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The Formation of Manganese Dendrites as the Mineral

Record of Flow Structures

Chapter · January 1994

DOI: 10.1007/978-3-662-07304-9_23

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The Formation ofManganese Dendrites as the Mineral Record ofFlow Structures 307

Tbe Formation oí Manganese Dendrites as tbe

Mineral Record oí Flow Structures

Juan M. García-Ruizl, Fermín Otáloral, Antonio Sanchez-Navas2 &

3Francisco 1. Higes-Rolando
lInstituto Andaluz de Geología Mediterránea. eSte-Universidad de Granada.
Fuentenueva s/n. Granada 18002. Spain
2Departamento de Mineralogía y Petrología, Universidad de Granada.
Fuentenueva s/n. Granada 18002. Spain.
~epartamento de Química Inorgánica. Universidad de Extremadura.
Campus Universitario. Av. de Elvas s/n. Badajoz 06071. Spain.

Abstract. Manganese oxide pattems known as "pyrolusite dendrites" are explained as the
result of the mineral record of flow structures in porous media. This interpretation is
supported by a) ftactal characterization, b) Mn profiles across the mineral pattem and the
matrix rocks, c) structures reminiscent offlow pattem observed at the scale afilie grain
size ofthe matrix rocks, d) the lack oflong-range arder ofthe manganese oxide particles
and e) the existence of clays and quartz grains of colloidal size intimately linked to the
manganese particles. This interpretation also explains other ftactal and non-ftactal
pattems accompanying the beautiful treelike ftactal forms associated with these
manganese oxide pattems.

Introduction

As pointed out by Potter & Rossman (1979), pyrolusite dendrites is a somewhat

misleading llame for the well-known tree-like patterns formed by manganese
oxide mineral s displayed by alI Natural History museums. Because of their very
common occurrence, the knowledge of the genetic conditions of the manganese
and iron delimites would be of great practical interest in understanding
geological environments. Nevertheless, they are considered today to be rather
meaningless structures in the deciphering of geological environments, probably
due to the uncertainty of their genesis.
These amazing tree-like pattems of manganese dendrites are ftactal objects, i.e. scale-
invariant structures (Mandelbrot 1982). In fact, the non-trivial dilation symmetry ofthese
structures was suggested by Swartzlow (1934) sixty years ago when he realized that as
for megascopic observation, "the microscope reveals a more detailed splitting and
bifurcation afilie branches as well as more details afilie irregularities afilie edges". This
author suggested that dendrites are formed by distribution of suspended material due to
surface tension of evaporating waters in a epigenetic environment and Schoedler (1851
cited by Swartzlow 1934) pointed out that the pattem obtained by pressing a clay layer
confined between two glass microslides is reminiscent of dendrites. Recently, Chopard et
al. (1991) proposed that dendrites can be explained by a diffusion controlled reaction
 308 García-Ruiz, J.M. et al.

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0.0 03 0.6 0.9 1.2 1.5 18 2.1 2.4 2.7 3.0
In I

Fig. 1. Two digitized images of manganese dendritic pattems and their respective fractal
dimension obtained by fue box-counting method. The number ofboxes N(l) of sirle length
1 (pixels) is plotted versus 1. Sample a) is a dendritic pattem observed between two
laminae of [me-grained calcarenite from a flysh facies. Sample b) was found on a cracked
surface of a limestone. Deviation from fue straight line for low values of 1 in Fig lb are
interpreted as the effect of a inner cut-off at 1= 4.5 pixels.

mechanism. In ibis chapter we present data supporting the idea that manganese
and iron dendrites are the mineral record of flow instabilities. The driving force
for the flow may arise from any type of geological pressure gradient (for instance
in a hydrothermal field) but in the absence of such an external driving force for
injection, we propase a self-fed mechanism operating during early diagenesis and
we discuss the geological plausibility of ibis process.
 TI Fonnation ofManganese Dendrites as the Mineral Record ofFlow Structures 309

