International Journal of Coal Geology 263 (2022) 104120

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International Journal of Coal Geology

journal homepage: www.elsevier.com/locate/coal

Invited Review Article

Understanding coal quality and the critical importance of comprehensive

coal analyses
James C. Hower a, b, *, Robert B. Finkelman c, Cortland F. Eble d, Barbara J. Arnold e
a
University of Kentucky, Center for Applied Energy Research, 2540 Research Park Drive, Lexington, KY 40511, USA
b
University of Kentucky, Department of Earth & Environmental Sciences, Lexington, KY 40506, USA
c
Geosciences Department, University of Texas at Dallas, Richardson, TX 75080, USA
d
University of Kentucky, Kentucky Geological Survey, Lexington, KY 40506, USA
e
Professor of Practice in Mining Engineering, The Pennsylvania State University, University Park, PA 16802, USA

A R T I C L E I N F O A B S T R A C T

Keywords: Coal is a remarkably complex combination of macerals and minerals and inorganic elements in organic associ­
Trace elements ations plus liquids, gases, and semi-solid organics, all overprinted by coal metamorphism. The proper charac­
Coal petrology terization of coal is necessary for academic research on coal origins and utilization and for the current and future
Minerals
industrial utilization of coal and coal by-products. A coal analysis scheme must be comprehensive because no one
Coal rank
Coal beneficiation
petrographic or chemical analysis stands alone. Coal rank, for example, can be expressed as vitrinite reflectance,
Coal utilization a petrographic parameter, or by a number of chemical parameters, such as heating value or carbon content. No
one parameter is reliable from lignite to meta-anthracite and, even at a single rank level, variations due to the
maceral content and aspects of the organic chemistry imply that a view of more than one parameter is necessary
to determine the coal rank.

1. Introduction Pennsylvania.2 Based on the chronology laid out by Van Krevelen

“To those that had the eyes to see, it has been obvious for a long time that
worthwhile coal research demands study of a large base of well characterized
coal samples.” (Given, 1984).
While the use of coal as a fuel is declining in many parts of the world,
its use remains as a reliable and often necessary source of energy and as
the feedstock for metallurgical and anode coke. Further, along with a
broader range of sources (Dutrow, 2022), interest has grown in the
utilization of coal and coal byproducts as a source of critical elements
and materials and for chemical feedstocks (Mullen, 2022). The proper
characterization of coal has always been a pressing but complex task.
Both organic and inorganic portions of the coal must be considered and
the complexity of rank-related changes in coal means that specific an­
alyses may not work equally well throughout the rank spectrum.
Certain analytical tests are rooted deep in the history of coal science;
for example, Matthew Carey Lea (1841)1 used proximate analyses to
assess coal metamorphism in the Southern Anthracite Field,
(1982), this was shortly after (by his consideration) the birth of coal
science in 1831 and the earliest chemical investigations of coal by
Regnault (1837). Other analyses are the result of more recent in­
novations; for example, 1983 marked the commercial introduction of
the now widely used inductively coupled plasma mass spectroscopy
(ICP-MS) (Yost, 2021). Within any one long-established database, it is
likely that successive techniques were used to produce the results;
therefore, older analyses may be less precise than desired. For example,
the analytical methods employed by The Pennsylvania State University
in the early years of their characterization efforts (Direct Current (DC)
Arc Emission Spectroscopy (installed in 1951; Harold Lovell personal
communication to Hower, 1976) (details of the technique in Grimes and
Marranzino (1968) and Suhr and Gong (1977)) were not as precise as
modern methods, so the rare earth elements (REE), aside from La and Ce,
were not detected. The U.S. Geological Survey’s National Coal Quality
Inventory experienced a similar evolution of analytical methods (Bragg
et al., 1998).

* Corresponding author at: University of Kentucky, Center for Applied Energy Research, 2540 Research Park Drive, Lexington, KY 40511, USA.
E-mail addresses: james.hower@uky.edu (J.C. Hower), bobf@utdallas.edu (R.B. Finkelman), eble@uky.edu (C.F. Eble), bja4@psu.edu (B.J. Arnold).
1
Although Taylor (1840a, 1840b), as contractor for Isaac Lea’s coal company, published the data first, Matthew Carey Lea, Isaac Lea’s son, was the originator of
the data. He submitted his paper the same year as Taylor’s published consulting reports. Lea was 17 years’ old at the time of the submission of the paper.
2
More than 180 years later, his analyses are still the results of record for the western part of the Southern Anthracite Field.

