An Exfoliated 2-D Egyptian Blue Nanosheet for Highly Selective Enrichment of Multi-Phosphorylated Peptides in Mass Spectrometric Analysis
An Exfoliated 2-D Egyptian Blue Nanosheet for Highly Selective Enrichment of Multi-Phosphorylated Peptides in Mass Spectrometric Analysis
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用于质谱分析中多磷酸化肽高选择性富集的剥离二维埃及蓝纳米片
DOI：
10.1002/chem.201704138
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发表时间：
2018
期刊：
影响因子：
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通讯作者：
Gu Zhi-Yuan
中科院分区：
文献类型：
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作者：
Yang Shi-Shu;Yu Hai-Xia;Wang Zi-Zhen;Liu Hai-Long;Zhang Hao;Yu Xizhong;Shang Wenbin;Chen Gui-Quan;Gu Zhi-Yuan
由于复杂生物样品中磷肽的丰度较低，磷肽富集对于磷蛋白谱分析是必不可少的。此外，多磷酸肽相对于单磷酸肽的选择性结合很少建立，但在真实的样品分析中强烈需要，特别是对于多位点磷酸化级联的细胞行为的研究。在这里，合成了埃及蓝（CaCuSi4O10），众所周知的古老颜料及其类似物（SrCuSi4O10和BaCuSi4O10）的二维（2D）纳米片，它们首次用于富集磷酸肽。令人惊讶的是，2D CaCuSi4O10纳米片对多磷酸化肽具有高度选择性，而不会在宽范围的酸性条件或缓冲液组成中富集单磷酸化肽。同时，SrCuSi4O10和BaCuSi4O10纳米片类似物没有表现出这种独特的选择性.此外，将埃及蓝纳米片的具有丰富CaII的良好且定义明确的2D形态应用于与阿尔茨海默病相关的前脑特异性PDK 1条件性敲除小鼠及其年龄匹配的同窝对照的皮质样品中。所制备的二维CaCuSi4O10纳米片不仅表现出特定的选择性，而且还表现出高灵敏度（检测限为4×10−7m）。
Phosphopeptide enrichment is essential for the phosphoprotein profiling, due to the low abundance in complex biological samples. Moreover, selective binding of multi‐phosphopeptides over mono‐phosphopeptides is rarely established, but strongly needed in real sample analysis, especially for the investigation of cell behaviors with the multisite phosphorylation cascades. Here two‐dimensional (2D) nanosheets were synthesized of Egyptian blue (CaCuSi4O10), the well‐known ancient pigment, and its analogues (SrCuSi4O10and BaCuSi4O10), which were employed in the enrichment of phosphopeptides for the first time. Surprisingly, the 2D CaCuSi4O10nanosheet was highly selective towards multi‐phosphopeptides without enriching the mono‐phosphorylated peptides in a wide range of acidic conditions or buffer compositions. Meanwhile, the SrCuSi4O10and BaCuSi4O10nanosheet analogues do not exhibit this unique selectivity. Moreover, the ultrathin and well‐defined 2D morphology, with abundant CaII, of Egyptian blue nanosheet was applied in cortical samples of forebrain specificPDK1conditional knockout mice and their age‐matched littermate controls, that are associated with Alzheimer's disease. The as‐prepared 2D CaCuSi4O10nanosheet not only showed specific selectivity, but also exhibited high sensitivity (detection limit of 4×10−7m).