Organic carbon distribution, speciation, and elemental correlations within soil microaggregates: Applications of STXM and NEXAFS spectroscopy     

Jiamin Wan  Tolek Tyliszczak  Tetsu K. Tokunaga 《Geochimica et cosmochimica acta》2007,71(22):5439-5449

Soils contain the largest inventory of organic carbon on the Earth’s surface. Therefore, it is important to understand how soil organic carbon (SOC) is distributed in soils. This study directly measured SOC distributions within soil microaggregates and its associations with major soil elements from three soil groups (Phaeozem, Cambisol, and Ultisol), using scanning transmission X-ray microscopy (STXM) and near-edge X-ray absorption fine structure (NEXAFS) spectroscopy at a spatial resolution of 30 nm. Unlike previous studies, small intact soil microaggregates were examined directly in order to avoid preparatory procedures that might alter C speciation. We found that SOC exists as distinct particles (10s to 100s of nm) and as ubiquitous thin coatings on clay minerals and iron-oxides coatings. The distinct SOC particles have higher fractions of aromatic C than the coatings. NEXAFS spectra of the C coatings within individual microaggregates were relatively similar. In the Phaeozem soil, the pervasive spectral features were those of phenolic and carboxylic C, while in the Cambisol soil the most common spectral feature was the carboxyl peak. The Ultisol soil displayed a diffuse distribution of aromatic, phenolic, and carboxylic C peaks over all surfaces. In general, a wide range of C functional groups coexist within individual microaggregates. In this work we were able to, for the first time, directly quantify the major mineral elemental (Si, Al, Ca, Fe, K, Ti) compositions simultaneously with C distribution and speciation at the nm to μm scale. These direct microscale measurements will help improve understanding on SOC-mineral associations in soil environments.  相似文献   

Composition and structural aspects of naturally occurring ferrihydrite     

A. Cristina Cismasu  F. Marc Michel  A. Patricia Tcaciuc  Tolek Tyliszczak  Gordon E. Brown  Jr 《Comptes Rendus Geoscience》2011,343(2-3):210-218

A series of naturally occurring ferrihydrites sampled from an acid mine drainage environment were characterized and compared with synthetic 2-line ferrihydrite using high energy X-ray total scattering and pair distribution function analysis, Scanning Transmission X-ray Microscopy (STXM), Transmission Electron Microscopy (TEM), BET N₂ surface area measurements, and chemical extractions in order to place constraints on their structural and physical properties as a function of composition. Overall, the short- and intermediate-range ordering of the natural samples is comparable to synthetic ferrihydrite. However, with increasing Al, Si, and organic matter contents, a decrease in particle size and an increase in structural disorder were observed. Silica is suspected to have a pronounced effect on the crystallinity of ferrihydrite as a result of its inhibitory effect on Fe polymerization and particle growth, and it is likely complexed at the surfaces of ferrihydrite nanoparticles. Aluminum, on the other hand may substitute for Fe³⁺ in natural ferrihydrite. Organic matter is pervasive and intimately associated with ferrihydrite aggregates, and its presence during ferrihydrite precipitation may have contributed to additional structural disorder. The increase in impurity content affects not only the particle size and structural order of ferrihydrite but may also have a significant effect on its surface reactivity.  相似文献   

Constraints on the formation environment of two chondrule‐like igneous particles from comet 81P/Wild 2          下载免费PDF全文

Zack Gainsforth  Anna L. Butterworth  Julien Stodolna  Andrew J. Westphal  Gary R. Huss  Kazu Nagashima  Ryan Ogliore  Donald E. Brownlee  David Joswiak  Tolek Tyliszczak  Alexandre S. Simionovici 《Meteoritics & planetary science》2015,50(5):976-1004

Using chemical and petrologic evidence and modeling, we deduce that two chondrule‐like particles named Iris and Callie, from Stardust cometary track C2052,12,74, formed in an environment very similar to that seen for type II chondrules in meteorites. Iris was heated near liquidus, equilibrated, and cooled at ≤100 °C h^‐1 and within ≈2 log units of the IW buffer with a high partial pressure of Na such as would be present with dust enrichments of ≈10³. There was no detectable metamorphic, nebular, or aqueous alteration. In previous work, Ogliore et al. (2012) reported that Iris formed late, >3 Myr after CAIs, assuming ²⁶Al was homogenously distributed, and was rich in heavy oxygen. Iris may be similar to assemblages found only in interplanetary dust particles and Stardust cometary samples called Kool particles. Callie is chemically and isotopically very similar, but not identical to Iris.  相似文献