https://doi.org/10.1016/j.coal.2022.104120
Received 29 August 2022; Received in revised form 7 October 2022; Accepted 8 October 2022
Available online 19 October 2022
0166-5162/© 2022 Elsevier B.V. All rights reserved.
J.C. Hower et al.
1.1. Basic principles of coal composition
Coal is a remarkably complex (primarily) biologic rock. Coal is a
function of three fundamental aspects, each a reflection of the origin and
diagenesis/metamorphism of the coal: organic petrological and
geochemical parameters, inorganic petrological and geochemical pa­
rameters, and coal rank. In simple terms, coal is the product of macerals,
minerals, and the degree of metamorphism (O’Keefe et al., 2013).
Ideally, each corner of the compositional triangle should be independent
of the others, with (1) the organic constituents, both the macerals and
the non-maceral organics; (2) the mineral matter, minerals, sulfur,
major oxides, and minor and trace elements; and (3) vitrinite reflectance
as an indicator of coal rank occupying the nodes. In practice, many of the
most important parameters in routine coal utilization, meaning the coal-
fired power industry and the manufacture of metallurgical coke, are a
function of a combination of the fundamental analytical parameters,
including:
• Hardgrove grindability index (HGI) - particularly important in
gauging a coal’s behavior in fines generation in coal preparation and
pre-combustion pulverization, is most directly related to the mac­
erals and the maceral group (microlithotype) composition, but also
dependent on rank and minerals (Hower, 1998; Hower et al., 2021a);
• Sulfur dioxide emissions - an expression of the amount of sulfur on
the basis of the heating value (kg SO2/GJ or lb. SO2/106 Btu);
• Heating (calorific) value - a “rank” parameter of fundamental
importance in coal purchases that is dependent on the maceral and
mineral composition as well as being a function of the coal
metamorphism.
As stated, coal is the product of all three fundamental parameters:
the maceral composition was determined in part by the original plant
material which was modified by the same environmental factors that
influenced the mineral and non-mineral (organically bound) trace metal
content of the coal, the rank was enhanced by lithostatic pressure and
the mineralizing fluids passing through the coal, and the functional
groups in peats and low-rank coals served to chelate minor elements.
The maceral composition is also a function of time and provenance, the
“fourth axis” of the compositional “triangle.” Simply stated, while in­
dividual macerals, for example, vitrinite, may carry the same name
through the ages of coal, a Pennsylvanian vitrinite originated from a
distinctly different plant than did an Eocene vitrinite (Jones et al., 1984;
Hower et al., 2007a, 2007b; Mastalerz et al., 2021). Similarly, caution
must be exercised in making iso-rank comparisons between macerals
from different regions (e.g., Permian coals of China and Mongolia vs. the
Northern Appalachian coalfield’s Dunkard Basin vs. the Gondwana
continents). The discussions by O’Keefe et al. (2013), Dai et al. (2020a,
2020b, 2021), and Hower et al. (2021b) concerning maceral origins,
coal geochemistry, and the interplay of coal metamorphism with both
macerals and geochemistry are thorough and will not be repeated here
but are useful in understanding the evolution of coal properties.
1.2. Implications for coal utilization
As noted above, coals of different ages, climates, and tectonic plates
can have distinctly different maceral distributions, ash yields, and other
properties. Yet, with an expansive export-import market, those coals can
end up in the same boilers or coke ovens. For example, Permian Gond­
wana coals from Queensland (Argus Media, 2022) and Tanzania
(Jumbe, 2022) were shipped to Poland and The Netherlands, respec­
tively, in the second quarter of 2022; Colombian coal reaches many
destinations in the Middle East, Europe, South America, and North
America (Statista, 2021); and the U.S.A. imported 1.32 Mt. (short) coal
from Colombia, Canada, Indonesia, China, France (offsetting lost im­
ports from Russia), and Mexico and exported 20.186 Mt. (short) coal to
more than 37 countries in the first quarter of 2022 (U.S. Energy
2
International Journal of Coal Geology 263 (2022) 104120
Information Administration, 2022). Coal can even be imported to power
plants within active coalfields, as demonstrated by the 2002 delivery of
Polish coal to power plants in the Western Kentucky coalfield (Stamper,
2002). At the time of this writing, coal is not cheap due to disruptions in
energy supplies.
Considering both coal origins and coal prices, the importance of
thorough coal testing is underscored. As a hypothetical example, equal-
rank bituminous coals from Tanzania and the United States imported
into The Netherlands,3 for example, could have markedly different
pulverization, combustibility, and ash fusion properties. The co-
pulverization and co-firing of both in a power plant could lead to
unanticipated problems if the individual nature of each coal and the
synergy of both coals was not fully understood. Protecting and under­
standing your investment with a comprehensive coal analysis makes
sense anytime, but particularly in the light of volatile coal markets.
1.3. Know your coal
“Know your coal” was the title of Peters et al.’s (1962) paper. The
path to knowing your coal is the management and understanding of the
chemical, mineralogic, and petrographic analyses. Our objective in this
essay is to emphasize the importance of the proper and thorough anal­
ysis of coal, both for the tasks at hand but also for the long view of their
utilization for applications not yet anticipated. These analyses are
important for the utilization of coal as well as for coal preparation, or
coal cleaning, as we strive to meet new challenges for mineral or element
recovery or rejection prior to utilization. As a means of reinforcing the
needs for coal analysis, we will examine case studies of macerals, min­
erals and the elements, and metamorphism. Throughout the discussion,
we keep an eye on the synergy between the analyses, the coal properties
they represent, and the consequent preparation and utilization of the
coal. Coal analyses are the foundation of coal science; without proper
analyses, the science cannot stand and without coal science there can be
unfortunate and costly consequences.
2. Show your work
2.1. Standards for analysis
No, not “show your work” in the sense of detailing all of the steps of a
proof in a mathematics test, but “show your work” in the sense of
providing the details of your experiment. This includes references to
national and/or international standard methods (Table 1 lists the ASTM
methods; also see Riley (2014)) and other publications such as the
modifications of petrographic nomenclature (International Committee
for Coal and Organic Petrology (ICCP), 1998, 2001; Sýkorová et al.,
2005; Pickel et al., 2017) and the discussions of lanthanide (Zygarlicke
et al., 2019) and other minor and trace element analytical procedures.
Include the certified standard materials used for instrument calibration
and for comparative purposes; the type of equipment used; a discussion
of any modifications or special procedures not included among the latter
details; and, just as important, the actual data. “Data” imply more than
just the numbers plotted on a graph. Data needs to be in an accessible
reference, an in-text table, or in an appendix or supplementary file that
can truly be used to not only test your hypothesis with existing or yet to
be developed techniques but also to provide the resources for the data
miners who are interested in, for example, the copper content of the coal
and not just the lanthanides emphasized in your study. Some of the most
highly cited publications in coal science, such as Ketris and Yudovich
(2009), were excavated from the foundations of numerous chemical
studies.
3
The Netherlands is the leading destination for U.S. coals (1st quarter sta­
tistics for 2022 suggest an annual rate exceeding 8 million metric tons) (U.S.
Energy Information Administration, 2022).
J.C. Hower et al.
Table 1
ASTM International standard methods for coal sampling and analysis. All should
be cited as “ASTM International” with the number immediately following the
designation indicating the year of original adoption or, in the case of revision,
the year of last revision and number in parentheses indicates the year of last
reapproval. For example, either “19” or “2019” indicates that the citation should
be to the year 2019. “e1” indicates an editorial change since the last revision or
reapproval. These are the short titles for the standards; the complete citations
are in the References.
ASTM International Method
ASTM International D167/
D167M-21a, 2021
ASTM International D197-19,
2019
ASTM International D291/
D291M-20, 2020
ASTM International D293/
D293M-18, 2018
ASTM International D388-19a,
2019
ASTM International D409/
D409M-16, 2016
ASTM International D440-07,
2019
ASTM International D441-07,
2019
ASTM International D720/
D720M-15, 2015
ASTM International D1412/
D1412M-20, 2020
ASTM International D1756-02,
2002
ASTM International D1757-03,
2003
ASTM International D1857/
D1857M-18, 2018
ASTM International D2361-02
(withdrawn 2008), 2008
ASTM International D2492-
02R12, 2012
ASTM International D2639/
D2639M Rev. 21A, 2021
ASTM International D2799-21,
2021
ASTM International D2961/
D2961M-19, 2019
ASTM International D3038/
D3038-93, 2018
ASTM International D3172-13,
2021
ASTM International D3173/
D3173M-17a, 2017
ASTM International D3174-12,
2012
ASTM International D3175-20,
2020
ASTM International D3176-15,
2015
ASTM International D3177-02
(2007), 2002
ASTM International D3178-89,
1989
ASTM International D3179-02,
2002
ASTM International D3302/
D3302M-15, 2015
ASTM International D3402/
D3402M-16, 2016
ASTM International D3682-13,
2013
ASTM International D3683-11,
2011
ASTM International D3684-01,
2006
ASTM International D3761-10,
2010
Analysis
Apparent and True Specific Gravity and Porosity
of Lump Coke
Sampling and Fineness Test for Pulverized Coal
Cubic Feet Weight of Crushed Bituminous Coal
Sieve Analysis of Coke
Standard classification of coals by rank
Grindability of Coal by Hardgrove Machine
Drop Shatter Test for Coal
Tumbler Test for Coal
Free Swelling Index of Coal
Equilibrium Moisture of Coal
Carbonate Carbon in Coal
Sulfate Sulfur in Ash from Coal and Coke Ash
Fusibility of Coal and Coke Ash
Chlorine in Coal
Forms of Sulfur in Coal
Plastic Properties of Coal
Microscopical Determination of Maceral
Composition of Coal
Total Moisture in Coal
Drop Shatter Test for Coke
Proximate Analysis of Coal and Coke
Moisture in Coal and Coke
Ash from Coal and Coke from Coal
Volatile Matter in Coal and Coke
Ultimate Analysis of Coal and Coke
Total Sulfur in Coal and Coke
Carbon and Hydrogen in Coal and Coke
Nitrogen in Coal and Coke
Total Moisture in Coal
Tumbler Test for Coke
Major and Minor Elements in Combustion
Residues from Coal Utilization Processes
Trace Elements in Coal and Coke Ash by AAS
Total Mercury in Coal by Oxygen Combustion
and Atomic Absorption Method
Total Fluorine in Coal by Oxygen Combustion
and Ion Selective Electrode Method
3
International Journal of Coal Geology 263 (2022) 104120
Table 1 (continued )
ASTM International Method Analysis
ASTM International D4208-19, Total Chlorine in Coal by Oxygen Combustion
2019 and Ion Selective Electrode Method
ASTM International D4239-17, Sulfur in Coal and Coke using High Temperature
2017 Tube Furnace Combustion
ASTM International D4326-21, Major and Minor Elements in Coal and Coke Ash
2021 by X-Ray Fluorescence
ASTM International D4371/ Washability Characteristics of Coal
D4371M-06, 2019
ASTM International D4606-15, Arsenic and Selenium in Coal by Hydride
2015 Generation Atomic Absorption Method
ASTM International D4749/ Sieve Analysis of Coal
D4749M-87, 2019
ASTM International D5016-16, Sulfur in Ash from Coal, Coke and Residues from
2016 Coal Combustion
ASTM International D5061-19, Microscopical Determination of Textural
2019 Components of Metallurgical Coke
ASTM International D5114/ Froth Floatation of Coal in a Mechanical Cell
D5114M-90, 2018
ASTM International D5142-09, Proximate Analysis of Coal and Coke by
2009 Instrumental Procedures
ASTM International D5341/ CRI and CSR of Coke
D5341M-14, 2014
ASTM International D5373-14, Instrumental Determination of Carbon-
2014 Hydrogen-Nitrogen in Coal and Coke
ASTM International D5515-21, Swelling Properties of Bituminous Coal Using a
2021 Dilatometer
ASTM International D5865-19, Gross Calorific Value of Coal and Coke
2019
ASTM International D5987-96, Total Fluorine in Coal and Coke
1996)
ASTM International D6172/ Volume of Bulk Material Using Contour and
D6172M-18, 2018 Cross-Section Procedure
ASTM International D6316-17, Total Combustible and Carbonate Carbon in Solid
2017 Residues from Coal and Coke
ASTM International D6347/ Bulk Density of Coal
D6347M-05, 2005
ASTM International D6349-21, Major and Minor Elements in Coal, Coke and
2021 Solid Residues from Combustion of Coal and
Coke by ICPAES
ASTM International D6357-19, Trace Elements in Coal, Coke, and Combustion
2019 Residues from Coal Utilization Processes by ICP-
AES, ICP-MS and GF-AAS
ASTM International D6414-14, Total Mercury in Coal and Coke Combustion
2014 Residues by Acid Extraction or Wet Oxidation
and CV-AAS
ASTM International D6721-01 Chlorine in Coal by Oxidative Hydrolysis
(2015), 2015 Microcoulometry
ASTM International D6722-11, Total Mercury in Coal and Coal Combustion
2011 Residues by Direct Combustion Analysis
ASTM International D7348-21, Loss on Ignition of Solid Combustion Residues
2021
ASTM International D8247-19, Total Fluorine and Total Chlorine in Coal
2019
2.2. Pitfalls of analysis
Publishing data that are not valid or that cannot be tested or repro­
duced is a waste of everyone’s time and can promulgate mistakes. Un­
intentional mistakes, improper standards, transcription errors,
typesetting errors, contaminated samples, etc., are all regrettable but
non-intentional errors. The deliberate publication of fabricated and/or
falsified data is a different problem; it should not happen and, when
identified, it should not be allowed to remain in the published literature4
4
At least, the error should be acknowledged. It is understood that the users of
the data are often distinct from the originator, thus they might not be aware of
the problems with the data. In that respect, while the falsified information can
be removed from the original electronic source or corrected in printed errata,
the data can live on in downloaded and printed copies.
J.C. Hower et al.
or in the on-line tabulations.5 The use of “qualified” data (for example,
values reported as below the detection limit) is another limitation on
data use. Data for elements having more than 25% qualified values
(including Au, the Pt-group metals, and the heavy REE) should not be
used for comparison purposes (statistical or otherwise) without
acknowledgement of the limitations and elements with 10 to 25%
qualified values (including ash fusion temperatures, forms of sulfur, and
certain of the REE) should be used with extreme caution for statistical
comparison purposes (Bragg et al., 1998).
Along with valid data, a proper geographic and stratigraphic location
of a sample is important. As an exception, though, the feed coal to a
power plant could come from multiple coal seams in multiple mines, so
this is not a universally applicable rule. Other than that example, in most
cases locations can be obtained from mine surveys6 or from GPS
readings.
2.3. Basis of reporting analyses
One of the most important aspects of “showing your work” revolves
around the basis of reporting — the moisture basis. For example, the
ASTM rank classification in Table 2 indicates analyses on dry mineral-
matter free and moist mineral matter free bases. Contracts for the sale
of coal are written on different moisture bases: dry, as-received, etc. A
moisture content must accompany analyses that are reported on any­
thing other than a “dry” basis.
Total moisture is analyzed as part of the proximate analysis, an
ASTM procedure calling for a sample to be subjected to a specific tem­
perature for a specific amount of time, to meet contractual obligations.
Total moisture is a combination of inherent moisture and surface
moisture, specifically the free moisture on the surface of coal. Surface
moisture can change rapidly through air drying or exposure to moisture.
Inherent moisture decreases with increasing coal rank and is measured
after holding a coal sample at a specified temperature and relative hu­
midity for a given time. Lignites can contain 30% or more inherent
moisture, subbituminous coals about 25%, lower rank bituminous coals
about 10% inherent moisture, and high rank bituminous coals and an­
thracites about 1–2% inherent moisture.
Coal cleaning technologies are, for the most part, water or media
based. The coal gets wet; the water needs to be removed and reused in
the preparation plant. Coal dewatering technologies, an inherent part of
beneficiation, remove the surface moisture based on dewatering forces,
such as vacuum, gravity, centrifugal forces, pressure, etc. The size and
specific gravity distributions of the coal (or refuse) to be dewatered also
play a role, as this determines the void space in which water can remain.
There are many other factors and, during development of dewatering
models for a US Department of Energy simulator project in the early
1990s, several were documented (Arnold, 1999).
Dewatering devices deal with mechanically removable surface
moisture. Drying will reduce additional surface moisture, and some
processes have been developed to remove some of the inherent or bed
moisture. You can report ash, sulfur, heating value, or other properties
based on any moisture condition as shown in Table 3, for example, “as
5
An excellent, albeit non-coal, example lies in the discovery that 15 years of
Alzheimer’s disease research and a large amount of government funding was
predicated upon fraudulently manipulated images in a 2006 paper (Piller,
2022).
6
Unless the coal is collected at the mine portal, the entrance to an under­
ground mine is not the location of the sample. As with falsified data, incorrect
locations, whether inadvertent or intentional, live on in the data and can be
difficult to excise from the scientific record.Not all problematic locations are
intentionally false. U.S. Bureau of Mines reports from the 1920’s through
1940’s gave locations in underground mines as related to the underground
surveying system. If the maps have not survived or are difficult to locate,
though, the locations cannot be precisely tied to a surface location.
4
International Journal of Coal Geology 263 (2022) 104120
determined” would be the moisture content of the sample when it was
analyzed. “As-received” would have implications for these analyses
when received by a customer. This implies that a sample was collected
and contained in a bag or drum without the opportunity for moisture to
enter or exit. “Dry” means without moisture following the ASTM pro­
cedure for total moisture. But in every case and for every analysis, the
associated moisture content must be included.
This brings us to the arbitrary “air-dried” analysis. What is air-dried?
One definition may be when the visible surface moisture was gone from
the coal even at the bottom of the pile. Is this for a certain time? Is this at
a certain temperature? Were fans blowing over the sample? Who de­
termines if the visible surface moisture is gone? If the total moisture is
then measured and other analyses performed, the analyses can be
expressed on a “dry” or an “air-dried” basis. This would be like the “as-
determined” value, reporting it at that particular “as-determined” value
of moisture. However, the “air-dried” condition is not for a specified
time at a specified relative humidity or temperature.
What happens if the sample is then subjected to wet sieving for
determining the size analysis and then all of these samples are “air-
dried?” The samples are then subjected to ash, sulfur, and heating value
analysis. Each of these samples must then have the measured “air-dried”
moisture reported so that each fraction can be adjusted to the “dry” basis
for doing any review of cumulative ash by size, for example. Each of
these size fractions will not dry to the same “air-dried” moisture.
It becomes further complicated when a sink/float or washability
analysis is reported on an “air-dried” basis. Each of the washability
fractions will not be air dried to the same moisture level either. The
moisture content of each fraction must be measured (according to ASTM
standards) and the other analyses reported on a dry basis to prepare
cumulative ash values (or sulfur, etc.). At a minimum, the “air-dried”
moisture must be included with any “air-dried” analysis.
3. Case studies
3.1. Macerals
3.1.1. Problems and pitfalls in the analysis of macerals
The coal petrographic nomenclature has been modified (Interna­
tional Committee for Coal and Organic Petrology (ICCP), 1998, 2001;
Sýkorová et al., 2005; Pickel et al., 2017) since the publication of Taylor
et al. (1998). Users and generators of petrographic data should be aware
of the changes throughout the history of maceral nomenclature. In some
cases, older nomenclature survives, such as the combination of the more
recently named funginite and secretinite appearing under the older
maceral name sclerotinite, not just in the older literature but also in
more recent papers. Unless good images accompany the paper, caution
should be applied in using the data. Most maceral identification and
virtually all measures of maceral reflectances are done with reflected-
light, oil-immersion optics (discussions in Taylor et al., 1998).
With the increase of rank, the reflectances of the maceral groups
converge (Taylor et al., 1998). This is particularly notable in the
convergence of liptinite and vitrinite reflectances by the medium vola­
tile bituminous to low volatile bituminous transition. Contrary to what
has been interpreted from Pickel et al. (2017), with some exceptions, the
liptinites are not absent in high-rank coals (Taylor et al., 1998, their figs.
4.12 f and g, p. 202 and figs. 5.3 c and d, p. 291; Hower et al., 2019, their
figs. 2-4; Hower et al., 2020b, their figs. 4-5; Hower et al., 2021b, their
figs. 1e and 1f). In the anthracite examined by Hower et al. (1994b),
liptinite, vitrinite, and inertinite macerals had the same random re­
flectances with the liptinites having the highest maximum and lowest
minimum reflectances. Along with the means of distinguishing liptinites
in cross-polarized light, essential in the petrographic analysis of high-
rank coals, observations of their morphology indicates that the liptin­
ites can survive to the higher ranks.
Overlapping reflectances between macerals and the reliance on
textural clues to distinguish certain macerals and submacerals implies
J.C. Hower et al. International Journal of Coal Geology 263 (2022) 104120

