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We earlier submitted a collection of three research reports, from Japan, which revealed detailed investigations into the upgrading of hydrocarbon liquids derived from coal, into products more akin to the liquid fuels were all familiar with; specifically, kerosene and gasoline.
The same sort of research has been underway much closer to home, but still not in Coal Country, though just as quietly, as the enclosed report, from Oklahoma State University, bears witness.
Comment follows:
"Catalysts for Upgrading Coal-Derived Liquids. Quarterly report, October-December, 1980.
Author: Crynes, B.L.
Report Number: DOE/ET/14876-T1; DOE Contract Number: AC22-79ET14876
Research Organization: Oklahoma State University, School of Chemical Engineering, Stillwater, OK
Abstract:
A linear relationship represents the hydrogenation activity decay of catalysts used in four experimental runs reported previously. The weight percent hydrogen in the reactor product oils plotted against oil-catalyst contact time for experimental runs ZBB, ZBC, ZBD, and ZBE reveals a linear decay rate of 0.0083 wt% hydrogen per hour. This is one quantitative measure of catalyst activity decay. The data for the plot incorporate three different catalysts or combinations used to process a PAMCO liquid at 1500 psig, 435C and LVHST of 2 hours. The data set covers run duration of up to 120 hours of oil-catalyst contact. An air driven hydrogen compressor was installed in the Catalyst Life Test Unit to reduce the costs associated with bottle hydrogen. Minor repairs were made on the oil feed pump. Five experimental runs were made with Shell 324 NiMo/Al catalyst using two feedstocks: (1) 40 wt% EDS/EDS raw solvent and (2) 30 wt% SRC-I creosote oil. The EDS feed oil proved to be rather easily hydrotreated as evidenced by 82 to 100% nitrogen removal, essentially complete desulfurization and no catalyst activity decay during 260 hours of continuous operation. Rapid coking resulted from the highly hydrogen deficient SRC/creosote mixture. The Shell 324 catalyst gave excellent hydrogenation of both liquids by increasing the hydrogen content of the product oils by about 3.8 wt%. This catalyst will be used in future studies; however, a new feedstock consisting of 30 wt% SRC-I/PAMCO process solvent will be assessed for use in catalyst decay mechanism studies."
First of all, this is just one "Quarterly report" for the US Department of Energy's Contract Number AC22-79ET14876: "Catalysts for Upgrading Coal-Derived Liquids". Where are the other quarterly reports? More importantly, where is the "Final Report"?
And: The research is, or was, being conducted in Oklahoma, where they might still have one or two little old scrape-and-shove surface mines that are active. In 1978, the most recent year we could find statistics for, Oklahoma produced about one tenth of one percent of our nation's coal. Might as well be in Japan. It's roughly the same as if the DOE had assigned a research project into the liquefaction of prairie grass, scrub brush and slaughter house renderings to West Virginia University.
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We submit these coal-to-liquid research selections, from Japan, only to support, and to illustrate the validity, of our thesis that coal-to-liquid conversion technologies are well-understood in many places throughout the world, and are undergoing continuous technical refinement and efficiency improvement.
We've edited the excerpts from the enclosed links to simplify, in as much as might be possible, the very technical jargon. What is presented should, again, just serve as added confirmation that coal can be converted into the liquid fuels and chemical raw materials we need. The question of why our abundant coal isn't yet being so utilized is one that needs answered.
The excerpts, with brief comment appended:
"Selective nuclear hydrogenation of naphthalene, anthracene and coal-derived oil over Ru supported on mixed oxide
Takeshi Kotanigawa, Mitsuyoshi Yamamoto and Tadashi Yoshida
Hokkaido National Industrial Research Institute, AIST, MITI Higashi-tsukisamu, Toyohira-ku, Sapporo 062, Japan
April 1997
Abstract:
The main objective of this paper is to investigate the possible ways to produce high-quality products for transportation fuels from heavy distillates. For this purpose (various weight percents of Ruthenium on Manganese, Zinc and Nickel Oxides) were used as catalysts for selective hydrogenation of napthalene, anthracene and Canadian Battle River coal-derived oil. The catalysts exhibited (various levels of activity). It was concluded that Ruthenium on non-acidic support showed the best performance.
Behavior of Hydrogen Transfer over Carbon-Supported Nickel Catalyst in Upgrading of Coal-Derived Liquid.
BINTANG B(Hniri) ZHANG Z-G(Hniri) NAGAISHI H(Hniri) YOSHIDA T(Hniri)
Nippon Kagakkai Hokkaido Shibu Kenkyu Happyokai Koen Yoshishu
Abstract
The focus of this study is to investigate the behavior of hydrogen transfer over active carbon and carbon-supported nickel catalysts in the hydrotreating of coal-derived oil. In this work, the effects of donor solvent and hydrogen gas on the hydrotreating of model compounds or coal oil were examined. (author abst.)"
