CN-122006686-A - High-efficiency selective adsorption SO2Amine functionalized rod-like MCM-41 adsorbent of (C)

Abstract

The invention discloses an amine functional rod-shaped MCM-41 adsorbent capable of efficiently and selectively adsorbing SO 2 and a preparation method thereof, belonging to the technical field of material preparation and environmental purification. The rod-shaped mesoporous MCM-41 carrier is synthesized by self-assembly by a co-template method, and a triethanolamine/imidazole eutectic solvent is further loaded on the carrier to form a composite adsorbent, SO that high-efficiency adsorption of SO 2 can be realized, and selective removal of SO 2 can be realized under an environment containing N 2 、CO 2 、H 2 O. The invention has simple preparation process, stable structure and good regeneration performance, is suitable for high-efficiency trapping of low-concentration SO 2 in industrial flue gas, and has remarkable environmental benefit and application prospect.

Inventors

• XIAO YIHONG
• LEI YUANYI
• LI YAN
• ZHENG YONG
• CHEN SHILONG
• LIU FUJIAN
• JIANG LILONG

Assignees

• 福州大学

Dates

Publication Date

20260512

Application Date

20260320

Claims (8)

1. 1. A preparation method of an amine functionalized rod-shaped MCM-41 adsorbent is characterized by comprising the following steps: s1, synthesizing a molecular sieve, namely adding a template agent and ammonia water into deionized water, stirring for 15min, adding tetraethyl orthosilicate serving as a silicon source, and continuously stirring for 5h; S2, preparing a eutectic solvent, namely mixing triethanolamine with imidazole, stirring for 24 hours at 50 ℃, and vacuum drying at 60 ℃ to obtain the triethanolamine/imidazole eutectic solvent; And S3, synthesizing the adsorbent, namely dispersing the eutectic solvent prepared by the S2 and the molecular sieve prepared by the S1 in methanol, continuously stirring at room temperature for 12 hours, and vacuum drying at 60 ℃ to obtain the amine functional rodlike MCM-41 adsorbent.
2. 2. The method according to claim 1, wherein in the step S1, the template agent is cetyl trimethyl ammonium bromide and tetrabutyl ammonium bromide.
3. 3. The method according to claim 1, wherein in step S1, the molar ratio of the reactants is CTAB: TBAB: NH 4 OH：TEOS：H 2 O=0.1:0.05-0.08:2.5:1:588.
4. 4. The method according to claim 1, wherein in the step S1, the stirring speed is 100-500rpm, the drying temperature is 80 ℃, the time is 24 hours, the baking temperature is 550 ℃, and the time is 5 hours.
5. 5. The method according to claim 1, wherein in step S2, the molar ratio of triethanolamine to imidazole is 1-2:1.
6. 6. The method according to claim 1, wherein in the step S3, the mass ratio of the eutectic solvent, methanol and molecular sieve is 2-3:10:1.
7. 7. An amine functionalized rod-shaped MCM-41 adsorbent made by the process of any one of claims 1-6.
8. 8. Use of an amine functional rod-like MCM-41 adsorbent prepared according to any one of claims 1-6 in a selective adsorption SO 2 reaction, wherein the amine functional rod-like MCM-41 adsorbent is selectively adsorbed to and removed from SO 2 in a mixed atmosphere containing 5-1000ppm SO 2 、10-25vol.%CO 2 、3-10vol.%H 2 O and the balance N 2 .

Description

Amine functional rod-shaped MCM-41 adsorbent capable of efficiently and selectively adsorbing SO 2 Technical Field The invention belongs to the technical field of material preparation and environmental purification, relates to a preparation technology and application of an amino functionalized rodlike MCM-41 adsorbent, and in particular relates to a method for synthesizing an MCM-41 material by using a triethanolamine/imidazole eutectic solvent functionalized co-template method and application of the MCM-41 material in high-selectivity removal of SO 2. Background Sulfur dioxide (SO 2) is used as colorless toxic gas, the emission of which is closely related to human industrial activities and energy consumption, and is one of core pollutants causing environmental problems such as acid rain, atmospheric pollution and the like. Therefore, the development of the efficient SO 2 removal technology reduces the concentration of the high-efficiency SO 2 in the atmosphere environment from the source, and has important practical significance for reducing the occurrence frequency and intensity of acid rain and guaranteeing the safety of ecological environment. In various SO 2 removal technologies, the adsorption method has been paid attention to because of the advantages of simple operation, low energy consumption, no secondary pollution and the like, wherein the amine functional material is proved to be a high-efficiency SO 2 adsorption system. The material can obviously increase the contact area of a gas-solid interface by loading the amine-containing functional component into the porous solid carrier pore canal, and simultaneously improve the mass transfer efficiency in the adsorption/desorption cycle process, thereby enhancing the adsorption performance of SO 2. Thus, in the development of new adsorbents, researchers have mostly cut into optimization from two core dimensions of functional components and support materials. On the one hand, the choice of the functional component is critical for optimizing the performance of the amine functionalized adsorbent. The triethanolamine and the imidazole both contain tertiary amine groups and have high affinity to SO 2, and the triethanolamine/imidazole (TI) eutectic solvent is synthesized by the triethanolamine and the imidazole, SO that the selective reversible adsorption of SO 2 can be realized by means of intermolecular hydrogen bond action and self alkalinity of the solvent, and high-quality functional component selection is provided for efficiently capturing SO 2. On the other hand, the structure and performance of the carrier directly determine the loading efficiency, dispersion uniformity and circulating stability of the adsorbent of the amine functional component, and are core factors influencing the removal effect of SO 2. In order to match the loading requirement of the TI eutectic solvent and improve the adsorption activity, the carrier needs to have high specific surface area, regular pore structure and good framework stability. Molecular sieve materials are considered to be excellent carriers for immobilizing amine functional components because of the combination of the above properties. The MCM-41 molecular sieve is taken as a typical mesoporous molecular sieve, has adjustable aperture, a highly ordered hexagonal mesoporous structure and large specific surface area, has good skeleton stability, can effectively maintain structural integrity in repeated adsorption and desorption cycles, can provide rich loading sites and uniform dispersion space for amine functional components, and further ensures the regeneration performance of the adsorbent. However, the morphology and the pore canal structure of the traditional MCM-41 molecular sieve still have an optimization space, and the composition of the template agent is a key factor for regulating the morphology, the pore size and the pore canal structure, namely, the suitability of the molecular sieve as a carrier can be further improved by constructing the rod-shaped MCM-41 by optimizing a template agent system. At present, related reports that a rodlike mesoporous MCM-41 molecular sieve is prepared by a co-template method and is used as a carrier to load TI eutectic solvent to prepare an amine functional adsorbent for SO 2 adsorption are not yet seen in the prior art. In view of the above, the invention innovatively adopts a co-template method to prepare a rod-shaped mesoporous MCM-41 molecular sieve as a carrier, loads TI amino functional eutectic solvent, and constructs an SO 2 adsorption system with high selectivity and high adsorption activity. The innovative design can fully exert the structural advantage of the rod-shaped MCM-41 and the amino function advantage of the TI eutectic solvent, and improves the utilization efficiency of the amine, SO that the high-efficiency purification of SO 2 in the actual industrial complex gas environment is realized, and the novel industrial complex gas environment has importa