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New insights on the immobilization of radioactive acidic liquid waste and cesium in amorphous aluminophosphate waste form 放射性酸性废液和铯在无定形磷酸铝废物形态中固定化的新认识
IF 13.1 1区 工程技术 Q1 CONSTRUCTION & BUILDING TECHNOLOGY Pub Date : 2026-05-01 Epub Date: 2026-02-14 DOI: 10.1016/j.cemconres.2026.108169
Byoungkwan Kim , Brant Walkley , Dinu Iuga , Raudhatul Islam Chaerun , Xiaobo Niu , Wooyong Um
Radioactive acidic liquid waste (RALW), generated during the Chemical Oxidation Reduction Decontamination (CORD) and High Permanganate CORD Ultraviolet (HP-CORD UV) process of primary systems in nuclear power plants, contains various heavy metals and various radionuclides. These are typically removed by organic ion exchange resins, producing large amounts of secondary spent ion exchange resins (spent IERs) waste. This study aimed to reduce spent IER generation by directly using unpurified RALW as mixing solution for amorphous aluminophosphate (AAP) waste forms which use acidic solution as a raw material. In addition, Cs that may be present in RALW was added at 10 wt% to investigate its effect on the AAP structure. Neither the use of RALW as mixing solution nor the addition of Cs significantly altered the mechanical strength of AAP waste forms. The presence of heavy metal in RALW did not substantially change the local structure of Al and P in the AAP matrix. Multiscale characterization showed that Cs was mainly immobilized by forming amorphous cesium aluminophosphate and through physical incorporation within the AAP matrix. This research demonstrates that RALW can be effectively used in AAP waste forms and provides direct evidence of Cs immobilization mechanisms in AAP systems.
放射性酸性废液(RALW)是核电站一次系统化学氧化还原除污(CORD)和高高锰酸盐CORD紫外线(HP-CORD UV)过程中产生的,含有多种重金属和多种放射性核素。这些通常由有机离子交换树脂去除,产生大量的二次废离子交换树脂(废IERs)废物。本研究旨在通过直接使用未纯化的RALW作为以酸性溶液为原料的无定形磷酸铝(AAP)废物形式的混合溶液来减少消耗的IER产生。此外,将RALW中可能存在的Cs以10 wt%的比例添加,以研究其对AAP结构的影响。使用RALW作为混合溶液和添加Cs都没有显著改变AAP废形态的机械强度。RALW中重金属的存在并未显著改变AAP基体中Al和P的局部结构。多尺度表征表明,Cs主要通过形成无定形的磷酸铝铯和在AAP基体内的物理掺入来固定。本研究表明,RALW可以有效地用于AAP废物形态,并为AAP系统中Cs的固定机制提供了直接证据。
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引用次数: 0
Influence of sodium ions on the synthesis and hydration of belite-ye'elimite-ternesite clinker 钠离子对白铝铁镁熟料合成及水化的影响
IF 13.1 1区 工程技术 Q1 CONSTRUCTION & BUILDING TECHNOLOGY Pub Date : 2026-05-01 Epub Date: 2026-02-05 DOI: 10.1016/j.cemconres.2026.108155
Jiahao Chu , Haixiao Xu , Weijie Yue , Xu Tao , Jinfeng Sun , Suhua Ma , Weifeng Li
In this study, the influences of sodium ions on the phase formation, microstructure, and hydration behavior of Belite-Ye'elimite-Ternesite (BYT) clinker were investigated. The results demonstrated that the incorporation of Na2O (derived from Na2CO3) significantly reduced the formation temperatures of primary phases—belite (2CaO·SiO2, C2S) and ye'elimite (4CaO·3Al2O3·SO3, C4A3$)—by 50 °C and 100 °C, respectively, and enhanced their formation kinetics at low temperatures (800–1000 °C). However, it also decreased the decomposition temperature of ye'elimite. The addition of Na2O had an adverse effect on the thermal stability of ternesite (5CaO·2SiO2·SO3, C5S2$), although a small amount of Na2O (≤0.5%) facilitated the formation of ternesite at low temperatures (850–950 °C). An excessive content of Na2O (≥2.0%) inhibited the formation of C5S2$ due to the reactions between Na2CO3 and CaSO4. Furthermore, Na2O stabilized β-C2S but induced lattice distortion in C4A3$. A low dosage of Na2O (0.5%) shortened the induction period by promoting AFt formation, whereas higher dosages (≥2.0%) eliminated it through rapid nucleation of U-phase (4CaO·Al2O3·1.85SO3·0.85Na2O·12H2O). The 30-h hydration degree decreased progressively with increasing Na2O dosage.
