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981.
982.
Albrecht Ł Jiang H Jørgensen KA 《Angewandte Chemie (International ed. in English)》2011,50(37):8492-8509
Asymmetric organocatalysis has been successfully incorporated in many multistep one-pot sequences to provide simple access to structurally complex target molecules in a highly stereoselective fashion. The key feature behind this success is the ability of organocatalyzed reactions to proceed efficiently in the presence of large amounts of spectator reagents. Additionally, owing to their organic nature and substoichiometric presence, organocatalysts are also expected to become innocent bystanders in subsequent transformations. In this Minireview, an easy-to-use classification and nomenclatural system that is capable of systematically and informatively describing each one-pot reaction is introduced, and selected important contributions within the field of organocatalytic one-pot reactions are reviewed according to this new system. Finally, future developments and perspectives in the field are discussed. 相似文献
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The method of native chemical ligation between an unprotected peptide α‐thioester and an N‐terminal cysteine–peptide to give a native peptide in aqueous solution is one of the most effective peptide ligation methods. In this work, a systematic theoretical study was carried out to fully understand the detailed mechanism of ligation. It was found that for the conventional native chemical ligation reaction between a peptide thioalkyl ester and a cysteine in combination with an added aryl thiol as catalyst, both the thiol‐thioester exchange step and the transthioesterification step proceed by an anionic concerted SN2 displacement mechanism, whereas the intramolecular rearrangement proceeds by an addition–elimination mechanism, and the rate‐limiting step is the thiol‐thioester exchange step. The theoretical method was then extended to study the detailed mechanism of the auxiliary‐mediated peptide ligation between a peptide thiophenyl ester and an N‐2‐mercaptobenzyl peptide in which both the thiol‐thioester exchange step and intramolecular acyl‐transfer step proceed by a concerted SN2‐type displacement mechanism. The energy barrier of the thiol‐thioester exchange step depends on the side‐chain steric hindrance of the C‐terminal amino acid, whereas that of the acyl‐transfer step depends on the side‐chain steric hindrance of the N‐terminal amino acid. 相似文献
989.
建立科学、有效、准确的空气质量预测系统,对于保护人们的身体健康和促进社会的和谐稳定具有重要的科学价值和实际意义。研究聚焦化工园区,基于物联网背景下企业排放实时数据,融合气象信息,采用多种有监督式机器学习(决策树、多元线性回归、Lasso回归、支持向量机、Xgboost、梯度提升机、Light GBM、MLP(多层感知觉神经网络))及改进的集成学习Stacking策略实现化工园区空气质量的预测,并识别影响大气污染的关键因素。结果表明:(1)Stacking策略下的预测框架与单模型预测结果相比有统计学意义上的显著提升。(2)在Stacking策略中,初级、次级学习器的选择策略影响预测的精度和泛化性,最佳模式为初级采用强学习器,次级使用线性模型。(3)在同一园区、不同企业污染物不同排放口对空气质量影响不同,研究结论可为政府监管部门对化工园区的治理和管控提供决策支持。 相似文献
990.
Edyta Janik Marcin Niemcewicz Marcin Podogrocki Michal Ceremuga Leslaw Gorniak Maksymilian Stela Michal Bijak 《Molecules (Basel, Switzerland)》2021,26(13)
Mycotoxins represent a wide range of secondary, naturally occurring and practically unavoidable fungal metabolites. They contaminate various agricultural commodities like cereals, maize, peanuts, fruits, and feed at any stage in pre- or post-harvest conditions. Consumption of mycotoxin-contaminated food and feed can cause acute or chronic toxicity in human and animals. The risk that is posed to public health have prompted the need to develop methods of analysis and detection of mycotoxins in food products. Mycotoxins wide range of structural diversity, high chemical stability, and low concentrations in tested samples require robust, effective, and comprehensible detection methods. This review summarizes current methods, such as chromatographic and immunochemical techniques, as well as novel, alternative approaches like biosensors, electronic noses, or molecularly imprinted polymers that have been successfully applied in detection and identification of various mycotoxins in food commodities. In order to highlight the significance of sampling and sample treatment in the analytical process, these steps have been comprehensively described. 相似文献