CAREER: Synthesis Methods to Control Framework Aluminum Distribution in Zeolites for NOx Pollution Abatement Catalysis

职业：控制沸石中骨架铝分布的合成方法，用于氮氧化物污染减排催化

• 批准号: 1552517
• 负责人: Rajamani Gounder
• 金额: $ 51.7万
• 依托单位: Purdue University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2016
• 资助国家: 美国
• 起止时间: 2016-02-15 至 2021-01-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1552517&HistoricalAwards=false
• 关键词: CAREER; Synthesis; Methods; Control; Framework

Abstract (Gounder; 1552517)This study will develop new synthesis strategies to control the distribution of aluminum (Al) active sites in zeolite catalysts used for nitrogen oxides (NOx) abatement and carbon feedstock conversion to fuels and chemicals. Tailoring active site proximity and distribution in zeolites will open new opportunities for catalytic innovation in both the environmental protection and carbon conversion areas, while also providing new insight into the chemistry of zeolite crystallization. The research will be linked with educational and mentoring initiatives in the STEM areas for students at all levels.Currently, there is little understanding of the relationships between the atomic arrangement of Al atoms in zeolites and the chemistry of the precursor solutions and gels used to synthesize them. This work is based on the hypothesis that the distribution of catalytically-relevant isolated and paired Al sites in zeolites can be controlled by the charge density of the synthesis gel. Isolated and paired Al sites have been shown by the principal investigator to play important roles in the selective catalytic reduction (SCR) of NOx using copper (Cu)-exchanged chabazite zeolites. The present study will develop predictive relations between synthesis gel charge density and paired Al density for a range of zeolites, establish relationships between the framework Al distribution and extraframework Cu distribution in Cu-zeolites, and determine their kinetic and mechanistic roles in the NOx SCR reaction. Building on prior collaborative research, the PI will utilize characterization tools that provide rapid quantification of the numbers of total and paired acid sites on proton- and metal-exchanged zeolites, thereby facilitating the development of synthesis-structure-function relationships that can be used to tailor zeolites for a range of applications.

摘要（Gounder;本研究将开发新的合成策略，以控制用于氮氧化物（NOx）减排和碳原料转化为燃料和化学品的沸石催化剂中铝（Al）活性位点的分布。 定制沸石中活性位点的接近度和分布将为环境保护和碳转化领域的催化创新开辟新的机会，同时也为沸石结晶的化学提供新的见解。 该研究将与STEM领域的教育和指导计划联系起来，面向各级学生。目前，人们对沸石中Al原子的原子排列与用于合成它们的前体溶液和凝胶的化学性质之间的关系知之甚少。 这项工作是基于这样的假设，即在沸石中的催化相关的孤立和配对的Al位点的分布可以通过合成凝胶的电荷密度来控制。 主要研究者已经表明，孤立的和成对的Al位点在使用铜（Cu）交换的菱沸石的NOx的选择性催化还原（SCR）中发挥重要作用。 本研究将开发一系列沸石的合成凝胶电荷密度和成对Al密度之间的预测关系，建立铜沸石中骨架Al分布和骨架外Cu分布之间的关系，并确定它们在NOx SCR反应中的动力学和机械作用。 在先前合作研究的基础上，PI将利用表征工具，快速定量质子和金属交换沸石上的总酸位点和成对酸位点的数量，从而促进合成-结构-功能关系的发展，这些关系可用于定制沸石的一系列应用。

项目成果

Mechanistic origins of the high-pressure inhibition of methanol dehydration rates in small-pore acidic zeolites

• DOI: 10.1016/j.jcat.2019.10.012
• 发表时间: 2019-12-01
• 期刊: JOURNAL OF CATALYSIS
• 影响因子: 7.3
• 作者: Di Iorio, John R.;Hoffman, Alexander J.;Gounder, Rajamani
• 通讯作者: Gounder, Rajamani

Introducing Catalytic Diversity into Single-Site Chabazite Zeolites of Fixed Composition via Synthetic Control of Active Site Proximity

• DOI: 10.1021/acscatal.7b01273
• 发表时间: 2017-10-01
• 期刊: ACS CATALYSIS
• 影响因子: 12.9
• 作者: Di Iorio, John R.;Nimlos, Claire T.;Gounder, Rajamani
• 通讯作者: Gounder, Rajamani

Effects of dioxygen pressure on rates of NOx selective catalytic reduction with NH3 on Cu-CHA zeolites

• DOI: 10.1016/j.jcat.2020.05.022
• 发表时间: 2020-09-01
• 期刊: JOURNAL OF CATALYSIS
• 影响因子: 7.3
• 作者: Jones, Casey B.;Khurana, Ishant;Gounder, Rajamani
• 通讯作者: Gounder, Rajamani

Spectroscopic and kinetic responses of Cu-SSZ-13 to SO2 exposure and implications for NOx selective catalytic reduction

• DOI: 10.1016/j.apcata.2019.01.024
• 发表时间: 2019-03
• 期刊: Applied Catalysis A: General
• 作者: Arthur J. Shiha;Ishant Khuranaa;Hui Lib;Juan Gonzáleza;Ashok Kumard;Christopher Paoluccib;Trevor M. Lardinoisa;Casey B. Jonesa;Jonatan D. Albarracin Caballeroa;Krishna Kamasamudramd;Aleksey Yezeretsd;W. N. Delgassa;Jeffrey T. Millera;Aída Luz Villac;William F. Schneiderb;Rajamani Goundera;Fabio H. Ribeiroa

Demonstrating Concepts in Catalysis, Renewable Energy, and Chemical Safety with the Catalytic Oxidation of Hydrogen

通过氢催化氧化展示催化、可再生能源和化学安全方面的概念

• DOI: 10.1021/acs.jchemed.1c00188
• 发表时间: 2021
• 期刊: Journal of Chemical Education
• 影响因子: 3
• 作者: Cybulskis, Viktor J.;Gawecki, Piotr;Zvinevich, Yury;Gounder, Rajamani;Ribeiro, Fabio H.
• 通讯作者: Ribeiro, Fabio H.