Fe Isotope Behav During Melt Peridotite Interact in Supra Subd Zone Ophiol From PDF

Iron isotope behavior during melt-peridotite interaction in
supra-subduction zone ophiolite from Northern Tibet
Long Zhang1, Wei-dong Sun2, 3, Zhao-Feng Zhang1, Yajun An1, and Fang Liu1
1
State Key Laboratory of Isotope Geochemistry, Guangzhou Institute of Geochemistry, Chinese
Academy of Sciences, Guangzhou 510640, China
2
Laboratory for Marine Mineral Resources, Qingdao National Laboratory for Marine Science and
Technology, Qingdao 266237, China
3
Center of Deep Sea Research, Institute of Oceanology, Chinese Academy of Sciences, Qingdao
266071, China
Corresponding author: Long Zhang (zhanglong@gig.ac.cn),

Wei-dong Sun (weidongsun@qdio.ac.cn).
Key points:
1. High-Cr and high-Al dunites reflect contrasting melt-peridotite interactions in
supra-subduction zone ophiolite from Northern Tibet.
2. 56Fe of peridotite was not shifted during serpentinization and carbonation.
3. High-Al dunite has limited 56Fe that overlaps with harzburgite, while high-Cr dunite has
varying 56Fe that inversely correlates with FeO.
Abstract
Melt-peridotite interaction has the ability to modify 56 Fe of peridotite. However, iron
isotopic fractionation during melt-peridotite interaction is not well understood at present. In
this study, we present high-precision iron isotopic data for serpentinized and carbonated
peridotite from the Yushigou supra-subduction zone ophiolite in the North Qilian orogen of
northern Tibet, to provide insights into iron isotope behavior during melt-peridotite
interaction in the mantle wedge. High-Cr and high-Al dunites coexist with harzburgite in the
This article has been accepted for publication and undergone full peer review but has not
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doi: 10.1029/2019JB018823
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Yushigou ophiolite. The high-Cr and high-Al dunites were produced by interaction of
peridotite with boninitic melt and tholeiitic melt, respectively. Serpentinization and
carbonation have negligible influence on 56Fe of the peridotite. The harzburgite mostly has
56Fe ranging from -0.055 ± 0.029‰ to 0.056 ± 0.030‰, which overlaps with 56Fe of
abyssal peridotite. The high-Al dunite is enriched in FeO, but it has 56Fe (0.004 ± 0.034‰ ~
0.083 ± 0.064‰) similar to the harzburgite. In contrast, the high-Cr dunite displays a large
range in 56Fe from -0.173 ± 0.017‰ to 0.173 ± 0.057‰. Moreover, 56Fe of the high-Cr
dunite is negatively correlated with its FeO content, which is ascribed to kinetic iron isotopic
fractionation during melt-peridotite interaction. Surprisingly, distinct iron isotope behavior
during melt-peridotite interaction recorded by the Yushigou peridotite can well explain the
large variation of FeO and 56Fe in abyssal peridotite and mantle wedge peridotite on a global
scale.
1. Introduction
Subduction zones are one of the major loci for generation of large amounts of magmas
on Earth, as fluids released by subducting slab trigger hydrous partial melting in the
overlying mantle wedge (Spandler & Pirard, 2013). As a direct witness, mantle wedge
peridotite is thus a prime target for deciphering petrogenesis of melts and recycling of crustal
components in subduction zones. However, only rare direct samples of mantle wedge
peridotite are exposed in active subduction zones, including subarc mantle xenolith entrained
in arc magmas (Arai & Ishimura, 2008), and forearc mantle peridotite outcropped on
non-accretionary trench wall (Birner et al., 2017) or erupted in mud volcanos (Parkinson &
Pearce, 1998). In contrast, forearc mantle peridotite is widely distributed in supra-subduction
zone (SSZ) ophiolite from fossil suture zones (Dilek & Furnes, 2011, 2014). Therefore,
forearc mantle peridotite from SSZ ophiolite can provide another approach for directly
studying petrogenetic processes in the shallow mantle wedge.
Forearc mantle peridotite has complex petro-geochemical composition due to interplay
between melt extraction, fluid metasomatism, and melt refertilization (Parkinson & Pearce,
1998; Morishita et al., 2011a, b; Cao et al., 2016; Birner et al., 2017). Forearc peridotite in
active subduction zones is mostly harzburgite, with subordinate dunite and lherzolite (Arai &
Ishimura, 2008). It generally represents highly refractory residue of the mantle wedge after
extensive hydrous melting in the presence of slab-derived fluids (Parkinson & Pearce, 1998;
Arai & Ishimura, 2008; Birner et al., 2017). However, melt-peridotite interaction is suggested

to be responsible for the genesis of some dunites (Parkinson & Pearce, 1998; Pearce et al.,
2000; Morishita et al., 2011b). In contrast, melt-peridotite interaction is more observable and
diverse in SSZ ophiolite, with development of pyroxenite, dunite, and even chromitite
(Batanova et al., 2011; Morishita et al., 2011a; Pirard et al., 2013; Le Roux et al., 2014; Arai
& Miura, 2016). Besides the formation of replacive peridotite, widespread occurrence of
secondary clinopyroxene and enrichment of highly incompatible elements (e.g., light rare
earth elements) in depleted mantle wedge harzburgite is also frequently ascribed to minor
post-melting melt impregnation (Parkinson & Pearce, 1998; Batanova et al., 2011; Le Roux
et al., 2014). Therefore, melt-peridotite interaction is vital in dictating petrological and
geochemical variety in the mantle wedge.
Iron isotopes have emerged as a new tracer for studying mantle processes in recent years,
which can shed light on partial melting, redox condition, fluid metasomatism, and melt
percolation in the mantle wedge (Dauphas et al., 2017). Based on the observation that
mid-ocean ridge basalts (MORB) have higher 56Fe than arc magmas on average (Dauphas et
al., 2009; Nebel et al., 2015; Foden et al., 2018; Williams et al., 2018), it has been proposed
that the mantle wedge is either reduced with chondritic 56Fe (Dauphas et al., 2009), or
oxidized with low 56Fe (Nebel et al., 2015; Sossi et al., 2016; Foden et al., 2018). Therefore,
56Fe of mantle wedge peridotite is a key to explain the discrepancy in 56Fe between MORB
and arc magmas. Several studies have devoted to investigating iron isotopic composition of
SSZ peridotite, which have shown considerable variation in 56Fe up to 0.5‰ (Williams et al.
2004, 2005; Weyer & Ionov, 2007; Chen et al., 2015; Su et al., 2015; Xiao et al., 2016; Zhang
et al., 2019). In particular, the reported large variation in 56Fe of SSZ peridotite is mainly
ascribed to pyroxenite, dunite, and chromitite, namely the products of intense melt-peridotite
interaction (Williams et al. 2004, 2005; Chen et al., 2015; Su et al., 2015; Xiao et al., 2016).
In this regard, melt percolation probably has great influence on iron isotopic composition of
SSZ peridotite. However, iron isotope behavior during melt-peridotite interaction in the
mantle wedge is at present not well understood, hindering constraint on iron isotopic
composition of the mantle wedge.
In this study, we present petrological, geochemical, and iron isotopic data for
serpentinized and carbonated peridotite in the Yushigou ophiolite from the North Qilian
orogen, northern Tibet. The Yushigou ophiolite is a typical SSZ ophiolite that crops out
versatile residual and replacive peridotite (Song et al., 2013). The petrological and whole
rock element data are used to constrain protolith nature of the peridotite and

