| Cite this article as: |
Xiaoyu Zhang, Chunquan Li, Shuilin Zheng, Yonghao Di, and Zhiming Sun, A review of the synthesis and application of zeolites from coal-based solid wastes, Int. J. Miner. Metall. Mater., 29(2022), No. 1, pp. 1-21. https://doi.org/10.1007/s12613-021-2256-8
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孙志明 E-mail: zhimingsun@cumtb.edu.cn
本文首先介绍了以煤矸石和粉煤灰为代表的煤基固废基本理化性质以及煤基固废合成分子筛的预处理工艺。煤基固废可以提供分子筛生成所需的硅、铝组分。但是，煤基固废中硅、铝元素的反应活性有待提高，并且煤基固废中存在许多不利于沸石化过程的杂质。因此，在合成分子筛之前，通常需要对煤基固废进行预处理，包括研磨、煅烧、酸浸等。研磨工艺能够通过粒度细化实现煤基固废比表面积以及杂质暴露量的增加，促使煤基固废表面产生更多缺陷位点，这有利于其进一步溶解。但研磨工艺不能完全活化煤基固废中的有效成分，而高温煅烧则可以更加彻底地活化煤基固废，并除去有机杂质。此外，一些会影响分子筛成核和结晶的碱金属氧化物，如Fe2O3、CaO、MgO及TiO2等，则需要通过酸处理消除。通过上述两种或三种预处理方法的联用，可以实现煤基固废的高效活化。然后，本文系统介绍了以煤基固废为原料合成分子筛的方法，包括水热晶化法、结构导向剂水热晶化法、碱熔辅助水热晶化法、超声或微波辅助水热晶化法、两步法、熔融盐法以及无溶剂法等。通过合理选用合成方法并调整制备参数，能够以各类煤基固废（不同硅铝比的煤矸石、粉煤灰）为原料合成不同类型的分子筛（如Na–X、Na–Y、Na–P、Na–P1、Na–A及方钠石等）。但是，一些具有特殊结构的分子筛（如ZSM-5、SSZ-13及ZK-5等），更易通过结构导向剂水热晶化法合成。当使用石英和长石含量较高的煤矸石或C级粉煤灰合成分子筛时，最好选用具有额外辅助（碱熔、超声波、微波）的方法，以优化煤基固废的沸石化过程。此外，本文还系统介绍了煤基固废分子筛在水污染治理、空气污染治理、重金属污染土壤修复、化学催化和储能材料中的应用现状。低硅铝比的煤基固废分子筛（如Na–X、Na–Y、Na–A、Na–P1等）通常具有较高的阳离子交换容量（CEC），这些分子筛在需要强离子交换能力的领域中具有较高应用潜力；具有高硅铝比的分子筛（如ZSM分子筛）的亲脂性、热稳定性和耐酸性更为出色，因此在某些有机催化过程中具有显著优势；分子筛在离子交换和吸附过程中的孔径效应也需要注意，直径小于分子筛孔径的目标颗粒才更易进入分子筛孔道。最后，本文对煤基固废分子筛的合成与应用发展方向与趋势进行了展望。文章认为，煤基固废分子筛的研究应以其在不同领域的大规模应用为目标导向，在进一步明晰煤基固废沸石化机理的基础上提升煤基固废的转化率及分子筛产品纯度，并注重开发低能耗及原料可循环的煤基固废沸石化工艺；辅助能量的引入对煤基固废的沸石化过程而言是非常重要的，碱溶辅助的超临界水热晶化法可能是一种高效快速的煤基固废沸石化工艺；在煤基固废分子筛应用开拓方面，作者认为，煤基固废分子筛的规模化使用应以商用分子筛的应用领域为参照，在许多商用分子筛的应用领域，煤基固废分子筛已初显替代潜力。
Zeolite derived from coal-based solid wastes (coal gangue and coal fly ash) can overcome the environmental problems caused by coal-based solid wastes and achieve valuable utilization. In this paper, the physicochemical properties of coal gangue and coal fly ash are introduced. The mechanism and application characteristics of the pretreatment processes for zeolite synthesis from coal-based solid wastes are also introduced. The synthesis processes of coal-based solid waste zeolite and their advantages and disadvantages are summarized. Furthermore, the application characteristics of various coal-based solid waste zeolites and their common application fields are illustrated. Finally, we propose an alkaline fusion-assisted supercritical hydrothermal crystallization as an efficient method for synthesizing coal-based solid waste zeolites. In addition, more attention should be given to the recycling of alkaline waste liquid and the application of coal-based solid waste zeolites in the field of volatile organic compound adsorption removal.
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