Research progress on the synthesis of zeolite from industrial ash rich in silicon and aluminium
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摘要:
沸石是一系列多孔硅铝酸盐材料的统称，因其具有较高的阳离子交换能力，作为吸附材料广泛应用于污水的净化和催化合成化学品等多个领域。燃煤灰渣、煤气化灰渣、铸造灰渣等工业灰渣含有大量的Si、Al元素，可以作为合成沸石的主要原料，达到资源化利用这些固体废物的目的。分析了燃煤灰渣、煤气化灰渣和铸造灰渣的形成和来源，对比三者的化学成分发现，燃煤灰渣的化学成分含量表现为SiO2>Al2O3>Fe2O3>CaO，煤气化灰渣的烧失量比较高，可达36.1%，铸造灰渣的硅铝比显著高于煤气化灰渣和燃煤灰渣。目前，3种灰渣中，燃煤灰渣的研究和利用比较多，而铸造灰渣和煤气化灰渣相对较少；铸造灰渣的Al2O3和SiO2的总含量比较高，烧失量和金属氧化物含量较低，是一种合成沸石的优质原料，可合成高品质沸石；煤气化灰渣的残碳含量比较高，在考虑煤气化灰渣Si、Al回收和利用的同时，还应充分考虑其残碳的资源化利用。
Abstract:A series of porous silicon aluminate materials is defined as zeolite, which is widely used in sewage purification, catalytic chemical synthesis and other fields due to its higher cation exchangeability. Coal ash, gasification ash, casting ash, and other industrial ashes may be used as the main raw materials for the synthesis of zeolite because they contained a large number of Si and Al elements, to achieve the purpose of resource utilization of these solid wastes. The formation and sources of coal ash, gasification ash and casting ash were analyzed. By comparing their chemical composition contents, it was found that the chemical composition contents of coal ash followed the order of SiO2>Al2O3>Fe2O3>CaO. The ignition loss of gasification ash was 36.1%, which was relatively higher, and the ratio of Si to Al was significantly higher in casting ash than those in gasification ash and coal ash. At present, among the three kinds of ashes, more research and utilization work had been done for coal ash, while less had been done for casting ash and gasification ash. The total content of Al2O3 and SiO2 in casting ash was relatively high, and its loss on ignition and metal oxide content was low. Casting ash was a high-quality raw material, which could be used to prepare high-quality zeolite. In addition to considering the recovery and utilization of Si and Al of gasification ash, its residual carbon should be fully utilized because the residual carbon content of gasification ash was relatively high.
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Key words:
- coal ash /
- gasification ash /
- casting ash /
- zeolite /
- resource utilization
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图 1 煤气化灰渣合成碳/沸石的X射线衍射
Figure 1. XRD patterns of carbon/zeolite synthesized by gasification ash
表 1 中国富含硅铝的工业灰渣化学组成
Table 1. Chemical composition of industrial ashes with higher content of silica and aluminium in China
% 灰渣 SiO2 Fe2O3 Al2O3 TiO2 CaO MgO Na2O K2O SO3 烧失量 燃煤灰渣 粉煤灰
[1,20-21]33.9~59.7 1.5~19.4 16.5~55.0 0.2~2.2 1.1~8.5 0.6~4.8 0.2~1.3 0.7~2.9 0~2.9 5.4~10.2 沸腾炉渣[1,22-23] 42.0~69.5 3.6~14.3 15.3~32.9 1.1~1.4 1.3~5.4 0.2~1.5 0.2~0.4 0.6~1.0 1.1~2.9 6.9~16.6 固硫灰渣 [1,5,17] 20.2~40.3 3.2~7.1 11.8~32.8 0.4~1.0 9.2~43.9 0.5~2.7 0.2~1.3 0.5~1.1 3.5~12.7 4.3~19.7 煤气化灰渣 细渣[24-26] 28.7~50.1 2.5~7.7 8.9~42.7 0.5~1.7 2.8~12.7 0.7~1.4 0.5~2.4 0.3~2.0 0.3~4.6 8.6~36.1 粗渣[24-26] 33.0~52.1 4.5~36.8 12.1~28.4 0.5~1.3 2.4~18.6 1.1~1.9 0.5~4.3 0.4~0.7 0.4~3.3 1.8~18.9 铸造灰渣 铸造废砂[3,26-28] 53.4~98.8 0.1~2.6 0.3~36.8 0.1~1.1 0~1.8 0~0.8 0~0.5 0~0.4 0.2~0.8 0.5~5.6 铸造粉尘[4,29-30] 41.1~93.2 0.4~4.7 1.5~22.4 0~4.9 0.3~4.6 0.6~6.2 1.1~1.4 0.1~4.6 0.3~13.3 
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表 2 合成沸石分子筛的主要工艺及其优缺点
Table 2. Main processes of synthesizing zeolite molecular sieves and their advantages and disadvantages
方法名称 主要材料 工艺 优缺点 传统水热法[10] 灰渣、碱液(NaOH、KOH、Na2CO3) 用碱液等与灰渣按照一定的固液比进行混合，陈化一定时间后放入反应釜中以适当温度进行晶化，经洗涤、干燥最终获得产品 工艺简单，成本低，但反应时间长，分子筛杂质多，纯度低，产量低 两步水热法[59] 灰渣、碱液、硅铝酸盐 将原料与碱液混合一段时间后，过滤并检测滤液中的硅铝含量，根据所测含量添加硅铝酸盐，晶化、洗涤、干燥获得最终产品 纯度较高，杂质少，但操作复杂，成本高 碱熔融法[60] 灰渣、固体碱、硅铝酸盐 采用碱熔焙烧的方法活化原料，将碱熔产物进行研磨，按需要添加硅铝源进行水热反应，随后洗涤、干燥获得分子筛产品 转化率高，分子筛纯度高，节省用水量，但煅烧成本高 晶种/模板剂合成法[13,61] 灰渣、碱溶液、晶种、模板剂 在晶化过程中，将晶种（天然沸石）/模板剂引入混匀的反应体系中，较低的温度下晶化，洗涤并干燥后得到成品 合成周期缩短，减少杂晶的生成，可合成特定产品，但操作复杂，增加成本，有机模板剂法可能具有毒性 逐步升温法[62] 灰渣、碱液 在晶化过程中先以较低温度时间下晶化一段时间，再升温晶化一段时间来得到目标产物 晶化时间缩短，粒径分布窄，
但相关研究较少超声波/微波辐射法[63] 灰渣、碱溶液 在晶化过程中使用微波/超声波照射合成沸目标产物 合成速率快，粒度均一，但缺乏大规模
工业试验
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