硅酸盐学报

颗粒态γ-C₂S、β-C₂S、C₃S矿物固碳速率的差异及微观机理

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许扬帆 ¹^,² , 钱春香 ¹^,² , 裴嘉炜 ¹^,²

硅酸盐学报 | 研究论文 2025,53(2): 325-338

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硅酸盐学报 |研究论文 2025 , 53 (2) : 325 -338

颗粒态γ-C₂S、β-C₂S、C₃S矿物固碳速率的差异及微观机理

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许扬帆¹^,², 钱春香¹^,², 裴嘉炜¹^,²

作者信息

^1．东南大学材料科学与工程学院，南京 211189

^2．东南大学绿色建材与固碳利用研究中心，南京 211189

通讯作者:

钱春香（1966—），女，博士，教授。

作者简介:

许扬帆（1996—），女，博士研究生。

Mechanism Investigation and Difference in Carbon Sequestration Rates of Granular γ-C₂S, β-C₂S and C₃S Minerals

Yangfan XU¹^,², Chunxiang QIAN¹^,², Jiawei PEI¹^,²

Affiliations

^1.School of Materials Science and Engineering, Southeast University, Nanjing 211189, China

^2.Research Center for Green Construction Materials & Carbon Utilization, Southeast University, Nanjing 211189, China

Corresponding Author:

QIAN Chunxiang (1966-), female, Ph.D., Professor. E-mail: cxqianseu1@163.com

XU Yangfan (1996-), female, Doctoral candidate. E-mail: xyflower23@163.com

出版时间: 2025-02-20 doi: 10.14062/j.issn.0454-5648.20240269

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摘要

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矿物固碳是当下极具环保价值和工业价值的研究之一。本工作深入研究了γ-C₂S、β-C₂S、C₃S 3种矿物固碳反应速率与反应接触面、微观演化之间的关联，揭示了固碳速率差异的微观机理。结果表明：γ-C₂S、β-C₂S固碳率发展规律相似，均符合BoxLucas1模型；2种C₂S颗粒表面的碳酸钙晶体以方解石为主，趋向（104）热力学稳定面优势生长。γ-C₂S颗粒表面的碳酸钙呈地幔生长到外延生长，前期的外延生长导致了更大的反应接触面，在反应后期仍具有反应活性，同时方解石晶粒尺寸较大；而β-C₂S呈外延生长到地幔生长，前期的地幔生长导致了较密集的成核，晶粒尺寸发展更稳定，后期反应能力较差。C₃S初期固碳反应最快，反应5 min后迅速停滞，符合缩核反应模型；反应初期，C₃S表面针状文石与立方状方解石错杂生长，其致密结构造成了固碳反应过早停滞，随着反应进行，文石向方解石转变。

关键词

硅酸二钙 / 硅酸三钙 / 固碳反应 / 碳酸钙 / 晶体生长

Abstract

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Introduction

Mineral carbon sequestration is a crucial area of research in both environmental protection and industry. While much of the existing research has focused on the direct carbon sequestration of minerals to enhance cementation properties, there is a gap in understanding the interface micro-structure evolution of mineral powder particles during the carbonization process for the use of supplementary cementing materials. This study delves into the investigation of three calcium silicate minerals found in steel slag, examining the single-particle carbonization reaction rate and the micro-evolution process of the reaction interface at a micron scale. The goal is to uncover the differences and mechanisms behind the carbon fixation reaction rates of these three calcium silicate minerals.

Methods

Three types of calcium silicate minerals, namely γ-C₂S, β-C₂S, and C₃S, were prepared using the sintering method. A time gradient experiment was conducted on these minerals, and the evolution of multi-scale products was observed and analyzed through various microscopic techniques. Quantitative analysis using XRD and TG-DTG was employed to compare the carbon sequestration rates of the three minerals, and reaction equations were constructed through fitting analysis. The morphology, crystal structure, and growth characteristics of calcium carbonate products during the carbon sequestration reactions of the three minerals were analyzed using SEM, TEM, and crystal size calculations. The correlation between the differences in carbon sequestration rates among the three minerals and the evolution of micro-structure was elucidated.

