| 项目编号: | 1454346
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| 项目名称: | CAREER: SusChEM: Development of Governing Mechanistic and Kinetic Models for the Selective Oxidative Cleavage of Levulinic Acid Over Supported Vanadium Oxides |
| 作者: | Jesse Bond
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| 承担单位: | Syracuse University
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| 批准年: | 2014
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| 开始日期: | 2015-01-01
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| 结束日期: | 2019-12-31
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| 资助金额: | USD530985
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| 资助来源: | US-NSF
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| 项目类别: | Standard Grant
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| 国家: | US
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| 语种: | 英语
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| 特色学科分类: | Engineering - Chemical, Bioengineering, Environmental, and Transport Systems
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| 英文关键词: | levulinic acid
; levulinic acid oxidation
; biomass
; vanadium oxide
; c4 diacid
; lewis acidity
; ongoing urban development initiative
; project
; acid site density
; c-c cleavage selectivity
; 4-oxopentanoic acid
; maleic acid
; influence
; terminal c-c cleavage
; oxidative ketone cleavage
; commercial development
; oxidative cleavage
; c-c
; microkinetic model
; succinic acid
; aerobic oxidative cleavage
; diacid formation
; vanadium loading
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| 英文摘要: | Abstract
PI: Jesse Q Bond
Proposal #: 1454346
Institution: Syracuse University
This project aims to develop a strategy for producing succinic acid and maleic acid from biomass. Traditionally, these commodity chemicals are made by oxidizing components of crude oil or natural gas, which is challenging. Instead, it may be possible to produce them more efficiently and inexpensively from sugar molecules, which can be extracted from biomass. This approach would require that we understand the reasons why certain catalysts and precursors deliver the desired products, while others do not. We anticipate that a technology that converts biomass and biomass derivatives to valuable products could help with commercial development of biomass processing industries. An educational component of the project will build a connection between Syracuse University students and communities in the city of Syracuse through service projects. The education program includes public workshops designed to improve public scientific literacy by educating participants on topics in energy and resource sustainability. Workshops will also outline effective methods for reducing society?s dependence on fossil resources and technology?s role in sustainability. The workshops will be facilitated by Syracuse University students as part of their undergraduate curriculum. These students will also work on design projects that incorporate new, energy- and resource-efficient technologies into ongoing urban development initiatives. This will allow them to use their training to improve their community and demonstrate the beneficial societal impacts of a STEM education.
This award supports the study of gas-phase, aerobic oxidative cleavage of bifunctional levulinic acid (4-oxopentanoic acid) over supported vanadium oxides to yield C4 diacids. Diacid formation occurs through cleavage of the terminal C-C bond in levulinic acid, which is not generally observed in monofunctional ketone analogs, such as 2-pentanone. The central hypothesis is that the structure and bifunctionality of levulinic acid underlie unique interactions with VOx sites that shift selectivity toward terminal C-C cleavage. The project seeks to identify descriptors that govern C-C cleavage selectivity during ketone oxidation.
This project will consider the influence of VOx speciation by measuring rates and selectivities of oxidative ketone cleavage over VOx/Al2O3 catalysts in which VOx phase and degree of polymerization are controlled by varying vanadium loading. The roles of Brønsted and Lewis acidity will be examined by studying oxidative cleavage over monolayer VOx/Al2O3 catalysts in which both acid site density and distribution are varied using acidic and basic modifiers. The influence of V-O-X bond character will be probed by comparing VOx sites on oxides that differ in reducibility. Isotopic tracing using 18O will identify the roles of lattice and chemisorbed oxygen during levulinic acid oxidation. Influences of ketone structure, steric interactions, and secondary functionality will be probed through a combination of kinetic and spectroscopic studies that contrast levulinic acid oxidation with that of various mono- and bifunctional ketone analogs. Electronic structure calculations will be used to build and parameterize a microkinetic model, which will reconcile first-principles expectations with experimental outcomes. Raman, UV-Vis, FTIR, and Temperature-Programmed spectroscopies (e.g., TPD, TPSR) will provide comprehensive characterization of site structure and chemical functionality. |
| 资源类型: | 项目
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| 标识符: | http://119.78.100.158/handle/2HF3EXSE/95235
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| Appears in Collections: | 影响、适应和脆弱性
气候减缓与适应
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| Recommended Citation: | |
Jesse Bond. CAREER: SusChEM: Development of Governing Mechanistic and Kinetic Models for the Selective Oxidative Cleavage of Levulinic Acid Over Supported Vanadium Oxides. 2014-01-01.
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