研究了钠离子对BYT熟料相形成、微观结构和水化行为的影响。结果表明,Na2O(来源于Na2CO3)的掺入显著降低了原生相白石(2CaO·SiO2, C2S)和叶极限相(4CaO·3Al2O3·SO3, C4A3$)的形成温度,分别降低了50℃和100℃,并增强了低温(800-1000℃)下的形成动力学。然而,它也降低了极限值的分解温度。Na2O的加入对铁氏体(5CaO·2SiO2·SO3, C5S2$)的热稳定性有不利影响,但少量Na2O(≤0.5%)有利于铁氏体在低温(850 ~ 950℃)下的形成。Na2O含量过高(≥2.0%)会抑制Na2CO3与CaSO4反应生成C5S2$。此外,Na2O稳定了β-C2S,但引起C4A3$的晶格畸变。低剂量Na2O(0.5%)通过促进AFt的形成缩短了诱导期,而高剂量Na2O(≥2.0%)通过u相(4CaO·Al2O3·1.85SO3·0.85Na2O·12H2O)的快速成核消除了诱导期。随着Na2O用量的增加,30 h水化程度逐渐降低。
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引用次数: 0
An investigation of sorption and shrinkage in cement paste using a novel framework integrating a DFT-based interlayer pore model 利用基于dft的层间孔隙模型的新框架研究水泥浆体的吸附和收缩
IF 13.1 1区 工程技术 Q1 CONSTRUCTION & BUILDING TECHNOLOGY Pub Date : 2026-05-01 Epub Date: 2026-02-13 DOI: 10.1016/j.cemconres.2026.108153
Peng Zhang , Xiao-Fei Hu , Ming-Feng Kai , Jian-Guo Dai
The complexity of cement paste's multiscale pore structure, encompassing interlayer, gel, and capillary pores, presents a significant modeling challenge due to the absence of a unified theory specifically addressing interlayer pores. A novel DFT-based interlayer pore model is developed and integrated into a physicochemical framework to simulate the water sorption and shrinkage of cement paste, and validated with extensive experimental data. Results reveal that sorption hysteresis arises from combined multiscale porosity at high relative humidity (RH) but is solely governed by interlayer pores at low RH, where, accordingly, the scanning loop hysteresis vanishes due to cavitation. Moreover, interlayer pores are the predominant source of macroscopic shrinkage and its hysteresis of cement paste, followed by the contribution from pore surface sorption. Elevated temperatures reduce both water content and shrinkage, with the impact being most significant on water content during desorption and on shrinkage during adsorption.
由于缺乏专门针对层间孔隙的统一理论,水泥浆体的多尺度孔隙结构(包括层间孔隙、凝胶孔隙和毛细孔隙)的复杂性给建模带来了重大挑战。建立了一种新的基于dft的层间孔隙模型,并将其整合到物理化学框架中来模拟水泥浆体的吸水和收缩,并通过大量的实验数据进行了验证。结果表明,在高相对湿度条件下,吸附滞后是由复合多尺度孔隙引起的,而在低相对湿度条件下,吸附滞后完全由层间孔隙控制,扫描环滞后由于空化而消失。层间孔隙是水泥浆体宏观收缩及其滞后的主要来源,其次是孔隙表面吸附的贡献。升高的温度降低了含水量和收缩率,其中对解吸过程中的含水量和吸附过程中的收缩率的影响最为显著。
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引用次数: 0
Enhanced flowability of metakaolin-blended cement through the synergistic effect of polycarboxylate superplasticizer and retarder: Competitive adsorption and retarded hydration 通过聚羧酸型高效减水剂和缓凝剂的协同作用增强偏高岭土水泥的流动性:竞争性吸附和缓凝水化
IF 13.1 1区 工程技术 Q1 CONSTRUCTION & BUILDING TECHNOLOGY Pub Date : 2026-04-01 Epub Date: 2026-01-19 DOI: 10.1016/j.cemconres.2026.108142
Ye Pan , Zichen Lu , Xinyang Li , Hongwei Tian , Zhen Xiang , Xiangming Kong , Zhenping Sun
The synergistic effect of polycarboxylate superplasticizer (PCE) and two typical retarders (sodium citrate (SC) and sucrose (SU)) on the flowability of metakaolin (MK)-blended cement (MKC) was investigated by mini-cone tests, rheometer, total organic carbon analysis, and calorimeter. Results show that the co-addition of retarder and PCE not only improves the initial flowability but also the flowability retention of MKC paste. Further analysis indicates that the synergistic effect on initial flowability essentially originates from the competitive adsorption of PCE and retarder. The competitive adsorption of retarder on ordinary Portland cement (OPC) could enable an increased amount of available PCE to be adsorbed on MK, which is beneficial for breaking MK agglomeration and ultimately leading to increased initial flowability. Increased flowability retention is attributed to retarded cement hydration and suppressed pozzolanic reactions of MK, which limit the formation of hydration products and the increase in new surface area, thereby slowing down the consumption of PCE.
