CAREER: SusChEM: Unlocking local solvation environments for energetically efficient hydrogenations with quantum chemistry
职业:SusChEM:通过量子化学解锁局部溶剂化环境,实现高能高效氢化
基本信息
- 批准号:1653392
- 负责人:
- 金额:$ 50万
- 依托单位:
- 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:2017-02-01 至 2024-01-31
- 项目状态:已结题
- 来源:
- 关键词:
项目摘要
The project addresses the production of carbon-neutral liquid fuels via electrocatalytic reduction of the greenhouse gas carbon dioxide (CO2) to methanol. Specifically, the study seeks to improve the efficiency and selectivity of current solvent-based electrochemical processes by advancing understanding of how aqueous electrolytes participate in the overall reaction mechanisms at the atomic scale. The research will be coupled with educational thrusts that engage students in grades 8-12 in learning about renewable energy catalysis and computational chemistry.The focus of the study will be to integrate high-level electronic structure theory, molecular dynamics, and machine learning to quantitatively understand how interactions between solvent molecules, salts, and co-solutes (i.e. "local solvation environments") regulate fundamental mechanisms of CO2 reduction (CO2R) into fuels. Four basic scientific questions will be addressed related to CO2R in the presence of aromatic N-heterocycles, here studied in the form of molecules and as nitrogen-doped carbon electrodes. These are 1) the identification of the most likely chemical functionalities (i.e. Lewis base, Brønsted acid, H-atom donor, hydride donor) that participate in energetically efficient CO2R into methanol; 2) quantitative predictions of the free energy barriers for different CO2 hydrogenation processes in different local solvation environments; 3) refined understanding of the level of computational modeling needed to reliably predict hydrogenation thermodynamics and kinetics in realistic electrochemical environments; and 4) generalized insight into the degree to which local solvation environments can be tuned to enhance the conversion of low-value carbon-containing feedstocks to liquid fuels. Graduate and undergraduate students will develop educational modules that combine concepts in renewable energy and introduce computational chemistry modeling. These modules will then be tested to determine their capacity to engage and excite students in the Pittsburgh Public School District about opportunities in STEM fields.
该项目致力于通过将温室气体二氧化碳(CO2)电催化还原为甲醇来生产碳中性液体燃料。 具体而言,该研究旨在通过推进对水性电解质如何在原子尺度上参与整体反应机制的理解来提高当前基于溶剂的电化学过程的效率和选择性。 该研究将结合教育推动力,让8-12年级的学生学习可再生能源催化和计算化学。研究的重点将是整合高级电子结构理论,分子动力学和机器学习,以定量了解溶剂分子,盐,和共溶质(即“局部溶剂化环境”)调节将CO2还原(CO2 R)成燃料的基本机制。 四个基本的科学问题将解决有关CO2 R在芳香族N-杂环的存在下,在这里研究的分子和氮掺杂的碳电极的形式。 这些是1)最可能的化学功能的鉴定(即刘易斯碱、布朗斯台德酸、H原子供体、氢化物供体)参与能量有效的CO2 R转化为甲醇; 2)定量预测不同局部溶剂化环境中不同CO2加氢过程的自由能垒; 3)精确理解在现实电化学环境中可靠预测氢化热力学和动力学所需的计算建模水平;和4)对局部溶剂化环境可被调节以增强低价值含碳原料向液体燃料的转化的程度的一般性洞察。研究生和本科生将开发教育模块,结合联合收割机概念,在可再生能源和介绍计算化学建模。然后,这些模块将进行测试,以确定其吸引和激发匹兹堡公立学区学生对STEM领域机会的能力。
项目成果
期刊论文数量(16)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
Thermodynamic Hydricities of Biomimetic Organic Hydride Donors
- DOI:10.1021/jacs.7b13526
- 发表时间:2018-04-04
- 期刊:
- 影响因子:15
- 作者:Ilic, Stefan;Kadel, Usha Pandey;Glusac, Ksenija D.
- 通讯作者:Glusac, Ksenija D.
First-principles modeling of chemistry in mixed solvents: Where to go from here?
- DOI:10.1063/1.5143207
- 发表时间:2020-04
- 期刊:
- 影响因子:0
- 作者:Alex M. Maldonado;Yasemin Basdogan;J. T. Berryman;S. Rempe;J. Keith
- 通讯作者:Alex M. Maldonado;Yasemin Basdogan;J. T. Berryman;S. Rempe;J. Keith
Quantifying Uncertainties in Solvation Procedures for Modeling Aqueous Phase Reaction Mechanisms
- DOI:10.1021/acs.jpca.0c08961
- 发表时间:2021-01-04
- 期刊:
- 影响因子:2.9
- 作者:Maldonado, Alex M.;Hagiwara, Satoshi;Keith, John A.
- 通讯作者:Keith, John A.
Quantum alchemy beyond singlets: Bonding in diatomic molecules with hydrogen
单线态之外的量子炼金术:双原子分子与氢的键合
- DOI:10.1063/5.0079487
- 发表时间:2022
- 期刊:
- 影响因子:0
- 作者:Eikey, Emily A.;Maldonado, Alex M.;Griego, Charles D.;von Rudorff, Guido Falk;Keith, John A.
- 通讯作者:Keith, John A.
Benchmarking Computational Alchemy for Carbide, Nitride, and Oxide Catalysts
- DOI:10.1002/adts.201800142
- 发表时间:2019-04-01
- 期刊:
- 影响因子:3.3
- 作者:Griego, Charles D.;Saravanan, Karthikeyan;Keith, John A.
