WV Coal Member Meeting 2024 1240x200 1 1

US Guv Refines Coal Liquids

This submission is lengthy and complex, and, sadly, incomplete; incomplete because a key research report file maintained by our Federal Government discloses itself to be damaged, and electronically unavailable.
 
Explanation follows multiple links and excerpts, with comment interspersed.
 
We present, first, a report of research from New Mexico State University, which starts us out on a path of discovery revealing that, not only does our Federal, US, Government know that coal can be converted, on a practical and profitable basis, into liquid fuels, but it has also been devoting considerable effort into refining the technology for refining those coal liquids, again on a practical and profitable basis, into direct replacements for the liquid fuels currently used by our transportation fleet and serviced by our transportation infrastructure. 
 
Note that the frequently-applied term "hydrotreating" relates to the chemical process of adding Hydrogen to the highly carbonaceous molecules of raw coal liquids, to convert them into something more akin to gasoline, diesel, and etc., the "hydrocarbon" liquids we're all familiar with.
 
As follows: 
 
 
"Title: Hydrotreating of Coal Liquids, Phase 2
 
Authors: Wilson, D.B.; Bogdanor, J.M.
 
Affiliation: New Mexico State University, Las Cruces, NM
 
Publication: Final Report; NMSU Department of Mechanical Engineering; June 1982.
 
Abstract:
 
The kinetic parameters for the pseudo first-order denitrogenation and desulfurization of an SASOL coal naphtha was studied. Only the fraction boiling over 95 C (at 25.8 mmHg) was hydrotreated due to the high volatility of the whole naphtha. Dodecane was used as a diluent to further reduce the volatility of the hydrotreated naphtha bottoms. A commercial Ni-Mo catalyst (HDS9A) was employed. Based on chromatographic results, nitrogen and sulfur were successfully removed from the naphtha bottoms. The mathematical model developed to describe the pseudo first-order denitrogenation and desulfurization of the naphtha bottoms in the semi-batch, slurry reactor was adequate to explain the experimental results."
 
First of all, these New Mexico researchers, in 1982, were working to refine a coal liquid produced by Sasol, in South Africa.
 
South Africa was already fueling her transportation fleet with liquid fuel made from coal in 1982, and had been for quite some time.
 
Couldn't we have just asked them how they refined it?
 
And, this is the "Final Report" of "Phase 2". Where is the report of "Phase 1"? And, how many "Phases" were there?
 
We follow up with a report from our own Federal Government, who also, in one of their research facilities suspiciously close to New Mexico State University, was, coincidentally, looking into the "Hydrotreating", the upgrading, of coal liquids. There are some genuinely significant references in this report, and we'll elaborate a few of them, throughout and following the lengthy, but we think justified, excerpt:
 
 
"HYDROTREATING OF COAL-DERIVED LIQUIDS
 
Frances V. Stohl. Stephen E. Lon. Kathleen V. Diegert.
David C. Goodnow, John 8. Oelfke
Sandia National Laboratories
Process Research Department 8212
Sandia National Laboratories
P.O. Box 5800
Albuquerque, NM 87185-0709
 
ABSTRACT
 
The objective of Sandia's refining of coal-derived liquids project is to determine the relationship between
hydrotreating conditions and product characteristics. The coal derived liquids used in this work were
produced in HTI's first proof-of-concept run using Illinois #6 coal. Samples of the whole coal liquid
product, distillate fractions of this liquid, and Criterion HDN-60 catalyst were obtained from Southwest
Research Inc. Hydrotreating experiments were performed using a continuous operation, unattended,
microflow reactor system. A factorial experimental design with three variables (temperature (310% to
388OC), liquid hourly space velocity (1 to 3 g/h/cm'(cat)), pressure (500 to 1000 psig H2)) is being used in
this project. Sulfur and nitrogen contents of the hydrotreated products were monitored during the
hydrotreating experiments to ensure that activity was lined out at each set of reaction conditions. Results
of hydrotreating the whole coal liquid showed that nitrogen values in the products ranged from 549 ppm
at 320°C, 3 g/h/cm'(cat), 500 psig H2 to 45 ppm at 4OO0C. 1 glhl cm'(cat). 1000 psig H2.
 