采用微锥试验、流变仪、总有机碳分析和量热法研究了聚羧酸酯型高效减水剂(PCE)与柠檬酸钠(SC)和蔗糖(SU)两种典型缓凝剂对偏高岭土水泥(MKC)流动性的协同作用。结果表明,缓速剂与PCE的共掺不仅提高了MKC膏体的初始流动性,而且提高了其流动性保持率。进一步分析表明,对初始流动性的协同效应主要来自于PCE和缓凝剂的竞争吸附。缓凝剂在普通硅酸盐水泥(OPC)上的竞争性吸附可以增加MK上有效PCE的吸附量,有利于破坏MK的结块,最终提高初始流动性。流动性保持性的增加是由于水泥水化迟缓和MK的火山灰反应受到抑制,这限制了水化产物的形成和新表面积的增加,从而减缓了PCE的消耗。
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引用次数: 0
Evaluation of atmospheric CO₂ sequestration by 50-year-old concrete structures based on 14C and 13C measurements 基于14C和13C测量的有50年历史的混凝土结构对大气CO 2封存的评价
IF 13.1 1区 工程技术 Q1 CONSTRUCTION & BUILDING TECHNOLOGY Pub Date : 2026-04-01 Epub Date: 2026-01-10 DOI: 10.1016/j.cemconres.2025.108129
Ippei Maruyama , Haruka Takahashi , Yoshihiro Asahara , Hidekazu Yoshida , Abudushalamu Aili , Masayo Minami
This study examines the long-term sequestration of atmospheric CO₂ as an inorganic carbonate through carbonation in concrete structures. Two buildings, each approximately 50 years old, were analyzed using two cores per structure. Measurements of radiocarbon (14C) concentration, δ13C, and total inorganic carbon (TIC) of the core samples were conducted. For one building containing limestone aggregate, additional analyses, visual inspection, polarized light microscopy, and X-ray diffraction with Rietveld refinement were performed to evaluate the material and mineral distributions. The results indicate that δ13C varies with pH changes during carbonation, while the concentration of 14C reflects the historical fluctuations in atmospheric 14C. By applying the √t relationship for carbonation depth, the amount of CO₂ fixed from the atmosphere can be determined, even in the presence of limestone aggregate. This study provides a methodology for assessing long-term CO₂ sequestration in existing concrete structures.