petro-geochemical changes during serpentinization and carbonation of the peridotite.
Melt-peridotite interaction is highlighted as the main cause of protolith diversity. Iron
isotopic composition of the peridotite is used to provide insights into iron isotopic
composition of the mantle wedge and iron isotope behavior during melt-peridotite interaction
in the mantle wedge. Ultimately, it is demonstrated that variation in iron isotopic composition
of mantle wedge peridotite is a direct result of complex and spatially restricted
melt-peridotite interactions that are likely acting in SSZ melting regions on a global scale.
2. Geological setting and samples

The North Qilian orogen is a typical oceanic suture zone in the northeastern margin of
the Qinghai-Tibetan plateau (Figure S1). It represents a subduction-accretion complex formed
due to oceanic subduction between the Alashan block and the Qilian block in the Early
Paleozoic (Song et al., 2013). The orogen is mainly composed of early Paleozoic ophiolite
complexes, blueschist- to eclogite-facies high-pressure low-temperature metamorphic rocks,
island arc volcanic rocks with granitic plutons, and Silurian flysch formations, which are
unconformably overlain by Devonian molasses and Carboniferous to Triassic sedimentary
covers (Song et al., 2013). Two separate ophiolite belts are distributed in the south and north
of the North Qilian orogen, respectively (Figure S1). Basaltic rocks from the south ophiolite
belt resemble MORB in geochemistry and are therefore suggested to be generated at mature
oceanic ridges (Song et al., 2013). Zircon in gabbros from the south ophiolite belt yields
U-Pb ages ranging from 550 to 496 Ma (Song et al., 2013). In contrast, the north ophiolite
belt is considered to be derived from a backarc basin, with gabbroic zircon yielding much
younger U-Pb ages of 490~448 Ma (Song et al., 2013).
This study focuses on the Yushigou ophiolite in the western part of the south ophiolite
belt (Figure S1). The Yushigou ophiolite suite occurs as nappes overthrusting onto the
Precambrian basement of the Qilian block to the south and bordering with Permian sediments
to the north. The ophiolite complex consists of ultramafic rocks, cumulate gabbros, pillow
basalts, and marine sedimentary rocks, which comprise a complete section of fossil oceanic
lithosphere. The fault-bounded ultramafic rocks are dominated by harzburgite, with
subordinate dunite, pyroxenite, and chromitite. Dunite and pyroxenite occur as dykes/bodies
in harzburgite, while chromitite is enveloped by dunite. Most peridotite is severely to
completely serpentinized, while fresh one is only exposed along the mountain ridge. In
addition, considerable peridotite is carbonated to varying extent, with outcrops of carbonated

serpentinite, talc-magnesite schist, and listvenite. Petrological and geochemical studies reveal
that fresh Yushigou harzburgite closely resembles highly refractory forearc mantle peridotite
with significant melt extraction and minimum melt refertillization, indicating SSZ origin of
the ophiolite (Song et al., 2009, 2013; Cao et al., 2015; Zhang et al., 2019).
In this study, serpentinized and carbonated peridotite samples were collected along the
mountain ridge in the headwater area of the west Yushigou creek. Fresh harzburgite,
non-carbonated serpentinite, and carbonated serpentinite occur consecutively along a ~300m
section, with non-carbonated serpentinite dominating over carbonated serpentinite and fresh
harzburgite. Non-carbonated serpentinite includes serpentinized harzburgite and
serpentinized dunite. Serpentinized harzburgite surrounds fresh harzburgite in the field. It is
generally dark, with coarse-grained relict orthopyroxene and shiny spinel observable in the
surface. Serpentinized dunite, with yellow green weathering surface, is present as a large
body between carbonated serpentinite and serpentinized harzburgite. Carbonated serpentinite
occurs as a raised lens between serpentinized dunite and listvenite. In contrast to darker
non-carbonated serpentinite, carbonated serpentinite is paler and whitish carbonate networks
are obvious in some samples.
3. Analytical methods
All the analyses were conducted at the State Key Laboratory of Isotope Geochemistry,
Guangzhou Institute of Geochemistry, Chinese Academy of Sciences. For bulk rock analyses,
rock powders were milled from fresh rock slabs without weathering crusts. Whole rock major
elements were analyzed by X-ray fluorescence spectrometry on glass disks prepared by
fusing rock powders with Li2B4O7. Loss of ignition (LOI), primarily ascribed to H2O and
CO2, was measured by weight difference following ignition of samples at high temperature.
Accuracy and precision were generally better than ±1% for major oxides. Whole rock trace
element concentrations were determined by a PerkinElmer Elan 6000 inductively coupled
plasma mass spectrometry on dilute HNO3 solution, after sample dissolution by concentrated
HF-HNO3-HClO4. Parr bombs were used to insure complete digestion of resistant minerals.
Accuracy and precision were commonly better than ±5% for most trace elements, but may
deteriorate to ±10~15% for some elements such as Nb, Ta, and rare earth elements (REE).
Major element compositions and back-scattered electron (BSE) images of mineral
phases in polished rock sections were obtained using a JEOL JXA-8100 electron microprobe.
The accelerating voltage, beam current, and beam radius were fixed at 15 kV, 20 nA, and 5

