Creating Heterogeneous Organic Amines for Glucose Isomerization to Fructose

生成异质有机胺以将葡萄糖异构化为果糖

• 批准号: 2015669
• 负责人: Nicholas Brunelli
• 金额: $ 33.83万
• 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: 2020
• 资助国家: 美国
• 起止时间: 2020-08-01 至 2024-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2015669&HistoricalAwards=false
• 关键词: Creating; Heterogeneous; Organic; Amines; Glucose

This project targets the design of heterogeneous catalysts for the conversion of biomass to chemicals and fuels. The researchers will study catalyst structure and performance aspects related to catalyst stability, activity, and product selectivity. The project will support transition to a clean-energy economy by improving the design of catalysts for manufacturing fuels and chemicals from bio-renewable feedstocks rather than fossil sources. The project will involve an educational outreach component that will seek to increase participation of women and underrepresented students in science, technology, engineering and mathematics (STEM) fields.Specifically, the project will investigate the synthesis-structure-reactivity of aminosilanes immobilized on heterogeneous silica supports for the isomerization of glucose to fructose. A series of heterogeneous catalysts containing different aminosilane designs will be tested to determine how the structure of the aminosilane can be modified to increase catalyst stability. Identifying a stable aminosilane structure will have broad implications for catalytic materials for all liquid-phase chemistry. Further, the work will examine how the reaction selectivity can be increased through modifying the reaction conditions, including the concentration of glucose. The complex reaction mixtures will be analyzed using advanced mass spectrometry techniques to determine how glucose concentration impacts the species formed. Finally, spectroscopy techniques including nuclear magnetic resonance (NMR) and fourier-transform infrared spectroscopy (FTIR) will be used to investigate amine-silanol interactions. These amine-silanol interactions have been implicated in reducing the activity of aminosilica materials. The spectroscopy will provide insights on how the structure of the aminosilane impacts amine-silanol interactions. The impact of the project can be substantial since it has the potential to provide new methods to create heterogeneous catalysts for aqueous phase reactions. The project involves a diverse team of students that will be trained in advanced catalytic material synthesis, characterization, and testing. More broadly, the project will broaden participation from underrepresented groups in STEM programs through interfacing with several existing programs at Ohio State University to demonstrate a classroom module to elementary school children to inspire future generations to pursue education in STEM-related fields.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

该项目的目标是设计用于将生物质转化为化学品和燃料的多相催化剂。研究人员将研究与催化剂稳定性、活性和产物选择性相关的催化剂结构和性能方面。 该项目将通过改进催化剂的设计来支持向清洁能源经济的过渡，以利用生物可再生原料而不是化石原料制造燃料和化学品。该项目将涉及教育推广部分，旨在提高女性和代表性不足的学生在科学、技术、工程和数学 (STEM) 领域的参与。具体来说，该项目将研究固定在异质二氧化硅上的氨基硅烷的合成-结构-反应性支持葡萄糖异构化为果糖。将测试一系列含有不同氨基硅烷设计的多相催化剂，以确定如何修改氨基硅烷的结构以提高催化剂稳定性。识别稳定的氨基硅烷结构将对所有液相化学的催化材料产生广泛的影响。此外，该工作还将研究如何通过改变反应条件（包括葡萄糖浓度）来提高反应选择性。将使用先进的质谱技术分析复杂的反应混合物，以确定葡萄糖浓度如何影响形成的物质。最后，包括核磁共振（NMR）和傅立叶变换红外光谱（FTIR）在内的光谱技术将用于研究胺-硅烷醇相互作用。这些胺-硅烷醇相互作用与氨基二氧化硅材料活性的降低有关。光谱学将提供有关氨基硅烷的结构如何影响胺-硅烷醇相互作用的见解。该项目的影响可能是巨大的，因为它有可能提供新方法来创建用于水相反应的非均相催化剂。该项目涉及一个多元化的学生团队，他们将接受先进催化材料合成、表征和测试方面的培训。更广泛地说，该项目将通过与俄亥俄州立大学的几个现有项目对接，扩大代表性不足群体对 STEM 项目的参与，向小学生展示课堂模块，以激励后代接受 STEM 相关领域的教育。该奖项反映了 NSF 的法定使命，并通过使用基金会的智力价值和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

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.

Evaluating the per site activity of common mesoporous materials as supports for aminosilica catalysts for the aldol reaction and condensation

评估普通介孔材料作为氨基二氧化硅催化剂载体用于羟醛反应和缩合的每位点活性

• DOI: 10.1016/j.apcata.2022.118997
• 发表时间: 2023-01
• 期刊: Applied Catalysis A: General
• 作者: Brizes, Michael;Chen, Jee;Pineault, Hannah;Brunelli, Nicholas A.
• 通讯作者: Brunelli, Nicholas A.