Article(id=1321944773104087959, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1321944712408314326, articleNumber=null, orderNo=null, doi=10.14062/j.issn.0454-5648.20250720, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1759075200000, receivedDateStr=2025-09-29, revisedDate=1760284800000, revisedDateStr=2025-10-13, acceptedDate=null, acceptedDateStr=null, onlineDate=1793105794454, onlineDateStr=2026-10-27, pubDate=1773936000000, pubDateStr=2026-03-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1793105794454, onlineIssueDateStr=2026-10-27, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1793105794454, creator=13701087609, updateTime=1793105794454, updator=13701087609, issue=Issue{id=1321944712408314326, tenantId=1146029695717560320, journalId=1263187385517883426, year='2026', volume='54', issue='3', pageStart='821', pageEnd='1176', issueExtLink='null', onlineDate='null', pubDate='1770652800000', pubDateStr='2026-02-10', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1793105779983, creator='13701087609', updateTime=1793105779983, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext=null, issueFiles=null, downloadFileDto=null}, startPage=957, endPage=969, ext={EN=ArticleExt(id=1321944774618231704, articleId=1321944773104087959, tenantId=1146029695717560320, journalId=1263187385517883426, language=EN, title=Solid Solution Tendency of Manganese Ions in Low Calcium Carbonatable Binder and Their Impact on Carbonation Performance, columnId=1321944713276535255, journalTitle=Journal of the Chinese Ceramic Society, columnName=Special Issue on Genes and AI-Based Design of Cement-Based Materials—Research Articles, runingTitle=null, highlight=null, articleAbstract=
Introduction The global cement industry is a major source of CO2 emissions, making its green transition an urgent priority. Utilizing industrial solid waste to prepare low calcium carbonatable binder (LCCB) is considered as a promising approach that can simultaneously achieve solid waste valorization and CO2 sequestration. However, some impurity ions commonly appeared in solid waste, such as Mn ions from manganese slag, can dissolve into the mineral phases of LCCB, affecting its structure and carbonation behavior. The mechanisms underlying these effects remain unclear, hindering the optimization of material performance. This study was to clarify the solid solution behavior of Mn ions in LCCB and their mechanism of action during the carbonation process. The doping behavior of Mn ions in the main mineral phases was analyzed and their influence on the carbonation reactivity and microstructural evolution of the material was discussed via combining density functional theory calculations with experimental validation. This work could provide a theoretical basis for the design of high-performance LCCB materials based on manganese-containing solid waste.
Methods LCCB clinker was synthesized with analytical-grade chemicals. To investigate the doping effect of Mn ions, MnO2 was incorporated at varying levels (i.e., 0%(in mass), 0.15%, 0.25%, and 0.50%). The raw mixtures were calcined at 1280 ℃ for 120 min, followed by rapid cooling. The resulting clinker was ground and subsequently compacted at 4 MPa to form the specimens, which were then subjected to carbonation curing in 0.3 MPa CO2 (99.9% purity) for 8 h. The microstructural morphology and elemental distribution were determined by scanning electron microscopy (SEM) equipped with energy-dispersive X-ray spectrometry (EDS) and backscattered electron (BSE) detection analysis. The phase composition was characterized by X-ray diffraction (XRD) coupled with Rietveld refinement. The CO2 uptake was determined by thermogravimetric analysis (TGA), while the carbonation reactivity was assessed by isothermal calorimetry. The pore structure was characterized by low-field nuclear magnetic resonance (LF-NMR). The compressive strength was measured on a WDW-200 testing machine at a constant loading rate of 0.5 mm/min. Furthermore, the crystal models of CS, C3S2, and C2AS were constructed based on the first-principles calculations to investigate the doping behavior of Mn ions.
