning of GMP synthetases entails bidirectional domain crosstalk, which leads to allosteric activation of the GATase domain, synchronization of catalytic events and tunnelling of ammonia. Herein, we have taken recourse to the analysis of structures of GMP synthetases, site-directed mutagenesis and steady-state and transient kinetics on the Plasmodium falciparum enzyme to decipher the molecular basis of catalysis in the ATPPase domain and domain crosstalk. Our results suggest an arrangement at the interdomain interface, of helices with residues that play roles in ATPPase catalysis as well as domain crosstalk enabling the coupling of ATPPase catalysis with GATase activation. Overall, the study enhances our understanding of GMP synthetases, which are drug targets in many infectious pathogens. 相似文献
5.
D‐psicose 3‐epimerase secretory overexpression,immobilization, and d‐psicose biotransformation,separation and crystallization 下载免费PDF全文
6.
为了研究微冻贮藏过程中鲈鱼质构特性与能量代谢酶和蛋白质氧化之间的关系,分析了3种不同处理方式(空气包装处理、真空包装处理、茶多酚结合真空包装处理)对微冻(-2℃)贮藏过程中鲈鱼的剪切力、组织结构、差式扫描量热曲线、十二烷基硫酸钠-聚丙烯酰胺凝胶电泳、巯基含量和3种能量代谢酶(乳酸脱氢酶、Ca2+-ATP酶、Mg2+-ATP酶)活力的影响。结果表明:随微冻贮藏时间的延长,3种不同处理方式下鲈鱼的剪切力、总巯基含量和能量代谢酶活力均显著下降(P0.05),而茶多酚结合真空包装处理组各指标显著高于其他两个处理组(P0.05),表明茶多酚对微冻贮藏过程中鲈鱼品质有保护作用。十二烷基硫酸钠-聚丙烯酰胺凝胶电泳图谱和差示扫描量热曲线结果表明,在微冻条件下贮藏21 d鲈鱼肌球蛋白发生轻微变性;经过相关性分析得出,3种能量代谢酶活力均与总巯基含量呈显著正相关(P0.01,r=0.99),表明ATP酶和乳酸脱氢酶活力与肌原纤维蛋白的降解密切关,总巯基含量和ATP酶活力、剪切力之间也呈现极显著正相关性(P0.01,r=0.92),表明鲈鱼肌原纤维蛋白氧化会导致质构的劣化。 相似文献
7.
Yasuha Watanabe Prof. Kenzo Fujimoto 《Chembiochem : a European journal of chemical biology》2020,21(22):3244-3248
The regulation of DNAzyme activity is an important problem for its in vivo applications. We achieved photochemical regulation of DNAzyme activity by using reversible DNA photo-crosslinking of 3-cyanovinylcarbazole (CNVK). The ODN containing CNVK photo-crosslinked to a pyrimidine base in the complementary strand after a few seconds of photoirradiation, and its photoadduct was split by photoirradiation of another wavelength. The activity of photo-crosslinked DNAzyme with CNVK was completely inhibited (OFF state). In contrast, after 312 nm irradiation, DNAzyme activity was recovered upon addition of a substrate strand (ON state). In addition, the photo-crosslinked DNAzyme is prone to enzymatic digestion by exonuclease. This photochemical OFF to ON switching with reversible DNA photo-crosslinking was regulated at the desired time and position; therefore, it might be possible to use it for in vivo application. 相似文献
8.
Dr. Katie R. Witkin Dr. Nicholas R. Vance Colleen Caldwell Dr. Quinn Li Dr. Liping Yu Prof. M. Ashley Spies 《ChemMedChem》2020,15(4):376-384
Glutamate racemases (GR) are members of the family of bacterial enzymes known as cofactor-independent racemases and epimerases and catalyze the stereoinversion of glutamate. D-amino acids are universally important for the proper construction of viable bacterial cell walls, and thus have been repeatedly validated as attractive targets for novel antimicrobial drug design. Significant aspects of the mechanism of this challenging stereoinversion remain unknown. The current study employs a combination of MD and QM/MM computational approaches to show that the GR from H. pylori must proceed via a pre-activation step, which is dependent on the enzyme's flexibility. This mechanism is starkly different from previously proposed mechanisms. These findings have immediate pharmaceutical relevance, as the H. pylori GR enzyme is a very attractive allosteric drug target. The results presented in this study offer a distinctly novel understanding of how AstraZeneca's lead series of inhibitors cripple the H. pylori GR's native motions, via prevention of this critical chemical pre-activation step. Our experimental studies, using SPR, fluorescence and NMR WaterLOGSY, show that H. pylori GR is not inhibited by the uncompetitive mechanism originally put forward by Lundqvist et al.. The current study supports a deep connection between native enzyme motions and chemical reactivity, which has strong relevance to the field of allosteric drug discovery. 相似文献
9.
为探究臭氧(ozone,O_3)对膨大剂(N-2-氯-4-吡啶基苯-N’-苯基脲,CPPU)处理秦美猕猴桃果实贮藏期间其品质劣变的抑制效果,本文以生长期使用了20 mg/L CPPU的秦美猕猴桃果实为试验材料,在0±1℃条件下贮藏。研究了10、40和70 mg/m~3 O_3处理对贮藏期间秦美猕猴桃果实的品质指标、乙烯释放量、呼吸强度以及抗性酶活性的影响。试验结果表明40 mg/m~3 O_3可以减缓CPPU处理的秦美猕猴桃品质的下降趋势,减轻了可滴定酸、Vc含量的下降,保持了较好的硬度,减缓了可溶性固形物含量的上升;抑制了乙烯释放量和呼吸强度,减少果实软化;并增加了苯丙氨酸解氨酶(Phenylalanine ammonia lyase,PAL)、β-1,3-葡聚糖酶(β-1,3-glucanase,GLU)、几丁质酶(Chitinase,CHI)的活性,从而减少了秦美猕猴桃果实的腐烂率。O_3处理能有效减轻CPPU处理对秦美猕猴桃果实产生的负面影响并延长贮藏时间。 相似文献
10.
生物活性肽是来源于蛋白质的多功能化合物,是可以调节生物机体的生命活动或具有生理活性作用的一类肽的总称。牡蛎肽又是生物活性肽的重要组成部分,含有丰富的蛋白质、人体必需的8种氨基酸、牛磺酸、维生素以及锌、硒、铁、铜、碘等微量元素;随着现代生物技术和医学技术的发展,制备牡蛎活性肽的方法多种,且牡蛎肽在抗氧化、降血糖、抗肿瘤、抑制血管紧张素转化酶(angiotensin converting enzyme,ACE)活性等方面具备特殊的生理活性。本文就牡蛎肽的制备以及牡蛎肽的生物活性等研究进行概述,为今后牡蛎肽的应用提供参考。 相似文献