Moons Sam J, Hornikx Daniël L A H, Aasted Mikkel K M, Pijnenborg Johan F A, Calzari Matteo, White Paul B, Narimatsu Yoshiki, Clausen Henrik, Wandall Hans H, Boltje Thomas J, Büll Christian
Cluster for Molecular Chemistry, Institute for Molecules and Materials, Radboud University Nijmegen Nijmegen The Netherlands
Department of Biomolecular Chemistry, Institute for Molecules and Materials, Radboud University Nijmegen Nijmegen The Netherlands
RSC Chem Biol. 2023 May 25;4(7):506-511. doi: 10.1039/d3cb00006k. eCollection 2023 Jul 5.
Sialic acids cap glycans displayed on mammalian glycoproteins and glycolipids and mediate many glycan-receptor interactions. Sialoglycans play a role in diseases such as cancer and infections where they facilitate immune evasion and metastasis or serve as cellular receptors for viruses, respectively. Strategies that specifically interfere with cellular sialoglycan biosynthesis, such as sialic acid mimetics that act as metabolic sialyltransferase inhibitors, enable research into the diverse biological functions of sialoglycans. Sialylation inhibitors are also emerging as potential therapeutics for cancer, infection, and other diseases. However, sialoglycans serve many important biological functions and systemic inhibition of sialoglycan biosynthesis can have adverse effects. To enable local and inducible inhibition of sialylation, we have synthesized and characterized a caged sialyltransferase inhibitor that can be selectively activated with UV-light. A photolabile protecting group was conjugated to a known sialyltransferase inhibitor (P-SiaFNEtoc). This yielded a photoactivatable inhibitor, UV-SiaFNEtoc, that remained inactive in human cell cultures and was readily activated through radiation with 365 nm UV light. Direct and short radiation of a human embryonic kidney (HEK293) cell monolayer was well-tolerated and resulted in photoactivation of the inhibitor and subsequent spatial restricted synthesis of asialoglycans. The developed photocaged sialic acid mimetic holds the potential to locally hinder the synthesis of sialoglycans through focused treatment with UV light and may be applied to bypass the adverse effects related to systemic loss of sialylation.
唾液酸覆盖在哺乳动物糖蛋白和糖脂上所展示的聚糖上,并介导许多聚糖-受体相互作用。唾液酸聚糖在癌症和感染等疾病中发挥作用,在这些疾病中,它们分别促进免疫逃逸和转移或充当病毒的细胞受体。特异性干扰细胞唾液酸聚糖生物合成的策略,如作为代谢唾液酸转移酶抑制剂的唾液酸模拟物,有助于研究唾液酸聚糖的多种生物学功能。唾液酸化抑制剂也正在成为癌症、感染和其他疾病的潜在治疗方法。然而,唾液酸聚糖具有许多重要的生物学功能,对唾液酸聚糖生物合成的全身抑制可能会产生不利影响。为了实现唾液酸化的局部和可诱导抑制,我们合成并表征了一种可被紫外光选择性激活的笼形唾液酸转移酶抑制剂。将一个光不稳定保护基团与一种已知的唾液酸转移酶抑制剂(P-SiaFNEtoc)偶联。这产生了一种光可激活抑制剂UV-SiaFNEtoc,它在人类细胞培养物中保持无活性,并通过365nm紫外光辐射很容易被激活。对人胚肾(HEK293)细胞单层进行直接和短时间辐射耐受性良好,并导致抑制剂的光激活以及随后无唾液酸聚糖的空间受限合成。所开发的光笼形唾液酸模拟物有可能通过紫外光聚焦处理局部阻碍唾液酸聚糖的合成,并可用于绕过与唾液酸化全身丧失相关的不利影响。