m, respectively. Counting times were 20s on peak and 10s on background for most elements.
Element contents were calibrated against silicate mineral standards and ZAF procedure was
used for correction of raw data. The analytical errors were usually within ±5%. In-situ Raman
spectra of minerals in polished sections were obtained by a WITec Alpha300R confocal
Raman microscope. A 488nm laser was used, with incident power of 5~10 mW and spot size
of <1 m. Raman spectra with wave numbers of 100~4000 cm-1 were accumulated by five
acquisition sequences of at least 5 seconds for each. Identification of Raman peaks, especially
serpentine polymorphs, was based on the RRUFF database (http://rruff.info) and literature
data (Rinaudo et al., 2003; Roumejon et al., 2015, 2018).
For iron isotope analyses, aliquots containing ~50 g iron were isolated from solutions
prepared for trace element analyses. The isolated solutions were transferred to Teflon beakers,
evaporated to dryness and dissolved in 6N HCl for chromatographic iron separation. Iron
purification was accomplished following well-established procedure of An et al. (2017),
which includes loading sample onto Bio-Rad AG1-X8 anion resin, eluting matrix with 6N
HCl, and collecting purified iron with 0.4N HCl and purified H2O. All solutions underwent
two passages through column chemistry to achieve high iron purity. Check on matrix washes
of each batch yielded >99.5% recovery rate for iron. Total procedural blank was <10 ng for
iron, which was negligible when compared with the amount of iron processed. Iron isotopic
ratios were analyzed by the sample-standard bracketing method with a Nu Plasma 1700
multi-collector inductively coupled plasma mass spectrometer, at a pseudo-high resolution
mode with a resolving power of >14000. Every sample was measured for three times and the
iron isotopic data are reported using the traditional  notation relative to the IRMM-14
standard:
iFe=[(iFe/54Fe)sample/(iFe/54Fe)IRMM-14-1]•1000, where i refers to 56 or 57.
External repeatability of δ56Fe for mono-elemental iron standard solution and international
geostandards is better than ±0.05‰ (2SD). International rock standards (including BHVO-2,
AGV-2, and W-2) and duplicate samples were also analyzed to monitor data quality.
4. Results
4.1 Petrography
The samples can be divided into non-carbonated serpentinite and carbonated serpentinite
based on the presence of carbonate or not. Judged from relict minerals and pseudomorph
textures, non-carbonated serpentinite includes serpentinized harzburgite and serpentinized

dunite. All three serpentine species, including lizardite, chrysotile, and antigorite, are
identified in the serpentinite samples. Under the microscope, lizardite is mostly yellow green
with pseudomorph textures (mesh or bastite), while chrysotile is usually whitish that occurs
as later veinlets. Antigorite only occurs in the carbonated serpentinite as radiating or
interpenetrating whitish blades. The serpentine polymorphs are further distinguished by their
different Raman spectra (Figure S2).
Relict spinel and orthopyroxene are common in serpentinized harzburgite (Figures 1a,
1b, and 1c), while relict olivine and clinopyroxene are rare (Figures 1a and 1b). Rare relict
clinopyroxene occurs as interstitial grains with cuspate endings, extending along boundaries
of neighboring relict orthopyroxene (Figure 1a). Relict olivine is replaced by mesh lizardite,
and highly fragmented orthopyroxene is replaced by bastite (Figures 1a and 1b). Relict spinel
is generally rimmed by a thin layer of magnetite. Mesh lizardite can develop core-rim texture
when no relict olivine is present (Figure 1c). However, mesh lizardite has occasionally
transformed into hourglass lizardite (Figure 1d). Small magnetite grains crystallize along the
boundaries of previous olivine and their trails depict triple junction texture of original
harzburgite (Figures 1b, 1c, and 1d). Bastite is generally more coarse-grained than mesh
lizardite (Figures 1b, 1c, and 1d), and cleavages of original orthopyroxene are sometimes
highlighted by lizardite with distinct extinction (Figure 1d). Chrysotile generally occurs as
later veinlets developing along lizardite boundaries or crosscutting lizardite (Figure 1d).
Serpentinized dunite is almost completely hydrated without relics of mantle minerals,
except for a few spinel grains. Compared with serpentinized harzburgite, serpentinized dunite
is characterized by the absence of bastite, and high amounts of opaque minerals (Figure 1e).
Lizardite is surrounded by magnetite arrays. Original spinel has mostly altered into
coarse-grained Cr-magnetite, which is generally surrounded by chlorite (Figure 1f).
Carbonated serpentinite mainly consists of lizardite, antigorite, chrysotile, magnesite,
spinel, and magnetite (Figure 2). Relict spinel rimmed by Cr-magnetite is common. Lizardite
is generally patchy without obvious pseudomorph texture (Figures 2a, 2b, and 2c), but it is
quite different from bastite. Antigorite mainly occurs as radiating blades in intimate
association with magnesite in the lizardite matrix (Figures 2a, 2b, and 2c). Chrysotile veinlet
crosscuts lizardite and is sporadically margined by magnesite (Figure 2a). One carbonated
serpentinite only contains interpenetrating antigorite with absence of lizardite and chrysotile
(Figure 2d). Magnesite is mostly fine-grained that occurs as connected networks, clustered
patches or disseminated grains.

4.2 Whole rock major and trace element compositions
Major and trace element contents of the serpentinized and carbonated peridotite are
listed in Table S1 and illustrated in Figures 3 and 4. The peridotite is characterized by high
SiO2, MgO, and FeO, and low Al2O3, Cr2O3, and CaO. Serpentinized harzburgite overlaps
with nearby fresh harzburgite in major oxides, except for its lower CaO (Figure 3c). Sample
17QH400 has lower FeO and Cr2O3 than rest of the samples. The serpentinized harzburgite is
compared with residues of anhydrous melting of fertile lherzolite KR-4003 (Herzberg, 2004)
and hydrous melting of silica-enriched mantle wedge HWM (Bénard et al., 2017) (Figures 3a,
3b, and 3e). In accordance with nearby fresh harzburgite, the serpentinized harzburgite has
higher SiO2 and lower Al2O3 than melting residue of KR-4003 at a given melting degree
(Figures 3a and b). Instead, it is generally consistent with melting residue of HWM.
Compared with serpentinized harzburgite, serpentinized dunite has lower SiO2 and higher
MgO, FeO, Al2O3, and Cr2O3. Furthermore, serpentinized dunite differs significantly from
melting residues of both KR-4003 and HMW. Carbonated serpentinite has slightly lower SiO2
and Al2O3 and higher MgO and FeO than serpentinized harzburgite. Moreover, it is generally
consistent with melting residue of HWM (Figures 3a, 3b, and 3e). Nevertheless, carbonated
serpentinite has higher Cr2O3 and CaO than serpentinized harzburgite (Figures 3c and 3d).
Serpentinized harzburgite plots slightly below the terrestrial array at the refractory end in the
plot of MgO/SiO2 versus Al2O3/SiO2 (Figure 3f). In contrast, carbonated serpentinite plots
above the terrestrial array, and serpentinized dunite deviate significantly from the terrestrial
array. Serpentinized harzburgite and serpentinized dunite experienced high degrees of
hydration with LOI of 12.62%~14.65%. Carbonated serpentinite contains more volatiles with
LOI of 18.14%~25.80%, which is mainly ascribed to the presence of carbonate.
The peridotite is depleted in most trace elements with respect to the chondrite and the
primitive mantle (Figure 4). Most serpentinized harzburgite samples have U-shaped REE
patterns that overlap with nearby fresh harzburgite (Figure 4a). They show a depletion in
middle REE (MREE) relative to light REE (LREE) and heavy REE (HREE), with (La/Sm)N
of 3.07~8.38 and (Gd/Yb)N of 0.09~0.20. Sample 17QH399 has low (La/Sm)N of 0.58, and
samples 17QH399, 17QH400, and 17QH412 have elevated MREE and HREE with (Gd/Yb) N
of 0.74~0.83. Serpentinized dunite has REE pattern generally similar to nearby fresh
harzburgite, except for lower HREE in two samples. In contrast with fresh harzburgite, some
serpentinite samples show conspicuous positive Eu anomalies. Carbonated serpentinite

generally has higher trace element contents than most non-carbonated serpentinite (Figures 4
and 5). It is enriched in LREE with (La/Sm)N of 4.81~13.95 and (La/Yb)N of 8.59~19.59,
respectively. Moreover, most carbonated serpentinite displays positive Cs, U, and Pb spikes
in the extended trace element diagram (Figure 4b).
4.3 Mineral major elements

