天然斜发沸石基方沸石及其改性对Pb2+的吸附性能

doi:10.16085/j.issn.1000-6613.2024-0365

化工进展 ›› 2025, Vol. 44 ›› Issue (3): 1726-1738.DOI: 10.16085/j.issn.1000-6613.2024-0365

天然斜发沸石基方沸石及其改性对Pb²⁺的吸附性能

张伊¹(), 么秋香², 孙鸣¹()

^1.西北大学化工学院，国家碳氢资源清洁利用国际科技合作基地，陕北能源先进化工利用技术教育部工程研究中心，陕西省洁净煤转化工程技术中心，陕西西安 710069
^2.西京学院电子信息学院，陕西西安 710123

收稿日期:2024-03-05 修回日期:2024-05-22 出版日期:2025-03-25 发布日期:2025-04-15
通讯作者: 孙鸣
作者简介:张伊（1998—），女，硕士研究生，研究方向为分子筛合成及吸附性能。E-mail：15388687315@163.com。
基金资助:
国家自然科学基金(22078266);国家重点研发计划(2023YFB4103400);陕西省重点研发计划(2024GX-YBXM-480);西京学院高层次人才专项(XJ21B10)

Adsorption performance of natural clinoptilolite based analcime and its modifications on Pb²⁺

ZHANG Yi¹(), YAO Qiuxiang², SUN Ming¹()

^1.School of Chemical Engineering, Northwest University, International Science & Technology Cooperation Base of MOST for Clean Utilization of Hydrocarbon Resources, Chemical Engineering Research Center of the Ministry of Education for Advanced Use Technology of Shanbei Energy, Shaanxi Research Center of Engineering Technology for Clean Coal Conversion, Collaborative Innovation Center for Development of Energy and Chemical Industry in Northern, Xi’an 710069, Shaanxi, China
^2.School of Electronic Information, Xijing University, Xi’an 710123, Shaanxi, China

Received:2024-03-05 Revised:2024-05-22 Online:2025-03-25 Published:2025-04-15
Contact: SUN Ming

摘要/Abstract

摘要：

首次以天然斜发沸石为原料，在无需额外添加硅铝源的基础上通过水热法制备方沸石（ANA），并采用NaOH和NaCl对ANA进行改性制得OH-ANA和Na-ANA。采用XRD、SEM、FTIR、BET、zeta电位和ICP-OES对合成沸石进行了表征，并研究了合成沸石对Pb²⁺的吸附性能。结果表明，改性后的Na-ANA和OH-ANA的比表面积均高于ANA，Na-ANA和OH-ANA对Pb²⁺最大吸附容量分别为96.00mg/g、125.54mg/g，均大于ANA的71.95mg/g，表明天然斜发沸石基方沸石在经过改性后吸附性能有所提升。ANA、Na-ANA和OH-ANA对Pb²⁺吸附是一个吸热的自发过程，符合伪二级动力学和Langmuir等温线模型，且吸附速率由外扩散和颗粒内扩散共同控制。材料表征结果显示，ANA、Na-ANA和OH-ANA对Pb²⁺吸附机理是静电吸引、离子交换和化学络合三者的协同作用。再生循环实验表明，OH-ANA材料具有良好的可再生性能。综上所述，ANA、Na-ANA和OH-ANA在去除重金属离子方面具有一定的应用潜力。

关键词: 天然斜发沸石, 水热法, 方沸石, 二价铅, 吸附性能

Abstract:

In this study, natural clinoptilolite was used for the first time as a raw material to synthesize analcime (ANA) by a hydrothermal method without the need for additional silicon-aluminium sources. The resulting ANA was further modified using NaOH and NaCl to obtain OH-ANA and Na-ANA. The synthesized zeolites were characterized by XRD, SEM, FTIR, BET, zeta potential and ICP-OES. The adsorption performance of the synthesized zeolites for Pb²⁺ was investigated. The results showed that the specific surface areas of modified Na-ANA and OH-ANA were higher than those of ANA. The maximum adsorption capacities of Na-ANA and OH-ANA for Pb²⁺ were 96.00mg/g and 125.54mg/g, respectively, both higher than that of ANA (71.95mg/g), indicating an improvement in the adsorption performance after modification. The adsorption of Pb²⁺ by ANA, Na-ANA and OH-ANA was an endothermic spontaneous process following pseudo-second-order kinetics and Langmuir isotherm models. The adsorption rate was controlled by both external and intraparticle diffusion. Material characterization results showed that the adsorption mechanisms involved the synergistic effects of electrostatic attraction, ion exchange and chemical complexation for ANA, Na-ANA and OH-ANA towards Pb²⁺. Regeneration cycle experiments showed that OH-ANA had good renewable properties. In conclusion, ANA, Na-ANA and OH-ANA had potential applications in the removal of heavy metal ions.

