Modeling and response surface methodology optimization of reaction parameters for aqueous mineral carbonation by steel slag

Zhenhao Wang, Chuanwen Zhao, Pu Huang, Yuxuan Zhang, Jian Sun
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Abstract

CO2 sequestration via mineralization of steel slag has received widespread attention due to its ability to achieve in-situ CO2 sequestration in steel industries and high-value utilization of steel slag. The final CO2 sequestration capacity of steel slag is closely related to the reaction parameters (i.e., reaction duration, reaction temperature, CO2vol concentration, and liquid-solid ratios) of mineralization. The reaction parameters may have synergistic effects on the ability of steel slag to sequestrate CO2. Therefore, the single-factor (one-factor-at-a-time) experimental strategy can't obtain optimal process parameters. Herein, response surface methodology and the Box-Behnken Design were employed in determining optimal conditions. It is found that the combined effects of CO2 concentration in combination with reaction temperature and liquid-solid ratio significantly influence the sequestration process (P = 0.0082 and P < 0.0001, respectively). Conversely, the combined effects of reaction duration with liquid-solid ratio and CO2 concentration were found to be less significant (P = 0.6905 and P = 0.6114, respectively). The reasons behind this observation can be ascribed to the focus of this research on the later stages of the reaction, during which it proceeds smoothly. Additionally, alterations in temperature, liquid-solid ratio, and CO2 concentration not only affect the initial pH, CO2 dissolution rate and quantity, and reaction kinetics but also alter the patterns of their collective impact on CO2 sequestration. The CO2 capture could reach 179.1 g-CO2/kg-steel slag at the optimal condition (i.e., 56.14 °C reaction temperature, 6.66 ml/g liquid-solid ratio, 44.53 wt.% CO2 concentration, and 286.73 mins reaction time), compared to single-factor stepwise optimization, which improves by about 9.84 %. Implementing this optimized mineralization process could enable the Chinese steel industry to capture an estimated 27.4 million tons of CO2 annually, based on an annual production of 153 million tons of steel slag.

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钢渣水溶液矿物碳化反应参数的建模和响应面方法优化
通过钢渣矿化进行二氧化碳封存因其能够实现钢铁工业的二氧化碳就地封存和钢渣的高值化利用而受到广泛关注。钢渣的最终二氧化碳封存能力与矿化反应参数(即反应时间、反应温度、二氧化碳体积浓度和液固比等)密切相关。反应参数可能会对钢渣封存二氧化碳的能力产生协同效应。因此,单因素(一次一个因素)实验策略无法获得最佳工艺参数。在此,我们采用了响应面方法和箱-贝肯设计(Box-Behnken Design)来确定最佳条件。研究发现,二氧化碳浓度、反应温度和液固比的综合效应对封存过程有显著影响(分别为 P = 0.0082 和 P < 0.0001)。相反,反应持续时间、液固比和二氧化碳浓度的综合影响则不太明显(分别为 P = 0.6905 和 P = 0.6114)。出现这种情况的原因可能是本研究的重点是反应的后期阶段,在此期间反应进展顺利。此外,温度、液固比和二氧化碳浓度的变化不仅会影响初始 pH 值、二氧化碳溶解速率和数量以及反应动力学,还会改变它们对二氧化碳封存的共同影响模式。在最佳条件下(即反应温度 56.14 ℃、液固比 6.66 ml/g、二氧化碳浓度 44.53 wt.%、反应时间 286.73 mins),二氧化碳捕集量可达 179.1 g-CO2/kg-钢渣,与单因素逐步优化相比,提高了约 9.84%。以中国钢铁行业年产 1.53 亿吨钢渣计算,采用这一优化矿化工艺每年可捕获约 2740 万吨二氧化碳。
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