Pattern Characterization

We list below several observational and analytical facts relevant to "pyrolusite

dendrites". The following account was made based upon OuTobservations in
Sierra Elvira (Granada, Spain) and the flysch of Tarifa (Cádiz, Spain) and from
descriptions collected from the literature:
1. As stated above, pyrolusite dendrites are fractal objects. We have selected for
this study two dendrite-like patterns from Tarifa (southern Spain) and one
specimen kindly supplied by Prof. Michael Russell from the University of
Glasgow. They were digitized (512 by 512 pixels) and their fractal dimension
D was measured by the box-counting method (Barnsley, 1988; Vicsek, 1989)
using an ad hoc computer programo The D value obtained from these selected
specimens was 1.69:J:0.01 (Fig. la) which practically matches that for
Laplacian growth patterns. This result agrees with Van Damme's conjecture
(1989) that the general appearance of the manganese delimites could be the
result of either a diffusion limited aggregation (Witten & Sander 1983) or a
viscous fingering (Vicsek 1989) process. It is important to note that the above
specimens were selected by a previous visual inspection of the branching
structures and chosen as typical manganese dendrites. However, these
beautiful patterns are usually accompanied by othér fractals in which the
width of the branches and the branching behaviour are different and there are
even non-dendritic and non-fractal patterns associated with the beautiful
dendrites having a D value of 1.70. When the above procedure of selection is
eliminated, other values for D are currentIy found (Figure lb and Chopard et
al. 1991). It follows that any explanatory theory of manganese pattern
formation must explain such a diversity of patterns.
2. The infrared study carried out by Potter & Rossman (1979) showed that
"pyrolusite dendrites" are formed by different mineral associations, their
composition being neither singular flor universal. According to these authors,
ring-structure manganese oxides such as Romanecheita (Ba,H20)2Mn5010
and those of the Hollandite (Al-2Mn8016; with A mainly Ba,K,Na,Pb,
Mn4+,Mn2+) group are the main components of manganese dendrites.
Accessory minerals, mainly carbonates and silicates, are not characteristic
and in most of the cases are the same as those appearing in the host rocks.
These authors also find that iron oxides, when present, are minar
components. However, it has to be noted that non-crystalline iron minerals
also form dendritic tree-like patterns.
3. Manganese dendrites are low-crystallinity producís. This conclusion was
reached using several techniques. The black scab (crust) of manganese
mineral s forming the dendritic patterns was removed with a graver. The
collected material was placed on a micro-sample holder and then analyzed by
the X-ray diffraction powder method using filtered copper radiation. The
bands corresponding to manganese oxides are broad and were investigated at
310 García-Ruiz,lM. et al.

Fig. 2. High resolution electron microscopy view ofMn oxide particles showing the lack
of long-range order. The small particle showing lattice structure is a clay mineral with a
10 Á interplanar d-spacing.

slow exploration (static record during ten seconds for every 0.02°). When
attempting to obtain the degree of crystallinity using the line profile method
(Sanchez-Navas 1989) we found a crystallinity degree below the range of
resolution for that method. Therefore, in arder to obtain the coherent domain
size we used high resolution transmission electron microscopy. For this
purpose a suspension of the manganese mínerals was made and part of the
salid was dispersed on a holey carbon grid. A transmission electron
mícroscopeoperatedat 100kV, with an objectiveapertureof 90 !lIDwas used
in arder to add 000 transmítted beam and diffusion haloes. Low beam current
and mínimum exposure were used to avoid beam damage. The study showed
the absence of even short range three-dimensional periodical structure and the
clear colloidal nature of the Mn 'delimites (Figure 2). This means that the
kinetics of fue precipitation process has been fast and irreversible enough to
I

The Fonnation ofManganese Dendrites as the Mineral Record ofFlow Structures 311

prevent any internal reorganization of the growth units into a periodical

lattice.
4. In agreement with 3), scanning electron microscopy views (Figure 3) clearly
show that there is no crystallographic continuity in the precipitate. The
scanning electron microscope was operated at 30 kV in back-scattered
electron (BSE) mode and at 15 kV in secondary electron (SE) mode. To
ensure that we were scanning on the Mn oxides, we previously obtained a
BSE image of the specimen and then in the same place we turned to SE
images. Under SEM, the material forming the dendrite shows a colloidal
aspect and appears coating the mineral grains forming the matrix rock. Figure
3 also shows the cracked surface of the colloidal phase and its penetration
through intergranular joints.
5. Chemical analyses show that the Mn-concentration profile has a negative
gradient towards the host rock ayer a narrow band (a few micrometers) and
then attains a zero-value outside the precipitate. This information was
obtained by using a electron microprobe operated at 30 kV in BSE mode.
Figure 4 shows an example ofthe results reported above.
6. Manganese (and iron) dendrites appear on or inside many different types of
rocks, such as limestone and sandstone which suggests that the mineralogy of
the host rock is not a limiting factor.
7. Unlike desert varnish (Perry & Adams 1978, Carlton 1978) manganese
dendrites are commonly associated with cracks and sedimentary laminations,
or in general with quasi two-dimensional spaces.

