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Medical Mineralogy and Geochemistry: An Interfacial Science

Article in Elements · December 2007

DOI: 10.2113/GSELEMENTS.3.6.381

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 Medical Mineralogy
and Geochemistry:
An Interfacial Science
Nita Sahai*
DOI: 10.2113/ GSELEMENTS .3.6.381

M
edical mineralogy and geochemistry is a highly interdisciplinary area these other research areas focus on
the organic and biological aspects
of research where the complexity of minerals and mineral surface of human health, with minimal
reactivity in the human body is emphasized. Research in this field appreciation for the richness and
will lead to an understanding of the biogeochemical processes responsible for complexity of the contributions of
inorganic solid phases in these
medical conditions, both normal and pathological, that involve the interaction processes. Seemingly trivial exam-
of dissolved inorganic species and bioorganic molecules with minerals. In this ples are provided by the terms sili-
article, I highlight some fundamental concepts and challenges in this endeavor, cosis and calcification of bones and
arteries, which are widely used in
and the subsequent articles provide overviews of specific topics. the medical literature but do not
specify the mineral actually
KEYWORDS: reaction mechanisms, mineral–water interface, biomolecules,
involved. These processes might
biominerals, bioceramics, speciation more appropriately be called quartz-
icosis and phosphatization
WHAT IS MEDICAL MINERALOGY (Glimcher 2006). Thus, I distinguish MMG from the related
AND GEOCHEMISTRY? research fields by the former’s emphasis on the critical role
The connection between human health and the environment played in the human body by naturally occurring inorganic
we live in has been appreciated by all cultures throughout solid phases, that is, by minerals, amorphous solids,
human history. The physical manifestation of this connec- nanocrystals, and nanoclusters. For brevity, and with apolo-
tion has been dramatically demonstrated by the toll on gies to mineralogists, in the subsequent discussion the term
human life caused by volcanic eruptions, earthquakes, hur- “mineral” will include true minerals and biominerals
ricanes, landslides, tsunamis, and other natural disasters, (which are composite materials), as well as inorganic amor-
and these effects may be considered under the term “geol- phous solids, nanoparticles, and nanoclusters.
ogy and human health.” Among the best-known examples
are the Vesuvian eruptions of 79 AD that buried Pompeii The range of issues includes the medical condition involving
and Herculaneum in Italy and the tsunamis represented in the specific mineral, the affected tissue or organ, the etiology
the beautiful nineteenth century Japanese woodblock of the condition, exposure pathways, geospatial relation-
prints by Katsushika Hokusai. ships, pathogenesis, the controlling equilibria and reaction
mechanisms, and the cure. In order to solve the pathological
Chemical links between the environment and human health, case, it is often necessary to understand the normal process.
however, tend to be more difficult to identify and understand For instance, understanding osteoporosis and normal bone
in terms of the biogeochemical mechanisms by which they mineralization go hand in hand. MMG, in other words,
affect human health. Lead (plumbum in Latin) in drinking- deals not only with medical problems but also with normal
water pipes (hence “plumbing”) and in pewter wine goblets physiological processes involving minerals and inorganic or
has been identified only in recent times as the source of organic species in the fluid phase.
widespread poisoning in ancient Rome. The importance of
such links is captured in classic textbooks on bioinorganic A partial list of MMG research topics is provided by the
chemistry (Fraústo da Silva and Williams 1991; Williams and recent volume 64 of the Reviews in Mineralogy & Geochemistry
Fraústo da Silva 1996). The field of medical mineralogy and series (Sahai and Schoonen 2006) and by the articles in this
geochemistry (MMG) focuses on understanding the equilibria issue of Elements. For example, the toxic and carcinogenic
and reaction pathways involving normal and pathological potential of mineral dusts inhaled into the lungs is related,
interactions of inorganic and organic chemical species in gas in part, to biochemical reaction mechanisms involving iron
or aqueous phases with naturally occurring, inorganic solid and reactive oxygen species that occur at the mineral sur-
phases within the human body. face (Fubini et al. 1987; Castranova et al. 1997; Huang et al.
2006; Schoonen et al. 2006; Fubini and Fenoglio 2007 this
Medical mineralogy and geochemistry as broadly described issue). Neurodegenerative disorders such as Guam amy-
here overlaps considerably with other areas of research, otrophic lateral sclerosis/parkinsonism-dementia complex
such as bioinorganic chemistry, biochemistry, epidemiology, (ALS/PDC) and Alzheimer’s disease (AD) may involve mis-
etiology (cause of disease), biomineralization, and biomaterials folding of specific proteins and, in some cases, are specific
(FIG. 1). The field also has connections to the huge biological to certain geographical locations such as Guam, West New
research areas of genetics, molecular biology, and cell biol- Guinea, and the Kii Peninsula of Japan (Gadjusek 1963; Garruto
ogy. The overlap is intentional and necessary, but many of and Yase 1986; Perl and Moalem 2006). An MMG approach
combined with geochemistry could also help address the
* Dept. of Geology & Geophysics, Dept. of Chemistry etiology, pathogenesis, geospatial foci, and potential
University of Wisconsin–Madison genetic–environmental interactions involved.
1215 W Dayton St, Madison, WI 53706, USA
E-mail: [email protected]

