煤固废基分子筛的制备及其应用进展

doi:10.16085/j.issn.1000-6613.2023-2107

摘要/Abstract

摘要：

从煤基固废高值化利用以及分子筛材料低成本制备两方面的迫切需求出发，本文以煤矸石、粉煤灰、煤气化渣和煤液化渣四种最主要的煤基固废为研究对象，从形成机制、化学组成、矿物性质以及结构与形貌特征等多方面阐述以其为原料制备分子筛的优势及可行性；系统总结了煤基固废活化预处理及晶化转化为分子筛的主要方法；以典型案例的形式，介绍并分析了煤固废基分子筛在气/液相吸附、多相催化等领域的应用优势。基于对煤固废基分子筛的制备、改性以及应用研究进展的综述与总结，提出了低能耗活化与晶化、骨架类型的拓展以及多领域应用探索三方面的研究趋势。

关键词: 煤基固废, 高值化利用, 分子筛, 低成本制备

Abstract:

High-value utilization of coal-based solid wastes is in urgent demands for the sustainable development of natural resources, and one promising strategy is to prepare zeolites by using coal-based solid wastes as raw materials. In this review, the formation mechanism and primary properties including chemical composition, mineral property, structural and morphological characteristics of four typical coal-based solid wastes (gangue, fly ash, gasification slag, and liquefaction slag) were introduced in detail. The main methods of activation pretreatments and zeolite crystallization were further summarized systematically. Moreover, the application advantages of zeolites prepared from coal-based solid wastes in gas/liquid adsorption and heterogeneous catalysis were discussed by specific cases. It is expected that more prospective studies on low-energy activation, diverse framework, and application exploration are highly desired for the synthesis and utilization of zeolites from coal-based solid wastes.

Key words: coal-based solid waste, high-value utilization, zeolite, low-cost production

中图分类号:

O611.4

张国卿, 宋舒波, 王兴瑞, 巩苗苗, 王旭, 许宇鸿, 冯继越, 张福扬, 陈汇勇. 煤固废基分子筛的制备及其应用进展[J]. 化工进展, 2024, 43(5): 2311-2323.

ZHANG Guoqing, SONG Shubo, WANG Xingrui, GONG Miaomiao, WANG Xu, XU Yuhong, FENG Jiyue, ZHANG Fuyang, CHEN Huiyong. Recent advances in the synthesis and application of zeolites from coal-based solid wastes[J]. Chemical Industry and Engineering Progress, 2024, 43(5): 2311-2323.

图/表 10

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处理利用方式	特点
摊铺、堆填	大批量处理；就地处理；无附加值
制备建筑材料	大批量处理；建筑材料质量较差；低附加值
提取有价元素	充分利用各类元素；工艺复杂；分离困难
制备土壤添加剂	大批量处理；需控制重金属污染
制备分子筛	处理量有限；元素利用合理；高附加值

处理利用方式	特点
摊铺、堆填	大批量处理；就地处理；无附加值
制备建筑材料	大批量处理；建筑材料质量较差；低附加值
提取有价元素	充分利用各类元素；工艺复杂；分离困难
制备土壤添加剂	大批量处理；需控制重金属污染
制备分子筛	处理量有限；元素利用合理；高附加值

主要类别	所属行业	特点	元素组成（质量分数）/%	矿物组成
煤矸石	采煤、洗选	块体；伴生矿物；元素组成复杂；含碳量高	SiO₂（30~65）、Al₂O₃（15~40）、Fe₂O₃（1~10）、CaO（1~3）、TiO₂（0.5~3.0）	石英、高岭石、蒙脱石、白云石
粉煤灰	热电	粉体；热加工产物；氧化物形态；	SiO₂（33~60）、Al₂O₃（17~35）、Fe₂O₃（1.5~15）、CaO（1~5）、MgO（0.5~2.2）	莫来石、石英
煤气化渣	煤化工	颗粒；硬度高；玻璃态；高温热处理产物	SiO₂（30~60）、Al₂O₃（15~30）、Fe₂O₃（2~15）、CaO（1~13）、NaO（0.5~3.0）	石英、方解石、莫来石
煤液化渣	煤化工	颗粒；掺混残余催化剂；组成复杂	SiO₂（5~50）、Al₂O₃（5~20）、Fe₂O₃（10~65）、CaO（5~20）、TiO₂（1~3）	钙长石、石英

主要类别	所属行业	特点	元素组成（质量分数）/%	矿物组成
煤矸石	采煤、洗选	块体；伴生矿物；元素组成复杂；含碳量高	SiO₂（30~65）、Al₂O₃（15~40）、Fe₂O₃（1~10）、CaO（1~3）、TiO₂（0.5~3.0）	石英、高岭石、蒙脱石、白云石
粉煤灰	热电	粉体；热加工产物；氧化物形态；	SiO₂（33~60）、Al₂O₃（17~35）、Fe₂O₃（1.5~15）、CaO（1~5）、MgO（0.5~2.2）	莫来石、石英
煤气化渣	煤化工	颗粒；硬度高；玻璃态；高温热处理产物	SiO₂（30~60）、Al₂O₃（15~30）、Fe₂O₃（2~15）、CaO（1~13）、NaO（0.5~3.0）	石英、方解石、莫来石
煤液化渣	煤化工	颗粒；掺混残余催化剂；组成复杂	SiO₂（5~50）、Al₂O₃（5~20）、Fe₂O₃（10~65）、CaO（5~20）、TiO₂（1~3）	钙长石、石英

分子筛名称	骨架类型	固废原料种类	活化方法	合成方法	参考文献
4A	LTA	粉煤灰	—	水热合成	[42]
NaA	LTA	煤矸石	热活化	水热合成	[44]
4A	LTA	煤气化渣	碱熔活化	水热合成	[47]
Zeolite A	LTA	粉煤灰	—	微波辅助合成	[66]
SCD-Y	FAU	煤矸石	热活化	水热合成	[45]
NaY	FAU	煤矸石	碱熔活化	水热合成	[34]
Zeolite X	FAU	粉煤灰	碱熔活化	水热合成	[22]
FAU	FAU	粉煤灰	碱熔活化	无溶剂合成	[62]
NaX	FAU	粉煤灰	碱熔活化	超声辅助合成	[68]
NaP1	GIS	粉煤灰	—	水热合成	[41]
NaP	GIS	煤气化渣	—	水热合成	[43]
P-zeolite	GIS	煤气化渣	碱熔活化	水热合成	[37]
Zeolite P1	GIS	粉煤灰	热活化	无溶剂合成	[31]
Analcime	ANA	煤矸石	—	水热合成	[39]
SSZ-13	CHA	煤矸石	—	水热合成	[40]
SSZ-13	CHA	煤矸石	—	超声辅助合成	[65]
ZSM-5	MFI	煤矸石	碱熔活化	无溶剂合成	[59]
ZSM-5	MFI	粉煤灰	碱熔活化	无溶剂合成	[63]
ZSM-5	MFI	煤气化渣	—	无溶剂合成	[64]
ZSM-5	MFI	粉煤灰	热活化	超声辅助合成	[67]
Cancrinite-type zeolite	CAN	粉煤灰	—	无溶剂合成	[61]