Table 2
American Society for Testing and Materials classification of coals by rank (ASTM International D388-19a, 2019).
Class/Group Fixed Volatile Calorific value limits, Agglomerating Character
carbon matter Btu/lb / MJ/kg
limits, % limits, % (moist * mineral matter free
(dry (dry basis)
mineral mineral
matter free matter free
basis) basis)

= or < > = or = or > <

> <

Anthracite
Meta-anthracite 98 – – 2 – – Nonagglomerating
Anthracite 92 98 2 8 – –
Semianthracite 86 92 8 14 – –
Bituminous
Low volatile 78 86 14 22 – – Commonly agglomerating (there may be nonagglomerating varieties with notable exceptions
Medium 69 78 22 31 – – in the high volatile C bituminous rank)
volatile
High volatile A – 69 31 – 14000**/ –
32.6
High volatile B – – – – 13000**/ 14,000/
30.2 32.6
High volatile C – – – – 11,500/26.7 13,000/
30.2
High volatile C 10,500/ 11,500 / Agglomerating
24.4 26.7
Subbituminous
Subbituminous A – – – – 10,500 / 11,500 / Nonagglomerating
24.4 26.7
Subbituminous B – – – – 9500 / 22.1 10,500 /
24.4
Subbituminous C – – – – 8300 / 19.3 9500 / 22.1
Lignitic
Lignite A – – – – 6300 / 14.7 8300 / 19.3
Lignite B – – – – – 6300 / 14.7

This classification does not include a few coals, principally nonbanded varieties, which have unusual physical and chemical properties and which come within the
limits of fixed carbon or calorific value of the high volatile bituminous and subbitumionus ranks. All these coals either contain less than 48% dry mineral matter free
fixed cabon or have more than 15,500 moist mineral matter free Btu per pound (Btu/lbx 2326 = kJ/kg).
*
Moist refers to coal containing its natural inherent moisture but not including visible water on the surface of the coal.
**
Coals having 69% or more fixed carbon on the dry mineral matter free basis shall be classified according to the fixed carbon, regardless of calorific value.

consisting of a 20-mesh sample,7 the examination of macerals and

Table 3
microlithotypes in, for example, the − 500-mesh (− 25-μm) fraction of a
Basis of Reporting (MJ/kg = (Btu/lb)/429.92).
pulverized power plant feed coal is a challenge. This is particularly true
A = ash Multiply by: for the microlithotype analyses, by definition, no particle would meet
M = moisture
Wanted the 50-μm threshold of the microlithotype definition,8 yet none of the
Given ad ar d daf optically identifiable particles should be ignored (Hower and Wagner,
2012). The contrast between determining microlithotypes on +50-μm
as-determined (100-Mar)/ 100/(100- 100/(100-
(ad) (100-Mad) Mad) Mad-Aad)
vs. -50-μm particles is illustrated on Fig. 1; the consequence of not
as-received (ar) (100-Mad)/ 100/(100- 100/(100- counting the − 50-μm particles would be the loss of information and the
(100-Mar) Mar) Mar-Aar) biasing of the results.
dry (d) (100-Mad)/ (100-Mar)/ 100/(100-
100 100 Aad)
3.1.2. Coking
dry ash free (100-Mad- (100-Mar- (100-Ad)/
(daf) Aad)/100 Aar)/100 100 The use of coal petrology in predicting the behavior of single coals
and coal blends in the production of metallurgical coke dates, at least, to
Example: A coal contains 13,000 Btu/lb. on a dry basis. What is the as-received
the studies of coals at the U.S. Bureau of Mines (USBM). Fieldner et al.’s
heating value at 6% as-received moisture?
(1937) thin-section-petrology-based study of the blending of an eastern
Dry Btu/lb. x (100 - As-received Moisture)/100 = As-received Btu/lb.
13,000 x ((100–6)/100) = 13,000 × 0.94 = 12,502 Btu/lb. (as-received).
Kentucky high volatile bituminous coal with the high volatile

that the particle size of particulate samples is an important, albeit in­ 7

direct, part of the maceral identification. For example, low-reflectance
semifusinite may not be distinguishable from vitrinite without the
observation of the open cell lumens typical of semifusinite. While this is
not a factor for the coarser particles in the typical petrographic pellet
Note, 20 mesh represents the top size of all the crushed coal. The fine
particles down to the optical limit are neither discarded in the sample prepa­
ration nor ignored in the maceral counting.
8
Note that macerals (− inite suffix) are the individual components of
microlithotypes (− ite suffix), the maceral assemblages, which, in turn are the
components of lithotypes (− ain suffix), the megascopically identifiable lithol­
ogies (after Taylor et al., 1998; discussions of microlithotype analysis by Hower
and Wagner, 2012).

