Nontarget Analysis of Oxygenates in Catalytic Fast Pyrolysis Biocrudes by Supercritical Fluid Chromatography High-Resolution Mass Spectrometry

Josephine S. Lübeck; Giorgio Tomasi; Kristoffer G. Poulsen; Ofei D. Mante; David C. Dayton; Sylvain Verdier; Jan H. Christensen

doi:10.1021/acs.energyfuels.8b02983

Nontarget Analysis of Oxygenates in Catalytic Fast Pyrolysis Biocrudes by Supercritical Fluid Chromatography High-Resolution Mass Spectrometry

Josephine S. Lübeck, Giorgio Tomasi, Kristoffer G. Poulsen, Ofei D. Mante, David C. Dayton, Sylvain Verdier, Jan H. Christensen^*

^*Corresponding author for this work

Section for Environmental Chemistry and Physics

2 Citations (Scopus)

Abstract

Catalytic fast pyrolysis (CFP) biocrudes can comprise up to 30 wt % of oxygen content in compounds such as polyphenols, acids, carbonyls, and anhydrosugars and thus require upgrading by, e.g., hydrotreatment, to produce transport fuels. The chemical characterization of phenolic and acidic compounds in biocrudes is of great importance to optimize the CFP process. In this study, an analytical workflow is proposed for nontarget chemical fingerprinting analysis of CFP biocrudes using supercritical fluid chromatography high-resolution mass spectrometry (SFC-HRMS) with negative electrospray ionization (ESI ^- ), followed by multivariate data analysis. The method was developed and tested on five biocrude samples from loblolly pine (Pinus taeda) with varying oxygen content (14.9-28.8 wt % wet basis) due to different CFP conditions. The pixel-based analysis displayed chemical variation between all samples. Twenty-four regions of interest were tentatively identified, including mono- and polyphenols, fatty acids, and methylated and methoxylated phenols. The identification workflow and MS/MS analysis were prioritized on the peaks with the highest relative concentration. The developed SFC-ESI ^- -HRMS method shows high repeatability and analyzed oxygen-containing compounds with hydroxyl and/or carboxyl moieties in combination with other moieties of up to 400 Da.

Original language	English
Journal	Energy and Fuels
Volume	33
Issue number	1
Pages (from-to)	296-306
Number of pages	11
ISSN	0887-0624
DOIs	https://doi.org/10.1021/acs.energyfuels.8b02983
Publication status	Published - 17 Jan 2019

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title = "Nontarget Analysis of Oxygenates in Catalytic Fast Pyrolysis Biocrudes by Supercritical Fluid Chromatography High-Resolution Mass Spectrometry",

abstract = " Catalytic fast pyrolysis (CFP) biocrudes can comprise up to 30 wt % of oxygen content in compounds such as polyphenols, acids, carbonyls, and anhydrosugars and thus require upgrading by, e.g., hydrotreatment, to produce transport fuels. The chemical characterization of phenolic and acidic compounds in biocrudes is of great importance to optimize the CFP process. In this study, an analytical workflow is proposed for nontarget chemical fingerprinting analysis of CFP biocrudes using supercritical fluid chromatography high-resolution mass spectrometry (SFC-HRMS) with negative electrospray ionization (ESI - ), followed by multivariate data analysis. The method was developed and tested on five biocrude samples from loblolly pine (Pinus taeda) with varying oxygen content (14.9-28.8 wt % wet basis) due to different CFP conditions. The pixel-based analysis displayed chemical variation between all samples. Twenty-four regions of interest were tentatively identified, including mono- and polyphenols, fatty acids, and methylated and methoxylated phenols. The identification workflow and MS/MS analysis were prioritized on the peaks with the highest relative concentration. The developed SFC-ESI - -HRMS method shows high repeatability and analyzed oxygen-containing compounds with hydroxyl and/or carboxyl moieties in combination with other moieties of up to 400 Da. ",

author = "L{\"u}beck, {Josephine S.} and Giorgio Tomasi and Poulsen, {Kristoffer G.} and Mante, {Ofei D.} and Dayton, {David C.} and Sylvain Verdier and Christensen, {Jan H.}",

year = "2019",

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doi = "10.1021/acs.energyfuels.8b02983",

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T1 - Nontarget Analysis of Oxygenates in Catalytic Fast Pyrolysis Biocrudes by Supercritical Fluid Chromatography High-Resolution Mass Spectrometry

AU - Lübeck, Josephine S.

AU - Tomasi, Giorgio

AU - Poulsen, Kristoffer G.

AU - Mante, Ofei D.

AU - Dayton, David C.

AU - Verdier, Sylvain

AU - Christensen, Jan H.

PY - 2019/1/17

Y1 - 2019/1/17

N2 - Catalytic fast pyrolysis (CFP) biocrudes can comprise up to 30 wt % of oxygen content in compounds such as polyphenols, acids, carbonyls, and anhydrosugars and thus require upgrading by, e.g., hydrotreatment, to produce transport fuels. The chemical characterization of phenolic and acidic compounds in biocrudes is of great importance to optimize the CFP process. In this study, an analytical workflow is proposed for nontarget chemical fingerprinting analysis of CFP biocrudes using supercritical fluid chromatography high-resolution mass spectrometry (SFC-HRMS) with negative electrospray ionization (ESI - ), followed by multivariate data analysis. The method was developed and tested on five biocrude samples from loblolly pine (Pinus taeda) with varying oxygen content (14.9-28.8 wt % wet basis) due to different CFP conditions. The pixel-based analysis displayed chemical variation between all samples. Twenty-four regions of interest were tentatively identified, including mono- and polyphenols, fatty acids, and methylated and methoxylated phenols. The identification workflow and MS/MS analysis were prioritized on the peaks with the highest relative concentration. The developed SFC-ESI - -HRMS method shows high repeatability and analyzed oxygen-containing compounds with hydroxyl and/or carboxyl moieties in combination with other moieties of up to 400 Da.

AB - Catalytic fast pyrolysis (CFP) biocrudes can comprise up to 30 wt % of oxygen content in compounds such as polyphenols, acids, carbonyls, and anhydrosugars and thus require upgrading by, e.g., hydrotreatment, to produce transport fuels. The chemical characterization of phenolic and acidic compounds in biocrudes is of great importance to optimize the CFP process. In this study, an analytical workflow is proposed for nontarget chemical fingerprinting analysis of CFP biocrudes using supercritical fluid chromatography high-resolution mass spectrometry (SFC-HRMS) with negative electrospray ionization (ESI - ), followed by multivariate data analysis. The method was developed and tested on five biocrude samples from loblolly pine (Pinus taeda) with varying oxygen content (14.9-28.8 wt % wet basis) due to different CFP conditions. The pixel-based analysis displayed chemical variation between all samples. Twenty-four regions of interest were tentatively identified, including mono- and polyphenols, fatty acids, and methylated and methoxylated phenols. The identification workflow and MS/MS analysis were prioritized on the peaks with the highest relative concentration. The developed SFC-ESI - -HRMS method shows high repeatability and analyzed oxygen-containing compounds with hydroxyl and/or carboxyl moieties in combination with other moieties of up to 400 Da.

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Nontarget Analysis of Oxygenates in Catalytic Fast Pyrolysis Biocrudes by Supercritical Fluid Chromatography High-Resolution Mass Spectrometry

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