Pearce J K, Kirste D, Dawson G W, Rudolph V, Southam G, Brink F, Paterson D J, Hall N, Sommacal S, Golding S D
Gas and Energy Transition Research Centre, University of Queensland, QLD, Australia; School of the Environment, University of Queensland, QLD, Australia.
Department of Earth Sciences, Simon Fraser University, BC, Canada.
Sci Total Environ. 2025 Feb 1;963:178391. doi: 10.1016/j.scitotenv.2025.178391. Epub 2025 Jan 15.
The transition to net zero emissions requires the capture of carbon dioxide from industrial point sources, and direct air capture (DAC) from the atmosphere for geological storage. Dissolved CO has reactivity to rock core, and while the majority of previous studies have concentrated on reservoir rock or cap-rock reactivity, the underlying seal formation may also react with CO. Drill core from the underlying seal of a target CO storage site was reacted at in situ conditions with pure CO, and compared with an impure CO stream with SO, NO and O that could be expected from hard to abate industries. Argillaceous sandstones, mudstones, coaly mudstones, and carbonate cemented sandstones of the Moolayember Formation, Bowen Basin, had significant natural alteration of feldspar to kaolinite creating porosity, with clays, siderite and textured ankerite filling and rimming porosities of 3.5 to 15.8 %. Synchrotron XFM quantified Mn mainly hosted in siderite veins and cements, Sr and Rb in feldspar, and Pb, Th and Sr in monazite. Pb was also in siderite; with As mainly in pyrite and associated with ankerite. On pure CO or impure CO reaction, ankerite and siderite dissolution, Fe-chlorite leaching, and apatite or sulphide alteration occurred. With the impure CO stream Fe-oxides precipitated on rock surfaces especially in argillaceous sandstone. Ferroan carbonates, calcite, and Fe oxides containing Cr were also precipitated. Ankerite and siderite dissolution released increasing concentrations of dissolved Ca, Mg and Mn from carbonate cemented core that were higher with mixed gas injection. Argillaceous sandstone however released higher concentrations Si, Rb, Co and Zn. Dissolved Fe initially increased then decreased in impure gas experiments via Fe oxide precipitation, and Pb, Ni, Cr, REE also increased and subsequently decreased. Geochemical modelling predicted that Fe was mobilised mainly from reaction of siderite and Fe chlorite. Mainly carbonates (siderite, ankerite) and chlorite dissolution released trace metals, with several metals also initially mobilised by desorption and exchange. Precipitated Fe oxides provided adsorption sites to adsorb a portion of metals from solution. These reactions are also relevant to CO streams from DAC that could be expected to contain O and to potential reactions in overlying aquifers.
向净零排放的转变需要从工业点源捕获二氧化碳，并从大气中直接捕获二氧化碳用于地质封存。溶解的CO与岩芯具有反应活性，虽然以前的大多数研究都集中在储层岩石或盖层岩石的反应活性上，但下伏的封闭地层也可能与CO发生反应。对目标CO储存地点下伏封闭层的岩芯在原位条件下与纯CO进行反应，并与来自难以减排行业的含有SO、NO和O的不纯CO流进行比较。 Bowen盆地Moolayember组的泥质砂岩、泥岩、含煤泥岩和碳酸盐胶结砂岩，长石显著自然蚀变为高岭石从而形成孔隙，粘土、菱铁矿和纹理状铁白云石填充并环绕孔隙，孔隙率为3.5%至15.8%。同步加速器X射线荧光光谱法（Synchrotron XFM）定量分析表明，Mn主要存在于菱铁矿脉和胶结物中，Sr和Rb存在于长石中，Pb、Th和Sr存在于独居石中。Pb也存在于菱铁矿中；As主要存在于黄铁矿中，并与铁白云石有关。在纯CO或不纯CO反应时，铁白云石和菱铁矿溶解、铁绿泥石浸出以及磷灰石或硫化物蚀变发生。在不纯CO流作用下，铁氧化物沉淀在岩石表面，尤其是在泥质砂岩中。含Cr的亚铁碳酸盐、方解石和铁氧化物也沉淀出来。铁白云石和菱铁矿溶解使碳酸盐胶结岩芯中溶解的Ca、Mg和Mn浓度增加，混合气体注入时浓度更高。然而，泥质砂岩释放出更高浓度的Si、Rb、Co和Zn。在不纯气体实验中，溶解的Fe最初增加，然后通过铁氧化物沉淀而减少，Pb、Ni、Cr、稀土元素（REE）也先增加后减少。地球化学模型预测，Fe主要从菱铁矿和铁绿泥石的反应中被 mobilised出来。主要是碳酸盐（菱铁矿、铁白云石）和绿泥石溶解释放出痕量金属，几种金属最初也通过解吸和交换被 mobilised出来。沉淀的铁氧化物提供了吸附位点，从溶液中吸附一部分金属。这些反应也与来自直接空气捕获（DAC）的预计含有O的CO流以及上覆含水层中的潜在反应有关。
原文中“mobilised”这个词在中文语境下较难找到完全对应的准确词汇，这里保留英文以便理解原文确切含义，你可根据具体专业背景来准确理解它在此处的意思。
