硅酸锂基吸附剂吸附CO<sub>2</sub>性能

摘要

以煤系高岭土酸处理后得到的物料为硅源，采用固相法和浸渍沉淀法制备硅酸锂基吸附剂，并通过浸渍沉淀法，添加不同比例的埃洛石纳米管，合成出可在500~650℃吸附CO₂的硅酸锂基吸附剂。通过X射线衍射分析仪（XRD）、扫描电子显微镜（SEM）、N₂等温吸附脱附分别观察和分析了样品的结构、形貌特征及比表面积，并使用差热-热重联重分析仪（DTA-TG）研究了样品对CO₂的吸附性能。实验结果表明，采用浸渍沉淀法制备的硅酸锂基吸附剂，颗粒较小、分布均匀，表面积较大，具有良好的吸附效果，其最大吸附量（质量分数，下同）可达35.74%，吸附效率为97.33%，明显优于固相法；通过掺杂适量的埃洛石纳米管，可在一定程度上改善吸附剂在500~650℃的吸附性能，当掺杂量为x=1.04%时所得吸附剂在500~650℃的吸附性能最佳，540℃时吸附量为12.78%，是未掺杂时的2.39倍。

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	谢洪燕
	丁彤
	李玉龙
	马智
	陈为强

关键词：硅酸锂；浸渍沉淀法；煤系高岭土；埃洛石纳米管； CO₂

Abstract：

Lithium orthosilicate based sorbents were prepared by solid-state method and impregnation-precipitation method, with SiO₂ as silicon source which was made from the waste residue of acid processing coal-kaolin. And lithium orthosilicate based sorbents doped with halloysite nanotubes exhibited excellent CO₂ absorption performance at 500-650℃, which were prepared by impregnation-precipitation method. The phase composition, morphologies and surface area were analyzed by XRD, SEM and N₂ adsorption-desorption isotherm,and CO₂ absorption performance was measured with a thermogravimetric analyzer. The results indicated that the absorption performance of Li₄SiO₄ made by impregnation-precipitation method, with small particles, particle size evenly distributed and large surface area, is better than Li₄SiO₄ made by solid method. And the maximum absorption capacity of lithium orthosilicate based sorbent made by impregnation-precipitation method reached 35.74% (704℃), corresponding to 97.33% efficiency. The absorption performance at 500℃ to 650℃ of sorbents can be improved greatly by doping aluminum with halloysite nanotubes. It was found that the sorbent got the best performance at 500℃ to 650℃ when x=1.04%, and the absorption capacity reached 12.78% at 540℃, which was 2.39 times as much as absorbent with non doping.

Keywords： lithium orthosilicate； impregnation-precipitation method； coal-kaolin； halloysite nanotubes； carbon dioxide

Received 2015-03-24;

Fund:

天津市自然科学基金（15JCYBJC23000）

Corresponding Authors: 丁彤,E-mail:hongyan1608@163.com。 Email: hongyan1608@163.com

About author: 谢洪燕(1988-),女,硕士研究生,主要从事高温CO₂吸附剂的研究。

引用本文:

谢洪燕, 丁彤, 李玉龙, 马智, 陈为强.硅酸锂基吸附剂吸附CO₂性能[J]. 化学工业与工程, 2017,34(1): 9-13

Xie Hongyan, Ding Tong, Li Yulong, Ma Zhi, Chen Weiqiang.Absorbing CO₂ by Lithium Orthosilicate Based Sorbents[J]. Chemcial Industry and Engineering, 2017,34(1): 9-13