Complete dataset for major element compositions of relict peridotite minerals in
representative samples is listed in Table S2, and data for spinel are illustrated in Figure 6.
Relict olivine, orthopyroxene, and clinopyroxene in serpentinized harzburgite has Mg#
(=Mg/(Mg+Fe)) of 0.911~0.916, 0.910~0.919, and 0.932~0.937, respectively. Relict spinel in
serpentinized harzburgite has Mg# and Cr# (=Cr/(Cr+Al)) of 0.403~0.595 and 0.613~0.738,
respectively. These values are similar to those reported for nearby fresh harzburgite. Spinel in
sample 17QH400 has lower Mg# than other samples. Spinel in serpentinized harzburgite with
elevated MREE-HREE has higher TiO2 than spinel in fresh harzburgite and other
serpentinized harzburgite samples. Mg# and Cr# of relict spinel in carbonated serpentinite
vary linearly from 0.338 to 0.596 and 0.726 to 0.845, respectively. Relict spinel in
serpentinized dunite has the lowest Cr# of 0.367~0.386 and highest Mg# of 0.651~0.676
among all samples. Spinel in both serpentinized dunite and carbonated serpentinite has higher
TiO2 than spinel in fresh harzburgite.
4.4 Iron isotopic composition

Iron isotopic data for the peridotite are reported in Table 1 and illustrated as a histogram
in Figure 7. Rock standards yield 56Fe in excellent agreement with recommended values
(Poitrasson & Freydier, 2005; Craddock & Dauphas, 2011; He et al., 2015). In addition,
duplicate analyses yield nearly identical 56Fe within errors. Serpentinized harzburgite has
relatively uniform 56Fe ranging from -0.055 ± 0.029‰ to 0.056 ± 0.030‰, but sample
17QH400 has higher 56Fe of 0.188 ± 0.039‰. 56Fe of serpentinized dunite is limited to
0.004 ± 0.034‰ ~ 0.083 ± 0.064‰. In contrast, 56Fe of carbonated serpentinite vary greatly
from -0.173 ± 0.017‰ to 0.173 ± 0.057‰.

5. Discussion
5.1 Melt-peridotite interaction in the ophiolite
Previous studies have revealed that Yushigou harzburgite is typical of highly depleted
forearc mantle wedge peridotite, with significant melt extraction and minor melt percolation
(Song et al., 2009; Cao et al., 2015; Zhang et al., 2019). Therefore, the closely associated
serpentinized and carbonated peridotite should have a similar SSZ origin. Nonetheless,
protolith nature of the serpentinized and carbonated peridotite varies greatly as revealed by its
diverse petrography and composition. The serpentinized harzburgite mostly has depleted
whole rock and relict mineral compositions overlapping with nearby fresh harzburgite
(Figures 3, 4, 5, and 6), implying the former as serpentinized counterpart of the latter. Fresh
and serpentinized harzburgite samples are enriched in SiO2 when compared with melting
residue of fertile lherzolite KR-4003 (Figure 3a), which is characteristic of mantle wedge
residual peridotite (Herzberg, 2004; Ionov, 2010; Bénard et al., 2017). Instead, they are
consistent with melting residue of HMW after 25~35% degrees of melt extraction (Figures 3a,
3b and 3e). Their origination from silica-enriched mantle wedge is also reinforced by their
lower MgO/SiO2 when compared with the terrestrial array (Figure 3f).
Despite overall depletion due to significant melt extraction, several lines of evidence
indicate that the serpentinized harzburgite has experienced melt refertilization. Clinopyroxene
should be eliminated from harzburgite after such high degrees of partial melting (Herzberg,
2004; Bénard et al., 2017). Therefore, presence of interstitial clinopyroxene in the
serpentinized harzburgite (Figure 1a) indicates its later-stage crystallization from percolating
melts. However, post-melting melt percolation should be limited as clinopyroxene is only a
minor mineral in the original harzburgite. Low REE contents of the serpentinized harzburgite
also indicate limited post-melting melt percolation, as small proportions of melts would be
adequate to modify the REE systematics of depleted harzburgite. Spinel in fresh and
serpentinized harzburgite has TiO2 generally comparable to spinel in modeled melting residue
(Figure 6b), which also implies minimal post-melting melt percolation. Three samples with
elevated Ti, MREE, and HREE (Figures 4a, 5a, and 5b) may have experienced more intense
interaction with melts, as reinforced by spinel with higher TiO2 in these samples than spinel
in fresh harzburgite.
Dunite in ophiolite can represent extreme mantle melting residue, cumulate of mafic
magmas or replacive product between residual peridotite and silica-unsaturated melts
(Kelemen et al., 1995; Suhr et al., 2003; Batanova et al., 2011; Pirard et al., 2013). The

serpentinized dunite in this study notably deviate from the melting trend of nearby
harzburgite (Figure 3), arguing against a residual origin. Cumulate dunite generally occurs as
layers in the crust-mantle transition zone along with cumulate gabbro and pyroxenite in
ophiolite (Pirard et al., 2013). However, the serpentinized dunite in this study occurs as a
large body adjacent to serpentinized harzburgite. Moreover, cumulate dunite generally has
Mg# significantly lower than harzburgite (Kelemen et al., 1995; Pirard et al., 2013; Su et al.,
2016), while the serpentinized dunite has Mg# only slightly lower than the serpentinized
harzburgite in Yushigou (Table S1). Therefore, a replacive origin is favored for the
serpentinized dunite. Considerable precipitation of low-Cr# spinel during melt percolation is
responsible for elevated Al2O3 and FeO of the serpentinized dunite (termed high-Al dunite),
though the spinel has mostly altered into Cr-magnetite and chlorite during serpentinization.
High Al2O3 and low spinel Cr# in the high-Al dunite thus imply its formation by interaction
of residual peridotite with Al2O3-rich tholeiitic melt.
Original mantle minerals and textures were mostly destroyed during serpentinization and
carbonation in the carbonated serpentinite. Nonetheless, bastite is lacking in the carbonated
serpentinite. This implies that lizardite in the carbonated serpentinite is exclusively
transformed from olivine, revealing that the carbonated serpentinite was probably also dunite.
However, the carbonated serpentinite is significantly different from the serpentinized high-Al
dunite mentioned above (Figures 3 and 6). It seems to comply with the melting trend of the
harzburgite, albeit with lower Al2 O3 and higher MgO than the harzburgite (Figures 3a, 3b,
and 3e). In addition, relict spinel in the carbonated serpentinite has higher Cr# than spinel in
the harzburgite (Figure 6). These observations intuitively demonstrate that the carbonated
serpentinite was originally residual dunite that is more depleted than the harzburgite.
However, the carbonated serpentinite has much higher Cr 2O3 and MgO/SiO2 than the
harzburgite (Figures 3d and 3f). Moreover, relict spinel in the carbonated serpentinite has
elevated TiO2 that is indicative of melt percolation. Therefore, the carbonated serpentinite
was also replacive dunite, but it should be produced by percolation of high-Cr# melt. In
contrast with overall FeO and Al2O3 enrichment in the high-Al dunite, FeO and Al2 O3 in the
carbonated serpentinite (termed high-Cr dunite) are not elevated except for one sample
(Figure 3e).
In summary, high-Cr and high-Al dunites coexist in the Yushigou ophiolite, which
represent distinct melt conduits in the forearc mantle. Similar observation of dunites with
diverse spinel Cr# has also been reported in the Izu-Bonin-Mariana forearc mantle (Morishita