(So, in a fashion similar to other suspicion-arousing Guv research into coal liquefaction, they saw fit to ship coal products, "Illinois #6 Coal", a few thousand miles to New Mexico for coal liquefaction research. We suppose the researchers at Southern Illinois University, who, as we've thoroughly documented, have been developing and refining coal liquefaction technologies, would be "amused", for want of a better term, to learn of it. We've no idea, yet, what "Criterion HDN-60 catalyst" might be, or who "Southwest Research Inc" are, but will try to find out. - JtM)
 
INTRODUCTION
 
DOWPETC's refining of coal liquids program is aimed at determining the most cost effective
combination of existing refinery processes and blending options necessary to upgrade direct and indirect
coal liquids into transportation fuels that meet year 2000 specifications. A main reason for this program
is that coal liquefaction processing has improved significantly since the last refining evaluation was done
by Sullivan and Frumkin (1) at Chevron in the early 1980s. In addition. a recent publication by Zhou.
Marano and Winschel (2) indicates that blending coal liquids with petroleum may allow refiners to
produce specification products with less refining than if each fraction was processed separately.
Sandia's role in this program is to develop a database relating hydrotreating parameters to feed and
product quality by experimentally evaluating options for hydrotreating whole coal liquids, distillate cuts of
coal liquids, petroleum, and blends of coal liquids with petroleum. Sandia's project is unique because our
small-scale, continuous operation flow reactor system enables us to evaluate many hydrotreating options
in a cost effective manner while keeping waste production to a minimum. Sandia's project is integrated
with other program participants including participants in the Refining and End-Use of Coal Liquids Study
project (Bechtel, Southwest Research Inc. (SwRI). Amoco. M. W. Kellogg). Hydrocarbon Technology Inc.
(HTI, formerly HRI) the MITRE Corporation, and PETC. Sandia's data will be used by other program
participants in refinery linear programming models to identify the most cost effective options for
introducing and processing coal liquids in a refinery. This paper will cover results obtained from
hydrotreating whole coal liquid product from HTl's first proof of concept run with Illinois #6 coal."
 
(We have documented "HTI" - Hydrocarbon Technologies - previously; but, who is "DOWPETC"?
 
And, note: "coal liquefaction processing has improved significantly since the last refining evaluation was done by Sullivan and Frumkin at Chevron in the early 1980s".
 
Did anyone know that Chevron was refining coal liquids in the "early 1980's"? Who was improving "coal liquefaction processing", and, where are the results, what were the improvements?  
 
Who is the "MITRE Corporation", and what is their connection to coal liquefaction? Who is Southwest Research?
 
We'll try to find out for you. We all know one of their above-documented partners: "Amoco". - JtM)
 
"EXPERIMENTAL PROCEDURES
 
Sandia's experimental procedures included using a factorial experimental design, hydrotreating the
whole coal-derived liquid, characterizing the feeds and hydrotreated products, and reporting results to
other program participants.
 
Continuous Operation Reactor Svstem: Sandia's hydrotreating studies are being performed using a
continuous operation, trickle-bed, microflow reactor system. The system has all required safety features
to enable it to be operated unattended. The capabilities of this reactor system include catalyst loadings
upto 25 cm', liquid flow rates from 0.05 to 4 cm'lmin. gas flows for hydrogen and nitrogen up to 2 Ilmin,
gas flows for H2S/H2 up to 0.5 Vmin. maximum temperature of 620°C, and a maximum pressure of 1800
psig. The reactor volume is 59 cm'. Four samples can be collected automatically during unattended
operation. For liquid hourly space velocities (LHSV) of 1 and 3 g/h/cm3(cat). samples would weigh about
7 and 22 g respectively.
 
Factorial ExDerimental Desian ("Factorial Experimental Design"??? - JtM): Based on experience, three parameters were chosen for the factorial experimental design (Figure 1): temperature, pressure, and LHSV. The ranges of hydrotreatingconditions used with the design were temperatures of 310 to 388%. pressures of 500 to 1000 psig HI, and LHSVs from 1 to 3 g/hlcm'(cat). Evaluation of the first set of hydrotreating conditions (388'C, 500 psig H2, 1g/h/cm'(cat)) was repeated once during the run and once at the end of the run so lhat effects of Catalyst deactivation could be determined. Prior to the use of the testing using the factorial experimental design, two additional sets of reaction conditions were evaluated to see the effects of high pressure and temperature: 388'C, 1500 psig HI, 1 g/h/cm3(cat) and 362OC.1500 psig H2, 1 g/h/cm3(cat).
 
