CAJ | 학술논문

采用晶化培育法制备了L沸石纳米晶簇,以其作为前驱体,并以3-三甲基甲硅烷基丙基十六烷基二甲基氯化铵(TPHAC)为模板剂,合成了微孔.介孔多级孔道L沸石(MeLTL沸石).通过X射线衍射(XRD)、氮气吸附.脱附、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、~(27)Al固体魔角核磁(~(27)Al MAS NMR)和吡啶傅立叶变换红外(Py-FTIR)等方法对MeLTL沸石进行了表征.研究结果表明,MeLTL沸石是由L沸石纳米晶簇自组装形成的,并具有介孔孔道和L沸石的微孔结构以及适宜的酸量与酸强度,其比表面积和孔体积分别高达611m~2·g~(-1)和0.696 cm~3·g~(-1).将MeLTL沸石作为添加剂引入柴油加氢脱硫催化剂载体中,并与添加L沸石、Al-MCM-41和仅以γ-Al_2O_3为载体的催化剂进行比较,其脱硫性能为最佳,经加氢后的柴油硫含量仅为9.3 μg·g~(-1),脱硫率达99.3%.
채용정화배육법제비료L비석납미정족,이기작위전구체,병이3-삼갑기갑규완기병기십륙완기이갑기록화안(TPHAC)위모판제,합성료미공.개공다급공도L비석(MeLTL비석).통과X사선연사(XRD)、담기흡부.탈부、소묘전자현미경(SEM)、투사전자현미경(TEM)、~(27)Al고체마각핵자(~(27)Al MAS NMR)화필정부립협변환홍외(Py-FTIR)등방법대MeLTL비석진행료표정.연구결과표명,MeLTL비석시유L비석납미정족자조장형성적,병구유개공공도화L비석적미공결구이급괄의적산량여산강도,기비표면적화공체적분별고체611m~2·g~(-1)화0.696 cm~3·g~(-1).장MeLTL비석작위첨가제인입시유가경탈류최화제재체중,병여첨가L비석、Al-MCM-41화부이γ-Al_2O_3위재체적최화제진행비교,기탈류성능위최가,경가경후적시유류함량부위9.3 μg·g~(-1),탈류솔체99.3%.
Zeolite MeLTL with a micro-mesoporous composite pore structure was synthesized by using nanocrystal clusters of zeolite L prepared by the crystallization nurturing method as a precursor and [3-(trimethoxysilyl)propyl]hexadecyldimethylammonium chloride (TPHAC) as the organic mesopore directing surfactant. Several techniques including X-ray diffraction (XRD), nitrogen adsorption-desorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM), ~(27)Al magic angle spinning nuclear magnetic resonance (~(27)Al MAS NMR), and Fourier transform infrared spectroscopy of pyridine adsorption (Py-FTIR) were used to characterize the samples. Results show that zeolite MeLTL is formed by the self-assembly of zeolite L nanocrystals, and it has bimodal pore distributions with a stepwise mesoporous structure and the microporous structure of zeolite L. The BET surface area and the pore volume increased significantly and were 611 m~2·g~(-1) and 0.696 cm~3·g~(-1), respectively. Zeolite MeLTL was composed of zeolite L units and this was responsible for the adequate surface acid amount and acid strength. As a result, the pore diffusion ability and the catalytic performance of zeolite MeLTL are enhanced by the improvement in textural properties. For diesel hydrodesulfurization, the catalyst introduced zeolite MeLTL gave better hydrodesulfurization activity compared to the catalysts introduced zeolite L or Al-MCM-41 or used bare γ-Al_2O_3 as a support. The sulfur content of diesel oil after hydrotreatment was 9.3 μg·g~(-1) and the desulfurization rate was 99.3%.