et al., 2011b). Furthermore, this is also comparable to the common coexistence of high-Cr
and high-Al chromitite in worldwide SSZ ophiolite (Zhou et al., 1998; Rollinson, 2008; Arai
& Miura, 2016). Melt in equilibrium with the high-Cr dunite is probably boninitic, as only
spinel crystallized from boninite has similar high Cr# (Fig. 6b; Barnes and Roeder, 2001;
Morishita et al., 2011b). In contrast, melt in equilibrium with the high-Al dunite is probably
MORB-like, as spinel in the high-Al dunite has high Al2O3 content overlapping with spinel
crystallized from MORB (Barnes and Roeder, 2001; Morishita et al., 2011b). In subduction
zones, forearc basalts (FAB) erupted immediately after subduction initiation have
compositions similar to MORB (Regan et al., 2017). Therefore, the high-Al dunite was
probably produced by interaction of residual peridotite with FAB. FAB eruption is followed
by boninitic lavas and typical arc lavas (Regan et al., 2017). In this regard, high-Al and
high-Cr dunites in the Yushigou ophiolite reflect changing styles of spatially restricted
melt-peridotite interactions in the forearc mantle in a time sequence due to changing
compositions of percolating melts.
5.2 Negligible iron isotopic fractionation during serpentinization and carbonation of the
peridotite
The effect of serpentinization and carbonation on iron isotopic composition of the
peridotite must be evaluated before discussing iron isotope behavior during melt-peridotite
interaction. Serpentinization of the peridotite is characterized by nearly complete reactions of
olivine into lizardite and magnetite, and orthopyroxene into bastite (Figure 1). Carbonated
serpentinite is featured by widespread development of carbonate and antigorite (Figure 2).
The serpentinized harzburgite, except for its lower CaO, has major and trace element
compositions mostly overlapping with fresh harzburgite (Figures 3, 4, and 5), reinforcing that
serpentinization is nearly “isochemical” (Mével, 2003; Deschamps et al., 2013). Instead, the
carbonated serpentinite is enriched in nearly all trace elements when compared with the
harzburgite, even for fluid immobile elements such as HREE, Ti, Nb, Ta, and Th (Figures 4
and 5). Notably, the carbonated serpentinite is enriched in U, Sr, and Ca, which is
characteristic of carbonate-derived fluids (Figures 5c and 5e). As the carbonated serpentinite
was originally replacive dunite, it should have trace element pattern similar to the harzburgite.
Therefore, enrichment of trace elements in the carbonated serpentinite was due to
introduction of these elements by carbonate fluids, with the mobility of these elements
enhanced by complexing with carbonate anion (Hinsken et al., 2017; Qiu & Zhu, 2018).

Hydrothermal fluids are expected to leach isotopically light iron during serpentinization
(Severmann et al., 2004; Scott et al., 2017). For fresh Yushigou harzburgite with average FeO
of 8.01% and 56Fe of 0.002‰ (Zhang et al., 2019) and hydrothermal fluids with 56Fe of
-0.300‰ (Severmann et al., 2004; Scott et al., 2017), shift in 56Fe of the harzburgite cannot
be observed under present analytical precision (>0.050‰) unless the harzburgite loses >1.15
wt% FeO during serpentinization. However, the Yushigou serpentinized harzburgite has FeO
similar to fresh harzburgite, arguing against large-scale mobility of iron during hydration.
Instead, iron is redistributed between lizardite and magnetite at the micro-scale during
serpentinization. Therefore, 56Fe of the Yushigou harzburgite was not disturbed during
serpentinization at the hand specimen scale. This is also verified by similar 56Fe of the fresh
harzburgite and the serpentinized harzburgite, despite their significant contrast in hydration
extents (Figure 8a). Similar conclusion can be reached for the high-Al and high-Cr dunites as
their serpentinization conditions should be similar to the harzburgite. Previous studies have
also revealed that 56Fe of peridotite is not systematically modified during hydration
(Craddock et al., 2013; Su et al., 2015). Negligible iron isotopic fractionation during
serpentinization is ascribed to low iron mobility in serpentinization fluids, which can hardly
deplete peridotite in FeO unless water/rock ratio is extremely high (Scott et al., 2017).
Compared with relatively closed-system element behavior during serpentinization,
carbonation is characterized by open-system fluid influx with introduction of nearly all trace
elements (Figures 4 and 5). In this regard, the mobility of iron may have also been enhanced
by complexing with carbonate anion. As iron-bearing carbonate can display extremely
negative 56Fe (Belshaw et al., 2000; Johnson et al., 2008) and carbonate anion preferentially
complex with isotopically light iron in fluids (Schauble, 2004; Fujii et al., 2014), transfer of
minor iron in carbonate fluids to peridotite can have the ability to significantly lower the
56Fe of peridotite. Previous study on subducted Alpine serpentinite has shown that transfer
of 0.1~0.4 wt% iron in carbonate fluids to serpentinite can lower the 56Fe of serpentinite by
0.200~0.300‰ (Debret et al., 2018). However, most Yushigou carbonated serpentinite
samples do not have negative 56Fe (Figures 7 and 8). In addition, a few carbonated
serpentinite samples have 56Fe higher than the harzburgite. Both observations argue against
iron isotopic variation due to carbonation, as 56 Fe variation due to carbonation is expected to
shift unidirectionally. Moreover, there is no systematic correlation between 56Fe of the
carbonated serpentinite and index of carbonate-derived fluids such as Sr/Y and (La/Sm) N
(Figures 8b and 8c). Therefore, 56Fe of the high-Cr dunite is not modified during

carbonation. This indicates that the carbonate fluids were originated from iron-poor carbonate
such as calcite and dolomite, and little iron was introduced to the high-Cr dunite during
carbonation. Otherwise, the carbonated serpentinite should have low 56Fe if it was infiltrated
by carbonate fluids derived from iron-rich carbonate such as siderite and ankerite (Debret et
al., 2018).
Overall, 56Fe of the peridotite was not shifted during serpentinization and carbonation.
The peridotite retained its original 56Fe after melt extraction and melt percolation.
5.3 Iron isotope behavior during melt-peridotite interaction