Statement oí the Problem

Crystalline dendritic patterns are ordered fractals where the anisotropy of the
crystal structure governs the growth process. On the contrary, the so-called
random dendritic fractals are patterns where the fluid structure created in the
growth environment dominates crystal anisotropy. Therefore, it is a requirement
for the formation of the random dendrites that the kinetics of the phase transition
be rastel than the kinetics of the pattern formation and consequently, the
precipitation process must be a highly irreversible one occurring at conditions far
from equilibrium. It follows from this consideration that the precipitate formed
must be a low crystallinity product and that the whole growth pattern must lack
any geometrical relationships derived from the crystal structure. According to
observational facts 1) 3) and 4), the so-called manganese delimites belong to this
group of random fractals. Beyond systematic terminology, this distinction is
important in building a model of their morphogenetical mechanisms.
According to observational fact 1), some of the patterns displayed by
manganese delimites have a visual appearance and a fractal dimension which are
typical of those patterns derived from the Laplace equation. Today we know
312 García-Ruiz, 1M. et al.

Fig. 3. Scarnring electron microscopy views of Mn oxihydroxide :tnillerals into fue

intergranular space between two calcitic grains. To enSille fuat we were scanning the Mn
oxides, we obtained previously a back scatiered electron image of fue specimen (a) and
then we turned to secondary electron mode (b). Note fuat fue material for:tnillg the
dendrite (the whitish regions in 3a) has a colloidal appearance, showing the penetration of
fue Mn coated clay :tnillerals(top-Ieft part offue image) through intergranular joints.
 The Fonnation ofManganese Dendrites as fue Mineral Record ofFlow StrucÍlUes 313

several chemical and physical Laplacian growth processes (Vicsek 1989) but on1y
two of them are relevant to the formation of the Mn dendrites. The first of these
processes leading to two-dimensional objects with fractal dimension around 1.7
are irreversible growth processes governed by the diffusional control of the
nutrient phase, the so-called diffusion-limited aggregation (DLA) model (Witten
& Sander 1983). The second one is the viscous fingers (VF) process (Van
Damme 1989, Feder 1988, Vicsek 1989) which is known to produce DLA-type
parterns when the less viscous fluid invades a more viscous and non-Newtonian
one. Despite the fact that one of the most important findings of the new physics
of partero formation is that both DLA and VF display the same fractal dimension
and that they can be described by the same formal equations (Daccord et al. 1986,
Paterson 1984), it is important to note that from a phenomenological viewpoint,
DLA and VF are c1early difIerent. As suggested by Van Damme, to reveal the
origin of the pyrolusite dendrites reduces to the choice of one of these growth
phenomena.

DLA Versus VF Mechanism

A diffusion limited aggregation mechanism requires a starting point or linear

sink of energy to create a positive concentration gradient in the surrounding
fluid, which must be maintained throughout the growth process. As the driving
force for precipitation here is the redox potential leading Mn2+ ions to be
oxidized, such a condition is difficult to fulfil in geological environments.
Furthermore, because oí the two-dimensional geometry of the manganese
dendrite, the chemical potential gradient must be created and maintained in
planes parallel to the bedding surfaces where chemical gradients are difficult to
imagine in a geological environment which, in accordance with observational
fact 6), must be a general one. Another argument against the DLA-type
mechanism is the Mn concentration profile around the manganese oxide
precipitate (observational fact n° 5, Figure 4). It is c1ear that apure DLA
mechanism cannot explain a sharp negative concentration gradient outside the
dendrite. It must also be taken into account that the manganese dendrites are in
Tarifa flysch associated with cracks and always parallel to sedimentary
laminations. Consequently, the supply of Mn for such a mechanism should be
placed in the planar region between cracks, that is, into the region where no Mn
has been detected. Recently, Chopard et al. (1991) proposed a genetic
mechanism supported by fractal characterization and computer simulations. They
suggest a model in which two chemical species counterdiffuse and interact,
forming a precipitate after an induction time during which fue reaction produCíS
can still diffuse. Chopard et al. were able to obtain the different values of fractal
dimension they measured for natural dendrites but have not Jet translated fue
computer simulation into a geochemical model. The colloidal structure of the
"'

