BGC-03 Biogeochemistry of DOM
Will different interpretation strategies of the same ultra-high-resolution mass spectrometry data tell different biogeochemical stories? A first assessment based on natural aquatic samples  (Invited)
Yuanbi Yi* , Department of Ocean Science and Hong Kong Branch of the Southern Marine Science and Engineering Guangdong Laboratory (Guangzhou), The Hong Kong University of Science and Technology, Hong Kong, Hong Kong SAR, China
Chen He, State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing, China
Katrin Klaproth, ICBM-MPI Bridging Group for Marine Geochemistry, Institute for Chemistry and Biology of the Marine Environment, Carl von Ossietzky University, Oldenburg, Germany
Julian Merder, Department of Global Ecology, Carnegie Institution for Science, Stanford, California
Yulin Qi, Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin 300072, China
Pingqing Fu, Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin 300072, China
Siliang Li, Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin 300072, China
Thorsten Dittmar, ICBM-MPI Bridging Group for Marine Geochemistry, Institute for Chemistry and Biology of the Marine Environment, Carl von Ossietzky University, Oldenburg, Germany
Quan Shi, State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing, China
Ding He, Department of Ocean Science and Hong Kong Branch of the Southern Marine Science and Engineering Guangdong Laboratory (Guangzhou), The Hong Kong University of Science and Technology, Hong Kong, Hong Kong SAR, China

Fourier ion cyclotron resonance mass spectrometry (FT-ICR MS), one of the state-of-the-art ultra-high-resolution techniques, is widely used in dissolved organic matter (DOM) research. As research focusing on the identification of DOM molecular fingerprints increases tremendously, there is and will be an urgent need to compare among studies. Hawkes et al. (2020) has provided exiting evidence that the data from the same reference samples but analyzed among operating instruments and user operation conditions can be reasonably compared. Nevertheless, they use the same data processing, statistical methodology and interpretation strategy, which is not the common case. In reality, different research groups usually use three different types of interpretation strategies, including in-house codes, open-source platforms, and commercial software. It is therefore critical that the community start exploring (i) if different interpretation strategies will impact the comparability of FT-ICR MS results, and (ii) if they do, will they affect our established understanding of biogeochemical interpretations? To simplify and preliminary address this question, we purposely selected DOM samples along a typical freshwater to marine continuum, the Yangtze River Estuary to East China Sea, to be measured by negative-ion mode electrospray ionization FT-ICR MS. We interpreted the raw MS data using three strategies, compared the results and evaluated the interpretation strategy-induced effects on biogeochemical interpretations. Our results show that different interpretation strategies have a non-negligible influence on the number of heteroatoms in the DOM but a less impact on peak abundance. A total of 3827 formulas accounting for 91.6±4.1% (on average) of the total intensity are assigned in all interpretation strategies, while 6546 formulas accounting for 8.4±4.1% (on average) are not commonly assigned in all three interpretation strategies. By correlating a series of molecular parameters from three interpretation strategies with salinity, we show strong evidence that (i) different interpretation strategies, once performed with caution, do not significantly affect the geochemical stories relied on DOM molecular composition, and (ii) comparison based on intensity results give more reliable results than the formular number alone. Moreover, we also provide raw data and interpreted data (by our three strategies) and encourage the community to compare their interpretation with ours. We aim to call attention to the community for improving the comparability of FT-ICR MS results and facilitating the integration of DOM molecular composition among studies.