下地幔温压条件下碳对(Mg,Fe)SiO<sub>3</sub>布里奇曼石的影响

苘廉洁; 苑洪胜; 秦礼萍; 张莉

doi:10.11858/gywlxb.20190788

下地幔温压条件下碳对(Mg,Fe)SiO₃布里奇曼石的影响

doi: 10.11858/gywlxb.20190788

苘廉洁^{1, 2,},
苑洪胜²,
秦礼萍¹,
张莉^2,*, ,

1.
中国科学技术大学地球和空间科学学院，安徽合肥　230026
2.
北京高压科学研究中心，北京　100094

基金项目: 国家自然科学基金（41574080, U1530402）；中国工程物理研究院院长基金（201402032）

详细信息

作者简介:
苘廉洁（1994－），男，硕士，主要从事深部地球科学研究. E-mail：lianjie.man@hpstar.ac.cn

通讯作者:
张　莉（1980－），女，博士，研究员，主要从事高压物理与深部地球科学研究.E-mail：zhangli@hpstar.ac.cn

中图分类号: O521.2
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出版历程
- 收稿日期: 2019-06-04
- 修回日期: 2019-07-24

Effects of Carbon on (Mg,Fe)SiO₃ Bridgmanite under the Lower Mantle Pressure-Temperature Conditions

MAN Lianjie^{1, 2
,},
YUAN Hongsheng²,
QIN Liping¹,
ZHANG Li^{2,*
, ,}

1.
School of Earth and Space Sciences, University of Science and Technology of China, Hefei 230026, China
2.
Center for High Pressure Science and Technology Advanced Research (HPSTAR), Beijing 100094, China

摘要

摘要: 利用激光加温金刚石对顶砧技术模拟下地幔温压条件（36～88 GPa, 1 850～2 800 K），探索了碳与含铁的(Mg,Fe)SiO₃布里奇曼石的相互作用过程。同步辐射X射线衍射实验表明，(Mg,Fe)SiO₃布里奇曼石与碳在大于42 GPa、2 000 K的温压条件下发生了氧化还原反应，即(Mg,Fe)SiO₃布里奇曼石中的二价铁（Fe²⁺）被单质碳还原成金属铁（Fe⁰）；而在较低的温压条件下，布里奇曼石中的Fe²⁺可以稳定存在。该结果表明，在下地幔深部的温压条件下，CCO缓冲的氧逸度值比IW缓冲更低，热力学计算结果也证实了这一结果。实验结果为地幔深部氧化还原条件的不均一性和局部极端还原状态的出现提供了解释。
- 布里奇曼石 /
- 深部碳 /
- 下地幔 /
- 氧化还原反应
Abstract: In this study we investigated the interaction of carbon with iron in the (Mg,Fe)SiO₃ bridgmanite under the conditions corresponding to the Earth’s lower mantle (36–88 GPa, 1 850–2 800 K) using a laser-heated diamond anvil cell. Synchrotron X-ray diffraction measurements of the run products showed that Fe²⁺ in bridgmanite can be reduced to metallic Fe by carbon under the pressure and temperature conditions higher than 42 GPa and 2 000 K. The coexisting metallic Fe and Fe-depleted bridgmanite in the run products suggests that the CCO buffer produces lower oxygen fugacity than the of Fe-FeO (IW) buffer, which is further confirmed by the thermodynamic calculation. The experimental results in this study could provide a potential explanation for the presence of redox heterogeneities and highly reducing regions in the deep mantle.
- bridgmanite /
- deep carbon /
- lower mantle /
- redox reaction

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图 1 高压样品的组装方式

Figure 1. Sample configuration for high pressure experiments

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图 2 样品Sa104-1在88 GPa的高压原位（a）和卸载至常温常压（b）的XRD谱 (Bdg、CS、Stv分别代表布里奇曼石、CaCl₂型结构的SiO₂、斯石英，hcp和bcc分别代表六方密堆积结构和体心立方结构的金属铁。高压下的XRD谱中没有发现相应压力下hcp-Fe ^[24]的衍射峰。)

Figure 2. XRD patterns of Sa104-1 at 88 GPa (a) and ambient conditions (b), respectively (Bdg=bridgmanite, CS=silica with the CaCl₂–type structure, Stv=stishovite, hcp=iron with the hexagonal close-packed structure, bcc=iron with the body-centered cubic structure. Diffraction peaks of the hcp-Fe ^[24] were not observed in the high-pressure XRD pattern.)

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图 3 Sa104-3样品在 36 GPa高压原位（a）和卸载至常温常压（b）的XRD谱（Bdg代表布里奇曼石，Stv代表斯石英，hcp和bcc分别指代六方密堆积结构和体心立方结构的金属铁。高压下或复原至常温常压后所采集的XRD谱中均没有观测到hcp-Fe或bcc-Fe ^[24]的衍射峰。）

Figure 3. XRD patterns of Sa104-3 at 36 GPa (a) and ambient conditions (b), respectively (Bdg=bridgmanite, CS=silica with the CaCl₂–type structure, Stv=stishovite, hcp=iron with the hexagonal close-packed structure, bcc=iron with the body-centered cubic structure. Diffraction peaks of either hcp-Fe or bcc-Fe ^[24] were not observed in the XRD patterns.)

