Sun Yan, Stransky Stephanie, Aguilan Jennifer, Brenowitz Michael, Sidoli Simone
Department of Biochemistry, Albert Einstein College of Medicine, New York, NY, USA.
Laboratory for Macromolecular Analysis and Proteomics Facility, Albert Einstein College of Medicine, New York, NY, USA.
MethodsX. 2021 Nov 18;8:101585. doi: 10.1016/j.mex.2021.101585. eCollection 2021.
DNA modifications are small covalent chemical groups that modify nucleotides to regulate DNA readout. Anomalous abundance and genome-wide localization of these modifications can negatively tune gene expression and propagate into unbalanced epigenetics regulation, which is known to be associated with multiple conditions such as cancer, diabetes and aging. We present a direct injection mass spectrometry (DI-MS) platform that offers fast, accurate and precise quantitation of global levels of DNA cytidine methylation (mC) and hydroxymethylation (hmC) in less than one minute per sample. On the contrary to most methods adopting mass spectrometry for the analysis of nucleotide modifications, in this DI-MS approach we eliminate the use of liquid chromatography, increasing throughput, eliminating issues of carryover and batch effects caused by column contamination across samples. In addition, potential biases in detection efficiency of modified nucleotides with different binding efficiency to stationary phases is eliminated, as no chromatographic separation is adopted. This method can analyze >1000 samples per day, overcoming the throughput of next-generation sequencing.•Direct injection mass spectrometry improves throughput and precision compared to liquid chromatography.•Direct injection can be used to quantify in less than one minute global levels of DNA methylation and hydroxymethylation.•The unbiased acquisition can be potentially utilized to analyze other nucleotide modifications.
DNA修饰是一类小的共价化学基团,可修饰核苷酸以调控DNA的读出。这些修饰的异常丰度和全基因组定位会对基因表达产生负面影响,并导致表观遗传学调控失衡,而这与癌症、糖尿病和衰老等多种病症相关。我们提出了一种直接进样质谱(DI-MS)平台,该平台能够在每个样品不到一分钟的时间内,快速、准确且精确地定量分析DNA胞嘧啶甲基化(mC)和羟甲基化(hmC)的整体水平。与大多数采用质谱分析核苷酸修饰的方法不同,在这种DI-MS方法中,我们省去了液相色谱的使用,提高了通量,消除了由于样品间柱污染导致的残留和批次效应问题。此外,由于不采用色谱分离,消除了不同结合效率的修饰核苷酸在固定相上检测效率的潜在偏差。该方法每天可分析超过1000个样品,克服了下一代测序的通量限制。
•与液相色谱相比,直接进样质谱提高了通量和精度。
•直接进样可在不到一分钟的时间内定量分析DNA甲基化和羟甲基化的整体水平。
•无偏差采集有可能用于分析其他核苷酸修饰。