Collaborative Research: SusChEM: Manipulation of Reaction Selectivity in the electrochemical environment for biomass-to-chemicals conversions
合作研究:SusChEM:生物质到化学品转化的电化学环境中反应选择性的操纵
基本信息
- 批准号:1665176
- 负责人:
- 金额:$ 43万
- 依托单位:
- 依托单位国家:美国
- 项目类别:Continuing Grant
- 财政年份:2017
- 资助国家:美国
- 起止时间:2017-09-01 至 2020-08-31
- 项目状态:已结题
- 来源:
- 关键词:
项目摘要
Manipulation of reaction selectivity in the electrochemical environment for biomass-to-chemicals conversions Fuels and chemicals derived from plant matter (biomass) are a promising means to sustainably meet demands for energy and commodity products. Biomass is a "carbon neutral" feedstock because it grows by incorporating CO2 from the atmosphere while only consuming solar energy. This project is finding new and efficient outlets to generate useful chemicals from components of biomass that are currently difficult to process. While most biomass conversions are presently performed using catalysts and energy supplied by heat, this work is exploiting unique aspects of electricity-driven catalytic reactions in order to achieve synthesis of useful chemicals at low temperatures and pressures. The electricity required for these processes may, in turn, be derived from renewable sources such as wind and solar. A fundamental approach is being taken in which experimental techniques that probe the nature of the catalytic reactions are combined with computer simulations to build a comprehensive picture of the factors that govern reaction selectivity and to design more efficient processes. Insights from this work have broader application in extending the scope of green chemistry. This research is also being used to promote science education by involving undergraduate student researchers for summer internships, and the PI's are additionally developing a series of interactive educational modules related to understanding the physical processes governing electro-catalytic reactions. This project is investigating electrochemical control over selectivity in the conversion of biomass-derived feedstocks to desired chemical targets. Electrochemical conversions offer advantages in sustainable processing since they generally operate at low temperatures and utilize aqueous feedstocks directly. Using selective oxidation of furfural and 5-hydroxymethyl furfural over Pt electrodes as probe systems, this work focuses on determining the different mechanisms by which selectivity can be manipulated through control over electrode potential and composition. Mechanisms being explored include differentiation of charge-transfer reactions relative to neutral atom transfer reactions, variation in surface coverage of oxygen and organic species, and the role of promoters with specific reactivity or geometry. Three complementary research approaches are being integrated to characterize these effects. Measurement of electrochemical kinetics on metal catalysts is combined with in-situ spectroscopy to identify reaction pathways; surface science experiments are used on a model Pt(111) surface to study oxidation elementary steps in detail; and finally, density functional theory calculations are used to investigate the same surface chemistry, including simulation of electric potential effects and the water-metal interface. The three research thrusts provide complementary information and enrich the depth of understanding of the electrochemical environment. Insights from this work have broader application in extending the scope of green chemistry and electrochemical synthetic routes. This research is also being used to promote science education by involving undergraduate student researchers for summer internships, and the PI's are additionally developing a series of interactive educational modules related to understanding the physical processes governing electro-catalytic reactions.
生物质化学转化电化学环境中反应选择性的控制 从植物物质(生物质)中提取的燃料和化学品是可持续地满足能源和商品需求的一种有希望的手段。生物质是一种“碳中性”原料,因为它通过吸收大气中的二氧化碳而生长,同时只消耗太阳能。该项目正在寻找新的有效途径,从目前难以加工的生物质成分中生产有用的化学品。 虽然目前大多数生物质转化是使用催化剂和热量提供的能量进行的,但这项工作正在利用电力驱动催化反应的独特方面,以便在低温和低压下合成有用的化学品。这些过程所需的电力又可以来自风能和太阳能等可再生能源。一个基本的方法正在采取的实验技术,探测催化反应的性质与计算机模拟相结合,以建立一个全面的图片的因素,控制反应的选择性和设计更有效的过程。从这项工作的见解有更广泛的应用在扩大绿色化学的范围。这项研究也被用来促进科学教育,让本科生研究人员参加暑期实习,PI还开发了一系列与理解电催化反应的物理过程有关的互动教育模块。 该项目正在研究生物质衍生原料转化为所需化学目标的选择性电化学控制。电化学转化在可持续加工中具有优势,因为它们通常在低温下操作并直接利用含水原料。 利用糠醛和5-羟甲基糠醛在铂电极上的选择性氧化作为探针系统,这项工作的重点是确定不同的机制,可以通过控制电极电位和组成来操纵选择性。正在探讨的机制包括分化的电荷转移反应相对于中性原子转移反应,在表面覆盖的氧和有机物种的变化,和特定的反应性或几何形状的促进剂的作用。三个互补的研究方法正在整合这些影响的特点。金属催化剂上的电化学动力学测量与原位光谱相结合,以确定反应途径;表面科学实验用于模型Pt(111)表面,以详细研究氧化基本步骤;最后,密度泛函理论计算用于研究相同的表面化学,包括模拟电势效应和水-金属界面。这三个研究重点提供了互补的信息,丰富了对电化学环境的理解深度。 从这项工作的见解在扩大绿色化学和电化学合成路线的范围有更广泛的应用。这项研究也被用来促进科学教育,让本科生研究人员参加暑期实习,PI还开发了一系列与理解电催化反应的物理过程有关的互动教育模块。
