SusChEM: A Mechanistic Approach to Understanding and Lowering the Overpotential for CO2 Reduction to C1 Organic Products

SusChEM:一种理解和降低 CO2 还原为 C1 有机产品的过电势的机械方法

基本信息

  • 批准号:
    1308652
  • 负责人:
  • 金额:
    $ 42万
  • 依托单位:
  • 依托单位国家:
    美国
  • 项目类别:
    Standard Grant
  • 财政年份:
    2013
  • 资助国家:
    美国
  • 起止时间:
    2013-09-15 至 2017-08-31
  • 项目状态:
    已结题

项目摘要

The NSF Chemical Catalysis Program supports the efforts of Professor Andrew B. Bocarsly of Princeton University to investigate the mechanisms of carbon dioxide (CO2) reduction to one carbon (C1) organic products: formic acid, formaldedhyde or methanol. In the case of methanol, a 6-electron, 6-proton reaction is required which can be undertaken using either a one-electron redox mediator or in some cases can be observed to occur via a direct CO2-surface interaction. In all cases, a complex reaction mechanism is implicated. The research group examines the rate limiting step(s) associated with the formation of formate, one of the major reaction products. Heterogeneous CO2 reduction at post-transition metal oxide interfaces, interface-free CO2 reduction using transition metal based molecular systems, and cyanogel systems for CO2 electroreduction are under study. The first two topics explore the critical question of the role of a reactive surface in the reaction pathway. To consider this question under kinetically limiting conditions leading to formate formation, the team examines anodized post transition metal electrodes. These materials are catalytic in the absence of an additional dissolved catalyst, allowing the research group to look specifically at the range of heterogeneous processes occurring directly at the electrode interface during CO2 reduction. The study is organized using periodic trends, with zinc, cadmium, indium, bismuth and lead selected as key systems. The second study attacks the problem from the opposite direction. In this study, aromatic amine catalysts are used to carry-out the reduction of CO2 in the absence of a surface. Here, advantage is taken of the photoexcited ruthenium(bipyridyl) systems, charge transfer quenched by an aromatic amine to generate CO2 reduction absent an electrode interface. The team also explores manganese complexes containing bisphosphinine (L2) ligands, in this regard. The final study uses cyanogel chemistry to both generate alloy materials that will facilitate the electrode-based studies, and to produce novel electrolytes that are known to have a high CO2 capacity. Understanding CO2 activation is a critical chemical challenge as it contributes to the development of new fuel resources and as well as potentially lowering greenhouse gases in the environment. In addition to its pivotal role in the education of next generation electrochemical researchers, who are key to an alternate energy future, this program impacts K-12 education by providing an excellent tool for teaching both students and teachers fundamental chemical concepts using the currently topical problem of greenhouse gas control as a motivating principle. Another important aspect of the proposed program is its close affiliation with an aggressive startup company that is focused on taking this research out of the laboratory and into the real world. Demonstration scale systems that will convert CO2 into commercial chemicals are planned.
美国国家科学基金会化学催化计划支持安德鲁教授B的努力。Bocarsly等研究了二氧化碳(CO2)还原为一碳(C1)有机产物:甲酸、甲醛或甲醇的机理。 在甲醇的情况下,需要6-电子、6-质子反应,其可以使用单电子氧化还原介体进行,或者在某些情况下可以观察到通过直接CO2-表面相互作用发生。 在所有情况下,都涉及复杂的反应机制。该研究小组研究了与甲酸盐形成相关的限速步骤,甲酸盐是主要反应产物之一。在后过渡金属氧化物界面处的非均相CO2还原、使用基于过渡金属的分子系统的无界面CO2还原以及用于CO2电还原的氰基凝胶系统正在研究中。前两个主题探讨了反应途径中的反应表面的作用的关键问题。 为了在导致甲酸盐形成的动力学限制条件下考虑这个问题,研究小组检查了阳极化后过渡金属电极。这些材料在没有额外溶解催化剂的情况下具有催化作用,使研究小组能够专门研究CO2还原过程中直接在电极界面发生的非均相过程的范围。本研究采用周期趋势组织,锌、镉、铟、铋和铅被选为关键系统。第二项研究从相反的方向攻击这个问题。在这项研究中,芳香胺催化剂用于进行CO2的还原在没有表面。在这里,利用光激发的钌(联吡啶)系统,电荷转移猝灭的芳香胺,以产生CO2还原缺乏电极界面。在这方面,该团队还探索了含有双膦(L2)配体的锰络合物。最后的研究使用氰凝胶化学来生成合金材料,这将有助于基于电极的研究,并产生已知具有高CO2容量的新型电解质。了解二氧化碳活化是一项关键的化学挑战,因为它有助于开发新的燃料资源,并可能降低环境中的温室气体。除了在下一代电化学研究人员的教育中发挥关键作用外,他们是替代能源未来的关键,该计划还通过提供一个极好的工具来影响K-12教育,该工具用于教授学生和教师的基本化学概念,使用当前热门的温室气体控制问题作为激励原则。该计划的另一个重要方面是它与一家积极的初创公司的密切联系,该公司专注于将这项研究从实验室带到真实的世界。计划将二氧化碳转化为商业化学品的示范规模系统。