ELEMENTS, VOL. 3, PP. 381–384 381 D ECEMBER 2007

 substrate in the stability and functioning of SLBs is only
now beginning to be studied. With their extensive knowl-
edge of oxide surface chemistry, geochemists could poten-
tially contribute significantly to this field.
As a final example, drugs and viable cells encapsulated
within oxide nanoparticles have been proposed for drug
delivery and cancer therapy (Livage and Coradin 2006).
Understanding the synthesis, reactivity, and cytotoxic and
carcinogenic potential of nanoparticles are all within the
scope of MMG (Livage and Coradin 2006).

SOLUTION CHEMISTRY: SPECIATION

AND BIOORGANIC MOLECULES
An accurate consideration of equilibria and reaction path-
ways between minerals and dissolved species—as well as
meaningful definitions of the terms bioavailability, bioac-
cessibility, biosolubility, and biopersistence for risk assess-
ment of toxic and carcinogenic compounds—requires an
accurate knowledge of aqueous speciation in the particular
FIGURE 1 Schematic diagram illustrating the overlap between med-
fluid. Excellent examples are provided in reviews of biolog-
ical mineralogy and geochemistry (MMG) and related
fields. Examples of MMG studies are also shown. Top, an elongated ical Al speciation (Martin 1991; Harris 1996; Stone 1997).
mineral fiber frustrates engulfment by a phagocyte (modified from Bice Solutions in different physiological environments vary in
Fubini, pers. commun.); left, molecular model of prion peptide terms of pH, ionic strength, and dissolved inorganic ionic
PrPsc(92-138) on montmorillonite surface (Chaperon, Charlet and concentrations, and the pH of some fluids even changes
Sahai, unpublished results); right, supported lipid bilayer at bioceramic
implant surface (modified from Kasemo 2002).
with conditions. Thus, gastric fluid varies between pH ~1.5
and 6.5 in the absence and presence of food; sweat pH
ranges from ~4 to 6.5; salivary pH changes from ~6.5 to 8 as
flow conditions change from low to high; interstitial
Prions are a type of misfolded protein that are the agents of
(between cells) blood plasma and extracellular lung fluid
transmissible spongiform encephalopathies (TSE) such as
have pH ~7.5, but extracellular lung fluid is slightly more
Creutzfeldt-Jakob disease and kuru in humans, mad cow
acidic at pH ~7; and macrophage lysosome has a low pH
disease or bovine spongiform encephalopathy, chronic
(~4.5) (Plumlee et al. 2006). To cite other examples, Na+, K+,
wasting disease in elk, deer, and moose, and scrapie in
and Cl- concentrations maintain osmotic balance across the
sheep (Prusiner 1982). The fate of prions, viruses, and other
cell membrane; in some cells, Ca2+ ions control the opening
proteins in the geological environment provides a fascinat-
of cell-membrane channels, thus regulating traffic across
ing and growing area of research (Bales et al. 1991, 1993;
the membrane; and trace elements such as Cu, Zn, and Mn
Schramm et al. 2006; Quiquampoix and Burns 2007 this
are usually involved in specific protein functions. Redox
issue; Charlet et al. 2008).
conditions also vary in different physiological environ-
The formation of bones, teeth, otoconia (calcite crystals in ments, from an oxygen partial pressure (pO2) of 0.132 atm
the inner ear for sensing gravity and acceleration), kidney in arterial blood to 0.02–0.05 atm in venous blood (Plumlee
stones, gout and gall stones, as well as the calcification of et al. 2006). Extremely toxic, reactive oxygen species (ROS)
vasculature present cases of normal and pathological bio- are generated inside immune system cells called leukocytes
mineralization (Glimcher 2006; Boskey 2007 this issue; in order to destroy pathogens such as bacteria, viruses, and
Wesson and Ward 2007 this issue). A combined approach inhaled dust particles. The concentration of ROS also
involving modern genetic, biochemical, spectroscopic, and depends on solution pO2, pH, etc.
microscopic methods of analysis, along with molecular
While the inorganic speciation is relatively well known in
modeling of proteins, peptides, and phospholipids, would
many cases, it is difficult to obtain information on the myr-
yield insight into the controlling mechanisms. The challenge
iad types of biological organic molecules and their concen-
in modeling reactions involving large mineral surfaces with
trations, which may also vary with time and conditions
biomolecules and water is the development of methods that
(e.g. the rate of physical exertion, time since eating, health
are computationally affordable yet accurate, especially for
status, and age of the individual). These bioorganic mole-
interfacial reactions (Harding and Duffy 2006).
cules can form complexes with ions, function in redox reac-
Related to bone and teeth mineralization is the area of bio- tions, and adsorb at mineral surfaces, thus affecting
materials synthesis for orthopaedic and dental implants. solution speciation as well as mineral surface reactivity.
The reactivity of oxide and silicate ceramic and composite One of the challenges in studying biomedical processes
biomaterials depends, in part, on the composition and from an inorganic physical chemistry perspective is the
structure of the ceramic, the rate at which it dissolves when existence of such gaps in our knowledge.
implanted in the body, and the cellular response elicited by
the ions leached from the bioceramic surface (Cerrutti and SIZE, HIERARCHICAL ARRANGEMENT,
Sahai 2006; Jones et al. 2007 this issue). The reactions AND TEMPORAL VARIATIONS
involved in the initial dissolution of the bioceramic when
implanted in vivo are very similar to silicate weathering in In addition to variations with time and conditions, bioor-
the geochemical environment! ganic molecules vary in size from several angstroms to tens
of nanometers. Further, bioorganic molecules are arranged
Supported lipid bilayers (SLB), as suggested by their name, at varying levels of organization, from dissolved enzymes,
are synthetic phospholipid bilayers deposited on oxide sur- vitamins, co-factors and other proteins to colloid-sized
faces and used as model cell-membranes (Cremer and Boxer polysaccharides, phospholipids, antigens, glycoproteins,
1999). Proteins may be embedded in the SLB that can bind etc., associated with the surfaces of micron-sized cells. For
to other proteins and molecules present in solution. Thus, example, a single molecule of aspartic acid is ~5Å long;
SLBs have potential applications as biosensors and in mak- dipalmitoylphosphocholine, a typical cell membrane–forming
ing biomaterials more biocompatible. The role of the oxide phospholipid, is ~3 nm in length; the infectious portion of

