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Cooperative chemical adsorption of acid gases in functionalized metal-organic frameworks

An acid gas, organic framework technology, applied in the field of metal-organic frameworks with metal atoms, which can solve problems such as reduced adsorption capacity

Active Publication Date: 2017-02-22
RGT UNIV OF CALIFORNIA
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0020] Although MOFs offer well-defined porosity, high surface area, and tunable chemical functionality, because many materials are hydrophilic and it has been observed that CO 2 The adsorption capacity is significantly reduced, which limits their applications

Method used

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  • Cooperative chemical adsorption of acid gases in functionalized metal-organic frameworks
  • Cooperative chemical adsorption of acid gases in functionalized metal-organic frameworks
  • Cooperative chemical adsorption of acid gases in functionalized metal-organic frameworks

Examples

Experimental program
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Effect test

example 1

[0107] To illustrate the present technique, several metal-organic frameworks (mmen-M 2 (dobpdc): mmen=N, N'-dimethylethylenediamine; M=Mg, Mn, Fe, Co, Zn; dobpdc 4- = 4,4'-Dioxybiphenyl-3,3'-dicarboxylate).

[0108] All reagents and solvents were purchased and were of reagent grade purity or higher; N,N'-dimethylethylenediamine (mmen) was dissolved in n-hexane to form a stock solution with a concentration of 10% v / v for amines functional reaction. mmen solution in N 2 stored in a 200 mL Schlenk bottle under conditioned conditions and by adding freshly ground CaH 2 Keep sewage free of moisture. Compound H 4 (dobpdc) was synthesized using conventional methods.

[0109] for Mg 2 (dobpdc) synthesis, the H 4 dobpdc (27.4mg, 0.10mmol) was added to a 20ml glass scintillation vial, followed by Mg(NO 3 ) 2 ·6H 2 O (64.0 mg, 0.25 mmol) and 10 ml of mixed solvent (55:45 MeOH:DMF). The scintillation vials were then sealed with polytetrafluoroethylene (PTFE) lined caps and plac...

example 2

[0113] To further illustrate the principle of operation of the method, spectroscopic and diffraction measurements were used to determine the sorbent (such as mmen-Mg 2 (dobpdc)) Adsorption of CO 2 The mechanism behind the formation of steep steps. In particular, in the isomeric compound mmen-Mn 2 Powder X-ray diffraction studies performed on (dobpdc) provide insight into the CO 2 How to key in specific structural information in the channel of the material. After exposing the sample to 5 bar CO 2 Diffraction data collected at 100K before or after showed only a 1.112(8)% shrinkage in unit cell volume, but exhibited large changes in the relative intensities of selected diffraction peaks.

[0114] By using the simulated annealing method, a complete structural model for data setting is formed, such as Rietveld refinement of the data after implementation by TOPAS-Academic software. When exposed to CO 2 Previously, the mmen molecule was bonded to the Mn through an amine group ...

example 3

[0118] CO 2 The adsorption mechanism suggests that changes in the metal-amine bond strength may provide a means to tune the position of the isotherm step. Measured Mmen-M 2 CO of (dobpdc)(M=Mg, Mn, Fe, Co, Ni, Zn) compounds at 25, 40, 50 and 75°C 2 Adsorption isotherm series. With the exception of Ni compounds that show conventional Langmuir-type adsorption behavior, all other materials show steep isotherm steps that shift to higher pressures with increasing temperature. The Hill coefficients of M=Mg, Mn, Fe, Co, and Zn are 10.6, 5.6, 7.5, 11.5, and 6.0, respectively, through the analysis of the isotherm ladder at 25°C, reflecting the CO 2 Synergy of adsorption mechanism.

[0119] For a given temperature, the step position varies in the order of Mg<Mn<Fe<Zn<Co, which agrees with the published series for the stability of octahedral transition metal compounds. Ni compounds do not have steps even under very high pressure conditions, due to the special stability of the Ni-mme...

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Abstract

A system and method for acid gas separations using porous frameworks of metal atoms coordinatively bound to polytopic linkers that are functionalized with basic nitrogen ligands that expose nitrogen atoms to the pore volumes forming adsorption sites. Adjacent basic nitrogen ligands on the metal-organic framework can form an ammonium from one ligand and a carbamate from the other. The formation of one ammonium carbamate pair influences the formation of ammonium carbamate on adjacent adsorption sites. Adsorption of acid gas at the adsorption sites form covalently linked aggregates of more than one ammonium carbamate ion pair. The acid gas adsorption isotherm can be tuned to match the step position with the partial pressure of acid gas in the gas mixture stream through manipulation of the metal-ligand bond strength by selection of the ligand, metal and polytopic linker materials.

Description

[0001] Cross References to Related Applications [0002] This application claims priority and benefit to US Provisional Patent Application No. 61 / 982,620, filed April 22, 2014, which is hereby incorporated by reference in its entirety. This application is also a continuation-in-part of U.S. Patent Application No. 14 / 228,532, filed March 28, 2014, the entire contents of which are hereby incorporated by reference; the U.S. Patent Application No. PCT / US2012 / 060915, a continuation under 35 U.S.C § 111(a) of PCT International Application filed October 18, 2012, the entire contents of which are hereby incorporated by reference; this PCT International Application claims Application No. 61 / 548,676, application The benefit of US Provisional Patent Application dated October 18, 2011, the entire contents of which are hereby incorporated by reference. This application claims priority to each of the above applications. [0003] The PCT International Publication No. of the PCT internationa...

Claims

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Application Information

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IPC IPC(8): B01D53/02B01D53/40
CPCB01D53/02B01D2253/204B01D2257/504B01J20/226B01J20/3085B01J20/3483B01J20/3425Y02C20/40
Inventor 杰弗里·朗托马斯·麦克唐纳
Owner RGT UNIV OF CALIFORNIA
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