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图 4 在两种不同温压条件下合成的布里奇曼石在卸压过程中的p-V关系：（a）在88 GPa、2 400 K温压条件下合成的Sa104-1样品；（b）在36 GPa、1 850 K温压条件下合成的Sa104-3样品

Figure 4. p-V relations on decompression of two bridgmanite samples synthesized under two different p-T conditions, respectively: (a) sample Sa104-1 synthesized under 88 GPa and 2 400 K; (b) sample Sa104-3 synthesized under 36 GPa and 1 850 K

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图 5 在常温常压下(Mg,Fe)SiO₃布里奇曼石的晶胞体积与含铁量的关系

Figure 5. Unit-cell volumes of (Mg,Fe)SiO₃ bridgmanite as a function of iron content under ambient conditions

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表 1 含碳的Mg_0.85Fe_0.15SiO_x凝胶样品合成条件和实验产物

Table 1. Experimental condition and run products of Mg_0.85Fe_0.15SiO_x gel (carbon bearing)

Sample	p/GPa	T/K	Pressure medium	Pressure marker	Run products
Sample	p/GPa	T/K	Pressure medium	Pressure marker	In situ	Ambient
Sa104-1	88(1)	2 400(100)	Ne	Ne	Bdg, CS	Bdg, Stv, bcc-Fe
Sa82-1	43(1)	2 800(200)	SiO₂	Au	Bdg, Stv	Bdg, Stv, bcc-Fe
Sa104-2	42(1)	2 000(100)	SiO₂	Au	Bdg, Stv	Bdg, Stv, bcc-Fe
Sa104-3	35(1)	1 850(100)	Ne	Ne	Bdg, Stv	Bdg, Stv
Notes: (1) Pressures were determined by the equations of state of Ne or Au^[21] after T quench, respectively; (2) Run products were identified by power XRD under high pressure and ambient conditions, respectively; (3) Bdg=bridgmanite, CS= silica with CaCl₂-type structure, Stv=stishovite, bcc-Fe=metallic iron with body-centered cubic structure.

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表 2 不同条件下合成的布里奇曼石的晶胞参数在卸压中随压力的变化

Table 2. Pressure-dependent unit-cell lattice parameters of bridgmanite synthesized under different pressure-temperature (p-T) conditions

Sample	p/GPa	a/Å	b/Å	c/Å	V/Å³
Sa104-1	88(1)	4.395(1)	4.624(1)	6.386(2)	129.79(4)
	87(1)	4.404(1)	4.624(1)	6.391(1)	130.13(3)
	82(1)	4.417(1)	4.640(1)	6.410(1)	131.37(3)
	80(1)	4.420(1)	4.646(1)	6.422(2)	131.88(5)
	71(1)	4.446(1)	4.673(1)	6.470(3)	134.38(5)
	Room pressure	4.778(2)	4.929(2)	6.899(3)	162.46(7)
Sa82-1	43(1)	4.557(1)	4.742(1)	6.591(1)	142.42(3)
Sa82-1	Room pressure	4.790(1)	4.922(1)	6.898(4)	162.62(7)
Sa104-2	42(1)	4.530(1)	4.707(1)	6.641(1)	141.59(3)
Sa104-2	Room pressure	4.779(1)	4.932(1)	6.898(1)	162.56(3)
Sa104-3	36(1)	4.597(1)	4.773(1)	6.643(1)	145.73(3)
	33(1)	4.601(1)	4.793(1)	6.653(1)	146.70(4)
	20(1)	4.677(1)	4.836(1)	6.758(2)	152.83(4)
	17(1)	4.747(1)	4.828(1)	6.721(2)	153.72(5)
	14(1)	4.701(1)	4.868(1)	6.779(1)	155.15(3)
	Room pressure	4.789(1)	4.938(1)	6.908(1)	163.36(3)
Note: (1) Pressures were determined by the equations of state of Ne or Au^[21] after T quench; (2) The data were collected along the decompression path.

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表 3 热状态方程参数

Table 3. Parameters for thermal equation of state

Material	V₀/(cm³·mol^–1)	K₀/GPa	${K_0'}$	γ₀	q	θ /K	Ref.
FeSiO₃(Bdg)	25.400	272	4.1	1.44	1.4	765	[47]
FeO(B1)	12.256	146.9	4.0	1.42	1.3	380	[42]
SiO₂(Stv)	14.017	302	5.24	1.71	1.0	1 109	[48]
SiO₂(CS)	14.017	341	3.2	2.14	1.0	1 109	[48]
Note: (1) V₀–volume at ambient conditions, K₀–bulk modulus, ${K_0'}$ –pressure derivative of K₀, γ₀–Grüneisen parameter at ambient conditions, q–logarithmic volume derivative of the Grüneisen parameter, θ–Debye temperature; (2) K₀ and ${K_0'}$ are parameters for Birch-Murnaghan equation of state, and γ₀, q₀ and θ are parameters used for Mie-Grüneisen relation.

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