氨气改性的NH3@MIL-53(Cr)吸附CO2和CH4的性能

doi:10.3969/j.issn.0438-1157.2014.05.028

化工学报

氨气改性的NH₃@MIL-53(Cr)吸附CO₂和CH₄的性能

杨琰¹, 王莎¹, 张志娟², 夏启斌¹, 李忠¹

1 华南理工大学化学与化工学院, 广东广州 510640;
2 暨南大学大气环境安全与污染控制研究所, 广东广州 510632

收稿日期:2014-02-17 修回日期:2014-03-26 出版日期:2014-05-05 发布日期:2014-05-05
通讯作者: 夏启斌
基金资助:
国家重点基础研究发展计划项目（2013CB733506）；国家自然科学基金项目（21176085）。

CO₂ and CH₄ adsorption performance of modified MIL-53(Cr) via ammonia vapor

YANG Yan¹, WANG Sha¹, ZHANG Zhijuan², XIAQibin¹, LI Zhong¹

1 School of Chemical Engineering, South China University of Technology, Guangzhou 510640, Guangdong, China;
2 Institute of Atmospheric Environment Safety and Pollution Control, Jinan University, Guangzhou 510632, Guangdong, China

Received:2014-02-17 Revised:2014-03-26 Online:2014-05-05 Published:2014-05-05
Supported by:
supported by the National Basic Research Program of China (2013CB733506) and the National Natural Science Foundation of China (21176085).

摘要/Abstract

摘要： 采取水热法成功合成MIL-53（Cr）晶体，分别应用0.1、1、3 mol·L^-1的氨气对MIL-53（Cr）进行改性，制得系列的NH₃@MIL-53（Cr）-1#，NH₃@MIL-53（Cr）-2#，NH₃@MIL-53（Cr）-3#。实验结果表明：与原始的MIL-53（Cr）晶体相比，尽管制得NH3@MIL-53（Cr）系列材料的比表面积依次减少，但其单位比表面积的CO₂吸附容量大小依次为：NH₃@MIL-53（Cr）-3#>NH₃@MIL-53（Cr）-2#>NH₃@MIL-53（Cr）-1#。表明氨气改性会使得材料表面的碱性增强，从而增强了其对酸性气体CO₂的吸附。此外，改性后的NH₃@MIL-53（Cr）对水蒸气的吸附量明显减少，表明其憎水性能得到改善。较高浓度氨气改性会导致材料的比表面积大幅下降，会引起单位质量吸附剂的吸附容量下降。用1 mol·L^-1浓度的氨气改性得到的NH3@MIL-53（Cr）-2#，不仅对CO₂的吸附容量最大，而且对CH₄的吸附容量明显下降，这将有助于进一步提高改性材料NH3@MIL-53（Cr）-2# 对CO₂/CH₄的吸附选择性。

关键词: MIL-53（Cr）, 二氧化碳, 甲烷, 水蒸气, 吸附, 氨气

Abstract: MIL-53(Cr)crystals were synthesized by the hydrothermal synthesis method, and then modified by ammonia vapor of different concentrations to obtain the modified materials NH₃@MIL-53(Cr). The CO₂ and water vapor isotherms on the NH₃@MIL-53(Cr)were determined by means of the gravity method. Although the specific surface area of the modified materials NH3@MIL-53(Cr)became smaller compared to original MIL-53(Cr), their CO₂ adsorption capacities per unit surface area of adsorbent became significantly higher, following the order: NH₃@MIL-53(Cr)-3#>NH₃@MIL-53(Cr)-2#>NH₃@MIL-53(Cr)-1#. In addition, Isotherms of water vapor on the modified samples NH3@MIL-53(Cr) were lower than those on the MIL-53(Cr), suggesting significant improvement of hydrophobicity of the modified samples. The CO₂ adsorption capacity of the NH₃@MIL-53(Cr)-2# modified by using ammonia vapor of 1 mol·L^-1 was the highest among the modified samples. More interestingly, the CO₂ adsorption performance of the modified sample NH3@MIL-53 (Cr)-2# was significantly improved, while its CH₄ adsorption performance was weakened, which would be helpful to enhance its selectivity for CO₂/CH₄ adsorption.

Key words: MIL-53(Cr), CO₂, CH₄, water vapor, adsorption, ammonia vapor

中图分类号:

TQ013

杨琰, 王莎, 张志娟, 夏启斌, 李忠. 氨气改性的NH₃@MIL-53(Cr)吸附CO₂和CH₄的性能[J]. 化工学报, DOI: 10.3969/j.issn.0438-1157.2014.05.028.