Key words: natural clinoptilolite, hydrothermal method, analcime, lead ion, adsorption performance

中图分类号:

X523

张伊, 么秋香, 孙鸣. 天然斜发沸石基方沸石及其改性对Pb²⁺的吸附性能[J]. 化工进展, 2025, 44(3): 1726-1738.

ZHANG Yi, YAO Qiuxiang, SUN Ming. Adsorption performance of natural clinoptilolite based analcime and its modifications on Pb²⁺[J]. Chemical Industry and Engineering Progress, 2025, 44(3): 1726-1738.

图/表 23

参考文献 46

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合成沸石材料	比表面积/m²·g^-1	孔容/cm³·g^-1	平均孔径/nm
ANA	7.9	0.049	16.3
Na-ANA	8.3	0.065	21.6
OH-ANA	11.1	0.057	20.7

合成沸石材料	比表面积/m²·g^-1	孔容/cm³·g^-1	平均孔径/nm
ANA	7.9	0.049	16.3
Na-ANA	8.3	0.065	21.6
OH-ANA	11.1	0.057	20.7

动力学模型	ANA	Na-ANA	OH-ANA
PFO
k₁/min^-1	0.0027	0.0029	0.0034
q_e/mg·g^-1	10.858	5.0527	1.3899
R₁²	0.7895	0.7416	0.6695
PSO
k₂/g·mg^-1·min^-1	0.0075	0.0183	0.0698
q_e/mg·g^-1	68.493	86.730	99.404
R₂²	0.9999	0.9999	0.9999
颗粒内扩散模型
阶段1
k_p1/mg·g^-1·min^-1	4.14	2.9812	1.2565
C₁/mg·g^-1	43.03	71.499	93.911
R₁²	0.9804	0.9756	0.9128
阶段2
k_p2/mg·g^-1·min^-1	1.48	0.4822	0.1209
C₂/mg·g^-1	54.96	81.934	98.168
R₂²	0.9764	0.9670	0.8149
阶段3
k_p3/mg·g^-1·min^-1	0.1046	0.0480	0.0120
C₃/mg·g^-1	66.20	85.731	99.174
R₃²	0.8810	0.8972	0.7339

动力学模型	ANA	Na-ANA	OH-ANA
PFO
k₁/min^-1	0.0027	0.0029	0.0034
q_e/mg·g^-1	10.858	5.0527	1.3899
R₁²	0.7895	0.7416	0.6695
PSO
k₂/g·mg^-1·min^-1	0.0075	0.0183	0.0698
q_e/mg·g^-1	68.493	86.730	99.404
R₂²	0.9999	0.9999	0.9999
颗粒内扩散模型
阶段1
k_p1/mg·g^-1·min^-1	4.14	2.9812	1.2565
C₁/mg·g^-1	43.03	71.499	93.911
R₁²	0.9804	0.9756	0.9128
阶段2
k_p2/mg·g^-1·min^-1	1.48	0.4822	0.1209
C₂/mg·g^-1	54.96	81.934	98.168
R₂²	0.9764	0.9670	0.8149
阶段3
k_p3/mg·g^-1·min^-1	0.1046	0.0480	0.0120
C₃/mg·g^-1	66.20	85.731	99.174
R₃²	0.8810	0.8972	0.7339

合成沸石材料	Langmuir			Freundlich
合成沸石材料	q_m/mg·g^-1	k_L/L·mg^-1	R²	1/n	k_F/mg·g^-1	R²
ANA	69.729	0.3825	0.9741	0.2395	23.4492	0.9081
Na-ANA	95.005	1.0122	0.9852	0.0476	39.1794	0.8143
OH-ANA	128.203	1.7122	0.9398	0.2229	58.9188	0.7042

天然斜发沸石基方沸石及其改性对Pb²⁺的吸附性能

Adsorption performance of natural clinoptilolite based analcime and its modifications on Pb²⁺

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吸附剂	pH	q_m/mg·g^-1	等温线模型	参考文献
沸石复合材料	6	47.619	Langmuir	[25]
沸石+凝灰岩	3.5	27.548	Langmuir	[26]
铁改性沸石	6.5	11.16	Langmuir	[27]
硅酸铝钠水合物/ANA	5.5	58.86	Langmuir	[28]
ZSM-5沸石	3	20.1	Langmuir	[29]
Y沸石	4.7	57.47	Langmuir	[30]
天然沸石	7	7.59	Langmuir	[31]
5A沸石	5.5	46.67	Langmuir	[32]
ZSM-5分子筛	4	14.39	Langmuir	[33]
ANA	5	69.729	Langmuir	本研究
Na-ANA	5	95.005	Langmuir	本研究
OH-ANA	5	128.203	Langmuir	本研究