Catalysts for Upgrading Coal-Derived Oils
Yoshimura, T. Sato, H. Shimada, N. Matsubayashi, A. Nishijima, T. Kameoka, H. Yanase, M. Watanabe, K. Masuda, Y. Kanda, and K. Ohsuka
J. Natl. Inst. Materials and Chem. Res., Vol.3, No.2, p.145, 1995
Abstract: Coal-derived oils were hydrotreated in two-stage catalytic processes or in single stage co-refining catalytic processes to produce high-quality oils. The former processes were much more flexible to control the quality of the final products such as gasoline and/or kerosene, depending on the reaction mode/severity of each state. In hydro-treating neat and low sulfur coal-derived oils, we developed a new type of (Nickel-Tungsten-Aluminum Oxide) hydro-treating catalyst for the first stage use, which catalyst had higher hydrogenation and "hydrodenitrogenation" activities and better activity maintenance than the conventional (Nickel-Molybdenum-Aluminum Oxide) catalysts. A new type of zeolite hydro-cracking catalyst, which showed high activity to convert (high temperature distillate) fraction with minimal gas make, was also developed for the second stage usage.In the latter co-refining process, where coal-derived oils were mixed with the proper fraction of petroleum oils and hydro-processed to get high-quality kerosene and/or diesel oils, (Ruthenium-Nickel-Molybdenum-Aluminum Oxide) catalysts were superior to (Nickel-Molybdenum-Aluminum Oxide) and (Nickel-Tungsten- Aluminum Oxide) catalysts. Spent Nickel-Tungsten and Nickel-Molybdenum catalysts were successfully cured by the oxidative regeneration under the low partial pressure of oxygen in the oxidizing gas and low oxidation temperature conditions."
First of all, the "heavy distillates" in the first abstract are intended to imply coal-derived oils. "Naphthalene" and "anthracene" are both constituents of crude coal "tar" or coal "oil", in the more traditional sense of those phrases.
Note, in the final abstract, mention of "processes (that) were (are) much more flexible to control the quality of the final products such as gasoline and/or kerosene"; and,. the "high activity" of a zeolite catalyst "to convert" products from "coal-derived oils" into "high-quality kerosene and/or diesel".
Zeolite catalysts, as we hope you'll recall, are at the heart of Exxon-Mobil's "MTG"(r) process which converts methanol to gasoline; methanol that's posited to be made from coal.
Again, the technical language might seem confusing, but the import is quite clear: We know how to convert coal into liquid hydrocarbon fuels.
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Following through on our assertions that the by-products of coal processing, specifically coal tars, can be beneficial additives for a coal-to-liquid fuel processor of appropriate design; and, that Big Oil knows all about the fact that coal can be efficiently converted into liquid petroleum substitutes, we present the enclosed report on liquefying coal, using a coal oil product, from Texaco.
As follows:
"Coal liquefaction using a hydrogenated creosote oil solvent: H-atom transfer from hydrogen donor components in the solvent
Erv J. Kuhlmann, Dick Y. Jung, Richard P. Guptill, Charles A. Dyke and Hyung K. Zang
Texaco Research Center, PO Box 509, Beacon, NY 12508, USA
Abstract
The presence of hydroaromatic, hydrogen donor components in a coal-derived solvent is one of the more important factors in the successful operation of a non-catalytic coal liquefaction process. Various hydrogen donor species present in a hydrogenated creosote oil have been identified. Their rate of disappearance under conditions that are consistent with a short residence time coal liquefaction process has been used to rank the reactivities of the various hydrogen donors. 1,2,3,10b-Tetrahydrofluoranthene was found to be an exceptional donor while 4,5-dihydropyrene, the hexahydropyrenes and 9,10-dihydrophenanthrene were found to be quite active. Sym.-octahydrophenanthrene and 2a,3,4,5-tetrahydroacenaphthene exhibited moderate activity. Tetralin and the four methyltetralin isomers were found to be unreactive under the coal liquefaction conditions employed."
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We offer this recent selection from a respected industry journal as more confirmation, not just of the fact that coal can be converted, on a practical basis, into liquid transportation fuels, but, that those coal-based fuels, as we have earlier documented, are, in some respects, better that the petroleum-based liquid fuels our transport system is currently based on.
The excerpt:
"Coal-Derived Fuel’s Advantages
Coal-derived liquid fuels are zero-sulfur paraffinic hydrocarbons that are similar to diesel. Because of its paraffinic nature, coal-derived diesel has a very high cetane number (about 75) compared to petroleum diesel (about 45). A high cetane number is necessary for efficient operation in diesel engines. The high paraffin content and low (less than 2% by volume) aromatic content also reduces particulate emissions. A test comparing coal-derived diesel with petroleum diesel on a 6.5-liter diesel engine for tactical vehicle applications showed that hydrocarbon emissions can be reduced by almost 50% compared to petroleum diesel. Carbon monoxide emissions were reduced by 50% and particulates by about 30%.