5
J.C. Hower et al.
Fig. 1. Relatively coarse (left) and fine (right) coal particles in an epoxy matrix with superposed 50-μm-diameter circles. On the coarse particle (left image), the 50-
μm-diameter circle encompasses a duroclarite microlithotype that fits well within the circle. Within the assemblage of fine particles on the right image, a semifusinite
maceral comprises the inertite microlithotype. None of the particles in the right image are large enough to meet the strict definition of a microlithotype, yet none of
them can be ignored if the coal sample maceral and microlithotype counting is to be considered. After Hower and Wagner (2012).
bituminous Pittsburgh coal and the low volatile bituminous Pocahontas
coal is a good example of work of the USBM.9 Other investigations
include those of Davis et al. (1942, 1943) on two other Kentucky coals.
Thermoplastic properties were measured on a Davis plastometer and an
Agde-Damm dilatometer, predecessors of the Gieseler and Audibert-
Arnu instruments in more common use today (Walters et al., 1963).
The modern integration of reflected-light coal petrography with coke
strength prediction began with the work of Andre H. Brisse (U.S. Steel)
and William Spackman (Penn State) in 1951 (Spackman, 2000).
Spackman broke with the Thiessen-Bureau of Mines thin-section petro­
graphic methods and nomenclature then prevailing in the United States
and employed Stopes’ maceral concept in his description of coals. By the
end of the decade and into the early 1960’s, coke strength prediction
methods developed along somewhat parallel paths in the Soviet Union
(Ammosov et al., 1957) and North America (Spackman et al., 1960;
Schapiro et al., 1961; Schapiro and Gray, 1961; Benedict and Berry,
1966; Berry et al., 1967; Gray et al., 1978; Spackman, 2000; Thompson,
2000; Dutcher and Crelling, 2000; North et al., 2018a, 2018b, 2019).
Basically, the goal of the petrographic method is to predict the results of
the ASTM tumbler test (the percentage of +1-in. (+2.54-cm) coke
remaining from a 10-kg sample of +2-in. (5.08-cm) coke subjected to
1400 revolutions in a 36-in. (91.44-cm) diameter drum at 24 rpm) or a
similar test. Fundamentally, the coke strength predictions, coke strength
after reaction (discussed in this section), and tests of the fluidity and
dilation of the melted coal (section 3.3.2) are used together to predict
the behavior of coals in coking. To determine the petrographic predic­
tion, the reactive macerals on a mineral-containing basis are prorated to
their respective V-types, with the V-types representing the level of vit­
rinite reflectance in 0.1%Rmax intervals.10 The composition balance
index (CBI) is determined as follows:
Optimum inert index = Σ (total reactive macerals/optimum inerts)V−
type
(1)
9
At the same time, the USBM was investigating the interface of petrology
with coal hydrogenation. Fisher et al. (1942) noted the correlation between
coal rank and type and hydrogenation yield, with lower ranks and high
anthraxylon (vitrinite) and liptinite producing the best yields.
10
As an example of the importance in evaluating the V-types, Li et al. (2022),
in a study of blends of ostensibly similar rank high volatile A/medium volatile
bituminous coals, found the coal with the lower V-types to have poorer coking
qualities.
6
International Journal of Coal Geology 263 (2022) 104120
(2)
CBI = total inerts/optimum inert index
Where inerts represent the percentage of the inertinite macerals and
the mineral matter and the optimum inert index is a known parameter
for each V-type. The Strength Index (SI) indicates the coke forming ca­
pacity of the reactive macerals, as follows:
Optimum strength = Σ (%reactive macerals x strength factor)V− (3)
type
SI = Optimum strength/total reactives (4)
The intersection of CBI and SI on a nomogram gives the predicted
ASTM tumbler coke stability. The International Standards Organiza­
tion’s Micum mechanical strength (M40) is related to the ASTM tumbler
stability as follows:
ASTM stability = 0.913 (M40 )–13.88 (5)
Coke strength after reaction (CSR) is a predictive parameter for the
coke degradation in the blast furnace, with higher CSR number corre­
sponding to improved blast furnace parameters. Inland Steel’s empirical
formula (after Valia, 1989), based on 28 single coals and 48 coal blends,
is:
CSR = 28.91 = 0.63 (plastic range)–CI (6)
Where the plastic range is the difference between the initial fluid and
the solidification temperatures from the Gieseler plastometry test and
CI, as follows:
CI = 9.64 (CaO+MgO+Fe2 O3 +Na2 O+K2 O)/(SiO2 +Al2 O3 )+14.04(Stotal )
(7)
where the major oxides and the S are on the ash basis of the tested
coal. CSI is an additive property, therefore the individual coals in a blend
can be evaluated individually or as components of blends (Valia et al.,
1989). Hower et al. (1994a) estimated the CBI, SI, M40, and CSR for a
series of high volatile A bituminous coking coals and blends from eastern
Kentucky.
3.1.3. Pulverization and grindability
Pulverized-coal combustion is the most widely used means of
burning coal. A century ago, the Keystone Coal Catalog (1922, p. 231;
later the Keystone Coal Industry Manual) could say that “… the quality
of coal is not of great importance.” Now it is universally acknowledged
that coal quality is of prime importance in the modern coal industry.
From the basic operations of the power plant to the layers of emissions
J.C. Hower et al.
controls, everything relies on the thorough understanding of the nature
of the coal being mined and burned.
3.1.3.1. Hardgrove grindability. The Hardgrove grindability index (HGI)
is used as a predictor of coal pulverization. Coal purchasing contracts
sometimes specify a cost adjustment in the case of deviations from a
minimum desired HGI; for example, the heating value of a supplied coal
may need to be increased by 200 Btu/lb. (0.46 MJ/kg) for every HGI unit
below 50 as an offset of the lost efficiency in the pulverization of the
harder coal (Hower, personal communication based on information
supplied by coal-fired power plants).
The HGI test uses a 50-g split of the − 16 + 30-mesh size (− 1.18 mm
+ 600 μm) test fraction. In the production of the test fraction, the top
size is constrained by the sample preparation process and no oversize
material is lost in the sample preparation. The − 30-mesh coal, however,
is discarded in the sample preparation. As discussed by Hower (1998;
and references therein) and Hower et al. (2021a), this means that the
test sample is biased towards the tougher liptinite-rich microlithotypes.
HGI is determined from the weight of the ground coal passing through a
200-mesh (75-μm) sieve following the ASTM D409 test procedure. The
predictions of the HGI from coal quality parameters tend to include a
measure of the ash content, the coal rank (Fig. 2), and a petrographic
parameter. Of the latter, while the liptinite content is a good first
approximation, at least for high volatile bituminous coals (Hower and
Wild, 1988), the microlithotype composition, including the measure of
the maceral content of the individual microlithotypes, is a better match
for the size distribution (size range) of the post-grinding fraction (Hower
and Wild, 1994; Trimble and Hower, 2000, 2003; Hower and Wagner,
2012; Hansen and Hower, 2014). Overall, for any given high volatile
bituminous rank (via vitrinite maximum reflectance), the HGI decreases
with an increase in liptinite, particularly as reflected in the amount and
composition of the liptinite-rich bimaceral (durite = liptinite + iner­
tinite >95%) and trimaceral (varying proportions of vitrinite, liptinite,
and inertinite groups, each >5%) microlithotypes.
HGI peaks in the medium volatile bituminous rank range (about
1.05–1.40% Rmax; Fig. 2).11 This implies that linear-regression pre­
dictions of grindability can only be made on either side of the medium
Fig. 2. Coal rank, plotted as vitrinite maximum reflectance, vs. Hardgrove
grindability index for 820 coals with ≤20% ash (dry basis) from the Penn State
University coal database. From Hower et al. (2021a, 2021b).
11
Many coal properties, such as HGI, but also including density and Gieseler
fluidity, pass through a maximum or minimum in the medium volatile bitu­
minous rank range (after Van Krevelen, 1993).
7
International Journal of Coal Geology 263 (2022) 104120
volatile / low volatile bituminous rank divide. Attempts at linear re­
gressions crossing the rank divide are doomed to fail owing to the
repeated HGI values at markedly different ranks Hower (2006) discus­
sion of Li et al. (2005)).
3.1.3.2. Coal pulverization. As with HGI, the pulverization of coal is
strongly related to its maceral and microlithotype content. As seen in
Fig. 3, vitrite, the microlithotype with >95% vitrinite, and duroclarite,
the trimacerite microlithotype with vitrinite > liptinite and inertinite,
show markedly different distributions in the size fractions of pulverized
coal from three power plants burning Central Appalachian coals. Dur­
oclarite, the most abundant trimacerite microlithotype in most Appa­
lachian coals, is a tough, hard-to-break microlithotype and is most
abundant in the coarser fractions of the pulverized feed. Vitrite, a brittle
microlithotype, is most abundant in the fine fractions. Different size
fractions produced from the same coal have markedly different petro­
graphic composition, as illustrated here (and by Spackman et al. (1960),
Bayer (1960), with discussions by Hower (1998)), and chemical
composition, as noted by Senior et al. (2000).
3.1.4. Combustion properties of coal
Among the coal characteristics important in combustion are heating
value, grindability, combustibility, and ash properties (Neavel, 1981b).
With a subtle deviation from Neavel’s (1981b) categories, Bengtsson
(1986) described four broad parameters that influenced the number of
combustion phases: vitrinite reflectance, particle size, temperature, and
petrographic composition. Despite the differences in nomenclature,
there are basic similarities between the lists. Heating value and vitrinite
reflectance are both rank parameters (section 3.3); although, as noted in
section 3.1.1, calorific value is related to the maceral content as well as
the coal rank. Grindability and particle size are also related (section
3.1.3), with particle size being a function of the grindability of the coal
and the energy expended in pulverization (Hower, 1998; Barranco et al.,
2006). Neavel’s (1981b) “Ash” characteristic includes not only the ash
composition (section 3.2.1), its slagging and fouling properties (section
3.2.3), and its transition from the feed coal to the fly ash and bottom ash
(section 3.2.2), but also the amount of ash as too much ash in the feed
coal leads to combustion and post-combustion ash handling problems. In
this respect, we note that the relatively low-ash coals commonly used in
some parts of the world are not readily available in some markets.
Combustibility, as discussed in this section, is considered here as the
combustion properties of the macerals (Bengtsson, 1984, 1986, 1987;
Fig. 3. Percentages of the microlithotypes vitrite (vitrinite>95%) and dur­
oclarite (vitrinite>liptinite or inertinite; each greater the 5%) for five size
fractions (plus-100 mesh to minus-500 mesh) of the pulverized coal from three
Central Appalachian power plants. After Hower (2008).
J.C. Hower et al.
Pregermain, 1988; Kruszewska, 1989, 1998; Crelling et al., 1992;
Thomas et al., 1993; Borrego et al., 1997; Biswas et al., 2007; Everson
et al., 2008; Potgieter-Vermaak et al., 2011; Malumbazo et al., 2012;
Stanger et al., 2013; Roberts et al., 2015; Louw et al., 2016; Guo et al.,
2020).
Bengtsson (1986) and Wu (2005), among others, noted the four
combustion phases for bituminous coals as gas phase ignition, gas phase
combustion, ignition of char, and combustion of char. Under some
conditions, the latter four combustion phases can be controlled by an
increase in coal rank, the transition from the clarite to vitrite to durite to
fusite microlithotypes, an increase in particle size, and a decrease in
temperature in the <1200 K range (Bengtsson, 1986).
Rank is an important consideration in combustion, with low-rank,
high-volatile coals being more ignitable. Combustion of low-volatile
coals requires added attention to the boiler design to achieve and sus­
tain combustion (Hough and Sanyal, 1987). In drop-tube-furnace studies
of a wide rank range of coals, Bengtsson (1986) found that a low volatile
bituminous coal had poor reactivity at 800 ◦ C, with it being only slightly
more reactive than an anthracite at 1000 ◦ C. Combustion temperatures
are also rank dependent (Bengtsson, 1986; Crelling et al., 1992; Bar­
ranco et al., 2003). The thermal swelling of vitrinite is rank dependent,
being greater in high volatile than in low volatile bituminous coals with
no swelling or pore formation in anthracites (Bengtsson, 1986; Hower
et al., 2017). Vitrinite with Rrandom < 0.5% initiated weight loss and heat
release at 200 ◦ C in contrast to >260 ◦ C for vitrinite with 1.4–1.5%
Rrandom (Bengtsson, 1986). Similarly, the time in which half of the
sample had reacted increased with an increase in rank and with
increased inertinite content.
The ordering of combustibility, therefore the temperature of com­
bustion, is considered to be liptinite<vitrinite<inertinite; explaining the
“clarite to vitrite to durite to fusite” ordering of transition of combustion
phases noted above. Liptinite can appear to be relatively unchanged in
partially combusted particles (Bengtsson, 1984; Crelling et al., 1992),
giving it the appearance of being less reactive than vitrinite and semi­
fusinite (Crelling et al., 1992). “Appearance” is the keyword in the latter
sentence; partially combusted macerals in fly ash, incompletely burned
particles that were carried through from the boiler, are rare. Their
scarcity indicates that caution must be exercised when considering their
place in the overall maceral reaction scheme.
Inertinite in the feed coal is an important contributor to carbon in the
fly ash (Yavorskii et al., 1968; Hower et al., 2017), with combustion
efficiencies generally having an inverse relationship to the amount of
inertinite macerals (Nandi et al., 1977). Semifusinites from Permian
Gondwana coals, however, proved to be more reactive than semi­
fusinites from other coals (Nandi, 1984). Kruszewska (1989), combining
maceral, reflectance, and experimental char analysis in an investigation
of the reactive/inert ratio of a variety of coals, found that semifusinite
and other lower-reflectance inertinite macerals were really semi-
reactive in combustion. While Pregermain (1988) found that there
were distinct thermogravimetric-analysis-determined burning profiles
from vitrinite-derived and inertinite-derived chars from a series of high
volatile bituminous coals, Thomas et al. (1993), Vleeskens et al. (1993),
and Borrego et al. (1997) determined that inertinite macerals are
combustible under the proper combustion conditions.
3.2. Minerals and inorganic elements
Ideally, determining the major mineral species present (i.e., quartz,
clays, carbonates, pyrite) can provide insights into the coal’s techno­
logical properties such as abrasion, slagging, fouling, and possible
environmental (acid mine drainage) and health impacts (black lung
disease). Semi-quantitative to quantitative mineralogy can be obtained
by X-ray diffraction (Ward, 2002, 2016.), ideally on a low-temperature
ash sample (Gluskoter, 1965). Scanning electron microscopy with an
energy dispersive X-ray detector will provide a qualitative assessment of
the minerals present plus information on their size distribution and
8
International Journal of Coal Geology 263 (2022) 104120
incorporated elements. Numerous other analytical tools, such as
described by Dai et al. (2021), can provide additional useful information
on the minerals in coal.
3.2.1. On the importance of a thorough assessment of elements
Certain coal analyses are fundamental to any study of coal. Among
these analyses are moisture, ash, and some representation of the coal
rank, be it heating value, volatile matter, vitrinite reflectance, among
other accepted parameters. For the sake of coal combustion applications,
we can add the total sulfur and mercury, at least, to the list of essential
analyses. Beyond that, it is desirable to obtain as complete a set of ele­
ments as the research goals and, realistically, the analytical budget will
permit. Analysis of the suite of the lanthanides, for example, without the
context of the total coal chemistry is not adequate.
Emissions of SO2, commonly reported in the US as lbs. SO2/106
Btu,12 became a consideration for US utilities with the passage of the
Clean Air Act in 1970 and its later amendments (US Environmental
Protection Agency, 2021a). In the 1990’s, the US Clean Air Act
amendments named 12 inorganics elements (Sb, As, Be, Cd, Cl, Cr, Co,
Pb, Mn, Hg, Ni, and Se) plus the radionuclides as being potentially
hazardous air pollutants (HAPs) (Akers and Dospoy, 1994; among
others). Ultimately, the emissions of Hg were regulated (US Environ­
mental Protection Agency, 2022). More recently, the US Department of
Energy (DOE), following up on assessments of critical minerals (Na­
tional Research Council, 2008) and several years of studies of DOE-
sponsored studies of REE, initiated regional studies of critical elements
(Fig. 4; Mullen, 2022). The latter is a prime example of the need to
analyze as many elements as budgets and available equipment will
allow. Neither the limited analyses of just the “potentially hazardous”
elements in the 1990’s nor the analyses of just the REE that became
important in the post-2010 push to increase domestic supplies of REE
would have been sufficient to meet the needs of the 2020’s expansion of
the latter effort into a broader portion of the periodic table.
The mode of occurrence of these elements plays an important role in
determining if they can be rejected (trace elements or hazardous air
pollutants) or recovered (REEs or other critical minerals) in coal prep­
aration plants. Akers and Dospoy (1994) provide a good description for
trace element mode of occurrence and the potential for the rejection or
recovery of certain elements. If the elements are in minerals that can be
liberated and separated in traditional coal preparation equipment, then
their rejection or recovery can be anticipated. However, many of these
elements are finely disseminated and hydrometallurgical processing
may be required. It should be noted that of the original 1990 Clean Air
Act amendment list of trace elements to be studied (Sb, As, Be, Cd, Cl, Cr,
Co, Pb, Mn, Hg, Ni, and Se) as hazardous air pollutants, Sb, As, Be, Cr,
Co, Mn, and Ni are now considered critical elements (Mullen, 2022).
If “do not falsify data” is the first commandment for coal geo­
chemists, then “do not censor the periodic table” should be the second.
Yet, in their wariness of and response to the US Environmental Protec­
tion Agency’s Coal Ash Rule (US Environmental Protection Agency,
2021b), among other regulations, some US coal producers and utilities
are increasingly cautious about the elements they allow researchers to
analyze (observation based on the decades-long personal experiences of
the authors). As the lists of critical elements and environmentally haz­
ardous elements overlap, such a cautious approach to data sharing and
to the generation of new data hinders the assessment of critical elements
in coal and coal-derived resources.
3.2.2. Pulverized coal vs. fly ash comparisons
How well does the composition of the pulverized coal translate into
the composition of the fly ash? Note that we are intentionally
12
Emission standards vary between countries. For example, in most European
countries, the value would be expressed in mg/m3 (= 8.14 × 10− 4 lb. 106 Btu)
(Smith and Nalbandian, 2000).
J.C. Hower et al. International Journal of Coal Geology 263 (2022) 104120

