Development of a next generation cracking catalyst based on analysis of acidic property and structure of active site on USY zeolite

基于USY沸石酸性和活性位点结构的新一代裂化催化剂的开发

• 批准号: 17560681
• 负责人: KATADA Naonobu
• 金额: $ 1.95万
• 依托单位: Tottori University
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (C)
• 财政年份: 2005
• 资助国家: 日本
• 起止时间: 2005 至 2007
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-17560681/
• 关键词: zeolite; alkane cracking; petroleum refinery; solid acid catalyst; ammonia IRMS-TPD; ultrastable Y zeolite; alkylation of aromatics; EDTA

Properties of Bronsted and Lewis acid sites and number of Bronsted acid strength of OH groups on various zeolites became able to be measured by developing the ammonia IRMS-TPD method. Treatment of USY zeolite with an EDTA-salt with neutral property increased strong Bronsted aridity. The presence of strained tetra-coordinated and extraframework Al species on EDTA-USY, this is considered to be the origin of the strong Bronsted acidity. This was identified by 16T NMR. By the IRMS-TPD, the string acidity of OH was directly observed, and this was the first direct observation of active site for alkane cracking on USY.Applying with quantum calculation, it was clarified that extraframework AlOH coordinated at the window of hexagonal prism enhanced the Bronsted acidity of adjacent OH. This is the origin of cracking activity of USY. At the same position, Ca etc. also enhanced the acidity.Thus the structure of alkane cracking site was clarified. Application of these catalysts to octane cracking showed a potential activity for next generation catalyst.In addition, acidic property of a mesoporous zeolite, which was expected to have a potential for cracking of heavy oil, has been analyzed for the first time. WO_3/ZrO_2 was also analyzed. A method for analysis of the adsorption heat of aromatic molecule on zeolite was developed.

Bronsted和Lewis酸位点的性质以及OH基团在各种沸石上的Bronsted Acid强度的数量，可以通过开发IRMS-TPD方法来测量。用具有中性特性的EDTA盐处理USY沸石的强化较强的布朗斯特式干旱。在Edta-usy上存在紧张的四链和外部炸药，这被认为是强bronsted酸度的起源。这是通过16T NMR确定的。通过IRMS-TPD，直接观察到OH的弦酸度，这是对烷烃在USY上开裂的活性位点的第一个直接观察。使用量子计算，可以澄清说，在六边形棱镜窗口中协调的外部框架ALOH增强了相邻OH的Bronsted Acudity。这是USY开裂活动的起源。在同一位置，CA等也增强了酸度。因此，阐明了烷烃开裂位点的结构。这些催化剂在辛烷值开裂中的施用显示了下一代催化剂的潜在活性。此外，首次分析了中孔沸石的酸性特性，预计中孔沸石有可能有可能破裂的重油。还分析了WO_3/ZRO_2。开发了一种分析芳族分子在沸石上的吸附热的方法。

项目成果

Cooperative effect induced by the mixing of Na-ZSM-5 and Pd/H3PW12O40/SiO2 in the selective catalytic reduction of NO with aromatic hydrocarbons

• DOI: 10.1016/j.apcatb.2007.04.008
• 发表时间: 2007-09
• 期刊: Applied Catalysis B-environmental
• 影响因子: 22.1
• 作者: R. Yoshimoto;T. Ninomiya;K. Okumura;M. Niwa

チタニア担持酸化タングステンモノレイヤー固体酸触媒によるエチレン水和

二氧化钛负载氧化钨单层固体酸催化剂乙烯水合

• 发表时间: 2007
• 作者: 片田直伸;井関洋平;志知 明;尾崎和洋;藤本憲一;椿 卓也;丹羽 幹;藤田伸夫;石野 巌
• 通讯作者: 石野 巌

アルカリ土類金属カチオン交換によるY型ゼオライトの酸性質と触媒活性の変化

碱土金属阳离子交换对Y型沸石酸性性能和催化活性的影响

• 发表时间: 2007
• 作者: 野田敬之;鈴木克生;片田直伸;丹羽 幹
• 通讯作者: 丹羽 幹

Thermal Transformation Process of a Keggin-Type Mixed Heteropoly Acid, H4PNbW 11O40, the Precursor of the H3PO4-WO3-Nb2O5 Catalyst

Keggin 型混合杂多酸 H4PNbW 11O40（H3PO4-WO3-Nb2O5 催化剂前体）的热转化过程

• 发表时间: 2007
• 期刊: J. Catal 245
• 作者: K. Okumura;K. Yamashita;K. Yamada;M. Niwa
• 通讯作者: M. Niwa

Changes in Acidic and Catalytic Properties by Cation Exchange of Y Zeolite with Alkaline Earths

Y型沸石与碱土的阳离子交换导致酸性和催化性能的变化

• 发表时间: 2007
• 作者: Takayuki;Noda;et. al.
• 通讯作者: et. al.