Mud Volcano Biogeochemistry

Helge Niemann

Contents
1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
2 Hydrocarbon Emissions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
3 Geochemical Forcing . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
4 Research Needs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9

Abstract
Mud volcanoes are frequently encountered geo-structures at active and passive
continental margins. In contrast to magmatic volcanoes, mud volcanoes are
marine or terrestrial, topographic elevation built from vertically rising fluidized
mud or mud breccia. Commonly, these structures have a crater, hummocky rim,
and caldera. Mud volcanism is triggered by various geological processes which
lead to a high pore fluid pressure at great depth, sediment instabilities, and a
subsequent discharge of mud, fluids, and gases such as hydrocarbons (mostly the
greenhouse gas methane). Although global estimates of methane emissions from
mud volcanoes vary over two orders of magnitude, mud volcanism could be an
important source for atmospheric methane. However, a substantial fraction of the
hydrocarbons are retained in the mud volcanoes surface sediments or, in the
particular case of marine mud volcanoes, are consumed by microbes in the water
column. In sediments, the upwelled hydrocarbons fuel a variety of free-living and

H. Niemann (*)
Department of Marine Microbiology & Biogeochemistry, and Utrecht University, NIOZ Royal
Netherlands Institute for Sea Research, ’t Horntje, the Netherlands
CAGE – Centre for Arctic Gas Hydrate, Environment and Climate, Department of Geology, UiT the
Arctic University of Norway, Tromsø, Norway
e-mail: [email protected]

# Springer International Publishing AG, part of Springer Nature 2018 1

H. Wilkes (ed.), Hydrocarbons, Oils and Lipids: Diversity, Origin, Chemistry and Fate,
Handbook of Hydrocarbon and Lipid Microbiology,
https://doi.org/10.1007/978-3-319-54529-5_28-1
2 H. Niemann

symbiotic, chemosynthetic communities that oxidize these with electron accep-

tors such as oxygen or sulfate from the water column or the atmosphere. The
activity of the chemosynthetic communities is regulated by the availability of
either electron donors (hydrocarbons) or acceptors which, in return, is determined
by mass transport processes. Most important in this context are the magnitudes of
upward advection of electron donors and the influx of electron acceptors due to
diffusion and bioirrigation.

1 Introduction

Mud volcanoes are geological structures bearing only little morphological resem-
blances to magmatic volcanoes. In contrast to true volcanoes which expel magmatic
material at plate boundaries and mantle plumes (Schmincke 2004), mud volcanoes
are formed by vigorous mud discharge that is often accompanied by fluid and gas
emissions commonly originating from a deep subsurface sedimentary sequence
(Brown 1990; Milkov 2000; Kopf 2002). Mud volcanoes have a long tradition of
scientific investigation and references were already made in historical documents
(e.g., “Naturalis Historia” by Pliny the Elder, first century AD). Nevertheless,
the diversity of mud volcano shapes as well geological causes responsible for
their formation leads to a variety of definitions and synonymous terms such
as mud volcano, mud pie, mud mound, and gryphon (among others). Hereafter, a
mud volcano is defined as a marine or terrestrial, topographic elevation built from
vertically rising fluidized mud or mud breccia (a mud matrix containing clasts and,
sometimes, rock fragments or evaporites originating from the geological section
through which the mud ascends; Norton 1917; Cita et al. 1981; Maignien et al. 2013;
Mazzini and Etiope 2017). Mud volcanism is caused by various geological processes
such as tectonic accretion and faulting, rapid burial of sediments due to slope failures
(olistostromes) or high sedimentation rates, and fluid emissions from mineral dehy-
dration as well as (true) volcanic and earth quake activities (Brown 1990; Milkov
2000; Kopf et al. 2001; Dimitrov 2002; Kopf 2002; Mellors et al. 2007; Manga et al.
2009). These processes can lead to an abnormally high pore fluid pressure and
sediment instabilities and consequently lead to the extrusion of mud, fluids, and
gases (usually through a central conduit) to the seafloor or earth surface (Fig. 1). A
crater or active center, hummocky rim, and surrounding caldera are common features
of mud volcanoes. However, the shape of the structure can range from amorphous
mud pies to conical formations, and their size varies from a few meters to kilometers
in circumference and a few decimeters to hundreds of meters in height. The viscosity
and density of the extruded material as well as the duration of eruption events and the
development stage of the edifice were identified as major factors determining the
shape of mud volcanoes (Lance et al. 1998; Murton and Biggs 2003; Stewart and
Davies 2006). In general, flat structures are composed of comparably liquid mud
matrixes, while high- and cone-shaped edifices are built of successively, super-
imposed flows of more viscous material. Mud volcanoes may thus erupt in regular
or irregular time intervals or emit mud, fluids, and gases continuously. In addition,
Mud Volcano Biogeochemistry 3

