基于电化学机理的铝酸钠溶液中黄铁矿的定向转化脱硫还原赤泥

IF 5.6 3区 材料科学 Q1 ELECTROCHEMISTRY Electrochimica Acta Pub Date : 2025-05-10 Epub Date: 2025-02-26 DOI:10.1016/j.electacta.2025.145926
Zhaohua Zeng , Guihua Liu , Tiangui Qi , Qiusheng Zhou , Zhihong Peng , Leiting Shen , Yilin Wang , Xiaobin Li , Yuming Zhang
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引用次数: 0

摘要

高浓度铝酸钠溶液中黄铁矿在高温下的定向转化有利于脱硫和赤泥的还原,实现含硫铝土矿的绿色利用。通过Bromley模型计算活度系数,得到了Fe-S-H2O在298 K和533 K时的φφ-ρ(Na2O)ρ(Na2O)图。调节电位、烧碱浓度和温度可以使黄铁矿定向转化为S2O32−和Fe3O4。随着烧碱浓度的增加,S2O32−和Fe3O4的稳定区域增大,而FeS和FeS2的稳定区域减小。黄铁矿的电化学反应取决于铝酸钠溶液中不同电位的含硫阴离子。由于S2优先吸附在黄铁矿上,且极易转化为S0,使薄而致密的S0层富集在黄铁矿表面,抑制了黄铁矿的反应。在室温下,S2O32−有助于在黄铁矿表面形成氢氧化铁层,然后在黄铁矿表面形成较厚的氢氧化铁和缺铁硫化物(Fe1-xS2)层,显著抑制了黄铁矿的反应。此外,S2−和S2O32−的负电位以及高温促进了磁铁矿的形成。在260℃条件下,添加1 g·L−1 NaNO3能抑制黄铁矿反应,抑制S2O32−的转化,抑制黄铁矿消解过程中磁铁矿的形成,而添加更多的NaNO3则能显著促进黄铁矿反应和赤铁矿的形成。阐述了黄铁矿定向转化的机理,提出了一种高效利用含硫铝土矿同步脱硅除硫、回收铁还原赤泥的绿色新工艺。研究结果揭示了拜耳液中黄铁矿的电化学反应机理,为脱硅脱硫和铁回收后赤泥还原提供了新的途径。
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Directional transformation of pyrite in sodium aluminate solution for desulfurization and the reduction of red mud based on electrochemical mechanism
The directional transformation of pyrite in the concentrated sodium aluminate solution at high temperatures will benefit the sulfur removal and the reduction of red mud, leading to green utilization of bauxite containing sulfur. After calculation of the activity coefficient through the Bromley model, φ-ρ(Na2O) diagrams of Fe-S-H2O were provided at 298 K and 533 K, respectively. Regulating the potential, caustic alkali concentration, and temperature allowed pyrite to directionally transform into S2O32− and Fe3O4. Increasing caustic alkali concentration enlarged the stable region of S2O32− and Fe3O4, while reducing the stable region of FeS and FeS2. The electrochemical reaction of pyrite depended on the sulfur-bearing anions with different potentials in the sodium aluminate solution. Owing to S2 preferentially adsorbed on the pyrite and readily changing into S0, the thin dense S0 layer enriched on the pyrite surface, inhibiting the reaction of pyrite. S2O32− contributed to the formation of an iron hydroxide layer on the pyrite surface at room temperature, the thick layer of iron hydroxide and iron-deficient sulfide (Fe1-xS2) on pyrite then remarkably restrained the reaction of pyrite. In addition, the negative potential from S2− and S2O32− and high temperatures promoted the formation of magnetite. Inhibiting pyrite reaction, transformation of S2O32−, and formation of magnetite in the digestion of pyrite were all achieved by adding 1 g·L−1 NaNO3, whereas more NaNO3 notably promoted pyrite reaction and formation of hematite at 260 ℃. The mechanism of the directional transformation of pyrite was elucidated, while a green novel process to efficiently utilize bauxite containing sulfur for synchronous desilication and sulfur removal, together with reduction of the red mud through iron recovery was provided. The results provide an insight into electrochemical reaction mechanism of pyrite in Bayer liquor, and novel approach to sulfur removal in desilication and the reduction of red mud after iron recovery.
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来源期刊
Electrochimica Acta
Electrochimica Acta 工程技术-电化学
CiteScore
11.30
自引率
6.10%
发文量
1634
审稿时长
41 days
期刊介绍: Electrochimica Acta is an international journal. It is intended for the publication of both original work and reviews in the field of electrochemistry. Electrochemistry should be interpreted to mean any of the research fields covered by the Divisions of the International Society of Electrochemistry listed below, as well as emerging scientific domains covered by ISE New Topics Committee.
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