O2/H2O/SO2 对改性富铁凹凸棒石高温吸附PbCl2 的影响

doi:10.16085/j.issn.1000-6613.2022-1188

摘要/Abstract

摘要：

通过盐酸活化和负载Fe₃O₄复合改性方式获得改性富铁凹凸棒石，探究O₂/H₂O/SO₂对其吸附高温炉内典型半挥发性重金属PbCl₂蒸气的影响，同时分析了吸附产物中铅物种的分布形态，并结合FTIR、BET、XRD和XPS等表征手段深入探究其对PbCl₂蒸气的吸附机制。结果表明，酸活化通过分解原矿中杂质提高表面活性位点占比，复合改性后铁基氧化物与凹凸棒石表面晶格氧形成的双活性吸附位点显著增加其PbCl₂吸附容量。当高温烟气中含有体积分数20%O₂、5%H₂O和400mL/m³ SO₂时，复合改性凹凸棒石的PbCl₂吸附容量较原凹凸棒石有显著提升，在负载质量比为1∶2的Fe/HFP₂样品中吸附容量最高可分别达到70.42mg/g、76.63mg/g和86.21mg/g，吸附效果优于高岭土。此外，在这些氛围下改性凹凸棒石吸附产物中铅的稳定分布形态含量高于高岭土，吸附产物更为稳定。

关键词: 氯化铅, 吸附, 吸附剂, 改性, 富铁凹凸棒石, 高温

Abstract:

Modified iron-rich attapulgite was obtained by hydrochloric acid activation and Fe₃O₄ composite modification. The effect of O₂/H₂O/SO₂ on the adsorption of typical semi-volatile heavy metal PbCl₂ vapor was investigated in a high-temperature furnace. Meanwhile, the distribution and morphology of lead species in the adsorption products were analyzed. FTIR, BET, XRD and XPS were used to investigate the adsorption mechanism. The results showed that acid activation increased the proportion of surface-active sites by decomposing the impurities in raw ore. The dual active adsorption sites formed from the composite modification by iron-based oxides and attapulgite surface lattice oxygen significantly increased the adsorption capacity of PbCl₂. When the flue gas contained 20% O₂, 5% H₂O and 400mL/m³ SO₂, the PbCl₂ adsorption capacity of the modified attapulgite was significantly higher than that of the original attapulgite. The highest adsorption capacities of 70.42mg/g, 76.63mg/g and 86.21mg/g were achieved in Fe/HFP₂ sample with a loading mass ratio of 1∶2, respectively, better than kaolinite. Furthermore, the content of stable distributed Pb in the adsorption products using modified attapulgite under these atmospheres was higher than that of kaolinite, indicating the adsorption products were more stable.

Key words: lead chloride, adsorption, adsorbents, modification, iron-rich attapulgite, high temperature

中图分类号:

X705

赵重阳, 赵磊, 石详文, 黄俊, 李治尧, 沈凯, 张亚平. O₂/H₂O/SO₂ 对改性富铁凹凸棒石高温吸附PbCl₂ 的影响[J]. 化工进展, 2023, 42(4): 2190-2200.

ZHAO Chongyang, ZHAO Lei, SHI Xiangwen, HUANG Jun, LI Zhiyao, SHEN Kai, ZHANG Yaping. Effect of O₂/H₂O/SO₂ on the adsorption of PbCl₂ by modified iron-rich attapulgite at high temperature[J]. Chemical Industry and Engineering Progress, 2023, 42(4): 2190-2200.

图/表 14

表1 吸附剂组成成分分析（质量分数） (%)

样品	SiO₂	Al₂O₃	Na₂O	Fe₂O₃	TiO₂	MgO	CaO	K₂O	P₂O₅
高岭土	49.52	39.91	0.06	0.92	0.61	0.35	0.06	1.82	0.09
富铁凹凸棒石	48.31	15.39	1.54	7.31	1.13	3.83	11.20	4.16	0.28

图1 气态PbCl2吸附测试实验系统

图2 改性吸附剂对PbCl2在不同烟气气氛中的吸附性能

图3 O2含量对改性吸附剂铅吸附性能的影响

图4 改性吸附剂在不同含水量下对PbCl2蒸气的吸附性能测试

图5 SO2存在下Fe/HFP2对PbCl2蒸气的评价结果

图6 改性富铁凹凸棒石的SEM分析

图7 改性凹凸棒石的XRD分析

图8 改性凹凸棒石Fe/HFP2的Fe 2p高分辨图谱

表2 不同样品中Fe2+和Fe3+的比例

样品	Fe(Ⅱ)/Fe(Ⅲ)（原子比）
Fe/HFP₂ - fresh	0.68
无O₂-Fe/HFP₂- adsorbed	0.47
10% O₂-Fe/HFP₂- adsorbed	0.42
20% O₂-Fe/HFP₂ - adsorbed	0.32
5% H₂O-Fe/HFP₂ - adsorbed	0.65
10% H₂O-Fe/HFP₂ - adsorbed	0.35

图9 Fe/HFP2的XPS谱图

图10 改性凹凸棒石的FTIR分析

图11 改性吸附剂的孔径分布曲线

表3 改性富铁凹凸棒石的物理化学特征

样品	比表面积/m²·g^-1	孔体积/cm³·g^-1	平均孔径/nm
FP	86.49	0.15	8.21
HFP	187.78	0.27	6.68
Fe/HFP₄	168.97	0.43	11.81
Fe/HFP₃	160.22	0.43	12.70
Fe/HFP₂	144.48	0.49	14.15
Fe/HFP₁	133.75	0.43	14.83

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O₂/H₂O/SO₂ 对改性富铁凹凸棒石高温吸附PbCl₂ 的影响

Effect of O₂/H₂O/SO₂ on the adsorption of PbCl₂ by modified iron-rich attapulgite at high temperature

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