Reactor Feeds and Catalvst: Sandia received (from SwRI) a sample of fresh Criterion HDNBO catalyst
end about 3.5 gallons of whole coal liquid product that was produced in HTl's first proof-of-concept run
using Illinois #6 coal. The whole coal liquid product was collected when HTl's third stage reactor was not
on line and while catalyst replacement was being used. Sandia's reactor was loaded with log of fresh
catalyst that was sulfided in situ using temperature staging. The presulfiding procedure consisted of
heating the catalyst to 177% under He. starting the flow of a 10 mol% H2S/H2 mixture and maintaining
17PC for 1 hour. The catalyst was then heated to 288°C under flowing H2W2 and maintained at 286%
for 1 hour. Ned the catalyst was heated to 4MoC under flowing HzS, the temperature was maintained at
404% for 1 hour. HzS flow was stopped and HI flow started.
 
TEMPERATURE
 
Analytical Procedures: Small samples were collected either manually or automatically throughout the
run. Nitrogen and sulfur analyses were used lo determine when line out was achieved at each reaction
condition. These analyses were performed using an Antek 7000 Sulfur 8 Nitrogen Analyzer with an
automatic sampler. Standards were prepared using phenanthridine for nitrogen, thianthrene for sulfur,
toluene for the solvent. and four lo five dilutions. Standards were measured at least twice and a
polynomialfit of the intensity versus concentration data was used for analysis of unknowns.
 
RESULTS AND DISCUSSION
 
Analyses of the whole coal liquid by HTI, SwRI, and Sandia are shown in Table 1. SwRl used their
measured specific gravity. Sandia used 0.9 glml for the first and second samples. Data for the second
sample was also calculated using SwRl's specific gravity to show the effect of different values. Results
show some variability but indicate the whole coal liquid has about 600 ppm nitrogen and 400 ppm sulfur."
 
(We have deleted from the excerpt numerous Figure references, and etc., covering multiple pages. - JtM)
 
"CONCLUSIONS AND FUTURE WORK
 
Results of this work show that good denitrogenation and good desulfurization can be obtained under
relatively mild conditions with coal liquids from current processes. AI the lowest severity condition. there
is only about 10% nitrogen removal, whereas at the highest severity condition, there is about 97%
nitrogen removal. Sulfur removal is good over the whole range of conditions and is greater than 95%.
Ongoing and future work will involve additional characterization of reaction products by techniques such
as distillation. PONA or PIONA analyses. density determinations, and proton NMR for hydrogen
distributions. Results will be corrected for catalyst deactivation and analyzed statistically to determine
the effects of process conditions on product quality. Future hydrotreating experiments will be performed
with distillate fractions of this coal liquid and with coal-derived liquids from subbituminous mI."
 
A complete report on all of all this effort just might, but only might, be available in hard copy form.
 
No guarantees, but we think the following link(s), with excerpted info, will get you to it:
 
 
You are accessing a document from the Department of Energy's (DOE) Information Bridge: DOE Scientific and Technical Information. This site is a product of DOE's Office of Scientific and Technical Information (OSTI) and is provided as a public service. Visit OSTI to utilize additional information resources in energy science and technology.

A microfiche or paper copy of this document is also available for sale to the public from the National Technical Information Service, Springfield, VA at www.ntis.gov. "
 
Our indigent circumstances prevent us from ordering a "paper copy", as much as we might like to have one. But, we think every US citizen in US Coal Country should have a paper copy of it, or at least a newspaper copy of the synopsis.
 
When we attempted to download this artifact, via a "View Document" link, we were informed, after a very lengthy wait, that the file was "damaged" and "unavailable". Perhaps you'll have better luck, but we doubt it.
 
We don't know how much more information it might contain, or how it might differ from, the "Hydrotreating" report from Sandia we referenced, above; but, It long ago became obvious to us that much coal-to-liquid research, much of the truth of it, is "unavailable".
 
Why that is the case should be pretty obvious to everyone by now, we think. The situation needs to be changed.
 
All of it should be available to everyone, especially everyone in US Coal Country.