YANG Yan, WANG Sha, ZHANG Zhijuan, XIAQibin, LI Zhong. CO₂ and CH₄ adsorption performance of modified MIL-53(Cr) via ammonia vapor[J]. CIESC Journal, DOI: 10.3969/j.issn.0438-1157.2014.05.028.

参考文献 20

[1]	Férey G. Hybrid porous solids: past, present, future [J]. Chem . Soc . Rev., 2008, 37(1): 191-214
[2]	Yang Q Y, Liu D H, Zhong C L, Li J R. Development of computational methodologies for metal-organic frameworks and their application in gas separations[J].Chem. Rev., 2013, 11(3): 8261-8323
[3]	Hiroyasu F, Kyle E C, Michael O K, Omar M,Yaghi O M. The chemistry and applications of metal-organic frameworks [J].Science, 2013, 34(1):1230444
[4]	Serre C, Millange F, Surble S. A route to the synthesis of trivalent transition-metal porous carboxylates with trimeric secondary building units [J]. Angew.Chem. Int. Ed., 2004, 43(46): 6286-6289
[5]	Millange F, Serre C, Guillou N. Structural effects of solvents on the breathing of metal-organic frameworks: an in situ diffraction study [J]. Angew.Chem. Int. Ed., 2008, 47(22): 4100-4105
[6]	Llewellyn P L, Bourrelly S, Serre C. Prediction of the conditions for breathing of metal organic frame work materials using a combination of X-ray powder diffraction, micro calorimetric, and molecular simulation [J]. J. Am. Chem. Soc., 2008, 130(38): 12808-12814
[7]	Llewellyn P L, Serre C, Férey G. Co-adsorption and separation of CO2-CH4 [J]. J. Am. Chem. Soc., 2009, 131(47): 17490-17499
[8]	Alexander V, Coudert F, Boutm A. Stress-based model for the breathing of metal-organic frameworks [J].J. Phys. Chem. Lett., 2010, 1(1): 445-449
[9]	David S C, Furio C, Robert G B. Sorption-induced breathing in the flexible metal organic framework MIL-53: force-field simulations and electronic structure analysis [J]. J. Phys. Chem. C, 2009, 113(2): 544-552
[10]	Huang Haifeng(黄海凤), Chu Xiang(褚翔), Lu Hanfeng(卢晗锋). Dynamic adsorption performances and breakthrough curve model of some aromatic VOCs on MCM-41 and SBA-15 [J]. J. Chem. Eng. of Chinese Univ. (高校化学工程学报), 2011, 25(2): 219-224
[11]	Yazayd?n A O, Snurr R Q, Park T H. Screening of metal organic frameworks for carbon dioxide capture from flue gas using a combined experimental and modeling approach [J]. J. Am. Chem. Soc., 2009, 131(51): 18198-18199
[12]	Alessandro D M, Smit B, Long J R. Carbon dioxide capture: prospects for new materials [J]. Angew.Chem. Int. Ed., 2010, 49(35): 6058-6082
[13]	Llewellyn P L, Bourrelly S, Serre C. How hydration drastically improves adsorption selectivity for CO2 over CH4 in the flexible chromium terephthalate MIL-53 [J]. J.Am .Chem Soc., 2002, 124(45): 13519-13526
[14]	Yaghi O M. Reticular synthesis and the design of new materials [J]. Nature, 2003, 423(6941): 705 -714
[15]	Seo J S.A homo-chiral metal-organic porous material for enation selective separation and catalysis [J]. Nature, 2000, 404(6781): 982-986
[16]	Bauer C, Serre T, Devic P, Horcajada J, Marrot G, Ferey N. High-throughput assisted rationalization of the formation of metal organic frameworks in the iron (III) amino terephthalate solved thermal system [J]. Inorg. Chem., 2008, 4(7): 7568-7576
[17]	Zhang Z J, Xian S K, Xia Q B, Wang H H, Li Z, Li J. Enhancement of CO2 adsorption and CO2/N2 selectivity on ZIF-8 via polysynthetical modification[J]. AIChE J., 2013, 59(6): 2195-2206
[18]	Zhang Z J, Li Z. Improvement of CO2 adsorption on ZIF-8 crystals modified by enhancing basicity of surface[J]. Chem. Eng. Sci., 2011, 6(6):4878
[19]	Liu D F, Wu Y B, Xia Q B, Li Zhong, Xi H X. Experimental and molecular simulation studies of CO2 adsorption on zeolite imidazole frameworks: ZIF-8 and amine-modified ZIF-8[J]. Adsorption, 2013, 19(1):25-37
[20]	Serre C, Millange F, Thouvenot C. Very large breathing effect in the first nano-porous chromium(Ⅲ)- based solids: MIL-53 or CrⅢ(OH)3. [J]. J. Am. Chem. Soc., 2002, 124(45): 13519-13526