- 通讯作者:Keith, John A.
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John Keith其他文献
Evaluation of the impact of sedative medication in patients admitted with a fractured neck of femur
- DOI:
10.7861/clinmed.20-2-s18 - 发表时间:
2020-03-01 - 期刊:
- 影响因子:
- 作者:
Olympio D’Souza;John Keith;Kaung Thu;Amit Singh;Indeera Shankla - 通讯作者:
Indeera Shankla
A Simplified Risk-Ranking System for Prioritizing Toxic Pollution Sites in Low- and Middle-Income Countries
- DOI:
10.1016/j.aogh.2014.09.001 - 发表时间:
2014-07-01 - 期刊:
- 影响因子:
- 作者:
Jack Caravanos;Sandra Gualtero;Russell Dowling;Bret Ericson;John Keith;David Hanrahan;Richard Fuller - 通讯作者:
Richard Fuller
Clinico-hemodynamic correlations in ventricular septal defect in childhood
- DOI:
10.1016/s0022-3476(66)80078-1 - 发表时间:
1966-09-01 - 期刊:
- 影响因子:
- 作者:
Vera Rose;George Collins;Langford Kidd;John Keith - 通讯作者:
John Keith
John Keith的其他文献
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{{ truncateString('John Keith', 18)}}的其他基金
Collaborative Research: Regulating homogeneous and heterogeneous mechanisms in six-electron water oxidation
合作研究:调节六电子水氧化的均相和非均相机制
- 批准号:
1856460 - 财政年份:2020
- 资助金额:
$ 50万 - 项目类别:
Standard Grant
SusChEM: Machine learning blueprints for greener chelants
SusChEM:绿色螯合剂的机器学习蓝图
- 批准号:
1705592 - 财政年份:2017
- 资助金额:
$ 50万 - 项目类别:
Standard Grant
相似海外基金
Collaborative Research: SUSCHEM: Engineering Polymer-Nanocatalyst Membranes for Direct Capture of CO2 and Electrochemical Conversion to C2+ Liquid Fuel
合作研究:SUSCHEM:用于直接捕获 CO2 和电化学转化为 C2 液体燃料的工程聚合物纳米催化剂膜
- 批准号:
2324346 - 财政年份:2023
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Collaborative Research: SUSCHEM: Engineering Polymer-Nanocatalyst Membranes for Direct Capture of CO2 and Electrochemical Conversion to C2+ Liquid Fuel
合作研究:SUSCHEM:用于直接捕获 CO2 和电化学转化为 C2 液体燃料的工程聚合物纳米催化剂膜
- 批准号:
2324345 - 财政年份:2023
- 资助金额:
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SusChEM: Harnessing Stable Peroxides for Selective Nitrogen Atom and Fluoroalkyl Transfer
SusChEM:利用稳定的过氧化物进行选择性氮原子和氟烷基转移
- 批准号:
2200040 - 财政年份:2022
- 资助金额:
$ 50万 - 项目类别:
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CAREER: SusChEM: Iron Catalysts for the Reduction of Amides
职业:SusChEM:用于还原酰胺的铁催化剂
- 批准号:
2146728 - 财政年份:2021
- 资助金额:
$ 50万 - 项目类别:
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CAREER: SusChEM: Renewable Biocatalysts for Degradation of Persistent Organic Contaminants Using Synthetic Biology
职业:SusChEM:利用合成生物学降解持久性有机污染物的可再生生物催化剂
- 批准号:
2154345 - 财政年份:2021
- 资助金额:
$ 50万 - 项目类别:
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SusChEM: C-H Bond Electroactivation of Nonpolar Organic Substrates in Water: Enzyme-Mediated Reaction Pathways in Microemulsions
SusChEM:水中非极性有机底物的 C-H 键电活化:微乳液中酶介导的反应途径
- 批准号:
2035669 - 财政年份:2021
- 资助金额:
$ 50万 - 项目类别:
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CAREER: SusChEM: Copper-Catalyzed Aerobic Dehydrogenative C-C Bond Formation through sp3 C-H Bond Functionalization
职业:SusChEM:通过 sp3 C-H 键功能化铜催化有氧脱氢 C-C 键形成
- 批准号:
2028770 - 财政年份:2020
- 资助金额:
$ 50万 - 项目类别:
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SusChEM: Non-precious metal substitution into hydrogenation metal alloy catalysts deposited onto redox active supports for facile nitrate destruction in drinking water
SusChEM:用非贵金属替代沉积在氧化还原活性载体上的氢化金属合金催化剂,以轻松破坏饮用水中的硝酸盐
- 批准号:
1922504 - 财政年份:2019
- 资助金额:
$ 50万 - 项目类别:
Standard Grant
SusChEM: Collaborative Research: Identification of the critical length scales and chemistries responsible for the anti-fouling properties of heterogeneous surfaces
SusChEM:合作研究:确定负责异质表面防污性能的临界长度尺度和化学成分
- 批准号:
2023847 - 财政年份:2019
- 资助金额:
$ 50万 - 项目类别:
Standard Grant
SusChem Collaborative Research: Process Optimization of Novel Routes for the Production of bio-based Para-Xylene
SusChem 合作研究:生物基对二甲苯生产新路线的工艺优化
- 批准号:
2005905 - 财政年份:2019
- 资助金额:
$ 50万 - 项目类别:
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