a b c d

continental slope

methane plume

chemosynthetic comunities

humocky rim

caldera

crater

central conduit

Fig. 1 Potential genesis of a gas emitting (marine) mud volcano. (a) High pore fluid pressure leads
to the formation of mud breccia at great depth where also gases (mainly methane) are produced.
(b) Overpressurized mud breccia and gases migrate along sediment instabilities to the seafloor
(c) which is eventually breached (d) and upheaved. (e) Scheme of the Haakon Mosby Mud Volcano.
At a “typical” mud volcano, mud and gases are transported through a central conduit and extruded
in a crater region. The crater is surrounded by a hummocky rim of displaced sediment material.
After an initial outburst and deflation of source material, a caldera (collapse structure) surrounds the
mud volcano. Surface sediments of mud volcanoes can support a wide range of free-living and
symbiotic, chemosynthetic organisms which oxidize the upwelled hydrocarbons and hydrogen
sulfide with oxidants such as oxygen, nitrate, or sulfate from the water column. Giant sulfide-
oxidizing bacteria forming white mats on the seafloor and symbiotic tube worms colonizing the
seafloor in meadow- or bush-like aggregations are prominent examples of chemosynthetic com-
munities, which are visible for the naked eye. a–d source: ARCHIMEDIX, e Sabine Lüdeling,
MedienIngenieure Bremen

they may also become inactive when the source of gas expansion and fluid flow stops
(Planke et al. 2003; Mazzini et al. 2009), but also new structures evolve such as the
terrestrial LUSI mud volcano in 2006 (Mazzini et al. 2007; Karyono et al. 2017).
Three types of mud volcano activity are distinguished (Dimitrov 2003 and references
therein):
4 H. Niemann

1. Lokbatan-type: This type of mud volcanism was named after the Lokbatan Mud
volcano, Azerbaijan. Lokbatan-type mud volcanoes are characterized by violent
outbreaks and long phases of dormancy.
2. Chikishlyar-type: Calm, relatively weak, and continuous venting of gas, water,
and mud are typical for this type of mud volcano.
3. Shugin-type: This type of mud volcanism is transitional between the other types,
characterized by long periods of weak activity interrupted by eruptive events.
Dimitrov (2003) suggested that this type of mud volcanism is the most common.

This distinction is based on terrestrial mud volcanism, which has been investi-
gated for a comparably long time. In some cases, also historical documents can be
used to infer the mode of activity (Aliyev et al. 2002). In contrast, most oceanic mud
volcanoes were discovered and investigated in the last decade, when appropriate
high-resolution geophysical tools became available to science which can resolve a
few m of difference in height above- or belowground. However, from the bathymetry
and sub-bottom structure, it cannot be resolved what activity type a particular mud
volcano may represent because eruptive events could be separated by (longer)
periods of dormancy (Feseker et al. 2009, 2014). In addition to the temporal
heterogeneity of activity, visual investigation of submarine mud volcanoes by
towed video cameras, submersibles, or remotely operating vehicles showed that
mud volcanism is also spatially diverse (Niemann et al. 2006b; Sauter et al. 2006,
Sahling et al. 2009). In general, a mud volcano has an active center above a central
conduit which is usually marked by steep temperature gradients, and seepage rates
decrease toward the periphery. However, the active center may not always be the
geographical center, and the activity may not follow a concentric arrangement. Our
knowledge about mud volcanoes in general and specific structures in particular is
therefore very sketchy.

