Mantle Heterogeneity Recorded by Mass⁃Independent Fractionation of Sulfur Isotopes and Dynamic Implications
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摘要:
硫是一种挥发性元素，在浅部岩浆过程（如分离结晶、岩浆脱气）中易产生硫同位素质量分馏效应（Mass-dependent fractionation of sulfur isotopes，MDF⁃S），对使用硫同位素组成来约束地幔主要化学储库的属性产生干扰.硫同位素非质量分馏效应（Mass-independent fractionation of sulfur isotopes，MIF-S）是硫同位素分馏行为偏离质量依赖关系的现象，主要通过含硫分子在高能紫外线照射下发生光化学反应产生，其分馏机制与地球早期大气演化关系密切.值得注意的是，MIF-S信号在太古代沉积岩中普遍存在，而在大氧化事件之后该信号却消失不见.硫同位素非质量分馏（MIF-S）不依赖地幔氧化还原状态和高温过程（如部分熔融、分离结晶、岩浆脱气），能够很好地规避浅部岩浆过程导致的硫同位素质量分馏，对理解板块构造启动、地幔氧化还原状态和深部物质循环至关重要.在简要介绍硫同位质量和非质量分馏理论的基础上，本文梳理了地幔主要地球化学储库的硫同位素组成，重点评述了近20年来硫同位素非质量分馏效应在地幔不均一性和板块构造启动时限等研究上的重要进展.
Abstract:Sulfur is a volatile element that is prone to mass-dependent fractionation of sulfur isotopes (MDF-S) during shallow magmatic processes (e.g., fractional crystallization and magma degassing), which limits us to constrain the properties of major mantle chemical reservoirs. The mass-independent fractionation of sulfur isotopes (MIF-S) is a phenomenon in which the fractionation behavior of sulfur isotopes deviates from the mass dependent relationship. MIF-S is mainly produced through photochemical reactions of sulfur-containing molecules under high-energy ultraviolet radiation, and its fractionation mechanism is closely related to the atmospheric evolution on early Earth. It is worth noting that MIF-S signals are commonly preserved in Archean sedimentary rocks, but they disappeared after the Great Oxidation Event (GOE). MIF-S does not rely on mantle redox states and high-temperature processes (such as partial melting, fractional crystallization, magma degassing), and can effectively avoid MDF-S driven by shallow magma processes. And so, MIF-S is crucial for understanding the onset of plate tectonics, mantle redox states, and deep material cycling. On the basis of a brief introduction to the theories of MDF-S and MIF-S, this review summarizes the sulfur isotope composition of major mantle chemical reservoirs, and focuses on the important progress in mantle heterogeneity and onset of plate tectonics recorded by MIF-S in the past two decades.
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图 1 年轻地质样品(< 2 Ga)多硫同位素(δ33S、δ34S、δ36S)之间的相关性
硫同位素质量分馏（MDF-S，Δ33S=0，Δ36S=0）和硫同位素非质量分馏（MIF-S，Δ33S≠0，Δ36S≠0）的定义来自文献（Farquhar et al.，2000；Johnston，2011）
Fig. 1. Relationships among multiple sulfur isotopes (δ33S, δ34S, δ36S) in young terrestrial samples (< 2 Ga)
