Neutral Loss Fragmentation Pattern Based Screening for Arginine-Rich Natural Products in Xenorhabdus and Photorhabdus
Neutral Loss Fragmentation Pattern Based Screening for Arginine-Rich Natural Products in Xenorhabdus and Photorhabdus
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DOI：
10.1021/ac300372p
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发表时间：
2012-08-21
影响因子：
7.4
通讯作者：
Bode, Helge B.
中科院分区：
文献类型：
--
作者：
Fuchs, Sebastian W.;Sachs, Christian C.;Bode, Helge B.
虽然天然产物具有一定程度的结构一致性，但它们具有不同的功能，如不同的氨基酸或酰基残基。在碰撞诱导解离过程中，一些天然产物表现出接近前体离子的保守碎裂模式。观察到的片段来自一组共享的中性损失，产生了一种独特的片段化模式，可以用作这些天然产物类别成员的指纹。采用MALDI-MS 2对69株大肠杆菌的培养上清进行分析，建立了包含各菌株MS 2数据的数据库。使用定制软件扫描该数据库以获得不同化合物的一致碎片化模式，重点是碎片离子与其前体离子的相对质量差异。鉴定了一组新的相关天然产物，包括来自16种不同菌株的25种不同的富含精氨酸的肽，由于其特征性的中性丢失片段化模式，并鉴定了8个化合物的结构。两个生物合成基因簇编码的非核糖体肽合成酶进行了鉴定，强调可能性，以确定一组结构和生物合成相关的天然产物的基础上，他们的中性损失片段化模式。
Although sharing a certain degree of structural uniformity, natural product classes exhibit variable functionalitics such as different amino acid or acyl residues. During collision induced dissociation, some natural products exhibit a conserved fragmentation pattern close to the precursor ion. The observed fragments result from a shared set of neutral losses, creating a unique fragmentation pattern, which can be used as a fingerprint for members of these natural product classes. The culture supernatants of 69 strains of the were analyzed by MALDI-MS2, and a database comprising MS2 data from each strain was established. This database was scanned for concordant fragmentation patterns of different compounds using a customized software, focusing on relative mass differences of the fragment ions to their precursor ion. A novel group of related natural products comprising 25 different arginine-rich peptides from 16 different strains was identified due to its characteristic neutral loss fragmentation pattern, and the structures of eight compounds were elucidated. Two biosynthesis gene clusters encoding nonribosomal peptide synthetases were identified, emphasizing the possibility to identify a group of structurally and biosynthetically related natural products based on their neutral loss fragmentation pattern.