Physical and chemical effects of H2O on mineral carbonation reactions in supercritical CO2

IF 3.1 3区地球科学 Q1 GEOCHEMISTRY & GEOPHYSICS

Applied Geochemistry Pub Date : 2023-08-01 DOI:10.1016/j.apgeochem.2023.105668

Sijia Dong , Tiange Xing , Liang Zhao , Chen Zhu , Xizhi Yao , Shuhan Zhao , Hui H. Teng

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引用次数: 0

Abstract

Mineral carbonation through reaction with supercritical CO₂ (scCO₂) is the ultimate pathway to permanent carbon storage for geological sequestration. Whether and how much H₂O is required for the scCO₂-mineral interaction to proceed readily, and the role of H₂O in the reaction have been actively researched topics. We designed and built a novel in situ Raman reactor to study the carbonation product during brucite [Mg(OH)₂]-scCO₂ interaction, and investigated the role of free H₂O by comparing the products in neat, H₂O, and formamide (FM) conditions. We introduced FM to provide a physical polarity environment similar to that of H₂O but without the chemical protonation effect. We further evaluated the role of structural H₂O by conducting experiments with periclase (MgO). The in situ Raman analysis revealed the occurrence of brucite carbonation both in the presence of H₂O and FM, demonstrating the effect of polarity in the reaction; in contrast, carbonation of periclase only occurred in H₂O-saturated scCO₂. The lack of carbonation of periclase with the presence of FM was attributed to the difficulty of magnesite mineralization, as CaCO₃ was able to form in the CaO-FM-scCO₂ system. Post-experimental X-ray diffractometry and Fourier-transform infrared spectrometry of the products showed that brucite carbonation yielded nesquehonite and hydromagnesite in H₂O and FM, respectively; whereas periclase-scCO₂ interaction in H₂O produced a mixture of the two products. Rate calculations suggested that the carbonation reaction was much faster in H₂O; nonetheless, 40–50% carbonation was still achieved in the Mg(OH)₂-FM-scCO₂ system after 330 h. Overall, our results showed that the brucite-scCO₂ reaction could proceed without H₂O under certain conditions – the polarity effect of H₂O/FM was large enough to break the Mg–OH and MgO–H bonds and promote the carbonation process.

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水对超临界CO2中矿物碳酸化反应的物理和化学影响

通过与超临界二氧化碳(scCO2)的反应，矿物碳酸化是地质封存永久碳储存的最终途径。scco2 -矿物的相互作用是否容易进行，需要多少水，以及水在反应中的作用一直是人们积极研究的课题。为了研究水镁石[Mg(OH)2]-scCO2相互作用过程中的碳化产物，我们设计并建造了一种新型的原位拉曼反应器，并通过比较纯水、水和甲酰胺(FM)条件下的碳化产物，研究了游离H2O的作用。我们引入FM是为了提供一个类似于H2O的物理极性环境，但没有化学质子化效应。我们通过对镁方石(MgO)的实验进一步评估了结构水的作用。原位拉曼分析结果表明，水镁石在H2O和FM存在下均发生碳酸化反应，表明极性对反应的影响;相比之下，方石石的碳化作用只发生在h2o饱和的scCO2中。由于CaCO3能够在CaO-FM-scCO2体系中形成，镁长石在FM存在时缺乏碳酸化，这归因于菱镁矿化困难。产物的x射线衍射和傅里叶变换红外光谱分析表明，水镁石碳酸化在H2O和FM中分别生成了菱镁石和氢菱镁石;而在H2O中，周镁质- scco2相互作用产生了这两种产物的混合物。速率计算表明，在H2O中碳化反应要快得多;但经过330 h后，Mg(OH)2-FM-scCO2体系仍能实现40-50%的碳酸化。综上所述，我们的结果表明，在一定条件下，水/FM的极性效应足以破坏Mg - OH和MgO-H键，促进碳酸化过程，水镁石- scco2反应可以在没有水的情况下进行。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Applied Geochemistry 地学-地球化学与地球物理

CiteScore

6.10

自引率

8.80%

发文量

272

审稿时长

65 days

期刊介绍： Applied Geochemistry is an international journal devoted to publication of original research papers, rapid research communications and selected review papers in geochemistry and urban geochemistry which have some practical application to an aspect of human endeavour, such as the preservation of the environment, health, waste disposal and the search for resources. Papers on applications of inorganic, organic and isotope geochemistry and geochemical processes are therefore welcome provided they meet the main criterion. Spatial and temporal monitoring case studies are only of interest to our international readership if they present new ideas of broad application. Topics covered include: (1) Environmental geochemistry (including natural and anthropogenic aspects, and protection and remediation strategies); (2) Hydrogeochemistry (surface and groundwater); (3) Medical (urban) geochemistry; (4) The search for energy resources (in particular unconventional oil and gas or emerging metal resources); (5) Energy exploitation (in particular geothermal energy and CCS); (6) Upgrading of energy and mineral resources where there is a direct geochemical application; and (7) Waste disposal, including nuclear waste disposal.