合成沸石材料	T/K	∆G/kJ·mol^-1	∆H/kJ·mol^-1	∆S/J·mol^-1·K^-1
ANA	298	-0.12	4.42	15.26
	308	-0.29
	318	-0.46
	328	-0.56
Na-ANA	298	-2.86	11.70	48.76
	308	-3.27
	318	-3.81
	328	-4.31
OH-ANA	298	-10.66	20.67	105.13
	308	-11.76
	318	-12.64
	328	-13.88

吸附剂	去除率/%		参考文献
吸附剂	循环0次	循环4次	参考文献
沸石咪唑骨架	79.77	51.18	[40]
壳聚糖复合材料	98.65	64.50	[41]
气凝胶	95.9	75.81	[42]
层状金属氧化物	75.97	7.76	[43]
复合吸附材料	92.21	66.65	[44]
多糖水凝胶	91.79	67.34	[45]
改性褐煤	91.55	53.14	[46]
OH-ANA	99.32	74.03	本研究

[1]	路广军, 韩晋钢, 陈英, 马志斌. 镁渣基多孔材料的制备及其对废水中Pb²⁺的吸附性能[J]. 化工进展, 2024, 43(4): 2126-2134.
[2]	单书月, 罗中秋, 周新涛, 尚波, 田鑫聪, 阎崔蓉. 钢渣构筑Fe-CSH吸附溶液中Pb(‍Ⅱ)、Cu(‍Ⅱ)、Zn(‍Ⅱ)性能及机理[J]. 化工进展, 2024, 43(10): 5867-5880.
[3]	任建鹏, 吴彩文, 刘慧君, 吴文娟. 木质素-聚苯胺复合材料的制备及对刚果红的吸附[J]. 化工进展, 2023, 42(6): 3087-3096.
[4]	王书燕, 张新波, 彭安萍, 刘阳, NGO HUU HAO, 郭文珊, 温海涛. 生物炭回收水中氮磷营养物质的研究进展与挑战[J]. 化工进展, 2023, 42(10): 5459-5469.
[5]	王妍, 秦振平, 刘越, 张文海, 郭红霞. 环糊精原位改性MoS₂管式陶瓷复合膜的制备及性能[J]. 化工进展, 2023, 42(10): 5373-5380.
[6]	周硕林, 赖金花, 游高林, 刘贤响, 尹笃林. 水热法制备质子化钛纳米管的影响因素及其应用研究进展[J]. 化工进展, 2021, 40(7): 3791-3802.
[7]	刘蜀疆, 陈占营, 赵永刚, 常印忠. 氙常温吸附性能与多孔碳材料孔径分布关联分析[J]. 化工进展, 2020, 39(S2): 243-250.
[8]	张凯, 韦秀丽, 王冰, 蒋滔, 刘科. Fe₃O₄改性水热炭活化过硫酸钠降解罗丹明B[J]. 化工进展, 2020, 39(7): 2867-2875.
[9]	闫茜, 谢谚, 盛学佳, 周志国, 杨洋洋, 王昕喆, 曲聪, 张福良. 超疏水纳米海绵制备及其二甲苯吸附性能[J]. 化工进展, 2020, 39(10): 4095-4101.
[10]	刘德钱,解强,万超然,邓锋,黄小晴,翟笑迪. 活性炭配炭的吸附性能及其与孔结构的关系[J]. 化工进展, 2019, 38(12): 5578-5586.
[11]	庄晓东,李荣兴,俞小花,谢刚,和晓才,徐庆鑫. 钛酸锂/石墨烯复合材料及电化学性能[J]. 化工进展, 2019, 38(10): 4659-4665.
[12]	洪碧云, 唐丽荣, 陈伟香, 黄彪. 碱木质素/聚乙烯亚胺碳点的制备及其对pH敏感性[J]. 化工进展, 2019, 38(04): 1970-1977.
[13]	朱赫男, 王志朴, 邢文龙, 舒新前. 污泥与生物质共热解制备生物质炭工艺优化及吸附性能[J]. 化工进展, 2018, 37(S1): 199-204.
[14]	冯艳艳, 黄宏斌, 杨文, 赖国勇, 赵文君. 镍钴双金属氢氧化物/乙炔黑复合材料的制备及其电化学性能[J]. 化工进展, 2018, 37(11): 4378-4383.
[15]	董道敏, 刘宾, 柴永明, 吴仪岚, 刘晨光. 动态水热法制备Silicalite-1分子筛膜包覆多孔缺陷Al₂O₃微球[J]. 化工进展, 2018, 37(10): 3943-3948.