Cobalt Substitution Slows Forsterite Carbonation in Low-Water Supercritical Carbon Dioxide

IF 2.9 3区化学 Q3 CHEMISTRY, PHYSICAL Physical Chemistry Chemical Physics Pub Date : 2024-10-09 DOI:10.1039/d4cp02092h

John Steven Loring, Tenley E Webb, Mark E Bowden, Mark H Engelhard, Sebastien Kerisit

引用次数: 0

Abstract

Cobalt recovery from low-grade mafic and ultramafic ores could be economically viable if combined with CO2 storage under low-water conditions, but the impact of Co on metal silicate carbonation and the fate of Co during the carbonation reaction must be understood. In this study, in situ infrared spectroscopy was used to investigate the carbonation of Co-doped forsterite ((Mg,Co)2SiO4) in thin water films in humidified supercritical CO2 at 50 °C and 90 bar. Rates of carbonation of Co-doped forsterite to Co-rich magnesite ((Mg,Co)CO3) increased with water film thickness but were at least 10 times smaller than previously measured for pure forsterite at similar conditions. We suggest that the smaller rates are due to thermodynamic drivers that cause water films on Co-doped forsterite to be much less oversaturated with respect to Co-doped magnesite, compared to the pure minerals.

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钴置换可减缓低水超临界二氧化碳中福斯特岩的碳化过程

如果在低水条件下结合二氧化碳封存，从低品位岩浆岩和超岩浆岩矿石中回收钴可能具有经济可行性，但必须了解钴对金属硅酸盐碳化的影响以及碳化反应过程中钴的去向。本研究采用原位红外光谱法研究了在 50 °C、90 巴的湿润超临界 CO2 条件下，水薄膜中掺有 Co 的绿柱石（(Mg,Co)2SiO4）的碳化过程。掺钴的绿柱石碳化成富钴菱镁矿（(Mg,Co)CO3）的速率随水膜厚度的增加而增加，但比以前在类似条件下测量纯绿柱石的速率至少小 10 倍。我们认为，与纯矿物相比，较小的速率是由于热力学驱动因素导致掺钴的绿柱石上的水膜相对于掺钴的菱镁矿的过饱和程度要低得多。

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

Physical Chemistry Chemical Physics 化学-物理：原子、分子和化学物理

CiteScore

5.50

自引率

9.10%

发文量

2675

审稿时长

2.0 months

期刊介绍： Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.