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Distribution and speciation of rare earth elements in coal combustion by-products via synchrotron microscopy and spectroscopy

Journal Article · · International Journal of Coal Geology
 [1];  [2];  [2]
  1. National Energy Technology Lab. (NETL), Pittsburgh, PA (United States). Research and Innovation Center; AECOM, Pittsburgh, PA (United States)
  2. National Energy Technology Lab. (NETL), Pittsburgh, PA (United States). Research and Innovation Center
Rare earth element (REE) binding environments and associated mineral phases in coal and coal combustion byproducts (CCBs) are not well understood. Advanced characterization of REEs' binding environments before, during, and after production can be vital in establishing an economically viable recovery method for REEs from these materials. Here, this study characterized different REE distributions, cerium (Ce) oxidation states, and Ce binding environments in 11 CCBs collected from various locales via X-ray fluorescence (XRF) elemental mapping and X-ray absorption near edge structure (XANES) at Stanford Synchrotron Radiation Lightsource (SSRL). Bulk Ce LIII edge XANES identified Ce(III) (>85%) as the predominant Ce oxidation state in all studied samples. Ce speciation and XRF elemental map analyses further reveal the REEs in studied samples can be (1) dispersed throughout the aluminosilicate glass phase, (2) as micro-particles in large glass grain, or (3) as independent trace phases in studied samples. Both fly ash and bottom ash contain mainly Ce(III) micro-hotspots (<40 μm), co-localization with a range of elements, including, but not limited to: P, S, Ca, Ti, and Mn. At microscale, Ce can change from Ce(III) to mixture of Ce(III) and Ce(IV) and to 100% Ce(IV) oxide, revealing potential REE-phase decomposition and oxidation in coal and coal combustion process. Our study also observed intraparticle and interparticle distribution difference between light REEs and heavy REEs. Finally, the synchrotron-based characterization confirmed the presence of these trace, previously only theorized, phases during the combustion process and ultimately may inform the simplification of separation and extraction processes for REE from different CCBs.
Research Organization:
National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)
Sponsoring Organization:
USDOE Office of Fossil Energy (FE); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
Grant/Contract Number:
FE0004000
OSTI ID:
1478326
Alternate ID(s):
OSTI ID: 1564518
Journal Information:
International Journal of Coal Geology, Journal Name: International Journal of Coal Geology Journal Issue: C Vol. 195; ISSN 0166-5162
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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The Occurrence and Concentration of Rare Earth Elements in Acid Mine Drainage and Treatment Byproducts. Part 2: Regional Survey of Northern and Central Appalachian Coal Basins journal October 2019
Atomic Spectrometry Update: review of advances in elemental speciation journal January 2016
Atomic spectrometry update: review of advances in elemental speciation journal January 2017
Differences in bulk and microscale yttrium speciation in coal combustion fly ash journal January 2018
Atomic Spectrometry Update: review of advances in elemental speciation journal January 2018
Atomic spectrometry update: review of advances in elemental speciation journal January 2019
Atomic spectrometry update: review of advances in elemental speciation journal January 2020
Distribution of rare earth and selected trace elements in combustion products of Yerkovetskoe brown coal deposit (Amur Region, Russia) journal July 2019
Structural Characterizations of Aluminosilicates in Two Types of Fly Ash Samples from Shanxi Province, North China journal June 2019

Figures / Tables (14)