Department of Cell and Systems Biology, University of Toronto, Toronto, Ontario, Canada M5S 3G5.
Department of Biology, University of Toronto-Mississauga, Mississauga, Ontario, Canada L5L 1C6.
Plant Physiol. 2022 Aug 1;189(4):2072-2090. doi: 10.1093/plphys/kiac207.
We present a methodology to survey central metabolism in 13CO2-labeled Arabidopsis (Arabidopsis thaliana) rosettes by ammonia positive chemical ionization-gas chromatography-mass spectrometry. This technique preserves the molecular ion cluster of methyloxime/trimethylsilyl-derivatized analytes up to 1 kDa, providing unambiguous nominal mass assignment of >200 central metabolites and 13C incorporation rates into a subset of 111 from the tricarboxylic acid (TCA) cycle, photorespiratory pathway, amino acid metabolism, shikimate pathway, and lipid and sugar metabolism. In short-term labeling assays, we observed plateau labeling of ∼35% for intermediates of the photorespiratory cycle except for glyoxylate, which reached only ∼4% labeling and was also present at molar concentrations several fold lower than other photorespiratory intermediates. This suggests photorespiratory flux may involve alternate intermediate pools besides the generally accepted route through glyoxylate. Untargeted scans showed that in illuminated leaves, noncyclic TCA cycle flux and citrate export to the cytosol revert to a cyclic flux mode following methyl jasmonate (MJ) treatment. MJ also caused a block in the photorespiratory transamination of glyoxylate to glycine. Salicylic acid treatment induced the opposite effects in both cases, indicating the antagonistic relationship of these defense signaling hormones is preserved at the metabolome level. We provide complete chemical ionization spectra for 203 Arabidopsis metabolites from central metabolism, which uniformly feature the unfragmented pseudomolecular ion as the base peak. This unbiased, soft ionization technique is a powerful screening tool to identify adaptive metabolic trends in photosynthetic tissue and represents an important advance in methodology to measure plant metabolic flux.
我们提出了一种方法,通过氨正化学电离-气相色谱-质谱法对 13CO2 标记的拟南芥(Arabidopsis thaliana) 叶片中的中心代谢物进行调查。该技术可保留甲肟/三甲基硅烷基衍生化分析物的分子离子簇,直至 1 kDa,从而提供 >200 种中心代谢物和 13C 掺入率的明确的名义质量分配,其中包括三羧酸(TCA)循环、光呼吸途径、氨基酸代谢、莽草酸途径以及脂质和糖代谢中的 111 种代谢物中的一部分。在短期标记实验中,我们观察到除了乙醛酸之外,光呼吸循环的中间体的标记达到约 35%的平台,而乙醛酸的标记仅达到约 4%,并且其摩尔浓度也比其他光呼吸中间体低几倍。这表明,除了通常通过乙醛酸的途径之外,光呼吸通量可能涉及替代的中间池。非靶向扫描表明,在照光的叶片中,非循环 TCA 循环通量和柠檬酸向细胞质的输出在茉莉酸甲酯(MJ)处理后恢复到循环通量模式。MJ 还导致乙醛酸到甘氨酸的光呼吸转氨作用受阻。水杨酸处理在这两种情况下都引起了相反的效果,表明这些防御信号激素在代谢组水平上保持着拮抗关系。我们提供了来自中心代谢物的 203 种拟南芥代谢物的完整化学电离光谱,它们均以未碎片化的准分子离子为基峰。这种无偏、软电离技术是一种强大的筛选工具,可用于识别光合作用组织中的适应性代谢趋势,代表了测量植物代谢通量的方法学的重要进展。