A potential approach to reducing CO2 emissions is to blend biomass with the coal feedstock. By doing so, the CO2 produced by the biomass fraction during production of the coal-derived fuel offsets the CO2 that was used up by the biomass during its growth phase by photosynthesis. Unfortunately, the logic cannot be extrapolated to a 100% biomass feed because of its low energy density and high moisture content (in comparison with coal) that leads to excessively high production and processing costs.
A recent study showed that by blending 15% to 30% biomass (by weight) with coal, the associated emissions can be 10% to 20% lower than the petroleum-derived fuel baseline.
In addition to environmental benefits, coal-derived liquid fuels have a high degree of thermal stability, which provides enhanced system performance for military aircraft. The DOD’s use of coal-derived liquid fuels could build public confidence and facilitate the introduction of such fuels into the private sector vehicle fleet."
We interrupt the excerpt so that we can emphasize the concluding paragraph:
"Overall, converting coal to liquid fuels is one element of an integrated approach that is needed to address fuel security. At least in the near term, it could bring a higher level of stability to world oil prices and to the global economy. Over the long term, it could serve as insurance for the U.S. (or any other oil-importing nation) against artificial or unwarranted price hikes from oil-producing countries."
It's difficult to state the benefits of coal conversion much better than that, except to offer the reminder that coal-to-liquid conversion technologies can be adapted to accept additional, renewable and CO2-recycling, biologically-based feed stocks, and be integrated with Sabatier-type processors for the direct capture and conversion of CO2 into even more hydrocarbon fuels and chemical manufacturing raw materials.
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Much has been made of "Tar Sand", or "Oil Sand", such as in Canada's massive and much-touted Athabasca deposit, as a resource that could help us overcome our liquid fuel shortfalls.
It could do that, but the public doesn't seem to understand, really, the true nature of such deposits and what the implications are of extraction and usage.
First, the "tar", in tar sands, is more appropriately referred to as "bitumen". It is a nearly-solid substance highly contaminated with inorganic, non-combustible waste which is directly analagous to the "ash" in coal.
It has been postulated, in fact, that tar sands are just organic deposits that got interrupted during the process of being turned into coal.
Nevertheless, tar sands do represent significant, exploitable deposits of organic material that can be employed to help us satisfy our liquid fuel needs.
What isn't too well-known, except in certain circles, is that coal, and especially some fuel-type liquids extracted from coal, are very beneficial agents needed to "upgrade" tar sand bitumen so that it can be further refined into a liquid petroleum substitutes.
The enclosed report, from Japan, is just one of many available attesting to the enhancement of oil sand refining attained through the employment of coal or, better, as explained following the excerpt, liquids derived from coal, in the processing of tar or oil sand bitumen.
As follows:
"Document title
Addition effects of coal-derived oil and coal on upgrading of oil sand bitumenAuthors
YOSHIDA T. ; NAGAISHI H. ; SASAKI M. ; YAMAMOTO M. ; KOTANIGAWA T. ; SASAKI A. ; IDOGAWA K. ; FUKUDA T. ; YOSHIDA R. ; MAEKAWA Y. ;Authors Affiliation
Hokkaido national industrial res. inst., MITI, Toyohira, Sapporo 062, JAPONAbstract
The mechanism of synergistic interaction between bitumen and coal in coprocessing was investigated in conjunction with hydrogen transfer between them. Two types of reaction systems were used in this work: the upgrading of bitumen and coal-derived oil, and the coprocessing of bitumen with either coal-derived oil or coal. Considerable retrogressive reaction was observed in the upgrading of bitumen alone at 450 °C but was effectively suppressed by the addition of either coal-derived oil or coal. These results strongly suggest that both coal-derived oil and coal act as good hydrogen donors or shuttlers in the coprocessing. Furthermore, their addition resulted in more production of light oil from bitumen. The conversion of coal into toluene solubles was influenced by the concentration of coal itself in the slurry feed, but the formation of distillable oil from coal seemed to be negligibly small."There is, obviously, much not fully-explained in the Abstract. But, "coal-derived oil" "suppressed" retrograde reaction of the oil sand bitumen. The implications are that coal-derived liquids are preferable to the use of coal itself, since, in the tar sand bitumen upgrading process, "the formation of distillable oil from coal (itself) seemed to be negligibly small". But, already-synthesized "coal-derived oil" acts as a "good hydrogen" donor for the tar sand bitumen, with resultant synergies for both.
It is noted that raw coal was not appreciably transformed into "distillable oil" during the bitumen processing; but, liquids derived from coal and tar sand bitumen can be co-processed together more efficiently, than the bitumen can be alone, into liquid fuel raw materials.
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