HMFI分子筛Bronsted酸性位点与碱性分子的作用机制  

Interaction mechanism of Bronsted acid sites and basic molecules in HMFI zeolites

作　　者：郑健 秦康 秦玉才[2] 宋丽娟[2] ZHENG Jian;QIN Kang;QIN Yu-Cai;SONG Li-Juan(SINOPEC Research Institute of Petroleum Processing Co.Ltd.,Beijing 100083,China;Key Laboratory of Petrochemical Catalysis Science and Technology,Liaoning Shihua University,Fushun 113001,China)

机构地区：[1]中石化石油化工科学研究院有限公司,北京100083 [2]辽宁石油化工大学辽宁省石油化工催化科学与技术重点实验室,抚顺113001

出　　处：《原子与分子物理学报》2025年第4期1-7,共7页Journal of Atomic and Molecular Physics

基　　金：中石化科研项目(323063)。

摘　　要：采用密度泛函理论(DFT)方法,以单铝、双铝和三铝酸性位点HMFI分子筛为模型分子筛,计算去质子化能考察HMFI分子筛的本征酸性,以NH_(3)分子作为模型分子,计算NH_(3)分子在HMFI分子筛中的吸附能与去质子化能进行关联性分析,并进一步考察NH_(3)分子与HMFI分子筛的作用机制.研究表明分子筛Bronsted酸(简称B酸)强度与B酸数量没有强相关性,在考虑B酸位数量的同时须考虑B酸位的分布.酸性位点数量和分布的差异均可以调控NH_(3)分子的吸附构象,并且可以通过调节HMFI分子筛孔道对分子施加相互作用的模式,解析分子的结构和电子性质,精准调控分子的进一步转化.此项工作可以为未来高效多孔材料有效物种活性位的构建提供新思路.Using density functional theory(DFT)method,the intrinsic acidity of HMFI zeolites with single aluminum,double aluminum,and triple aluminum acid sites were investigated by calculating the deprotonation energies,the correlation between adsorption energies of NH_(3) and deprotonation energies in HMFI zeolites was analyzed by taking NH_(3) as model molecules,and the interaction mechanism between NH_(3) molecules and HMFI zeolites was further investigated.The results indicate that there is no strong correlation between acid strength of the Br nsted acid sites(BAS)and the number of the BAS in HMFI zeolites,thus the distribution of BAS should also be taken into account when considering the number of BAS.The number and distribution of BAS can regulate the adsorption conformation of NH_(3) molecules,and the further conversion of molecules can be precisely controlled by adjusting the interaction mode of HMFI zeolites and molecules and analyzing the structural and electronic properties of molecules.This work can provide new ideas for the construction of effective species sites in efficient porous materials in the future.

关 键 词：密度泛函理论 HMFI分子筛 Bronsted酸性质 吸附性能 

分 类 号：O643.36[理学—物理化学]