本研究考察了通过混凝土结构中的碳化作用对大气中二氧化碳作为无机碳酸盐的长期封存。两栋大约有50年历史的建筑,每个结构使用两个核心进行分析。测定了岩心样品的放射性碳(14C)浓度、δ13C和总无机碳(TIC)。对于一个含有石灰石骨料的建筑,进行了额外的分析、目视检查、偏振光显微镜和Rietveld细化的x射线衍射来评估材料和矿物分布。结果表明,碳酸化过程中δ13C随pH变化而变化,而14C浓度反映了大气14C的历史波动。通过应用碳酸化深度的√t关系,可以确定大气中固定的CO₂的量,即使存在石灰石骨料。该研究为评估现有混凝土结构的长期CO₂封存提供了一种方法。
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引用次数: 0
Elucidating the behavior, kinetics and mechanism of wet carbonation in ternesite 阐述了镁铁石湿碳化的行为、动力学和机理
IF 13.1 1区 工程技术 Q1 CONSTRUCTION & BUILDING TECHNOLOGY Pub Date : 2026-04-01 Epub Date: 2026-01-21 DOI: 10.1016/j.cemconres.2026.108144
Jixin Zhang , Kai Cui , Jun Chang
In this study, the carbonation kinetics, phase development, and microstructure evolution of ternesite (C5S2$) phase were investigated via wet carbonation. The results indicated that ternesite exhibited remarkable carbonation reactivity, achieving approximately 95% completion of the carbonation reaction within 15 min and facilitating CO2 sequestration exceeding 340 g per kilogram of ternesite. The main carbonation products identified were aragonite, calcite, gypsum, and silica gel (Si-gel). The carbonation kinetics conformed to the surface coverage model, with the reaction proceeding through distinct stages of acceleration, deceleration, and stabilization, ultimately resulting in the formation of a “core-shell” structure. Notably, the crystalline phase of calcium carbonate (CC) underwent spontaneous transformation during the carbonation of ternesite. It is observed that CC exhibited a polycrystalline structure and underwent a distinct phase transformation from calcite to aragonite. The resulting CC was predominantly metastable, exhibiting low crystallinity and reduced crystallite size. These characteristics are attributed to the intrinsic properties of ternesite, particularly the presence of SO42− ions, which promote the formation and stabilization of metastable aragonite. Furthermore, the changes in crystalline and morphology of CC, induced by dissolution and re-precipitation process, disrupted the CC layer and thereby facilitated the release of another significant product, Si-gel. These distinctive carbonation behaviors suggest that ternesite has potential for broader applications, including its use as a supplementary cementitious material or as a precursor for the synthesis of high value-added products such as aragonite whiskers and nano-sized SiO2.
本文研究了湿法碳化法对铁氏体(C5S2$)相的碳化动力学、相发育和微观结构演变的影响。结果表明,钛辉石具有显著的碳化反应活性,在15 min内完成约95%的碳化反应,每千克钛辉石的CO2固存量超过340 g。鉴定出的主要碳酸化产物为文石、方解石、石膏和硅胶。碳化动力学符合表面覆盖模型,反应过程经历了不同的加速、减速和稳定阶段,最终形成“核-壳”结构。值得注意的是,碳酸钙(CC)的结晶相在钙镁石碳酸化过程中发生了自发转变。观察到CC呈现出多晶结构,并经历了明显的方解石到文石的相变。所得到的CC主要是亚稳态的,表现出低结晶度和减小的晶粒尺寸。这些特征是由于文石的固有性质,特别是SO42−离子的存在,促进了亚稳文石的形成和稳定。此外,由溶解和再沉淀过程引起的CC晶体和形态的变化破坏了CC层,从而促进了另一重要产物Si-gel的释放。这些独特的碳化行为表明钛石具有更广泛的应用潜力,包括作为补充胶凝材料或作为合成高附加值产品(如文石晶须和纳米SiO2)的前驱体。
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引用次数: 0
Insights into the nano- and microstructures of cementitious materials using synchrotron X-rays 利用同步加速器x射线观察胶凝材料的纳米和微观结构
IF 13.1 1区 工程技术 Q1 CONSTRUCTION & BUILDING TECHNOLOGY Pub Date : 2026-04-01 Epub Date: 2026-01-27 DOI: 10.1016/j.cemconres.2026.108150
Miguel A.G. Aranda , Angeles G. De la Torre , Susan A. Bernal , John L. Provis
Synchrotron X-ray techniques have been extensively applied to characterise the mineralogy of anhydrous cementitious materials, the hydration processes and products in cementitious systems, and the alterations induced by different environmental exposure conditions. However, with changes in cement compositions and performance requirements, and an increased focus on materials design for sustainability, there is now strong emphasis on the use of advanced analytical tools to bring fundamentally based, multi-scale, multi-modal, spatially-resolved and/or time-resolved understanding of the physico-chemical factors influencing cementitious materials in the fluid, hardening and cured states. Beamline-based analysis complements conventional laboratory techniques, bringing unique capabilities to develop high-level insights. Here we provide a critical overview of the application of synchrotron radiation-based techniques to cementitious materials, and the opportunities and research needs to unlock their full potential for their use in future cement materials research, including issues related to handling and processing the very large datasets that can be generated.
