工程科学学报2025,Vol.47Issue(1):170-178,9.DOI:10.13374/j.issn2095-9389.2024.04.22.001
基于载锰沸石分子筛的臭氧催化分解特性
Catalytic decomposition of ozone in air by Mn-modified zeolite molecular sieves
摘要
Abstract
Ozone is a significant indoor air pollutant found in our daily lives.To effectively purify this pollutant at its source,it is essential to develop a high-efficiency ozone decomposition converter,with the catalyst being its pivotal component.This study investigates the catalytic performance of modified zeolites for ozone decomposition by adjusting their topological structure,cation form,modification,and drying methods to enhance their adsorption and catalytic properties.The Mn-USY-DT/WB zeolite catalyst demonstrated effective and stable ozone purification for more than 30 h at-5℃and 720000 h-1,outperforming commercial MnO2 catalysts in regeneration.X-ray photoelectron spectroscopy(XPS)characterization revealed that the decrease in the average oxidation state of Mn decreased from 2.95 to 2.81 after regeneration.The X-ray diffraction(XRD)results show that the cationic modification did not alter the crystal structure of the zeolite molecular sieve.The BET results indicate a slight reduction in the specific surface area of the modified samples,with Mn-USY-YX showing a significant drop to 146 m2·g-1 owing to the formation of a large number of hydrates during the liquid phase sampling,which was difficult to remove by calcination.The primary pore sizes varied among the samples,with the USY series at approximately 0.74 nm,Mn-Beta-DT zeolite at 0.58 nm,and Mn-ZSM-5-DT at 0.55 nm.The EDS images of the sample show that the content of Mn in Mn-USY-YX was low and that the Mn distribution was distinct.The Mn distribution in the Mn-USY-DT/WB sample was uniform,mostly in a linear arrangement along the crystal structure.The Mn element was obviously aggregated in the Mn-USY-DT/CG sample.Adjusting modification and drying methods helps preserve metal cationic clusters within the zeolite skeleton,preventing aggregation and enhancing catalyst activity.We propose a mechanism for long-term stable catalysis of ozone based on the coordination of ozone molecule adsorption and catalytic decomposition on zeolite,explaining the observed efficiency over time.The optimized zeolite powder was coated on a glass fiber support to obtain a low-gas-resistance monolithic honeycomb catalyst that maintains≥99.9%efficiency for over 1000 h in practical applications.关键词
臭氧/催化剂/沸石分子筛/整体式蜂窝催化剂/再生Key words
ozone/catalyst/zeolite molecular sieves/monolithic honeycomb catalyst/regeneration分类
化学化工引用本文复制引用
陈浩玥,郭卓男,刘应书,杨雄,裴有康,李子宜..基于载锰沸石分子筛的臭氧催化分解特性[J].工程科学学报,2025,47(1):170-178,9.基金项目
国家自然科学基金资助项目(52370107) (52370107)
北京市自然科学基金资助项目(L233015) (L233015)
北京市科技新星计划(20240484685) (20240484685)