氨气改性的NH₃@MIL-53(Cr)吸附CO₂和CH₄的性能

CO₂ and CH₄ adsorption performance of modified MIL-53(Cr) via ammonia vapor

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

参考文献 20

相关文章 15

编辑推荐

Metrics

本文评价

[1]	晁京伟, 许嘉兴, 李廷贤. 基于无管束蒸发换热强化策略的吸附热池的供热性能研究[J]. 化工学报, 2023, 74(S1): 302-310.
[2]	宋瑞涛, 王派, 王云鹏, 李敏霞, 党超镔, 陈振国, 童欢, 周佳琦. 二氧化碳直接蒸发冰场排管内流动沸腾换热数值模拟分析[J]. 化工学报, 2023, 74(S1): 96-103.
[3]	张义飞, 刘舫辰, 张双星, 杜文静. 超临界二氧化碳用印刷电路板式换热器性能分析[J]. 化工学报, 2023, 74(S1): 183-190.
[4]	杨学金, 杨金涛, 宁平, 王访, 宋晓双, 贾丽娟, 冯嘉予. 剧毒气体PH₃的干法净化技术研究进展[J]. 化工学报, 2023, 74(9): 3742-3755.
[5]	程业品, 胡达清, 徐奕莎, 刘华彦, 卢晗锋, 崔国凯. 离子液体基低共熔溶剂在转化CO₂中的应用[J]. 化工学报, 2023, 74(9): 3640-3653.
[6]	盛冰纯, 于建国, 林森. 铝基锂吸附剂分离高钠型地下卤水锂资源过程研究[J]. 化工学报, 2023, 74(8): 3375-3385.
[7]	张瑞航, 曹潘, 杨锋, 李昆, 肖朋, 邓春, 刘蓓, 孙长宇, 陈光进. ZIF-8纳米流体天然气乙烷回收工艺的产品纯度关键影响因素分析[J]. 化工学报, 2023, 74(8): 3386-3393.
[8]	杨菲菲, 赵世熙, 周维, 倪中海. Sn掺杂的In₂O₃催化CO₂选择性加氢制甲醇[J]. 化工学报, 2023, 74(8): 3366-3374.
[9]	洪瑞, 袁宝强, 杜文静. 垂直上升管内超临界二氧化碳传热恶化机理分析[J]. 化工学报, 2023, 74(8): 3309-3319.
[10]	高燕, 伍鹏, 尚超, 胡泽君, 陈晓东. 基于双流体喷嘴的磁性琼脂糖微球的制备及其蛋白吸附性能探究[J]. 化工学报, 2023, 74(8): 3457-3471.
[11]	陈吉, 洪泽, 雷昭, 凌强, 赵志刚, 彭陈辉, 崔平. 基于分子动力学的焦炭溶损反应及其机理研究[J]. 化工学报, 2023, 74(7): 2935-2946.
[12]	刘晓洋, 喻健良, 侯玉洁, 闫兴清, 张振华, 吕先舒. 螺旋微通道对掺氢甲烷爆轰传播的影响[J]. 化工学报, 2023, 74(7): 3139-3148.
[13]	王杰, 丘晓琳, 赵烨, 刘鑫洋, 韩忠强, 许雍, 蒋文瀚. 聚电解质静电沉积改性PHBV抗氧化膜的制备与性能研究[J]. 化工学报, 2023, 74(7): 3068-3078.
[14]	张琦钰, 高利军, 苏宇航, 马晓博, 王翊丞, 张亚婷, 胡超. 碳基催化材料在电化学还原二氧化碳中的研究进展[J]. 化工学报, 2023, 74(7): 2753-2772.
[15]	牛超, 沈胜强, 杨艳, 潘泊年, 李熠桥. 甲烷BOG喷射器流动过程计算与性能分析[J]. 化工学报, 2023, 74(7): 2858-2868.