Near-edge X-ray absorption fine structure (NEXAFS) spectroscopy for mapping nano-scale distribution of organic carbon forms in soil: Application to black carbon particles

Johannes Lehmann, Biqing Liang, Dawit Solomon, Mirna Lerotic, Flavio Luizão, James Kinyangi, Thorsten Schäfer, Sue Wirick, Chris Jacobsen

Research output: Contribution to journalArticle

170 Citations (Scopus)

Abstract

Small-scale heterogeneity of organic carbon (C) forms in soils is poorly quantified since appropriate analytical techniques were not available up to now. Specifically, tools for the identification of functional groups on the surface of micrometer-sized black C particles were not available up to now. Scanning Transmission X-ray Microscopy (STXM) using synchrotron radiation was used in conjunction with Near-Edge X-ray Absorption Fine Structure (NEXAFS) spectroscopy to investigate nano-scale distribution (50-nm resolution) of C forms in black C particles and compared to synchrotron-based FTIR spectroscopy. A new embedding technique was developed that did not build on a C-based embedding medium and did not pose the risk of heat damage to the sample. Elemental sulfur (S) was melted to 220°C until it polymerized and quenched with liquid N2 to obtain a very viscous plastic S in which the black C could be embedded until it hardened to a noncrystalline state and was ultrasectioned. Principal component and cluster analysis followed by singular value decomposition was able to resolve distinct areas in a black carbon particle. The core of the studied biomass-derived black C particles was highly aromatic even after thousands of years of exposure in soil and resembled the spectral characteristics of fresh charcoal. Surrounding this core and on the surface of the black C particle, however, much larger proportions of carboxylic and phenolic C forms were identified that were spatially and structurally distinct from the core of the particle. Cluster analysis provided evidence for both oxidation of the black C particle itself as well as adsorption of non-black C. NEXAFS spectroscopy has great potential to allow new insight into black C properties with important implications for biogeochemical cycles such as mineralization of black C in soils and sediments, and adsorption of C, nutrients, and pollutants as well as transport in the geosphere, hydrosphere, and atmosphere.

Original languageEnglish
Pages (from-to)1-12
Number of pages12
JournalGlobal Biogeochemical Cycles
Volume19
Issue number1
DOIs
Publication statusPublished - 2005 Mar 1

Fingerprint

X ray absorption near edge structure spectroscopy
Soot
black carbon
Organic carbon
organic carbon
spectroscopy
Cluster analysis
Soils
Hydrosphere
Adsorption
soil
Wave transmission
Charcoal
Singular value decomposition
Synchrotron radiation
Synchrotrons
Sulfur
Principal component analysis
Functional groups
Nutrients

All Science Journal Classification (ASJC) codes

  • Global and Planetary Change
  • Environmental Chemistry
  • Environmental Science(all)
  • Atmospheric Science

Cite this

Lehmann, Johannes ; Liang, Biqing ; Solomon, Dawit ; Lerotic, Mirna ; Luizão, Flavio ; Kinyangi, James ; Schäfer, Thorsten ; Wirick, Sue ; Jacobsen, Chris. / Near-edge X-ray absorption fine structure (NEXAFS) spectroscopy for mapping nano-scale distribution of organic carbon forms in soil : Application to black carbon particles. In: Global Biogeochemical Cycles. 2005 ; Vol. 19, No. 1. pp. 1-12.
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Near-edge X-ray absorption fine structure (NEXAFS) spectroscopy for mapping nano-scale distribution of organic carbon forms in soil : Application to black carbon particles. / Lehmann, Johannes; Liang, Biqing; Solomon, Dawit; Lerotic, Mirna; Luizão, Flavio; Kinyangi, James; Schäfer, Thorsten; Wirick, Sue; Jacobsen, Chris.

In: Global Biogeochemical Cycles, Vol. 19, No. 1, 01.03.2005, p. 1-12.

Research output: Contribution to journalArticle

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