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Alkali metal cation doping of metal-organic framework for enhancing carbon dioxide adsorption capacity

Journal of Energy Chemistry 2014年第4期23卷 468-474页

作者： Yan Cao Yunxia Zhao Fujiao Song Qin Zhong School of Chemical Engineering Nanjing University of Science and Technology School of Environmental Science and Engineering Yancheng Institute of Technology

Metal-organic frameworks （MOFs） have attracted much attention as adsorbents for the separation of CO2 from flue gas or natural gas. Here, a typical metal-organic framework HKUST-I（also named Cu-BTC or MOF-199） was chemically reduced by doping it with alkali metals （Li, Na and K） and they were further used to investigate their CO2 adsorption capacities. The structural information, surface chemistry and thermal behavior of the prepared adsorbent samples were characterized by X-ray powder diffraction （XRD）, thermo-gravimetric analysis （TGA） and nitrogen adsorption-desorption isotherm analysis. The results showed that the CO2 storage capacity of HKUST-1 doped with moderate quantities of Li＋, Na＋ and K＋, individually, was greater than that of unmodified HKUST-1. The highest CO2 adsorption uptake of 8.64 mmol/g was obtained with 1K-HKUST-1, and it was ca. 11% increase in adsorption capacity at 298 K and 18 bar as compared with HKUST- 1. Moreover, adsorption tests showed that HKUST-1 and 1K-HKUST-1 displayed much higher adsorption capacities of CO2 than those of N2. Finally, the adsorption/desorption cycle experiment revealed that the adsorption performance of 1K-HKUST-1 was fairly stable, without obvious deterioration in the adsorption capacity of CO2 after 10 cycles.

关键词： metal-organic framework HKUST-1 carbon dioxide adsorption alkali metals cation doping adsorption-desorption cycles

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Numerical simulations and comparative analysis of two- and three-dimensional circulating fluidized bed reactors for CO2 capture

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Chinese Journal of Chemical Engineering 2020年第12期28卷 2955-2967页

作者： Yefeng Zhou Yifan Han Yujian Lu Hongcun Bai Xiayi Hu Xincheng Zhang Fanghua Xie Xiao Luo Jingdai Wang Yongrong Yang National&Local United Engineering Research Centre for Chemical Process Simulation and Intensification Chemical Process Simulation and Optimization Engineering Research Center of Ministry of EducationXiangtan UniversityXiangtan 411105China State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering Ningxia UniversityYinchuan 750021China College of Chemistry and Chemical Engineering Hunan UniversityChangsha 410082China State Key Laboratory of Chemical Engineering College of Chemical and Biological EngineeringDepartment of Chemical EngineeringZhejiang UniversityHangzhou 310027China

carbon dioxide(CO2),the main gas emitted from fossil burning,is the primary contributor to global warming.Circulating fluidized bed reactor(CFBR)is proved as an energy-efficient method for post-combustion CO2 capture.The numerical simulation by computational fluid dynamics(CFD)is believed as a promising tool to study CO2 adsorption process in CFBR.Although three-dimensional(3D)simulations were proved to have better predicting performance with the experimental results,two-dimensional(2D)simulations have been widely reported for qualitative and quantitative studies on gas-solid behavior in CFBR for its higher computational efficiency recently.However,the discrepancies between 2D and 3D simulations have rarely been evaluated by detailed study.Considering that the differences between the 2D and 3D simulations will vary substantially with the changes of independent operating conditions,it is beneficial to lower computational costs to clarify the effects of dimensionality on the numerical CO2 adsorption runs under various operating conditions.In this work,the comparative analysis for CO2 adsorption in 2D and 3D simulations was conducted to enlighten the effects of dimensionality on the hydrodynamics and reaction behaviors,in which the separation rate,species distribution and hydrodynamic characteristics were comparatively studied for both model frames.With both accuracy and computational costs considered,the viable suggestions were provided in selecting appropriate model frame for the studies on optimization of operating conditions,which directly affect the capture and energy efficiencies of cyclic CO2 capture process in CFBR.

关键词： Two-and three-dimensional simulations Circulating fluidized bed reactor carbon dioxide adsorption Computational fluid dynamics Operating conditions

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Capture of carbon dioxide from flue gas on TEPA-grafted metal-organic framework Mg_2 (dobdc)

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Journal of Environmental Sciences 2013年第10期25卷 2081-2087页

作者： Yan Cao Fujiao Song Yunxia Zhao Qin Zhong School of Chemical Engineering Nanjing University of Science and Technology School of Environmental Science and Engineering Yancheng Institute of Technology

carbon dioxide （CO2） adsorption on a standard metal-organic framework Mg2（dobdc）（Mg/DOBDC or Mg-MOF-74） and a tetraethylenepentamine （TEPA） modified Mgz（dobdc）（TEPA-Mg/DOBDC） were investigated and compared. The structural information, surface chemistry and thermal behavior of the adsorbent samples were characterized by X-ray powder diffraction （XRD）, infrared spectroscopy （IR）, thermogravimetric analysis （TGA） and nitrogen adsorption-desorption isotherm analysis. CO2 adsorption capacity was measured by dynamic adsorption experiments with N2-CO2 mixed gases at 60℃. Results showed that the CO2 adsorption capacity of Mg/DOBDC was significantly improved after amine modification, with an increase from 2.67 to 6.06 mmol CO2/g adsorbent. Moreover, CO2 adsorption on the TEPA-Mg/DOBDC adsorbent was promoted by water vapor, and the adsorption capacity was enhanced to 8.31 mmol CO2/g absorbent. The adsorption capacity of the TEPA-Mg/DOBDC adsorbent dropped only 3% after 5 consecutive adsorption]desorption cycles. Therefore, this kind of adsorbent can be considered as a promising material for the capture of CO2 from flue gas.

关键词： metal-organic framework amine modification carbon dioxide adsorption

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Microwave-assisted Ionothermal Synthesis and Characteriza- tion of Zeolitic Imidazolate Framework-8

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Chinese Journal of Chemistry 2012年第5期30卷 1040-1044页

作者：杨丽莎卢惠民 School of Materials Science and Engineering Beihang UniversityBeijing 100191China

The zeolitic imidazolate framework-8 （ZIF-8） was successfully synthesized using ionic liquids as struc- ture-directing agent under microwave irradiation. Ionic liquids are green solvents with low vapour pressure and good thermal stability. They are appropriate templates for microporous materials and ideal microwave absorbers. The microwave-assisted ionothermal synthesis applied in this paper was expected to be a promising method for the preparation of microporous materials. Results showed that the as-synthesized samples （300---500 nm in diameter） could be synthesized in a short time （60 min） and possessed regular morphology, stable structure and high thermal stability （up to 720 ~C in argon atmosphere）. Nitrogen adsorption-desorption test illustrated that samples produced by microwave heating had a higher surface area. carbon dioxide adsorption test indicated that the samples synthe- sized by microwave heating had better carbon dioxide adsorption ability than those by conventional heating.

关键词： microporous materials ionic liquids microwave carbon dioxide adsorption ZIF-8

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