The serpentinized harzburgite, except for one outlier, display a limited range in 56Fe
(Figures 7 and 8). In accordance with nearby fresh harzburgite (Zhang et al., 2019), the
serpentinized harzburgite has average 56Fe (0.011 ± 0.029‰) similar to abyssal peridotite
(with average 56Fe of 0.010 ± 0.007‰; Craddock et al., 2013). As the harzburgite is
representative of mantle wedge peridotite, it is inferred that residual peridotite in the mantle
wedge probably has 56Fe similar to abyssal peridotite. This is augmented by other studies on
arc peridotite that show similar distribution of 56Fe to that of abyssal peridotite (Figures 7
and 8; Weyer & Ionov, 2007; Su et al., 2015). Though minor melt percolated the harzburgite
at post-melting stage, it should have negligible effect on 56Fe of the harzburgite as the
percolating melt is limited in mass and does not have extreme 56Fe (Zhang et al., 2019).
Indeed, both 56Fe of the fresh and serpentinized harzburgite is not correlated with index of
melt addition (Figure 8c). Moreover, the three serpentinized harzburgite samples with more
intense melt percolation have 56Fe similar to other harzburgite samples.
In contrast with the harzburgite, the high-Cr dunite shows a large range in 56Fe, which
can be significantly distinct from that of abyssal peridotite (Figures 7 and 8). Previous iron
isotopic studies on SSZ replacive peridotite (dunite, pyroxenite, and chromitite) have also
shown considerable variation in 56Fe up to 0.5‰ (Williams et al. 2004, 2005; Chen et al.,
2015; Su et al., 2015; Xiao et al., 2016). The Yushigou high-Cr dunite is categorized into
three types based on distinct FeO and 56Fe (Figure 8d): (1) Three samples have FeO and
56Fe similar to the harzburgite; (2) Two samples, plus one serpentinized harzburgite, have
significantly higher 56Fe than rest of the samples. Moreover, these samples are characterized
by the lowest FeO among all samples; (3) One sample, with notably higher Al2O3, Cr2O3, and
FeO, has significantly lower 56Fe than rest of the samples. The high-Al dunite is termed as

type (4) dunite, with 56Fe similar to the harzburgite albeit elevated FeO. Surprisingly, this
categorization can well cover replacive peridotite with varying FeO and 56Fe from SSZ
ophiolite and abyssal basin in the literature (Figure 8d), indicating common mechanisms that
lead to distinct iron isotope behavior during melt-peridotite interaction in the mantle wedge
and the oceanic mantle.
Overlapping FeO between type (1) dunite and the harzburgite indicates that neither net
addition nor loss of iron occurred during the formation of type (1) dunite. In this regard, iron
isotopic fractionation can only occur through iron exchange between melt and minerals. 56Fe
of type (1) dunite is determined by 56Fe of olivine as spinel has negligible weight in whole
rock FeO and 56 Fe. Assuming Fe3+/ƩFe of 0.25 for boninitic melt (Brounce et al. 2015) and
equilibrium temperature of 1000 ºC, 56Fe fractionation between melt and olivine calculated
by force constant from Dauphas et al. (2014) is 0.07‰. Taken initial 56Fe of reacting
peridotite as average 56Fe of the fresh and serpentinized harzburgite (0.004 ± 0.014‰) and
initial 56Fe of percolating melt similar to average 56Fe reported for boninite (0.028 ±
0.008‰; Dauphas et al., 2009), 56Fe of resultant dunite should be limited to -0.042~0.004‰.
This variation can be hardly detected under current analytical precision. Furthermore,
calculated upper and lower limit 56Fe of the dunite is achieved under infinitely small and
great melt/peridotite ratio, respectively. Actual 56Fe of the dunite should be higher than the
lower limit. Overall, simple calculation shows 56Fe of type (1) dunite should not be
significantly shifted during melt percolation. Indeed, 56Fe of type (1) dunite remains the
same as that of the harzburgite.
Significantly lower FeO and higher 56Fe of type (2) dunite than the harzburgite
indicates preferentially loss of isotopically light iron. Three processes can deplete peridotite
in iron, namely partial melting, serpentinization, and melt percolation. Though partial melting
can deplete residual peridotite in FeO at extremely high melting degrees (Figure 4e), partial
melting cannot explain the high 56Fe of type (2) dunite as it can only lower 56Fe of residual
peridotite (Dauphas et al., 2009; Craddock et al., 2013; Foden et al., 2018). Moreover, type (2)
dunite is not residual dunite, as concluded in section 5.1. As discussed in section 5.2, iron loss
at extremely high water/rock ratio during serpentinization can explain the high 56Fe and low
FeO of peridotite, as only ferrous iron with low 56Fe is soluble in hydrothermal fluids (Scott
et al., 2017). However, a simple mass balance calculation as that in section 5.2 reveals
that >2.00 wt% FeO must be lost for 56Fe of the peridotite to be higher than 0.100‰, which