Results and discussion This study reveals that Mn ion doping significantly enhances the carbonation hardening performance of LCCB via reducing the total bond order density of Ca—O bonds. Mn ions preferentially occupy Ca sites in LCCB, primarily because this substitution pathway has the lowest defect formation energy, and the resulting Mn-O bonds exhibit a chemical environment that is highly similar to the original Ca—O bonds, while maintaining analogous orbital hybridization characteristics. At an MnO2 doping level of 0.5%, the material properties are improved. After 8-h carbonation, the compressive strength is increased by 80.70%, compared to the blank group, and the porosity is decreased to 20.29%. Mn doping promotes the formation of more CaCO3, and its content is increased by 47.42% relative to the blank group, significantly increasing the proportion and thermal stability of calcite. The carbonation reaction calorimetry analysis shows that the exothermic peak and cumulative heat release in the doped system both increase, indicating a higher degree of reaction. The aforementioned enhancement effects are mainly attributed to the reduction in the total bond order density of Ca—O bonds due to Mn doping, which weakens the lattice's restraint on Ca2+, thereby promoting its dissolution and accelerating the carbonation reaction process. The microstructural analysis demonstrates that Mn doping leads to carbonation products dominated by layered calcite, forming a dense network-like skeleton. Meanwhile, unreacted mineral phases are encapsulated by amorphous phases, and CaCO3 effectively fills pores, collectively contributing to the improvement in mechanical properties. This research provides a theoretical basis for the high-value utilization of manganese-containing solid waste in low-carbon cementitious materials.
Conclusions The results indicated that Mn ion doping and its promoting effect on carbonation performance could be highly significant, especially at the optimal doping level (i.e., 0.5%). Under this condition, the carbonated samples exhibited a compressive strength increase of 80.70%, a porosity reduction of 20.29%, and a CO2 uptake enhancement of 47.42%, compared to the blank group. Mn ions could substitute Ca sites and dissolve into various mineral phases of LCCB, inducing a lattice contraction and a rightward shift in diffraction peaks. This could weaken the total bond order density of Ca—O bonds, facilitating Ca2+ dissolution and accelerating the carbonation reaction process. Furthermore, doping could promote the formation of calcite with a higher thermal stability, whose layered stacking structure significantly improved the material densification and mechanical properties. This study could provide a theoretical basis and technical pathway for the resource utilization of manganese-containing solid waste in high-performance, low-carbon cementitious materials, having an important value for promoting the green transition of the cement industry.
, authors=Qixiang WU, Zuolin WANG, Yuhan WANG, Genshen LI, Songhui LIU, Xuemao GUAN, Xinhao WANG, Tongjing LIU, Jianping ZHU, authorsList=Qixiang WU, Zuolin WANG, Yuhan WANG, Genshen LI, Songhui LIU, Xuemao GUAN, Xinhao WANG, Tongjing LIU, Jianping ZHU, authorCompany=null, correspAuthors=Jianping ZHU, authorNote=
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全球水泥工业的碳排放问题日趋严峻，冶金固废中重金属离子的迁移与积累也带来潜在环境风险。本工作以锰渣等典型固废中所含的锰（Mn）离子为研究对象，综合运用第一性原理计算与多尺度实验方法，系统探讨了Mn离子在低钙固碳胶凝材料（LCCB）中的固溶倾向及对其碳化硬化性能和碳化活性的作用机制。结果表明，Mn离子在LCCB各矿物相中倾向于取代Ca位点。适量Mn离子可显著提升材料的碳化硬化性能，在最优掺量下，碳化8 h后试样的抗压强度较空白组提高80.70%，孔隙率降至20.29%，CaCO3生成量增加47.42%，方解石含量及其热稳定性提高，碳化反应放热增强。机理分析表明，Mn离子的掺杂降低了Ca—O键的总键序密度，削弱了晶格对Ca2+的束缚，从而促进其溶出并加快碳化反应进程。本工作为含锰固废在高性能固碳材料中的资源化利用提供了理论依据与技术参考。
, authors=武琦翔, 王祚麟, 王雨晗, 李根深, 刘松辉, 管学茂, 王心昊, 刘彤景, 朱建平, authorsList=武琦翔, 王祚麟, 王雨晗, 李根深, 刘松辉, 管学茂, 王心昊, 刘彤景, 朱建平, authorCompany=null, correspAuthors=朱建平, authorNote=
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朱建平（1978—），男，博士，教授。
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WU Qixiang (1995-), male, Doctoral candidate. E-mail: 512740415@qq.com
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WU Qixiang (1995-), male, Doctoral candidate. E-mail: 512740415@qq.com
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武琦翔（1995—），男，博士研究生。
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武琦翔（1995—），男，博士研究生。
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