期刊
ACS NANO
卷 11, 期 9, 页码 9500-9513出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.7b05328
关键词
MALDI matrix; carbon nanomaterials; mass spectrometry imaging; biomolecules; DFT calculations
类别
资金
- National Science and Technology Major Project Fund [2011ZX02707]
- National Basic Research Program of China (973 Program) [2013CB932702]
- National Natural Science Foundation of China [21275106, 51422207, 21575095, 11374221, 51132006, 51572179, 21471106, 21501126, 11574224, 21320102003]
- Specialized Research Fund for the Doctoral Program of Higher Education [20123201110018]
- Collaborative Innovation Center of Suzhou Nano Science and Technology
- Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
- China Postdoctoral Science Foundation [2016M591901]
- 1000 Youth Talents plan of the Global Expert Recruitment Program
Small molecules play critical roles in life science, yet their facile detection and imaging in physiological or pathological settings remain a challenge. Matrix-assisted laser desorption ionization mass spectrometry (MALDI MS) is a powerful tool for molecular analysis. However, conventional organic matrices (CHCA, DHB, etc.) used in assisting analyte ionization suffer from intensive background noise in the mass region below m/z 700, which hinders MALDI MS applications for small-molecule detection. Here, we report that a hydroxyl-group dominated graphite dot (GD) matrix overcomes limitations of conventional matrices and allows MALDI MS to be used in fast and high throughput analysis of small biomolecules. GDs exhibit extremely low background noise and ultrahigh sensitivity (with limit of detection <1 fmol) in MALDI MS. This approach allows identification of complex oligosaccharides, detection of low-molecular weight components in traditional Chinese herbs, and facile analysis of puerarin and its metabolites in serum without purification. Moreover, we show that the GDs provide an effective matrix for the direct imaging or spatiotemporal mapping of small molecules and their metabolites (m/z < 700) simultaneously at the suborgan tissue level. Density functional theory calculations further provide the mechanistic basis of GDs as an effective MALDI matrix in both the positive-ion and negative-ion modes. Collectively, our work uncovered a useful matrix which reshapes MALDI MS technology for a wide range of applications in biology and medicine.
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