Acceleration of hydrogen production during water-olivine-CO2 reactions via high-temperature-facilitated Fe(II) release

Acceleration of hydrogen production during water-olivine-CO2 reactions via high-temperature-facilitated Fe(II) release
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DOI:
10.1016/j.ijhydene.2019.03.119
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发表时间:
2019-05
影响因子:
7.2
通讯作者:
Jiajie Wang;N. Watanabe;A. Okamoto;Kengo Nakamura;T. Komai
Jiajie Wang;N. Watanabe;A. Okamoto;Kengo Nakamura;T. Komai
中科院分区:
工程技术2区
文献类型:
--
作者:
Jiajie Wang;N. Watanabe;A. Okamoto;Kengo Nakamura;T. Komai

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在 225–300 °C 的富 CO2 (0.5 mol/L NaHCO3) 和无 CO2 条件下,研究了温度对橄榄石 [(Mg,Fe)2SiO4] 蚀变中氢气 (H2) 产生的影响。在富含 CO2 的条件下,H2 生成速率表现出强烈的温度依赖性,其中当 ≥275 °C 时,速率急剧增加,而在无 CO2 条件下的速率对温度的依赖性较小。在300°C富含CO2的条件下,氢气生成速率比无CO2条件下快3倍,同时相当数量的CO2以菱镁矿[(Mg,Fe)CO3]的形式储存。在富含CO2的条件下升高温度促进了橄榄石的消耗,同时抑制水镁石[(Mg,Fe)(OH)2]的形成和Fe(II)进入次生矿物,从而促进Fe(II)释放和氧化产生H2。首次揭示水-橄榄石-CO2反应过程中H2的产生通过高温促进Fe(II)的释放而显着加速。
The effects of temperature on hydrogen (H2) production in the alteration of olivine [(Mg,Fe)2SiO4] have been investigated under both CO2-rich (0.5 mol/L NaHCO3) and CO2-free conditions at 225–300 °C. Under CO2-rich conditions, H2production rates showed strong temperature dependence, where the rate drastically increased for ≥275 °C, while the rate in CO2-free conditions was less temperature-dependent. At 300 °C under CO2-rich conditions, the H2generation rate was 3 times faster than that under CO2-free conditions, and a considerable amount of CO2was simultaneously stored as magnesite [(Mg,Fe)CO3]. Increasing the temperature under CO2-rich conditions promoted olivine consumption, while suppressing both brucite [(Mg,Fe)(OH)2] formation and incorporation of Fe(II) into secondary minerals, thus facilitating Fe(II) release and oxidation to produce H2. It has been revealed for the first time that H2production during water-olivine-CO2reactions is markedly accelerated via high-temperature-facilitated Fe(II) release.