Fig. 4. Critical elements as defined by the US Department of Energy (Mullen, 2022).

mentioning the pulverized coal, i.e., the actual boiler feed. The pulver­
ization process removes some rock, including the coarse sulfides, from
the feed, notably impacting the minor and trace element composition of
the resulting fly ash (Hower et al., 2020a). Meij (1994) divided major,
minor, and trace elements into Group 1 (trapped with bottom ash and fly
ash), Group 2 (trapped with fly ash), and Group 3 (elements prone to
escaping with the flue gas) (Fig. 5). The resulting Venn diagram of the
elements, while a useful guide, is imperfect, first because some elements
have mixed behaviors, hence the overlaps between the groups; second
because the capture of some elements, such as Hg, is also a function of
the carbon content of the fly ash; and third because the increase in flue
gas desulfurization and Hg-capture technologies has reduced the emis­
sion of some volatile elements. As an additional caveat, both pre-
combustion handling of the coal and the post-combustion handling of
the bottom ash and fly ash can add non-coal elements to the combustion
products. This could be in the form of contaminants from mining,
beneficiation, or pulverization; non-coal additives to the fuel, such as
tires or petroleum coke (Hower et al., 2005a, 2005b, 2007a, 2007b);
reagents used in Hg capture from the flue gas + fly ash stream (Hood
et al., 2016); or incidental contamination during the collection of the
ashes. As an example of the latter factor, the finding of high levels of Pb
in the bottom ash of a Kentucky power plant turned out to be from the
remnants of lead shotgun pellets used to dislodge slag from the boiler
tubes (Finkelman and Eble, unpublished data from 1994 to 1995 U.S.
Geological Survey study).
Comparisons between the pulverized coal and 1st-row-ESP fly ash for
the 2002, 2007, and 2012 sampling at Kentucky power plants (Hower
Table 4
Pearson correlations for major oxides and minor elements between the pulver­
ized coal and the 1st-row-ESP fly ash (after data from Hower et al., 2005, 2009,
2014). The “Meij group” is after Meij (1994) with reference to Fig. 5. The 1 × 2
and 2 × 3 designate elements in the overlapping segments of Meij’s Venn
diagram.
Pearson corr. Meij group

Zr 0.981 1
Sr 0.949 1
Cr 0.946 1×2
MgO 0.925
Ba 0.922 1×2
Mo 0.916 2×3
TiO2 0.908 1
V 0.900 2
CaO 0.895 1
Al2O3 0.886 1
Fe2O3 0.857 1
Mn 0.855 1
P2O5 0.845 2
Cd 0.838 2×3
Co 0.825 2
Sb 0.775 2×3
SiO2 0.769 1
K2O 0.713 1
Ni 0.652 2
As 0.594 2×3
Pb 0.577 2×3
Zn 0.541 2×3
Na2O 0.495 1×2
Rb 0.428 1×2
SO3 0.347 3
Fig. 5. Grouping of elements captured by bottom ash or fly ash or emitted with
Cu 0.271 2
the flue gas. Modified by Hower et al. (2020a) after Meij (1994).

9
J.C. Hower et al. International Journal of Coal Geology 263 (2022) 104120

et al., 2005a, 2005b, 2009, 2014) (Table S1 in the Supplementary files) were provided by Smith et al. (1986) and Rimmer and Price (1988).
show that the behavior of the elements is irregular (Table 4). The Group The key boiler impacts of the minerals in coal are fouling, the loose
1 elements have the highest and tightest distribution, with an average low-T deposits in the cooler parts of the boiler system or the sintered
Pearson correlation coefficient of 0.868. The overlapping 1 and 2 high-T deposits in the superheater and reheater sections of the boiler,
Groups, group 2, and the overlapping 2 and 3 Groups have similar av­ and slagging, the build-up of liquid and semi-liquid phases on the boiler
erages, with correlation coefficients ranging from 0.698 to 0.707. The tubes. The deposits can contribute to erosion, corrosion, and the deposits
high correlations of pulverized coal to fly ash among low-concentration on boiler tubes and water walls can inhibit the transfer of heat and the
elements (Mo, Cd, Sb) in the overlapping Group 2 and 3 range production of steam (discussions by Berkowitz, 1979; Schobert, 1987;
contributed to the seemingly high average for the group. Similarly, the Babcock and Wilcox Co., 2005, chapter 21). With a few exceptions, such
poor correlation of Cu compared to other Group 2 elements drove down as quartz, the temperatures in pulverized-fuel combustion will melt or
that group’s average. Overall, there are no exact correlations between vaporize most of the minerals. The major oxides, therefore, become the
the Meij (1994) distributions and the experiences in several Kentucky basic unit in the consideration of the behavior of inorganics in coal
power plants because of the variations in feed coals, operating condi­ combustion. The base/acid ratio is the basis for the estimation of the
tions, and efficiency of ash collection between units at one collection total coal alkalis and the slagging and fouling propensities (after
time and the variation within individual units over the course of several Wingartner, 1974):
years. Further, limiting the comparison to just the first ESP row, while
Base/acid = (Fe2 O3 + CaO + MgO + Na2 O + K2 O)/(SiO2 + Al2 O3 + TiO2 )
justified based on the number of available sampling points, created a
bias against the more volatile elements that are relatively more abun­ (8)
dant in the cooler, more distant rows of the ESP array. The chemical data where the oxides are expressed as percentages of the ash. The
from Mardon and Hower (2004; Table S2 in the Supplementary files) resulting parameters are:
illustrates the concentration of the volatile elements, such as Zn and As,
Slagging factor = (Base/acid) • Sdry basis (9)
towards the back rows of the ESPs in contrast to elements with little
variation between rows, such as the REE (discussed below) and Zr.
Fouling factor = (Base/acid) • Na2 O (10)
In general, we have fewer comparisons between the REE in the
pulverized coal and in the fly ashes, the most abundant coal combustion ( )/
Total coal alkali = (Na2 O + 0.6589 K2 O) • ashdry basis 100 (11)
byproduct and one target for potential extraction of critical elements.
Taggart et al. (2016) focused on the study of fly ashes, many of which The critical ranges for the indices are provided in Table 5.
were obtained from the University of Kentucky Center for Applied En­
ergy Research (CAER). Some of the Taggart et al. (2016) samples did not 3.2.4. Health aspects
have analyses of the accompanying pulverized coal samples. Mardon Coal represents the ‘perfect storm’ in capturing and concentrating
and Hower (2004) study of a single-seam (a Fire Clay correlative)/ elements that are economically valuable (e.g., Ge, U, Se, Ag), cause
single-mine coal feed at a Kentucky power plant, planned as a study of technological problems (e.g., P, Cl), and that can cause health problems
the partitioning of Hg, proved to be a comprehensive examination of the (e.g., As, F, Hg, Se). These elements can be captured by the organic
distribution of REE from the mine to the fly ash and bottom ash at the matter, washed in with the mineral detrital matter, or deposited from
power plant. In their analyses of the pulverized feed coal (dry ash basis), volcanic ash fallout. Many of these elements are incorporated in the coal
two rows of mechanical (cyclone) fly ashes (four hoppers sampled in cleat and fractures by fluids, both hot and cold, that percolate through
each row), three rows of ESP fly ashes (two hoppers sampled in each the permeable coal over geologic time after its formation.
row), and the bottom ash, the individual lanthanide elements in the Though most of the coals being mined have low to modest concen­
bottom ash and fly ashes (all on the dry ash basis) fall within the ±30% tration of these valuable, troublesome, and dangerous elements, coals
range of the pulverized feed coal (data in Mardon and Hower, 2004; data with extraordinarily high concentrations of these elements have been
with the percentage range calculations in Table S2). Between eight to 10 used in primarily residential situations, resulting in widespread and
of the 15 ashes for the light REE and six to 10 of the ashes agree for the severe health problems. Examples include the As-rich coals that were
heavy REE at the ±10% level. For the Light REE/Heavy REE ratio, 13 of used in Guizhou Province, China. A sample of these coals contained
the 15 ashes are within ±10% of the pulverized coal. Overall, the REE more than 35,000 ppm As (ash basis) (Belkin et al., 1997). Thousands of
behavior for this well-characterized power plant agrees with Meij’s people in the region showed visible symptoms of arsenic poisoning
(1994) assignment of the REE to the Type 1 elements, the elements including hyper-pigmentation, hyper- and hypo-keratosis, Bowen’s
trapped in the bottom ash and fly ash.
Table 5
3.2.3. Implications of mineral matter in coal combustion
Fouling and slagging index critical values for bituminous and low-rank coals
Several recent reviews of coal geochemistry and mineralogy discuss (after Wingartner, 1974).
the element/mineral associations and their implications (Ward, 2002,
Low Medium High Severe
2016; Matjie et al., 2011; Creelman et al., 2013; Liu et al., 2018; Dai
et al., 2018, 2020b, 2021; Finkelman et al., 2019). Aspects of the Bituminous coals
Fouling
behavior of minerals and their associated elements in combustion and
Fouling factor <0.2 0.2–0.5 0.5–1.0 >1.0
the partitioning of elements in the ash collection system was discussed Total coal alkali % <0.3 0.3–0.45 0.45–0.6 >0.6
above (sections 3.2.1 and 3.2.2), and the health implications of in­ % Chlorine in coal <0.2 0.2–0.3 0.3–0.5 >0.5
organics in coal will be discussed below (section 3.2.4). Here we deal Slagging
with post-combustion/pre-ash collection aspects of minerals and Slagging factor <0.6 0.6–2.0 2.0–2.6 >2.6

elements.
Ash fusion temperatures provide a means of predicting the softening Low rank coals
and melting temperatures of coal ashes prior to combustion. As the ash Fouling
%NaO2 in ash <0.5 0.5–1.0 1.0–2.5 >2.5
fusion temperatures of coal ashes within a blend are not necessarily if <25% CaO in ash <25 15–25 <15
linear, mathematical methods have been employed to estimate the Slagging
thermal behavior of ashes (Huffman et al., 1981; Huggins et al., 1981; Base/acid <0.5 0.5–1.0 1.0–1.75
Gray, 1987; Yan et al., 2019; Li et al., 2020a, 2020b; among others). Fe2O3/CaO in ash <0.3 0.3–3.0 ca. 1.0
Summaries of the ash fusion characteristics of Central Appalachian coals >3.0