同步加速器x射线技术已被广泛应用于表征无水胶凝材料的矿物学、胶凝体系中的水化过程和产物,以及不同环境暴露条件引起的变化。然而,随着水泥成分和性能要求的变化,以及对材料可持续性设计的日益关注,现在非常重视使用先进的分析工具,以从根本上、多尺度、多模式、空间分辨率和/或时间分辨率来理解影响胶凝材料在流体、硬化和固化状态下的物理化学因素。基于光束线的分析补充了传统的实验室技术,带来了独特的能力,以开发高层次的见解。在这里,我们提供了基于同步辐射技术在水泥材料中的应用的关键概述,以及在未来水泥材料研究中释放其全部潜力的机会和研究需求,包括与处理和处理可能产生的非常大的数据集相关的问题。
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引用次数: 0
The dynamic dissolution mechanism of copper ions on the surface of hydrated calcium silicate (C-S-H): A molecular simulation study based on MetaDynamics 铜离子在水合硅酸钙(C-S-H)表面的动态溶解机理:基于元动力学的分子模拟研究
IF 13.1 1区 工程技术 Q1 CONSTRUCTION & BUILDING TECHNOLOGY Pub Date : 2026-04-01 Epub Date: 2026-01-23 DOI: 10.1016/j.cemconres.2026.108140
Yue Zhang , Fengxiao Zhu , Pan Wang , Muhan Wang , Xinpeng Wang , Yunqi Liu , Jing Guan , Fengxia Xu , Yizhao Gao , Peixuan Shen , Dongshuai Hou
Immobilizing Cu2+ from copper tailings in cement is crucial, yet its atomic-scale mechanism remains poorly understood. Using ab initio metadynamics, we delineate the complete multi-step leaching pathway of Cu2+ from a C-S-H surface, characterized by two distinct energy barriers. Initial detachment involves a stepwise ligand exchange, with the first barrier primarily dictated by the rupture of the Cu-Osi covalent bond. A highly stable, singly-anchored intermediate (State C) is maintained by a novel “triple-lock” of secondary interactions: a direct H-bond, a water-mediated bridge, and Ca-Ow coordination. This robust anchoring significantly contributes to the higher second energy barrier for complete dissolution. Final desorption is governed by a compensatory mechanism where the hydrated ion reinforces internal stability as the “triple-lock” gradually weakens. Crucially, Cu2+ adopts a labile, four-coordinate geometry throughout, challenging previous rigid six-coordinate models and offering fundamental insights for designing environmentally robust cementitious materials.
水泥中铜尾矿中Cu2+的固定化至关重要,但其原子尺度机制尚不清楚。利用从头算元动力学,我们描绘了从C-S-H表面上Cu2+的完整多步骤浸出过程,其特征是两个不同的能量势垒。初始分离涉及逐步的配体交换,第一个势垒主要由Cu-Osi共价键的断裂决定。高度稳定的单锚定中间体(状态C)是由一种新型的“三重锁”二级相互作用维持的:直接氢键、水介导的桥和Ca-Ow配位。这种坚固的锚定显著地促进了完全溶解的更高的第二能垒。最终的解吸是由一种补偿机制控制的,当“三重锁”逐渐减弱时,水合离子加强了内部稳定性。至关重要的是,Cu2+采用了一种不稳定的四坐标几何结构,挑战了以前的刚性六坐标模型,并为设计环保坚固的胶凝材料提供了基本见解。
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引用次数: 0
Adsorption mechanism of PCE superplasticizers in alkali activated materials containing silica fume PCE高效减水剂在含硅灰碱活性材料中的吸附机理
IF 13.1 1区 工程技术 Q1 CONSTRUCTION & BUILDING TECHNOLOGY Pub Date : 2026-04-01 Epub Date: 2026-01-21 DOI: 10.1016/j.cemconres.2026.108143
Denis Kosenko , Alexander Wetzel , Bernhard Middendorf
Fluorescence and scanning electron microscopy were used to investigate hydroxide-activated slag-silica fume-based AAM mixes containing PCE superplasticizers. By applying two distinct fluorescent markers, the competitive adsorption of two PCEs with differing charge densities was observed. The results indicate that each PCE exhibits a location-specific affinity for certain topographical features of the precursor surface, as adsorption on the amorphous material is heterogeneous and varies significantly between the superplasticizers. Through the location-dependent investigations, the PCE on particle coverage levels of the particles were approximated at specific times and correlated with rheological measurements. A high charge density causes a high initial dispersion of the paste with a rapidly decreasing effect, while a lower charge density has a weaker but more persistent effect effect. A comparison of the spatially resolved adsorption derived from the fluorescence signal with the obtained scanning electron microscopy investigations shows that the tested PCEs used attach primarily to the early formed reaction products.
