Performance improvement and the mechanisms of red mud oxygen carrier in chemical looping gasification using strontium doping strategy

IF 13.2 1区 工程技术 Q1 ENGINEERING, CHEMICAL Chemical Engineering Journal Pub Date : 2025-02-22 DOI:10.1016/j.cej.2025.160772
Xiao Li, Rui Dong, Rumeng Zhang, Yi Zhang, Pengfei Lu, Xianliang Meng, Pei Li
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Abstract

Red mud, a kind of solid waste from aluminum industry, is rich in Fe2O3, which may serve as oxygen carrier in chemical looping gasification process. However, its inborn properties have brought about inevitable disadvantages, such as low reactivity. In order to enhance performance of red mud, strontium doping strategy was adopted and the mechanisms of promotive effects of strontium were investigated in this work. The results indicate that the temperature required for triggering gasification reactions was lowered by strontium. Meanwhile, strontium addition suppressed the reactions between lattice oxygens and CO. Therefore, syngas yield showed a clear upward trend with high strontium content, reaching up to 122.42 mmol/g at maximum. Gas product distribution was significantly influenced by reaction temperature, found to be optimal at 1050 °C. As the quantity of oxygen carrier added increased, tar cracking was promoted. Nevertheless, syngas underwent deep oxidation with O/C ratio exceeding three. Regarding mechanisms, after strontium was doped, Fe element mainly existed in the form of SrFeO3 and SrFe12O19. Sr-Fe-O solid solution was formed within red mud and it induced local stress, leading to that fissure progression to deeper levels and facilitating lattice oxygen migration. Moreover, strontium increased specific surface area and pore volume of oxygen carrier while reducing pore size. H2-TPR curves of red mud exhibited two obvious peaks corresponding to separate reduction of Fe2O3 → FeO → Fe. In contrast, oxygen carrier doped with strontium only displayed a single peak owing to direct reduction of SrFeO3 and SrFe12O19 to Fe. To conclude, strontium doping strategy is proved to be feasible for the complex reaction systems represented by red mud to achieve control of chemical looping gasification process.
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采用锶掺杂策略改善赤泥氧载体化学环气化性能及机理
赤泥是铝工业的一种固体废弃物,富含Fe2O3,可作为化学环气化过程中的氧载体。然而,其固有的性质也带来了不可避免的缺点,如反应性低。为了提高赤泥的性能,采用了锶掺杂策略,并对锶的促进作用机制进行了研究。结果表明,锶降低了气化反应所需的温度。同时,锶的加入抑制了晶格氧与CO的反应,因此,在锶含量较高的情况下,合成气产率有明显的上升趋势,最高可达122.42 mmol/g。反应温度对产物分布有显著影响,反应温度为1050 ℃时产物分布最优。随着氧载体添加量的增加,焦油裂解速度加快。合成气发生深度氧化,O/C值大于3。在机理上,锶掺杂后,铁元素主要以SrFeO3和SrFe12O19的形式存在。赤泥内部形成Sr-Fe-O固溶体,引起局部应力,导致裂缝向深部发展,促进晶格氧迁移。此外,锶增加了氧载体的比表面积和孔容,减小了孔隙尺寸。赤泥的H2-TPR曲线呈现出两个明显的峰,对应于Fe2O3分别还原 → FeO → Fe。相比之下,掺杂锶的氧载流子由于SrFeO3和SrFe12O19直接还原为Fe,只显示出单峰。综上所述,锶掺杂策略在以赤泥为代表的复杂反应体系中实现化学环气化过程控制是可行的。
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来源期刊
Chemical Engineering Journal
Chemical Engineering Journal 工程技术-工程:化工
CiteScore
21.70
自引率
9.30%
发文量
6781
审稿时长
2.4 months
期刊介绍: The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.
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