摘要：Rapid carbon mineralization has been achieved in basaltic rocks; however, the fundamental chemical mechanisms governing the interactions of CO2-rock remain unclear. Here, ab initio molecular dynamics simulations were performed to elucidate the surface reaction of CO2using three basaltic minerals. To mimic natural conditions, the mineral surfaces were first hydrolyzed by water exposure. The simulation provides molecular-scale evidence that naturally occurring basaltic mineral surfaces are CO2-active. Three previously unrecognized pathways were revealed, distinct from the conventional dissolution–precipitation paradigm. These pathways involve CO2directly reacting with hydrolyzed mineral surfaces, at nonbridging oxygens (NBOs) and metal-coordinated hydroxyl groups, forming stable carbonate (CO32–), bicarbonate (HCO3–), and hydrogen pyrocarbonate (HC2O5–) species. The surface reaction capacity exhibits a first-order dependence on the density of NBOs. The presence of interfacial water plays a dual role in modulating the CO2chemisorption. We find that the surface reaction induces coordination distortion at metal sites, potentially lowering the dissolution energy barrier of carbonated metal ions and facilitating a self-sustaining cycle of surface reactivity renewal. These findings establish the existence of CO2surface reactions as a critical yet overlooked driver of enhanced carbon mineralization in basaltic systems. ? 2025 The Authors. Published by American Chemical Society

ISSN号：0013-936X

卷、期、页：卷59期28页14410-14418

发表日期：2025-07-22

影响因子：0.000000

期刊分区（SCI为中科院分区）：一区

收录情况：SCI（科学引文索引印刷版）,EI（工程索引）,SCIE（科学引文索引网络版）

发表期刊名称：Environmental Science and Technology

参与作者：Shao, Zihua,Liang, Yunfeng,Cui, Wuge,Jo, Gyuhwan,Usui, Keishi,Taniguchi, Tomohiro,Tsuji, Takeshi

第一作者：贾冀辉

论文类型：期刊论文

论文概要：Shao, Zihua,贾冀辉,Liang, Yunfeng,Cui, Wuge,Jo, Gyuhwan,Usui, Keishi,Taniguchi, Tomohiro,Tsuji, Takeshi，Surface Reaction of CO2with Basaltic Minerals as a Mechanism for Carbon Mineralization，Environmental Science and Technology，2025，卷59期28页14410-14418

论文题目：Surface Reaction of CO2with Basaltic Minerals as a Mechanism for Carbon Mineralization