Laboratory of Analytical, Bioanalytical Sciences and Miniaturization, Chemistry, Biology and Innovation (CBI) UMR 8231, ESPCI Paris PSL, CNRS, PSL Research University, Paris, France.
Université Paris Cité, INSERM, "Pathophysiology & Pharmacotoxicology of the Human Placenta, pre & postnatal Microbiota", 3PHM, F-75006 Paris, France.
J Pharm Biomed Anal. 2024 May 15;242:116022. doi: 10.1016/j.jpba.2024.116022. Epub 2024 Feb 8.
Human chorionic gonadotropin (hCG) is constituted of the hCGα and hCGβ subunits and is a highly glycosylated protein. Affinity supports based on immobilized Concanavalin A (Con A) lectin were used in solid phase extraction (SPE) to fractionate the hCG glycoforms according to their glycosylation state. For the first time, the lectin SPE fractions were off-line analysed by a nano liquid chromatography - high-resolution mass spectrometry (nanoLC-HRMS) method keeping the glycoforms intact. For this, home-made Con A sorbents were prepared by immobilizing lectin on Sepharose with a mean grafting yield of 98.2% (relative standard deviation (RSD) of 3.5%, n = 15). A capacity of about 100 μg of purified urinary hCG (uhCG) per ml of sorbent, grafted with a density of 10 mg of Con A per ml, was estimated. Average extraction yields of around 60% for both hCGα and hCGβ glycoforms were obtained after optimization of the extraction protocol. Intra- and inter-assay evaluation led to average RSD values of around 10%, indicating a repeatable extraction procedure. Similar results were obtained with commercial Con A-based sorbents but only after their 3rd use or after an extensive pre-conditioning step. Finally, the Con A SPE led to the fractionation of some glycoforms of uhCG, allowing the detection of an hCGα glycoform with two tetra-antennary N-glycans that couldn't be detected by direct analysis in nanoLC-HRMS without Con A SPE. Regarding a recombinant hCG, a fractionation was also observed leading to the detection of unretained hCGα glycoforms with tri-antennary N-glycans. Therefore, the combination of lectin SPE with intact protein analysis by nanoLC-HRMS can contribute to a more detailed glycosylation characterization of the hCG protein.
人绒毛膜促性腺激素(hCG)由 hCGα 和 hCGβ 亚基组成,是一种高度糖基化的蛋白质。基于固定化刀豆球蛋白 A(Con A)凝集素的亲和载体被用于固相萃取(SPE),根据糖基化状态对 hCG 糖型进行分级。这是首次采用纳米液相色谱 - 高分辨率质谱(nanoLC-HRMS)方法在线下分析凝集素 SPE 级分,同时保持糖型完整。为此,通过将凝集素固定在琼脂糖上,制备了自制的 Con A 吸附剂,接枝产率约为 98.2%(相对标准偏差(RSD)为 3.5%,n=15)。估计每毫升吸附剂可结合约 100μg 纯化的尿液 hCG(uhCG),结合密度约为 10mg/ml 的 Con A。通过优化萃取方案,获得了 hCGα 和 hCGβ 糖型的平均萃取率约为 60%。内标和间标评估的平均 RSD 值约为 10%,表明萃取程序具有重复性。使用商业 Con A 基吸附剂也可获得类似的结果,但仅在第 3 次使用或经过广泛的预处理步骤后才能获得。最后,Con A SPE 导致 uhCG 的一些糖型得到分级,这使得能够检测到在没有 Con A SPE 的情况下直接在 nanoLC-HRMS 中无法检测到的具有两个四天线 N-聚糖的 hCGα 糖型。对于重组 hCG,也观察到了分级,导致检测到未保留的具有三天线 N-聚糖的 hCGα 糖型。因此,凝集素 SPE 与 nanoLC-HRMS 对完整蛋白质分析的结合,可以有助于更详细地研究 hCG 蛋白的糖基化特征。