Comprehensive profiling of ribonucleosides modification by affinity zirconium oxide-silica composite monolithic column online solid-phase microextraction - Mass spectrometry analysis
Comprehensive profiling of ribonucleosides modification by affinity zirconium oxide-silica composite monolithic column online solid-phase microextraction - Mass spectrometry analysis
复制标题
亲和氧化锆-二氧化硅复合整体柱在线固相微萃取对核糖核苷修饰的综合分析-质谱分析
DOI：
10.1016/j.chroma.2016.07.086
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发表时间：
2016
影响因子：
4.1
通讯作者：
Feng Yu-Qi
中科院分区：
文献类型：
--
作者：
Jiang Han-Peng;Chu Jie-Mei;Lan Meng-Dan;Liu Ping;Yang Na;Zheng Fang;Yuan Bi-Feng;Feng Yu-Qi
More than 140 modified ribonucleosides have been identified in RNA. Determination of endogenous modified ribonucleosides in biological fluids may serve as non-invasive disease diagnostic strategy. However, detection of the modified ribonucleosides in biological fluids is challenging, especially for the low abundant modified ribonucleosides due to the serious matrix interferences of biological fluids. Here, we developed a facile preparation strategy and successfully synthesized zirconium oxide-silica (ZrO2/SiO2) composite capillary monolithic column that exhibited excellent performance for the selective enrichment ofcis-diol-containing compounds. Compared with the boronate-based affinity monolith, the ZrO2/SiO2monolith showed ∼2 orders of magnitude higher extraction capacity and can be used under physiological pH (pH 6.5–7.5). Using the prepared ZrO2/SiO2composite monolith as the trapping column and reversed-phase C18 column as the analytical column, we further established an online solid-phase microextraction (SPME) in combination with liquid chromatography-mass spectrometry (online SPME-LC–MS/MS) analysis for the comprehensive profiling of ribonucleosides modification in human urine. Our results showed that 68cis-diol-containing ribosylated compounds were identified in human urine, which is, to the best of our knowledge, the highest numbers ofcis-diol-containing compounds were determined in a single analysis. It is worth noting that four modified ribonucleosides were discovered in the human urine for the first time. In addition, the quantification results from the pooled urine samples showed that compared to healthy controls, the contents of sixteen ribose conjugates in the urine of gastric cancer, eleven in esophagus cancer and seven in lymphoma increased more than two folds. Among these ribose conjugates, four ribose conjugates increased more than two folds in both gastric cancer and esophagus cancer; three ribose conjugates increased more than two folds in both gastric cancer and lymphoma; one ribose conjugate increased more than two folds in both esophagus cancer and lymphoma. The developed analytical method provides a good platform to study the modified ribonucleosides in human body fluids.