314 García-Ruiz, J.M. et al.

manganese oxides, the manganese profile concentration and the coexistence of

well-differentiated Mn and Fe dendrites seems difficnlt to explain by a reaction-
controlled precipitation with diffusional transporto Nevertheless, fue existence of
banding structures and isolated DLA-like clusters suggests that the Chopard et
al. model is also worth developing and that further studies on fue interaction
between physical instabilities and chemical reactions, that is, on the mineral
record of tlow patterns, are required. Another mechanism for the formation of
IIpyrolusitedendrites" was proposed by Swartzlow (1934) supported by laboratory
experiments of evaporation oí solutions under capillary torees. This mechanism
led to the type of pattem later studied by Hazlehurst (1941) who named
them"structural precipitates", which are interesting fractal aggregates but in OUT
opinion this evaporation mechanism cannot explain the observational facts
described above.
Viscous fingering is a pattem created when one tluid pushes another of higher
viscosity. The experimental device for studying two-dimensional viscous tlow is
the Hele-Shaw cell, Le., two glass plates separated by a gap typically of two
millimetres. Pionering experiments using this geometry were carried out by
Schoedler (1851 cited by Swartzlow 1934) to create air dendrites on cIays. The

Fig. 4. Mn profile across a dendrite obtained by electron microprobe chemical analysis.

Image width is around 70 J.1m.
 The Fonnation ofManganese Dendrites as fue Mineral Record ofFlow Stl1lctures 315

unstable interface between the two fluids bifurcates iteratively and therefore a
branched treelike structure reminiscent of manganese dendrites is obtained. The
main parameter controlling the interfacial pattern is the critical wavelength
b2
A= -*-, r
(jJ2 vV

where b and 'UJare the thickness and the width of the cell respectively, /l is the
difference in fluid viscosity, y the surface tension and V the velocity of the
injected fluido Today it is well known that viscous fingering have a fractal
behaviour when either the pushed fluid is a non-Newtonian one or it occurs luto
porous media. The type of fractal obtained depends on the applied flow cates and
the surface tension between the fluids (Lenormand & Daccord 1988). In porous
media, for very low values of V (or according to the previous equation, for larger
cell thickness) the fluid provokes an invasive percolation pattern with a
calculated fractal dimension D = 1.82 (Stauffer 1985). This pattern changes for
larger V values and after a crossover it becomes a fractal structure with a
D = 1.70, visually rerniniscent of DLA patterns (Lenormand & Daccord 1988).
This situation accounts very well for the geometrical properties of manganese
dendrites and their related structures. First, as described above, the fractal
dimension of typical Mn dendrites with a DLA-like morphology matches the one
expected for viscous fingers at high injection cates. Because of their beauty, Mn
dendrites are by far the best known patterns, but as stated in observational fact
nol, there are many other accompanying deposits which show other kinds of
patterns. Among them, invasive percolation and other patterns with fractal
dimensions and visual geometry ilifficult to explain by aggregation under
diffusional control are the most developed. These accompanying non-dendritic
patterns also can be explained by the viscous fingering mechanism. For a given
value of the injection flow, the parameter b may adopt small local changes but
large enough to produce the well-known change of regime provoked by variations
in V. Thus, the VF mechanism explains not only the beautiful treelike fractal
growth, but also the fractal and non-fractal patterns accompanying them, which
constitute the majority of manganese oxides. Unlike a DLA-type mechanism, the
viscous fingering approach is consistent with the manganese profiles across the
rack matrix containing the dendrites (observational fact nOS).Morec:vu, the SEM
views (Figure 3) of Mn dendrites suggest the existence of flo\.v patterns
surrounding the quartz and calcite grains of the rack and high resolution electron
microscopy shows that the Mn oxides closely adhere to clay particles a!¡d quartz
grains with a colloidal size which also suggests that a high viscosity colloidal
fluid was pushed by the Mn2+-rich injected fluido
The above discussion indicates a genetic mechanism for the formation of
manganese dendrites based on the mineralization of fluid structures. These fluid
structures occur during the invasion of sedimentary discontinuities or in general,
low attachment surfaces, by a fluid rising through cracks. The cracks (or
sedimentary laminations) are the conduits for Mn2+ and Fe2+, and the surfaces
316 García-Ruiz, J.M. et al.