2 Hydrocarbon Emissions

The processes leading to mud volcanism on the continents as well as at active and
passive continental margins are generally related to fluid and gas flow. Subsurface
muds and shales in mud volcano-hosting regions often contain high amounts of
methane and other hydrocarbons of thermogenic and/or microbial origin. Conse-
quently, mud flows can be accompanied by vigorous gas expulsions, which may
even ignite in contact with the atmosphere in terrestrial systems (Milkov 2000; Kopf
2002; Charlou et al. 2003; Somoza et al. 2003). Good examples for violent gas
emissions from such structures are the terrestrial Lokbatan and the deepwater
Haakon Mosby Mud Volcano. Since the early nineteenth century, the Lokbatan
Mud Volcano has erupted more than 20 times, sometimes very violently with flames
reaching more than 500 m height (Aliyev et al. 2002; Mukhtarov et al. 2003).
At Haakon Mosby, a gigantic methane plume of about 600 m was visible on echo
sounder systems during several cruises, and jets of methane emitted from the
seafloor were observed during submersible dives (Vogt et al. 1997; Sauter et al.
Mud Volcano Biogeochemistry 5

2006). The annual methane discharge from Haakon Mosby was estimated with 8–35
Mmol (0.1–0.5 Gg) of which free gas accounted for 60–90% (Niemann et al. 2006b;
Sauter et al. 2006). About 650 to 900 terrestrial mud volcanoes are known (Kopf
2003), but global estimates for marine mud volcanoes range between 800 and
100,000 (Milkov 2000; Dimitrov 2002, 2003; Kopf 2003; Milkov et al. 2003).
For submarine mud volcanoes, it is often not known if and when these structures
emit methane. As a result, global assessments of methane emissions from mud
volcanoes vary considerably. It has been suggested that terrestrial and shallow-
water mud volcanoes contribute between 2.2 and 6 Tg year
1 of methane to the
atmosphere (Dimitrov 2003; Milkov et al. 2003) and that 27 Tg year
1 of methane
may escape from deepwater mud volcanoes (Milkov et al. 2003). Revised estimates
of the total methane emission from mud volcanoes range between 35–45 Tg year
1
(Etiope and Milkov 2004) and 30–70 Tg year
1 (Etiope and Klusman 2002) and –
when using only known structures and correcting for the size of the edifice – between
0.3 Tg year
1 (Kopf 2003) and 1.4 Tg year
1 (Kopf 2002). In comparison to the
annual methane emissions to the atmosphere (526–852 Tg year
1, Kirschke et al.
2013), mud volcanism may consequently be an important source for atmospheric
methane. Nevertheless, a substantial fraction of methane released from marine mud
volcanoes is probably consumed by aerobic methanotrophic bacteria (See Chapters
on aerobic methane oxidation in Vol. 2 ▶ “Microbial Utilization Of Hydrocarbons,
Oils And Lipids” of this edition) in the water column (Reeburgh 2007), though their
activity can be very low (Damm and Budéus 2003). This might be related to current
dynamics and/or water column stratification regimes, which were found to cause
spatiotemporal heterogeneity of aerobic methane oxidation at other methane seeps
(Steinle et al. 2015, 2016).

3 Geochemical Forcing

In surface sediments of mud volcanoes, potential electron donors such as hydrocar-

bons and hydrogen sulfide from deeper sediment layers meet electron acceptors such
as oxygen, nitrate/nitrite, oxidized metals, and sulfate, which are formed in surface
sediments or originate from the water column or atmosphere. In such redox transi-
tion zones, mud volcanoes were found to support a wide range of free-living and
symbiotic chemosynthetic organisms utilizing the subsurface energy sources (also
known as “geofuels”) (Fig. 1). Thereby, chemosynthetic organisms reduce the efflux
of reduced molecules to the hydro- and atmosphere (See Chapters on hydrocarbon
and sulphur oxidising microbes in Vol. 2 ▶ “Microbial Utilization Of Hydrocarbons,
Oils And Lipids” of this edition) (Olu et al. 1997; Joye et al. 2005; Alain et al. 2006;
Niemann et al. 2006a, b; Jørgensen and Boetius 2007; Knittel and Boetius 2009).
Furthermore, chemosynthetic communities can also serve as an important food
source for other marine organisms (Niemann et al. 2013). The most important
metabolic pathways are methanotrophy (anaerobic oxidation of methane, AOM;
and aerobic oxidation of methane, MOx), anaerobic and aerobic degradation of
hydrocarbons, thiotrophy (sulfide oxidation), and in some systems also iron
6 H. Niemann

