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ACS Nano. 2017 Sep 26;11(9):9500-9513. doi: 10.1021/acsnano.7b05328. Epub 2017 Sep 1.

Hydroxyl-Group-Dominated Graphite Dots Reshape Laser Desorption/Ionization Mass Spectrometry for Small Biomolecular Analysis and Imaging.

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School of Basic Medical Sciences, Beijing University of Chinese Medicine , Beijing 100029, China.
Center of Electron Microscopy and State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University , Hangzhou, Zhejiang Province 310027, China.
College of Life Science and Oceanography, Shenzhen Key Laboratory of Marine Bioresources and Ecology, Shenzhen University , Shenzhen, Guangdong Province 518060, China.
Department of Chemistry, Columbia University , New York, New York 10027, United States.
Department of Materials Science and Engineering, Technion Israel Institute of Technology , Haifa 3200003, Israel.


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.


DFT calculations; MALDI matrix; biomolecules; carbon nanomaterials; mass spectrometry imaging

[Indexed for MEDLINE]

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