γ型硅酸二钙（γ-C₂S）基固碳胶凝材料是一种具有快硬高强、永久封存CO₂等特性的新型低碳胶凝材料。然而，在实际生产中，工业原料或固体废弃物的使用会在原有钙、硅体系中引入的铁、铝杂质，在高温煅烧时形成铁相固溶体（Ca₂Al_xFe_2–xO₅，0≤x<1.4）。现有研究认为铁相自身的碳化活性较低，但其在固碳胶凝材料复合体系中的作用机制尚不明确。本研究选取一种典型的铁相组成—铁铝酸四钙（C₄AF），旨在系统揭示其对γ-C₂S基固碳胶凝材料碳化性能的影响规律。实验制备了高纯度的C₄AF单矿以及γ-C₂S基固碳胶凝材料，并采用ICP、QXRD、SEM等测试方法对不同C₄AF含量样品的碳化性能及产物的组成结构进行表征。结果表明，C₄AF在γ-C₂S基固碳胶凝材料体系中具有显著的碳化促进作用。当C₄AF含量为30 wt.%时，碳化样品的抗压强度提升53.25%，达120.9 MPa。C₄AF一方面通过抑制碳化前期剧烈放热、减缓水分蒸发，为后期反应的持续进行创造条件；另一方面通过调控碳酸钙晶型，显著提高纳米级球霰石的含量，有效降低制品孔隙率。研究为优化固碳胶凝材料的组成设计及含铁、铝固废的高效利用提供了重要的理论依据。

γ-Dicalcium silicate (γ-C₂S)-based carbonatable binder is a novel low-carbon cementitious material featuring rapid hardening, high strength, and permanent CO₂ sequestration. However, during actual production, the use of industrial raw materials or solid wastes introduces iron and aluminum impurities into the original calcium‑silicate system, forming ferrite solid solutions (Ca₂Al_xFe_2-xO₅, 0≤x<1.4) upon high‑temperature calcination. Existing studies generally consider the intrinsic carbonation reactivity of ferrite phases to be low, yet their role in the composite system of carbonatable binders remains unclear. In this study, a typical ferrite phase composition, tetracalcium aluminoferrite (C₄AF), was selected to systematically reveal its influence on the carbonation performance of γ-C₂S ‑based carbonatable binders. High‑purity C₄AF single mineral and γ-C₂S‑based carbonatable binder were prepared, and the carbonation performance as well as the composition and structure of the products of samples with different C₄AF contents were characterized by ICP, QXRD, SEM, and other techniques. The results show that C₄AF plays a significant promoting role in the γ-C₂S‑based carbonatable binder system. At a C₄AF content of 30 wt.%, the compressive strength of the carbonated specimens increased by 53.25%, reaching 120.9 MPa. On one hand, C₄AF inhibits the vigorous exothermic reaction at the early carbonation stage and slows down water evaporation, thereby creating favorable conditions for sustained later‑stage reactions. On the other hand, it regulates the calcium carbonate polymorph, significantly increasing the content of nano‑sized vaterite and effectively reducing the porosity of the products. This study provides an important theoretical basis for optimizing the composition design of carbonatable binder and the efficient utilization of iron‑ and aluminum‑containing solid waste.