CAREER: Increasing Catalytic Selectivity for Isomerization of Glucose to Fructose using Paired Lewis Acid Sites

职业：使用成对路易斯酸位点提高葡萄糖异构化为果糖的催化选择性

• 批准号: 1653587
• 负责人: Nicholas Brunelli
• 金额: $ 52.97万
• 依托单位: Ohio State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2017
• 资助国家: 美国
• 起止时间: 2017-03-01 至 2023-02-28
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1653587&HistoricalAwards=false
• 关键词: CAREER; Increasing; Catalytic; Selectivity; Isomerization

The study targets design of heterogeneous catalysts for the liquid-phase isomerization of glucose to fructose, a key step in the valorization of biomass to chemicals and fuels. The authors utilize a bio-inspired catalyst design approach that has the potential to reduce cost of bio-renewable processing, increasing the economic competitiveness with fossil fuel sources of bio-derived chemicals and fuels. Integrated into the catalyst design approach is an educational outreach program that will increase participation of women and underrepresented minorities in STEM fields.Specifically, the PI seeks to synthesize catalytic materials containing well-defined paired catalytic sites on a solid silica support to increase the catalytic activity and selectivity for the isomerization of glucose to fructose. The paired site design utilizes a bio-inspired approach, translating the paired catalytic site of enzymes into a heterogeneous catalytic material. The proposed work will focus on developing a hydrothermal synthesis method that will incorporate paired sites into the zeolite framework. The work will seek to tune the catalytic performance through changing the composition of the pairs to demonstrate the mechanistic impact of paired sites. The study will also develop advanced spectroscopic methods to help identify the formation of paired catalytic sites. The technological impact of the project can be substantial since it will add a new dimension to the ability to tune catalytic performance and provide a method to increase the selectivity for biomass conversion to fructose and decrease associated energy costs. Overall, this would create a more economically viable route than currently available to produce high fructose corn syrup, biomass-derived polymers, or commodity chemicals. The work will be performed by a diverse team of students that will be trained in advanced catalytic material synthesis and testing. In addition to undergraduate and graduate education opportunities, the project will interface with several existing programs at Ohio State University to create a classroom module for students and a project to introduce the concepts of size-selective separation of zeolitic materials ? a critical feature of these materials ? to elementary school children to inspire future generations to pursue education in STEM-related fields. The filtration module will be made available through the PI website to expand the impact of the outreach efforts.

该研究的目标是设计用于葡萄糖液相异构化为果糖的多相催化剂，这是将生物质转化为化学品和燃料的关键步骤。作者利用仿生催化剂设计方法，该方法有可能降低生物可再生加工的成本，提高生物衍生化学品和燃料与化石燃料来源的经济竞争力。催化剂设计方法中融入了一项教育推广计划，该计划将增加女性和代表性不足的少数群体在 STEM 领域的参与。具体来说，PI 寻求合成在固体二氧化硅载体上包含明确配对催化位点的催化材料，以提高催化活性以及葡萄糖异构化为果糖的选择性。配对位点设计采用仿生方法，将酶的配对催化位点转化为异质催化材料。拟议的工作将集中于开发一种水热合成方法，将配对位点纳入沸石框架中。这项工作将寻求通过改变配对的组成来调整催化性能，以证明配对位点的机械影响。该研究还将开发先进的光谱方法来帮助识别配对催化位点的形成。该项目的技术影响可能是巨大的，因为它将为调整催化性能的能力增加一个新的维度，并提供一种提高生物质转化为果糖的选择性并降低相关能源成本的方法。总体而言，这将创造一条比目前生产高果糖玉米糖浆、生物质衍生聚合物或商品化学品更经济可行的路线。这项工作将由一个多元化的学生团队来完成，他们将接受先进催化材料合成和测试的培训。除了本科生和研究生教育机会外，该项目还将与俄亥俄州立大学的几个现有项目相结合，为学生创建一个课堂模块和一个介绍沸石材料尺寸选择性分离概念的项目？这些材料的一个关键特性是什么？面向小学生，激励后代追求 STEM 相关领域的教育。过滤模块将通过 PI 网站提供，以扩大外展工作的影响。

项目成果

Utilizing imogolite nanotubes as a tunable catalytic material for the selective isomerization of glucose to fructose

利用伊毛缟石纳米管作为可调催化材料用于葡萄糖选择性异构化为果糖

• DOI: 10.1016/j.cattod.2018.07.059
• 发表时间: 2019-02-15
• 期刊: Catalysis Today
• 影响因子: 5.3
• 作者: Nathaniel S. Olson;N. Deshp;e;e;S. Gunduz;U. Ozkan;N. Brunelli
• 通讯作者: N. Brunelli

Synthesis and catalytic testing of Lewis acidic nano zeolite Beta for epoxide ring opening with alcohols

Lewis酸性纳米β沸石的合成及醇类环氧化物开环催化测试

• DOI: 10.1016/j.apcata.2019.03.009
• 发表时间: 2019-05-05
• 期刊: Applied Catalysis A: General
• 作者: Aamena Parulkar;Ale;er P. Spanos;er;N. Deshp;e;e;N. Brunelli
• 通讯作者: N. Brunelli

Investigating the impact of micropore volume of aminosilica functionalized SBA-15 on catalytic activity for amine-catalyzed reactions

研究氨基二氧化硅功能化SBA-15的微孔体积对胺催化反应的催化活性的影响

• DOI: 10.1016/j.jcat.2022.09.016
• 发表时间: 2022-10
• 期刊: Journal of Catalysis
• 影响因子: 7.3
• 作者: Deshpande, Nitish;Chen, Jee;Kobayashi, Takeshi;Cho, Eun Hyun;Pineault, Hannah;Lin, Li;Brunelli, Nicholas A.
• 通讯作者: Brunelli, Nicholas A.

Jet-mixing reactor for the production of monodisperse silver nanoparticles using a reduced amount of capping agent

使用减少量的封端剂生产单分散银纳米粒子的喷射混合反应器

• DOI: 10.1039/c9re00152b
• 发表时间: 2019-09-27
• 期刊: Reaction Chemistry & Engineering
• 影响因子: 3.9
• 作者: Pinaki Ranadive;Aamena Parulkar;N. Brunelli
• 通讯作者: N. Brunelli

Enhancing hydrophobicity and catalytic activity of nano-Sn-Beta for alcohol ring opening of epoxides through post-synthetic treatment with fluoride

通过氟化物后合成处理增强纳米Sn-Beta的疏水性和对环氧化物醇开环的催化活性

• DOI: 10.1016/j.jcat.2021.10.023
• 发表时间: 2021-12
• 期刊: Journal of Catalysis
• 影响因子: 7.3
• 作者: Spanos, Alexander P.;Parulkar, Aamena;Brunelli, Nicholas A.
• 通讯作者: Brunelli, Nicholas A.