Geochemical behavior and recycling of sulfur in subduction zones
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摘要:
俯冲带是全球最大的物质循环系统，控制着硫(S)在地球内部圈层及表层的循环，影响着大气圈、水圈、生物圈、岩石圈的稳定性以及地球的宜居性。厘清S在俯冲带中的地球化学行为和循环特征对理解地球各储库的氧化还原状态、岩浆作用与演化、成矿物质聚集、以及地球大气成分等具有重要意义。本文首先总结了进入俯冲带之前的大洋岩石圈的S结构模型，对S在大洋板片中的分布状态和地球化学特征进行了系统归纳。随后，系统阐述了俯冲带高压-超高压变质岩记录的板片变质及脱水过程中硫的地球化学行为。岩石学研究表明俯冲板片中的S多以硫化物相存在，硫酸盐矿物在弧前深度就已被释放或分解。相较于熔体，俯冲带流体中S的溶解度更高，是运移硫的更有效方式。DEW模型计算结果显示，流体中S含量总体较低，但在俯冲板片~90km处其含量有一个峰值(浓度0.5%~1.0%)。岩相学证据、地球化学测试结果、磷灰石S近边吸收结构(S-XANES)特征以及模拟结果都显示俯冲深部流体中S多以HS-及H2S形式存在，不含大量的SO42-及硫酸盐；中fS2流体有利于S迁移出俯冲板片，从而促进俯冲带大规模S循环，而高fS2流体在流-岩交换过程沿流体通道发生S的锁固作用而不利于俯冲带S循环。质量平衡计算显示全球俯冲带S输入通量为4.65×1013g/yr，弧下深度板片S输出通量为2.91×1012g/yr，板片-岛弧S循环效率仅6.3%。俯冲板片在弧下深度可能存在一个短暂高效的S释放窗口，释放流体的δ34S值为-2.1±3.0‰。基于高压-超高压变质岩中硫化物的研究，初步厘清了俯冲板片中S的地球化学行为，首次从板片角度全面、定量地限定了俯冲带的脱硫通量、效率、种型和同位素特征，提出俯冲带循环的S不是岛弧岩浆的氧化剂，与岛弧环境的正δ34S值也无直接因果联系，对解析俯冲带S循环和理解地球长期的S循环具有重要意义。最后，本文还展望了俯冲带S循环的未来发展方向，应在俯冲带流体氧化还原性质(硫酸盐的命运)、俯冲沉积物对S循环的制约、俯冲带环境下多硫同位素的分馏效应、S循环与其它挥发分(如C等)循环之间的耦合关系、地球历史上深部S循环等方向做出探索，更深入地理解俯冲带及全球S循环过程。
Abstract:Subduction zone is the largest material recycling system on the Earth, mediating the sulfur exchange between Earth's interior and surface. Sulfur is one of the key elements that connects the atmo-, hydro-, bio-, and lithosphere and plays a critical role in Earth habitability. Knowing the behavior and recycling of S in the subduction zone is critical to understand the redox state of geological reservoirs, arc magmatism and ore metallogenesis, as well as change and evolution of Earth's atmosphere. This paper first presents the sulfur structure in the pre-subduction oceanic lithosphere, reviewing the occurrences of S-bearing phases and their geochemical compositions. Then, this study systematically reviews the S behavior during the metamorphic and dehydration processes in the subducted slab recorded by high-pressure and ultrahigh-pressure (HP-UHP) metamorphic rocks. Petrologic investigation shows that S in the subducting slab occurs mostly in the form of sulfide, and that sulfate is mostly dissolved or broken down at the fore-arc depths. Sulfur solubility in slab fluids is much higher in comparison to melts, suggesting that fluid is the more effective agent for transferring S from the slab to the mantle wedge. DEW (Deep Earth Water) modeling indicates that S concentration in slab fluids is generally low; however, it reveals a distinct [S] peak (0.5%~1.0%) at ~90km depth. All evidence from petrologic observations, chemical analyses, apatite S-XANES (X-ray Absorption Near Edge Structure) characteristics, and DEW modeling show that S species in slab fluids are dominated by reduced HS- and H2S at given subduction zone P-T-fO2 conditions, without significant SO42- or sulfate. Medium-fS2 fluids can transport S and thus are effective in transferring S out of the slab, whereas high-fS2 fluids cause S sequestration along fluid pathways and considerably reduce long-distance S transfer. Mass-balance calculations demonstrate that the global S influx is estimated at 4.65×1013g/yr, slab outflux at 2.91×1012g/yr at sub-arc depth, resulting in a slab-arc S recycling efficiency of ~6.3%. A major S release window is constrained at depths of 70~100km, during which the released slab fluid has a negative δ34S value of -2.1±3.0‰. Based on researches of HP-UHP metamorphic rocks, the recent studies shed light on the S behavior in the subduction zone, and for the first time from the slab perspective, reveal the slab desulfuration flux and efficiency, sulfur species and isotopic composition during the slab-arc S recycling. It is suggested that slab S is not an oxidant accounting for the high fO2 of arc magmas and also not related to the heavy δ34S signature observed in arc volcanic rocks. The study sheds light on S recycling in subduction zone and long-term global S cycle. At the end, this paper proposes some research directions in the future that will likely be fruitful in understanding subduction zone S recycling, including redox state of slab fluids (fate of sulfate), controls of metasediment on sulfur cycle, multiple sulfur isotope fractionation in subduction environment, the coupling/decoupling recycling between S and other volatiles (C and etc.), and deep sulfur cycle through geological time.
