Adsorptive removal of nitrogen-containing compounds from fuel by metal-organic frameworks

能源化学(英文) ›› 2013, Vol. 22 ›› Issue (6): 869-875.

Adsorptive removal of nitrogen-containing compounds from fuel by metal-organic frameworks

Zhaoyang Wang, Zhiguo Sun, Linghao Kong, Gang Li

State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, Liaoning, China

收稿日期:2013-04-24 修回日期:2013-06-28 出版日期:2013-11-20 发布日期:2013-11-28
通讯作者: Gang Li
基金资助:
This work was supported by the Program for New Century Excellent Talents in University (NCET-04-0270) and National Basic Research Program of China (2011CB201301).

Adsorptive removal of nitrogen-containing compounds from fuel by metal-organic frameworks

Zhaoyang Wang, Zhiguo Sun, Linghao Kong, Gang Li

State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, Liaoning, China

Received:2013-04-24 Revised:2013-06-28 Online:2013-11-20 Published:2013-11-28
Supported by:
This work was supported by the Program for New Century Excellent Talents in University (NCET-04-0270) and National Basic Research Program of China (2011CB201301).

摘要/Abstract

摘要： The adsorptive denitrogenation from fuels over three metal-organic frameworks (MIL-96(Al), MIL-53(Al) and MIL-101(Cr)) was studied by batch adsorption experiments. Four nitrogen-containing compounds (NCCs) pyridine, pyrrole, quinoline and indole were used as model NCCs in fuels to study the adsorption mechanism. The physicochemical properties of the adsorbents were characterized by XRD, N₂ physical adsorption, FT-IR spectrum and Hammett indicator method. The metal-organic frameworks (MOFs), especially the MIL-101(Cr) containing Lewis acid sites as well as high specific surface area, can adsorb large quantities of NCCs from fuels. In addition, the adsorptive capacity over MIL-101(Cr) will be different for NCCs with different basicity. The stronger basicity of the NCC is, the more it can be absorbed over MIL-101(Cr). Furthermore, pore size and shape also affect the adsorption capacity for a given adsorbate, which can be proved by the adsorption over MIL-53(Al) and MIL-96(Al). The pseudo-second-order kinetic model and Langmuir equation can be used to describe kinetics and thermodynamics of the adsorption process, respectively. Finally, the regeneration of the used adsorbent has been conducted successfully by just washing it with ethanol.

关键词: metal-organic framework, nitrogen-containing compound, adsorptive denitrogenation, denitrogenation kinetics, denitrogenation thermodynamics

Abstract: The adsorptive denitrogenation from fuels over three metal-organic frameworks (MIL-96(Al), MIL-53(Al) and MIL-101(Cr)) was studied by batch adsorption experiments. Four nitrogen-containing compounds (NCCs) pyridine, pyrrole, quinoline and indole were used as model NCCs in fuels to study the adsorption mechanism. The physicochemical properties of the adsorbents were characterized by XRD, N₂ physical adsorption, FT-IR spectrum and Hammett indicator method. The metal-organic frameworks (MOFs), especially the MIL-101(Cr) containing Lewis acid sites as well as high specific surface area, can adsorb large quantities of NCCs from fuels. In addition, the adsorptive capacity over MIL-101(Cr) will be different for NCCs with different basicity. The stronger basicity of the NCC is, the more it can be absorbed over MIL-101(Cr). Furthermore, pore size and shape also affect the adsorption capacity for a given adsorbate, which can be proved by the adsorption over MIL-53(Al) and MIL-96(Al). The pseudo-second-order kinetic model and Langmuir equation can be used to describe kinetics and thermodynamics of the adsorption process, respectively. Finally, the regeneration of the used adsorbent has been conducted successfully by just washing it with ethanol.

Key words: metal-organic framework, nitrogen-containing compound, adsorptive denitrogenation, denitrogenation kinetics, denitrogenation thermodynamics

Zhaoyang Wang, Zhiguo Sun, Linghao Kong, Gang Li. Adsorptive removal of nitrogen-containing compounds from fuel by metal-organic frameworks[J]. 能源化学(英文), 2013, 22(6): 869-875.

Zhaoyang Wang, Zhiguo Sun, Linghao Kong, Gang Li. Adsorptive removal of nitrogen-containing compounds from fuel by metal-organic frameworks[J]. Journal of Energy Chemistry, 2013, 22(6): 869-875.

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Adsorptive removal of nitrogen-containing compounds from fuel by metal-organic frameworks

Adsorptive removal of nitrogen-containing compounds from fuel by metal-organic frameworks

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