is apparently not the case for type (2) dunite. Therefore, iron loss during melt-peridotite
interaction with preferentially dissolution of isotopically light iron into melt conduits (Zhao et
al., 2012, 2015, 2017) is the most probable cause for elevated 56Fe and depleted FeO of type
(2) dunite. Similar to type (1) dunite,56Fe of type (2) dunite is also determined by 56Fe of
olivine. As discussed above, equilibrium iron isotopic fractionation between olivine and melt
does not have the ability to significantly modify the 56Fe of peridotite during melt
percolation. Instead, kinetic diffusion of iron during melt-peridotite interaction can cause
extremely large iron isotopic fractionation (Zhao et al., 2012, 2015, 2017). Therefore, type (2)
dunite with high 56Fe and low FeO experienced kinetic loss of iron during melt-peridotite
interaction.
Compared with the harzburgite, significantly higher FeO and lower 56Fe of type (3)
dunite indicates gain of isotopically light iron during melt-peridotite interaction. High FeO of
type (3) dunite is reflected by its high modal Cr-spinel up to 10%. Previous studies have also
reported that Cr-spinel/chromite-rich dunite and chromitite generally display significantly
negative 56Fe (Williams et al. 2004, 2005; Chen et al., 2015; Xiao et al., 2016). In this regard,
negative 56Fe of type (3) dunite is probably linked to oversaturation of Cr-spinel during melt
percolation. It has firstly to be estimated whether cumulate of olivine and Cr-spinel can
explain the low 56Fe of type (3) dunite, as olivine has 56Fe lower than basaltic melt at
equilibrium conditions (Dauphas et al., 2014), and Cr-spinel has even lower 56Fe than
olivine (Zhang et al., 2019). 56Fe fractionation between melt and olivine is taken as 0.07‰
as inferred in the above discussion. Equilibrium56Fe fractionation between melt and
Cr-spinel cannot be theoretically calculated as proper force constant for Cr-spinel is lacking.
However, Zhang et al (2019) shows that Cr-spinel in nearby fresh harzburgite is 0.05~0.10‰
lower than olivine in 56Fe. Cr-spinel in type (3) dunite is similar to Cr-spinel in the
harzburgite, with only slightly higher Cr#. Therefore, its 56Fe should also be 0.05~0.10‰
lower than that of olivine at equilibrium conditions. A large volume of melt is needed to
precipitate 10% Cr-spinel in type (3) dunite as basaltic melt has low Cr 2O3 in general. In this
regard, FeO and 56Fe of the percolating melt should not be significantly modified during
interaction with peridotite. A mass balance calculation shows that 56Fe of type (3) dunite
should be -0.08‰, assuming equilibrium cumulate of olivine and Cr-spinel during
melt-peridotite interaction. The calculated 56Fe is notably higher than actual value,
indicating iron isotope disequilibrium during melt percolation. Therefore, kinetic diffusion

with preferentially gain of isotopically light iron is the most plausible process responsible for
the isotope disequilibrium. In fact, scavenge of nutrients from a large system of wall rock is
necessary for the formation of chromite-rich dunite and chromitite (Arai & Miura, 2016). In
this regard, type (3) dunite is supplementary to type (2) dunite, with isotopically light iron
lost from type (2) dunite transported to type (3) dunite. Gain or loss of iron during melt
percolation in the dunite is thus controlled by the saturation of Cr-spinel or not.
Type (4) dunite is also enriched in FeO, but it has 56Fe overlapping with the harzburgite.
In this regard, type (4) dunite is similar to iron-enriched abyssal peridotite, as they have
overlapping 56Fe, and both are formed by interaction of peridotite with tholeiitic melt. As
type (4) dunite does not have abnormal 56 Fe, equilibrium process is probably adequate to
explain its 56Fe variation. Assuming Fe3+/ƩFe of the tholeiitic melt is similar to average
MORB (0.14; Zhang et al., 2018), 56Fe fractionation between melt and olivine calculated by
force constant from Dauphas et al. (2014) is 0.04‰ . If the tholeiitic melt has 56 Fe identical
to average MORB (0.105 ± 0.006 ‰; Teng et al., 2013) and reacting peridotite has initial
56Fe similar to the harzburgite, 56Fe of olivine should be limited to 0.004~0.064‰ under
equilibrium conditions. 56Fe of replacive high-Al dunite should be slightly higher than
constituting olivine as Al-rich spinel has 56Fe 0~0.05‰ higher than coexisting olivine
(Roskosz et al., 2015). Moreover, more precipitation of spinel would cause the dunite to be
more enriched in FeO and higher in 56 Fe, which can probably explain the crude correlation
between FeO and 56Fe in type (4) dunite.
Therefore, 56Fe of iron-enriched type (4) dunite and abyssal peridotite is dictated by
equilibrium crystallization of olivine and spinel. This indicates that kinetic diffusion of iron
was limited during the formation of type (4) dunite, which is in stark contrast to iron-enriched
type (3) dunite. The contrast is probably ascribed to distinct compositions of percolating
melts that precipitated high-Al spinel in type (4) dunite and high-Cr spinel in type (3) dunite,
respectively. For interaction of peridotite with high-Cr boninitic melt, spinel has a large
stability field and is easy to crystallize (Arai & Miura, 2016). Saturation of spinel would
cause strong chemical gradient in the melt conduit with diffusion of iron from a large system
(including surrounding dunite and country mantle peridotite) into crystallization site of spinel.
This can explain the large 56Fe variation due to kinetic iron diffusion in the high-Cr dunite.
In contrast, spinel has a much smaller stability field during interaction of peridotite with
low-Cr tholeiitic melt (Arai & Miura, 2016). In this regard, spinel crystallization and
associated iron diffusion should be much more limited when compared with that of high-Cr

melt. Therefore, 56Fe of resultant high-Al dunite cannot be significantly modified due to lack
of kinetic iron diffusion.
In summary, kinetic iron diffusion during interaction of peridotite with boninitic melt
can give rise to large 56Fe variation in high-Cr dunite. In contrast, 56Fe variation during
interaction of peridotite with tholeiitic melt is limited due to suppressed iron diffusion. In this
regard, melt composition is vital in controlling iron isotope behavior during melt-peridotite
interaction. Percolating of melts with different compositions is probably responsible for
variation of 56Fe and FeO in the mantle wedge and oceanic mantle on a global scale.
6. Conclusions
The Yushigou serpentinized harzburgite represents serpentinized counterpart of residual
forearc mantle peridotite that experienced large degrees of melt extraction and minor extents
of melt percolation. Instead, carbonated high-Cr dunite and serpentinized high-Al dunite were
produced by interaction of residual peridotite with boninitic melt and tholeiitic melt,
respectively.56Fe of the peridotite was not modified during serpentinization and carbonation.
The serpentinized harzburgite and high-Al dunite have 56Fe overlapping with abyssal
peridotite. In contrast, the high-Cr dunite displays a large variation in 56Fe. 56Fe of high-Cr
dunite with FeO similar to the harzburgite was not shifted during melt-peridotite interaction.
Instead, high-Cr dunite with low FeO has significantly higher 56Fe than rest of the samples,
which is ascribed to preferentially loss of light iron into melt conduit during melt-peridotite
interaction. Meanwhile, high-Cr dunite with enriched FeO has notably lower 56Fe than other
samples, indicating preferential gain of kinetically diffused light iron during melt-peridotite
interaction. Above all, distinct FeO and 56Fe in abyssal and SSZ peridotite can be explained
by similar processes as the Yushigou peridotite.
Acknowledgments
This study was supported by funds from the Strategic Priority Research Program of the
Chinese Academy of Sciences (XDB18000000), the National Key R&D Program of China
(2016YFC0600408), the Natural Science Foundation of China (41703029), and the China
Postdoctoral Science Foundation (2016LH00023). Analytical results for whole rock and
representative minerals are listed in the supporting information and can be found on figshare
(doi:10.6084/m9.figshare.9968414). We thank two anonymous reviewers for their
constructive reviews and John Lassiter for his suggestions and editorial handling. This is

contribution No. IS-0000 from GIGCAS.
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Table 1. Iron isotopic compositions of rock standard and Yushigou peridotite.
Sample 56Fe 2SD 57Fe 2SD
W-2 0.049 0.051 0.061 0.108