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Key words:
- Subduction zone /
- Sulfur recycling /
- HP-UHP metamorphic rocks /
- Slab fluids /
- Arc fO2
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图 1
大洋岩石圈剖面结构(a)及各岩性序列对总质量(b)、含水量(c)和含硫量(d)的质量占比
Figure 1.
Schematic lithologic successions of typical oceanic lithosphere (a) and their mass (b), water (c), sulfur (d) proportions categorized by source
图 2
俯冲洋壳高压-超高压变质岩中含硫相的岩相学特征
Figure 2.
Photomicrographs of sulfides in oceanic HP-UHP metamorphic rocks
图 3
利用DEW模型计算的俯冲基性洋壳释放流体中的[S]及种型比例(据Li et al., 2020修改)
Figure 3.
Sulfur concentration and species in slab fluids calculated by the DEW model (modified after Li et al., 2020)
图 4
高压榴辉岩脉体中磷灰石的S-XANES光谱(据Li et al., 2021b修改)
Figure 4.
Sulfur XANES spectra of apatite in the eclogite-facies vein(modified after Li et al., 2021b)
图 5
不同性质流体作用下流体-岩石反应过程中S的迁移、交换、再分配示意图(据Li et al., 2021b修改)
Figure 5.
Schematic illustration of the sulfide transformation and redistribution during fluid-rock interaction caused by Fe-rich medium fS2 fluid (a, b) and Fe-poor high fS2 fluid (c, d)(modified after Li et al., 2021b)
图 6
俯冲大洋板片各岩性对S的输入通量(a)、输出通量(b)的贡献及俯冲带在不同深度的S释放分布(c)
Figure 6.
Subduction sulfur input (a) and output (b) categorized by source, and estimated slab sulfur outflux categorized by depth (c)
图 7
俯冲带硫循环模型(据Li et al., 2020修改)
Figure 7.
Diagram illustrating fluid-mediated sulfur cycle in the subduction zone(modified after Li et al., 2020)
表 1
标准大洋岩石圈板片的硫结构
Table 1.
Sulfur structure in the pre-subduction oceanic lithosphere
序号 俯冲洋壳岩性序列 厚度(m) 密度(g/cm3) S含量(×10-6) δ34S (‰) 参考文献 1 沉积物 平均300 2.50 6000 (均值) -17.0 Goldhaber, 2003 2 玄武岩火山层序 平均600 2.76 940 (均值) -6.0 Alt and Shanks, 2011 3 硫酸盐脉(硬石膏) 不均一分布于2与6中，约为洋壳总S量的1% Alt, 1995 4 过渡带(强矿化带) 15 2.80 9740±6900 +3.0 Alt, 1995 5 过渡带 100 2.80 3150±4300 +3.0 Alt, 1995 6 席状岩墙群(上部) 平均300 2.92 610±300 +0.6 Alt, 1995 7 席状岩墙群(下部) 平均500 2.92 620±340 +2.0 Alt, 1995 8 辉长岩(蚀变层) 500 2.98 230±190 +0.4 Alt, 1995 9 辉长岩 5000 2.98 620±180 +0.1 Alt, 1995 10 蛇纹石化地幔 2000 2.80 200±180 +7.3 Schwarzenbach et al., 2016 总板片 9315 *4.65×1013 g/yr -3.6 Li et al., 2020 注：*该数值指进入俯冲带的全球板片携带的S通量 
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