ELEMENTS 382 D ECEMBER 2007

a prion protein is estimated at ~10–30 nm; the core of apo- models for flow through porous media, may shed some
ferritin protein, within which ferrihydrite is located, has a much-needed light (Kufahl and Saha 1990; Dillaman et al.
diameter of ~6 nm, and the apoferritin cage itself is ~12 nm 1991; Hillsley and Frangos 1994).
across. Accordingly, the principles of solution chemistry, col-
loid and surface chemistry, and bulk materials chemistry Surface-controlled reaction mechanisms are also critical in
will need to be applied. some processes, as exemplified by the ROS and other gen-
erated on freshly fractured minerals in mining, blasting and
The mineral phases associated with biomedical processes construction activities or radicals created in the mineral due
also range in size and in hierarchical arrangement. For to the presence of ferrous iron or other impurities, as in the
instance, the calcium phosphate phase associated with mature case of anthracitic coal (Schoonen at al. 2006; Huang et a al.
bone is a non-stoichiometric, Ca-deficient, carbonate- 2006; Fubini and Fenoglio 2007). The interaction of soluble,
enriched hydroxylapatite and occurs as plate-shaped nano- acidic proteins with dissolved ions and mineral surfaces in
sized crystals 30–45 nm long and wide and ~2–3 nm thick. the nucleation and growth of biominerals such as apatite in
The crystals are arranged with their c-axes parallel to the bone and teeth, calcite otoconia in the inner ear, and the
long axes of collagen fibrils, and the fibrils themselves have pathological mineralization of calcium oxalate as kidney
a very particular three-dimensional arrangement. This spe- stones and of uric acid crystals in the joints in gout provide
cific, hierarchical arrangement of the organic collagen matrix additional examples of heterogeneous reaction mechanisms
and the inorganic calcium phosphate crystals gives bone its in MMG.
fabric and mechanical properties, while the small surface
area of the crystals imparts to them a high surface reactivity, ESTIMATION OF SURFACE AREA
which is required for a mineral that acts as a reservoir of cal-
cium (Glimcher 2006). Moreover, unlike many other bio- Although the importance of reactive surface area of minerals
minerals, bone is resorbed and continually “turned over.” is appreciated, the specific surface is operationally determined
Osteoporosis occurs when the rate of resorption is greater by a N2 or Ar gas adsorption isotherm such as the Brunauer-
than the rate of bone formation. Thus, the composition, size Emmett-Teller (BET) isotherm. Even this value, however,
and, possibly, even the precursor calcium phosphate phase may not accurately represent the actual surface area involved
associated with bone vary with the age of the bone and the in the reaction. For instance, the size of inhaled particles is
age of the individual. In other words, changes occur over an important factor in controlling whether they are cleared
space and time, so it is critical to understand that variations from the respiratory tract or whether they accumulate in
in the volume of tissue analyzed relative to the spatial reso- the lungs, where they may cause respiratory disorders and
lution of the spectroscopic or microscopic analytical method cancer over long periods of exposure. The aggregation of
could yield very different results (Glimcher 2006). smaller particles into larger ones may reduce the effective
surface area accessible to larger biomolecules, while smaller
In teeth, nanocrystals of apatite associated with collagen are inorganic ions such as H+ or metal ions may access the entire
found in the dentin, but enamel contains much larger surface area represented by the BET value. The amount of
(micron-sized) and better-organized apatite crystals (fewer adsorbed biomolecule per unit surface area will then appear
