Li Tuo, Luo Youyi, Liu Changhong, Lu Xuan, Feng Baomin
College of Life and Health, Dalian University, Dalian 116622, China.
Int J Mol Sci. 2025 Mar 29;26(7):3167. doi: 10.3390/ijms26073167.
Archaeal lipids, defining a primordial life domain alongside Bacteria and Eukarya, are distinguished by their unique glycerol-1-phosphate backbone and ether-linked isoprenoid chains. Serving as critical geochemical biomarkers, archaeal lipids like glycerol dialkyl glycerol tetraethers (GDGTs) underpin paleoclimate proxies, while their phylum-specific distributions illuminate phylogenetic divergence. Despite the maturity of Mass Spectrometry-based quantitative biomarkers-predominantly those with established structures-becoming well-established in geochemical research, systematic investigation of archaeal lipids as natural products has notably lagged. This deficit manifests across three key dimensions: (1) Extraction methodology lacks universal protocols adapted to diverse archaeal taxa and sample matrices. While comparative studies exist, theoretical frameworks guiding method selection remain underexplored. (2) Purification challenges persist due to the unique structures and complex isomerization profiles of archaeal lipids, hindering standardized separation protocols. (3) Most critically, structural characterization predominantly depends on decades-old foundational studies. However, the existing reviews prioritize chemical structural, biosynthetic, and applied aspects of archaeal lipids over analytical workflows. This review addresses this gap by adopting a natural product chemistry perspective, integrating three key aspects: (1) the clarification of applicable objects, scopes, and methodological mechanisms of various extraction technologies for archaeal lipids, encompassing both cultured and environmental samples; (2) the elucidation of separation principles underlying polar-gradient lipid fractionation processes, leveraging advanced chromatographic technologies; (3) the detailed exploration of applications for NMR in resolving complex lipid structures, with specialized emphasis on determining the stereochemical configuration. By synthesizing six decades of methodological evolution, we establish a comprehensive analytical framework, from lipids extraction to structural identification. This integrated approach constructs a systematic methodological paradigm for archaeal lipid analysis, bridging theoretical principles with practical implementation.
古菌脂质与细菌和真核生物一起构成了一个原始生命域,其独特之处在于具有甘油-1-磷酸主链和醚键连接的类异戊二烯链。作为关键的地球化学生物标志物,甘油二烷基甘油四醚(GDGTs)等古菌脂质是古气候代理指标的基础,而它们在门水平上的分布则揭示了系统发育差异。尽管基于质谱的定量生物标志物(主要是那些结构已确定的)在地球化学研究中已成熟并得到广泛应用,但对古菌脂质作为天然产物的系统研究却明显滞后。这一不足体现在三个关键方面:(1)提取方法缺乏适用于不同古菌类群和样品基质的通用方案。虽然存在比较研究,但指导方法选择的理论框架仍未得到充分探索。(2)由于古菌脂质的独特结构和复杂的异构化特征,纯化挑战依然存在,这阻碍了标准化分离方案的制定。(3)最关键的是,结构表征主要依赖于数十年前的基础研究。然而,现有综述在分析工作流程方面,更侧重于古菌脂质的化学结构、生物合成和应用方面。本综述通过采用天然产物化学的视角来弥补这一差距,整合了三个关键方面:(1)阐明古菌脂质各种提取技术的适用对象、范围和方法机制,涵盖培养样品和环境样品;(2)利用先进的色谱技术,阐明极性梯度脂质分级分离过程的分离原理;(3)详细探讨核磁共振在解析复杂脂质结构中的应用,特别强调确定立体化学构型。通过综合六十年来的方法演变,我们建立了一个从脂质提取到结构鉴定的全面分析框架。这种综合方法构建了一个用于古菌脂质分析的系统方法范式,将理论原理与实际操作联系起来。