oxidation (Omoregie et al. 2008). The distribution of chemosynthetic communities

strongly depends on the availability of electron donors and acceptors, which in
return is regulated by physical mass transport processes and biological activities
(de Beer et al. 2006; Niemann et al. 2006b; Lösekann et al. 2007, Soetaert et al.
2012). Advection accounts for the majority of upward transport of electron donors
from deeper sediment layers, while diffusion and bioirrigation are responsible for
most of the influx of electron acceptors from the atmosphere or the water column
into the mud volcano sediments.
Advective transport at mud volcanoes is in the form of mud, fluid, and free gas
flow (see Sect. 1) (Fig. 1). Direct measurements of advection are scarce (Linke et al.
1994; Brown et al. 2005; Sauter et al. 2006; Mazzini et al. 2007, Feseker et al. 2009,
2014). In particular, rates of free gas and mud flow are poorly resolved. For gas flow,
this may improve in the future as a result of new echo sounder tools allowing to
quantify gas bubbles in the water column (Schneider von Deimling et al. 2007;
Ostrovsky et al. 2008; Nikolovska et al. 2008; Muyakshin and Sauter 2010; Veloso
et al. 2015) Also, the effect of mud and free gas flow on the distribution of
chemosynthetic communities is mostly unknown. Fluid flow rates, on the other
hand, can be modelled from geochemical pore water gradients and heat flow
measurements, which allows for a comparably high temporal and spatial resolution.
Recorded values for fluid flow at active mud volcanoes are typically a few centime-
ters to several meters per year (Table 1). Except for the spatial and temporal
heterogeneity of mud volcano activity, advective pore water transport is a linear
process, and the advective flux (Ja), i.e., the amount of pore water solute crossing a
given area per time, is determined by the flow velocity (va) and the concentration (C)
of the solute:

J a ¼ va C (1)

(note that C has to be corrected for porosity – ϕ).

The underlying mechanism of diffusion is Brownian motion (Einstein 1905),
which, for biogeochemical reactions, can be simplified to the heat-induced, non-
directional movement of atoms/molecules in water. Diffusive transport can be
illustrated by assuming two spatially separated entities in sediments or the water
column with high and low concentrations of a given solute. The dissolved atoms/
molecules will move randomly between both units. But more atoms/molecules will
move from the unit of high concentration than from the unit of low concentration.
This consequently leads to a net transport to the unit of low concentration until both
units are equal in concentration. From this simple example, it is apparent that the
concentration difference is an important factor determining diffusive flux. The
second important factor is the net velocity of the movement. However, in contrast
to the linear mode of advective flow, diffusion is random. A diffusing atom/molecule
will not move in one direction but, in a simplified manner, forward and backward.
As a result and when considering a large number of atoms/molecules, the mean
travelled net distance (L) increases only by the square root of time (t):
Mud Volcano Biogeochemistry 7

Table 1 Fluid flow velocities (va; in cm year
1) at selected submarine mud volcanoes
Structure Location va Ref.
Haakon Mosby Barents Sea 40–600 de Beer et al. 2006, Kaul et al. 2006
Dvurechenski Black Sea 8–25 Aloisi et al. 2004
Capt. Arutyunov Gulf of Cadiz 10–15 Hensen et al. 2007
Mound 12 East Pacific 10 Linke et al. 2005
Atlante West Atlantic <1–10 Henry et al. 1996, Olu et al. 1997
Kazan Mediterranean 4 Haese et al. 2006

pffiffiffiffiffiffiffiffi
L¼ 2Dt ; (2)

where D, the diffusion coefficient, is a compound-specific constant usually

expressed in cm2 year
1 (note that D has to be corrected for temperature (T) and
ϕ), e.g., Boudreau 1997). Equation (2) has the rather counterintuitive implication that
the net velocity of diffusion (vd) decreases with increasing diffusion distance:
 
vd ¼ L t ¼ 2D L
(3)

Important electron donors and acceptors at mud volcanoes only need about a ms
to travel a distance of 1 μm but already a day for 1 cm and some month for 10 cm
(Table 2)! The diffusive flux (Jd) is hence determined by the concentration difference
(dC), the diffusion distance (dx), and D. Assuming steady-state conditions, i.e., none
of the factors determining the flux changes over the time period of measurement, Jd,
can be calculated according to Fick’s first law of diffusion (Fick 1855; Berner 1980;
Boudreau 1997):