项目成果
期刊论文数量(6)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
Identifying “Optimal” Electrocatalysts: Impact of Operating Potential and Charge Transfer Model
识别“最佳”电催化剂:工作潜力和电荷转移模型的影响
- DOI:10.1021/acscatal.7b03235
- 发表时间:2017
- 期刊:
- 影响因子:12.9
- 作者:Román, Alex M.;Dudoff, Jessica;Baz, Adam;Holewinski, Adam
- 通讯作者:Holewinski, Adam
Accelerating Electro-oxidation Turnover Rates via Potential-Modulated Stimulation of Electrocatalytic Activity
- DOI:10.1021/acs.iecr.0c04414
- 发表时间:2020-11
- 期刊:
- 影响因子:4.2
- 作者:A. Román;Taylor D. Spivey;J. Medlin;Adam Holewinski
- 通讯作者:A. Román;Taylor D. Spivey;J. Medlin;Adam Holewinski
Insight into the Oxidation Mechanism of Furanic Compounds on Pt(111)
呋喃类化合物在Pt(111)上的氧化机理研究
- DOI:10.1021/acscatal.9b03983
- 发表时间:2019
- 期刊:
- 影响因子:12.9
- 作者:Mark, Lesli O.;Agrawal, Naveen;Román, Alex M.;Holewinski, Adam;Janik, Michael J.;Medlin, J. Will
- 通讯作者:Medlin, J. Will
Elucidating Acidic Electro-Oxidation Pathways of Furfural on Platinum
- DOI:10.1021/acscatal.9b02656
- 发表时间:2019-11-01
- 期刊:
- 影响因子:12.9
- 作者:Roman, Alex M.;Hasse, Joseph C.;Holewinski, Adam
- 通讯作者:Holewinski, Adam
Electro-oxidation of furfural on gold is limited by furoate self-assembly
- DOI:10.1016/j.jcat.2020.08.034
- 发表时间:2020-11-01
- 期刊:
- 影响因子:7.3
- 作者:Roman, Alex M.;Agrawal, Naveen;Holewinski, Adam
- 通讯作者:Holewinski, Adam
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Adam Holewinski其他文献
Impact of pretreatment and thiol modifiers on the partial oxidation of glutaraldehyde using Pd/Alsub2/subOsub3/sub
预处理和硫醇改性剂对使用 Pd/Al₂O₃ 进行戊二醛部分氧化的影响
- DOI:
10.1016/j.apcata.2023.119229 - 发表时间:
2023-07-05 - 期刊:
- 影响因子:4.800
- 作者:
Faysal M. Al Khulaifi;Yousef A. Alsunni;Charles B. Musgrave;Adam Holewinski;J. Will Medlin - 通讯作者:
J. Will Medlin
Predicting macro-kinetic observables with the generalized degree of rate control in electrocatalysis
用电催化中速率控制的广义程度来预测宏观动力学可观测值
- DOI:
- 发表时间:
2021 - 期刊:
- 影响因子:0
- 作者:
A. Baz;Adam Holewinski - 通讯作者:
Adam Holewinski
Hydride transfer gets a recharge
氢化物转移得到了补充
- DOI:
10.1038/s41929-023-00946-z - 发表时间:
2023-04-26 - 期刊:
- 影响因子:44.600
- 作者:
Adam Holewinski - 通讯作者:
Adam Holewinski
Electrochemical reduction selectivity of crotonaldehyde on copper
巴豆醛对铜的电化学还原选择性
- DOI:
- 发表时间:
2020 - 期刊:
- 影响因子:2.9
- 作者:
Zachary J. Barton;G. H. Garrett;Nicholas Kurtyka;Taylor D. Spivey;Joshua A. Schaidle;Adam Holewinski - 通讯作者:
Adam Holewinski
Adam Holewinski的其他文献
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{{ truncateString('Adam Holewinski', 18)}}的其他基金
Understanding electrochemical hydrogenation reactions over post-transition metal electrodes: the role of incidental mediators and metastable phases
了解后过渡金属电极上的电化学氢化反应:偶然介体和亚稳态相的作用
- 批准号:
2301381 - 财政年份:2023
- 资助金额:
$ 43万 - 项目类别:
Standard Grant
NSF-DFG Echem: CAS: Cooperativity Between Immobilized Redox Mediators for Selective Anodic Biomass Valorization
NSF-DFG Echem:CAS:固定化氧化还原介体之间的协同作用,用于选择性阳极生物质增值
- 批准号:
2055689 - 财政年份:2021
- 资助金额:
$ 43万 - 项目类别:
Standard Grant
CAREER: Understanding Bifunctionality in Organic Electro-oxidation Catalysis
职业:了解有机电氧化催化中的双功能
- 批准号:
1944834 - 财政年份:2020
- 资助金额:
$ 43万 - 项目类别:
Continuing Grant
MRI: Acquisition of a High-Sensitivity Low-Energy Ion Scattering (HS-LEIS) Spectrometer with Multiple Reactive Environment Transfer for Interrogating Surfaces and Interfaces
MRI:获取具有多个反应环境传输功能的高灵敏度低能量离子散射 (HS-LEIS) 光谱仪,用于询问表面和界面
- 批准号:
1919845 - 财政年份:2019
- 资助金额:
$ 43万 - 项目类别:
Standard Grant
EAGER: Identifying Active Sites in Electrocatalysis by Steady-State Isotope-Transient Technique
EAGER:通过稳态同位素瞬态技术识别电催化活性位点
- 批准号:
1835967 - 财政年份:2018
- 资助金额:
$ 43万 - 项目类别:
Standard Grant
Mixed Ion Electron Conductor (MIEC) Cascade Electrodes for High Density Energy Storage in Li2O2
用于 Li2O2 高密度储能的混合离子电子导体 (MIEC) 级联电极
- 批准号:
1806059 - 财政年份:2018
- 资助金额:
$ 43万 - 项目类别:
Standard Grant
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