Results and discussion

γ-C₂S had the highest carbon sequestration rate, which was 47.40% after 2880 min of carbon sequestration, reaching 92.65% of the theoretical carbon sequestration, and still had an exposed reaction surface at the later stage of the reaction. During the carbon sequestration process of β-C₂S, the carbon sequestration rate increases and the particle size, grain size and structure distribution of the product calcium carbonate aggregate are relatively stable. C₃S has the highest carbon sequestration rate. Due to its high reactivity, C₃S stagnates rapidly after 5 min, and then the carbon sequestration rate increases slowly, but the crystal shape of surface calcium carbonate products changes with time.

The carbon sequestration reaction processes of γ-C₂S and β-C₂S conform to BoxLucas1 model. The first 60 min is the rapid carbon sequestration stage of γ-C₂S and β-C₂S, and the inflection point of reaction rate reduction occurs in 180 min and 360 min respectively, and the reaction plateau begins at 360 min. The carbon sequestration reaction of C₃S is consistent with the nuclear shrinkage reaction model, and almost stops after 5 min. The calcite produced by the three minerals tend to grow on the (104) rhomboid plane, and the growth of calcite is controlled by the competition between grain growth and grain size reduction.

γ-C₂S and β-C₂S carbon fixation product calcium carbonate is mainly calcite, C₃S carbon fixation product calcium carbonate also contains relatively more aragonite. The growth of calcium carbonate products on the surface of γ-C₂S particles shows a transition from epitaxial growth to mantle growth. The epitaxial growth in the early stage leads to more reaction surfaces and increases the grain size of calcite. The growth of calcium carbonate products on the surface of β-C₂S particles is from mantle growth to epitaxial growth. The mantle growth in the early stage leads to denser nucleation, and the reaction ability is poor in the later stage, but the grain size development is more stable. On the surface of C₃S, calcite and aragonite are mixed, and the composite structure of acicular aragonite and brick calcite hinders the gas-solid contact reaction.

Conclusions

The development rules of carbon sequestration rate of γ-C₂S and β-C₂S are similar, and both conform to BoxLucas1 model; The calcium carbonate crystals on the surface of the two C₂S particles are dominated by calcite, and tend to grow more preferentially on the (104) thermo-dynamically stable surface. The calcium carbonate on the surface of γ-C₂S particles grows from mantle to epitaxial. The epitaxial growth in the early stage leads to a larger reaction contact surface, and it still has reactive activity in the late stage, and the calcite grain size is larger. However, β-C₂S epitaxial growth to mantle growth, the early mantle growth led to denser nucleation, the late reaction ability is poor, the grain size development is more stable. Due to its high calcium content, C₃S has the fastest carbon sequestration reaction at the initial stage, and quickly stops after 5 minutes of reaction, which conforms to the nuclear shrinkage reaction model. C₃S presents different product evolution rules: In the early stage of carbon sequestration reaction, acicular aragonite and cubic calcite on the surface of C₃S are mixed, and its dense structure causes premature stagnation of carbon sequestration reaction. As the reaction proceeds, aragonite is transformed into calcite.

Key words

dicalcium silicate / tricalcium silicate / carbon sequestration / calcium carbonate / crystal growth

引用本文

许扬帆, 钱春香, 裴嘉炜. 颗粒态γ-C₂S、β-C₂S、C₃S矿物固碳速率的差异及微观机理. 硅酸盐学报, 2025 , 53 (2) : 325 -338 . DOI: 10.14062/j.issn.0454-5648.20240269

Yangfan XU, Chunxiang QIAN, Jiawei PEI. Mechanism Investigation and Difference in Carbon Sequestration Rates of Granular γ-C₂S, β-C₂S and C₃S Minerals[J]. Journal of the Chinese Ceramic Society, 2025 , 53 (2) : 325 -338 . DOI: 10.14062/j.issn.0454-5648.20240269

基金

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国家重点研发计划项目(2021YFB3802000; 2021YFB3802004)
国家自然科学基金项目(52172016; 51738003)

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2025年第53卷第2期

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文章信息

doi: 10.14062/j.issn.0454-5648.20240269

接收时间：2024-04-08
首发时间：2026-10-22
出版时间：2025-02-20

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出版历史

收稿日期：2024-04-08
修回日期：2024-05-04

基金

国家重点研发计划项目(2021YFB3802000; 2021YFB3802004)

国家自然科学基金项目(52172016; 51738003)

作者信息

^1．东南大学材料科学与工程学院，南京 211189

^2．东南大学绿色建材与固碳利用研究中心，南京 211189

通讯作者:

钱春香（1966—），女，博士，教授。

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20240269

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2种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

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