CAREER:Elucidating Molecular Level Interplay Between Catalysts and Electrolytes in Electrochemical Reduction of CO2
职业:阐明二氧化碳电化学还原过程中催化剂和电解质之间的分子水平相互作用
基本信息
- 批准号:1651625
- 负责人:
- 金额:$ 52.35万
- 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:2017-02-15 至 2022-01-31
- 项目状态:已结题
- 来源:
- 关键词:
项目摘要
The project addresses electrochemical reduction of the greenhouse gas carbon dioxide (ERCO2) - a critical step in sustainable strategies for generating fuels and commodity chemicals. More efficient and cost-effective routes for ERCO2 are needed for technological viability. In particular, interactions between the electrolyte and the electrocatalyst in ERCO2 cells are largely responsible for the overall performance of the system, yet are not well understood. The project addresses this need by employing a suite of advanced chemical characterization techniques to gain insight for the design of more effective polymer electrolytes and nanostructured catalysts. The project will also increase education and public awareness of the economic and environmental impact of electrochemical processes for converting CO2 to fuels and chemicals.A combination of in-situ surface-specific spectroscopic, electrokinetic, and isotope labeling techniques will be employed to elucidate the mechanism of the electrode surface-mediated ECRCO2 and its interplay with cations and anions in the electrolyte at the molecular level. Bicarbonate, the most commonly used anion in ECRCO2, is proposed to enhance the reaction rate by increasing the effective CO2 concentration at the electrode surface via the dynamic CO2-bicarbonate equilibrium. Moreover, electrostatically bound cations could reduce the access of reactants to the surface via site blocking at negative electrode potentials. Correlation between the structure of organic cations and the site blocking effect will be established. Insights gained in these mechanistic studies will be used in the design of polymer electrolytes for future ECRCO2 devices. Further, design principles for nanostructured catalysts with minimum transport limitation will be extracted by developing an experimental method to measure the pH, and in turn CO2 concentration, within 10 nm from the electrode surface in-situ. More broadly, special emphasis will be paid to attracting and retaining students from underrepresented groups in science, technology, engineering and mathematics (STEM) programs via a mobile device based software platform (the "GreenTech" app) to provide education and awareness of the need for sustainable and environmentally benign energy utilization.
该项目涉及温室气体二氧化碳(ERCO 2)的电化学还原-这是产生燃料和商品化学品的可持续战略的关键一步。 为了技术可行性,需要更有效和更具成本效益的ERCO 2路线。 特别是,ERCO 2电池中电解质和电催化剂之间的相互作用在很大程度上决定了系统的整体性能,但尚未得到很好的理解。该项目通过采用一套先进的化学表征技术来解决这一需求,以获得设计更有效的聚合物电解质和纳米结构催化剂的洞察力。该项目还将提高教育和公众对电化学过程的经济和环境影响的认识,以将CO2转化为燃料和化学品。结合原位表面特异性光谱,电动力学和同位素标记技术,将在分子水平上阐明电极表面介导的ECRCO 2及其与电解质中阳离子和阴离子相互作用的机制。重碳酸根是ECRCO 2中最常用的阴离子,通过动态CO2-碳酸氢根平衡提高电极表面的有效CO2浓度来提高反应速率。此外,静电结合的阳离子可以通过在负电极电位下的位点阻断来减少反应物对表面的访问。将建立有机阳离子结构和位点阻断效应之间的相关性。在这些机理研究中获得的见解将用于未来ECRCO 2设备的聚合物电解质的设计。此外,纳米结构的催化剂与最小的传输限制的设计原则将提取开发一种实验方法来测量的pH值,并反过来CO2浓度,在10 nm内从电极表面原位。 更广泛地说,将特别重视通过基于移动终端的软件平台(“GreenTech”应用程序)吸引和留住科学、技术、工程和数学(STEM)课程中代表性不足的群体的学生,以提供可持续和环保能源利用的教育和意识。
项目成果
期刊论文数量(7)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
Potential Routes and Mitigation Strategies for Contamination in Interfacial Specific Infrared Spectroelectrochemical Studies
- DOI:10.1021/acs.jpcc.8b05634
- 发表时间:2018-11-01
- 期刊:
- 影响因子:3.7
- 作者:Dunwell, Marco;Yang, Xuan;Xu, Bingjun
- 通讯作者:Xu, Bingjun
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Bingjun Xu其他文献
Coupled cation–electron transfer at the Pt(111)/perfluoro-sulfonic acid ionomer interface and its impact on the oxygen reduction reaction kinetics
铂(111)/全氟磺酸离聚物界面处的耦合阳离子-电子转移及其对氧还原反应动力学的影响
- DOI:
10.1038/s41929-024-01279-1 - 发表时间:
2025-01-13 - 期刊:
- 影响因子:44.600
- 作者:
Kaiyue Zhao;Mingchuan Luo;Yongfan Zhang;Xiaoxia Chang;Bingjun Xu - 通讯作者:
Bingjun Xu
Dual-function of alcohols in gold-mediated selective coupling of amines and alcohols.
金介导的胺和醇的选择性偶联中醇的双重功能。
- DOI:
10.1002/chem.201103232 - 发表时间:
2012 - 期刊:
- 影响因子:0
- 作者:
Bingjun Xu;R. Madix;C. Friend - 通讯作者:
C. Friend
Facilitating catalytic research via better data reporting and curation: A case study of propane dehydrogenation on Ga/H-ZSM-5
- DOI:
10.1016/j.jcat.2024.115838 - 发表时间:
2024-12-01 - 期刊:
- 影响因子:
- 作者:
Zhaoqi Zhao;Bingjun Xu - 通讯作者:
Bingjun Xu
Erratum to: Origin and effect of surface oxygen-containing species on electrochemical CO or CO2 reduction reactions
- DOI:
10.1007/s11426-023-1736-3 - 发表时间:
2023-10-20 - 期刊:
- 影响因子:9.700
- 作者:
Xiaoxia Chang;Ming He;Qi Lu;Bingjun Xu - 通讯作者:
Bingjun Xu
π-Interactions between Cyclic Carbocations and Aromatics Cause Zeolite Deactivation in Methanol-to-Hydrocarbon Conversion
- DOI:
10.3866/pku.whxb202012031 - 发表时间:
2020 - 期刊:
- 影响因子:10.9
- 作者:
Bingjun Xu - 通讯作者:
Bingjun Xu
Bingjun Xu的其他文献
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{{ truncateString('Bingjun Xu', 18)}}的其他基金
Hydrogen oxidation reaction at alkaline polymer electrochemical interfaces: Achieving mechanistic understanding through surface sensitive spectroscopy
碱性聚合物电化学界面的氢氧化反应:通过表面敏感光谱实现机理理解
- 批准号:
1566138 - 财政年份:2016
- 资助金额:
$ 52.35万 - 项目类别:
Standard Grant
Production of Renewable Acrylic Acid via Catalytic Dehydration of Lactic Acid: Mechanistic Studies and Catalysts Design
通过乳酸催化脱水生产可再生丙烯酸:机理研究和催化剂设计
- 批准号:
1437129 - 财政年份:2014
- 资助金额:
$ 52.35万 - 项目类别:
Standard Grant
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