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Title: Size Dependent Catalytic Activity of Iron (0) Nanoparticles as Hydrogenation Catalysts.

Abstract

Abstract not provided.

Authors:
; ; ;
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1377746
Report Number(s):
SAND2016-8160C
646807
DOE Contract Number:
AC04-94AL85000
Resource Type:
Conference
Resource Relation:
Conference: Proposed for presentation at the American Chemical Society held August 20-25, 2016 in Philadelphia , Pennsylvania.
Country of Publication:
United States
Language:
English

Citation Formats

Bleier, Grant Christopher, Huber, Dale L., Simocko, Chester K, and Watt, John Daniel. Size Dependent Catalytic Activity of Iron (0) Nanoparticles as Hydrogenation Catalysts.. United States: N. p., 2016. Web.
Bleier, Grant Christopher, Huber, Dale L., Simocko, Chester K, & Watt, John Daniel. Size Dependent Catalytic Activity of Iron (0) Nanoparticles as Hydrogenation Catalysts.. United States.
Bleier, Grant Christopher, Huber, Dale L., Simocko, Chester K, and Watt, John Daniel. 2016. "Size Dependent Catalytic Activity of Iron (0) Nanoparticles as Hydrogenation Catalysts.". United States. doi:. https://www.osti.gov/servlets/purl/1377746.
@article{osti_1377746,
title = {Size Dependent Catalytic Activity of Iron (0) Nanoparticles as Hydrogenation Catalysts.},
author = {Bleier, Grant Christopher and Huber, Dale L. and Simocko, Chester K and Watt, John Daniel},
abstractNote = {Abstract not provided.},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = 2016,
month = 8
}

Conference:
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  • The catalytic properties of catalysts that are active in a short-residence time coal hydrogenation reactor are discussed. Zinc halides and stannous chloride are found to be among the most active of a large number of catalysts tested. Surface acidities are determined by titration with amine bases. The acidity of these catalysts and of coals impregnated with these catalysts are compared with those of catalysts active in long-residence time batch coal-hydrogenation experiments and in other hydrogenation reactions. The activity of these catalysts in other chemical reactions are discussed in terms of their activity in coal hydrogenation.
  • The objective of this work was to determine how adsorption, catalytic and electronic properties of iron are affected by crystallite size and metal-support interactions. Adsorption, physical/chemical, and catalytic properties of 1, 3, and 10 wt.% Fe/activated carbon catalysts were investigated. From measurements of activity and selectivity for CO hydrogenation at 1 atm, H/sub 2//CO = 2 and 450-530 K, it is evident that initial and steady-state specific activities and olefin/paraffin ratio decrease with decreasing metal crystallite size. Contrary to previous reports activity of well dispersed Fe/C decreases very significantly with time. Moessbauer spectroscopy data provide evidence that small superparamagnetic clustersmore » of iron metal are the predominant iron phases in 1 and 3% Fe/carbon. The electron density of these tiny metal clusters is different from that of large iron crystallites, suggesting an electronic interaction between the support and metal.« less
  • Catalysts prepared by impregnating or ion-exchanging a CaY zeolite with a nickel nitrate solution to 5.19 and 5.78Vertical Bar3< by wt Ni, respectively, were reduced in flowing hydrogen at 450/sup 0/C for 6-24 hr. The metal surface area of the fresh catalysts, determined from hydrogen chemisorption, increased with increasing reduction time. For both impregnated and ion-exchanged Ni/CaY, maximum activities (calculated as the turnover numbers) for CO methanation determined in a fixed-bed differential reactor at 250/sup 0/-350/sup 0/C and 3.1:1 H/sub 2//CO ratio occurred at an average nickel crystallite size of approx. 14 nm, measured from X-ray diffraction line broadening. Atmore » this optimum crystallite size, which corresponded to a reduction time of 18 hr, the impregnated Ni/CaY catalyst was approx. 30Vertical Bar3< more active than the ion-exchanged catalyst, but a 5.75Vertical Bar3< Ni/g-Al/sub 2/O/sub 3/ catalyst prepared by impregnation was more active than either of the zeolite-supported catalysts.« less
  • Reduced iron added at 14.3% by wt to a 1:2 coal/solvent (light recycle oil) slurry in coal liquefaction experiments with Kentucky bituminous coal carried out in a stirred (1000 rpm) autoclave at 410/sup 0/C and 2000 psig hydrogen was about as efficient a desulfurization agent as commercial Co-Mo-Al catalyst (Comox 451), by reacting directly with hydrogen sulfide. It increased the yields of the oil fraction and pyridine soluble products, because of the catalytic activity of the formed iron sulfides and in contrast to the more hydrogenation-selective Co-Mo-al, did not increase hydrogen consumption. SRC mineral residue from the filter cake ofmore » the Wilsonville SRC pilot plant was ineffective in hydrodesulfurization and increased hydrogen consumption. Adequate liquefaction yields (90 to 91%) and superior desulfurization rates were achieved at 380/sup 0/C and 1000 psi hydrogen. Iron is thus the prime candidate as the additive for the SRC I process, to produce a solid, low-sulfur boiler fuel with minimum hydrogen consumption. In the SRC II process, where a more hydrogenated liquid product is desired, the recycle of SRC residue would be preferred.« less
  • The efficiency of the initial reactions of coal during coal liquefaction will have significant impacts on downstream processing (including catalyst usage, reaction severity, product yields, product quality) and hence on process economics. Reactions that result in compounds with low molecular weights and decreased boiling points are beneficial, whereas retrogressive reactions, which yield higher molecular weight compounds that are refractory to further processing, decrease process efficiency. Likewise, reactions that result in decreased sulfur, nitrogen, and oxygen contents and increased hydrogen contents in the products are beneficial. The use of unsupported fine-particle (<40 nm) catalysts during initial coal processing has the potentialmore » to enhance desired reactions and minimize retrogressive reactions. The potential advantages of using fine-particle size catalysts include improved dispersion of the catalyst, improved coal/catalyst contact, and the potential for using low amounts ([le]0.5% based on the weight of coal) of these novel catalysts due to their very high surface areas. These catalysts could be combined with the coal or coal-solvent mixture as either active catalysts or catalyst precursors that would be activated in situ. Several methods of combining catalyst and coal, such as physical mixing or using a catalyst-hydrogen donor slurry, are possible. Ideally the fine-particle catalysts would be inexpensive enough to be disposable.« less