substitutions, vacancies, and other defects), which are asso- to be anomalously low. Similar considerations apply to
ciated with the protein amelogenin. Moreover, teeth are nanoparticles encapsulating drugs, genes, or viable cells for
not normally resorbed (excluding pathological formation of use as targeted delivery agents in the treatment of cancer
caries or tooth decay), suggesting different mechanisms of and other diseases.
growth compared to bone. It would, therefore, be simplistic
to state that our bones and teeth are composed of hydroxyl- THE TOOL KIT
apatite. It is crucial to recognize this complexity of biomin-
erals when trying to understand the reaction equilibria and From the preceding discussion, it is apparent that the med-
mechanisms involved in controlling their formation (and ical mineralogist and geochemist must use an impressive
destruction, in the case of bone). array of tools in order to analyze, characterize, and study
inorganic species, bioorganic molecules, and minerals in
aqueous solutions across a variety of spatial and temporal
REACTION KINETICS scales in controlled laboratory experiments. It is even more
The interactions of minerals with dissolved inorganic and challenging to make measurements in vivo. Geochemists
organic species occur dynamically, so it is important to con- and mineralogists are already skilled in dealing with similar
sider reaction rates and pathways. For instance, silicate bio- complexities in the geological environment and in the use
ceramics of specific chemical compositions dissolve when of advanced spectroscopic, microscopic, and solution analysis
implanted in bone in the body, with leaching of Ca2+ and methods, as well as quantum and classical approaches to
silicic acid from the implant and subsequent deposition of modeling reactions at the molecular scale. Collaboration with
a new layer of hydroxylapatite at the implant surface. This researchers in the chemical, biological, and biomedical fields
apatite layer provides a stronger bone–implant bond and is also inevitable in order to carry out the complementary
faster postsurgery recovery times. In this scenario, the rate and necessary genetic, cellular, and biomolecular studies.
at which blood plasma flows past a silicate bioceramic
orthopaedic implant may control the silicate dissolution THE MENTAL CHALLENGE
rate and the deposition rate of the hydroxylapatite layer,
thus affecting the quality of the bone–implant bond, the There are many intellectual challenges in the MMG field,
postsurgical recovery time, and the lifetime of the implant and I have attempted to address some of them above. I dis-
in the patient. Poiseuille studied blood flow in capillaries tinguish these from “mental challenges,” by which I mean
and veins as early as 1815, so one might imagine that the the effort required to establish such interdisciplinary col-
rate of blood flow should be well known by now. It may, laborations, find the appropriate research funding, and deal
therefore, be surprising to learn that this parameter is actu- with journal editors and reviewers who resist publishing the
ally very poorly known. Blood flow rates vary from one results of such work. In short, educational outreach must be
organ or tissue to another, with different types and levels of targeted not only at the general public but also at our own
activity, and with the age and health of the individual, and community of geoscientists and at the larger community of
the practical difficulties in measuring in vivo flow rates are chemists, biologists, and biomedical researchers. The task is
obvious. In such situations, fluid mechanics models, including difficult but not impossible, as evidenced by the existing
collaborations among biomedical researchers, clinical med-
ical practitioners, and certain geochemistry and mineralogy

