An evaluation of static ToF-SIMS analysis of environmental organics

Xiao Sui; Xiao Ying Yu

doi:10.1016/j.heliyon.2024.e37913

An evaluation of static ToF-SIMS analysis of environmental organics

Xiao Sui, Xiao Ying Yu

Advanced Nuclear Materials

Research output: Contribution to journal › Article › peer-review

Abstract

Time-of-flight secondary ion mass spectrometry (ToF-SIMS) has been extensively used in surface analysis due to its high mass resolution, sensitivity, and mass spectral imaging capabilities. Static ToF-SIMS has mainly been used for solid material analysis; however, its application in environmental organics is limited. During SIMS spectral analysis, relative mass accuracy and measurement repeatability are key factors for obtaining reliable speciation and acquiring chemical insights of the specimens. Herein, we provide an evaluation of four environmentally relevant organic systems, including glyoxal, pyruvic acid, oil-in-water emulsion, and carbon dioxide (CO₂) capture solvent (i.e., N-2-ethoxyethyl-3-morpholinopropan-1-amine, EMMPA), to show the spectral measurement repeatability when using static ToF-SIMS. First, sample preparation is essential in acquiring accurate and reproducible results in ToF-SIMS analysis. The mass spectral results show that characteristic peaks observed can be distinguished with reasonable confidence by comparing the observed mass to charge ratios (m/z) to theoretical ones. The statistical analysis of peak areas indicates that the peak area and/or peak height measurement ratios are satisfactory among replicates. Compared with previous studies, the bismuth cluster primary ion beam, namely Bi₃⁺, has less fragmentation than Bi⁺. Therefore, Bi₃⁺ is deemed more suitable for organic analysis using static SIMS. Our results show that ToF-SIMS offers a viable approach to study environmental organics including but not limited to aqueous aerosols, wastewater emulsions, and CO₂ capture solvents. It is expected that future studies will expand organic speciation with high fidelity due to the continued advancement of SIMS as a sensitive analysis technique.

Original language	English
Article number	e37913
Journal	Heliyon
Volume	10
Issue number	18
DOIs	https://doi.org/10.1016/j.heliyon.2024.e37913
State	Published - Sep 30 2024

Funding

Funding for Xiao Sui was provided by Natural Science Foundation of Shandong Province, grant number ZR2022QB137. Experimental efforts were supported by the strategic Laboratory Directed Research and Development (LDRD) of the Physical Sciences Directorate of the Oak Ridge National Laboratory (ORNL). Preparation of the manuscript was supported partially by the U. S. Department of Energy (DOE) Environmental Management (EM) program award 277636.Oak Ridge National Laboratory (ORNL) is managed by UT-Battelle, LLC, for the U. S. Department of Energy (DOE) under contract number DE-AC05-00OR22725. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). Funding for Xiao Sui was provided by Natural Science Foundation of Shandong Province, grant number ZR2022QB137. Experimental efforts were supported by the strategic Laboratory Directed Research and Development (LDRD) of the Physical Sciences Directorate of the Oak Ridge National Laboratory (ORNL). Preparation of the manuscript was supported partially by the U. S. Department of Energy (DOE) Environmental Management (EM) program award 277636. Oak Ridge National Laboratory (ORNL) is managed by UT-Battelle, LLC, for the U. S. Department of Energy (DOE) under contract number DE-AC05-00OR22725. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ).

Keywords

Aqueous organic aerosol
Emulsion
Organics
Solvent
Spectral repeatability
ToF-SIMS

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10.1016/j.heliyon.2024.e37913

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title = "An evaluation of static ToF-SIMS analysis of environmental organics",

abstract = "Time-of-flight secondary ion mass spectrometry (ToF-SIMS) has been extensively used in surface analysis due to its high mass resolution, sensitivity, and mass spectral imaging capabilities. Static ToF-SIMS has mainly been used for solid material analysis; however, its application in environmental organics is limited. During SIMS spectral analysis, relative mass accuracy and measurement repeatability are key factors for obtaining reliable speciation and acquiring chemical insights of the specimens. Herein, we provide an evaluation of four environmentally relevant organic systems, including glyoxal, pyruvic acid, oil-in-water emulsion, and carbon dioxide (CO2) capture solvent (i.e., N-2-ethoxyethyl-3-morpholinopropan-1-amine, EMMPA), to show the spectral measurement repeatability when using static ToF-SIMS. First, sample preparation is essential in acquiring accurate and reproducible results in ToF-SIMS analysis. The mass spectral results show that characteristic peaks observed can be distinguished with reasonable confidence by comparing the observed mass to charge ratios (m/z) to theoretical ones. The statistical analysis of peak areas indicates that the peak area and/or peak height measurement ratios are satisfactory among replicates. Compared with previous studies, the bismuth cluster primary ion beam, namely Bi3+, has less fragmentation than Bi+. Therefore, Bi3+ is deemed more suitable for organic analysis using static SIMS. Our results show that ToF-SIMS offers a viable approach to study environmental organics including but not limited to aqueous aerosols, wastewater emulsions, and CO2 capture solvents. It is expected that future studies will expand organic speciation with high fidelity due to the continued advancement of SIMS as a sensitive analysis technique.",

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AB - Time-of-flight secondary ion mass spectrometry (ToF-SIMS) has been extensively used in surface analysis due to its high mass resolution, sensitivity, and mass spectral imaging capabilities. Static ToF-SIMS has mainly been used for solid material analysis; however, its application in environmental organics is limited. During SIMS spectral analysis, relative mass accuracy and measurement repeatability are key factors for obtaining reliable speciation and acquiring chemical insights of the specimens. Herein, we provide an evaluation of four environmentally relevant organic systems, including glyoxal, pyruvic acid, oil-in-water emulsion, and carbon dioxide (CO2) capture solvent (i.e., N-2-ethoxyethyl-3-morpholinopropan-1-amine, EMMPA), to show the spectral measurement repeatability when using static ToF-SIMS. First, sample preparation is essential in acquiring accurate and reproducible results in ToF-SIMS analysis. The mass spectral results show that characteristic peaks observed can be distinguished with reasonable confidence by comparing the observed mass to charge ratios (m/z) to theoretical ones. The statistical analysis of peak areas indicates that the peak area and/or peak height measurement ratios are satisfactory among replicates. Compared with previous studies, the bismuth cluster primary ion beam, namely Bi3+, has less fragmentation than Bi+. Therefore, Bi3+ is deemed more suitable for organic analysis using static SIMS. Our results show that ToF-SIMS offers a viable approach to study environmental organics including but not limited to aqueous aerosols, wastewater emulsions, and CO2 capture solvents. It is expected that future studies will expand organic speciation with high fidelity due to the continued advancement of SIMS as a sensitive analysis technique.

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An evaluation of static ToF-SIMS analysis of environmental organics

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Keywords

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