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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
Analytical Chemistry ( IF 6.7 ) Pub Date : 2021-09-14 , DOI: 10.1021/acs.analchem.1c02710
Cunhao Cui 1 , Xiamin Chen 1 , Chunjiang Liu 1 , Yanan Zhu 1 , Linyu Zhu 1 , Jianfeng Ouyang 1 , Yang Shen 1 , Zhongyue Zhou 1 , Fei Qi 1
Affiliation  

Process 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.

中文翻译:

多相催化反应的原位反应器集成电喷雾电离质谱及其在高压液相木质素解聚过程分析中的应用

木质素解聚等多相催化反应的过程分析对于在分子水平上理解反应机理至关重要,但由于条件苛刻,它总是具有挑战性。在此,我们通过反应器集成电喷雾电离 (R-ESI) 技术将微批次反应器与高分辨率质谱 (MS) 相结合,报告了一种操作过程分析策略。R-ESI-MS 将传统原位 MS 的应用扩展到非均相和高压液相系统。通过这种策略,我们展示了在操作条件(甲醇溶剂,260°C,~8 MPa)下木质素解聚过程中一系列单体、二聚体和低聚物的演变,这是对渐进解聚途径和证据的首次实验阐明活性单体的再聚合。所提出的 R-ESI-MS 在探测木质素的解聚中间体方面至关重要;它还为在操作条件下多相催化反应的过程分析提供了灵活的策略。
更新日期:2021-09-28
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