ELEMENTS 383 D ECEMBER 2007

 groups in the United States and internationally; by forward- for developing an improved understanding of the reaction
looking organizations such as the Mineralogical Society of mechanisms that control normal and pathological responses
America (MSA) and its journals/journal editors at American to minerals in the human body. Advances can only be made
Mineralogist who are now beginning to accept manuscripts by creating a dialogue among biochemists, molecular biol-
in MMG. Equally important are the logistical and financial ogists, biomedical engineers, epidemiologists, biogeochemists,
support provided by the MSA, the Geochemical Society, and mineralogists, so that we may better understand each
and by specific programs within NSF, DOE, and the USGS other’s scientific dialects and share the insights gained. The
towards a Medical Mineralogy and Geochemistry short course following articles are a step in that direction, and I thank
in December 2006, and the growing number of books and the invited authors for their contributions.
conference symposia in this subject area in the past five years.
ACKNOWLEDGMENTS
CONCLUSION Funding was provided by a National Scientific Foundation
MMG is an interfacial science in at least two senses. First, CAREER Award – Geobiology and Low-Temperature Geo-
the reactions of interest involve biomolecule or cell surface chemistry program (EAR 0346689), American Chemical
interactions with mineral surfaces in aqueous solutions. Society Petroleum Research Fund (41777-AC2), and faculty
Moreover, MMG requires conceptual development and the “start-up” funds from the University of Wisconsin–Madison.
application of tools across the interface of different scien- I thank Profs. Clark Johnson, Alan Stone, John Valley, and
tific disciplines. The continued growth of medical mineral- my research group for their support and thought-provoking
ogy and geochemistry lies in characterizing mineral–solution discussions, and Dr. Prof. Mel Glimcher has been a source of
interactions at the nanoscale and in complex systems. The inspiration for the past several years as an example of what
interplay between experimental and modeling work is vital can be achieved by rigorous, interdisciplinary thinking. 

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ELEMENTS 384 D ECEMBER 2007

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