采用荧光显微镜和扫描电镜对含PCE高效减水剂的氢氧化物活化渣-硅烟基AAM混合物进行了研究。应用两种不同的荧光标记,观察了两种不同电荷密度的pce的竞争吸附。结果表明,每个PCE对前驱体表面的某些地形特征表现出特定位置的亲和力,因为在非晶材料上的吸附是不均匀的,并且在不同的高效减水剂之间差异很大。通过位置相关的研究,在特定时间,颗粒覆盖水平的PCE近似与流变测量相关联。高电荷密度导致膏体初始分散度高且效果迅速降低,而低电荷密度则具有较弱但更持久的效果。由荧光信号得到的空间分辨吸附与扫描电镜观察结果的比较表明,所测试的pce主要附着在早期形成的反应产物上。
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引用次数: 0
Environmental assessment of several paths toward a carbon neutral ready-mixed concrete sector 通往碳中性预拌混凝土行业的几种途径的环境评估
IF 13.1 1区 工程技术 Q1 CONSTRUCTION & BUILDING TECHNOLOGY Pub Date : 2026-04-01 Epub Date: 2026-01-28 DOI: 10.1016/j.cemconres.2026.108148
Snežana Marinković , Petar Bajić , Nikola Tošić
To prevent serious consequences of climate change, it is essential to reduce greenhouse gas emissions, especially CO₂. The concrete industry, largely made up of ready-mixed reinforced concrete (RC), is a key part, as concrete is produced more than all other construction materials combined. This study evaluates decarbonization strategies in the RC sector, including low-clinker concrete (concrete with limestone calcined clay cement - LC3 and high-volume limestone powder concrete - HVLPC), carbon capture and storage (CCS) and concrete with carbonated recycled aggregates (CRAC). Life cycle assessment was conducted on a typical RC floor slab under current and future conditions, including CCS and full electricity decarbonization. Results show a 60%–90% CO₂ reduction at the concrete level, but only ∼50% overall due to reinforcement impact—insufficient for net-zero under the assumptions made in this study. The best option combines HVLPC, oxyfuel CCS, and green electricity. With CCS and fully decarbonized electricity implemented in the future scenario, differences between conventional and low-clinker concretes drop below 10%. Possible mitigation strategies that can contribute to achieving carbon neutrality in the RC sector are decarbonization of the steel sector, increasing bioenergy and/or green hydrogen use in the kiln's fuel mix and decarbonization of transport.
为了防止气候变化的严重后果,必须减少温室气体,特别是二氧化碳的排放。混凝土工业,主要由预拌钢筋混凝土(RC)组成,是一个关键部分,因为混凝土的产量超过了所有其他建筑材料的总和。本研究评估了混凝土行业的脱碳策略,包括低熟料混凝土(石灰石煅烧粘土水泥混凝土- LC3和大体积石灰石粉末混凝土- HVLPC),碳捕获和储存(CCS)和碳化再生骨料混凝土(CRAC)。对某典型RC楼盖在当前和未来条件下进行了生命周期评估,包括CCS和全电脱碳。结果显示,在混凝土层面上,二氧化碳减少了60%-90%,但由于钢筋的影响,总体上只减少了~ 50%——在本研究的假设下,这不足以实现净零排放。最好的选择是结合HVLPC、氧燃料CCS和绿色电力。随着CCS和完全脱碳电力在未来的实施,传统混凝土和低熟料混凝土之间的差异将降至10%以下。有助于在钢筋混凝土部门实现碳中和的可能缓解战略有:钢铁部门脱碳、在窑炉燃料组合中增加生物能源和/或绿色氢的使用以及运输脱碳。
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引用次数: 0
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Cement and Concrete Research
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