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In Situ Reactor-Integrated Electrospray Ionization Mass Spectrometry for Heterogeneous Catalytic Reactions and Its Application in the Process Analysis of High-Pressure Liquid-Phase Lignin Depolymerization
journal contribution
posted on 2021-09-14, 16:38 authored by Cunhao Cui, Xiamin Chen, Chunjiang Liu, Yanan Zhu, Linyu Zhu, Jianfeng Ouyang, Yang Shen, Zhongyue Zhou, Fei QiProcess
analysis of heterogeneous catalytic reactions such as lignin
depolymerization is essential to understand the reaction mechanism
at the molecular level, but it is always challenging due to harsh
conditions. Herein, we report an operando process analysis strategy
by combining a microbatch reactor with high-resolution mass spectrometry
(MS) via a reactor-integrated electrospray ionization (R-ESI) technique.
R-ESI-MS expands the applications of traditional in situ MS to a heterogeneous
and high-pressure liquid-phase system. With this strategy, we present
the evolution of a series of monomers, dimers, and oligomers during
lignin depolymerization under operando conditions (methanol solvent,
260 °C, ∼8 MPa), which is the first experimental elucidation
of a progressive depolymerization pathway and evidence of repolymerization
of active monomers. The proposed R-ESI-MS is crucial in probing depolymerization
intermediates of lignin; it also provides a flexible strategy for
process analysis of heterogeneous catalytic reactions under operando
conditions.
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resolution mass spectrometryintegrated electrospray ionizationfirst experimental elucidationalways challenging due260 ° cprogressive depolymerization pathwayprobing depolymerization intermediatesheterogeneous catalytic reactionslignin depolymerizationreaction mechanismprocess analysispressure liquidphase systemoperando conditionsmolecular levelmethanol solventharsh conditionsalso provides