10
J.C. Hower et al.
Disease, and squamous cell carcinoma. Hundreds reportedly died from
exposure to arsenic mobilized by residential combustion of the As-rich
coal.
In the same region and elsewhere in China, millions of people suf­
fered from dental and skeletal fluorosis. Most of these health problems
were likely caused by the residential use of hand-made briquettes con­
taining F-rich soil as a binder. But some of the coal had exceptionally
high concentrations of F. In a rural village in Guizhou Province many
elderly people had lost their eyesight (Finkelman et al., 1999).
High concentrations (~55 ppm versus a coal average of 0.16 ppm) of
Hg in coal being used in homes were suggested as the cause of blindness
(Finkelman et al., 2002). In the Donbas region of Ukraine and Russia,
coal has been reported with Hg concentrations of about one weight
percent (Kolker et al., 2009).
The use of high-Se stone coal in China has been cited as the cause of
selenosis manifested by the loss of fingernails and toenails and the yel­
lowing of the skin (Zheng et al., 1992). Among other elements, Be
emitted from a commercial coal-burning power plant has been suggested
as causing loss of hearing in children living in the vicinity of a Czech
power plant (Petanova and Bencko, 2020). Chromium in coal is another
concern. Although the levels of Cr in coal are usually quite modest and
most, if not all, the Cr is tri-valent Cr, a generally benign form, when coal
is combusted, the Cr is concentrated in the fly ash and a portion is
converted to the hexavalent form, a highly dangerous compound (Sheps
et al., 1999).
Even some of the minerals in coal have been reported to cause health
problems. Huang et al. (2004) suggested that high concentrations of
pyrite in coal contribute to coal workers pneumoconiosis. Large et al.
(2009) believed that the exceptionally high abundance of fine-grained
quartz in coal (silicosis) was an important contributory factor in the
extraordinary high incidence of lung cancer among women in Xuan Wei
County, Yunnan Province, China. Silicosis is not limited to one country
nor just to coal mining. One of the most tragic examples comes from the
early 1930’s construction of the Hawk’s Nest drainage tunnel in central
West Virginia in which silicosis was responsible for an estimated 476 to
1000 deaths (Cherniak, 1986).
Admittedly, these are just a few examples of the health impacts
caused by coal use. Nevertheless, the possibility exists that using coal
with unusually high concentrations of potentially harmful elements can
contribute to health problems. A routine analysis of the coal to deter­
mine trace element concentration can prevent further health problems.
3.3. Coal rank
Coal rank is defined by several parameters throughout the rank
range, from heating value and moisture in lower rank coal (lignite and
subbituminous), to volatile matter/fixed carbon and total carbon
(proximate and ultimate analyses) in high and medium volatile bitu­
minous rank coal through, at least, semi-anthracite, and hydrogen and
X-ray diffraction properties at the highest ranks (Taylor et al., 1998).
Vitrinite reflectance is used throughout much of the rank range. It is of
marginal value at low ranks, however, both because of its limited range
and because of the difficulty in finding enough of the proper huminite
maceral to make a significant number of measurements. Although vit­
rinite reflectance might usually be a parameter free of external in­
fluences, perhydrous (H-rich owing to marine influences) vitrinite will
have a lower reflectance than ‘normal’ vitrinite of the same rank (Hutton
and Cook, 1980; Kalkreuth, 1982; Price and Barker, 1985; Gurba and
Ward, 1998; Petersen and Vosgerau, 1999; Li et al., 2010; Mendonça
Filho et al., 2010).
Owing to the variations in the chemistry of the macerals, particularly
among low-rank coals, the maceral content can be an important factor in
the determination of the chemical coal rank parameters. Although
equilibrium moisture and heating value are more common parameters,
no single rank parameter is ideal for low-rank coals.
11
International Journal of Coal Geology 263 (2022) 104120
3.3.1. Tax implications of coal rank
3.3.1.1. Black Lung Benefits Act of 1977 and coal rank implications. The
Black Lung Benefits Act of 1977 (Internal Revenue Service Code Section
4121) exempts lignite from the excise tax imposed by the act (Apel,
1988; Watts and Gaggini, 1988). In 1986, the US Internal Revenue
Service ruled that excess water (meaning water added during prepara­
tion and storage minus the equilibrium moisture (see Luppens (1988)
comments about equilibrium moisture) could be subtracted from the
taxable weight of coal of any rank (Watts and Gaggini, 1988).
3.3.1.2. Surface Mine Control and Reclamation Act of 1977 rank classi­
fication. In the United States, the Surface Mine Control and Reclamation
Act of 1977 (SMCRA) prescribes reclamation fees based on the coal rank,
with lignite calling for a lower fee than subbituminous C rank coal.13
The latter rank boundary is defined by the gross calorific value, with
8300 Btu/lb. (19.31 MJ/kg) on the moist, mineral-matter free basis
being the division between the ranks (lignite being on the lower side of
the boundary) (ASTM D 388). The differences in heating value between
and among the liptinite and humic macerals would imply that the subtle
variations in heating value between different layers of the coal or be­
tween different tracts within the same property could compel a coal
company to, at least, attempt to adjust its reclamation fees according to
coal rank and maceral variations.
In the case of Wyodak Resources Development Corp. v. The United
States, the plaintiffs argued that because some layers of the thick (±24
m) Powder River Basin (Wyoming) coal fell below the ASTM-specified
rank boundary, they were entitled to a refund of SMCRA reclamation
fees (Wheeler, 2017). A 2009 ruling by the US Internal Revenue Service
(IRS) concerning a similar exemption for lignite under the Black Lung
Excise Tax (BLET) stated that a company could gain an exemption if
ASTM standards were applied in testing the coal rank and if the taxpayer
“operates a mine from which taxable coal [subbituminous rank] and
nontaxable lignite are extracted.” In that case, the IRS did grant a refund
of a portion of the BLET, giving Wyodak hope that they could prevail in
the SMCRA case. Wyodak, however, relied upon partial samples of the
whole seam, sampling either the lowermost 15 ft (4.57 m) or selected
lithologies. The ASTM guidelines for rank determination (ASTM Inter­
national D388-19a, 2019) call for an averaging of the gross calorific
value of not less than three, and preferably five or more, full seam or
core samples from an area of no more than 4 mi2 (10.36 km2). The
government’s witness, coal geologist James Luppens (emeritus, U.S.
Geological Survey), noted that small-scale variations in the maceral
content could impact the apparent rank of individual layers. While
small-scale variations were the basis of Wyodak’s claim, since the ASTM
guidelines call for whole-seam sampling in order to average out the
small-scale variations, Judge Thomas Wheeler ruled against the Wyodak
Resources Development Corp. claim for a refund of the reclamation fees.
3.3.1.3. Canadian tariffs on bituminous coal. Tax and tariff situations are
not new, nor are they confined to low-rank coals. On 13 May 1887,
Canada removed an import duty on anthracite while retaining a 60
cents/ton duty on bituminous coals (Canada House of Commons, 1926).
Canada classified the Bernice coalfield, Sullivan County, Pennsylvania,
as bituminous14 but protests from the State Line and Sullivan Railroad
Company hauling the coal and from Pennsylvania State Geologist J.
Peter Lesley prompted Thomas Hayes, Ontario School of Chemistry and
Pharmacy, to analyze the coal in February 1888. His analysis prompted
the proper reclassification of the coal to anthracite (Claghorn, 1889).
13
$0.35/short ton for subbituminous and higher rank surface-mined coal vs.
the lesser of 2% of the value of the coal at the mine or $0.10/short ton for
lignite.
14
The mischaracterization of the Bernice coal stems from the classification of
an apparently weathered semianthracite as a bituminous coal (Platt, 1880).
J.C. Hower et al.
From the perspective of the anthracite industry, the removal of the tariff
resulted in exports to Canada increasing from 995.4 kt in 1886, the last
full year the duty was in place, to more than 2.1 Mt. in 1888 with exports
continuing in the 1.2–1.57 Mt. range through at least 1896 (Anonymous,
n.d).
In these tax and tariff examples, the proper rank classification ulti­
mately was of benefit to the coal company. In the Wyodak case, it could
be argued that, although they were liable for a higher tax rate, their
reputation as a producer of subbituminous coal was intact. Lignite has a
reputation as a coal that cannot be shipped far owing to the amount of
moisture in the fuel; it is usually a product for mine-mouth power plants
or similar facilities. In the Bernice coalfield case, the coal was ultimately
classified as an anthracite and, as a result, the exports to Canada
increased.
3.3.2. Expansion and fluid properties of coal
3.3.2.1. Coal fluidity. The expansive/fluid/thermoplastic properties,
implying successive softening, swelling, and resolidifying/coking, of
coal encompass all three corners of the compositional triangle. The
expansion and fluid properties of coal have implications in coking, coal-
to-liquids technologies, and the manufacture of carbon products from
coal feedstocks.
In general, the thermoplastic range of coal spans the bituminous rank
range (the caking coals, with coking coals being a subset of the caking
coals), with the fluidity peaking in the upper high volatile A to medium
volatile bituminous rank range (Fig. 6).15 Various tests for fluidity and
expansion are described by Davis (1978), Berkowitz (1979, 1985),
Zimmerman (1979), and Hessley et al. (1986). Rank is the first consid­
eration in determining the thermoplastic properties, with the maceral
and mineral composition and aspects of the elemental composition
Fig. 6. Gieseler fluidity (ln (ddpm)) vs. vitrinite maximum reflectance (%Rmax)
for coals from the Penn State University data base. Coals with a fluidity higher
than ln (30,000) = 10.3089 have fluidities that exceed the measuring capability
of the instrument.
15
The typical machine used for the measurement of the Gieseler plasticity
measures the fluidity in the artificial parameter of “dial divisions per minute
(ddpm)”, typically peaking at 28,000 to 30,000 ddpm. Lloyd et al. (1984a,
1990) overcame this limitation by plotting the natural logarithm of the ddpm
along melting and coking slopes vs. T for the 3 ◦ C/min ramp or vs. time for the
isothermal runs and calculating the ln ddpm of the intercept of the two slopes.
The test calls for <40-mesh coal heated at a ramp of 3 ◦ C/min in a crucible and
stirred at a constant torque of 40 g-in (9.957 mN-m [milli Newton – meter] in S.
I. units).
12
International Journal of Coal Geology 263 (2022) 104120
playing roles in their expression. The apparent coal rank can be decep­
tive. Certain Illinois Basin coals (in this example, Pennsylvanian coals
from Daviess and Henderson counties, Kentucky) have vitrinite
maximum reflectances from 0.37–0.44% (CAER analyses) along with
Free Swelling Indices (FSI) up to 4 (Bragg et al., 1998). While the vit­
rinite reflectances are an apparent overlap with the subbituminous rank
range, the FSI is a clear indication that the coals are high volatile C
bituminous caking coals.
While the Gieseler plasticity test, a common tool in the examination
of coal’s thermoplastic properties, is usually conducted at atmospheric
pressures using a heating ramp of 3 ◦ C/min, Lloyd et al. (1984a, 1984b,
1984c, 1989, 1990) experimented with both isothermal and pressurized
Gieseler plasticity studies of high-vitrinite, high volatile C through A
bituminous coals. Rees and Pierron (1954, 1955) and Pierron and Rees
(1960) discussed the fundamentals of coal thermoplasticity, including
the role of mineral and inert maceral diluents in diminishing the fluidity.
Neavel (1976, 1981a), Given et al. (1986), Lin et al. (1986), Lynch et al.
(1988), Derbyshire et al. (1989), Sakurovs (2000), and Sahoo et al.
(2022) further discussed and debated the basic principles of thermo­
plasticity and coal structure.
Following Ignasiak et al.’s (1978) discussion of the enhanced ther­
moplastic properties of the high-organic-S Raša coal, Croatia, Waddell
et al. (1978) and Yarzab et al. (1980) noted the implications of the
amounts of organic S on the liquefaction potential of coals. While the
Paleocene Raša coal has unusual thermoplastic properties (for example,
see White et al., 1990), Ignasiak et al. (1978) underestimated the coal
rank, considering it to be lignite instead of high volatile B bituminous
(after Medunić et al., 2020), thus over-emphasizing its deviation from
normal caking behavior. No doubt, while the thermoplasticity described
by Ignasiak et al. (1978) is extraordinary, the coal is not a lignite with
caking properties.
Comparing the high volatile A bituminous Manchester coal (south­
eastern Kentucky) investigated by Cole and Williams (1981) with similar
rank, but generally higher sulfur coals from western Kentucky (Lloyd
et al., 1984a, 1984b, 1984c, 1989, 1990), it was apparent that the
Manchester coals had a lower Gieseler plasticity except in cases where
the Manchester coals also had an organic S content approximating the
western Kentucky coals. Senftle and Davis (1982), in a study of the high
volatile through low volatile bituminous Lower Kittanning coal in the
Northern Appalachian coal basin, also observed that, for a tight vitrinite
reflectance (rank) range, the higher organic-S coals had a higher plas­
ticity (Fig. 7; Table 6). Note that the lowest rank coals (0.60%Rmax) have
Fig. 7. Gieseler fluidity (ddpm) vs. organic sulfur (%, daf) for selected vitrinite
reflectances for vitrinite concentrates of the Lower Kittanning coal in western
Pennsylvania. The coals at 30,000 ddpm reached the mechanical limit of the
Gieseler apparatus and likely would have higher fluidities. After Senftle and
Davis (1982).
J.C. Hower et al. International Journal of Coal Geology 263 (2022) 104120

Table 6
Organic S, vitrinite maximum
reflectance, and fluidity
(ddpm = dial division per
minute) for vitrinite concen­
trates of the Lower Kittanning
coal, western Pennsylvania,
after Senftle and Davis (1982).
A caveat, to keep most of the
readings below the machine
limit of 30,000 ddpm, the tor­
que was halved, resulting in an
approximately 10× decrease
in the fluidity values. Conse­
quently, the results in the third
column are relative to each
other but are not comparable
to other experiments. The
values in the shaded blocks are
plotted on Fig. 7.

