Cross-coupling reactions have been well received as one of the most popular protocols for ketone synthesis. As an important coupling partner, bench-stable and commercially available alkyl boronic acids are widely used in transition metal catalysis, but they are rarely utilized as radical precursors for acylative coupling reactions. Herein, we reported an energy-transfer-enabled radical acylation using free alkyl boronic acids via NHC/photo dual catalysis. This protocol could efficiently promote the Suzuki-type cross-coupling between alkyl boronic acids and acyl imidazoles as well as the multicomponent alkylacylations of alkenes, thus producing various ketones with structural diversity. Additionally, ketone products can readily transform into a large number of structurally interesting fine chemicals. Preliminary mechanistic studies shed light on the unique radical reaction mechanism.

Gasdermin D (GSDMD)-mediated pyroptosis and downstream inflammation are important self-protection mechanisms against stimuli and infections. Hosts can defend against intracellular bacterial infections by inducing cell pyroptosis, which triggers the clearance of pathogens. However, pyroptosis is a double-edged sword. Numerous studies have revealed the relationship between abnormal GSDMD activation and various inflammatory diseases, including sepsis, coronavirus disease 2019 (COVID-19), neurodegenerative diseases, nonalcoholic steatohepatitis (NASH), inflammatory bowel disease (IBD), and malignant tumors. GSDMD, a key pyroptosis-executing protein, is linked to inflammatory signal transduction, activation of various inflammasomes, and the release of downstream inflammatory cytokines. Thus, inhibiting GSDMD activation is considered an effective strategy for treating related inflammatory diseases. The study of the mechanism of GSDMD activation, the formation of GSDMD membrane pores, and the regulatory strategy of GSDMD-mediated pyroptosis is currently a hot topic. Moreover, studies of the structure of caspase-GSDMD complexes and more in-depth molecular mechanisms provide multiple strategies for the development of GSDMD inhibitors. This review will mainly discuss the structures of GSDMD and GSDMD pores, activation pathways, GSDMD-mediated diseases, and the development of GSDMD inhibitors.

Construction of pyrrolidinyl-spiroindoles with easily available starting materials has attracted considerable attention from the synthesis community and is in great demand. Here, we describe a base-promoted formal (3 + 2) cycloaddition of α-halohydroxamates with alkenyl-iminoindolines. The present methodology features mild reaction conditions and a broad substrate scope with up to 99% yield and excellent diastereoselectivity. The versatility of this approach is demonstrated through valuable synthetic transformations. Preliminary mechanistic studies shed light on the mechanism of this cycloaddition process.

以酯基烯丙基锍盐作为起始原料,在碱的作用下,与醌亚胺类化合物经氧杂[3+3]串联环化反应,以中等收率合成了一系列苯并吡喃衍生物.并进一步以对氨基(羟基)酚类化合物为底物,经原位氧化串联氧杂[3+3]环化反应,通过"一锅法"更为高效的实现了目标骨架的构建.代表产物的结构经X-ray单晶衍射确证,所有化合物的结构经1 H NMR,13 C NMR和HR-MS(ESI-TOF)表征.

以环庚酮及环己(庚)胺为起始原料,经溴代、环化和脱硫等反应,以良好的收率合成了环烷基取代的新型噻唑骨架的氮杂环卡宾催化剂.结果表明:在该催化剂催化下成功地实现了烯烃的自由基氟烷基酰化反应,并以中等收率完成了三种类型的γ-氟烷基取代酮的高效合成.所得化合物通过1 H NMR,13 C NMR,19 F NMR和HR-MS(ESI-TOF)进行表征.

吲哚作为一种重要的杂环骨架,广泛存在于具有生物活性的天然产物和药物分子中.因此,发展结构新颖的含有吲哚骨架的合成砌块,对于吲哚衍生物的合成具有十分重要的研究意义.近年来,2-吲哚亚胺因易于制备与良好的反应活性引起了研究者的兴趣,其通过串联环化反应合成吲哚衍生物已经成为吲哚并环骨架构建中的一种重要途径.本文综述了 2-吲哚亚胺在吲哚并环骨架构建中的研究进展,包括(2+2)环化反应、(3+3)环化反应与多组分串联环化过程.

以取代靛红酸酐为起始原料,二甲基亚砜(DMSO)为反应溶剂,在三乙烯二胺(DABCO)的作用下加热至80℃,与取代靛红经形式上的(4+2)环化反应以81％ ～94％的收率合成了一系列色胺酮衍生物.化合物结构经1 H NMR,13 C NMR和HR-MS(ESI-TOF)表征.该制备方法不仅避免了反应过程中金属的使用,而且后处理简单、无需柱层析,在减小对环境影响的同时提升了合成效率.在此基础上,通过最小抑菌浓度(MIC)试验初步揭示了化合物3g良好的体外抗菌活性(<4μg·mL-1).