Modeling and experimental validation of carbonation mechanism of ye’elimite-gypsum-water system

IF 3.4 3区工程技术 Q2 CONSTRUCTION & BUILDING TECHNOLOGY

Materials and Structures Pub Date : 2025-05-08 DOI:10.1617/s11527-025-02662-5

Yangyang Zhang, Qunli Zhang, Jun Chang, Hang Yang, Siqi Ding, Xiaozhou Liu, Kai Wu, Qingxin Zhao

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Abstract

Calcium sulfoaluminate cement is a promising low-carbon alternative to Portland cement, and the carbonation of its hydration products influences its mechanical performance. However, a comprehensive theoretical model describing its carbonation mechanism remains elusive. This paper established a theoretical reaction range, including different zones and boundaries for ye’elimite (C₄A₃S̅)-gypsum (CS̅H₂)-water (H₂O)-carbon dioxide (CO₂) system via priority-based theoretical calculations of chemical reactions. The reactions and product evolution within each boundary and zone were summarized. A theoretical database was obtained, including the change of Gibbs energy and enthalpy, solid volume and chemical volume, and the theoretical carbon absorption. Calculation results reveal that the reactions of each zone and boundary occur spontaneously and exothermically. The solid volume increases, while the chemical volume decreases conversely. The maximum carbon absorption of 1 mol C₄A₃S̅ is 3 mol theoretically regardless of the amount of gypsum. The modeling obtained by Gibbs Energy Minimization software (GEMS-PSI) and experimental verification were carried out to validate the fidelity of the established theoretical reaction range, which demonstrate that the evolution of carbonation products in each zone and boundary was in line with the theoretical calculations. Compared with GEMS modeling, the theoretical reaction range can distinguish the source of ettringite in detail, and provide a more direct and insightful representation of carbonation process.

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石灰-石膏-水体系碳酸化机理建模与实验验证

硫铝酸钙水泥是一种很有前途的低碳硅酸盐水泥替代品，其水化产物的碳化影响其力学性能。然而，一个全面的理论模型描述其碳化机理仍然是难以捉摸的。本文通过基于优先级的化学反应理论计算，建立了极限值(C4A3S - H2O)-石膏(CS - H2)-水(H2O)-二氧化碳（CO2）体系的理论反应范围，包括不同的区域和边界。总结了各边界和区域内的反应和产物演化。建立了包括吉布斯能和焓的变化、固体体积和化学体积以及理论碳吸收率的理论数据库。计算结果表明，各区域和边界的反应是自发和放热的。固体体积增大，化学体积减小。无论石膏用量多少，1 mol C4A3S的最大吸碳量理论上均为3 mol。利用Gibbs Energy Minimization软件（GEMS-PSI）建立模型并进行实验验证，验证了建立的理论反应范围的保真度，表明各区域和边界碳酸化产物的演化与理论计算一致。与GEMS模型相比，理论反应范围可以更详细地区分钙矾石的来源，为碳酸化过程提供更直接、更深刻的表征。

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

Materials and Structures 工程技术-材料科学：综合

CiteScore

6.40

自引率

7.90%

发文量

222

审稿时长

5.9 months

期刊介绍： Materials and Structures, the flagship publication of the International Union of Laboratories and Experts in Construction Materials, Systems and Structures (RILEM), provides a unique international and interdisciplinary forum for new research findings on the performance of construction materials. A leader in cutting-edge research, the journal is dedicated to the publication of high quality papers examining the fundamental properties of building materials, their characterization and processing techniques, modeling, standardization of test methods, and the application of research results in building and civil engineering. Materials and Structures also publishes comprehensive reports prepared by the RILEM’s technical committees.