[1] 曲建升,曾静静,张志强. 国际主要温室气体排放数据集比较分析研究[J]. 地球科学进展, 2008, 23(1):47-54 Qu Jiansheng, Ceng Jingjing, Zhang Zhiqiang. The research on comparative analysis of international main greenhouse gas emissions data[J]. Advances in Earth Science, 2008, 23(1):47-54(in Chinese)
[2] Internation Energy Agency. CO₂ emissions from fuel combustion highlights[R]. Paris:IEA, 2012:7-16
[3] Radfarnia H R, Iliuta M C. Development of zirconium-stabilized calcium oxide absorbent for cyclic high-temperature CO₂ capture[J]. Industrial & Engineering Chemistry Research, 2012, 51:10390-10398
[4] Oliveira E L G, Grande C A, Rodrigues A E. CO₂ sorption on hydrotalcite and alkali-modif?ed (K and Cs) hydrotalcites at high temperatures[J]. Separation and Purif?cation Technology, 2008, 62:137-147
[5] Puccini M, Seggiani M, Vitolo S. Lithium silicate pellets for CO₂ capture at high temperature[J]. Chemical Engineering Transactions, 2013, 35:373-378
[6] 刘玉兰,丁彤,马智,等. 煤系高岭土为硅源制备硅酸锂及其对CO₂的吸附性能[J]. 化学工业与工程, 2013, 30(5):11-15 Liu Yulan, Ding Tong, Ma Zhi, et al. CO₂ absorption performance of Li₄SiO₄ prepared from coal-Kaolin[J]. Chemical Industry and Engineering, 2013, 30(5):11-15(in Chinese)
[7] 佚名. 日本开发出硅酸锂新材料[J]. 化工矿物与加工, 2001, 30(11):34-34 Anonymous. A new lithium silicate materials developed by Japan[J]. IM&P, 2001, 30(11):34-34(in Chinese)
[8] Kato M, Nakagawa K. New series of lithium containing complex oxides, lithium silicates, for application as a high temperature CO₂ absorbent[J]. Journal of the ceramic society of Japan, 2001, 109(11):911-914
[9] Kato M, Yoshikawa S, Nakagawa K. Carbon dioxide absorption by lithium orthosilicate in a wide range of temperature and carbon dioxide concentrations[J]. Journal of Materials Science Letters, 2002, 21:485-487
[10] 刘杨. 吸附强化甲烷水蒸汽重整制氢系统-Li₄SiO₄吸附剂制备、改性及CO₂吸附动力学研究[D]. 上海:华东理工大学, 2013 Liu Yang. Sorption enhanced steam methane reforming for hydrogen production-preparation and CO₂ absorption kinetic investigation of Li₄SiO₄[D]. Shanghai:East China University of Science and Technology, 2013(in Chinese)
[11] Venegas M J, Fregoso-Israel E, Escamilla R, et al. Kinetic and reaction mechanism of CO₂ sorption on Li₄SiO₄:Study of the particle size effect[J]. Ind Eng Chem Res, 2007, 46:2407-2412
[12] Chowdhury M B I, Quddus M R, deLasa H I. CO₂ capture with a novel solid fluidizable sorbent:Thermodynamics and temperature programmed carbonation-decarbonation[J]. Chemical Engineering Journal, 2013, 232:139-148
[13] Ortiz-Landeros J, Gòmez-Yãñez C, Palacios-Romero L M, et al. Structural and thermochemical chemisorption of CO₂ on Li_4+x(Si_1-xAl_x)O₄ and Li_4-x(Si_1-xV_x)O₄ solid solutions[J]. J Phys Chem A, 2012, 116:3163-3171
[14] Huggins R A. Recent results on lithium ion conductors[J]. Electrochimica Acta, 1977, 22(7):773-781
[15] Yang A, Wang H, Li W, et al. Synthesis of lithium metasilicate powders at low temperature via mechanical milling[J]. Am Ceram Soc, 2012, 95(6):1818-1821
[16] Bailey S W. Crystal structures of clay minerals and their X-ray identification:Structures of layer silicates[M]. Brindley G W, Brown G Ed. London:Mineralogical Society, 1980
[17] 景瑞芳. 埃洛石纳米管及高岭土纳米管脱硫性能的研究[D]. 天津:天津大学, 2013 Jing Ruifang. Study on desulfurization performance of halloysite nanotubes and Kaolin nanotubes[D]. Tianjin:Tianjin University, 2013(in Chinese)
[18] Shan S, Li S, Jia Q, et al. Impregnation precipitation preparation and kinetic analysis of Li₄SiO₄-based sorbents with fast CO₂ adsorption rate[J]. Industrial & Engineering Chemistry Research, 2013, 52(21):6941-6945