J d ¼ D  dC =dx (4)

For short distances and high concentration differences (i.e., a steep concentration
gradient – dC/dx), diffusion is hence an efficient transport mechanism.
The transport of electron acceptors due to bioirrigation activities is a known but
poorly quantified phenomenon at marine mud volcanoes (Haese et al. 2006;
Niemann et al. 2006b; Soetaert et al. 2012) and other types of cold seeps (Haese
2002; Treude et al. 2003; Cordes et al. 2005, Fischer et al. 2012). Many mud
volcanoes host large populations of chemosynthetic megafauna such as tube
worms and bivalves mining for sulfide and methane. Thereby, oxygenated and
sulfate-rich sea water is flushed through, e.g., burrows into deeper sediment layers
where it becomes available for free-living chemosynthetic microbes. Furthermore,
some thiotrophic tube worms are known to secret sulfate actively through posterior
body parts to fuel sulfate reduction in the sediment. The flux via bioirrigation (Jb) is
solely dependent on the faunal (pumping) activity as well as their extension into the
sediment. Jb can be calculated from the concentration differences of nonreactive
tracers such, as e.g., silica or bromide (Wallmann et al. 1997; Haese 2002; Haese
et al. 2006):
8 H. Niemann

Table 2 Diffusion distance (L ) in relation to diffusion time (t) and velocity (vd) of methane,
sulphate and oxygen in sediments at a “typical” submarine mud volcano (T ~3  C; 80%)
methane sulphate oxygen
L t vd t vd t vd
1 μm 0.8 ms 40 km 1.3 ms 24 km year
1 0.7 ms 48 km year
1
year
1
1 mm 13.2 min 40 m year
1 22 min 24 m year
1 11 min 48 m year
1
1 cm 22 h 4 m year
1 36 h 2.4 m year
1 18 h 4.8 m year
1
10 cm 92 d 0.4 m year
1 150 d 0.24 m year
1 76 d 0.48 m year
1
1m 25 year 4 cm year
1 41 year 2.4 cm year
1 21 year 4.8 cm year
1
10 m 2.5 4 mm year
1 4.1 2.4 mm 2.1 kyear 4.8 mm
kyear kyear year
1 year
1
100 m 250 0.4 mm 413 0.24 mm 209 0.48 mm
kyear year
1 kyear year
1 kyear year
1
1 km 25 40 μm 41 24 μm year
1 209 48 μm year
1
Myear year
1 Myear Myear

J a ¼ αhðC 0
C x Þ (5)

where α is the nonlocal exchange coefficient (in year
1, dependent of faunal

community composition and density) which has to be modelled from pore water
concentration profiles. h is the thickness of the zone in which the transport occurs,
and C0 and Cx are the concentrations of the tracer in the bottom water and at depth,
respectively. The few estimates available to date indicate that fluid flow due to
bioirrigation may be 2–3 orders of magnitude higher than the purely physical
transport (Wallmann et al. 1997; Haese et al. 2006). Because of the different
modes and magnitudes of transport, the redox transition zones are found at various
depths in mud volcano sediments ranging from the sediment surface to meters below
sediment surface. For sediments devoid of burrowing megafauna, the depth is
determined by the velocity of upward fluid flow (de Beer et al. 2006).

4 Research Needs

Due to the high spatial and temporal variability of fluid flow at mud volcanoes, and
the many questions remaining to the functioning and interaction of geophysical
forces as drivers of mud volcanism, there are still many open questions as to the
trigger, sources, and change of their activity and longevity. For submarine mud
volcanoes, an important issue is the relation between gas and fluid flow, heat
transport, and the formation/dissociation of gas hydrates as well as its consequences
for the distribution and activity of faunal communities. Furthermore, the magnitude
and spatial heterogeneity of hydrocarbon emission from marine mud volcanoes are
not well constrained, and we know very little about the dynamics of microbial
degradation of hydrocarbons in the water column above active mud volcanoes.
One of the best studied mud volcanoes in this regard is the Haakon Mosby Mud
Mud Volcano Biogeochemistry 9

Volcano, which has been chosen as a site for long-term observation of geophysical
and biogeochemical processes of mud volcanism. Specifically for terrestrial mud
volcanoes, very little is known about the occurrence, phylogeny, ecology, and
activity of chemosynthetic communities.

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