Fig. 8. (A) Gieseler fluidity (ln (ddpm)) vs. vitrinite maximum reflectance (%
Rmax) and (B) Gieseler fluidity (ddpm) vs. organic sulfur (%, daf) for coals
analyzed by Lloyd et al. (1990). Note that the ln (fluidity) > 10.3089 were
estimated from the intersection of the natural logarithms of the melting and
coking slopes.

negligible fluidities; thus, the differentiation with respect to organic

sulfur is more evident at the higher ranks. Lloyd et al. (1990) also
demonstrated a relationship between organic S and fluidity (Fig. 8).
Clark et al. (1984), in an energy dispersive X-ray spectroscopy study of
organic S in coal and in the solid residues from Gieseler runs, found that
vitrinite macerals with high organic S in the raw coal, upon heating, lost
organic S at a faster rate than vitrinite macerals with low organic S.
Discussion of the implications of the use of high-organic-S coal in coking
is found in Shen et al. (2021).
Dilatometry, as determined on an Arnu or similar dilatometer,
measures the initial thermal contraction of a coal followed by, in some
case, its expansion. Bland et al. (1983) examined the dilatant behavior of
a number of the coarser fractions of western Kentucky clean coals in an
Arnu dilatometer. In general, this represented the same suite of coals
examined by Lloyd et al. (1984a, 1984b, 1984c, 1989, 1990). The
contraction and expansion percentages for the coals are plotted on
Fig. 9. While the comparison to coal rank without the consideration of
other properties is a simplification, we do know from the Bland et al. and
Lloyd et al. studies that the coals have high vitrinite contents. While
there is no systematic trend for contraction versus rank, the dilation Fig. 9. Coal rank, as vitrinite maximum reflectance, vs. Arnu dilatometry
contraction and dilation percentages for a suite of western Kentucky clean coals
increases with an increase in coal rank, peaking at about 90% dilation
(after Bland et al., 1983).
for coals with 0.70–0.75%Rmax. A few high volatile C bituminous coals
did not expand following the initial contraction.

13
J.C. Hower et al.
3.3.2.2. Coal oxidation as reflected in the thermoplastic properties. Unless
extraordinary measures are taken, such as the storage of the coal under
an inert gas (Vorres, 1990; Glick et al., 2005), oxidation of coal will be
an issue. While this is a serious issue with coking properties (Gray et al.,
1976; Larsen et al., 1986; Gray, 1991; Markova and Ruschev, 1993;
Rouzaud et al., 1994; Alvarez et al., 1998), Senftle and Davis (1982)
demonstrated that the deterioration of Gieseler fluidity with oxidation
did not imply that the liquefaction conversion of the coal would be
significantly impacted.
Senftle and Davis (1982) noted that the fluidity of two high volatile A
bituminous coals (Pennsylvanian Pittsburgh seam from Pennsylvania
(PSOC-1099) and Cretaceous Upper Sunnyside seam from Utah (PSOC-
1116)) stored in air at room temperature dropped rapidly within the first
20 days after crushing to the − 40-mesh test size. The softening and
maximum fluidity temperatures increased with increased oxidation.
Jung (1935) also reported a decrease in the maximum fluidity T with
oxidation. Loison et al. (1963) noted that low-rank coals oxidize at a
faster rate than high-rank coals.
Lloyd et al. (1984a) weathered one of their coals at 20–40% relative
humidity and 22–25 ◦ C in an open container. Through six months of
measurements, they found that the fluidity (reported as the natural
logarithm of the dial divisions per minute (ddpm)) decreased with a
slope of − 0.0081/day, translating into a decrease from about 28,000
ddpm to 6455 ddpm over the course of six months.
O’Hare (1980, personal communication from Andy O’Hare to Linda
Yates; notes on file in the University of Kentucky Center for Applied
Energy Research’s Applied Petrology Laboratory) investigated decreases
in thermoplasticity due to (1) oxidation in conjunction with grinding
(more surface area leading to more oxidation) vs. (2) the increased
packing density of fine particles leading to a reduced plasticity. Running
different combinations of − 60-mesh (− 250 μm) coal both with and
without the − 325-mesh (− 44 μm) fraction, he determined that the in­
clusion of the fines decreased the plasticity owing to the greater packing
density. Senftle and Davis (1982) made a similar observation in an
experiment with PSOC-1099 and PSOC-1116. Several caveats must be
considered in the O’Hare experiment: (1) the ASTM D2639 standard
calls for a − 40-mesh (− 400 μm) sample; (2) the importance of the
packing density diminishes after the coal begins to soften and should be
irrelevant once the coal is melted (assuming that the coal actually ach­
ieves full melting); and (3) the petrography, both macerals and minerals,
of the test fractions were not considered. For this and any other similar
comparisons, point 3 may be the most important consideration because
the elimination of a certain particle-size range implies that the samples
(in this case the comparison of two discrete particle-size ranges), albeit
of the same rank, are different (see section 3.1.3). The latter consider­
ation may offset his determination that the packing density may be more
important than the oxidation associated with a reduction in particle size.
Todoschuk and Giroux (2019, 2020) investigated the oxidation of
coal at the industrial scale. The ArcelorMittal Dofasco steel plant in
Hamilton, Ontario, cannot receive coal during the winter months due to
the closure of the Welland Canal (Lake Erie to Lake Ontario). Conse­
quently, their coal stockpile is subject to weathering. To understand the
coal properties and to anticipate problems with coke manufacture, they
run weekly, at least, Gieseler and Arnu tests on each of their component
coals. While the maximum Gieseler fluidity and Arnu dilation were good
predictors of the coal’s plastic properties and its ability to coke, the
temperature range between the softening and coking points proved to be
a more reliable and robust measurement. Appalachian and Western
Canadian coals of the same rank exhibited slightly different properties
owing to the higher inertinite content of the Canadian coals.
3.3.3. High-rank (Rmax > 1%) relationships among rank parameters
Aside from the complications of maceral variations, coal rank, as
defined by a limited range of chemical parameters from the proximate or
ultimate analysis, suffers from ratio correlation problems. Within the
proximate analysis (moisture, ash, volatile matter (VM), fixed carbon
14
International Journal of Coal Geology 263 (2022) 104120
(FC)), fixed carbon is defined as 100% minus the other parameters.
Nevertheless, the use of VM + FC (on the dry, ash-free basis VM + FC =
100%) as a statistical parameter has been observed in the coal science
literature (Ürünveren et al., 2020). Within the ultimate analysis (mois­
ture, ash, C, H, N, Stotal, O by difference), the use of total S rather than
organic S is a complication for all coals (Given and Yarzab, 1978); for
high-S coals, a negative Oxygen, which is not a valid value, can result
from the calculations.
Within the higher rank coals, the progressive loss of functional
groups through the progressive aromatization of the coal results in a
high C content and a decrease in H and N (the elements discussed in this
paragraph are on the dry, ash-free basis). With a constant sum of 100%,
this means that the concentrations of the elements are autocorrelated, as
seen in the relationship between C and H (Fig. 10). The relationship
between H and N, relatively minor contributors to the coal by this rank
(H + N < 8.5%), is more diffuse owing to the broader distribution of N in
medium and low volatile bituminous coals (Fig. 11). Hydrogen and the
vitrinite maximum reflectance are highly correlated among the high-
rank coals, at least until about 5% Rmax (Fig. 12). Weisenberger et al.
(2020) noted inflections in the relationship between both H (daf) and
vitrinite maximum reflectance versus thermal diffusivity and thermal
conductivity in the lower H (<2.3%) and higher Rmax (>5.15%) ranges
((Fig. 13) and Silva et al. (2020), via High-resolution transmission
electron microscopy (HRTEM), observed changes in vitrinite structure in
>5% Rmax vitrinite versus lower reflectance anthracitic vitrinite. Li et al.
(2019, 2020a, 2020b), Zhang et al. (2021), and Yuan et al. (2022)
described the structure of anthracites and the natural transition to
graphitic structures. The changes in vitrinite structure and properties
described by Weisenberger et al. (2020) and Silva et al. (2020) could be
related to the noisier >5%Rmax vs. H relationship. Additional studies
would be necessary to explore this trend more fully. In any case, the
inter-relationships between coal rank parameters enforces the advan­
tage of relying on multiple tools in the assessment of rank.
3.3.4. Implications for coal preparation
Several rank related parameters are summarized in Table 7 after
Aplan (1993), who modified and supplemented data from an essay by
Given (1984). These have implications for coal cleaning, especially for
froth flotation, which is based on a coal’s hydrophobicity, and dew­
atering. The rank of coal dictates the requirements for flotation reagents
as the natural hydrophobicity of coal for the vitrinite maceral peaks at
about the medium or low volatile bituminous rank (Arnold and Aplan,
Fig. 10. Relationship between C and H (both, dry, ash-free basis) for Penn­
sylvania, West Virginia, and Virginia coals with Rmax > 1%. Data tied to vit­
rinite reflectance is from the Penn State University database. Additional data for
Pennsylvania anthracites is from Bragg et al. (1998).
J.C. Hower et al.
Fig. 11. Relationship between H and N (both, dry, ash-free basis) for Penn­
sylvania, West Virginia, and Virginia coals with Rmax > 1%. Data is from the
Penn State University database.
Fig. 12. Relationship between H (dry, ash-free basis) and vitrinite maximum
reflectance (%Rmax) for Pennsylvania, West Virginia, and Virginia coals with
Rmax > 1%. Data is from the Penn State University database.
1989). Understanding the surface charge of coal and the minerals in the
coal has implications for thickening and dewatering coal and refuse to
meet specifications for utilization or for disposal, respectively.
The Hardgrove grindability index and friability also change with
rank. For coal preparation, this affects the size distribution of coal
feeding a plant and the potential for degradation within a plant. As
previously stated, the maceral analysis also affects the Hardgrove
grindability index. This combination of rank and maceral content are
critical in plant circuit design. Higher levels of fusinite in higher rank
coals can create a situation with excessive fines and the need for
considerable capacity in the fine’s circuits. Fusinite is much less hy­
drophobic than its associated vitrinite (Arnold and Aplan, 1989),
resulting in reduced floatability for high fusinite content coals such as
those in British Columbia, Canada (Arnold, personal experience).
The size distribution of a plant feed, perhaps the most important
analysis required when designing a coal preparation plant, determines
the loadings in each plant circuit. Underestimating the fines content of
the preparation plant feed (and the breakage in a plant) results in un­
dersized screens, fine coal cleaning operations, fine dewatering circuits,
tailings thickeners, and fine waste disposal requirements. This will
15
International Journal of Coal Geology 263 (2022) 104120
greatly influence the overall capacity of the preparation plant, as the
feed rate to the plant will need to be decreased to allow the fines pro­
cessing and handling equipment to operate properly. Undersized screens
will not allow the efficient removal of fines from the coarse coal cleaning
circuits, and these coarse coal cleaning circuits will not operate at top
efficiency with excessive fines present.
It is always best to determine the plant feed size distribution and
washability from a sample of run-of-mine coal, if possible. However,
many preparation plant designs must rely on core samples, typically
either 50 mm or 200 mm in diameter. These diameters certainly limit
the evaluation of top size in the run of mine coal or the feed to the plant
and the washability analysis for any coarser coal fractions.
The techniques used to determine size distributions and washability
in preparation plants from core data give mixed results. Many coal
properties need to be considered, including rank (related to the Hard­
grove grindability index (HGI)), maceral or coal type, mineral content,
and mining or handling operations. The development of empirical tests,
which include drop shatter techniques and dry and/or wet tumbling
techniques, needs to consider coals that cover ranges in these properties.
Many investigators have evaluated these procedures, including Wilson
and Leonard (2000) in the US and the Australian Coal Association
Research Program (ACARP) (Swanson and Fletcher, 1993) evaluations
of parameters for breakage tests. ACARP specifically uses drop shatter
tests followed by both dry and wet tumbling tests. These have been
successful in determining run of mine size distributions and washability
analyses for Australian coals. Butcher (1985) and others in Canada and
Leach et al. (2007) for South African coals have evaluated the ACARP
procedures for coals in those countries.
The application of the ACARP procedure to all coals should be
considered carefully based on the previously mentioned coal parame­
ters. As early as 1963, Harrison (1963) evaluated breakage tests on Il­
linois (US) coal and related breakage and size distributions to the
petrology of the coal. Harrison’s (1963) conclusions should be consid­
ered for coals having differing maceral and coal type analyses. He
concluded that lithotypes influence breakage, with fusain bands and
partings resulting in preferential breakage. The thickness of vitrains and
the type of breakage will influence the fines content. Liptinites tend to
stay in the coarse fractions, while fusains without mineral matter break
easily and report to the finest sizes. Harrison’s final conclusion encom­
passed the main topics of this paper: a knowledge of petrographic
composition, rank, and chemical composition is vital to optimize coal
preparation and utilization.
These points have implications for particle breakage in mining,
handling, and processing. It is important to not just analyze coal simply
for overall chemical composition or maceral content. The combinations
of the lithotypes of vitrain, clarain, durain, and fusain will impact the
breakage. It is important to study the core samples at this level as well.
This analysis could determine any changes that need to be made to the
ACARP drop shatter and dry and wet tumbling procedures to provide a
sample that represents the run of mine coal.
Indeed, shortcomings are given for the ACARP technique that imply
that coal producers need to develop their own specific treatment pro­
cedures to better predict the plant feed size distribution and washability
for coals with differing properties. In the 1993 ACARP Size Distribution
Workshop, the shortcomings, quoted after their list, were noted by
Swanson and Fletcher (1993). These were also related to the main topics
of this paper: coal type (petrography) is not considered, Hardgrove
grindability index correlations are uncertain, and clay content will also
affect results. In addition, the mining, handling, and preparation pro­
cesses are not considered.
Leach et al. (2007) began using the ACARP procedure for South Af­
rican coals to provide a size distribution and washability analysis for the
design of new coal preparation plants. However, they determined that
modified times for the dry and wet tumbling steps were required since
the standard breakage tests did not reflect the breakage in the run of
mine coal in South Africa as seam blasting is used prior to mining. Once
J.C. Hower et al. International Journal of Coal Geology 263 (2022) 104120