项目成果

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Andrew Bocarsly其他文献

Andrew Bocarsly的其他文献

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{{ truncateString('Andrew Bocarsly', 18)}}的其他基金

Interrelated Photo and Electrocatalytic Processes for the Reduction of CO2: Controlling Multiproton/Multielectron Events
用于还原二氧化碳的相关光催化和电催化过程:控制多质子/多电子事件
  • 批准号:
    1800400
  • 财政年份:
    2018
  • 资助金额:
    $ 42万
  • 项目类别:
    Standard Grant
Structure and Dynamics in Heterogeneous Reactions
非均相反应中的结构和动力学
  • 批准号:
    1506989
  • 财政年份:
    2015
  • 资助金额:
    $ 42万
  • 项目类别:
    Continuing Grant
Structure and Dynamics of Heterogeneous Reactions
多相反应的结构和动力学
  • 批准号:
    1213216
  • 财政年份:
    2012
  • 资助金额:
    $ 42万
  • 项目类别:
    Standard Grant
A Study of Charge Transfer Processes in the Catalyzed Conversion of Carbon Dioxide to Methanol and Higher Order Alcohols
二氧化碳催化转化为甲醇和高阶醇的电荷转移过程研究
  • 批准号:
    0911114
  • 财政年份:
    2009
  • 资助金额:
    $ 42万
  • 项目类别:
    Standard Grant
Cyanogels: From Nano-Alloys to New Materials
氰凝胶:从纳米合金到新材料
  • 批准号:
    0616475
  • 财政年份:
    2006
  • 资助金额:
    $ 42万
  • 项目类别:
    Standard Grant
Dynamics of Heterogeneous Reactions
非均相反应动力学
  • 批准号:
    0313801
  • 财政年份:
    2003
  • 资助金额:
    $ 42万
  • 项目类别:
    Continuing Grant
Dynamics of Heterogeneous Reactions
非均相反应动力学
  • 批准号:
    9986950
  • 财政年份:
    2000
  • 资助金额:
    $ 42万
  • 项目类别:
    Continuing Grant
Cyanogels: A Coordination Polymer Based System for the Synthesis of Solid-State Materials Via Sol-Gel Processing
氰凝胶:一种基于配位聚合物的系统,用于通过溶胶-凝胶加工合成固态材料
  • 批准号:
    0079169
  • 财政年份:
    2000
  • 资助金额:
    $ 42万
  • 项目类别:
    Standard Grant
Dynamics of Heterogeneous Reactions
非均相反应动力学
  • 批准号:
    9619190
  • 财政年份:
    1997
  • 资助金额:
    $ 42万
  • 项目类别:
    Continuing Grant
U.S.-India Cooperative Research: Studies of Cynometalate Modified Electrodes-Electrocatalysis and Sensor Development,Award in Indian and U.S. Currency
美印合作研究:氰金属盐修饰电极-电催化和传感器开发研究,获印度和美国货币奖
  • 批准号:
    9604863
  • 财政年份:
    1997
  • 资助金额:
    $ 42万
  • 项目类别:
    Standard Grant

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