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碳捕集系统的界面见解:一氧化碳在单乙醇胺水溶液表面的吸收

Interfacial Insights into a Carbon Capture System: CO Uptake to an Aqueous Monoethanolamine Surface.

作者信息

McWilliams Laura E, Valley Nicholas A, Vincent Nina M, Richmond Geraldine L

机构信息

Department of Chemistry, University of Oregon , Eugene, Oregon 97403, United States.

California Northstate University College of Health Sciences , Rancho Cordova, California 95670, United States.

出版信息

J Phys Chem A. 2017 Oct 19;121(41):7956-7967. doi: 10.1021/acs.jpca.7b07742. Epub 2017 Oct 9.

Abstract

Monoethanolamine (MEA) is a benchmark scrubber for CO gas emissions reductions. Preliminary studies have indicated surface monoethanolamine could influence the greater chemistry of CO uptake. MEA is known to be surface active and orients at aqueous surfaces such that its nitrogen lone pair electrons are pointing toward the gas phase. This MEA orientation has the potential to facilitate CO surface chemistry; however, a thorough description of the chemistry at play during this important carbon capture reaction is lacking. These studies investigate the surface behavior of MEA during CO gas flow, monitoring product formation and species migration. A combination of experimental vibrational sum frequency spectroscopy (VSFS), surface tensiometry, molecular dynamics simulations, and density functional calculations are used to investigate this complex chemistry. CO is shown to react with MEA, perturbing the interface and leading to the presence of carbamic acid in the surface region. However, throughout this chemistry the surface remains largely populated by unreacted MEA. These studies provide insight into this important carbon capture reaction and provide a framework for future work examining interfacial reactions and dynamics.

摘要

单乙醇胺(MEA)是用于减少一氧化碳气体排放的一种基准吸收剂。初步研究表明,表面单乙醇胺可能会影响一氧化碳吸收的更复杂化学过程。已知MEA具有表面活性,且在水表面定向排列,使其氮孤对电子指向气相。这种MEA的取向有可能促进一氧化碳的表面化学过程;然而,对于这一重要碳捕获反应过程中发生的化学过程,仍缺乏全面的描述。这些研究考察了在一氧化碳气流中MEA的表面行为,监测产物形成和物种迁移。结合实验振动和频光谱(VSFS)、表面张力测定法、分子动力学模拟以及密度泛函计算来研究这种复杂的化学过程。结果表明,一氧化碳与MEA发生反应,扰动了界面,导致表面区域存在氨基甲酸。然而,在整个化学过程中,表面主要仍由未反应的MEA占据。这些研究为这一重要的碳捕获反应提供了深入了解,并为未来研究界面反应和动力学提供了框架。

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