Fig. 13. Thermal diffusivity (mm2/s) and thermal conductivity (W/m-K) vs, vitrinite maximum reflectance (%Rmax) for Pennsylvania anthracites (after Weisenberger
et al., 2020).

Table 7
Approximate values of some coal properties in different rank ranges (dry, mineral matter free basis unless noted) (Aplan, 1993, modified and expanded from the
original tabulation of Given, 1984).
Property Lignite Subbit. High Volatile Bituminous Bituminous Anthracite

C B A Medium Low
Volatile Volatile

Equilibrium moisture, % 35 16–29 12 7 4 3 3 5.5

Volatile matter, % 33–62 60 34–52 36–50 31–50 20–31 10–20 <10
Calorific value, moist mineral matter free, 7000 / 16.3 10,000 / 12,000 / 13,500 / 14,500 / 15,000 / 34.9 15,800 / 15,200 /
Btu/lb. / MJ/kg 23.3 27.9 31.4 33.7 36.7 35.3
%C, average 73 76 80 82 85 89 91 95.5
%C, range 66–76 71–81 76–84 79–85 83–89 86–92 87–92 92–97
%H 4.5 5 5.5 5.5 5.5 4.5 3.5 2.5
%O 25–16 25–11 18–8 13–7 13–4 4–3 3 2
%O as OH 11–7 9–5 9–4 6–3 6–2 3–1 3–1 1–0
%O as COOH 10–6 9–4 low Tr-? 0 0 0 0
Aromatic C atoms % of total C 50 65 ? ? 75 80–85 85–90 90–95
Ave. number of benzene rings/layer 1–2 ? 2–3 5? >25?
Reflectance, %, vitrinite 0.2–0.3 0.3–0.4 0.5 0.6 0.6–1.0 1.4 1.8 4
Plasticity and coke formation no no yes yes yes yes yes no
Hydrophobicity ←decreases ←decreases ←decreases ←decreases ←← maximum →→ decreases
Point of zero charge (PZC) pH 2 2 ←decreases ←decreases ←decreases 7–8 7–8 Variable
Density (He), vitrinite ←increases ←increases ←increases ←increases minimum greatly increases→
Surface area (CO2) m2/g 250 100–300 100–220 100–220 100–220 200–250 200–250 200–400
Hardgrove grindability index 35–50 40–55 45–80 45–80 45–80 70–115 70–115 25–50
Friability, avg., % 12 20–30 43 43 43 70 70 33

these modifications were made, the predictions for size distribution and
washability were improved significantly.
It is important to note that all of these size distribution analyses are
conducted using wet screening techniques. The use of wet screening
should also be applied when testing any bulk samples as dry fines can
cling to coarse particles. In addition, the presence of any clay minerals
will be better accommodated with wet screening techniques as the clay-
bearing rocks will break down during handling and processing. Some
techniques call for soaking the coal sample in water for several minutes
to mimic this breakdown in the plant. This will certainly be necessary in
considering the size distribution to commercial-scale beneficiation.
Another important aspect of this analysis is the presence of out of
seam dilution that may add to the mineral content of the run of mine
coal through the mining of any floor or roof rock or partings. In surface
mines, it is easier to limit the amount of out of seam dilution that will
enter the preparation plant. However, for any underground mines, it will
be important to add additional mineral matter to the projections for size
distribution and washability.
4. Summary
Coal analyses are the foundation of coal science; without proper
analyses, the science cannot stand and without coal science there will be
unfortunate and costly consequences. A thorough, well-vetted analysis
scheme provides the underpinning of everything from the execution of
an exploration program; to the marketing, beneficiation, and utilization;
to the development of new markets. Further, adherence to proper
analytical methods demonstrates the reliability of the product and the
company or researcher behind the product and offers legal protection in
the event of problems with the coal.
Part of this foundation is also the understanding of the analyses and
their meaning in the broader concept of coal quality. The analyses are
interconnected through the organic petrology, the mineral and
elemental analyses, and the determination of the coal rank by chemical
and/or petrographic means. No one analysis stands alone. None of the
analyses are just numbers on a laboratory report or a spreadsheet.
Together, the components of a thorough analytical scheme create a
synergy in which the prospects for coal utilization can be realized.

16
J.C. Hower et al.
Declaration of Competing Interest
The authors declare no conflicts of interest.
Data availability
Data will be made available on request.
Acknowledgements
Over the course of the ca. 170 years of combined experience in coal
science between the authors, many people have influenced our views of
coal analyses. Other than his co-authors on this paper, among Hower’s
influences, he counts Norm Suhr, Alan Davis, and Peter Given at Penn
State; John Kuhn, Gerald Thomas, Shelley Hopps, and Tonya Morgan at
the Center for Applied Energy Research (CAER); Dave Robertson at the
University of Kentucky and later the University of Missouri; Bill Lloyd
and John Riley at Western Kentucky University (WKU) (Lloyd was at the
CAER prior to becoming a dean at WKU); Leslie Ruppert and Allan
Kolker at the U.S. Geological Survey; and Leroy Jacobs and Jane Thomas
of Wyoming Analytical Laboratories. On-going discussions, usually over
long distances, with Dal Swaine, Yakov Yudovich, Greta Eskenazy,
Shifeng Dai, Vladimir Seredin, and Colin Ward focused his views of coal
geochemistry and mineralogy. Ralph Gray influenced his studies of
Hardgrove grindability. Richard Winschel (CONSOL) and John Popp
(Alliance Coal and later at Natural Resource Partners) taught him the
importance of looking to the needs of industry, not just academia. Dis­
cussions with the many students (from high school through graduate
school), co-workers, and visiting scholars passing through his laboratory
developed the views of coal petrology and coal science seen in his
published work.
Finkelman benefitted from discussions with many USGS colleagues
including Irv Breger, Blaine Cecil, Ron Stanton, and Peter Zubovic,
collaborations with Harvey Belkin, Linda Bragg, Allan Kolker, Bill Orem,
Curtis Palmer, and Hal Gluskoter (Exxon and later at the USGS) had a
significant positive impact on coal research and his career. Others with
whom he benefitted from discussions and collaborations include Sergei
Arbuzov, Shifeng Dai, Dan Casagrande, Greta Eskanazy, Fred Price,
Glenn Stracher, Yugang Tang, Vladimir Seredin, and Baoshan Zheng. To
all these and more he owes a debt of gratitude.
Arnold also counts Peter Given at Penn State as one of her heroes. His
course on organic geochemistry especially related to sulfur in coal has
played a role in her understanding of the chemistry, especially the sur­
face chemistry, of coals. Dr. Arnold also had the opportunity to work
with Ralph Gray on coal petrology related to samples for her M.S. Thesis,
which was funded by US Steel Research– Coal froth flotation: The effects
of petrological and mineralogical constituents. She credits Alan Davis (Penn
State) for his contributions to that work as a member of her committee.
Her coal and mineral processing expertise was first developed through
course work and research at Penn State with Peter Luckie (“there is no
such thing as coal, there are coals”), Richard Hogg, and Leonard Austin,
along with adjunct faculty member Richard Klimpel. Her experience at
the Electric Power Research Institute’s Coal Cleaning Test Facility (later
CQ Inc.) shaped her knowledge of coal handling and blending related to
coal preparation. Above all, she credits her dedication to coal prepara­
tion, especially froth flotation, and to the mining industry to her mentor
and thesis advisor, Frank F. Aplan. Without his guidance in surface
chemistry related to clays and coals, she would not have developed the
understanding of the role of water quality and the importance of all
mineralogic and petrologic components in coals as well as their appli­
cation to other minerals.
While this essay was not directly supported by any of the US
Department of Energy’s CORE-CM projects, our work on several of these
projects and the conversations with individuals involved on all of the
projects has made us more fully appreciate the renewed interest in coal
and coal products as a source of critical elements and advanced
17
International Journal of Coal Geology 263 (2022) 104120
materials. We are keenly aware of the need for an understanding of the
complex properties of coal and the appreciation of the array of tests
employed to analyze those properties.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.coal.2022.104120.
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