Standard* Duplicate 0.049 0.032 0.067 0.062
BHVO-2 0.093 0.060 0.139 0.053
Duplicate 0.117 0.055 0.173 0.036
AGV-2 0.109 0.038 0.173 0.059
17QH386 -0.012 0.021 -0.005 0.048
Carbonated 17QH387 -0.173 0.017 -0.253 0.065
serpentinite 17QH389 0.018 0.056 0.019 0.053
17QH390 0.173 0.057 0.238 0.082
Duplicate 0.169 0.047 0.264 0.051
17QH391 0.096 0.042 0.171 0.139
17QH393 0.041 0.007 0.045 0.075
17QH394 0.083 0.064 0.134 0.075
Serpentinized
dunite 17QH395 0.054 0.030 0.081 0.075
17QH401 0.004 0.034 0.009 0.037
17QH402 0.024 0.026 0.039 0.020
17QH399 0.040 0.040 0.057 0.031
17QH400 0.188 0.039 0.284 0.198
17QH405 -0.032 0.049 -0.041 0.143
17QH406 0.013 0.053 0.039 0.056
Serpentinized
17QH408 0.056 0.030 0.039 0.073
harzburgite
17QH410 0.016 0.023 -0.016 0.033
17QH411 0.038 0.034 0.022 0.056
17QH412 -0.039 0.044 -0.074 0.041
17QH414 -0.055 0.029 -0.085 0.006
17QH421 -0.002 0.061 0.009 0.030
Duplicate 0.005 0.061 0.010 0.057
17QH426 0.056 0.042 0.075 0.061
Duplicate 0.042 0.058 0.083 0.057
*Standards measured in the same batch as Zhang et al. (2019).

Figure 1. Microphotograph of serpentinized peridotite. (a) Interstitial clinopyroxene (Cpx)
with cuspate endings extends along orthopyroxene (Opx) boundaries in serpentinized
harzburgite. Orthopyroxene is altered into lizardite (Lz) along fractures. (b) Replacement of
olivine (Ol) by mesh lizardite and orthopyroxene by bastite (Bas) in serpentinized harzburgite.
Magnetite (Mag) crystallizes along the boundaries of previous olivine. (c) Relict spinel (Spl),
bastite, and mesh lizardite with core-rim texture in serpentinized harzburgite. (d) Chrysotile
(Ctl) veinlets developing along lizardite boundaries or crosscutting lizardite in serpentinized
harzburgite. (e) Lizardite surrounded by magnetite arrays in serpentinized dunite. Rare relict
spinel can be observed. (f) Spinel altered into Cr-magnetite and chlorite in serpentinized
dunite. Yellow circles labelled with letters represent spots for in-situ Raman analyses
presented in Figure S2. The scale bar is 200 m.

Figure 2. Microphotograph of carbonated peridotite. (a) Complex chrysotile veinlets
associated with magnesite. Sporadic antigorite (Atg) blades occur in the lizardite matrix. (b)
Magnesite patches and networks. (c) BSE image showing radiating antigorite blades closely
associated with magnesite. (d) Sample 17QH387 with antigorite as the sole serpentine.
Yellow circles labelled with letters represent spots for in-situ Raman analyses presented in
Figure S2. The scale bar is 200 m.

Figure 3. Co-variation plots for bulk rock major elements of the serpentinized and
carbonated peridotite. The peridotite is compared with modelled residues of anhydrous
melting of fertile lherzolite KR-4003 at 1~3 Gpa (Herzberg, 2004) and hydrous melting of
silica-enriched mantle wedge HMW at 1Gpa with 0.1~1% water (Bénard et al., 2017) in (a),
(b), and (e). Percentages labelling dotted lines represent degrees of melt extraction in the
modelled melting residue. Composition of the depleted mantle (DM) in (e) is from Salters
and Stracke (2004), and the terrestrial array is after Jagoutz et al. (1979) and Hart and Zindler
(1986). Data for nearby fresh harzburgite are from Zhang et al. (2019).

Figure 4. (a) Chondrite-normalized REE pattern and (b) primitive mantle-normalized
spider-diagram for the serpentinized and carbonated peridotite. Chondrite REE values are
from Sun and McDonough (1989), and primitive mantle element values are from
McDonough and Sun (1995).

Figure 5. Co-variation plots of (a) Ti vs. Yb, (b) (Gd/Yb)N vs. (La/Sm)N, (c) U vs. Nb, (d) Pb
vs. Th, (e) Sr vs. CaO, and (f) Rb vs. Cs for the serpentinized and carbonated peridotite.
Magmatic arrays in (c) and (d) are fitted after oceanic basalts from PetDB database
(http://www.earthchem.org/petdb). Data for abyssal and forearc serpentinite in (c), (d), and (f)
are from Peters et al. (2017). Data for nearby fresh harzburgite are from Zhang et al. (2019).

Figure 6. Co-variation plot of (a) Cr# vs. Mg# and (b) Cr# vs. TiO2 in relict spinel from the
serpentinized and carbonated peridotite. Data for abyssal peridotite are from Warren (2016),
and data for forearc peridotite are from Ishii et al. (1992), Parkinson and Pearce (1998),
Pearce et al. (2000), and Birner et al. (2017). Data for nearby fresh harzburgite are from
Zhang et al. (2019). Only 95% confidence eclipses are shown for the abyssal and forearc
peridotite. (b) is modified after Pearce et al. (2000), with BON and IAT denoting boninite and
island arc tholeiite, respectively. The curve labelled with percentages in (b) represents
modelled spinel composition during partial melting of fertile MORB mantle, with the
percentages denoting melting degrees.

Figure 7. Histogram showing iron isotopic composition of the serpentinized and carbonated
peridotite. 56Fe of nearby fresh harzburgite (Zhang et al. 2019), abyssal peridotite (Craddock
et al., 2013), and arc peridotite (William et al., 2004, 2005; Weyer & Ionov, 2007; Su et al.,
2015) are also shown for comparison.

Figure 8. Co-variation plots of 56Fe vs. (a) LOI, (b) Sr/Y, (c) (La/Sm)N, and (d) FeO for the
serpentinized and carbonated peridotite. Data source is similar to Figure 7.

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Iron isotope behavior during melt-peridotite interaction in

supra-subduction zone ophiolite from Northern Tibet

Corresponding author: Long Zhang (zhanglong@gig.ac.cn),

©2019 American Geophysical Union. All rights reserved.

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2. Geological setting and samples

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4.3 Mineral major elements

4.4 Iron isotopic composition

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5.3 Iron isotope behavior during melt-peridotite interaction

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Sample 56Fe 2SD 57Fe 2SD

W-2 0.049 0.051 0.061 0.108

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