oí low cohesion associated with them allow the development oí narrow gaps
which in many cases are the ¡oei íor pattern íormation. It is thereíore reasonable
to think that the existence oí rough impermeable pairs oí quasi-parallel surfaces
with a gap between them led to the íormation oí natural Hele Shaw cells.
The most intuitive source (and probably the most general Que) oí Mn2+ and
Fe2+ is the rige oí enriched solutions through the cracks. However, even in the
absence oí such an "external" source, we propase a genetic model using a self-íed
system that could account íor those geological scenarios where the existence oí an
external source oí manganese and iron solutions is difficult to support. We start
from a sedimentary material undergoing fracturing and compaction during early
diagenesis. It íollows that the host rock body to be injected must be at least
partially cemented and must preserve some bedding discontinuities. Also, the
injected fluid must displace another oí higher viscosity. Thus, the pattern
íormation should be generated during diagenesis, when a colloidal suspension
fills the interbedding laminations and cavities oí the sedimentary materials.
Under these conditions, the injection oí a rising solution rich in Mn2+ into a
natural Hele Shaw cell with rough surfaces containing a colloidal suspension wiIl
produce either the dendritic pattern with 0=1. 70, the invasive percolation pattern
wiili 0=1.82, or an intermediate pattern somewhere in the range between these
two values (Lenormand & Daccord 1988). The width and thickness oí the gap,
the roughness oí the surfaces, the pressure oí the injection fluid and the viscosity
oí the pushed fluid are the parameters controIling the great variety oí dendritic
and non-dendritic patterns observed in field studies and extending the range oí
possible D values. From the Eh-pH diagram íor Mn and Fe oxides, sediments
containing Mn4+ and Fe3+ compounds are reduced after being buried below the
anoxic-oxic interphase, and thus enriched in Mn2+ and Fe2+. Compaction and
cracking events provoke the upward injection oí these solutions which travel
through the cracks oí the sedimentary body and invade the upper a1ka1ineand
oxygenated zone, pushing the colloidal suspension that fills the sedimentary
laminations and consequentIy forming the dendritic patterns. Under such
conditions Mn2+ will precipitate as y-MnOOH (via Mn(OH>2 Mn304 plus 6-
MnOOH) and Fe2+ as y-FeOOH (Giovanoli 1980), both in the íorm oí low
crystallinity colloidal precipitates. The Mn3+ oxides are intermediate phases that
later convert to manganese oí higher oxidation states. This mechanism oí
íormation also explains the Mn-concentration profile obtained by electron
microprobe chemical analysis (Fig. 4), which has a negative gradient towards the
host rock ayer a narrow band oí a íew micrometers and attains a zero-value
outside the precipitate (a similar behaviour was íound íor Fe3+). Finally,
preservation oí the pattern can be produced by three mechanisms working
simultaneously: a) the cementation oí the host rocks which obstructs the
intraporous diffusion oí reducing agents, b) the plugging oí the system by the
íormation oí colloidal iron oxides, and c) the exhaustion oí the source oí reducing
agents. We have simulated this mechanism in the laboratory. A reservoir was
filled with a colloidal suspension oí yFeOOH and yMnOOH oxide partic1es.
The Formation ofManganese Dendrites as fue Mineral Record ofFlow Stl1lctmes 317

Three 5 mm thick glass disks were piled and the surfaces between them coated
with tooth paste, a material made 99% of colloidal silica. The pile was immersed
in the manganese solution and then a set of fractures was provoked by impacting
a hammer on the glass píleo After a couple of minutes, dendritic patterns were
observed in the silica thin layer (Fig. 5). A difIerent chemical system waS also
tried: the colloidal silica was replaced by a suspension of day with BaO solution
and the pile was now immersed in a true solution ofFe2+ and Mn2+. Details on
the similarities and difIerences of these laboratory model and real manganese
dendrites will be published elsewhere.

Fig. 5. Laboratory analogous ofthe self-fed mechanism proposed in this work.

Acknowledgements. This work was carried out under financial support from
CICYT Project PB92-1137 and the Junta de Andalucía. We acknowledge Tamás
Vicsek, Eugene Stanley and Michael Russell for their useful comments on this
work.
r 318 García-Ruiz,lM. et al.

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