图 2 洋岛玄武岩Pb-Sr-Nd-S同位素组成和地幔端元组分
MORB.洋脊玄武岩；OIB.洋岛玄武岩；EM1.Ⅰ型富集地幔端元；EM2.Ⅱ型富集地幔端元；HIMU.高铀/铅比值地幔端元.数据源：洋脊玄武岩和洋岛玄武岩数据分别引自PetDB数据库（http://www.earthchem.org/petdb）和GEOROC数据库（http://georoc.mpch-mainz.gwdg.de/georoc）；Pitcairn洋岛玄武岩数据引自Delavault et al.（2016）；南大西洋EM1型洋脊玄武岩数据引自Labidi et al.（2013）；亏损地幔（DMM）和岛弧玄武岩δ34S数据分别引自Labidi et al.（2013）和Muth and Wallace（2021）；济南辉长岩和其余δ34S数据引自Zhang et al.（2020）
Fig. 2. Pb-Sr-Nd-S isotopes of oceanic-island basalts (OIBs) and mantle end members
图 3 岩浆脱气诱导硫同位素质量分馏
加那利群岛和月球硫同位素数据分别引自Beaudry et al.（2018）和Saal and Hauri（2021）
Fig. 3. Degassing-induced mass-dependent fractionation of sulfur isotopes
图 4 沉积物中δ34S和Δ33S随时间的演化序列Fig.4δ34S和Δ33S versus sedimentary age
沉积物多硫同位素数据引自Claire et al.（2014）；地质历史时期大气氧浓度和页岩U含量数据引自Zhang et al.（2020）；地幔氧逸度数据引自Aulbach and Stagno（2016）
图 5 沉积物中硫化物和硫酸盐的多硫同位素组成
沉积硫同位素数据引自Claire et al.（2014）
Fig. 5. Δ33S versus δ34S and Δ36S for sedimentary sulfides and sulfates
图 6 洋岛玄武岩的Δ33S和34S组成
原位硫同位素数据来源：Mangaia洋岛玄武岩数据引自Cabral et al.（2013）；Pitcairn洋岛玄武岩数据引自Delavault et al.（2016）；金刚石中硫化物包裹体（Farquhar et al.，2002；Cartigny et al.，2009；Thomassot et al.，2009；Smit et al.，2019）；侏罗纪变蛇绿岩中硫化物（Genot et al.，2024）.全岩硫同位素数据来源：南大西洋EM1型洋脊玄武岩数据（Labidi et al.，2013）；Mangaia洋岛玄武岩（Dottin III et al.，2020a）；Pitcairn洋岛玄武岩（Labidi et al.，2022）；冰岛玄武岩（Ranta et al.，2022）；Samoa洋岛玄武岩（Labidi et al.，2015；Dottin III et al.，2020b）；St. Helena洋岛玄武岩（Δ33S=0.014‰±0.010‰；δ34S > 0.5‰）（Cartigny，2015）；Canary洋岛玄武岩（Beaudry et al.，2018）；Garrett玄武岩（Labidi and Cartigny，2016）；Pacific- Antarctic洋脊玄武岩（Labidi et al.，2014）；Kimberley金伯利岩（Fitzpayne et al.，2021）；济南辉长岩（Zhang et al.，2020）
Fig. 6. Δ33S versus δ34S for oceanic-island basalts (OIBs)
图 7 金刚石中硫化物包裹体、橄榄岩和岩浆岩记录的MIF-S(Δ33S)信号随时间的演化
数据来源：始太古代角闪岩（Caro et al.，2025）；始太古代橄榄岩（Lewis et al.，2023）；金刚石中硫化物包裹体（Farquhar et al.，2002；Cartigny et al.，2009；Thomassot et al.，2009；Smit et al.，2019）；太古代TTG（Caro et al.，2025）；元古代花岗岩类（LaFlamme et al.，2018）；Belingwe科马提岩（Kubota et al.，2022）；Kimberley金伯利岩（Fitzpayne et al.，2021）
Fig. 7. MIF-S (Δ33S) signature of sulfide inclusions in diamonds, peridotites and magmatic rocks changed with time
图 8 太古代硫循环与板块构造启动的概念模型
a.始太古代无板块构造，地表物质无法进入地球内部，对应的古老克拉通地幔没有MIF-S信号；b.始太古代以来板块构造启动，地表物质随俯冲作用进入地球内部，在始太古代‒古元古代地幔岩石和金刚石中显示MIF-S信号.修改自Smit et al.（2019）
Fig. 8. Model of the Archean sulfur cycle and the onset of plate tectonics
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